Electrocatalytic oxidation of cellulose at a gold electrode.

PubMed

Sugano, Yasuhito; Latonen, Rose-Marie; Akieh-Pirkanniemi, Marceline; Bobacka, Johan; Ivaska, Ari

2014-08-01

The electrochemical properties of cellulose dissolved in NaOH solution at a Au surface were investigated by cyclic voltammetry, FTIR spectroscopy, the electrochemical quartz crystal microbalance technique, and electrochemical impedance spectroscopy. The reaction products were characterized by SEM, TEM, and FTIR and NMR spectroscopy. The results imply that cellulose is irreversibly oxidized. Adsorption and desorption of hydroxide ions at the Au surface during potential cycling have an important catalytic role in the reaction (e.g., approach of cellulose to the electrode surface, electron transfer, adsorption/desorption of the reaction species at the electrode surface). Moreover, two types of cellulose derivatives were obtained as products. One is a water-soluble cellulose derivative in which some hydroxyl groups are oxidized to carboxylic groups. The other derivative is a water-insoluble hybrid material composed of cellulose and Au nanoparticles (≈4 nm). Furthermore, a reaction scheme of the electrocatalytic oxidation of cellulose at a gold electrode in a basic medium is proposed. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electrochemical and in vitro neuronal recording characteristics of multi-electrode arrays surface-modified with electro-co-deposited gold-platinum nanoparticles.

PubMed

Kim, Yong Hee; Kim, Ah Young; Kim, Gook Hwa; Han, Young Hwan; Chung, Myung-Ae; Jung, Sang-Don

2016-02-01

In order to complement the high impedance electrical property of gold nanoparticles (Au NPs) we have performed electro-co-deposition of gold-platinum nanoparticles (Au-Pt NPs) onto the Au multi-electrode array (MEA) and modified the Au-Pt NPs surface with cell adhesive poly-D-lysine via thiol chemistry based covalent binding. The Au-Pt NPs were analyzed to have bimetallic nature not the mixture of Au NPs and Pt NPs by X-ray diffraction analysis and to have impedance value (4.0 × 10(4) Ω (at 1 kHz)) comparable to that of Pt NPs. The performance of Au-Pt NP-modified MEAs was also checked in relation to neuronal signal recording. The noise level in Au-Pt NP-modified MEAs was lower than in that of Au NP-modified MEA.

Facile fabrication of network film electrodes with ultrathin Au nanowires for nonenzymatic glucose sensing and glucose/O2 fuel cell.

PubMed

Yang, Lu; Zhang, Yijia; Chu, Mi; Deng, Wenfang; Tan, Yueming; Ma, Ming; Su, Xiaoli; Xie, Qingji; Yao, Shuozhuo

2014-02-15

We report here on the facile fabrication of network film electrodes with ultrathin Au nanowires (AuNWs) and their electrochemical applications for high-performance nonenzymatic glucose sensing and glucose/O2 fuel cell under physiological conditions (pH 7.4, containing 0.15M Cl(-)). AuNWs with an average diameter of ~7 or 2 nm were prepared and can self-assemble into robust network films on common electrodes. The network film electrode fabricated with 2-nm AuNWs exhibits high sensitivity (56.0 μA cm(-2)mM(-1)), low detection limit (20 μM), short response time (within 10s), excellent selectivity, and good storage stability for nonenzymatic glucose sensing. Glucose/O2 fuel cells were constructed using network film electrodes as the anode and commercial Pt/C catalyst modified glassy carbon electrode as cathode. The glucose/O2 fuel cell using 2-nm AuNWs as anode catalyst output a maximum power density of is 126 μW cm(-2), an open-circuit cell voltage of 0.425 V, and a short-circuit current density of 1.34 mA cm(-2), respectively. Due to the higher specific electroactive surface area of 2-nm AuNWs, the network film electrode fabricated with 2-nm AuNWs exhibited higher electrocatalytic activity toward glucose oxidation than the network film electrode fabricated with 7-nm AuNWs. The network film electrode exhibits high electrocatalytic activity toward glucose oxidation under physiological conditions, which is helpful for constructing implantable electronic devices. © 2013 Elsevier B.V. All rights reserved.

Shell-isolated nanoparticle-enhanced Raman spectroscopy study of the adsorption behaviour of DNA bases on Au(111) electrode surfaces.

PubMed

Wen, Bao-Ying; Jin, Xi; Li, Yue; Wang, Ya-Hao; Li, Chao-Yu; Liang, Miao-Miao; Panneerselvam, Rajapandiyan; Xu, Qing-Chi; Wu, De-Yin; Yang, Zhi-Lin; Li, Jian-Feng; Tian, Zhong-Qun

2016-06-21

For the first time, we used the electrochemical shell-isolated nanoparticle-enhanced Raman spectroscopy (EC-SHINERS) technique to in situ characterize the adsorption behaviour of four DNA bases (adenine, guanine, thymine, and cytosine) on atomically flat Au(111) electrode surfaces. The spectroscopic results of the various molecules reveal similar features, such as the adsorption-induced reconstruction of the Au(111) surface and the drastic Raman intensity reduction of the ring breathing modes after the lifting reconstruction. As a preliminary study of the photo-induced charge transfer (PICT) mechanism, the in situ spectroscopic results obtained on single crystal surfaces are excellently illustrated with electrochemical data.

Selective electrochemical detection of 2,4,6-trinitrotoluene (TNT) in water based on poly(styrene-co-acrylic acid) PSA/SiO2/Fe3O4/AuNPs/lignin-modified glassy carbon electrode.

PubMed

Mahmoud, Khaled A; Abdel-Wahab, Ahmed; Zourob, Mohammed

2015-01-01

A new versatile electrochemical sensor based on poly(styrene-co-acrylic acid) PSA/SiO2/Fe3O4/AuNPs/lignin (L-MMS) modified glassy carbon electrode (GCE) was developed for the selective detection of trace trinitrotoluene (TNT) from aqueous media with high sensitivity. The fabricated magnetic microspheres were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and X-ray photoelectron spectroscopy (XPS). L-MMS films were cast on the GCE surface to fabricate the TNT sensing electrode. The limit of detection (LOD) of TNT determined by the amperometric i-t curve reached 35 pM. The lignin film and well packed Fe3O4/AuNPs facilitated the pre-concentration of trace TNT on the electrode surface resulting in a fast amperometric response of 3 seconds near the detection limit. The high sensitivity and excellent catalytic activity of the modified electrode could be attributed to the lignin layer and highly packed Fe3O4/AuNPs on the electrode surface. The total recovery of TNT from tapwater and seawater matrices was 98% and 96%, respectively. The electrode film was highly stable after five repeated adsorption/desorption cycles. The new electrochemical sensing scheme provides a highly selective, sensitive and versatile assay for the in-situ detection of TNT in complex water media.

Construction of an electrochemical sensor based on the electrodeposition of Au-Pt nanoparticles mixtures on multi-walled carbon nanotubes film for voltammetric determination of cefotaxime.

PubMed

Shahrokhian, Saeed; Rastgar, Shokoufeh

2012-06-07

Mixtures of gold-platinum nanoparticles (Au-PtNPs) are fabricated consecutively on a multi-walled carbon nanotubes (MWNT) coated glassy carbon electrode (GCE) by the electrodeposition method. The surface morphology and nature of the hybrid film (Au-PtNPs/MWCNT) deposited on glassy carbon electrodes is characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) techniques. The modified electrode is used as a new and sensitive electrochemical sensor for the voltammetric determination of cefotaxime (CFX). The electrochemical behavior of CFX is investigated on the surface of the modified electrode using linear sweep voltammetry (LSV). The results of voltammetric studies exhibited a considerable improvement in the oxidation peak current of CFX compared to glassy carbon electrodes individually coated with MWCNT or Au-PtNPs. Under the optimized conditions, the modified electrode showed a wide linear dynamic range of 0.004-10.0 μM with a detection limit of 1.0 nM for the voltammetric determination of CFX. The modified electrode was successfully applied for the accurate determination of trace amounts of CFX in pharmaceutical and clinical preparations.

Influence of aluminum oxide film on thermocompression bonding of gold wire to evaporated aluminum film

NASA Technical Reports Server (NTRS)

Iwata, S.; Ishizaka, A.; Yamamoto, H.

1984-01-01

The influence of Al surface condition on the thermocompression bonding of Au wires to Al electrodes for integrated electric circuits was studied. Au wires were connected to Al electrodes by nail-head bonding after various Al surface treatments. Bonding was evaluated by measuring the wire pull strength and fraction of the number of failures at Au-Al bonds to the total number of failures. Dependence of the fraction on applied load was derived theoretically with a parameter named critical load to take into consideration the differences in Al surface condition. The relation also held explicately for various surface treatments. Characterization of the Al surface was carried out by electron microscopy for chemical analysis.

Anisotropic In Situ-Coated AuNPs on Screen-Printed Carbon Surface for Enhanced Prostate-Specific Antigen Impedimetric Aptasensor

NASA Astrophysics Data System (ADS)

Do, Tram T. N.; Van Phi, Toan; Nguy, Tin Phan; Wagner, Patrick; Eersels, Kasper; Vestergaard, Mun'delanji C.; Truong, Lien T. N.

2017-06-01

An impedimetric aptasensor has been used to study the effect of charge transfer on the binding of prostate-specific antigen (PSA) to its aptamer. Full understanding of this mechanism will be beneficial to further improve its sensitivity for PSA detection in human semen at physiologically relevant concentrations. Bare gold electrodes (SPAuEs) and gold nanoparticles (AuNPs)-coated screen-printed carbon ink electrodes (AuNPs/SPCEs) were coated with aptamer solution at various concentrations and the sensor response to increasing PSA concentration in buffer solution examined. AuNPs were deposited onto carbon electrodes in 10 cycles. AuNPs/SPCEs were then coated with a self-assembled monolayer (SAM) of 16-mercaptohexadecanoic acid prior to aptamer immobilization at dose of 5 μg mL-1. The results indicate that anisotropic AuNPs/SPCEs outperform bare gold electrodes in terms of decreased amount of aptamer bunches as well as the number of intermediate PSA-aptamer complexes formed on the electrode surface. The key finding is that the fabricated aptasensor is sensitive enough [limit of detection (LoD) 1.95 ng mL-1] for early diagnosis of prostate cancer and displays linear response in the physiologically relevant concentration range (0 ng mL-1 to 10 ng mL-1), as shown by the calibration curve of the relative change in electron transfer resistance (Δ R CT) versus PSA concentration when aptamer/SAM/AuNPs/SPCEs were exposed to buffer containing PSA at different concentrations.

Electrochemical Determination of Food Preservative Nitrite with Gold Nanoparticles/p-Aminothiophenol-Modified Gold Electrode

PubMed Central

Üzer, Ayşem; Sağlam, Şener; Can, Ziya; Erçağ, Erol; Apak, Reşat

2016-01-01

Due to the negative impact of nitrate and nitrite on human health, their presence exceeding acceptable levels is not desired in foodstuffs. Thus, nitrite determination at low concentrations is a major challenge in electroanalytical chemistry, which can be achieved by fast, cheap, and safe electrochemical sensors. In this work, the working electrode (Au) was functionalized with p-aminothiophenol (p-ATP) and modified with gold nanoparticles (Au-NPs) to manufacture the final (Au/p-ATP-Aunano) electrode in a two-step procedure. In the first step, p-ATP was electropolymerized on the electrode surface to obtain a polyaminothiophenol (PATP) coating. In the second step, Au/p-ATP-Aunano working electrode was prepared by coating the surface with the use of HAuCl4 solution and cyclic voltammetry. Determination of aqueous nitrite samples was performed with the proposed electrode (Au/p-ATP-Aunano) using square wave voltammetry (SWV) in pH 4 buffer medium. Characteristic peak potential of nitrite samples was 0.76 V, and linear calibration curves of current intensity versus concentration was linear in the range of 0.5–50 mg·L−1 nitrite with a limit of detection (LOD) of 0.12 mg·L−1. Alternatively, nitrite in sausage samples could be colorimetrically determined with high sensitivity by means of p-ATP‒modified gold nanoparticles (AuNPs) and naphthylethylene diamine as coupling agents for azo-dye formation due to enhanced charge-transfer interactions with the AuNPs surface. The slopes of the calibration lines in pure NO2− solution and in sausage sample solution, to which different concentrations of NO2− standards were added, were not significantly different from each other, confirming the robustness and interference tolerance of the method. The proposed voltammetric sensing method was validated against the colorimetric nanosensing method in sausage samples. PMID:27490543

A facile approach for reducing the working voltage of Au/TiO2/Au nanostructured memristors by enhancing the local electric field

NASA Astrophysics Data System (ADS)

Arab Bafrani, Hamidreza; Ebrahimi, Mahdi; Bagheri Shouraki, Saeed; Moshfegh, Alireza Z.

2018-01-01

Memristor devices have attracted tremendous interest due to different applications ranging from nonvolatile data storage to neuromorphic computing units. Exploring the role of surface roughness of the bottom electrode (BE)/active layer interface provides useful guidelines for the optimization of the memristor switching performance. This study focuses on the effect of surface roughness of the BE electrode on the switching characteristics of Au/TiO2/Au three-layer memristor devices. An optimized wet-etching treatment condition was found to modify the surface roughness of the Au BE where the measurement results indicate that the roughness of the Au BE is affected by both duration time and solution concentrations of the wet-etching process. Then we fabricated arrays of TiO2-based nanostructured memristors sandwiched between two sets of cross-bar Au electrode lines (junction area 900 μm2). The results revealed a reduction in the working voltages in current-voltage characteristic of the device performance when increasing the surface roughness at the Au(BE)/TiO2 active layer interface. The set voltage of the device (Vset) significantly decreased from 2.26-1.93 V when we increased the interface roughness from 4.2-13.1 nm. The present work provides information for better understanding the switching mechanism of titanium-dioxide-based devices, and it can be inferred that enhancing the roughness of the Au BE/TiO2 active layer interface leads to a localized non-uniform electric field distribution that plays a vital role in reducing the energy consumption of the device.

Enhanced photoelectrochemical DNA sensor based on TiO2/Au hybrid structure.

PubMed

Liu, Xing-Pei; Chen, Jing-Shuai; Mao, Chang-Jie; Niu, He-Lin; Song, Ji-Ming; Jin, Bao-Kang

2018-05-23

A novel enhanced photoelectrochemical DNA sensor, based on a TiO 2 /Au hybrid electrode structure, was developed to detect target DNA. The sensor was developed by successively modifying fluorine-tin oxide (FTO) electrodes with TiO 2 nanoparticles, gold (Au) nanoparticles, hairpin DNA (DNA1), and CdSe-COOH quantum dots (QDs), which acted as signal amplification factors. In the absence of target DNA, the incubated DNA1 hairpin and the CdSe-COOH QDs were in close contact with the TiO 2 /Au electrode surface, leading to an enhanced photocurrent intensity due to the sensitization effect. After incubation of the modified electrode with the target DNA, the hairpin DNA changed into a double helix structure, and the CdSe QDs moved away from the TiO 2 /Au electrode surface, leading to a decreased sensitization effect and photoelectrochemical signal intensity. This novel DNA sensor exhibited stable, sensitive and reproducible detection of DNA from 0.1 μM to 10 fM, with a lower detection limit of 3 fM. It provided good specificity, reproducibility, stability and is a promising strategy for the detection of a variety of other DNA targets, for early clinical diagnosis of various diseases. Copyright © 2018 Elsevier B.V. All rights reserved.

A novel alcohol dehydrogenase biosensor based on solid-state electrogenerated chemiluminescence by assembling dehydrogenase to Ru(bpy)(3)2+-Au nanoparticles aggregates.

PubMed

Zhang, Lihua; Xu, Zhiai; Sun, Xuping; Dong, Shaojun

2007-01-15

Based on electrogenerated chemiluminescence (ECL), a novel method for fabrication of alcohol dehydrogenase (ADH) biosensor by self-assembling ADH to Ru(bpy)(3)(2+)-AuNPs aggregates (Ru-AuNPs) on indium tin oxide (ITO) electrode surface has been developed. Positively charged Ru(bpy)(3)(2+) could be immobilized stably on the electrode surface with negatively charged AuNPs in the form of aggregate via electrostatic interaction. On the other hand, AuNPs are favourable candidates for the immobilization of enzymes because amine groups and cysteine residues in the enzymes are known to bind strongly with AuNPs. Moreover, AuNPs can act as tiny conduction centers to facilitate the transfer of electrons. Such biosensor combined enzymatic selectivity with the sensitivity of ECL detection for quantification of enzyme substrate, and it displayed wide linear range, high sensitivity and good stability.

Conductive polymer/reduced graphene oxide/Au nano particles as efficient composite materials in electrochemical supercapacitors

NASA Astrophysics Data System (ADS)

Shabani Shayeh, J.; Ehsani, A.; Ganjali, M. R.; Norouzi, P.; Jaleh, B.

2015-10-01

Polyaniline/reduced graphene oxide/Au nano particles (PANI/rGO/AuNPs) as a hybrid supercapacitor were deposited on a glassy carbon electrode (GCE) by cyclic voltammetry (CV) method as ternary composites and their electrochemical performance was evaluated in acidic medium. Scanning electron micrographs clearly revealed the formation of nanocomposites on the surface of the working electrode. Scanning electron micrographs (SEM) clearly revealed the formation of nanocomposites on the surface of working electrode. Different electrochemical methods including galvanostatic charge-discharge (CD) experiments, cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were carried out in order to investigate the applicability of the system as a supercapacitor. Based on the cyclic voltammogram results obtained, PANI/rGO/AuNPs gave higher specific capacitance, power and energy values than PANI at a current density of 1 mA cm-2. Specific capacitance (SC) of PANI and PANI/rGO/AuNPs electrodes calculated using CV method are 190 and 303 F g-1, respectively. The present study introduces new nanocomposite materials for electrochemical redox capacitors with advantages including long life cycle and stability due to synergistic effects of each component.

Friction force microscopy at a regularly stepped Au(665) electrode: Anisotropy effects

NASA Astrophysics Data System (ADS)

Podgaynyy, Nikolay; Iqbal, Shahid; Baltruschat, Helmut

2015-01-01

Using friction force microscopy, friction was determined for the AFM-tip scanning parallel and vertically to the monoatomic steps of Au(665) electrode for different coverages of Cu in sulfuric acid. When the tip was scanning parallel to the steps, the results were similar to those obtained before for a Au(111) surface: a higher coverage of Cu leads to an increased friction. However, differently from Au(111), no transitions in the friction coefficient were observed with increasing load. Atomic stick slip was observed both for the Au surface and the √{ 3} × √{ 3} honeycomb Cu adlayer with a Cu coverage of 2/3. When the tip was scanning perpendicular to the steps, friction did not depend much on coverage; astonishingly, atomic stick slip was also observed.

Gold nanoparticles-based electrochemical method for the detection of protein kinase with a peptide-like inhibitor as the bioreceptor

PubMed Central

Sun, Kai; Chang, Yong; Zhou, Binbin; Wang, Xiaojin; Liu, Lin

2017-01-01

This article presents a general method for the detection of protein kinase with a peptide-like kinase inhibitor as the bioreceptor, and it was done by converting gold nanoparticles (AuNPs)-based colorimetric assay into sensitive electrochemical analysis. In the colorimetric assay, the kinase-specific aptameric peptide triggered the aggregation of AuNPs in solution. However, the specific binding of peptide to the target protein (kinase) inhibited its ability to trigger the assembly of AuNPs. In the electrochemical analysis, peptides immobilized on a gold electrode and presented as solution triggered together the in situ formation of AuNPs-based network architecture on the electrode surface. Nevertheless, the formation of peptide–kinase complex on the electrode surface made the peptide-triggered AuNPs assembly difficult. Electrochemical impedance spectroscopy was used to measure the change in surface property in the binding events. When a ferrocene-labeled peptide (Fc-peptide) was used in this design, the network of AuNPs/Fc-peptide produced a good voltammetric signal. The competitive assay allowed for the detection of protein kinase A with a detection limit of 20 mU/mL. This work should be valuable for designing novel optical or electronic biosensors and likely lead to many detection applications. PMID:28331314

A surface-enhanced infrared absorption spectroscopic study of pH dependent water adsorption on Au

NASA Astrophysics Data System (ADS)

Dunwell, Marco; Yan, Yushan; Xu, Bingjun

2016-08-01

The potential dependent behavior of near-surface water on Au film electrodes in acidic and alkaline solutions is studied using a combination of attenuated total reflectance surface enhanced infrared spectroscopy and chronoamperometry. In acid, sharp νOH peaks appear at 3583 cm- 1 at high potentials attributed to non-H-bonded water coadsorbed in the hydration sphere of perchlorate near the electrode surface. Adsorbed hydronium bending mode at near 1680 cm- 1 is observed at low potentials in low pH solutions (1.4, 4.0, 6.8). At high pH (10.0, 12.3), a potential-dependent OH stretching band assigned to adsorbed hydroxide emerges from 3400-3506 cm- 1. The observation of adsorbed hydroxide, even on a weakly oxophilic metal such as Au, provides the framework for further studies of hydroxide adsorption on other electrodes to determine the role of adsorbed hydroxide on important reactions such as the hydrogen oxidation reaction.

Gold dendrites Co-deposited with M13 virus as a biosensor platform for nitrite ions.

PubMed

Seo, Yeji; Manivannan, Shanmugam; Kang, Inhak; Lee, Seung-Wuk; Kim, Kyuwon

2017-08-15

We developed a biosensor for nitrite ion on an electrode surface modified with M13 viruses and gold nanostructures. Gold dendritic nanostructures (Au-DNs) are electrochemically co-deposited from 4E peptides engineered M13 virus (M13 4E ) mixed electrolyte on to the ITO electrode. The M13 4E could specifically nucleate Au precursor (Gold (III) chloride), which enable the efficient growth of dendritic nanostructures, whereas such dendritic structures were not obtained in the presence of wild-type and Y3E peptides engineered M13 viruses. The structural features of the Au-DNs and their interfacing mechanism with ITO electrode are characterized by SEM, EDX and XRD analyses. The growth of Au-DNs at ITO electrode has been monitored by time dependent SEM study. The M13 4E induces the formation and plays a crucial role in shaping the dendritic morphology for Au. Biosensor electrode was constructed using Au-DNs modified electrode for nitrite ions and found improved sensitivity relative to the sensor electrode prepared from wild-type M13, Y3E peptides engineered M13 and without M13. Sensor electrode exhibited good selectivity toward target analyte from the possible interferences. Furthermore, 4E native peptides were used as additive to deposit Au nanostructures and it is compared with the structure and reactivity of the Au nanostructures prepared in the presence of M13 4E . Our novel biosensor fabrication can be extended to other metal and metal oxide nanostructures and its application might be useful to develop novel biosensor electrode for variety of biomolecules. Copyright © 2017 Elsevier B.V. All rights reserved.

DNA bases assembled on the Au(110)/electrolyte interface: a combined experimental and theoretical study.

PubMed

Salvatore, Princia; Nazmutdinov, Renat R; Ulstrup, Jens; Zhang, Jingdong

2015-02-19

Among the low-index single-crystal gold surfaces, the Au(110) surface is the most active toward molecular adsorption and the one with fewest electrochemical adsorption data reported. Cyclic voltammetry (CV), electrochemically controlled scanning tunneling microscopy (EC-STM), and density functional theory (DFT) calculations have been employed in the present study to address the adsorption of the four nucleobases adenine (A), cytosine (C), guanine (G), and thymine (T), on the Au(110)-electrode surface. Au(110) undergoes reconstruction to the (1 × 3) surface in electrochemical environment, accompanied by a pair of strong voltammetry peaks in the double-layer region in acid solutions. Adsorption of the DNA bases gives featureless voltammograms with lower double-layer capacitance, suggesting that all the bases are chemisorbed on the Au(110) surface. Further investigation of the surface structures of the adlayers of the four DNA bases by EC-STM disclosed lifting of the Au(110) reconstruction, specific molecular packing in dense monolayers, and pH dependence of the A and G adsorption. DFT computations based on a cluster model for the Au(110) surface were performed to investigate the adsorption energy and geometry of the DNA bases in different adsorbate orientations. The optimized geometry is further used to compute models for STM images which are compared with the recorded STM images. This has provided insight into the physical nature of the adsorption. The specific orientations of A, C, G, and T on Au(110) and the nature of the physical adsorbate/surface interaction based on the combination of the experimental and theoretical studies are proposed, and differences from nucleobase adsorption on Au(111)- and Au(100)-electrode surfaces are discussed.

Integrated nanoparticle-biomolecule systems for biosensing and bioelectronics.

PubMed

Willner, Itamar; Baron, Ronan; Willner, Bilha

2007-04-15

The similar dimensions of biomolecules such as enzymes, antibodies or DNA, and metallic or semiconductor nanoparticles (NPs) enable the synthesis of biomolecule-NP hybrid systems where the unique electronic, photonic and catalytic properties of NPs are combined with the specific recognition and biocatalytic properties of biomolecules. The unique functions of biomolecule-NP hybrid systems are discussed with several examples: (i) the electrical contacting of redox enzymes with electrodes is the basis for the development of enzymatic electrodes for amperometric biosensors or biofuel cell elements. The reconstitution of the apo-glucose oxidase or apo-glucose dehydrogenase on flavin adenine dinucleotide (FAD)-functionalized Au NPs (1.4 nm) associated with electrodes, or on pyrroloquinoline quinone (PQQ)-functionalized Au NPs (1.4 nm) associated with electrodes, respectively, yields electrically contacted enzyme electrodes. The aligned, reconstituted enzymes on the electrode surfaces reveal effective electrical contacting, and the glucose oxidase and glucose dehydrogenase reveal turnover rates of 5000 and 11,800 s(-1), respectively. (ii) The photoexcitation of semiconductor nanoparticles yields fluorescence with a wavelength controlled by the size of the NPs. The fluorescence functions of semiconductor NPs are used to develop a fluorescence resonance energy transfer (FRET) assay for nucleic acids, and specifically, for analyzing telomerase activity in cancer cells. CdSe-ZnS NPs are functionalized by a primer recognized by telomerase, and this is elongated by telomerase extracted from HeLa cancer cells in the presence of dNTPs and Texas-red-functionalized dUTP. The dye integrated into the telomers allows the FRET process that is intensified as telomerization proceeds. Also, the photoexcited electron-hole pair generated in semiconductor NPs is used to generate photocurrents in a CdS-DNA hybrid system associated with an electrode. A redox-active intercalator, methylene blue, was incorporated into a CdS-duplex DNA monolayer associated with a Au electrode, and this facilitated the electron transfer between the electrode and the CdS NPs. The direction of the photocurrent was controlled by the oxidation state of the intercalator. (iii) Biocatalysts grow metallic NPs, and the absorbance of the NPs provides a means to assay the biocatalytic transformations. This is exemplified with the glucose oxidase-induced growth of Au NPs and with the tyrosinase-stimulated growth of Au NPs, in the presence of glucose or tyrosine, respectively. The biocatalytic growth of the metallic NPs is used to grow nanowires on surfaces. Glucose oxidase or alkaline phosphatase functionalized with Au NPs (1.4 nm) acted as 'biocatalytic inks' for the synthesis of metallic nanowires. The deposition of the Au NP-modified glucose oxidase, or the Au NP-modified alkaline phosphatase on Si surfaces by dip-pen nanolithography led to biocatalytic templates, that after interaction with glucose/AuCl4- or p-aminophenolphosphate/Ag+, allowed the synthesis of Au nanowires or Ag nanowires, respectively.

Au nanostructure-decorated TiO2 nanowires exhibiting photoactivity across entire UV-visible region for photoelectrochemical water splitting.

PubMed

Pu, Ying-Chih; Wang, Gongming; Chang, Kao-Der; Ling, Yichuan; Lin, Yin-Kai; Fitzmorris, Bob C; Liu, Chia-Ming; Lu, Xihong; Tong, Yexiang; Zhang, Jin Z; Hsu, Yung-Jung; Li, Yat

2013-08-14

Here we demonstrate that the photoactivity of Au-decorated TiO2 electrodes for photoelectrochemical water oxidation can be effectively enhanced in the entire UV-visible region from 300 to 800 nm by manipulating the shape of the decorated Au nanostructures. The samples were prepared by carefully depositing Au nanoparticles (NPs), Au nanorods (NRs), and a mixture of Au NPs and NRs on the surface of TiO2 nanowire arrays. As compared with bare TiO2, Au NP-decorated TiO2 nanowire electrodes exhibited significantly enhanced photoactivity in both the UV and visible regions. For Au NR-decorated TiO2 electrodes, the photoactivity enhancement was, however, observed in the visible region only, with the largest photocurrent generation achieved at 710 nm. Significantly, TiO2 nanowires deposited with a mixture of Au NPs and NRs showed enhanced photoactivity in the entire UV-visible region. Monochromatic incident photon-to-electron conversion efficiency measurements indicated that excitation of surface plasmon resonance of Au is responsible for the enhanced photoactivity of Au nanostructure-decorated TiO2 nanowires. Photovoltage experiment showed that the enhanced photoactivity of Au NP-decorated TiO2 in the UV region was attributable to the effective surface passivation of Au NPs. Furthermore, 3D finite-difference time domain simulation was performed to investigate the electrical field amplification at the interface between Au nanostructures and TiO2 upon SPR excitation. The results suggested that the enhanced photoactivity of Au NP-decorated TiO2 in the UV region was partially due to the increased optical absorption of TiO2 associated with SPR electrical field amplification. The current study could provide a new paradigm for designing plasmonic metal/semiconductor composite systems to effectively harvest the entire UV-visible light for solar fuel production.

Polymer coating behavior of Rayleigh-SAW resonators with gold electrode structure for gas sensor applications.

PubMed

Avramov, Ivan D; Länge, Kerstin; Rupp, Swen; Rapp, Bastian; Rapp, Michael

2007-01-01

Results from systematic polymer coating experiments on surface acoustic wave (SAW) resonators and coupled resonator filters (CRF) on ST-cut quartz with a corrosion-proof electrode structure entirely made of gold (Au) are presented and compared with data from similar SAW devices using aluminium (Al) electrodes. The recently developed Au devices are intended to replace their earlier Al counterparts in sensor systems operating in highly reactive chemical gas environments. Solid parylene C and soft poly[chlorotrifluoroethylene-co-vinylidene fluoride] (PCFV) polymer films are deposited under identical conditions onto the surface of Al and Au devices. The electrical performance of the Parylene C coated devices is monitored online during film deposition. The PCVF coated devices are evaluated after film deposition. The experimental data show that the Au devices can stand up to 40% thicker solid films for the same amount of loss increase than the Al devices and retain better resonance and phase characteristics. The frequency sensitivities of Au and Al devices to parylene C deposition are nearly identical. After coating with soft PCFV sensing film, the Au devices provide up to two times higher gas sensitivity when probed with cooling agent, octane, or tetrachloroethylene.

Oxidation and sensing of ascorbic acid and dopamine on self-assembled gold nanoparticles incorporated within polyaniline film

NASA Astrophysics Data System (ADS)

Chu, Wenya; Zhou, Qun; Li, Shuangshuang; Zhao, Wei; Li, Na; Zheng, Junwei

2015-10-01

Electrochemical biosensors based on conducting polymers incorporated with metallic nanoparticles can greatly enhance sensitivity and selectivity. Herein, we report a facile fabrication approach for polyaniline (PAN) incorporated with a gold nanoparticle (AuNP) composite electrode by electrodeposition of PAN on a self-assembled AuNP layer on the surface of an indium tin oxide electrode. The resulting AuNP/PAN composite electrode exhibits a remarkable synergistic effect on the electrocatalytic oxidation of ascorbic acid (AA) and dopamine (DA). It is demonstrated that the oxidation reaction of AA mainly occurs at AuNPs inside the PAN film as the ascorbate anions are doped into the polymer during the oxidation of the PAN film. Conversely, the oxidation of positively charged DA may only take place at the PAN/solution interface. The different mechanisms of the electrode reactions result in the oxidation of AA and DA occurring at different potentials. As a result, the AuNP/PAN composite electrode can be employed to simultaneously detect AA and DA with a good linear range, high sensitivity, and low detection limit.

Construction of novel electrochemical immunosensor for detection of prostate specific antigen using ferrocene-PAMAM dendrimers.

PubMed

Çevik, Emre; Bahar, Özlem; Şenel, Mehmet; Abasıyanık, M Fatih

2016-12-15

In this study, an immunosensor was designed to utilize for the detection of prostate specific antigen (PSA) based on three different generations (G1, G2 and G3) of ferrocene (Fc) cored polyamidiamine dendrimers (Fc-PAMAM) gold (Au) electrode. The self-assembled monolayer principle (SAM) was used to fabricate the sensitive, selective and disposable immunosensor electrodes. In electrode fabrication cysteamine (Cys) was the first agent covalently linked on the Au electrode surface. Immobilized redox center (ferrocene) cored PAMAM dendrimers served as a layer for the further binding of biological components. The monoclonal antibody of PSA (anti-PSA) was covalently immobilized on dendrimers which were attached onto the modified Au surface (Au/Cys/Fc-PAMAMs/anti-PSA). PSA levels were quantitatively analyzed by using electrochemical differential pulse voltammetry (DPV) whose lowest detection limit was calculated as 0.001ngmL(-1). The Au/Cys/FcPAMAM/anti-PSA immunosensor showed excellent performance for PSA at the pulse amplitude; 50mV and the scan rate; 10mV/s in a wide linear concentration range of 0.01ng-100ngmL(-1). Analytical performance and specificity assays were carried out using human serum and different proteins. Copyright © 2016 Elsevier B.V. All rights reserved.

Bimetallic Pt-Au nanocatalysts electrochemically deposited on boron-doped diamond electrodes for nonenzymatic glucose detection.

PubMed

Nantaphol, Siriwan; Watanabe, Takeshi; Nomura, Naohiro; Siangproh, Weena; Chailapakul, Orawon; Einaga, Yasuaki

2017-12-15

The enormous demand for medical diagnostics has encouraged the fabrication of high- performance sensing platforms for the detection of glucose. Nonenzymatic glucose sensors are coming ever closer to being used in practical applications. Bimetallic catalysts have been shown to be superior to single metal catalysts in that they have greater activity and selectivity. Here, we demonstrate the preparation, characterization, and electrocatalytic characteristics of a new bimetallic Pt/Au nanocatalyst. This nanocatalyst can easily be synthesized by electrodeposition by sequentially depositing Au and Pt on the surface of a boron-doped diamond (BDD) electrode. We characterized the nanocatalyst by scanning electron microscopy (SEM), X-ray diffraction (XRD), and voltammetry. The morphology and composition of the nanocatalyst can be easily controlled by adjusting the electrodeposition process and the molar ratio between the Pt and Au precursors. The electrocatalytic characteristics of a Pt/Au/BDD electrode for the nonenzymatic oxidation of glucose were systematically investigated by cyclic voltammetry. The electrode exhibits higher catalytic activity for glucose oxidation than Pt/BDD and Au/BDD electrodes. The best catalytic activity and stability was obtained with a Pt:Au molar ratio of 50:50. Moreover, the presence of Au can significantly enhance the long-term stability and poisoning tolerance during the electro-oxidation of glucose. Measurements of glucose using the Pt/Au/BDD electrode were linear in the range from 0.01 to 7.5mM, with a detection limit of 0.0077mM glucose. The proposed electrode performs selective electrochemical analysis of glucose in the presence of common interfering species (e.g., acetaminophen, uric and ascorbic acids), avoiding the generation of overlapping signals from such species. Copyright © 2017 Elsevier B.V. All rights reserved.

Fabrication of Lab-on-Paper Using Porous Au-Paper Electrode: Application to Tumor Marker Electrochemical Immunoassays.

PubMed

Ge, Shenguang; Zhang, Yan; Yan, Mei; Huang, Jiadong; Yu, Jinghua

2017-01-01

A simple, low-cost, and sensitive electrochemical lab-on-paper assay is developed based on a novel gold nanoparticle modified porous paper working electrode for use in point-of-care testing (POCT). Electrochemical methods are introduced for lab-on-paper based on screen-printed paper electrodes. To further improve specificity, performance, and sensitivity for point-of-care testing, a novel porous Au-paper working electrode (Au-PWE) is designed for lab-on-paper using growth of an interconnected Au nanoparticle (NP) layer on the surface of cellulose fibers in order to enhance the conductivity of the paper sample zone and immobilize the primary antibodies (Ab1). With a sandwich-type immunoassay format, Pd-Au bimetallic nanoparticles possessing peroxidase-like activity are used as a matrix to immobilize secondary antibodies (Ab2) for rapid detection of targets. This lab-on-paper based immunodevice is applied to the diagnosis of a cancer biomarker in clinical serum samples.

Role of Au(NPs) in the enhanced response of Au(NPs)-decorated MWCNT electrochemical biosensor

PubMed Central

Mehmood, Shahid; Ciancio, Regina; Carlino, Elvio; Bhatti, Arshad S

2018-01-01

Background The combination of Au-metallic-NPs and CNTs are a new class of hybrid nanomaterials for the development of electrochemical biosensor. Concentration of Au(nanoparticles [NPs]) in the electrochemical biosensor is crucial for the efficient charge transfer between the Au-NPs-MWCNTs modified electrode and electrolytic solution. Methods In this work, the charge transfer kinetics in the glassy carbon electrode (GCE) modified with Au(NPs)–multiwalled carbon nanotube (MWCNT) nanohybrid with varied concentrations of Au(NPs) in the range 40–100 nM was studied using electrochemical impedance spectroscopy (EIS). Field emission scanning electron microscopy and transmission electron microscopy confirmed the attachment of Au(NPs) on the surface of MWCNTs. Results The cyclic voltammetry and EIS results showed that the charge transfer mechanism was diffusion controlled and the rate of charge transfer was dependent on the concentration of Au(NPs) in the nanohybrid. The formation of spherical diffusion zone, which was dependent on the concentration of Au(NPs) in nanohybrids, was attributed to result in 3 times the increase in the charge transfer rate ks, 5 times increase in mass transfer, and 5% (9%) increase in Ipa (Ipc) observed in cyclic voltammetry in 80 nM Au(NP) nanohybrid-modified GCE from MWCNT-modified GCE. The work was extended to probe the effect of charge transfer rates at various concentrations of Au(NPs) in the nanohybrid-modified electrodes in the presence of Escherichia coli. The cyclic voltammetry results clearly showed the best results for 80 nM Au(NPs) in nanohybrid electrode. Conclusion The present study suggested that the formation of spherical diffusion zone in nanohybrid-modified electrodes is critical for the enhanced electrochemical biosensing applications. PMID:29713161

STM investigations of Au(1 1 1) electrodes coated with vitamin B 12 derivatives

NASA Astrophysics Data System (ADS)

Szőcs, E.; Durrer, L.; Luginbühl, R.; Simic, N.; Viana, A. S.; Abrantes, L. M.; Keese, R.; Siegenthaler, H.

2006-01-01

Vitamin B 12 derivatives immobilized at flame-annealed Au(1 1 1) electrode surfaces have been investigated in close correlation with their structural properties and spatial arrangement at the electrode substrate by scanning tunneling microscopy (STM) in air and in aqueous 0.1 M NaClO 4 solution. The investigated compounds were symmetrical (B 12C 10S-SC 10B 12) and nonsymmetrical (B 12C 10S-SC 10) dialkyl disulfide derivatives of vitamin B 12, attached to the electrode surfaces by the S-Au bond. The ex situ and in situ STM experiments show the formation of a surface layer, whose packing density and structure is presumably controlled by the spatial arrangement of the large cobyrinate head groups. In presence of the symmetrical B 12 compound, a disordered surface layer is observed. Voltammetric investigations show that, in 0.1 M NaClO 4, this layer becomes unstable at potentials approximately ⩽ -1000 mV vs. MSE and is almost completely removed at more negative potentials. The STM imaging properties of the nonsymmetrical B 12 surface layer show a significant dependence on the tunneling distance. In particular, at small tunneling distances, a highly regular hexagonal surface pattern is observed that suggests strongly the presence of an ordered surface assembly. Modeling of the B 12 head group has been performed to provide information for a structure-related interpretation of the high-resolution STM images. The investigations are first STM results obtained at such B 12 modified electrodes.

Charge-Carrier-Scattering Spectroscopy With BEEM

NASA Technical Reports Server (NTRS)

Hecht, Michael H.; Bell, Lloyd D.; Kaiser, William J.

1992-01-01

Ballistic-electron-emission microscopy (BEEM) constitutes basis of new spectroscopy of scattering of electrons and holes. Pointed tip electrode scans near surface of metal about 100 angstrom thick on semiconductor. Principle similar to scanning tunneling microscope, except metal acts as third electrode. Used to investigate transport phenomena, scattering phenomena, and creation of hot charge carriers in Au/Si and Au/GaAs metal/semiconductor microstructures.

A hybrid DNA-templated gold nanocluster for enhanced enzymatic reduction of oxygen

DOE PAGES

Chakraborty, Saumen; Babanova, Sofia; Rocha, Reginaldo C.; ...

2015-08-19

We report the synthesis and characterization of a new DNA-templated gold nanocluster (AuNC) of ~1 nm in diameter and possessing ~7 Au atoms. When integrated with bilirubin oxidase (BOD) and single walled carbon nanotubes (SWNTs), the AuNC acts as an enhancer of electron transfer (ET) and lowers the overpotential of electrocatalytic oxygen reduction reaction (ORR) by ~15 mV as compared to the enzyme alone. In addition, the presence of AuNC causes significant enhancements in the electrocatalytic current densities at the electrode. Control experiments show that such enhancement of ORR by the AuNC is specific to nanoclusters and not to plasmonicmore » gold particles. Rotating ring disk electrode (RRDE) measurements confirm 4e– reduction of O 2 to H 2O with minimal production of H 2O 2, suggesting that the presence of AuNC does not perturb the mechanism of ORR catalyzed by the enzyme. This unique role of the AuNC as enhancer of ET at the enzyme-electrode interface makes it a potential candidate for the development of cathodes in enzymatic fuel cells, which often suffer from poor electronic communication between the electrode surface and the enzyme active site. In conclusion, the AuNC displays phosphorescence with large Stokes shift and microsecond lifetime.« less

Synthesis of water soluble chitosan stabilized gold nanoparticles and determination of uric acid

NASA Astrophysics Data System (ADS)

Lanh Le, Thi; Khieu Dinh, Quang; Hoa Tran, Thai; Nguyen, Hai Phong; Le Hien Hoang, Thi; Hien Nguyen, Quoc

2014-06-01

Gold nanoparticles (Au-NPs) have been successfully synthesized by utilizing water soluble chitosan as reducing and stabilizing agent. The colloidal Au-NPs were characterized by UV-Vis spectroscopy and transmission electron microscopy (TEM). The results showed that the colloidal Au-NPs had a plasmon absorption band with maximum wavelength in the range of 520-526 nm and the diameters were about 8-15 nm. In addition, a new Au-NPs-modified electrode was fabricated by self-assembling Au-NPs to the surface of the L-cysteine-modified glassy carbon electrode (Au-NPs/L-Cys/GCE). The Au-NPs-modified electrode showed an excellent character for electro-catalytic oxidization of uric acid (UA) in 0.1 mol L-1 phosphate buffer solution (pH 3.2). Using differential pulse anodic stripping voltammetry (DP-ASV), a high selectivity for determination of UA has been explored for the Au-NPs-modified electrode. DP-ASV peak currents of UA increased linearly with their concentration at the range of 2.0 × 10-6 to 4.0 × 10-5 mol L-1 with the detection limit of 2.7 × 10-6 mol L-1 for UA. The proposed method was applied for the detection of UA in human urine and serum samples with satisfactory results.

Highly sensitive electrochemical detection of cocaine on graphene/AuNP modified electrode via catalytic redox-recycling amplification.

PubMed

Jiang, Bingying; Wang, Min; Chen, Ying; Xie, Jiaqing; Xiang, Yun

2012-02-15

We demonstrated a new strategy for highly sensitive electrochemical detection of cocaine by using two engineered aptamers in connection to redox-recycling signal amplification. The graphene/AuNP nanocomposites were electrochemically deposited on a screen printed carbon electrode to enhance the electron transfers. The cocaine primary binding aptamers were self-assembled on the electrode surface through sulfur-Au interactions. The presence of the target cocaine and the biotin-modified secondary binding aptamers leads to the formation of sandwich complexes on the electrode surface. The streptavidin-conjugated alkaline phosphatases (ALPs) were used as labels to generate quantitative signals. The addition of the ALP substrate and the co-reactant NADH results in the formation of a redox cycle between the enzymatic product and the electrochemically oxidized species and the signal is thus significantly amplified. Because of the effective modification of the sensing surface and signal amplification, low nanomolar (1 nM) detection limit for cocaine is achieved. The proposed aptamer-based sandwich sensing approach for amplified detection of cocaine thus opens new opportunities for highly sensitive determination of other small molecules. Copyright © 2011 Elsevier B.V. All rights reserved.

Single-step fabrication of electrodes with controlled nanostructured surface roughness using optically-induced electrodeposition

NASA Astrophysics Data System (ADS)

Liu, N.; Li, M.; Liu, L.; Yang, Y.; Mai, J.; Pu, H.; Sun, Y.; Li, W. J.

2018-02-01

The customized fabrication of microelectrodes from gold nanoparticles (AuNPs) has attracted much attention due to their numerous applications in chemistry and biomedical engineering, such as for surface-enhanced Raman spectroscopy (SERS) and as catalyst sites for electrochemistry. Herein, we present a novel optically-induced electrodeposition (OED) method for rapidly fabricating gold electrodes which are also surface-modified with nanoparticles in one single step. The electrodeposition mechanism, with respect to the applied AC voltage signal and the elapsed deposition time, on the resulting morphology and particle sizes was investigated. The results from SEM and AFM analysis demonstrated that 80-200 nm gold particles can be formed on the surface of the gold electrodes. Simultaneously, both the size of the nanoparticles and the roughness of the fabricated electrodes can be regulated by the deposition time. Compared to state-of-the-art methods for fabricating microelectrodes with AuNPs, such as nano-seed-mediated growth and conventional electrodeposition, this OED technique has several advantages including: (1) electrode fabrication and surface modification using nanoparticles are completed in a single step, eliminating the need for prefabricating micro electrodes; (2) the patterning of electrodes is defined using a digitally-customized, projected optical image rather than using fixed physical masks; and (3) both the fabrication and surface modification processes are rapid, and the entire fabrication process only requires less than 6 s.

Fabrication of sensitive enzymatic biosensor based on multi-layered reduced graphene oxide added PtAu nanoparticles-modified hybrid electrode

PubMed Central

Hossain, Md Faruk; Park, Jae Y.

2017-01-01

A highly sensitive amperometric glucose sensor was developed by immobilization of glucose oxidase (GOx) onto multi-layer reduced graphene oxide (MRGO) sheets decorated with platinum and gold flower-like nanoparticles (PtAuNPs) modified Au substrate electrode. The fabricated MRGO/PtAuNPs modified hybrid electrode demonstrated high electrocatalytic activities toward oxidation of H2O2, to which it had a wide linear response that ranged from 0.5 to 8 mM (R2 = 0.997), and high sensitivity of 506.25 μA/mMcm2. Furthermore, glucose oxidase-chitosan composite and cationic polydiallyldimethylammonium chloride (PDDA) were assembled by a casting method on the surface of MRGO/PtAuNPs modified electrode. This as-fabricated hybrid biosensor electrode exhibited high electrocatalytic activity for the detection of glucose in PBS. It demonstrated good analytical properties in terms of a low detection limit of 1 μM (signal-to-noise ratio of 3), short response time (3 s), high sensitivity (17.85 μA/mMcm2), and a wide linear range (0.01–8 mM) for glucose sensing. These results reveal that the newly developed sensing electrode offers great promise for new type enzymatic biosensor applications. PMID:28333943

Direct electrochemical oxidation of S-captopril using gold electrodes modified with graphene-AuAg nanocomposites

PubMed Central

Pogacean, Florina; Biris, Alexandru R; Coros, Maria; Lazar, Mihaela Diana; Watanabe, Fumiya; Kannarpady, Ganesh K; Al Said, Said A Farha; Biris, Alexandru S; Pruneanu, Stela

2014-01-01

In this paper, we present a novel approach for the electrochemical detection of S-captopril based on graphene AuAg nanostructures used to modify an Au electrode. Multi-layer graphene (Gr) sheets decorated with embedded bimetallic AuAg nanoparticles were successfully synthesized catalytically with methane as the carbon source. The two catalytic systems contained 1.0 wt% Ag and 1.0 wt% Au, while the second had a larger concentration of metals (1.5 wt% Ag and 1.5 wt% Au) and was used for the synthesis of the Gr-AuAg-1 and Gr-AuAg-1.5 multicomponent samples. High-resolution transmission electron microscopy analysis indicated the presence of graphene flakes that had regular shapes (square or rectangular) and dimensions in the tens to hundreds of nanometers. We found that the size of the embedded AuAg nanoparticles varied between 5 and 100 nm, with the majority being smaller than 20 nm. Advanced scanning transmission electron microscopy studies indicated a bimetallic characteristic of the metallic clusters. The resulting Gr-AuAg-1 and Gr-AuAg-1.5 samples were used to modify the surface of commonly used Au substrates and subsequently employed for the direct electrochemical oxidation of S-captopril. By comparing the differential pulse voltammograms recorded with the two modified electrodes at various concentrations of captopril, the peak current was determined to be well-defined, even at relatively low concentration (10−5 M), for the Au/Gr-AuAg-1.5 electrode. In contrast, the signals recorded with the Au/Gr-AuAg-1 electrode were poorly defined within a 5×10−6 to 5×10−3 M concentration range, and many of them overlapped with the background. Such composite materials could find significant applications in nanotechnology, sensing, or nanomedicine. PMID:24596464

Highly sensitive quartz crystal microbalance based biosensor using Au dendrite structure

NASA Astrophysics Data System (ADS)

Asai, Naoto; Terasawa, Hideaki; Shimizu, Tomohiro; Shingubara, Shoso; Ito, Takeshi

2018-02-01

A Au dendrite structure was obtained by only electroplating under a suitable potential. A blanch like nanostructure was formed along the crystal orientation. In this study, we attempted to fabricate a Au dendrite structure on the electrode of a quartz crystal by electroplating to increase the specific surface area. We estimated the effective surface area by cyclic voltammetry (CV) and monitored the frequency shift induced by antigen-antibody interaction by the quartz crystal microbalance (QCM) method. The dendrite structure with the largest surface area was formed under -0.95 V for 5 min. In the measurement of the antigen-antibody interaction, the frequency shifts of 40, 80, and 110 Hz were obtained with the dendrite structured QCM chips formed at the above potential for 1, 1.5, and 2.0 min, respectively. The sensitivity was improved compared with that QCM chip having a flat surface electrode.

Disordered array of Au covered Silicon nanowires for SERS biosensing combined with electrochemical detection

NASA Astrophysics Data System (ADS)

Convertino, Annalisa; Mussi, Valentina; Maiolo, Luca

2016-04-01

We report on highly disordered array of Au coated silicon nanowires (Au/SiNWs) as surface enhanced Raman scattering (SERS) probe combined with electrochemical detection for biosensing applications. SiNWs, few microns long, were grown by plasma enhanced chemical vapor deposition on common microscope slides and covered by Au evaporated film, 150 nm thick. The capability of the resulting composite structure to act as SERS biosensor was studied via the biotin-avidin interaction: the Raman signal obtained from this structure allowed to follow each surface modification step as well as to detect efficiently avidin molecules over a broad range of concentrations from micromolar down to the nanomolar values. The metallic coverage wrapping SiNWs was exploited also to obtain a dual detection of the same bioanalyte by electrochemical impedance spectroscopy (EIS). Indeed, the SERS signal and impedance modifications induced by the biomolecule perturbations on the metalized surface of the NWs were monitored on the very same three-electrode device with the Au/SiNWs acting as both working electrode and SERS probe.

High surface area electrodes by template-free self-assembled hierarchical porous gold architecture.

PubMed

Morag, Ahiud; Golub, Tatiana; Becker, James; Jelinek, Raz

2016-06-15

The electrode active surface area is a crucial determinant in many electrochemical applications and devices. Porous metal substrates have been employed in electrode design, however construction of such materials generally involves multistep processes, generating in many instances electrodes exhibiting incomplete access to internal pore surfaces. Here we describe fabrication of electrodes comprising hierarchical, nano-to-microscale porous gold matrix, synthesized through spontaneous crystallization of gold thiocyanate in water. Cyclic voltammetry analysis revealed that the specific surface area of the conductive nanoporous Au microwires was very high and depended only upon the amount of gold used, not electrode areas or geometries. Application of the electrode in a pseudo-capacitor device is presented. Copyright © 2016 Elsevier Inc. All rights reserved.

Modification of Patterned Nanoporous Gold Thin Film Electrodes via Electro-annealing and Electrochemical Etching

NASA Astrophysics Data System (ADS)

Dorofeeva, Tatiana

Nanostructured materials have had a major impact on various fields, including medicine, catalysis, and energy storage, for the major part due to unique phenomena that arise at nanoscale. For this reason, there is a sustained need for new nanostructured materials, techniques to pattern them, and methods to precisely control their nanostructure. To that end, the primary focus of this dissertation is to demonstrate novel techniques to fabricate and tailor the morphology of a class of nanoporous metals, obtained by a process known as dealloying. In this process, while the less noble constituent of an alloy is chemically dissolved, surface-diffusion of the more noble constituent leads to self-assembly of a bicontinuous ligament network with characteristic porosity of ˜70% and ligament diameter of 10s of nanometers. As a model material produced by dealloying, this work employ nanoporous gold (np-Au), which has attracted significant attention of desirable features, such as high effective surface area, electrical conductivity, well-defined thiol-based surface modification strategies, microfabrication-compatibility, and biocompatibility. The most commonly method used to modify the morphology of np-Au is thermal treatment, where the enhanced diffusivity of the surface atoms leads to ligament (and consequently pore) coarsening. This method, however, is not conducive to modifying the morphology of thin films at specific locations on the film, which is necessary for creating devices that may need to contain different morphologies on a single device. In addition, coarsening attained by thermal treatment also leads to an undesirable reduction in effective surface area. In response to these challenges, this work demonstrates two different techniques that enables in situ modification of np-Au thin film electrodes obtained by sputter-deposition of a precursors silver-rich gold-silver alloy. The first method, referred to as electro-annealing, is achieved by injecting electrical current to np-Au electrodes, which leads coarsening due to a combination of Joule heating and other mechanisms. This method offers the capability to anneal different electrodes to varying degrees of coarsening in one step, by employing electrodes patterns with different cross-sectional areas - easily attained since np-Au can be patterned into arbitrary shapes via photolithography - to control electrode resistivity, thus current density and the amount of electro-annealing of an electrode. A surprising finding was that electro-annealing lead to electrode coarsening at much lower temperatures than conventional thermal treatment, which was attributed to augmented electron-surface atom interactions at high current densities that may in turn enhance surface atom diffusivity. A major advantage of electro-annealing is the ability to monitor the resistance change of the electrode (surrogate for electrode morphology) in real-time and vary the electro-annealing current accordingly to establish a closed-loop electro-annealing configuration. In nanostructured materials, the electrical resistance is often a function of nanostructure, thus changes in resistance can be directly linked to morphological changes of the electrode. Examination of the underlying mechanisms of nanostructure-dependent resistance change revealed that both ligament diameter and grain size play a role in dictating the observed electrode resistance change. The second method relies on electrochemical etching of ligaments to modify electrode morphology in order to maintain both a high effective surface area and large pores for unhindered transport of molecules to/from the ligament surfaces - an important consideration for many physico-chemical processes, such fuel cells, electrochemical sensors, and drug delivery platforms. The advantage of this method over purely chemical approach is that while an entire sample in exposed to the chemical reagent, the etching process does not occur until the necessary electrochemical potential is applied. Similar to the electro-annealing methods, electrical addressability allows for differentially modifying the morphology individual electrodes on a single substrate. The results of this study also revealed that electrochemical etching is a combination of coarsening and etching processes, where the optimization of etching parameters makes it possible precisely control the etching by favoring one process over the other. In summary, the two techniques, taken together in combination with np-Au's compatibility with microfabrication processes, can be extended to create multiple electrode arrays that display different morphologies for studying structure?property relationships and tuning catalysts/sensors for optimal performance.

N-Heterocyclic-Carbene-Treated Gold Surfaces in Pentacene Organic Field-Effect Transistors: Improved Stability and Contact at the Interface.

PubMed

Lv, Aifeng; Freitag, Matthias; Chepiga, Kathryn M; Schäfer, Andreas H; Glorius, Frank; Chi, Lifeng

2018-04-16

N-Heterocyclic carbenes (NHCs), which react with the surface of Au electrodes, have been successfully applied in pentacene transistors. With the application of NHCs, the charge-carrier mobility of pentacene transistors increased by five times, while the contact resistance at the pentacene-Au interface was reduced by 85 %. Even after annealing the NHC-Au electrodes at 200 °C for 2 h before pentacene deposition, the charge-carrier mobility of the pentacene transistors did not decrease. The distinguished performance makes NHCs as excellent alternatives to thiols as metal modifiers for the application in organic field-effect transistors (OFETs). © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Immunosensor based on electrodeposition of gold-nanoparticles and ionic liquid composite for detection of Salmonella pullorum.

PubMed

Wang, Dan; Dou, Wenchao; Zhao, Guangying; Chen, Yan

2014-11-01

In order to increase the reproducibility and stability of electrochemical immunosensor, which is a key issue for its application and popularization, an accurate and stable immunosensor for rapid detection of Salmonella pullorum (S. pullorum) was proposed in this study. The immunosensor was fabricated by modifying Screen-printed Carbon Electrode (SPCE) with electrodeposited gold nanoparticles (AuNPs), HRP-labeled anti-S. pullorum and ionic liquids (ILs) (AuNP/HRP/IL). AuNPs are electrodeposited on the working electrode surface to increase the amount of antibodies that bind to the electrode and then modified with ILs to protect the antibodies from being inactivated in the test environment and maintain their biological activity and the stability of the detection electrode. The electrochemical characteristics of the stepwise modified electrodes and the detection of S. pullorum were investigated by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). As shown in the results of the experiments, AuNPs with unique electrochemical properties as well as biocompatibility characteristics have been proven to be able to strengthen the antibody combination effectively and to increase the electrochemical response signal. In addition, a crucial assessment regarding implementation of stability and reproducibility analysis of a range of immunosensors is provided. We found that application of AuNPs/ILs in the immune modified electrodes showed obvious improvement when compared with other groups. Given their high levels of reproducibility, stability, target specificity and sensitivity, AuNPs and ILs were considered to be excellent elements for electrode modification. Copyright © 2014 Elsevier B.V. All rights reserved.

Glucose biosensor from covalent immobilization of chitosan-coupled carbon nanotubes on polyaniline-modified gold electrode.

PubMed

Wan, Dong; Yuan, Shaojun; Li, G L; Neoh, K G; Kang, E T

2010-11-01

An amperometric glucose biosensor was prepared using polyaniline (PANI) and chitosan-coupled carbon nanotubes (CS-CNTs) as the signal amplifiers and glucose oxidase (GOD) as the glucose detector on a gold electrode (the Au-g-PANI-c-(CS-CNTs)-GOD biosensor). The PANI layer was prepared via oxidative graft polymerization of aniline from the gold electrode surface premodified by self-assembled monolayer of 4-aminothiophenol. CS-CNTs were covalently coupled to the PANI-modified gold substrate using glutaradehyde as a bifunctional linker. GOD was then covalently bonded to the pendant hydroxyl groups of chitosan using 1,4-carbonyldiimidazole as the bifunctional linker. The surface functionalization processes were ascertained by X-ray photoelectron spectroscopy (XPS) analyses. The field emission scanning electron microscopy (FESEM) images of the Au-g-PANI-c-(CS-CNTs) electrode revealed the formation of a three-dimensional surface network structure. The electrode could thus provide a more spatially biocompatible microenvironment to enhance the amount and biocatalytic activity of the immobilized enzyme and to better mediate the electron transfer. The resulting Au-g-PANI-c-(CS-CNTs)-GOD biosensor exhibited a linear response to glucose in the concentration range of 1-20 mM, good sensitivity (21 μA/(mM·cm(2))), good reproducibility, and retention of >80% of the initial response current after 2 months of storage.

Bubble electrodeposition of gold porous nanocorals for the enzymatic and non-enzymatic detection of glucose.

PubMed

Sanzó, Gabriella; Taurino, Irene; Antiochia, Riccarda; Gorton, Lo; Favero, Gabriele; Mazzei, Franco; De Micheli, Giovanni; Carrara, Sandro

2016-12-01

Au nanocorals are grown on gold screen-printed electrodes (SPEs) by using a novel and simple one-step electrodeposition process. Scanning electron microscopy was used for the morphological characterization. The devices were assembled on a three-electrode SPE system, which is flexible and mass producible. The electroactive surface area, determined by cyclic voltammetry in sulphuric acid, was found to be 0.07±0.01cm(2) and 35.3±2.7cm(2) for bare Au and nanocoral Au, respectively. The nanocoral modified SPEs were used to develop an enzymatic glucose biosensor based on H2O2 detection. Au nanocoral electrodes showed a higher sensitivity of 48.3±0.9μA/(mMcm(2)) at +0.45V vs Ag|AgCl compared to a value of 24.6±1.3μA/(mMcm(2)) at +0.70V vs Ag|AgCl obtained with bare Au electrodes. However, the modified electrodes have indeed proven to be extremely powerful for the direct detection of glucose with a non-enzymatic approach. The results confirmed a clear peak observed by using nanocoral Au electrode even in the presence of chloride ions at physiological concentration. Amperometric study carried out at +0.15V vs Ag|AgCl in the presence of 0.12M NaCl showed a linear range for glucose between 0.1 and 13mM. Copyright © 2016. Published by Elsevier B.V.

An electrochemical biosensor based on nanoporous stainless steel modified by gold and palladium nanoparticles for simultaneous determination of levodopa and uric acid.

PubMed

Rezaei, Behzad; Shams-Ghahfarokhi, Leila; Havakeshian, Elaheh; Ensafi, Ali A

2016-09-01

In this paper, an electrochemical biosensor based on gold and palladium nano particles-modified nanoporous stainless steel (Au-Pd/NPSS) electrode has been introduced for the simultaneous determination of levodopa (LD) and uric acid (UA). To prepare the electrode, the stainless steel was anodized to fabricate NPSS and then Cu was electrodeposited onto the nanoporous steel by applying the multiple step potential. Finally, the electrode was immersed into a gold and palladium precursor's solution by the atomic ratio of 9:1 to form Au-Pd/NPSS through the galvanic replacement reaction. Morphological aspects, structural properties and the electroanalytical behavior of the Au-Pd/NPSS electrode were studied using field emission scanning electron microscopy (FE-SEM), energy dispersive X-ray spectroscopy (EDX), X-ray diffraction (XRD), electrochemical impedance spectroscopy (EIS) and voltammetric techniques. Also, differential pulse voltammetry (DPV) was used for the simultaneous determination of LD and UA. According to results, the surface of Au-Pd/NPSS electrode contained Au and Pd nanoparticles with an average diameter of 75nm. The electrode acted better than Au/NPSS and Pd/NPSS electrodes for the simultaneous determination of LD and UA, with the peak separation potential of about 220mV. Also, the calibration plot for LD was in two linear concentration ranges of 5.0-10.0 and 10.0-55.0μmolL(-1) and for UA, it was in the range of 100-1200μmolL(-1). The detection limit for LD and UA was 0.2 and 15μmolL(-1), respectively. The modified electrode had a good performance for LD and UA detection in urine, blood serum and levodopa C-Forte tablet. Copyright © 2016 Elsevier B.V. All rights reserved.

Electrochemical sensor based on electrodeposited graphene-Au modified electrode and nanoAu carrier amplified signal strategy for attomolar mercury detection.

PubMed

Zhang, Yi; Zeng, Guang Ming; Tang, Lin; Chen, Jun; Zhu, Yuan; He, Xiao Xiao; He, Yan

2015-01-20

An electrochemical sensor was developed for attomolar Hg(2+) detection. Three single-stranded DNA probes were rationally designed for selective and sensitive detection of the target, which combined T-Hg(2+)-T coordination chemistry and the characteristic of convenient modification of electrochemical signal indicator. Graphene and nanoAu were successively electrodeposited on a glass carbon electrode surface to improve the electrode conductivity and functionalize with the 10-mer thymine-rich DNA probe (P1). NanoAu carriers functionalized with 29-mer guanine-rich DNA probe (P3) labeled methyl blue (MB-nanoAu-P 3s) were used to further strengthen signal response. In the presence of Hg(2+), a T-T mismatched dsDNA would occur between P1 and a 22-mer thymine-rich DNA probe (P2) on the electrode surface due to T-Hg(2+)-T coordination chemistry. Followed by adding the MB-nanoAu-P 3s for hybridization with P2, square wave voltammetry was executed. Under optimal conditions, Hg(2+) could be detected in the range from 1.0 aM to 100 nM with a detection limit of 0.001 aM. Selectivity measurements reveal that the sensor is specific for Hg(2+) even with interference by high concentrations of other metal ions. Three different environmental samples were analyzed by the sensor and the results were compared with that from an atomic fluorescence spectrometry. The developed sensor was demonstrated to achieve excellent detectability. It may be applied to development of ultrasensitive detection strategies.

Surface electrochemistry of CO on reconstructed gold single crystal surfaces studied by infrared reflection absorption spectroscopy and rotating disk electrode.

PubMed

Blizanac, Berislav B; Arenz, Matthias; Ross, Philip N; Marković, Nenad M

2004-08-18

The electrooxidation of CO has been studied on reconstructed gold single-crystal surfaces by a combination of electrochemical (EC) and infrared reflection absorption spectroscopy (IRAS) measurements. Emphasis is placed on relating the vibrational properties of the CO adlayer to the voltammetric and other macroscopic electrochemical responses, including rotating disk electrode measurements of the catalytic activity. The IRAS data show that the C-O stretching frequencies are strongly dependent on the surface orientation and can be observed in the range 1940-1990 cm(-1) for the 3-fold bridging, 2005-2070 cm(-1) for the 2-fold bridging, and 2115-2140 for the terminal position. The most complex CO spectra are found for the Au(110)-(1 x 2) surface, i.e., a band near 1965 cm(-1), with the second, weaker band shifted positively by about 45 cm(-1) and, finally, a weak band near 2115 cm(-1). While the C-O stretching frequencies for a CO adlayer adsorbed on Au(111)-(1 x 23) show nu(CO) bands at 2029-2069 cm(-1) and at 1944-1986 cm(-1), on the Au(100)-"hex" surface a single CO band is observed at 2004-2029 cm(-1). In the "argon-purged" solution, the terminal nu(CO) band on Au(110)-(1 x 2) and the 3-fold bridging band on the Au(111)-(1 x 23) disappear entirely. The IRAS/EC data show that the kinetics of CO oxidation are structure sensitive; i.e., the onset of CO oxidation increases in the order Au(110)-(1 x 2) > or = Au(100)-"hex" > Au(111)-(1 x 23). Possible explanations for the structure sensitivity are discussed.

In Vivo Neural Recording and Electrochemical Performance of Microelectrode Arrays Modified by Rough-Surfaced AuPt Alloy Nanoparticles with Nanoporosity

PubMed Central

Zhao, Zongya; Gong, Ruxue; Zheng, Liang; Wang, Jue

2016-01-01

In order to reduce the impedance and improve in vivo neural recording performance of our developed Michigan type silicon electrodes, rough-surfaced AuPt alloy nanoparticles with nanoporosity were deposited on gold microelectrode sites through electro-co-deposition of Au-Pt-Cu alloy nanoparticles, followed by chemical dealloying Cu. The AuPt alloy nanoparticles modified gold microelectrode sites were characterized by scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and in vivo neural recording experiment. The SEM images showed that the prepared AuPt alloy nanoparticles exhibited cauliflower-like shapes and possessed very rough surfaces with many different sizes of pores. Average impedance of rough-surfaced AuPt alloy nanoparticles modified sites was 0.23 MΩ at 1 kHz, which was only 4.7% of that of bare gold microelectrode sites (4.9 MΩ), and corresponding in vitro background noise in the range of 1 Hz to 7500 Hz decreased to 7.5 μVrms from 34.1 μVrms at bare gold microelectrode sites. Spontaneous spike signal recording was used to evaluate in vivo neural recording performance of modified microelectrode sites, and results showed that rough-surfaced AuPt alloy nanoparticles modified microelectrode sites exhibited higher average spike signal-to-noise ratio (SNR) of 4.8 in lateral globus pallidus (GPe) due to lower background noise compared to control microelectrodes. Electro-co-deposition of Au-Pt-Cu alloy nanoparticles combined with chemical dealloying Cu was a convenient way for increasing the effective surface area of microelectrode sites, which could reduce electrode impedance and improve the quality of in vivo spike signal recording. PMID:27827893

Simple fabrication of pineapple root-like palladium-gold catalysts as the high-efficiency cathode in direct peroxide-peroxide fuel cells.

PubMed

Wang, Xin; Ye, Ke; Sun, Ce; Zhang, Hongyu; Zhu, Kai; Cheng, Kui; Wang, Guiling; Cao, Dianxue

2017-07-15

Pd-Au/TiC electrodes with various three-dimensional structures are obtained by the pulsed potential electro-deposition in PdCl 2 /HAuCl 4 electrolytes. The morphologies of Pd-Au/TiC composite catalysts are significantly dependent on the component of deposited solutions. The surface appearance of Pd-Au catalysts changes from rime-shaped structure, to feather-like construction, then to pineapple root-like structure and finally to flower-like configuration with the increase of PdCl 2 content in electrolytes. These particular three-dimensional structures may be very suitable for H 2 O 2 electro-reduction, which assures a high utilization of Pd-Au catalysts and provides a large specific surface area. The electro-catalytic activities of H 2 O 2 reduction on the Pd-Au/TiC electrodes improve as increasing the Pd content in Pd-Au alloy catalysts. The pineapple root-like Pd 5 Au 1 /TiC electrode reveals remarkably excellent electrochemical property and desirable stability for catalyzing H 2 O 2 reduction in acid media. The direct peroxide-peroxide fuel cells with a 10 cm 3 min -1 flow rate display the open circuit voltage (OCV) of 0.85V and the peak power density of 56.5mWcm -2 at 155mAcm -2 with desirable cell stability, which is much higher than those previously reported. Copyright © 2017 Elsevier Inc. All rights reserved.

Synthesis and electrocatalytic activity of Au/Pt bimetallic nanodendrites for ethanol oxidation in alkaline medium.

PubMed

Han, Xinyi; Wang, Dawei; Liu, Dong; Huang, Jianshe; You, Tianyan

2012-02-01

Gold/Platinum (Au/Pt) bimetallic nanodendrites were successfully synthesized through seeded growth method using preformed Au nanodendrites as seeds and ascorbic acid as reductant. Cyclic voltammograms (CVs) of a series of Au/Pt nanodendrites modified electrodes in 1M KOH solution containing 1M ethanol showed that the electrocatalyst with a molar ratio (Au:Pt) of 3 exhibited the highest peak current density and the lowest onset potential. The peak current density of ethanol electro-oxidation on the Au(3)Pt(1) nanodendrites modified glassy carbon electrode (Au(3)Pt(1) electrode) is about 16, 12.5, and 4.5 times higher than those on the polycrystalline Pt electrode, polycrystalline Au electrode, and Au nanodendrites modified glassy carbon electrode (Au dendrites electrode), respectively. The oxidation peak potential of ethanol electro-oxidation on the Au(3)Pt(1) electrode is about 299 and 276 mV lower than those on the polycrystalline Au electrode and Au dendrites electrode, respectively. These results demonstrated that the Au/Pt bimetallic nanodendrites may find potential application in alkaline direct ethanol fuel cells (ADEFCs). Copyright © 2011 Elsevier Inc. All rights reserved.

Development of paper-gate transistor toward direct detection from microbiological fluids

NASA Astrophysics Data System (ADS)

Kajisa, Taira; Sakata, Toshiya

2017-04-01

In this study, a paper-gate transistor was developed to detect glucose using an extended-gate field-effect transistor (FET). A filter paper was used as an extended gate electrode, in which Au nanoparticles (AuNPs) modified with phenylboronic acids (PBAs) were included. PBA-AuNPs play an important role as a support to not only be entrapped in cellulose fibrils but also bind to the targeted glucose in a paper. The surface properties of PBA-AuNPs were investigated to elucidate the electrical properties of the paper-gate electrode using an absorption spectrum and a zeta potential analysis. Moreover, the paper-gate electrode enabled us to detect glucose at the micromolar level on the basis of the principle of FET devices. A platform based on the paper-gate transistor is suitable for a highly sensitive system to detect glucose in trace samples such as tears, sweat, and saliva in the future.

Nanoscale Polysulfides Reactors Achieved by Chemical Au-S Interaction: Improving the Performance of Li-S Batteries on the Electrode Level.

PubMed

Fan, Chao-Ying; Xiao, Pin; Li, Huan-Huan; Wang, Hai-Feng; Zhang, Lin-Lin; Sun, Hai-Zhu; Wu, Xing-Long; Xie, Hai-Ming; Zhang, Jing-Ping

2015-12-23

In this work, the chemical interaction of cathode and lithium polysulfides (LiPSs), which is a more targeted approach for completely preventing the shuttle of LiPSs in lithium-sulfur (Li-S) batteries, has been established on the electrode level. Through simply posttreating the ordinary sulfur cathode in atmospheric environment just for several minutes, the Au nanoparticles (Au NPs) were well-decorated on/in the surface and pores of the electrode composed of commercial acetylene black (CB) and sulfur powder. The Au NPs can covalently stabilize the sulfur/LiPSs, which is advantageous for restricting the shuttle effect. Moreover, the LiPSs reservoirs of Au NPs with high conductivity can significantly control the deposition of the trapped LiPSs, contributing to the uniform distribution of sulfur species upon charging/discharging. The slight modification of the cathode with <3 wt % Au NPs has favorably prospered the cycle capacity and stability of Li-S batteries. Moreover, this cathode exhibited an excellent anti-self-discharge ability. The slight decoration for the ordinary electrode, which can be easily accessed in the industrial process, provides a facile strategy for improving the performance of commercial carbon-based Li-S batteries toward practical application.

Electrocatalytic Reduction of CO 2 at Au Nanoparticle Electrodes: Effects of Interfacial Chemistry on Reduction Behavior

DOE PAGES

Andrews, Evan; Katla, Sai; Kumar, Challa; ...

2015-09-12

Nanoscale Au electrocatalysts demonstrate the extraordinary ability to reduce CO 2 at low overpotentials with high selectivity to CO. Here, we investigate the role of surface chemistry on CO 2 reduction behavior using Au 25 and 5 nm Au nanoparticles. Onset potentials for CO 2 reduction at Au 25 nanoparticles in Nafion binders are shifted anodically by 190 mV while the hydrogen evolution reaction is shifted cathodically by 300 mV relative to Au foil. The net effect of this beneficial separation in onset potentials is relatively high Faradayic efficiencies for CO (90% at 0.8 V versus RHE) at high currentmore » densities. Experimental results show Faradayic efficiencies for CO are greatest using electrodes made with Nafion-immobilized Au 25 nanoparticles. Likewise, CO 2 reduction onset potential shifts are greater for smaller nanoparticles and when Nafion binders are used instead of (sulfonate-free) polyvinylidene fluoride. X-ray photoelectron spectroscopy analysis reveals Au nanoparticles may react with the sulfonates of Nafion binders. Here, the results suggest sulfonate interfaces may alter the binding energies of key species or lead to favorable reconstructions, either of which ultimately results in remarkable improvements in Faradayic efficiencies relative to Au foil electrodes.« less

Adsorption of Pyridine at the Au(100)-Solution Interface.

DTIC Science & Technology

1987-09-25

quatiatively characterize the energetics of pyridine adsorption onto a gold ( 100) single crystal electrode surface. Over the potential region investigated...0.8 to +0.6 A., three orientationis of the pyridine molecules on the gold surface have been observed. The pyridine orientation Is strongly 1nflue ied by...the electrode potential. At a positively charged surface, the pyridine assumes a verticle orientation with .fie nitrogen atom facing the gold surface

Construction and direct electrochemistry of orientation controlled laccase electrode.

PubMed

Li, Ying; Zhang, Jiwei; Huang, Xirong; Wang, Tianhong

2014-03-28

A laccase has multiple redox centres. Chemisorption of laccases on a gold electrode through a polypeptide tag introduced at the protein surface provides an isotropic orientation of laccases on the Au surface, which allows the orientation dependent study of the direct electrochemistry of laccase. In this paper, using genetic engineering technology, two forms of recombinant laccase which has Cys-6×His tag at the N or C terminus were generated. Via the Au-S linkage, the recombinant laccase was assembled orientationally on gold electrode. A direct electron transfer and a bioelectrocatalytic activity toward oxygen reduction were observed on the two orientation controlled laccase electrodes, but their electrochemical behaviors were found to be quite different. The orientation of laccase on the gold electrode affects both the electron transfer pathway and the electron transfer efficiency of O2 reduction. The present study is helpful not only to the in-depth understanding of the direct electrochemistry of laccase, but also to the development of laccase-based biofuel cells. Copyright © 2014 Elsevier Inc. All rights reserved.

Synthesis of one-dimensional gold nanostructures and the electrochemical application of the nanohybrid containing functionalized graphene oxide for cholesterol biosensing.

PubMed

Nandini, Seetharamaiah; Nalini, Seetharamaiah; Reddy, M B Madhusudana; Suresh, Gurukar Shivappa; Melo, Jose Savio; Niranjana, Pathappa; Sanetuntikul, Jakkid; Shanmugam, Sangaraju

2016-08-01

This manuscript reports a new approach for the synthesis of one dimensional gold nanostructure (AuNs) and its application in the development of cholesterol biosensor. Au nanostructures have been synthesized by exploiting β-diphenylalanine (β-FF) as an sacrificial template, whereas the Au nanoparticles (AuNPs) were synthesized by ultrasound irradiation. X-ray diffractometer (XRD), scanning electron microscope (SEM) and energy dispersive analysis of X-rays (EDAX) have been employed to characterize the morphology and composition of the prepared samples. With the aim to develop a highly sensitive cholesterol biosensor, cholesterol oxidase (ChOx) was immobilized on AuNs which were appended on the graphite (Gr) electrode via chemisorption onto thiol-functionalized graphene oxide (GO-SH). This Gr/GO-SH/AuNs/ChOx biosensor has been characterized using cyclic voltammetry (CV), electrochemical impedance spectroscopy and chronoamperometry. CV results indicated a direct electron transfer between the enzyme and the electrode surface. A new potentiostat intermitant titration technique (PITT) has been studied to determine the diffusion coefficient and maxima potential value. The proposed biosensor showed rapid response, high sensitivity, wide linear range and low detection limit. Furthermore, our AuNs modified electrode showed excellent selectivity, repeatability, reproducibility and long term stability. The proposed electrode has also been used successfully to determine cholesterol in serum samples. Copyright © 2016 Elsevier B.V. All rights reserved.

Thermo-compressive transfer printing for facile alignment and robust device integration of nanowires.

PubMed

Lee, Won Seok; Won, Sejeong; Park, Jeunghee; Lee, Jihye; Park, Inkyu

2012-06-07

Controlled alignment and mechanically robust bonding between nanowires (NWs) and electrodes are essential requirements for reliable operation of functional NW-based electronic devices. In this work, we developed a novel process for the alignment and bonding between NWs and metal electrodes by using thermo-compressive transfer printing. In this process, bottom-up synthesized NWs were aligned in parallel by shear loading onto the intermediate substrate and then finally transferred onto the target substrate with low melting temperature metal electrodes. In particular, multi-layer (e.g. Cr/Au/In/Au and Cr/Cu/In/Au) metal electrodes are softened at low temperatures (below 100 °C) and facilitate submergence of aligned NWs into the surface of electrodes at a moderate pressure (∼5 bar). By using this thermo-compressive transfer printing process, robust electrical and mechanical contact between NWs and metal electrodes can be realized. This method is believed to be very useful for the large-area fabrication of NW-based electrical devices with improved mechanical robustness, electrical contact resistance, and reliability.

Nanoscale Au-In alloy-oxide core-shell particles as electrocatalysts for efficient hydroquinone detection

DOE PAGES

Sutter, E.; Tong, X.; Medina-Plaza, C.; ...

2015-10-09

The presence of hydroquinone (HQ), a phenol ubiquitous in nature and widely used in industry, needs to be monitored because of its toxicity to the environment. Here we demonstrate efficient detection of HQ using simple, fast, and noninvasive electrochemical measurements on indium tin oxide (ITO) electrodes modified with nanoparticles comprising bimetallic Au–In cores and mixed Au–In oxide shells. Whereas bare ITO electrodes show very low activity for the detection of HQ, their modification with Au–In core–shell nanoparticles induces a pronounced shift of the oxidation peak to lower potentials, i.e., facilitated oxidation. The response of the different electrodes was correlated withmore » the initial composition of the bimetallic nanoparticle cores, which in turn determined the amount of Au and In stabilized on the surface of the amorphous Au–In oxide shells available for the electrochemical reaction. While adding core–shell nanostructures with different compositions of the alloy core facilitates the electrocatalytic (reduction-) oxidation of HQ, the activity is highest for particles with AuIn cores (i.e., a Au:In ratio of 1). This optimal system is found to follow a single pathway, the two-electron oxidation of the quinone–hydroquinone couple, which gives rise to high oxidation peaks and is most effective in facilitating the electrode-to-analyte charge transfer and thus detection. The limits of detection (LOD) decreased when increasing the amount of Au exposed on the surface of the amorphous Au–In oxide shells. As a result the LODs were in the range of 10 –5 – 10 –6 M and were lower than those obtained using bulk Au.« less

Sensitive detection of microRNAs based on the conversion of colorimetric assay into electrochemical analysis with duplex-specific nuclease-assisted signal amplification

PubMed Central

Xia, Ning; Liu, Ke; Zhou, Yingying; Li, Yuanyuan; Yi, Xinyao

2017-01-01

miRNAs have emerged as new biomarkers for the detection of a wide variety of cancers. By employing duplex-specific nuclease for signal amplification and gold nanoparticles (AuNPs) as the carriers of detection probes, a novel electrochemical assay of miRNAs was performed. The method is based on conversion of the well-known colorimetric assay into electrochemical analysis with enhanced sensitivity. DNA capture probes immobilized on the electrode surface and ferrocene (Fc)-labeled DNA detection probes (denoted “Fc-DNA-Fc”) presented in the solution induced the assembly of positively charged AuNPs on the electrode surface through the electrostatic interaction. As a result, a large number of Fc-DNA-Fc molecules were attached on the electrode surface, thus amplifying the electrochemical signal. When duplex-specific nuclease was added to recycle the process of miRNA-initiated digestion of the immobilized DNA probes, Fc-DNA-Fc-induced assembly of AuNPs on the electrode surface could not occur. This resulted in a significant fall in the oxidation current of Fc. The current was found to be inversely proportional to the concentration of miRNAs in the range of 0–25 fM, and a detection limit of 0.1 fM was achieved. Moreover, this work presents a new method for converting colorimetric assays into sensitive electrochemical analyses, and thus would be valuable for design of novel chemical/biosensors. PMID:28761341

Novel surface diffusion characteristics for a robust pentacene derivative on Au(1 1 1) surfaces

NASA Astrophysics Data System (ADS)

Miller, Ryan A.; Larson, Amanda; Pohl, Karsten

2017-06-01

Molecular dynamics simulations have been performed in both the ab initio and classical mechanics frameworks of 5,6,7-trithiapentacene-13-one (TTPO) molecules on flat Au(1 1 1) surfaces. Results show new surface diffusion characteristics including a strong preference for the molecule to align its long axis parallel to the sixfold Au(1 1 1) symmetry directions and subsequently diffuse along these close-packed directions, and a calculated activation energy for diffusion of 0.142 eV, about four times larger than that for pure pentacene on Au. The temperature-dependent diffusion coefficients were calculated to help quantify the molecular mobility during the experimentally observed process of forming self-assembled monolayers on gold electrodes.

Kinetics of Electrocatalysis of Dibromoalkyl Reductions Using Electrodes with Covalently Immobilized Metallotetraphenylporphyrins.

DTIC Science & Technology

1981-01-29

Technical Report Using Electrodes with Covalently Immobilized Metal l otetraphenyl porphyri ns G. PERFORMING ORG. REPORT NUMBER 7. AU𔄁IOR(’.) 0...and CH2BrCHBrCH 3 at the surfaces of electrodes to which cobalt(II) or copper (II) tetra(p-aminophenyl)porphyrin has been covalently attached is strongly...27514 ABSTRACT The reduction of PhCHBrCH 2 Br, PhCHBrCHBrPh, and CH2BrCHBrCH3 at the surfaces of electrodes to which cobalt(lI) or copper (If) tetra(p

Functionalization of gold and graphene electrodes by p-maleimido-phenyl towards thiol-sensing systems investigated by EQCM and IR ellipsometric spectroscopy

NASA Astrophysics Data System (ADS)

Neubert, Tilmann J.; Rösicke, Felix; Sun, Guoguang; Janietz, Silvia; Gluba, Marc A.; Hinrichs, Karsten; Nickel, Norbert H.; Rappich, Jörg

2017-11-01

Electrografting of gold and graphene surfaces by functional p-(N-maleimido)phenyl groups was performed by reduction of p-(N-maleimido)phenyldiazonium tetrafluoroborate. The reduction was carried out using cyclic voltammetry coupled with micro-gravimetric measurements by means of electrochemical quartz crystal microbalance (EQCM). The overall deposited mass on gold was higher than on graphene. However, the Faradaic efficiency was lower on Au (14%) compared to graphene (22%) after the first potential scan. Subsequently, the maleimide functional groups have been tested for immobilization of terminal thiols using (4-nitrobenzyl)mercaptan for the functionalized graphene surface and a cysteine-modified peptide for the functionalized gold surface. The functionalization by p-(N-maleimido)phenyl groups and the following thiol coupling of the particular surface was proven by infrared spectroscopic ellipsometry (IRSE). In addition, the interaction of the tetrabutylammonium and tetrafluoroborate ions present in the electrolyte with the Au and graphene electrodes was investigated by EQCM and revealed less electrostatic interaction of graphene with these ions in solution compared to the metal (Au) surface.

Gold-copper bimetallic nanoparticles supported on nano P zeolite modified carbon paste electrode as an efficient electrocatalyst and sensitive sensor for determination of hydrazine.

PubMed

Amiripour, Fatemeh; Azizi, Seyed Naser; Ghasemi, Shahram

2018-06-01

In this report, a facile, efficient and low cost electrochemical sensor based on bimetallic Au-Cu nanoparticles supported on P nanozeolite modified carbon paste electrode (Au-Cu/NPZ/CPE) was constructed and its efficiency for determination of hydrazine in trace level was studied. For this purpose, agro waste material, stem sweep ash (SSA) was employed as the starting material (silica source) for the synthesis of nano P zeolite (NPZ). After characterization of the synthesized NPZ by analytical instruments (scanning electronic microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD) and Fourier transform infrared (FT-IR) spectroscopy), construction of Au-Cu/NPZ/CPE was performed by three steps procedure involving preparation of nano P zeolite modified carbon paste electrode (NPZ/CPE), introducing Cu +2 ions into nano zeolite structure by ion exchange and electrochemical reduction of Cu +2 ions upon applying constant potential. This procedure is followed by partial replacement of Cu by Au due to galvanic replacement reaction (GRR). The electrochemical properties of hydrazine at the surface of Au-Cu/NPZ/CPE was evaluated using cyclic voltammetry (CV), amperometry, and chronoamperometry methods in 0.1 M phosphate buffer solution (PBS). It was found that the prepared sensor has higher electrocatalytic activity at a relatively lower potential compared to other modified electrodes including Au/NPZ/CPE, Cu/NPZ/CPE, Au-Cu/CPE and etc. Moreover, the proposed electrochemical sensor presented the favorable analytical properties for determination of hydrazine such as low detection limit (0.04 µM), rapid response time (3 s), wide linear range (0.01-150 mM), and high sensitivity (99.53 µA mM -1 ) that are related to the synergic effect of bimetallic of Au-Cu, porous structure and enough surface area of NPZ. In addition, capability of Au-Cu/NPZ/CPE sensor was successfully tested in real samples with good accuracy and precision. Copyright © 2018 Elsevier B.V. All rights reserved.

Highly Ordered Periodic Au/TiO₂ Hetero-Nanostructures for Plasmon-Induced Enhancement of the Activity and Stability for Ethanol Electro-oxidation.

PubMed

Jin, Zhao; Wang, Qiyu; Zheng, Weitao; Cui, Xiaoqiang

2016-03-02

The catalytic electro-oxidation of ethanol is the essential technique for direct alcohol fuel cells (DAFCs) in the area of alternative energy for the ability of converting the chemical energy of alcohol into the electric energy directly. Developing highly efficient and stable electrode materials with antipoisoning ability for ethanol electro-oxidation remains a challenge. A highly ordered periodic Au-nanoparticle (NP)-decorated bilayer TiO2 nanotube (BTNT) heteronanostructure was fabricated by a two-step anodic oxidation of Ti foil and the subsequent photoreduction of HAuCl4. The plasmon-induced charge separation on the heterointerface of Au/TiO2 electrode enhances the electrocatalytic activity and stability for the ethanol oxidation under visible light irradiation. The highly ordered periodic heterostructure on the electrode surface enhanced the light harvesting and led to the greater performance of ethanol electro-oxidation under irradiation compared with the ordinary Au NPs-decorated monolayer TiO2 nanotube (MTNT). This novel Au/TiO2 electrode also performed a self-cleaning property under visible light attributed to the enhanced electro-oxidation of the adsorbed intermediates. This light-driven enhancement of the electrochemical performances provides a development strategy for the design and construction of DAFCs.

Electrochemical determination of dopamine and ascorbic acid at a novel gold nanoparticles distributed poly(4-aminothiophenol) modified electrode.

PubMed

Gopalan, Anantha Iyengar; Lee, Kwang-Pill; Manesh, Kalayil Manian; Santhosh, Padmanabhan; Kim, Jun Heon; Kang, Jae Soo

2007-03-15

A modified electrode is fabricated by embedding gold nanoparticles into a layer of electroactive polymer, poly(4-aminothiophenol) (PAT) on the surface of glassy carbon (GC) electrode. Cyclic voltammetry (CV) is performed to deposit PAT and concomitantly deposit Au nanoparticles. Field emission transmission electron microscopic image of the modified electrode, PAT-Au(nano)-ME, indicates the presence of uniformly distributed Au nanoparticles having the sizes of 8-10nm. Electrochemical behavior of the PAT-Au(nano)-ME towards detection of ascorbic acid (AA) and dopamine (DA) is studied using CV. Electrocatalytic determination of DA in the presence of fixed concentration of AA and vice versa, are studied using differential pulse voltammetry (DPV). PAT-Au(nano)-ME exhibits two well defined anodic peaks at the potential of 75 and 400mV for the oxidation of AA and DA, respectively with a potential difference of 325mV. Further, the simultaneous determination of AA and DA is studied by varying the concentration of AA and DA. PAT-Au(nano)-ME exhibits selectivity and sensitivity for the simultaneous determination of AA and DA without fouling by the oxidation products of AA or DA. PAT and Au nanoparticles provide synergic influence on the accurate electrochemical determination of AA or DA from a mixture having any one of the component (AA or DA) in excess. The practical analytical utilities of the PAT-Au(nano)-ME are demonstrated by the determination of DA and AA in dopamine hydrochloride injection and human blood serum samples.

Sensitive Adsorptive Voltammetric Method for Determination of Bisphenol A by Gold Nanoparticle/Polyvinylpyrrolidone-Modified Pencil Graphite Electrode

PubMed Central

Yaman, Yesim Tugce; Abaci, Serdar

2016-01-01

A novel electrochemical sensor gold nanoparticle (AuNP)/polyvinylpyrrolidone (PVP) modified pencil graphite electrode (PGE) was developed for the ultrasensitive determination of Bisphenol A (BPA). The gold nanoparticles were electrodeposited by constant potential electrolysis and PVP was attached by passive adsorption onto the electrode surface. The electrode surfaces were characterized by electrochemical impedance spectroscopy (EIS) and scanning electron microscopy (SEM). The parameters that affected the experimental conditions were researched and optimized. The AuNP/PVP/PGE sensor provided high sensitivity and selectivity for BPA recognition by using square wave adsorptive stripping voltammetry (SWAdSV). Under optimized conditions, the detection limit was found to be 1.0 nM. This new sensor system offered the advantages of simple fabrication which aided the expeditious replication, low cost, fast response, high sensitivity and low background current for BPA. This new sensor system was successfully tested for the detection of the amount of BPA in bottled drinking water with high reliability. PMID:27231912

Efficient electrocatalytic conversion of CO.sub.2 to CO using ligand-protected Au.sub.25 clusters

DOEpatents

Kauffman, Douglas; Matranga, Christopher; Qian, Huifeng; Jin, Rongchao; Alfonso, Dominic R.

2015-09-22

An apparatus and method for CO.sub.2 reduction using an Au.sub.25 electrode. The Au.sub.25 electrode is comprised of ligand-protected Au.sub.25 having a structure comprising an icosahedral core of 13 atoms surrounded by a shell of six semi-ring structures bonded to the core of 13 atoms, where each semi-ring structure is typically --SR--Au--SR--Au--SR or --SeR--Au--SeR--Au--SeR. The 12 semi-ring gold atoms within the six semi-ring structures are stellated on 12 of the 20 faces of the icosahedron of the Au.sub.13 core, and organic ligand --SR or --SeR groups are bonded to the Au.sub.13 core with sulfur or selenium atoms. The Au.sub.25 electrode and a counter-electrode are in contact with an electrolyte comprising CO.sub.2 and H+, and a potential of at least -0.1 volts is applied from the Au.sub.25 electrode to the counter-electrode.

Electrode quenching control for highly efficient CsPbBr3 perovskite light-emitting diodes via surface plasmon resonance and enhanced hole injection by Au nanoparticles.

PubMed

Meng, Yan; Wu, Xiaoyan; Xiong, Ziyang; Lin, Chunyan; Xiong, Zuhong; Blount, Ethan; Chen, Ping

2018-04-27

Compared to organic-inorganic hybrid metal halide perovskites, all-inorganic cesium lead halides (e.g, CsPbBr 3 ) hold greater promise in being emissive materials for light-emitting diodes owing to their superior optoelectronic properties as well as their higher stabilities. However, there is still considerable potential for breakthroughs in the current efficiency of CsPbBr 3 perovskite light-emitting diodes (PeLEDs). Electrode quenching is one of the main problems limiting the current efficiency of PeLEDs when poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) is used as the hole injection layer. In this work, electrode quenching control was realized via incorporating Au NPs into PEDOT:PSS. As a result, the CsPbBr 3 PeLEDs realized an improvement in maximum luminescence ranging from ∼2348 to ∼7660 cd m -2 (∼226% enhancement) and current efficiency from 1.65 to 3.08 cd A -1 (∼86% enhancement). Such substantial enhancement of the electroluminescent performance can be attributed to effective electrode quenching control at the PEDOT:PSS/CsPbBr 3 perovskite interface via the combined effects of local surface plasma resonance coupling and enhanced hole transportation in the PEDOT:PSS layer by Au nanoparticles.

Electrode quenching control for highly efficient CsPbBr3 perovskite light-emitting diodes via surface plasmon resonance and enhanced hole injection by Au nanoparticles

NASA Astrophysics Data System (ADS)

Meng, Yan; Wu, Xiaoyan; Xiong, Ziyang; Lin, Chunyan; Xiong, Zuhong; Blount, Ethan; Chen, Ping

2018-04-01

Compared to organic-inorganic hybrid metal halide perovskites, all-inorganic cesium lead halides (e.g, CsPbBr3) hold greater promise in being emissive materials for light-emitting diodes owing to their superior optoelectronic properties as well as their higher stabilities. However, there is still considerable potential for breakthroughs in the current efficiency of CsPbBr3 perovskite light-emitting diodes (PeLEDs). Electrode quenching is one of the main problems limiting the current efficiency of PeLEDs when poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) is used as the hole injection layer. In this work, electrode quenching control was realized via incorporating Au NPs into PEDOT:PSS. As a result, the CsPbBr3 PeLEDs realized an improvement in maximum luminescence ranging from ˜2348 to ˜7660 cd m-2 (˜226% enhancement) and current efficiency from 1.65 to 3.08 cd A-1 (˜86% enhancement). Such substantial enhancement of the electroluminescent performance can be attributed to effective electrode quenching control at the PEDOT:PSS/CsPbBr3 perovskite interface via the combined effects of local surface plasma resonance coupling and enhanced hole transportation in the PEDOT:PSS layer by Au nanoparticles.

DNAzyme-functionalized gold-palladium hybrid nanostructures for triple signal amplification of impedimetric immunosensor.

PubMed

Hou, Li; Gao, Zhuangqiang; Xu, Mingdi; Cao, Xia; Wu, Xiaoping; Chen, Guonan; Tang, Dianping

2014-04-15

A highly sensitive and selective impedimetric immunosensor with triple signal amplification was designed for ultrasensitive detection of prostate-specific antigen (PSA) by using anti-PSA antibody and DNAzyme-functionalized gold-palladium hybrid nanotags (Ab2-AuPd-DNA). The signal was amplified based on the Ab2-AuPd-DNA toward the catalytic precipitation of 4-choloro-1-naphthol (4-CN). DNAzyme (as a kind of peroxidase mimic) could catalyze the oxidation of 4-CN, whilst AuPd hybrid nanostructures could not only provide a large surface coverage for immobilization of biomolecules but also promote 4-CN oxidation to some extent. The produced insoluble benzo-4-chlorohexadienone via 4-CN was coated on the electrode surface, and hindered the electron transfer between the solution and the electrode, thereby increasing the Faradaic impedance of the base electrode. Three labeling strategies including Ab2-AuNP, Ab2-AuPd and Ab2-AuPd-DNA were investigated for determination of PSA, and improved analytical features were obtained with the Ab2-AuPd-DNA strategy. Under optimal conditions, the dynamic concentration range of the impedimetric immunosensor spanned from 1.0 pg mL(-1) to 50 ng mL(-1) PSA with a detection limit of 0.73 pg mL(-1). Intra- and inter-assay coefficients of variation were below 8.5% and 9.5%, respectively. Importantly, no significant differences at the 0.05 significance level were encountered in the analysis of 6 clinical serum specimens and 6 diluted standards between the impedimetric immunosensor and the commercialized electrochemiluminescent method for PSA detection. © 2013 Published by Elsevier B.V.

Controlled Vectorial Electron Transfer and Photoelectrochemical Applications of Layered Relay/Photosensitizer-Imprinted Au Nanoparticle Architectures on Electrodes.

PubMed

Metzger, Tzuriel S; Tel-Vered, Ran; Willner, Itamar

2016-03-23

Two configurations of molecularly imprinted bis-aniline-bridged Au nanoparticles (NPs) for the specific binding of the electron acceptor N,N'-dimethyl-4,4'-bipyridinium (MV(2+) ) and for the photosensitizer Zn(II)-protoporphyrin IX (Zn(II)-PP-IX) are assembled on electrodes, and the photoelectrochemical features of the two configurations are discussed. Configuration I includes the MV(2+) -imprinted Au NPs matrix as a base layer, on which the Zn(II)-PP-IX-imprinted Au NPs layer is deposited, while configuration II consists of a bilayer corresponding to the reversed imprinting order. Irradiation of the two electrodes in the presence of a benzoquinone/benzohydroquinone redox probe yields photocurrents of unique features: (i) Whereas configuration I yields an anodic photocurrent, the photocurrent generated by configuration II is cathodic. (ii) The photocurrents obtained upon irradiation of the imprinted electrodes are substantially higher as compared to the nonimprinted surfaces. The high photocurrents generated by the imprinted Au NPs-modified electrodes are attributed to the effective loading of the imprinted matrices with the MV(2+) and Zn(II)-PP-IX units and to the effective charge separation proceeding in the systems. The directional anodic/cathodic photocurrents are rationalized in terms of vectorial electron transfer processes dictated by the imprinting order and by the redox potentials of the photosensitizer/electron acceptor units associated with the imprinted sites in the two configurations. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Simple and rapid mercury ion selective electrode based on 1-undecanethiol assembled Au substrate and its recognition mechanism.

PubMed

Li, Xian-Qing; Liang, Hai-Qing; Cao, Zhong; Xiao, Qing; Xiao, Zhong-Liang; Song, Liu-Bin; Chen, Dan; Wang, Fu-Liang

2017-03-01

A simple and rapid mercury ion selective electrode based on 1-undecanethiol (1-UDT) assembled Au substrate (Au/1-UDT) has been well constructed. 1-UDT was for the purpose of generating self-assembled monolayer on gold surface to recognize Hg 2+ in aqueous solution, which had a working concentration range of 1.0×10 -8 -1.0×10 -4 molL -1 , with a Nernst response slope of 28.83±0.4mV/-pC, a detection limit of 4.5×10 -9 molL -1 , and a good selectivity over the other tested cations. Also, the Au/1-UDT possessed good reproducibility, stability, and short response time. The recovery obtained for the determination of mercury ion in practical tremella samples was in the range of 99.8-103.4%. Combined electrochemical analysis and X-ray photoelectron spectroscopy (XPS) with quantum chemical computation, the probable recognition mechanism of the electrode for selective recognition of Hg 2+ has been investigated. The covalent bond formed between mercury and sulfur is stronger than the one between gold and sulfur and thus prevents the adsorption of 1-UDT molecules on the gold surface. The quantum chemical computation with density functional theory further demonstrates that the strong interaction between the mercury atom and the sulfur atom on the gold surface leads to the gold sulfur bond ruptured and the gold mercury metallophilic interaction. Copyright © 2016 Elsevier B.V. All rights reserved.

A biosensor for cholesterol based on gold nanoparticles-catalyzed luminol electrogenerated chemiluminescence.

PubMed

Zhang, Meihe; Yuan, Ruo; Chai, Yaqin; Chen, Shihong; Zhong, Huaan; Wang, Cun; Cheng, Yinfeng

2012-02-15

A novel cholesterol biosensor was prepared based on gold nanoparticles-catalyzed luminol electrogenerated chemiluminescence (ECL). Firstly, l-cysteine-reduced graphene oxide composites were modified on the surface of a glassy carbon electrode. Then, gold nanoparticles (AuNPs) were self-assembled on it. Subsequently, cholesterol oxidase (ChOx) was adsorbed on the surface of AuNPs to construct a cholesterol biosensor. The stepwise fabrication processes were characterized with cyclic voltammetry and atomic force microscopy. The ECL behaviors of the biosensor were also investigated. It was found that AuNPs not only provided larger surface area for higher ChOx loading but also formed the nano-structured interface on the electrode surface to improve the analytical performance of the ECL biosensor for cholesterol. Besides, based on the efficient catalytic ability of AuNPs to luminol ECL, the response of the biosensor to cholesterol was linear range from 3.3 μM to 1.0 mM with a detection limit of 1.1 μM (S/N=3). In addition, the prepared ECL biosensor exhibited satisfying reproducibility, stability and selectivity. Taking into account the advantages of ECL, we confidently expect that ECL would have potential applications in biotechnology and clinical diagnosis. Copyright © 2011 Elsevier B.V. All rights reserved.

Temperature effects on the atomic structure and kinetics in single crystal electrochemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gründer, Yvonne; Markovic, Nenad M.; Thompson, Paul

2015-01-01

The influence of temperature on the atomic structure at the electrochemical interface has been studied using in-situ surface x-ray scattering (SXS) during the formation of metal monolayers on a Au(111) electrode. For the surface reconstruction of Au(111), higher temperatures increase the mobility of surface atoms in the unreconstructed phase which then determines the surface ordering during the formation of the reconstruction. For the underpotential deposition (UPD) systems, the surface diffusion of the depositing metal adatoms is significantly reduced at low temperatures which results in the frustration of ordered structures in the case of Cu UPD, occurring on a Br-modified surface,more » and in the formation of a disordered Ag monolayer during Ag UPD. The results indicate that temperature changes affect the mass transport and diffusion of metal adatoms on the electrode surface. This demonstrates the importance of including temperature as a variable in studying surface structure and reactions at the electrochemical interface.« less

Electrochemical and PM-IRRAS Studies of the Effect of Cholesterol on the Structure of a DMPC Bilayer Supported at an Au (111) Electrode Surface, Part 1: Properties of the Acyl Chains

PubMed Central

Bin, Xiaomin; Horswell, Sarah L.; Lipkowski, Jacek

2005-01-01

Charge density measurements and polarization modulation infrared reflection absorption spectroscopy were employed to investigate the spreading of small unilamellar vesicles of a dimyristoylphosphatidylcholine (DMPC)/cholesterol (7:3 molar ratio) mixture onto an Au (111) electrode surface. The electrochemical experiments demonstrated that vesicles fuse and spread onto the Au (111) electrode surface, forming a bilayer, at rational potentials −0.4 V < (E − Epzc) < 0.4 V or field strength <6×107 V m−1. Polarization modulation infrared reflection absorption spectroscopy experiments provided information concerning the conformation and orientation of the acyl chains of DMPC molecules. Deuterated DMPC was used to subtract the contribution of C-H stretching bands of cholesterol and of the polar head region of DMPC from spectra in the C-H stretching region. The absorption spectra of the C-H stretch bands in the acyl chains were determined in this way. The properties of the DMPC/cholesterol bilayer have been compared with the properties of a pure DMPC bilayer. The presence of 30% cholesterol gives a thicker and more fluid bilayer characterized by a lower capacity and lower tilt angle of the acyl chains. PMID:15849259

Hg(2+) detection using a disposable and miniaturized screen-printed electrode modified with nanocomposite carbon black and gold nanoparticles.

PubMed

Cinti, Stefano; Santella, Francesco; Moscone, Danila; Arduini, Fabiana

2016-05-01

A miniaturized screen-printed electrode (SPE) modified with a carbon black-gold nanoparticle (CBNP-AuNP) nanocomposite has been developed as an electrochemical sensor for the detection of inorganic mercury ions (Hg(2+)). The working electrode surface has been modified with nanocomposite constituted of CBNPs and AuNPs by an easy drop casting procedure that makes this approach extendible to an automatable mass production of modified SPEs. Square wave anodic stripping voltammetry (SWASV) was adopted to perform Hg(2+) detection, revealing satisfactory sensitivity and detection limit, equal to 14 μA ppb(-1) cm(-2) and 3 ppb, respectively. The applicability of the CBNP-AuNP-SPE for the determination of inorganic mercury has been assessed in river water by a simple filtration and acidification of the sample as well as in soil by means of a facile acidic extraction procedure assisted by ultrasound.

Nonenzymatic Wearable Sensor for Electrochemical Analysis of Perspiration Glucose.

PubMed

Zhu, Xiaofei; Ju, Yinhui; Chen, Jian; Liu, Deye; Liu, Hong

2018-05-25

We report a nonenzymatic wearable sensor for electrochemical analysis of perspiration glucose. Multipotential steps are applied on a Au electrode, including a high negative pretreatment potential step for proton reduction which produces a localized alkaline condition, a moderate potential step for electrocatalytic oxidation of glucose under the alkaline condition, and a positive potential step to clean and reactivate the electrode surface for the next detection. Fluorocarbon-based materials were coated on the Au electrode for improving the selectivity and robustness of the sensor. A fully integrated wristband is developed for continuous real-time monitoring of perspiration glucose during physical activities, and uploading the test result to a smartphone app via Bluetooth.

Polyelectrolyte Multilayer-Treated Electrodes for Real-Time Electronic Sensing of Cell Proliferation

PubMed Central

Mijares, Geraldine I.; Reyes, Darwin R.; Geist, Jon; Gaitan, Michael; Polk, Brian J.; DeVoe, Don L.

2010-01-01

We report on the use of polyelectrolyte multilayer (PEM) coatings as a non-biological surface preparation to facilitate uniform cell attachment and growth on patterned thin-film gold (Au) electrodes on glass for impedance-based measurements. Extracellular matrix (ECM) proteins are commonly utilized as cell adhesion promoters for electrodes; however, they exhibit degradation over time, thereby imposing limitations on the duration of conductance-based biosensor experiments. The motivation for the use of PEM coatings arises from their long-term surface stability as promoters for cell attachment, patterning, and culture. In this work, a cell proliferation monitoring device was fabricated. It consisted of thin-film Au electrodes deposited with a titanium-tungsten (TiW) adhesion layer that were patterned on a glass substrate and passivated to create active electrode areas. The electrode surfaces were then treated with a poly(ethyleneimine) (PEI) anchoring layer and subsequent bilayers of sodium poly(styrene sulfonate) (PSS) and poly(allylamine hydrochloride) (PAH). NIH-3T3 mouse embryonic fibroblast cells were cultured on the device, observed by optical microscopy, and showed uniform growth characteristics similar to those observed on a traditional polystyrene cell culture dish. The optical observations were correlated to electrical measurements on the PEM-treated electrodes, which exhibited a rise in impedance with cell proliferation and stabilized to an approximate 15 % increase as the culture approached confluency. In conclusion, cells proliferate uniformly over gold and glass PEM-treated surfaces, making them useful for continuous impedance-based, real-time monitoring of cell proliferation and for the determination of cell growth rate in cellular assays. PMID:27134780

Required Equipment for Photo-Switchable Donor-Acceptor (D-A) Dyad Interfacial Self-Assembled Monolayers for Organic Photovoltaic Cells

DTIC Science & Technology

2014-01-24

Interfacial Tuning via Electron-Blocking/Hole-Transport Layers and Indium Tin Oxide Surface Treatment in Bulk- Heterojunction Organic Photovoltaic Cells...devices Figure 3 shows the compounds we prepared to assemble on gold (Au) surfaces. Results of TPA-C60 dyads (1 and 2) self-assembled on Au electrodes...surface hydroxyl groups, respectively, we decided to prepare compounds 5-7 to attach as SAMs, see Figure 5. Difficulties and unexpected problems

Development of amperometric lysine biosensors based on Au nanoparticles/multiwalled carbon nanotubes/polymers modified Au electrodes.

PubMed

Chauhan, Nidhi; Singh, Anamika; Narang, Jagriti; Dahiya, Swati; Pundir, C S

2012-11-07

The construction of two amperometric l-lysine biosensors is described in this study. The construction comprises the covalent immobilization of lysine oxidase (LOx) onto nanocomposite composed of gold nanoparticles (AuNPs) and carboxylated multiwalled carbon nanotubes (c-MWCNT), decorated on (i) polyaniline (PANI) and (ii) poly 1,2 diaminobenzene (DAB), electrodeposited on Au electrodes. The biosensors were characterized by scanning electron microscopy (SEM), Fourier transform infrared (FTIR) and electrochemical impedance spectroscopy (EIS) studies. The optimum response (current) was observed within 2 s at pH 7.0 and 25 °C for LOx/AuNPs/c-MWCNT/PANI/Au, and 4 s at pH 7.0 and 30 °C for LOx/AuNPs/c-MWCNT/DAB/Au electrodes. There was a linear relationship between current and lysine concentration ranging from 5.0 to 600 μM for LOx/AuNPs/c-MWCNT/PANI/Au with a detection limit of 5.0 μM, and 20 to 600 μM for the LOx/AuNPs/c-MWCNT/DAB/Au electrode with a detection limit of 20 μM. The PANI modified electrode was in good agreement with the standard HPLC method, with a better correlation (r = 0.992) compared to the DAB modified electrode (r = 0.986). These observations revealed that the PANI modified Au electrode was better than the DAB modified electrode, and hence it was employed for the determination of lysine in milk, pharmaceutical tablets and sera. The PANI modified electrode showed a half life of 120 days, compared to that of 90 days for the DAB modified electrode, after their 100 uses, when stored at 4 °C.

Nanoporous-Gold-Based Electrode Morphology Libraries for Investigating Structure-Property Relationships in Nucleic Acid Based Electrochemical Biosensors.

PubMed

Matharu, Zimple; Daggumati, Pallavi; Wang, Ling; Dorofeeva, Tatiana S; Li, Zidong; Seker, Erkin

2017-04-19

Nanoporous gold (np-Au) electrode coatings significantly enhance the performance of electrochemical nucleic acid biosensors because of their three-dimensional nanoscale network, high electrical conductivity, facile surface functionalization, and biocompatibility. Contrary to planar electrodes, the np-Au electrodes also exhibit sensitive detection in the presence of common biofouling media due to their porous structure. However, the pore size of the nanomatrix plays a critical role in dictating the extent of biomolecular capture and transport. Small pores perform better in the case of target detection in complex samples by filtering out the large nonspecific proteins. On the other hand, larger pores increase the accessibility of target nucleic acids in the nanoporous structure, enhancing the detection limits of the sensor at the expense of more interference from biofouling molecules. Here, we report a microfabricated np-Au multiple electrode array that displays a range of electrode morphologies on the same chip for identifying feature sizes that reduce the nonspecific adsorption of proteins but facilitate the permeation of target DNA molecules into the pores. We demonstrate the utility of the electrode morphology library in studying DNA functionalization and target detection in complex biological media with a special emphasis on revealing ranges of electrode morphologies that mutually enhance the limit of detection and biofouling resilience. We expect this technique to assist in the development of high-performance biosensors for point-of-care diagnostics and facilitate studies on the electrode structure-property relationships in potential applications ranging from neural electrodes to catalysts.

Amplified biosensing using the horseradish peroxidase-mimicking DNAzyme as an electrocatalyst.

PubMed

Pelossof, Gilad; Tel-Vered, Ran; Elbaz, Johann; Willner, Itamar

2010-06-01

The hemin/G-quadruplex horseradish peroxidase-mimicking DNAzyme is assembled on Au electrodes. It reveals bioelectrocatalytic properties and electrocatalyzes the reduction of H(2)O(2). The bioelectrocatalytic functions of the hemin/G-quadruplex DNAzyme are used to develop electrochemical sensors that follow the activity of glucose oxidase and biosensors for the detection of DNA or low-molecular-weight substrates (adenosine monophosphate, AMP). Hairpin nucleic structures that include the G-quadruplex sequence in a caged configuration and the nucleic acid sequence complementary to the analyte DNA, or the aptamer sequence for AMP, are immobilized on Au-electrode surfaces. In the presence of the DNA analyte, or AMP, the hairpin structures are opened, and the hemin/G-quadruplex horseradish peroxidase-mimicking DNAzyme structures are generated on the electrode surfaces. The bioelectrocatalytic cathodic currents generated by the functionalized electrodes, upon the electrochemical reduction of H(2)O(2), provide a quantitative measure for the detection of the target analytes. The DNA target was analyzed with a detection limit of 1 x 10(-12) M, while the detection limit for analyzing AMP was 1 x 10(-6) M. Methods to regenerate the sensing surfaces are presented.

RGO/Au NPs/N-doped CNTs supported on nickel foam as an anode for enzymatic biofuel cells.

PubMed

Zhang, He; Zhang, Lingling; Han, Yujie; Yu, You; Xu, Miao; Zhang, Xueping; Huang, Liang; Dong, Shaojun

2017-11-15

In this study, three-dimensional reduced graphene oxide/Au NPs/nitrogen-doped carbon nanotubes (RGO/Au NPs/N-doped CNTs) assembly supported on nickel foam was utilized as an anode for enzymatic biofuel cells (EBFCs). 3D RGO/Au NPs was obtained by electrodepositing reduced graphene oxide on nickel foam (Ni foam), while Au NPs were co-deposited during the process. Afterwards, nitrogen doped CNTs (N-CNTs) were allowed to grow seamlessly on the surfaces of 3D RGO/Au NPs via a simple chemical vapor deposition (CVD) process. In this nanostructure, Au NPs co-deposition and nitrogen doping offer more active sites for bioelectrocatalysis. Additionally, N-CNTs were demonstrated providing high specific surface area for enzyme immobilization and facilitating the electron transfer between glucose oxidase (GOx) and electrode. The resulting bioanode achieved efficient glucose oxidation with high current densities of 7.02mAcm -2 (0.3V vs. Ag/AgCl). Coupling with a Pt cathode, the fabricated glucose/air biofuel cell exhibited an open-circuit potential of 0.32V and generated a maximum power density 235µWcm -2 at 0.15V. This novel electrode substrate achieved high performance in current density at bioelectrochemical systems and could be useful for further exploiting the application of three dimensional carbon-based nanomaterials in EBFCs. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrasensitive Determination of Piroxicam at Diflunisal-Derived Gold Nanoparticle-Modified Glassy Carbon Electrode

NASA Astrophysics Data System (ADS)

Shaikh, Tayyaba; uddin, SiraJ; Talpur, Farah N.; Khaskeli, Abdul R.; Agheem, Muhammad H.; Shah, Muhammad R.; Sherazi, Tufail H.; Siddiqui, Samia

2017-10-01

We present a simple and green approach for synthesis of gold nanoparticles (AuNps) using analgesic drug diflunisal (DF) as capping and stabilizing agent in aqueous solution. Characterization of the synthesized diflunisal-derived gold nanoparticles (DF-AuNps) was performed by ultraviolet-visible (UV-Vis) spectroscopy, revealing the surface plasmon absorption band at 520 nm under optimized experimental conditions. Fourier-transform infrared (FTIR) spectroscopy established the effective interaction of the capping agent with the AuNps. Topographical features of the synthesized DF-AuNps were assessed by atomic force microscopy (AFM), revealing average particle height of 29 nm to 32 nm. X-ray diffractometry was used to study the crystalline nature, revealing that the synthesized DF-AuNps possessed excellent crystalline properties. The synthesized DF-AuNps were employed to modify the surface of glassy carbon electrode (GCE) for selective determination of piroxicam (PX) using differential pulse voltammetry technique. The fabricated Nafion/DF-AuNps/GCE sensor exhibited high sensitivity compared with bare GCE. The current response of the fabricated sensor was found to be linear in the PX concentration range of 0.5 μM to 50 μM, with limit of detection (LOD) and limit of quantification (LOQ) of 50 nM and 150 nM, respectively. The proposed sensor was successfully utilized for sensitive and rapid determination of PX in human serum, urine, and pharmaceutical samples.

The Enhanced Photo-Electrochemical Detection of Uric Acid on Au Nanoparticles Modified Glassy Carbon Electrode

NASA Astrophysics Data System (ADS)

Shi, Yuting; Wang, Jin; Li, Shumin; Yan, Bo; Xu, Hui; Zhang, Ke; Du, Yukou

2017-07-01

In this work, a sensitive and novel method for determining uric acid (UA) has been developed, in which the glassy carbon electrode (GCE) was modified with electrodeposition Au nanoparticles and used to monitor the concentration of UA with the assistant of visible light illumination. The morphology of the Au nanoparticles deposited on GCE surface were characterized by scanning electron microscope (SEM) and the nanoparticles were found to be well-dispersed spheres with the average diameter approaching 26.1 nm. A series of cyclic voltammetry (CV) and differential pulse voltammetry (DPV) measurements have revealed that the introduction of visible light can greatly enhance both the strength and stability of response current due to the surface plasmon resonance (SPR). Specifically, the DPV showed a linear relationship between peak current and UA concentration in the range of 2.8 to 57.5 μM with the equation of I pa (μA) = 0.0121 c UA (μM) + 0.3122 ( R 2 = 0.9987). Herein, the visible light illuminated Au/GCE possesses a potential to be a sensitive electrochemical sensor in the future.

On-Chip Supercapacitor Electrode Based On Polypyrrole Deposited Into Nanoporous Au Scaffold

NASA Astrophysics Data System (ADS)

Lu, P.; Ohlckers, P.; Chen, X. Y.

2016-11-01

On-chip supercapacitors hold the potential promise for serving as the energy storage units in integrated circuit system, due to their much higher energy density in comparison with conventional dielectric capacitors, high power density and long-term cycling stability. In this study, nanoporous Au (NP-Au) film on-chip was employed as the electrode scaffold to help increase the electrolyte-accessible area for active material. Pseudo-capacitive polypyrrole (PPY) with high theoretical capacitance was deposited into the NP-Au scaffold, to construct the tailored NP-Au/PPY hybrid on-chip electrode with improved areal capacitance. Half cell test in three- electrode system revealed the improved capacitor performance of nanoporous Au supported PPY electrode, compared to the densely packed PPY nanowire film electrode on planer Au substrate (Au/PPY). The areal capacitance of 37 mF/cm2∼10 mV/s, 32 mF/cm2∼50 mV/s, 28 mF/cm2∼100 mV/s, 16 mF/cm2∼500 mV/s, were offered by NP-Au/PPY. Also, the cycling performance was enhanced via using NP-Au scaffold. The developed NP-Au/PPY on-chip electrode demonstrated herein paves a feasible pathway to employ dealloying derived porous metal as the scaffold for improving both the energy density and cycling performance for supercapacitor electrodes.

M13 Virus-Incorporated Biotemplates on Electrode Surfaces To Nucleate Metal Nanostructures by Electrodeposition.

PubMed

Manivannan, Shanmugam; Kang, Inhak; Seo, Yeji; Jin, Hyo-Eon; Lee, Seung-Wuk; Kim, Kyuwon

2017-09-27

We report a virus-incorporated biological template (biotemplate) on electrode surfaces and its use in electrochemical nucleation of metal nanocomposites as an electrocatalytic material for energy applications. The biotemplate was developed with M13 virus (M13) incorporated in a silicate sol-gel matrix as a scaffold to nucleate Au-Pt alloy nanostructures by electrodeposition, together with reduced graphene oxide (rGO). The phage when engineered with Y3E peptides could nucleate Au-Pt alloy nanostructures, which ensured adequate packing density, simultaneous stabilization of rGO, and a significantly increased electrochemically active surface area. Investigation of the electrocatalytic activity of the resulting sol-gel composite catalyst toward methanol oxidation in an alkaline medium showed that this catalyst had mass activity greater than that of the biotemplate containing wild-type M13 and that of monometallic Pt and other Au-Pt nanostructures with different compositions and supports. M13 in the nanocomposite materials provided a close contact between the Au-Pt alloy nanostructures and rGO. In addition, it facilitated the availability of an OH - -rich environment to the catalyst. As a result, efficient electron transfer and a synergistic catalytic effect of the Au and Pt in the alloy nanostructures toward methanol oxidation were observed. Our nanocomposite synthesis on the novel biotemplate and its application might be useful for developing novel clean and green energy-generating and energy-storage materials.

Sensitive electrochemical immunosensor for α-synuclein based on dual signal amplification using PAMAM dendrimer-encapsulated Au and enhanced gold nanoparticle labels.

PubMed

An, Yarui; Jiang, Xiaoli; Bi, Wenji; Chen, Hua; Jin, Litong; Zhang, Shengping; Wang, Chuangui; Zhang, Wen

2012-02-15

A novel electrochemical immunosensor for sensitive detection of α-synuclein (α-SYN), a very important neuronal protein, has been developed based on dual signal amplification strategy. Herein, G4-polyamidoamine dendrimer-encapsulated Au nanoparticles (PAMAM-Au nanocomposites) were covalently bound on the poly-o-aminobenzoic acid (poly-o-ABA), which was initially electropolymerized on the electrode surface to perform abundant carboxyl groups. The formed immunosensor platform, PAMAM-Au, was proved to provide numerous amino groups to allow highly dense immobilization of antigen, and facilitate the improvement of electrochemical responses as well. Subsequently, the enhanced gold nanoparticle labels ({HRP-Ab(2)-GNPs}) were fabricated by immobilizing horseradish peroxidase-secondary antibody (HRP-Ab(2)) on the surface of gold nanoparticles (GNPs). After an immunoassay process, the {HRP-Ab(2)-GNPs} labels were introduced onto the electrode surface, and produced an electrocatalytic response by reduction of hydrogen peroxide (H(2)O(2)) in the presence of enzymatically oxidized thionine. On the basis of the dual signal amplification of PAMAM-Au and {HRP-Ab(2)-GNPs} labels, the designed immunosensor displayed an excellent analytical performance with high sensitivity and stability. This developed strategy was successfully proved as a simple, cost-effective method, and could be easily extended to other protein analysis schemes. Copyright © 2011 Elsevier B.V. All rights reserved.

Oxygen reduction reaction (orr) on bimetallic AuPt and AuPd(1 0 0)-electrodes: Effects of the heteroatomic junction on the reaction paths

NASA Astrophysics Data System (ADS)

Schulte, E.; Belletti, G.; Arce, M.; Quaino, P.

2018-05-01

The seek for materials to enhance the oxygen reduction reaction (orr) rate is a highly relevant topic due to its implication in fuel cell devices. Herein, the orr on bimetallic electrocatalysts based on Au-M (M = Pt, Pd) has been studied computationally, by performing density functional theory calculations. Bimetallic (1 0 0) electrode surfaces with two different Au:M ratios were proposed, and two possible pathways, associative and dissociative, were considered for the orr. Changes in the electronic properties of these materials with respect to the pure metals were acknowledged to gain understanding in the overall reactivity trend. The effect of the bimetallic junction on the stability of the intermediates O2 and OOH was also evaluated by means of geometrical and energetic parameters; being the intermediates preferably adsorbed on Pt/Pd atoms, but presenting in some cases higher adsorption energies compared with bare metals. Finally, the kinetics of the Osbnd O bond breaking in O2∗ and OOH∗ adsorbed intermediates in the bimetallic materials and the influence of the Au-M junction were studied by means of the nudge elastic-band method. A barrierless process for the scission of O2∗ was found in Au-M for the higher M ratios. Surprisingly, for Au-M with lower M ratios, the barriers were much lower than for pure Au surfaces, suggesting a highly reactive surface towards the orr. The Osbnd O scission of the OOH∗ was found to be a barrierless process in Ausbnd Pt systems and nearly barrierless in all Ausbnd Pd systems, implying that the reduction ofO2 in these systems proceeds via the full reduction of O2 to H2O , avoiding H2O2 formation.

Study of the Electrocatalytic Activity of Cerium Oxide and Gold-Studded Cerium Oxide Nanoparticles Using a Sonogel-Carbon Material as Supporting Electrode: Electroanalytical Study in Apple Juice for Babies

PubMed Central

Abdelrahim, M. Yahia M.; Benjamin, Stephen R.; Cubillana-Aguilera, Laura Ma; Naranjo-Rodríguez, Ignacio; Hidalgo-Hidalgo de Cisneros, Josè L.; Delgado, Juan Josè; Palacios-Santander, Josè Ma

2013-01-01

The present work reports a study of the electrocatalytic activity of CeO2 nanoparticles and gold sononanoparticles (AuSNPs)/CeO2 nanocomposite, deposited on the surface of a Sonogel-Carbon (SNGC) matrix used as supporting electrode and the application of the sensing devices built with them to the determination of ascorbic acid (AA) used as a benchmark analyte. Cyclic voltammetry (CV) and differential pulse voltammetry (DPV) were used to investigate the electrocatalytic behavior of CeO2- and AuSNPs/CeO2-modified SNGC electrodes, utilizing different concentrations of CeO2 nanoparticles and different AuSNPs:CeO2 w/w ratios. The best detection and quantification limits, obtained for CeO2 (10.0 mg·mL−1)- and AuSNPs/CeO2 (3.25% w/w)-modified SNGC electrodes, were 1.59 × 10−6 and 5.32 × 10−6 M, and 2.93 × 10−6 and 9.77 × 10−6 M, respectively, with reproducibility values of 5.78% and 6.24%, respectively, for a linear concentration range from 1.5 μM to 4.0 mM of AA. The electrochemical devices were tested for the determination of AA in commercial apple juice for babies. The results were compared with those obtained by applying high performance liquid chromatography (HPLC) as a reference method. Recovery errors below 5% were obtained in most cases, with standard deviations lower than 3% for all the modified SNGC electrodes. Bare, CeO2- and AuSNPs/CeO2-modified SNGC electrodes were structurally characterized using scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). AuSNPs and AuSNPs/CeO2 nanocomposite were characterized by UV-vis spectroscopy and X-ray diffraction (XRD), and information about their size distribution and shape was obtained by transmission electron microscopy (TEM;. The advantages of employing CeO2 nanoparticles and AuSNPs/CeO2 nanocomposite in SNGC supporting material are also described. This research suggests that the modified electrode can be a very promising voltammetric sensor for the determination of electroactive species of interest in real samples. PMID:23584124

Study of the electrocatalytic activity of cerium oxide and gold-studded cerium oxide nanoparticles using a Sonogel-Carbon material as supporting electrode: electroanalytical study in apple juice for babies.

PubMed

Abdelrahim, M Yahia M; Benjamin, Stephen R; Cubillana-Aguilera, Laura Ma; Naranjo-Rodríguez, Ignacio; de Cisneros, José L Hidalgo-Hidalgo; Delgado, Juan José; Palacios-Santander, José Ma

2013-04-12

The present work reports a study of the electrocatalytic activity of CeO2 nanoparticles and gold sononanoparticles (AuSNPs)/CeO2 nanocomposite, deposited on the surface of a Sonogel-Carbon (SNGC) matrix used as supporting electrode and the application of the sensing devices built with them to the determination of ascorbic acid (AA) used as a benchmark analyte. Cyclic voltammetry (CV) and differential pulse voltammetry (DPV) were used to investigate the electrocatalytic behavior of CeO2- and AuSNPs/CeO2-modified SNGC electrodes, utilizing different concentrations of CeO2 nanoparticles and different AuSNPs:CeO2 w/w ratios. The best detection and quantification limits, obtained for CeO2 (10.0 mg·mL(-1))- and AuSNPs/CeO2 (3.25% w/w)-modified SNGC electrodes, were 1.59 × 10(-6) and 5.32 × 10(-6) M, and 2.93 × 10(-6) and 9.77 × 10(-6) M, respectively, with reproducibility values of 5.78% and 6.24%, respectively, for a linear concentration range from 1.5 µM to 4.0 mM of AA. The electrochemical devices were tested for the determination of AA in commercial apple juice for babies. The results were compared with those obtained by applying high performance liquid chromatography (HPLC) as a reference method. Recovery errors below 5% were obtained in most cases, with standard deviations lower than 3% for all the modified SNGC electrodes. Bare, CeO2- and AuSNPs/CeO2-modified SNGC electrodes were structurally characterized using scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDS). AuSNPs and AuSNPs/CeO2 nanocomposite were characterized by UV-vis spectroscopy and X-ray diffraction (XRD), and information about their size distribution and shape was obtained by transmission electron microscopy (TEM). The advantages of employing CeO2 nanoparticles and AuSNPs/CeO2 nanocomposite in SNGC supporting material are also described. This research suggests that the modified electrode can be a very promising voltammetric sensor for the determination of electroactive species of interest in real samples.

An ultrasensitive luminol cathodic electrochemiluminescence immunosensor based on glucose oxidase and nanocomposites: graphene-carbon nanotubes and gold-platinum alloy.

PubMed

Jiang, Xinya; Chai, Yaqin; Yuan, Ruo; Cao, Yaling; Chen, Yingfeng; Wang, Haijun; Gan, Xianxue

2013-06-14

In the present study, a novel and ultrasensitive electrochemiluminescence (ECL) immunosensor based on luminol cathodic ECL was fabricated by using Au nanoparticles and Pt nanoparticles (nano-AuPt) electrodeposited on graphene-carbon nanotubes nanocomposite as platform for the detection of carcinoembryonic antigen (CEA). For this introduced immunosensor, graphene (GR) and single wall carbon nanotubes (CNTs) dispersed in chitosan (Chi-GR-CNTs) were firstly decorated on the bare gold electrode (GE) surface. Then nano-AuPt were electrodeposited (DpAu-Pt) on the Chi-GR-CNTs modified electrode. Subsequently, glucose oxidase (GOD) was employed to block the non-specific sites of electrode surface. When glucose was present in the working buffer solution, GOD immediately catalyzed the oxidation of glucose to in situ generate hydrogen peroxide (H2O2), which could subsequently promote the oxidation of luminol with an amplified cathodic ECL signal. The proposed immunosensor was performed at low potential (-0.1 to 0.4V) and low concentration of luminol. The CEA was determined in the range of 0.1 pg mL(-1) to 40 ng mL(-1) with a limit of detection down to 0.03 pg mL(-1) (SN(-1)=3). Moreover, with excellent sensitivity, selectivity, stability and simplicity, the as-proposed luminol-based ECL immunosensor provided great potential in clinical applications. Copyright © 2013 Elsevier B.V. All rights reserved.

Plasmonic-enhanced graphene flake counter electrodes for dye-sensitized solar cells

NASA Astrophysics Data System (ADS)

Kim, Hyun-Young; Lee, Myung Woo; Song, Da Hyun; Yoon, Hyeok Jin; Suh, Jung Sang

2017-06-01

A plasmonic-enhanced graphene flake counter electrode for dye-sensitized solar cells (DSSCs) was fabricated by immobilization of gold nanoparticles (NPs) on fluorine-doped tin oxide (FTO) glass and the deposition of a thin layer of graphene flakes. The graphene flakes, fabricated using a thermal plasma jet system, were very thin and pure and had good crystallinity. Even though their average size is larger than 100 nm, they had great dispersibility in common solvents. Their relatively large size and good crystallinity resulted in good conductivity, and their good dispersibility allowed us to fabricate relatively uniform films. The efficiency of the DSSC with a graphene flake/Au NP/FTO counter electrode was as much as 9.78%, which is higher than that with a conventional Pt/FTO (9.08%) or graphene flake/FTO (8.98%) counter electrode. Using cyclic voltammograms and electrochemical impedance spectroscopy and by measuring the incident photo-conversion efficiency, we proved that by the localized surface plasmon resonance effect of the Au NPs included between the graphene flakes and FTO, the charge-transfer resistance at the electrode/electrolyte interface was decreased. Consequently, the catalytic rate for I- regeneration improved, and the energy conversion efficiency of the DSSC with a graphene flake/Au NP/FTO counter electrode improved.

Enzymatic biosensor based on entrapment of d-amino acid oxidase on gold nanofilm/MWCNTs nanocomposite modified glassy carbon electrode by sol-gel network: Analytical applications for d-alanine in human serum.

PubMed

Shoja, Yalda; Rafati, Amir Abbas; Ghodsi, Javad

2017-05-01

Sensing and determination of d-alanine is studied by using an enzymatic biosensor which was constructed on the basis of d-amino acid oxidase (DAAO) immobilization by sol-gel film onto glassy carbon electrode surface modified with nanocomposite of gold nanofilm (Au-NF) and multiwalled carbon nanotubes (MWCNTs). The Au-NF/MWCNT nanocomposite was prepared by applying the potentiostatic technique for electrodeposition of Au-NF on the MWCNT immobilized on glassy carbon electrode surface. The modified electrode is investigated by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), linear sweep voltammetry (LSV) and cyclic voltammetry(CV) techniques. The linear sweep voltammetry was used for determination of d-alanine and the results showed an excellent linear relationship between biosensor response and d-alanine concentration ranging from 0.25μM to 4.5μM with correction coefficient of 0.999 (n=20). Detection limit for the fabricated sensor was calculated about 20nM (for S/N=3) and sensitivity was about 56.1μAμM -1 cm -2 . The developed biosensor exhibited rapid and accurate response to d-alanine, a good stability (4 weeks) and an average recovery of 98.9% in human serum samples. Copyright © 2017 Elsevier Inc. All rights reserved.

Green synthesis and characterization of novel gold nanocomposites for electrochemical sensing applications.

PubMed

Tanwar, Shivani; Ho, Ja-an Annie; Magi, Emanuele

2013-12-15

Synthesis, characterization and application of Au-PANI-Calix and Au-PANI-Nap nanocomposites, is reported herein. An easy template free green synthesis is proposed and discussed for easy expediency. A variety of analytical techniques were used to characterize the nanocomposites: UV-vis spectroscopy, Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, Dynamic light scattering (DLS), X-ray diffraction (XRD), Energy-dispersive X-ray spectroscopy (EDX), and X-ray photoelectron spectroscopy (XPS) were used to characterize the nanocomposites. Surface morphology was studied by transmission electron microscopy (TEM). The nanocomposites were immobilized on screen-printed electrode and showed electroactivity in neutral pH, making them promising candidates for various analytical applications. A sensitive and selective detection of Cu(2+) was perceived on the Au-PANI-Calix modified electrode with no interference from ions K(+), Ni(2+), Co(2+), Pb(2+), Cr(3+) with a detection limit of 10nM. The copper detection is facilitated for accessible ligation with 4-sulfocalix[4]arene, so as the Cu(II)-Calix complex formed. The electrode modified with Au-PANI-Nap showed sensing application towards H2O2 with a detection limit of 1 μM. The modified electrodes were reproducible and stable for 2 months. © 2013 Elsevier B.V. All rights reserved.

Direct electron transfer of glucose oxidase and biosensing for glucose based on PDDA-capped gold nanoparticle modified graphene/multi-walled carbon nanotubes electrode.

PubMed

Yu, Yanyan; Chen, Zuanguang; He, Sijing; Zhang, Beibei; Li, Xinchun; Yao, Meicun

2014-02-15

In this work, poly (diallyldimethylammonium chloride) (PDDA)-capped gold nanoparticles (AuNPs) functionalized graphene (G)/multi-walled carbon nanotubes (MWCNTs) nanocomposites were fabricated. Based on the electrostatic attraction, the G/MWCNTs hybrid material can be decorated with AuNPs uniformly and densely. The new hierarchical nanostructure can provide a larger surface area and a more favorable microenvironment for electron transfer. The AuNPs/G/MWCNTs nanocomposite was used as a novel immobilization platform for glucose oxidase (GOD). Direct electron transfer (DET) was achieved between GOD and the electrode. Field emission scanning electron microscopy (FESEM), UV-vis spectroscopy and cyclic voltammetry (CV) were used to characterize the electrochemical biosensor. The glucose biosensor fabricated based on GOD electrode modified with AuNPs/G/MWCNTs demonstrated satisfactory analytical performance with high sensitivity (29.72mAM(-1)cm(-2)) and low limit of detection (4.8 µM). The heterogeneous electron transfer rate constant (ΚS) and the apparent Michaelis-Menten constant (Km) of GOD were calculated to be 11.18s(-1) and 2.09 mM, respectively. With satisfactory selectivity, reproducibility, and stability, the nanostructure we proposed offered an alternative for electrode fabricating and glucose biosensing. © 2013 Elsevier B.V. All rights reserved.

Degradation of bisphenol A in aqueous solution by H2O2-assisted photoelectrocatalytic oxidation.

PubMed

Xie, Yi-Bing; Li, Xiang-Zhong

2006-12-01

A series of titanium dioxide (TiO(2)/Ti) film electrodes were prepared from titanium (Ti) metal mesh by an improved anodic oxidation process and were further modified by photochemically depositing gold (Au) on the TiO(2) film surface as Au-TiO(2)/Ti film electrodes. The morphological characteristics, crystal structure and photoelectroreactivity of both the TiO(2)/Ti and Au-TiO(2)/Ti electrodes were studied. The experiments confirmed that the gold modification of TiO(2) film could enhance the efficiency of e(-)/h(+) separation on the TiO(2) conduction band and resulted in the higher photocatalytic (PC) and photoelectrocatalytic (PEC) activity under UV or visible illumination. To further enhance the TiO(2) PEC reaction, a reticulated vitreous carbon (RVC) electrode was applied in the same reaction system as the cathode to electrically generate H(2)O(2) in the aqueous solution. The experiments demonstrated that such a H(2)O(2)-assisted TiO(2) PEC reaction system could achieve a much better performance of BPA degradation in aqueous solution due to an interactive effect among TiO(2), Au, and H(2)O(2). It may have good potential for application in water and wastewater treatment in the future.

Direct electrochemistry and intramolecular electron transfer of ascorbate oxidase confined on L-cysteine self-assembled gold electrode.

PubMed

Patil, Bhushan; Kobayashi, Yoshiki; Fujikawa, Shigenori; Okajima, Takeyoshi; Mao, Lanqun; Ohsaka, Takeo

2014-02-01

A direct electrochemistry and intramolecular electron transfer of multicopper oxidases are of a great importance for the fabrication of these enzyme-based bioelectrochemical-devices. Ascorbate oxidase from Acremonium sp. (ASOM) has been successfully immobilized via a chemisorptive interaction on the l-cysteine self-assembled monolayer modified gold electrode (cys-SAM/AuE). Thermodynamics and kinetics of adsorption of ASOM on the cys-SAM/AuE were studied using cyclic voltammetry. A well-defined redox wave centered at 166±3mV (vs. Ag│AgCl│KCl(sat.)) was observed in 5.0mM phosphate buffer solution (pH7.0) at the fabricated ASOM electrode, abbreviated as ASOM/cys-SAM/AuE, confirming a direct electrochemistry, i.e., a direct electron transfer (DET) between ASOM and cys-SAM/AuE. The direct electrochemistry of ASOM was further confirmed by taking into account the chemical oxidation of ascorbic acid (AA) by O2 via an intramolecular electron transfer in the ASOM as well as the electrocatalytic oxidation of AA at the ASOM/cys-SAM/AuE. Thermodynamics and kinetics of the adsorption of ASOM on the cys-SAM/AuE have been elaborated along with its direct electron transfer at the modified electrodes on the basis of its intramolecular electron transfer and electrocatalytic activity towards ascorbic acid oxidation and O2 reduction. ASOM saturated surface area was obtained as 2.41×10(-11)molcm(-2) with the apparent adsorption coefficient of 1.63×10(6)Lmol(-1). The ASOM confined on the cys-SAM/AuE possesses its essential enzymatic function. © 2013.

Influence of Adsorbed Hydroxyl and Carbon Monoxide on Potential-Induced Reconstruction of Au(100) as Examined by Scanning Tunneling Microscopy

DTIC Science & Technology

1994-02-01

years have witnessed substantial advances in our knowledge of metal reconstruction in electrochemical systems, primarily for low-index gold surfaces in...index gold surfaces, reconstruction can be formed or removed by applying electrode potentials corresponding to negative or positive electronic charge...potential and gold oxidation regions, for Au(100) in 0.1 M KOH, obtained in a conventional electrochemical cell (solid trace). The voltammetric

Layer-by-Layer Self-Assembling Gold Nanorods and Glucose Oxidase onto Carbon Nanotubes Functionalized Sol-Gel Matrix for an Amperometric Glucose Biosensor.

PubMed

Wu, Baoyan; Hou, Shihua; Miao, Zhiying; Zhang, Cong; Ji, Yanhong

2015-09-18

A novel amperometric glucose biosensor was fabricated by layer-by-layer self-assembly of gold nanorods (AuNRs) and glucose oxidase (GOD) onto single-walled carbon nanotubes (SWCNTs)-functionalized three-dimensional sol-gel matrix. A thiolated aqueous silica sol containing SWCNTs was first assembled on the surface of a cleaned Au electrode, and then the alternate self-assembly of AuNRs and GOD were repeated to assemble multilayer films of AuNRs-GOD onto SWCNTs-functionalized silica gel for optimizing the biosensor. Among the resulting glucose biosensors, the four layers of AuNRs-GOD-modified electrode showed the best performance. The sol-SWCNTs-(AuNRs- GOD)₄/Au biosensor exhibited a good linear range of 0.01-8 mM glucose, high sensitivity of 1.08 μA/mM, and fast amperometric response within 4 s. The good performance of the proposed glucose biosensor could be mainly attributed to the advantages of the three-dimensional sol-gel matrix and stereo self-assembly films, and the natural features of one-dimensional nanostructure SWCNTs and AuNRs. This study may provide a new facile way to fabricate the enzyme-based biosensor with high performance.

Construction and direct electrochemistry of orientation controlled laccase electrode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Ying; Zhang, Jiwei; Huang, Xirong, E-mail: xrhuang@sdu.edu.cn

2014-03-28

Highlights: • A recombinant laccase with Cys-6×His tag at the N or C terminus was generated. • Orientation controlled laccase electrodes were constructed via self assembly. • The electrochemical behavior of laccase electrodes was orientation dependent. • The C terminus tagged laccase was better for bioelectrocatalytic reduction of O{sub 2}. - Abstract: A laccase has multiple redox centres. Chemisorption of laccases on a gold electrode through a polypeptide tag introduced at the protein surface provides an isotropic orientation of laccases on the Au surface, which allows the orientation dependent study of the direct electrochemistry of laccase. In this paper, usingmore » genetic engineering technology, two forms of recombinant laccase which has Cys-6×His tag at the N or C terminus were generated. Via the Au-S linkage, the recombinant laccase was assembled orientationally on gold electrode. A direct electron transfer and a bioelectrocatalytic activity toward oxygen reduction were observed on the two orientation controlled laccase electrodes, but their electrochemical behaviors were found to be quite different. The orientation of laccase on the gold electrode affects both the electron transfer pathway and the electron transfer efficiency of O{sub 2} reduction. The present study is helpful not only to the in-depth understanding of the direct electrochemistry of laccase, but also to the development of laccase-based biofuel cells.« less

Electrochemical oxidation of hydrazine and its derivatives on the surface of metal electrodes in alkaline media

NASA Astrophysics Data System (ADS)

Asazawa, Koichiro; Yamada, Koji; Tanaka, Hirohisa; Taniguchi, Masatoshi; Oguro, Keisuke

Electrochemical oxidation of hydrazine and its derivatives on the surface of various metal electrodes in alkaline media was investigated. A comparison of various polycrystalline metal electrodes (Ni, Co, Fe, Cu, Ag, Au, and Pt) showed that Co and Ni electrodes have a lower onset potential for hydrazine oxidation than the Pt electrode. The onset oxidation potential of APA (aminopolyacrylamide), a hydrazine derivative (-0.127 V vs. reversible hydrogen electrode, RHE), was similar to that of hydrazine hydrate (-0.178 V vs. RHE) in the case of the Co electrode. APA oxidation was possible because of hydrazine desorption that was caused by APA hydrolysis. The hydrolysis reaction was brought about by a heat treatment. This result suggests that the hydrazine hydrolysis reaction of hydrazine derivatives makes it possible to store hydrazine hydrate safely.

Inhibited proton transfer enhances Au-catalyzed CO2-to-fuels selectivity.

PubMed

Wuttig, Anna; Yaguchi, Momo; Motobayashi, Kenta; Osawa, Masatoshi; Surendranath, Yogesh

2016-08-09

CO2 reduction in aqueous electrolytes suffers efficiency losses because of the simultaneous reduction of water to H2 We combine in situ surface-enhanced IR absorption spectroscopy (SEIRAS) and electrochemical kinetic studies to probe the mechanistic basis for kinetic bifurcation between H2 and CO production on polycrystalline Au electrodes. Under the conditions of CO2 reduction catalysis, electrogenerated CO species are irreversibly bound to Au in a bridging mode at a surface coverage of ∼0.2 and act as kinetically inert spectators. Electrokinetic data are consistent with a mechanism of CO production involving rate-limiting, single-electron transfer to CO2 with concomitant adsorption to surface active sites followed by rapid one-electron, two-proton transfer and CO liberation from the surface. In contrast, the data suggest an H2 evolution mechanism involving rate-limiting, single-electron transfer coupled with proton transfer from bicarbonate, hydronium, and/or carbonic acid to form adsorbed H species followed by rapid one-electron, one-proton, or H recombination reactions. The disparate proton coupling requirements for CO and H2 production establish a mechanistic basis for reaction selectivity in electrocatalytic fuel formation, and the high population of spectator CO species highlights the complex heterogeneity of electrode surfaces under conditions of fuel-forming electrocatalysis.

High performance capacitive deionization using modified ZIF-8-derived, N-doped porous carbon with improved conductivity.

PubMed

Li, Yang; Kim, Jeonghun; Wang, Jie; Liu, Nei-Ling; Bando, Yoshio; Alshehri, Abdulmohsen Ali; Yamauchi, Yusuke; Hou, Chia-Hung; Wu, Kevin C-W

2018-06-05

Zeolitic imidazolate framework (ZIF) composite-derived carbon exhibiting large surface area and high micropore volume is demonstrated to be a promising electrode material for the capacitive deionization (CDI) application. However, some inherent serious issues (e.g., low electrical conductivity, narrow pore size, relatively low pore volume, etc.) are still observed for nitrogen-doped porous carbon particles, which restrict their CDI performance. To solve the above-mentioned problems, herein, we prepared gold-nanoparticle-embedded ZIF-8-derived nitrogen-doped carbon calcined at 800 °C (Au@NC800) and PEDOT doped-NC-800 (NC800-PEDOT). The newly generated NC800-PEDOT and Au@NC800 electrodes exhibited notably increased conductivity, and they also achieved high electrosorption capacities of 16.18 mg g-1 and 14.31 mg g-1, respectively, which were much higher than that of NC800 (8.36 mg g-1). Au@NC800 and NC800-PEDOT can be promisingly applicable as highly efficient CDI electrode materials.

In vitro biocompatibility and electrical stability of thick-film platinum/gold alloy electrodes printed on alumina

NASA Astrophysics Data System (ADS)

Carnicer-Lombarte, Alejandro; Lancashire, Henry T.; Vanhoestenberghe, Anne

2017-06-01

Objective. High-density electrode arrays are a powerful tool in both clinical neuroscience and basic research. However, current manufacturing techniques require the use of specialised techniques and equipment, which are available to few labs. We have developed a high-density electrode array with customisable design, manufactured using simple printing techniques and with commercially available materials. Approach. Electrode arrays were manufactured by thick-film printing a platinum-gold alloy (Pt/Au) and an insulating dielectric on 96% alumina ceramic plates. Arrays were conditioned in serum and serum-free conditions, with and without 1 kHz, 200 µA, charge balanced stimulation for up to 21 d. Array biocompatibility was assessed using an extract assay and a PC-12 cell contact assay. Electrode impedance, charge storage capacity and charge injection capacity were before and after array conditioning. Main results. The manufactured Pt/Au electrodes have a highly porous surface and exhibit electrical properties comparable to arrays manufactured using alternative techniques. Materials used in array manufacture were found to be non-toxic to L929 fibroblasts by extract assay, and neuronal-like PC-12 cells adhered and extended neurites on the array surfaces. Arrays remained functional after long-term delivery of electrical pulses while exposed to protein-rich environments. Charge storage capacities and charge injection capacities increased following stimulation accounted for by an increase in surface index (real surface area) observed by vertical scanning interferometry. Further, we observed accumulation of proteins at the electrode sites following conditioning in the presence of serum. Significance. This study demonstrates the in vitro biocompatibility of commercially available thick-film printing materials. The printing technique is both simple and versatile, with layouts readily modified to produce customized electrode arrays. Thick-film electrode arrays are an attractive tool that may be implemented for general tissue engineering and neuroscience research.

Direct patterning of gold nanoparticles using flexographic printing for biosensing applications

NASA Astrophysics Data System (ADS)

Benson, Jamie; Fung, Chung Man; Lloyd, Jonathan Stephen; Deganello, Davide; Smith, Nathan Andrew; Teng, Kar Seng

2015-03-01

In this paper, we have presented the use of flexographic printing techniques in the selective patterning of gold nanoparticles (AuNPs) onto a substrate. Highly uniform coverage of AuNPs was selectively patterned on the substrate surface, which was subsequently used in the development of a glucose sensor. These AuNPs provide a biocompatible site for the attachment of enzymes and offer high sensitivity in the detection of glucose due to their large surface to volume ratio. The average size of the printed AuNPs is less than 60 nm. Glucose sensing tests were performed using printed carbon-AuNP electrodes functionalized with glucose oxidase (GOx). The results showed a high sensitivity of 5.52 μA mM-1 cm-2 with a detection limit of 26 μM. We have demonstrated the fabrication of AuNP-based biosensors using flexographic printing, which is ideal for low-cost, high-volume production of the devices.

Fabrication of a novel quartz micromachined gyroscope

NASA Astrophysics Data System (ADS)

Xie, Liqiang; Xing, Jianchun; Wang, Haoxu; Wu, Xuezhong

2015-04-01

A novel quartz micromachined gyroscope is proposed in this paper. The novel gyroscope is realized by quartz anisotropic wet etching and 3-dimensional electrodes deposition. In the quartz wet etching process, the quality of Cr/Au mask films affecting the process are studied by experiment. An excellent mask film with 100 Å Cr and 2000 Å Au is achieved by optimization of experimental parameters. Crystal facets after etching seriously affect the following sidewall electrodes deposition process and the structure's mechanical behaviours. Removal of crystal facets is successfully implemented by increasing etching time based on etching rate ratios between facets and crystal planes. In the electrodes deposition process, an aperture mask evaporation method is employed to prepare electrodes on 3-dimensional surfaces of the gyroscope structure. The alignments among the aperture masks are realized by the ABM™ Mask Aligner System. Based on the processes described above, a z-axis quartz gyroscope is fabricated successfully.

In situ STM imaging of the structures of pentacene molecules adsorbed on Au(111).

PubMed

Pong, Ifan; Yau, Shuehlin; Huang, Peng-Yi; Chen, Ming-Chou; Hu, Tarng-Shiang; Yang, Yawchia; Lee, Yuh-Lang

2009-09-01

In situ scanning tunneling microscope (STM) was used to examine the spatial structures of pentacene molecules adsorbed onto a Au(111) single-crystal electrode from a benzene dosing solution containing 16-400 microM pentacene. Molecular-resolution STM imaging conducted in 0.1 M HClO(4) revealed highly ordered pentacene structures of ( radical31 x radical31)R8.9 degrees , (3 x 10), ( radical31 x 10), and ( radical7 x 2 radical7)R19.1 degrees adsorbed on the reconstructed Au(111) electrode dosed with different pentacene solutions. These pentacene structures and the reconstructed Au(111) substrate were stable between 0.2 and 0.8 V [vs reversible hydrogen electrode, RHE]. Increasing the potential to E > 0.8 V lifted the reconstructed Au(111) surface and disrupted the ordered pentacene adlattices simultaneously. Ordered pentacene structures could be restored by applying potentials negative enough to reinforce the reconstructed Au(111). At potentials negative of 0.2 V, the adsorption of protons became increasingly important to displace adsorbed pentacene admolecules. Although the reconstructed Au(111) structure was not essential to produce ordered pentacene adlayers, it seemed to help the adsorption of pentacene molecules in a long-range ordered pattern. At room temperature (25 degrees C), approximately 100 pentacene molecules seen in STM images could rotate and align themselves to a neighboring domain in 10 s, suggesting that pentacene admolecules could be mobile on Au(111) under the STM imaging conditions of -150 mV in bias voltage and 1 nA in feedback current.

Surface studies of Li-ion and Mg battery electrodes

NASA Astrophysics Data System (ADS)

Esbenshade, Jennifer

This dissertation focuses on studies of the surfaces of both Li-ion and Mg-ion battery electrodes. A fundamental understanding of processes occurring at the electrode surface is vital to the development of advanced battery systems. Additionally, modifications to the electrode surfaces are made and further characterized for improved performance. LiMn2O4 Cathodes for Li-ion Batteries: Effect of Mn in electrolyte on anode and Au coating to minimize dissolution: LiMn2O4 (LMO) is known to dissolve Mn ions with cycling. This section focuses on both the effect of the dissolution of Mn2+ into the electrolyte as well as Au coating on the LMO to improve electrochemical performance. Electrochemical quartz crystal microbalance (EQCM) was used to monitor changes in mass on the anode, SEM and AES were used to observe changes in surface morphology and chemical composition, and potentiostatic voltammetry was used to monitor charge and discharge capacity. The effect of Cu2+ addition in place of Mn2+ was also studied, as Cu is known to form an underpotential deposition (UPD) monolayer on Au electrodes. Following this, LMO particles were coated with a Au shell by a simple and scalable electroless deposition for use as Li-ion battery cathodes. The Au shell was intended to limit the capacity fade commonly seen with LMO cathodes by reducing the dissolution of Mn. Characterization by SEM, TEM, EELS, and AFM showed that the Au shell was approximately 3 nm thick. The Au shell prevented much of the Mn from dissolving in the electrolyte with 82% and 88% less dissolved Mn in the electrolyte at room temperature and 65 ºC, respectively, as compared to the uncoated LMO. Electrochemical performance studies with half cells showed that the Au shell maintained a higher discharge capacity over 400 cycles by nearly 30% with 110 mA hr g-1 for the 400th cycle as compared to a commercial LMO at 85 mA hr g-1. Similarly, the capacity fade was reduced in full cells: the coated LMO had 47% greater capacity after 400 cycles over the control. Dimensionally Controlled Lithiation of Thin Film and Multilayer Conversion Li-ion Battery Anodes: Oxide conversion reactions are an alternative approach for high capacity Li-ion batteries, but are known to suffer from structural irreversibility associated with the phase separation and reconstitution of reduced metal species and Li2O. The morphology of the reduced metal species is thought to play a critical role in the electrochemical properties of a conversion material. In this section, a model electrode is used with alternating layers of Cr and CrOx to better understand and control these phase changes in real-time and at molecular length scales. Despite lacking crystallinity at the atomic scale, this superstructure is observed (with XR) to lithiate and delithiate in a purely one-dimensional manner, preserving the layered structure. The XR data show that the metal layers act as nucleation sites for the reduction of chromium in the conversion reaction. Irreversibility during delithiation is due to the formation of a ternary phase, LiCrO2, which can be further delithiated at higher potentials. The results reveal that the combination of confining lithiation to nanoscale sheets of Li2O and the availability of reaction sites in the metal layers in the layered structure is a strategy for improving the reversibility and mass transport properties that can be used in a wide range of conversion materials. Following the Cr/CrOx study, the next step was to study intermetallics which can electrochemically alloy to Li4.4M (M = Si, Ge, Sn, etc.), providing order-of-magnitude increases in energy density. The energy density of Si may be combined with the structural reversibility of an intercalation material using a Si/metal silicide multilayer (ML). In operando XR confirms the ML's structural reversibility during Li insertion and extraction, despite an overall 3.3-fold vertical expansion. The ML electrodes also show enhanced long-term cyclability and rate capabilities relative to a comparable Si thin film electrode. This intercalation behavior found by dimensionally constraining Si lithiation promises applicability to a range of conversion reactions. Improving Electrodeposition of Mg through an Open Circuit Potential Hold: In this section, in situ XRD, XPS, SEM and electrochemical methods were used to interrogate the mechanism of Mg electrodeposition from PhMgCl/AlCl3 (APC) and EtMgCl electrolytes. An open circuit potential (OCP) pause following Mg deposition led to retained enhancement of Mg deposition and stripping kinetics along with lowered overpotentials for both. In situ XRD demonstrated that the OCP pause led to a more polycrystalline deposits relative to that without the pause, while SEM presented micrographs that showed smaller deposits with an OCP hold. The improvement is attributed to an 'enhancement layer' that formed on the electrode during the OCP hold. Analysis of XPS data suggests that this 'enhancement layer' consists of Mg and Cl retained on the electrode surface, possibly following electrode depassivation.

Porphyran-capped gold nanoparticles modified carbon paste electrode: a simple and efficient electrochemical sensor for the sensitive determination of 5-fluorouracil

NASA Astrophysics Data System (ADS)

Lima, Dhésmon; Calaça, Giselle Nathaly; Viana, Adriano Gonçalves; Pessôa, Christiana Andrade

2018-01-01

The application of carbon paste electrodes modified with porphyran-capped gold nanoparticles (CPE/AuNps-PFR) to detect an important anticancer drug, 5-fluorouracil (5-FU), is described. Gold nanoparticles (AuNps) were synthesized through a green one-pot route, by using porphyran (PFR) (a sulfated polysaccharide extracted from red seaweed) as reducing and stabilizing agent. The reaction temperature and the concentrations of AuCl4- and PFR for AuNps-PFR synthesis were optimized by using a 23 full factorial design with central point assayed in triplicate. The smallest particle size (128.7 nm, obtained by DLS) was achieved by employing a temperature of 70 °C and AuCl4- and PFR concentrations equal to 2.5 mmol L-1 and 0.25 mg mL-1, respectively. The AuNps-PFR nanocomposite was characterized by UV-vis spectroscopy, FTIR, DLS, TEM, XRD and zeta potential, which proved that PFR was effective at reducing and capping the AuNps. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) experiments showed that the nanocomposite could enhance the electrochemical performance of the electrodes, as a consequence of the high conductivity and large surface area presented by the AuNps. The CPE/AuNps-PFR was able to electrocatalyze the oxidation of 5-FU by CV and differential pulse voltammetry (DPV). A linear relationship between the DPV peak currents and 5-FU concentration was verified in the range from 29.9 to 234 μmol L-1 in 0.04 mol L-1 BR buffer solution pH 8.0. Detection and quantification limits were found to be 0.66 and 2.22 μmol L-1, respectively. Besides the good sensitivity, CPE/AuNps-PFR showed reproducibility and did not suffer significant interference from potentially electroative biological compounds. The good analytical performance of the modified electrode was confirmed for determining 5-FU in pharmaceutical formulations, with good percent recoveries (ranging from 96.6 to 101.4%) and an acceptable relative standard deviation (RSD = 2.80%).

Detection of Quinoline in G. boninense-Infected Plants Using Functionalized Multi-Walled Carbon Nanotubes: A Field Study.

PubMed

Akanbi, Fowotade Sulayman; Yusof, Nor Azah; Abdullah, Jaafar; Sulaiman, Yusran; Hushiarian, Roozbeh

2017-07-01

Carbon nanotubes (CNTs) reinforced with gold nanoparticles (AuNPs) and chitosan nanoparticles (CTSNPs) were anchored on a screen-printed electrode to fabricate a multi-walled structure for the detection of quinoline. The surface morphology of the nanocomposites and the modified electrode was examined by an ultra-high resolution field emission scanning electron microscope (FESEM), and Fourier-transform infrared (FT-IR) spectroscopy was used to confirm the presence of specific functional groups on the multi-walled carbon nanotubes MWCNTs. Cyclic voltammetry (CV) and linear sweep voltammetry (LSV) were used to monitor the layer-by-layer assembly of ultra-thin films of nanocomposites on the surface of the electrode and other electrochemical characterizations. Under optimized conditions, the novel sensor displayed outstanding electrochemical reactivity towards the electro-oxidation of quinoline. The linear range was fixed between 0.0004 and 1.0 μM, with a limit of detection (LOD) of 3.75 nM. The fabricated electrode exhibited high stability with excellent sensitivity and selectivity, specifically attributable to the salient characteristics of AuNPs, CTSNPs, and MWCNTs and the synergistic inter-relationship between them. The newly developed electrode was tested in the field. The Ipa increased with an increase in the amount of quinoline solution added, and the peak potential deviated minimally, depicting the real capability of the newly fabricated electrode.

Detection of Quinoline in G. boninense-Infected Plants Using Functionalized Multi-Walled Carbon Nanotubes: A Field Study

PubMed Central

Akanbi, Fowotade Sulayman; Yusof, Nor Azah; Abdullah, Jaafar; Sulaiman, Yusran; Hushiarian, Roozbeh

2017-01-01

Carbon nanotubes (CNTs) reinforced with gold nanoparticles (AuNPs) and chitosan nanoparticles (CTSNPs) were anchored on a screen-printed electrode to fabricate a multi-walled structure for the detection of quinoline. The surface morphology of the nanocomposites and the modified electrode was examined by an ultra-high resolution field emission scanning electron microscope (FESEM), and Fourier-transform infrared (FT-IR) spectroscopy was used to confirm the presence of specific functional groups on the multi-walled carbon nanotubes MWCNTs. Cyclic voltammetry (CV) and linear sweep voltammetry (LSV) were used to monitor the layer-by-layer assembly of ultra-thin films of nanocomposites on the surface of the electrode and other electrochemical characterizations. Under optimized conditions, the novel sensor displayed outstanding electrochemical reactivity towards the electro-oxidation of quinoline. The linear range was fixed between 0.0004 and 1.0 μM, with a limit of detection (LOD) of 3.75 nM. The fabricated electrode exhibited high stability with excellent sensitivity and selectivity, specifically attributable to the salient characteristics of AuNPs, CTSNPs, and MWCNTs and the synergistic inter-relationship between them. The newly developed electrode was tested in the field. The Ipa increased with an increase in the amount of quinoline solution added, and the peak potential deviated minimally, depicting the real capability of the newly fabricated electrode. PMID:28671561

Layer-by-Layer Self-Assembling Gold Nanorods and Glucose Oxidase onto Carbon Nanotubes Functionalized Sol-Gel Matrix for an Amperometric Glucose Biosensor

PubMed Central

Wu, Baoyan; Hou, Shihua; Miao, Zhiying; Zhang, Cong; Ji, Yanhong

2015-01-01

A novel amperometric glucose biosensor was fabricated by layer-by-layer self-assembly of gold nanorods (AuNRs) and glucose oxidase (GOD) onto single-walled carbon nanotubes (SWCNTs)-functionalized three-dimensional sol-gel matrix. A thiolated aqueous silica sol containing SWCNTs was first assembled on the surface of a cleaned Au electrode, and then the alternate self-assembly of AuNRs and GOD were repeated to assemble multilayer films of AuNRs-GOD onto SWCNTs-functionalized silica gel for optimizing the biosensor. Among the resulting glucose biosensors, the four layers of AuNRs-GOD-modified electrode showed the best performance. The sol-SWCNTs-(AuNRs-GOD)4/Au biosensor exhibited a good linear range of 0.01–8 mM glucose, high sensitivity of 1.08 μA/mM, and fast amperometric response within 4 s. The good performance of the proposed glucose biosensor could be mainly attributed to the advantages of the three-dimensional sol-gel matrix and stereo self-assembly films, and the natural features of one-dimensional nanostructure SWCNTs and AuNRs. This study may provide a new facile way to fabricate the enzyme-based biosensor with high performance. PMID:28347080

Impedance Biosensing to detect food allergens, endocrine disrupting chemicals, and food pathogens

NASA Astrophysics Data System (ADS)

Radhakrishnan, Rajeswaran

Electrochemical impedance biosensors can be viewed as an AC electroanalytical method for the analyte detection in the fields of biomedicine, environmental monitoring, and food and agriculture, amongst others. The most common format for AC impedance biosensing involves surface immobilization of an antibody, receptor protein, DNA strand, or other species capable of bio-recognition, and AC impedance detection of the binding event. Technological application of AC impedance biosensors has been hindered by several obstacles, including the more complex circuitry required for AC relative to DC electrochemistry, chemical and physical interference arising from non-specific adsorption, and the stability and reproducibility of protein immobilization. One focus of these PhD studies is on methods to reduce or compensate for non-specific adsorption, including sample dilution, site blocking with BSA, and the use of control electrodes onto which reference antibodies are immobilized. Examples that will be presented include impedance detection of food pathogens, such as Listeria monocytogenes, using a mouse monoclonal antibody immobilized onto an Au electrode. This yields detection limits of 5 CFU/ml and 4 CFU/ml for ideal solutions and filtered tomato extract, respectively. Control experiments with an Au electrode onto which a mouse monoclonal antibody to GAPDH is immobilized demonstrate that non-specific adsorption is insignificant for the system and methodology studied here. Control experiments with Salmonella enterica demonstrate no cross-reactivity to this food pathogen. In addition, Detection of two endocrine-disrupting chemicals (EDC), norfluoxetine and BDE-47, is reported here by impedance biosensing, with a detection limit of 8.5 and 1.3 ng/ml for norfluoxetine and BDE-47, respectively. Additional research has focused on alternative substrates and linker chemistries for protein immobilization, including the use of degenerate (highly doped) Si and bidendate thiol monolayer onto Au. Advantages of degenerate Si include a simpler equivalent circuit, simple and reproducible surface preparation, easy incorporation into ULSI devices, and the greater strength of Si-C bonds (~520 kJ/mole) relative to Au-S bonds (125-150 kJ/mole). New results demonstrating antibody regeneration atop degenerate (highly doped) Si are also reported. Using 0.2 M KSCN and 10 mM HF for antibody regeneration, peanut protein Ara h 1 is detected daily during a thirty-day trial. An impedance biosensor is reported that employs the bidentate thiol 16-[3,5-bis(mercaptomethyl)phenoxy]-hexadecanoic acid (BMPHA) to immobilize the mouse monoclonal antibody to peanut protein Ara h 1. The detection limit for Ara h 1 is approximately 0.71 ng/mL (0.01 nM), which is about one order of magnitude lower than that obtained for antibody immobilization atop the monodendate thiol, 16-mercaptohexadecanoic acid (16 MHA). Antibody regeneration was studied daily using a gentle denaturing agent, 0.2 M KSCN at pH 7.3. The antibody-coated on Au electrodes retained activity towards Ara h1 for 10 and 20 days of regeneration of the monodendate- and BMPHA-coated Au electrodes, respectively. This prolonged activity illustrates the superior stability of protein films atop the BMPHA bidentate thiol- coated Au electrode relative to the 16-MHA monodendate thiol-coated Au electrode.

Polarization of gold in nanopores leads to ion current rectification

DOE PAGES

Yang, Crystal; Hinkle, Preston; Menestrina, Justin; ...

2016-10-03

Biomimetic nanopores with rectifying properties are relevant components of ionic switches, ionic circuits, and biological sensors. Rectification indicates that currents for voltages of one polarity are higher than currents for voltages of the opposite polarity. Ion current rectification requires the presence of surface charges on the pore walls, achieved either by the attachment of charged groups or in multielectrode systems by applying voltage to integrated gate electrodes. Here we present a simpler concept for introducing surface charges via polarization of a thin layer of Au present at one entrance of a silicon nitride nanopore. In an electric field applied bymore » two electrodes placed in bulk solution on both sides of the membrane, the Au layer polarizes such that excess positive charge locally concentrates at one end and negative charge concentrates at the other end. Consequently, a junction is formed between zones with enhanced anion and cation concentrations in the solution adjacent to the Au layer. This bipolar double layer together with enhanced cation concentration in a negatively charged silicon nitride nanopore leads to voltage-controlled surface-charge patterns and ion current rectification. The experimental findings are supported by numerical modeling that confirm modulation of ionic concentrations by the Au layer and ion current rectification even in low-aspect ratio nanopores. Lastly, our findings enable a new strategy for creating ionic circuits with diodes and transistors.« less

Electrochemical analysis of gold-coated magnetic nanoparticles for detecting immunological interaction

NASA Astrophysics Data System (ADS)

Pham, Thao Thi-Hien; Sim, Sang Jun

2010-01-01

An electrochemical impedance immunosensor was developed for detecting the immunological interaction between human immunoglobulin (IgG) and protein A from Staphylococcus aureus based on the immobilization of human IgG on the surface of modified gold-coated magnetic nanoparticles. The nanoparticles with an Au shell and Fe oxide cores were functionalized by a self-assembled monolayer of 11-mercaptoundecanoic acid. The electrochemical analysis was conducted on the modified magnetic carbon paste electrodes with the nanoparticles. The magnetic nanoparticles were attached to the surface of the magnetic carbon paste electrodes via magnetic force. The cyclic voltammetry technique and electrochemical impedance spectroscopy measurements of the magnetic carbon paste electrodes coated with magnetic nanoparticles-human IgG complex showed changes in its alternating current (AC) response both after the modification of the surface of the electrode and the addition of protein A. The immunological interaction between human IgG on the surface of the modified magnetic carbon paste electrodes and protein A in the solution could be successfully monitored.

Amperometric determination of total phenolic content in wine by laccase immobilized onto silver nanoparticles/zinc oxide nanoparticles modified gold electrode.

PubMed

Chawla, Sheetal; Rawal, Rachna; Kumar, Dheeraj; Pundir, Chandra Shekhar

2012-11-01

A method is described for construction of a highly sensitive amperometric biosensor for measurement of total phenolic compounds in wine by immobilizing laccase covalently onto nanocomposite of silver nanoparticles (AgNPs)/zinc oxide nanoparticles (ZnONPs) electrochemically deposited onto gold (Au) electrode. Scanning electron microscopy, X-ray diffraction, and electrochemical impedance spectroscopy were applied for characterization of the surface morphology of the modified electrode, and cyclic voltammetry was used to investigate the electrochemical properties of the proposed electrode toward the oxidation of guaiacol. The linearity between the oxidation current and the guaiacol concentration was obtained in a range of 0.1 to 500μM with a detection limit of 0.05μM (signal-to-noise ratio (S/N)=3) and sensitivity of 0.71μAμM(-1)cm(-2). The electrode showed increased oxidation and reduced reduction current with the deposition of AgNPs/ZnONPs on it. R(CT) values of ZnONPs/Au, AgNPs/ZnONPs/Au, and laccase/AgNPs/ZnONPs/Au electrode were 220, 175, and 380Ω, respectively. The biosensor showed an optimal response within 8s at pH 6.0 (0.1M acetate buffer) and 35°C when operated at 0.22V against Ag/AgCl. Analytical recovery of added guaiacol was 98%. The method showed a good correlation (r=0.99) with the standard spectrophotometric method, with the regression equation being y=1.0053x-3.5541. The biosensor lost 25% of its initial activity after 200 uses over 5months. Copyright © 2012 Elsevier Inc. All rights reserved.

I Situ Structural Study of Underpotential Deposition and Electrocatalysis on GOLD(111) Electrodes

NASA Astrophysics Data System (ADS)

Chen, Chun-Hsien

This thesis work has studied systems of Bi, Pb, Ag, and Hg underpotential deposition (UPD) on Au(111) electrodes. The application of the atomic force microscope (AFM), the scanning tunneling microscope (STM), and the surface x-ray scattering (SXS) to these UPD studies has provided in situ measurements from which we investigate factors that determine UPD surface structures and correlate these structures with surface reactivity. For all the UPD systems in this thesis work, atomic level features of the electrode surface have been revealed. In the case of Pb UPD, Pb starts to deposit by forming islands which exhibit a hexagonal close packed structure of Pb adatoms, while, in the other systems, the UPD adatoms form open lattices. In the Bi and Pb studies, we correlate the activities of the modified surface toward electroreduction of H_2O_2 with the adlattice structures. A heterobimetallic bridge model for H_2O_2 on the surface could explain the enhanced reactivity. The full monolayers of Bi and Hg, rhombohedral metals, form rectangular lattice structures on the hexagonal Au(111) surfaces. The partial charge retention on the Bi and Hg adatom opens the adlayer structure when the coverage is less than a full monolayer. The structure of the first submonolayers of Ag UPD is electrolyte-dependent. The electrode surface exhibits 3 x 3 and 4 x 4 overlayer structures in solutions containing sulfate and nitrate, respectively. In perchloric acid another open structure is observed and a close-packed monolayer is formed in acetic acid. The different monolayer structures give rise to packing densities which correlate with electrolyte size. This implies that the anions participate in reducing metal ions.

Morphology and conductivity of Au films on polydimethylsiloxane using (3-mercaptopropyl)trimethoxysilane (MPTMS) as an adhesion promoter

NASA Astrophysics Data System (ADS)

Osmani, Bekim; Deyhle, Hans; Weiss, Florian M.; Töpper, Tino; Karapetkova, Maria; Leung, Vanessa; Müller, Bert

2016-04-01

Dielectric elastomer actuators (DEA) are often referred to as artificial muscles due to their high specific continuous power, which is comparable to that of human skeletal muscles, and because of their millisecond response time. We intend to use nanometer-thin DEA as medical implant actuators and sensors to be operated at voltages as low as a few tens of volts. The conductivity of the electrode and the impact of its stiffness on the stacked structure are key to the design and operation of future devices. The stiffness of sputtered Au electrodes on polydimethylsiloxane (PDMS) was characterized using AFM nanoindentation techniques. 2500 nanoindentations were performed on 10 x 10 μm2 regions at loads of 100 to 400 nN using a spherical tip with a radius of (522 +/- 2) nm. Stiffness maps based on the Hertz model were calculated using the Nanosurf Flex-ANA system. The low adhesion of Au to PDMS has been reported in the literature and leads to the formation of Au-nanoclusters. The size of the nanoclusters was (25 +/- 10) nm and can be explained by the low surface energy of PDMS leading to a Volmer-Weber growth mode. Therefore, we propose (3-mercaptopropyl)trimethoxysilane (MPTMS) as a molecular adhesive to promote the adhesion between the PDMS and Au electrode. A beneficial side effect of these self-assembling monolayers is the significant improvement of the electrode's conductivity as determined by four-point probe measurements. Therefore, the application of a soft adhesive layer for building a dielectric elastomer actuator appears promising.

Ternary Au/ZnO/rGO nanocomposites electrodes for high performance electrochemical storage devices

NASA Astrophysics Data System (ADS)

Chaudhary, Manchal; Doong, Ruey-an; Kumar, Nagesh; Tseng, Tseung Yuen

2017-10-01

The combination of metal and metal oxide nanoparticles with reduced graphene oxides (rGO) is an active electrode material for electrochemical storage devices. Herein, we have, for the first time, reported the fabrication of ternary Au/ZnO/rGO nanocomposites by using a rapid and environmentally friendly microwave-assisted hydrothermal method for high performance supercapacitor applications. The ZnO/rGO provides excellent electrical conductivity and good macro/mesopore structures, which can facilitate the rapid electrons and ions transport. The Au nanoparticles with particle sizes of 7-12 nm are homogeneously distributed onto the ZnO/rGO surface to enhance the electrochemical performance by retaining the capacitance at high current density. The Au/ZnO/rGO nanocomposites, prepared with the optimized rGO amount of 100 mg exhibit a high specific capacitance of 875 and 424 F g-1 at current densities of 1 and 20 A g-1, respectively, in 2 M KOH. In addition, the energy and power densities of ternary Au/ZnO/rGO can be up to 17.6-36.5 Wh kg-1 and 0.27-5.42 kW kg-1, respectively. Results obtained in this study clearly demonstrate the excellence of ternary Au/ZnO/rGO nanocomposites as the active electrode materials for electrochemical pseudocapacitor performance and can open an avenue to fabricate metal/metal oxide/rGO nanocomposites for electrochemical storage devices with both high energy and power densities.

Immobilization of myoglobin on Au nanoparticle-decorated carbon nanotube/polytyramine composite as a mediator-free H2O2 and nitrite biosensor

PubMed Central

Vilian, A. T. Ezhil; Veeramani, Vediyappan; Chen, Shen-Ming; Madhu, Rajesh; Kwak, Cheol Hwan; Huh, Yun Suk; Han, Young-Kyu

2015-01-01

A novel composite film was designed for use as a highly selective mediator-free amperometric biosensor, and a method was created for accomplishing direct electrochemistry of myoglobin on a multi-walled carbon nanotube and tyramine-modified composite decorated with Au nanoparticles on a glassy carbon electrode. The ultraviolet-visible and electrochemical impedance spectroscopy results showed that myoglobin retained its native conformation in the interaction with Au-PTy-f-MWCNT. The surface coverage of Mb-heme-Fe(II)/(III) immobilized on Au-PTy-f-MWCNT and the heterogeneous electron-transfer rate constant were 2.12 × 10−9 mol cm−2 and 4.86 s−1, respectively, indicating a higher loading capacity of the nanocomposite for direct electron transfer of Mb onto the electrode surface. The proposed Mb/Au-PTy-f-MWCNT biofilm exhibited excellent electrocatalytic behavior toward the reduction of H2O2 and the oxidation of nitrite with linear ranges of 2 to 5000 μM and 1 to 8000 μM and lower detection limits of 0.01 μM and 0.002 μM, respectively. An apparent Michaelis-Menten constant of 0.12 mM indicated that the Mb immobilized on the Au-PTy-f-MWCNT film retained its native activity. This biosensor can be successfully applied to detect H2O2 and nitrite in disinfectant cream, eye drops, pickle juice, and milk samples. PMID:26672985

Gold nanoparticles modified electrode via simple electrografting of in situ generated mercaptophenyl diazonium cations for development of DNA electrochemical biosensor.

PubMed

Li, Feng; Feng, Yan; Dong, Pingjun; Yang, Limin; Tang, Bo

2011-01-15

A novel protocol for development of DNA electrochemical biosensor based on gold nanoparticles (AuNPs) modified glassy carbon electrode (GCE) was proposed, which was carried out by the self-assembly of AuNPs on the mercaptophenyl film (MPF) via simple electrografting of in situ generated mercaptophenyl diazonium cations. The resulting MPF was covalently immobilized on GCE surface via C-C bond with high stability, which was desirable in fabrication of excellent performance biosensors. Probe DNA was self-assembled on AuNPs through the well-known Au-thiol binding. The recognition of fabricated DNA electrochemical biosensor toward complementary single-stranded DNA was determined by differential pulse voltammetry with the use of Co(phen)(3)(3+) as the electrochemical indicator. Taking advantage of amplification effects of AuNPs and stability of MPF, the developed biosensor could detect target DNA with the detection limit of 7.2×10(-11) M, which also exhibits good selectivity, stability and regeneration ability for DNA detection. Copyright © 2010 Elsevier B.V. All rights reserved.

Direct electrochemistry of Shewanella loihica PV-4 on gold nanoparticles-modified boron-doped diamond electrodes fabricated by layer-by-layer technique.

PubMed

Wu, Wenguo; Xie, Ronggang; Bai, Linling; Tang, Zuming; Gu, Zhongze

2012-05-01

Microbial Fuel Cells (MFCs) are robust devices capable of taping biological energy, converting pollutants into electricity through renewable biomass. The fabrication of nanostructured electrodes with good bio- and electrochemical activity, play a profound role in promoting power generation of MFCs. Au nanoparticles (AuNPs)-modified Boron-Doped Diamond (BDD) electrodes are fabricated by layer-by-layer (LBL) self-assembly technique and used for the direct electrochemistry of Shewanella loihica PV-4 in an electrochemical cell. Experimental results show that the peak current densities generated on the Au/PAH multilayer-modified BDD electrodes increased from 1.25 to 2.93 microA/cm(-2) as the layer increased from 0 to 6. Different cell morphologies of S. loihica PV-4 were also observed on the electrodes and the highest density of cells was attached on the (Au/PAH)6/BDD electrode with well-formed three-dimensional nanostructure. The electrochemistry of S. loihica PV-4 was enhanced on the (Au/PAH)4/BDD electrode due to the appropriate amount of AuNPsand thickness of PAH layer.

A repeatable assembling and disassembling electrochemical aptamer cytosensor for ultrasensitive and highly selective detection of human liver cancer cells.

PubMed

Sun, Duanping; Lu, Jing; Chen, Zuanguang; Yu, Yanyan; Mo, Manni

2015-07-23

In this work, a repeatable assembling and disassembling electrochemical aptamer cytosensor was proposed for the sensitive detection of human liver hepatocellular carcinoma cells (HepG2) based on a dual recognition and signal amplification strategy. A high-affinity thiolated TLS11a aptamer, covalently attached to a gold electrode through Au-thiol interactions, was adopted to recognize and capture the target HepG2 cells. Meanwhile, the G-quadruplex/hemin/aptamer and horseradish peroxidase (HRP) modified gold nanoparticles (G-quadruplex/hemin/aptamer-AuNPs-HRP) nanoprobe was designed. It could be used for electrochemical cytosensing with specific recognition and enzymatic signal amplification of HRP and G-quadruplex/hemin HRP-mimicking DNAzyme. With the nanoprobes as recognizing probes, the HepG2 cancer cells were captured to fabricate an aptamer-cell-nanoprobes sandwich-like superstructure on a gold electrode surface. The proposed electrochemical cytosensor delivered a wide detection range from 1×10(2) to 1×10(7) cells mL(-1) and high sensitivity with a low detection limit of 30 cells mL(-1). Furthermore, after the electrochemical detection, the activation potential of -0.9 to -1.7V was performed to break Au-thiol bond and regenerate a bare gold electrode surface, while maintaining the good characteristic of being used repeatedly. The changes of gold electrode behavior after assembling and desorption processes were investigated by electrochemical impedance spectroscopy and cyclic voltammetry techniques. These results indicate that the cytosensor has great potential in disease diagnostic of cancers and opens new insight into the reusable gold electrode with repeatable assembling and disassembling in the electrochemical sensing. Copyright © 2015 Elsevier B.V. All rights reserved.

Amperometric determination of acetylcholine-A neurotransmitter, by chitosan/gold-coated ferric oxide nanoparticles modified gold electrode.

PubMed

Chauhan, Nidhi; Pundir, C S

2014-11-15

An amperometric acetylcholine biosensor was constructed by co-immobilizing covalently, a mixture of acetylcholinesterase (AChE) and choline oxidase (ChO) onto nanocomposite of chitosan (CHIT)/gold-coated ferric oxide nanoparticles (Fe@AuNPs) electrodeposited onto surface of a Au electrode and using it as a working electrode, Ag/AgCl as reference electrode and Pt wire as auxiliary electrode connected through potentiostat. The biosensor is based on electrochemical measurement of H2O2 generated from oxidation of choline by immobilized ChO, which in turn is produced from hydrolysis of acetylcholine by immobilized AChE. The biosensor exhibited optimum response within 3s at +0.2V, pH 7.0 and 30°C. The enzyme electrode had a linear working range of 0.005-400 µM, with a detection limit of 0.005 µM for acetylcholine. The biosensor measured plasma acetylcholine in apparently healthy and persons suffering from Alzheimer's disease. The enzyme electrode was unaffected by a number of serum substances but lost 50% of its initial activity after its 100 uses over a period of 3 months, when stored at 4°C. Copyright © 2014 Elsevier B.V. All rights reserved.

A highly selective and sensitive cocaine aptasensor based on covalent attachment of the aptamer-functionalized AuNPs onto nanocomposite as the support platform.

PubMed

Roushani, Mahmoud; Shahdost-Fard, Faezeh

2015-01-01

Based on the conformational changes of the aptamer-functionalized gold nanoparticles (AuNPs) onto MWCNTs/IL/Chit nanocomposite as the support platform, we have developed a sensitive and selective electrochemical aptasensor for the detection of cocaine. The 5'-amine-3'-AuNP terminated aptamer is covalently attached to a MWCNTs/IL/Chit nanocomposite. The interaction of cocaine with the aptamer functionalized AuNP caused the aptamer to be folded and the AuNPs with negative charge at the end of the aptamer came to the near of electrode surface therefore, the electron transfer between ferricyanide (K3Fe(CN)6) as redox probe and electrode surface was inhibited. A decreased current of (K3Fe(CN)6) was monitored by differential pulse voltammetry technique. In an optimized condition the calibration curve for cocaine concentration was linear up to 11 μM with detection limit (signal-to-noise ratio of 3) of 100 pM. To test the selectivity of the prepared aptasensor sensing platform applicability, some analgesic drugs as the interferes were examined. The potential of the aptasensor was successfully applied for measuring cocaine concentration in human blood serum. Based on our experiments it can be said that the present method is absolutely beneficial in developing other electrochemical aptasensor. Copyright © 2014 Elsevier B.V. All rights reserved.

Broadband absorption enhancement in amorphous Si solar cells using metal gratings and surface texturing

NASA Astrophysics Data System (ADS)

Magdi, Sara; Swillam, Mohamed A.

2017-02-01

The efficiencies of thin film amorphous silicon (a-Si) solar cells are restricted by the small thickness required for efficient carrier collection. This thickness limitations result in poor light absorption. In this work, broadband absorption enhancement is theoretically achieved in a-Si solar cells by using nanostructured back electrode along with surface texturing. The back electrode is formed of Au nanogratings and the surface texturing consists of Si nanocones. The results were then compared to random texturing surfaces. Three dimensional finite difference time domain (FDTD) simulations are used to design and optimize the structure. The Au nanogratings achieved absorption enhancement in the long wavelengths due to sunlight coupling to surface plasmon polaritons (SPP) modes. High absorption enhancement was achieved at short wavelengths due to the decreased reflection and enhanced scattering inside the a-Si absorbing layer. Optimizations have been performed to obtain the optimal geometrical parameters for both the nanogratings and the periodic texturing. In addition, an enhancement factor (i.e. absorbed power in nanostructured device/absorbed power in reference device) was calculated to evaluate the enhancement obtained due to the incorporation of each nanostructure.

An amperometric glutamate biosensor based on immobilization of glutamate oxidase onto carboxylated multiwalled carbon nanotubes/gold nanoparticles/chitosan composite film modified Au electrode.

PubMed

Batra, Bhawna; Pundir, C S

2013-09-15

A method is described for the construction of a novel amperometric glutamate biosensor based on covalent immobilization of glutamate oxidase (GluOx) onto, carboxylated multi walled carbon nanotubes (cMWCNT), gold nanoparticles (AuNPs) and chitosan (CHIT) composite film electrodeposited on the surface of a Au electrode. The GluOx/cMWCNT/AuNP/CHIT modified Au electrode was characterized by scanning electron microscopy (SEM), fourier transform infra-red (FTIR) spectroscopy, electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). The biosensor measured current due to electrons generated at 0.135V against Ag/AgCl from H2O2, which is produced from glutamate by immobilized GluOx. The biosensor showed optimum response within 2s at pH 7.5 and 35°C. A linear relationship was obtained between a wide glutamate concentration range (5-500μM) and current (μA) under optimum conditions. The biosensor showed high sensitivity (155nA/μM/cm(2)), low detection limit (1.6μM) and good storage stability. The biosensor was unaffected by a number of serum substances at their physiological concentrations. The biosensor was evaluated and employed for determination of glutamate in sera from apparently healthy subjects and persons suffering from epilepsy. Copyright © 2013 Elsevier B.V. All rights reserved.

Plasmonic enhancement of visible-light water splitting with Au-TiO2 composite aerogels

NASA Astrophysics Data System (ADS)

Desario, Paul A.; Pietron, Jeremy J.; Devantier, Devyn E.; Brintlinger, Todd H.; Stroud, Rhonda M.; Rolison, Debra R.

2013-08-01

We demonstrate plasmonic enhancement of visible-light-driven splitting of water at three-dimensionally (3D) networked gold-titania (Au-TiO2) aerogels. The sol-gel-derived ultraporous composite nanoarchitecture, which contains 1 to 8.5 wt% Au nanoparticles and titania in the anatase form, retains the high surface area and mesoporosity of unmodified TiO2 aerogels and maintains stable dispersion of the ~5 nm Au guests. A broad surface plasmon resonance (SPR) feature centered at ~550 nm is present for the Au-TiO2 aerogels, but not Au-free TiO2 aerogels, and spans a wide range of the visible spectrum. Gold-derived SPR in Au-TiO2 aerogels cast as films on transparent electrodes drives photoelectrochemical oxidation of aqueous hydroxide and extends the photocatalytic activity of TiO2 from the ultraviolet region to visible wavelengths exceeding 700 nm. Films of Au-TiO2 aerogels in which Au nanoparticles are deposited on pre-formed TiO2 aerogels by a deposition-precipitation method (DP Au/TiO2) also photoelectrochemically oxidize aqueous hydroxide, but less efficiently than 3D Au-TiO2, despite having an essentially identical Au nanoparticle weight fraction and size distribution. For example, 3D Au-TiO2 containing 1 wt% Au is as active as DP Au/TiO2 with 4 wt% Au. The higher photocatalytic activity of 3D Au-TiO2 derives only in part from its ability to retain the surface area and porosity of unmodified TiO2 aerogel. The magnitude of improvement indicates that in the 3D arrangement either a more accessible photoelectrochemical reaction interphase (three-phase boundary) exists or more efficient conversion of excited surface plasmons into charge carriers occurs, thereby amplifying reactivity over DP Au/TiO2. The difference in photocatalytic efficiency between the two forms of Au-TiO2 demonstrates the importance of defining the structure of Au||TiO2 interfaces within catalytic Au-TiO2 nanoarchitectures.We demonstrate plasmonic enhancement of visible-light-driven splitting of water at three-dimensionally (3D) networked gold-titania (Au-TiO2) aerogels. The sol-gel-derived ultraporous composite nanoarchitecture, which contains 1 to 8.5 wt% Au nanoparticles and titania in the anatase form, retains the high surface area and mesoporosity of unmodified TiO2 aerogels and maintains stable dispersion of the ~5 nm Au guests. A broad surface plasmon resonance (SPR) feature centered at ~550 nm is present for the Au-TiO2 aerogels, but not Au-free TiO2 aerogels, and spans a wide range of the visible spectrum. Gold-derived SPR in Au-TiO2 aerogels cast as films on transparent electrodes drives photoelectrochemical oxidation of aqueous hydroxide and extends the photocatalytic activity of TiO2 from the ultraviolet region to visible wavelengths exceeding 700 nm. Films of Au-TiO2 aerogels in which Au nanoparticles are deposited on pre-formed TiO2 aerogels by a deposition-precipitation method (DP Au/TiO2) also photoelectrochemically oxidize aqueous hydroxide, but less efficiently than 3D Au-TiO2, despite having an essentially identical Au nanoparticle weight fraction and size distribution. For example, 3D Au-TiO2 containing 1 wt% Au is as active as DP Au/TiO2 with 4 wt% Au. The higher photocatalytic activity of 3D Au-TiO2 derives only in part from its ability to retain the surface area and porosity of unmodified TiO2 aerogel. The magnitude of improvement indicates that in the 3D arrangement either a more accessible photoelectrochemical reaction interphase (three-phase boundary) exists or more efficient conversion of excited surface plasmons into charge carriers occurs, thereby amplifying reactivity over DP Au/TiO2. The difference in photocatalytic efficiency between the two forms of Au-TiO2 demonstrates the importance of defining the structure of Au||TiO2 interfaces within catalytic Au-TiO2 nanoarchitectures. Electronic supplementary information (ESI) available: Nitrogen physisorption isotherms; Au4f X-ray photoelectron spectra; TEM-derived distributions of Au size and aspect ratio; relative IPCE enhancement ratio. See DOI: 10.1039/c3nr01429k

Proximity hybridization-regulated electrogenerated chemiluminescence bioassay of α-fetoprotein via target-induced quenching mechanism.

PubMed

Gao, Hongfang; Wang, Xiaofei; Li, Man; Qi, Honglan; Gao, Qiang; Zhang, Chengxiao

2017-12-15

A proximity hybridization-regulated electrogenerated chemiluminescence (PLA-ECL) bioassay was developed for the detection of α-fetoprotein (AFP) on basis of the sensitization of gold nanoparticles (AuNPs) and target-induced quenching mechanism. Ru(bpy) 3 2+ was used as ECL signal while ferrocene (Fc) was used as ECL quencher. Ru(bpy) 3 2+ was electrostatically adsorbed into the AuNPs/Nafion film prepared by casting the mixture of Nafion and AuNPs onto the surface of glassy carbon electrode (GCE) to form an ECL platform (Ru(bpy) 3 2+ /AuNPs/Nafion/GCE), which displayed strong ECL emissions. A recognition platform was fabricated by self-assembling a capture DNA via thiol-gold bond on the surface of Ru(bpy) 3 2+ /AuNPs/Nafion/GCE. After sandwich immunoassay and proximity hybridization assay among capture DNA, AFP, a pair of antibody-oligonucleotide conjugates and a signal probe (DNA-Fc), Fc in DNA-Fc was brought close to the surface of electrode in conjunction with target induced ECL quenching. The ECL intensity decreased with the increasing concentration of the AFP and AFP was monitored with a linear range of 0.05-50ng/mL along with a detection limit of 0.04ng/mL. The ECL bioassay is successfully applied to the detection of AFP in serum samples with one-step recognition, short operating time and good accuracy. This method displays great potential for point-of-care testing and commercial application. Copyright © 2017 Elsevier B.V. All rights reserved.

Preparation, Modification, Characterization, and Biosensing Application of Nanoporous Gold Using Electrochemical Techniques

PubMed Central

Neupane, Dharmendra; Nepal, Bishal; Mikhaylov, Vasilii; Stine, Keith J.

2018-01-01

Nanoporous gold (np-Au), because of its high surface area-to-volume ratio, excellent conductivity, chemical inertness, physical stability, biocompatibility, easily tunable pores, and plasmonic properties, has attracted much interested in the field of nanotechnology. It has promising applications in the fields of catalysis, bio/chemical sensing, drug delivery, biomolecules separation and purification, fuel cell development, surface-chemistry-driven actuation, and supercapacitor design. Many chemical and electrochemical procedures are known for the preparation of np-Au. Recently, researchers are focusing on easier and controlled ways to tune the pores and ligaments size of np-Au for its use in different applications. Electrochemical methods have good control over fine-tuning pore and ligament sizes. The np-Au electrodes that are prepared using electrochemical techniques are robust and are easier to handle for their use in electrochemical biosensing. Here, we review different electrochemical strategies for the preparation, post-modification, and characterization of np-Au along with the synergistic use of both electrochemistry and np-Au for applications in biosensing. PMID:29547580

Preparation, Modification, Characterization, and Biosensing Application of Nanoporous Gold Using Electrochemical Techniques.

PubMed

Bhattarai, Jay K; Neupane, Dharmendra; Nepal, Bishal; Mikhaylov, Vasilii; Demchenko, Alexei V; Stine, Keith J

2018-03-16

Nanoporous gold (np-Au), because of its high surface area-to-volume ratio, excellent conductivity, chemical inertness, physical stability, biocompatibility, easily tunable pores, and plasmonic properties, has attracted much interested in the field of nanotechnology. It has promising applications in the fields of catalysis, bio/chemical sensing, drug delivery, biomolecules separation and purification, fuel cell development, surface-chemistry-driven actuation, and supercapacitor design. Many chemical and electrochemical procedures are known for the preparation of np-Au. Recently, researchers are focusing on easier and controlled ways to tune the pores and ligaments size of np-Au for its use in different applications. Electrochemical methods have good control over fine-tuning pore and ligament sizes. The np-Au electrodes that are prepared using electrochemical techniques are robust and are easier to handle for their use in electrochemical biosensing. Here, we review different electrochemical strategies for the preparation, post-modification, and characterization of np-Au along with the synergistic use of both electrochemistry and np-Au for applications in biosensing.

In vivo CH3(CH2)11SAu SAM electrodes in the beating heart: in situ analytical studies relevant to pacemakers and interstitial biosensors.

PubMed

Chou, Howard A; Zavitz, Daniel H; Ovadia, Marc

2003-01-01

To study in vivo modification of the SAM equivalent circuit when a highly ordered SAM is used as a bioelectrode, dodecanethiolate SAM-Au intramuscular electrodes were studied in living rat heart in a challenging in situ perfused rat model by impedance spectroscopy, cyclic voltammetry, and neutron activation analysis (NAA). The SAM layer experienced disintegration in vivo biological system, as NAA detected the presence of Au atoms that had leached into the surrounding living tissue. Therefore, the underlying Au surface became exposed during biological implant. Study by impedance spectroscopy, however, revealed perfect capacitive behavior for the SAM, similar to in vitro behavior. Electrodes showed a pure capacitive Nyquist plot with 86.1-89.4 degrees near-vertical line segments as the equivalent circuit locus, as for a parallel plate capacitor. Impedance magnitude varied linearly with 1/omega excluding diffusionally limited ionic charge transport. There was no diffusional conductive element Z(W infinity ) or spatially confined Warburg impedance Z(D). The effect of in vivo exposure of a highly ordered SAM is a 'sealing over' effect of new defects by the binding of proteinaceous or lipid species in the biological milieu, a fact of significance for SAM electrodes used either as pacemaker electrodes or as a platform for in vivo biosensors.

High-Quality AZO/Au/AZO Sandwich Film with Ultralow Optical Loss and Resistivity for Transparent Flexible Electrodes.

PubMed

Zhou, Hua; Xie, Jing; Mai, Manfang; Wang, Jing; Shen, Xiangqian; Wang, Shuying; Zhang, Lihua; Kisslinger, Kim; Wang, Hui-Qiong; Zhang, Jinxing; Li, Yu; Deng, Junhong; Ke, Shanming; Zeng, Xierong

2018-05-09

Transparent flexible electrodes are in ever-growing demand for modern stretchable optoelectronic devices, such as display technologies, solar cells, and smart windows. Such sandwich-film-electrodes deposited on polymer substrates are unattainable because of the low quality of the films, inducing a relatively large optical loss and resistivity as well as a difficulty in elucidating the interference behavior of light. In this article, we report a high-quality AZO/Au/AZO sandwich film with excellent optoelectronic performance, e.g., an average transmittance of about 81.7% (including the substrate contribution) over the visible range, a sheet resistance of 5 Ω/sq, and a figure-of-merit (FoM) factor of ∼55.1. These values are well ahead of those previously reported for sandwich-film-electrodes. Additionally, the interference behaviors of light modulated by the coat and metal layers have been explored with the employment of transmittance spectra and numerical simulations. In particular, a heater device based on an AZO/Au/AZO sandwich film exhibits high performance such as short response time (∼5 s) and uniform temperature field. This work provides a deep insight into the improvement of the film quality of the sandwich electrodes and the design of high-performance transparent flexible devices by the application of a flexible substrate with an atomically smooth surface.

Growth of copper phthalocyanine rods on Au plasmon electrodes through micelle disruption methods.

PubMed

Chen, Wei-Hung; Ko, Wen-Yin; Chen, Ying-Shiou; Cheng, Ching-Yuan; Chan, Chi-Ming; Lin, Kuan-Jiuh

2010-02-16

To improve the efficiency of the photocurrent conversion process, we have utilized copper phthalocyanine (CuPc) rods, which are capable of enhancing the interfacial area of electron transport and plasmonic gold nanoparticles (Au NPs), which can increase the separation and photogeneration of excitons, to produce a more effective system. In-plane horizontal CuPc rods, with diameters ranging from 0.2 to 1.5 microm, were electrodeposited onto the surface of plasmonic (Au NP) monolayers predeposited onto ITO substrates through electrolytic micelle disruption (EMD) methods.

Interface electronic structures of reversible double-docking self-assembled monolayers on an Au(111) surface

PubMed Central

Zhang, Tian; Ma, Zhongyun; Wang, Linjun; Xi, Jinyang; Shuai, Zhigang

2014-01-01

Double-docking self-assembled monolayers (DDSAMs), namely self-assembled monolayers (SAMs) formed by molecules possessing two docking groups, provide great flexibility to tune the work function of metal electrodes and the tunnelling barrier between metal electrodes and the SAMs, and thus offer promising applications in both organic and molecular electronics. Based on the dispersion-corrected density functional theory (DFT) in comparison with conventional DFT, we carry out a systematic investigation on the dual configurations of a series of DDSAMs on an Au(111) surface. Through analysing the interface electronic structures, we obtain the relationship between single molecular properties and the SAM-induced work-function modification as well as the level alignment between the metal Fermi level and molecular frontier states. The two possible conformations of one type of DDSAM on a metal surface reveal a strong difference in the work-function modification and the electron/hole tunnelling barriers. Fermi-level pinning is found to be a key factor to understand the interface electronic properties. PMID:24615153

Intensification of electrochemiluminescence of luminol on TiO2 supported Au atomic cluster nano-hybrid modified electrode.

PubMed

Yu, Zhimin; Wei, Xiuhua; Yan, Jilin; Tu, Yifeng

2012-04-21

With TiO(2) nanoparticles as carrier, a supported nano-material of Au atomic cluster/TiO(2) nano-hybrid was synthesized. It was then modified onto the surface of indium tin oxide (ITO) by Nafion to act as a working electrode for exciting the electrochemiluminescence (ECL) of luminol. The properties of the nano-hybrid and the modified electrode were characterized by XRD, XPS, electronic microscopy, electrochemistry and spectroscopy. The experimental results demonstrated that the modification of this nano-hybrid onto the ITO electrode efficiently intensified the ECL of luminol. It was also revealed that the ECL intensity of luminol on this modified electrode showed very sensitive responses to oxygen and hydrogen peroxide. The detection limits for dissolved oxygen and hydrogen peroxide were 2 μg L(-1) and 5.5 × 10(-12) M, respectively. Besides the discussion of the intensifying mechanism of this nano-hybrid for ECL of luminol, the developed method was also applied for monitoring dissolved oxygen and evaluating the scavenging efficiency of reactive oxygen species of the Ganoderma lucidum spore.

Ag/Au/Polypyrrole Core-shell Nanowire Network for Transparent, Stretchable and Flexible Supercapacitor in Wearable Energy Devices

NASA Astrophysics Data System (ADS)

Moon, Hyunjin; Lee, Habeom; Kwon, Jinhyeong; Suh, Young Duk; Kim, Dong Kwan; Ha, Inho; Yeo, Junyeob; Hong, Sukjoon; Ko, Seung Hwan

2017-02-01

Transparent and stretchable energy storage devices have attracted significant interest due to their potential to be applied to biocompatible and wearable electronics. Supercapacitors that use the reversible faradaic redox reaction of conducting polymer have a higher specific capacitance as compared with electrical double-layer capacitors. Typically, the conducting polymer electrode is fabricated through direct electropolymerization on the current collector. However, no research have been conducted on metal nanowires as current collectors for the direct electropolymerization, even though the metal nanowire network structure has proven to be superior as a transparent, flexible, and stretchable electrode platform because the conducting polymer’s redox potential for polymerization is higher than that of widely studied metal nanowires such as silver and copper. In this study, we demonstrated a highly transparent and stretchable supercapacitor by developing Ag/Au/Polypyrrole core-shell nanowire networks as electrode by coating the surface of Ag NWs with a thin layer of gold, which provide higher redox potential than the electropolymerizable monomer. The Ag/Au/Polypyrrole core-shell nanowire networks demonstrated superior mechanical stability under various mechanical bending and stretching. In addition, proposed supercapacitors showed fine optical transmittance together with fivefold improved areal capacitance compared to pristine Ag/Au core-shell nanowire mesh-based supercapacitors.

Ag/Au/Polypyrrole Core-shell Nanowire Network for Transparent, Stretchable and Flexible Supercapacitor in Wearable Energy Devices

PubMed Central

Moon, Hyunjin; Lee, Habeom; Kwon, Jinhyeong; Suh, Young Duk; Kim, Dong Kwan; Ha, Inho; Yeo, Junyeob; Hong, Sukjoon; Ko, Seung Hwan

2017-01-01

Transparent and stretchable energy storage devices have attracted significant interest due to their potential to be applied to biocompatible and wearable electronics. Supercapacitors that use the reversible faradaic redox reaction of conducting polymer have a higher specific capacitance as compared with electrical double-layer capacitors. Typically, the conducting polymer electrode is fabricated through direct electropolymerization on the current collector. However, no research have been conducted on metal nanowires as current collectors for the direct electropolymerization, even though the metal nanowire network structure has proven to be superior as a transparent, flexible, and stretchable electrode platform because the conducting polymer’s redox potential for polymerization is higher than that of widely studied metal nanowires such as silver and copper. In this study, we demonstrated a highly transparent and stretchable supercapacitor by developing Ag/Au/Polypyrrole core-shell nanowire networks as electrode by coating the surface of Ag NWs with a thin layer of gold, which provide higher redox potential than the electropolymerizable monomer. The Ag/Au/Polypyrrole core-shell nanowire networks demonstrated superior mechanical stability under various mechanical bending and stretching. In addition, proposed supercapacitors showed fine optical transmittance together with fivefold improved areal capacitance compared to pristine Ag/Au core-shell nanowire mesh-based supercapacitors. PMID:28155913

A novel self-powered and sensitive label-free DNA biosensor in microbial fuel cell.

PubMed

Asghary, Maryam; Raoof, Jahan Bakhsh; Rahimnejad, Mostafa; Ojani, Reza

2016-08-15

In this work, a novel self-powered, sensitive, low-cost, and label-free DNA biosensor is reported by applying a two-chambered microbial fuel cell (MFC) as a power supply. A graphite electrode and an Au nanoparticles modified graphite electrode (AuNP/graphite electrode) were used as anode and cathode in the MFC system, respectively. The active biocatalyst in the anodic chamber was a mixed culture of microorganisms. The sensing element of the biosensor was fabricated by the well-known Au-thiol binding the ssDNA probe on the surface of an AuNP/graphite cathode. Electrons produced by microorganisms were transported from the anode to the cathode through an external circuit, which could be detected by the terminal multi-meter detector. The difference between power densities of the ssDNA probe modified cathode in the absence and presence of complementary sequence served as the detection signal of the DNA hybridization with detection limit of 3.1nM. Thereafter, this biosensor was employed for diagnosis and determination of complementary sequence in a human serum sample. The hybridization specificity studies further revealed that the developed DNA biosensor could distinguish fully complementary sequences from one-base mismatched and non-complementary sequences. Copyright © 2016 Elsevier B.V. All rights reserved.

Development of neuraminidase detection using gold nanoparticles boron-doped diamond electrodes.

PubMed

Wahyuni, Wulan T; Ivandini, Tribidasari A; Saepudin, Endang; Einaga, Yasuaki

2016-03-15

Gold nanoparticles-modified boron-doped diamond (AuNPs-BDD) electrodes, which were prepared with a self-assembly deposition of AuNPs at amine-terminated boron-doped diamond, were examined for voltammetric detection of neuraminidase (NA). The detection method was performed based on the difference of electrochemical responses of zanamivir at gold surface before and after the reaction with NA in phosphate buffer solution (PBS, pH 5.5). A linear calibration curve for zanamivir in 0.1 M PBS in the absence of NA was achieved in the concentration range of 1 × 10(-6) to 1 × 10(-5) M (R(2) = 0.99) with an estimated limit of detection (LOD) of 2.29 × 10(-6) M. Furthermore, using its reaction with 1.00 × 10(-5) M zanamivir, a linear calibration curve of NA can be obtained in the concentration range of 0-12 mU (R(2) = 0.99) with an estimated LOD of 0.12 mU. High reproducibility was shown with a relative standard deviation (RSD) of 1.14% (n = 30). These performances could be maintained when the detection was performed in mucin matrix. Comparison performed using gold-modified BDD (Au-BDD) electrodes suggested that the good performance of the detection method is due to the stability of the gold particles position at the BDD surface. Copyright © 2016 Elsevier Inc. All rights reserved.

Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lapp, Aliya S.; Duan, Zhiyao; Marcella, Nicholas

In this report we examine the structure of bimetallic nanomaterials prepared by an electrochemical approach known as hydride-terminated (HT) electrodeposition. It has been shown previously that this method can lead to deposition of a single Pt monolayer on bulk-phase Au surfaces. Specifically, under appropriate electrochemical conditions and using a solution containing PtCl 4 2-, a monolayer of Pt atoms electrodeposits onto bulk-phase Au immediately followed by a monolayer of H atoms. The H-atom capping layer prevents deposition of Pt multilayers. We applied this method to ~1.6 nm Au nanoparticles (AuNPs) immobilized on an inert electrode surface. In contrast to themore » well-defined, segregated Au/Pt structure of the bulk-phase surface, we observe that HT electrodeposition leads to the formation of AuPt quasi-random alloy NPs rather than the core@shell structure anticipated from earlier reports relating to deposition onto bulk phases. The results provide a good example of how the phase behavior of macro materials does not always translate to the nano world. A key component of this study was the structure determination of the AuPt NPs, which required a combination of electrochemical methods, electron microscopy, X-ray absorption spectroscopy, and theory (DFT and MD).« less

Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized using a Direct Electrochemical Method

DOE PAGES

Lapp, Aliya S.; Duan, Zhiyao; Marcella, Nicholas; ...

2018-06-01

In this report we examine the structure of bimetallic nanomaterials prepared by an electrochemical approach known as hydride-terminated (HT) electrodeposition. It has been shown previously that this method can lead to deposition of a single Pt monolayer on bulk-phase Au surfaces. Specifically, under appropriate electrochemical conditions and using a solution containing PtCl 4 2-, a monolayer of Pt atoms electrodeposits onto bulk-phase Au immediately followed by a monolayer of H atoms. The H-atom capping layer prevents deposition of Pt multilayers. We applied this method to ~1.6 nm Au nanoparticles (AuNPs) immobilized on an inert electrode surface. In contrast to themore » well-defined, segregated Au/Pt structure of the bulk-phase surface, we observe that HT electrodeposition leads to the formation of AuPt quasi-random alloy NPs rather than the core@shell structure anticipated from earlier reports relating to deposition onto bulk phases. The results provide a good example of how the phase behavior of macro materials does not always translate to the nano world. A key component of this study was the structure determination of the AuPt NPs, which required a combination of electrochemical methods, electron microscopy, X-ray absorption spectroscopy, and theory (DFT and MD).« less

Experimental and Theoretical Structural Investigation of AuPt Nanoparticles Synthesized Using a Direct Electrochemical Method.

PubMed

Lapp, Aliya S; Duan, Zhiyao; Marcella, Nicholas; Luo, Long; Genc, Arda; Ringnalda, Jan; Frenkel, Anatoly I; Henkelman, Graeme; Crooks, Richard M

2018-05-11

In this report, we examine the structure of bimetallic nanomaterials prepared by an electrochemical approach known as hydride-terminated (HT) electrodeposition. It has been shown previously that this method can lead to deposition of a single Pt monolayer on bulk-phase Au surfaces. Specifically, under appropriate electrochemical conditions and using a solution containing PtCl 4 2- , a monolayer of Pt atoms electrodeposits onto bulk-phase Au immediately followed by a monolayer of H atoms. The H atom capping layer prevents deposition of Pt multilayers. We applied this method to ∼1.6 nm Au nanoparticles (AuNPs) immobilized on an inert electrode surface. In contrast to the well-defined, segregated Au/Pt structure of the bulk-phase surface, we observe that HT electrodeposition leads to the formation of AuPt quasi-random alloy NPs rather than the core@shell structure anticipated from earlier reports relating to deposition onto bulk phases. The results provide a good example of how the phase behavior of macro materials does not always translate to the nano world. A key component of this study was the structure determination of the AuPt NPs, which required a combination of electrochemical methods, electron microscopy, X-ray absorption spectroscopy, and theory (DFT and MD).

Enhanced photoelectrocatalytic performance of α-Fe2O3 thin films by surface plasmon resonance of Au nanoparticles coupled with surface passivation by atom layer deposition of Al2O3.

PubMed

Liu, Yuting; Xu, Zhen; Yin, Min; Fan, Haowen; Cheng, Weijie; Lu, Linfeng; Song, Ye; Ma, Jing; Zhu, Xufei

2015-12-01

The short lifetime of photogenerated charge carriers of hematite (α-Fe2O3) thin films strongly hindered the PEC performances. Herein, α-Fe2O3 thin films with surface nanowire were synthesized by electrodeposition and post annealing method for photoelectrocatalytic (PEC) water splitting. The thickness of the α-Fe2O3 films can be precisely controlled by adjusting the duration of the electrodeposition. The Au nanoparticles (NPs) and Al2O3 shell by atom layer deposition were further introduced to modify the photoelectrodes. Different constructions were made with different deposition orders of Au and Al2O3 on Fe2O3 films. The Fe2O3-Au-Al2O3 construction shows the best PEC performance with 1.78 times enhancement by localized surface plasmon resonance (LSPR) of NPs in conjunction with surface passivation of Al2O3 shells. Numerical simulation was carried out to investigate the promotion mechanisms. The high PEC performance for Fe2O3-Au-Al2O3 construction electrode could be attributed to the Al2O3 intensified LSPR, effective surface passivation by Al2O3 coating, and the efficient charge transfer due to the Fe2O3-Au Schottky junctions.

Sensitive electrochemiluminescence biosensor based on Au-ITO hybrid bipolar electrode amplification system for cell surface protein detection.

PubMed

Wu, Mei-Sheng; Yuan, Da-Jing; Xu, Jing-Juan; Chen, Hong-Yuan

2013-12-17

Here we developed a novel hybrid bipolar electrode (BPE)-electrochemiluminescence (ECL) biosensor based on hybrid bipolar electrode (BPE) for the measurement of cancer cell surface protein using ferrocence (Fc) labeled aptamer as signal recognition and amplification probe. According to the electric neutrality of BPE, the cathode of U-shaped ITO BPE was electrochemically deposited by Au nanoparticles (NPs) to enhance its conductivity and surface area, decrease the overpotential of O2 reduction, which would correspondingly increase the oxidation current of Ru(bpy)3(2+)/tripropylamine (TPA) on the anode of BPE and resulting a ∼4-fold enhancement of ECL intensity. Then a signal amplification strategy was designed by introducing Fc modified aptamer on the anode surface of BPE through hybridization for detecting the amount of mucin-1 on MCF-7 cells. The presence of Fc could not only inhibit the oxidation of Ru(bpy)3(2+) because of its lower oxidation potential, its oxidation product Fc(+) could also quench the ECL of Ru(bpy)3(2+)/TPA by efficient energy-transfer from the excited-state Ru(bpy)3(2+)* to Fc(+), making the ECL intensity greatly quenched. On the basis of the cathodic Au NPs induced ECL enhancing coupled with anodic Fc induced signal quenching amplification, the approach allowed detection of mucin-1 aptamer at a concentration down to 0.5 fM and was capable of detecting a minimum of 20 MCF-7 cells. Besides, the amount of mucin-1 on MCF-7 cells was calculated to be 9041 ± 388 molecules/cell. This approach therefore shows great promise in bioanalysis.

Fabrication, characterisation and voltammetric studies of gold amalgam nanoparticle modified electrodes.

PubMed

Welch, Christine M; Nekrassova, Olga; Dai, Xuan; Hyde, Michael E; Compton, Richard G

2004-09-20

The tabrication, characterisation, and electroanalytical application of gold and gold amalgam nanoparticles on glassy carbon electrodes is examined. Once the deposition parameters for gold nanoparticle electrodes were optimised, the analytical utility of the electrodes was examined in CrIII electroanalysis. It was found that gold nanoparticle modified (Au-NM) electrodes possess higher sensitivity than gold macroelectrodes. In addition, gold amalgam nanoparticle modified (AuHg-NM) electrodes were fabricated and characterised. The response of those electrodes was recorded in the presence of important environmental analytes (heavy metal cations). It was found AuHg-NM electrodes demonstrate a unique voltammetric behaviour and can be applied for electroanalysis when enhanced sensitivity is crucial.

Photovoltaic enhancement due to surface-plasmon assisted visible-light absorption at the inartificial surface of lead zirconate-titanate film

NASA Astrophysics Data System (ADS)

Zheng, Fengang; Zhang, Peng; Wang, Xiaofeng; Huang, Wen; Zhang, Jinxing; Shen, Mingrong; Dong, Wen; Fang, Liang; Bai, Yongbin; Shen, Xiaoqing; Sun, Hua; Hao, Jianhua

2014-02-01

PZT film of 300 nm thickness was deposited on tin indium oxide (ITO) coated quartz by a sol-gel method. Four metal electrodes, such as Pt, Au, Cu and Ag, were used as top electrodes deposited on the same PZT film by sputtering at room temperature. In ITO-PZT-Ag and ITO-PZT-Au structures, the visible light (400-700 nm) can be absorbed partially by a PZT film, and the maximum efficiency of photoelectric conversion of the ITO-PZT-Ag structure was enhanced to 0.42% (100 mW cm-2, AM 1.5G), which is about 15 times higher than that of the ITO-PZT-Pt structure. Numerical simulations show that the natural random roughness of polycrystalline-PZT-metal interface can offer a possibility of coupling between the incident photons and SPs at the metal surface. The coincidence between the calculated SP properties and the measured EQE spectra reveals the SP origin of the photovoltaic enhancement in these ITO-PZT-metal structures, and the improved photocurrent output is caused by the enhanced optical absorption in the PZT region near the metal surface, rather than by the direct charge-transfer process between two materials.PZT film of 300 nm thickness was deposited on tin indium oxide (ITO) coated quartz by a sol-gel method. Four metal electrodes, such as Pt, Au, Cu and Ag, were used as top electrodes deposited on the same PZT film by sputtering at room temperature. In ITO-PZT-Ag and ITO-PZT-Au structures, the visible light (400-700 nm) can be absorbed partially by a PZT film, and the maximum efficiency of photoelectric conversion of the ITO-PZT-Ag structure was enhanced to 0.42% (100 mW cm-2, AM 1.5G), which is about 15 times higher than that of the ITO-PZT-Pt structure. Numerical simulations show that the natural random roughness of polycrystalline-PZT-metal interface can offer a possibility of coupling between the incident photons and SPs at the metal surface. The coincidence between the calculated SP properties and the measured EQE spectra reveals the SP origin of the photovoltaic enhancement in these ITO-PZT-metal structures, and the improved photocurrent output is caused by the enhanced optical absorption in the PZT region near the metal surface, rather than by the direct charge-transfer process between two materials. Electronic supplementary information (ESI) available. See DOI: 10.1039/c3nr05757g

One-Step Electrochemical Fabrication of Reduced Graphene Oxide/Gold Nanoparticles Nanocomposite-Modified Electrode for Simultaneous Detection of Dopamine, Ascorbic Acid, and Uric Acid

PubMed Central

Lee, Chang-Seuk; Yu, Su Hwan; Kim, Tae Hyun

2017-01-01

Here, we introduce the preparation of the hybrid nanocomposite-modified electrode consisting of reduced graphene oxide (RGO) and gold nanoparticles (AuNPs) using the one-step electrochemical method, allowing for the simultaneous and individual detection of dopamine (DA), ascorbic acid (AA), and uric acid (UA). RGO/AuNPs nanocomposite was formed on a glassy carbon electrode by the co-reduction of GO and Au3+ using the potentiodynamic method. The RGO/AuNPs nanocomposite-modified electrode was produced by subjecting a mixed solution of GO and Au3+ to cyclic sweeping from −1.5 V to 0.8 V (vs. Ag/AgCl) at a scan rate 10 mV/s for 3 cycles. The modified electrode was characterized by scanning electron microscopy, Raman spectroscopy, contact angle measurement, electrochemical impedance spectroscopy, and cyclic voltammetry. Voltammetry results confirm that the RGO/AuNPs nanocomposite-modified electrode has high catalytic activity and good resolution for the detection of DA, AA, and UA. The RGO/AuNPs nanocomposite-modified electrode exhibits stable amperometric responses for DA, AA, and UA, respectively, and its detection limits were estimated to be 0.14, 9.5, and 25 μM. The modified electrode shows high selectivity towards the determination of DA, AA, or UA in the presence of potentially active bioelements. In addition, the resulting sensor exhibits many advantages such as fast amperometric response, excellent operational stability, and appropriate practicality. PMID:29301209

Carbon Dioxide Gas Sensors and Method of Manufacturing and Using Same

NASA Technical Reports Server (NTRS)

Liu, Chung Chiun (Inventor); Ward, Benjamin J. (Inventor); Hunter, Gary W. (Inventor); Xu, Jennifer C. (Inventor)

2011-01-01

A gas sensor includes a substrate and a pair of interdigitated metal electrodes selected from the group consisting of Pt, Pd, Au, Ir, Ag, Ru, Rh, In, and Os. The electrodes each include an upper surface. A first solid electrolyte resides between the interdigitated electrodes and partially engages the upper surfaces of the electrodes. The first solid electrolyte is selected from the group consisting of NASICON, LISICON, KSICON, and .beta.''-Alumina (beta prime-prime alumina in which when prepared as an electrolyte is complexed with a mobile ion selected from the group consisting of Na.sup.+, K.sup.+, Li.sup.+, Ag.sup.+, H.sup.+, Pb.sup.2+, Sr.sup.2+ or Ba.sup.2+). A second electrolyte partially engages the upper surfaces of the electrodes and engages the first solid electrolyte in at least one point. The second electrolyte is selected from the group of compounds consisting of Na.sup.+, K.sup.+, Li.sup.+, Ag.sup.+, H.sup.+, Pb.sup.2+, Sr.sup.2+ or Ba.sup.2+ ions or combinations thereof.

Total inorganic arsenic detection in real water samples using anodic stripping voltammetry and a gold-coated diamond thin-film electrode.

PubMed

Song, Yang; Swain, Greg M

2007-06-12

An accurate method for total inorganic arsenic determination in real water samples was developed using differential pulse anodic stripping voltammetry (DPASV) and a Au-coated boron-doped diamond thin-film electrode. Keys to the method are the use of a conducting diamond platform and solid phase extraction for sample preparation. In the method, the As(III) present in the sample is first detected by DPASV. The As(V) present is then reduced to As(III) by reaction with Na2SO3 and this is followed by a second detection of As(III) by DPASV. Interfering metal ions (e.g., Cu(II)) that cause decreased electrode response sensitivity for arsenic in real samples are removed by solid phase extraction as part of the sample preparation. For example, Cu(II) caused a 30% decrease in the As stripping peak current at a solution concentration ratio of 3:1 (Cu(II)/As(III)). This loss was mitigated by passage of the solution through a Chelex 100 cation exchange resin. After passage, only a 5% As stripping current response loss was seen. The effect of organic matter on the Au-coated diamond electrode response for As(III) was also evaluated. Humic acid at a 5 ppm concentration caused only a 9% decrease in the As stripping peak charge for Au-coated diamond. By comparison, a 50% response decrease was observed for Au foil. Clearly, the chemical properties of the diamond surface in the vicinity of the metal deposits inhibit molecular adsorption on at least some of the Au surface. The method provided reproducible and accurate results for total inorganic arsenic in two contaminated water samples provided by the U.S. Bureau of Reclamation. The total inorganic As concentration in the two samples, quantified by the standard addition method, was 23.2+/-2.9 ppb for UV plant influent water and 16.4+/-0.9 ppb for Well 119 water (n=4). These values differed from the specified concentrations by less than 4%.

Production of gold nanoparticles by electrode-respiring Geobacter sulfurreducens biofilms

PubMed Central

Tanzil, Abid H.; Sultana, Sujala T.; Saunders, Steven R.; Dohnalkova, Alice C.; Shi, Liang; Davenport, Emily; Ha, Phuc; Beyenal, Haluk

2017-01-01

The goal of this work was to synthesize gold nanoparticles (AuNPs) using electrode-respiring Geobacter sulfurreducens biofilms. We found that AuNPs are generated in the extracellular matrix of Geobacter biofilms and have an average particle size of 20 nm. The formation of AuNPs was verified using TEM, FTIR and EDX. We also found that the extracellular substances extracted from electrode-respiring G. sulfurreducens biofilms reduce Au3+ to AuNPs. From FTIR spectra, it appears that reduced sugars were involved in the bioreduction and synthesis of AuNPs and that amine groups acted as the major biomolecules involved in binding. PMID:27866628

Multivalent interaction based carbohydrate biosensors for signal amplification

PubMed Central

Wang, Yanyan; Chalagalla, Srinivas; Li, Tiehai; Sun, Xue-long; Zhao, Wei; Wang, Peng; Zeng, Xiangqun

2010-01-01

Multivalent interaction between boronic acids immobilized on Quartz Crystal Microbalance (QCM) sensor surface and the carbohydrates modified Au - nanoparticle (AuNP) has been demonstrated for the development of a sensitive carbohydrate biosensor. Briefly, a boronic acid - containing polymer (boropolymer) as multivalent carbohydrate receptor was oriented immobilized on the cysteamine coated electrode through isourea bond formation. Carbohydrates were conjugated to AuNPs to generate a multivalent carbohydrates moiety to amplify the response signal. Thus, the binding of the carbohydrate conjugated AuNPs to the boropolymer surface are multivalent which could simultaneously increase the binding affinity and specificity. We systematically studied the binding between five carbohydrate conjugated AuNPs and the boropolymer. Our studies show that the associate constant (Ka) was in the order of fucose < glucose < mannose < galactose < maltose. A linear response in the range from 23 µM to 3.83 mM was observed for mannose conjugated AuNPs and the boropolymer recognition elements, with the lower detection limit of 1.5 µM for the carbohydrate analytes. Furthermore, the multivalent binding between carbohydrates and boronic acids are reversible and allow the regeneration of boropolymer surface by using 1M acetic acid so as to sequentially capture and release the carbohydrate analytes. PMID:20863680

Top-Contact Pentacene-Based Organic Thin Film Transistor (OTFT) with N, N'-Bis(3-Methyl Phenyl)- N, N'-Diphenyl Benzidine (TPD)/Au Bilayer Source-Drain Electrode

NASA Astrophysics Data System (ADS)

Borthakur, Tribeni; Sarma, Ranjit

2018-01-01

A top-contact Pentacene-based organic thin film transistor (OTFT) with N, N'-Bis (3-methyl phenyl)- N, N'-diphenyl benzidine (TPD)/Au bilayer source-drain electrode is reported. The devices with TPD/Au bilayer source-drain (S-D) electrodes show better performance than the single layer S-D electrode OTFT devices. The field-effect mobility of 4.13 cm2 v-1 s-1, the on-off ratio of 1.86 × 107, the threshold voltage of -4 v and the subthreshold slope of .27 v/decade, respectively, are obtained from the device with a TPD/Au bilayer source-drain electrode.

Label-free impedimetric aptasensor for detection of femtomole level acetamiprid using gold nanoparticles decorated multiwalled carbon nanotube-reduced graphene oxide nanoribbon composites.

PubMed

Fei, Airong; Liu, Qian; Huan, Juan; Qian, Jing; Dong, Xiaoya; Qiu, Baijing; Mao, Hanping; Wang, Kun

2015-08-15

Gold nanoparticles (Au NPs) decorated multiwalled carbon nanotube-reduced graphene oxide nanoribbon (Au/MWCNT-rGONR) composites were synthesized by a one-pot reaction. By employing the resulting Au/MWCNT-rGONR composites as the support for aptamer immobilization, we developed an ultrasensitive label-free electrochemical impedimetric aptasensor for acetamiprid detection, which was based on that the variation of electron transfer resistance was relevant to the formation of acetamiprid-aptamer complex at the modified electrode surface. Compared with pure Au NPs and MWCNT-rGONR, the Au/MWCNT-rGONR composites modified electrode was the most sensitive aptasensing platform for the determination of acetamiprid. The proposed aptasensor displayed a linear response for acetamiprid in the range from 5×10(-14) M to 1×10(-5) M with an extremely low detection limit of 1.7×10(-14) M (S/N=3). In addition, this impedimetric aptasensor possessed great advantages including the simple operation process, low-cost, selectivity and sensitivity, which provided a promising model for the aptamer-based detection with a direct impedimetric method. Copyright © 2015 Elsevier B.V. All rights reserved.

Transparent, broadband, flexible, and bifacial-operable photodetectors containing a large-area graphene-gold oxide heterojunction.

PubMed

Liu, Yu-Lun; Yu, Chen-Chieh; Lin, Keng-Te; Yang, Tai-Chi; Wang, En-Yun; Chen, Hsuen-Li; Chen, Li-Chyong; Chen, Kuei-Hsien

2015-05-26

In this study, we combine graphene with gold oxide (AuOx), a transparent and high-work-function electrode material, to achieve a high-efficient, low-bias, large-area, flexible, transparent, broadband, and bifacial-operable photodetector. The photodetector operates through hot electrons being generated in the graphene and charge separation occurring at the AuOx-graphene heterojunction. The large-area graphene covering the AuOx electrode efficiently prevented reduction of its surface; it also acted as a square-centimeter-scale active area for light harvesting and photodetection. Our graphene/AuOx photodetector displays high responsivity under low-intensity light illumination, demonstrating picowatt sensitivity in the ultraviolet regime and nanowatt sensitivity in the infrared regime for optical telecommunication. In addition, this photodetector not only exhibited broadband (from UV to IR) high responsivity-3300 A W(-1) at 310 nm (UV), 58 A W(-1) at 500 nm (visible), and 9 A W(-1) at 1550 nm (IR)-but also required only a low applied bias (0.1 V). The hot-carrier-assisted photoresponse was excellent, especially in the short-wavelength regime. In addition, the graphene/AuOx photodetector exhibited great flexibility and stability. Moreover, such vertical heterojunction-based graphene/AuOx photodetectors should be compatible with other transparent optoelectronic devices, suggesting applications in flexible and wearable optoelectronic technologies.

Facile construction of a highly sensitive DNA biosensor by in-situ assembly of electro-active tags on hairpin-structured probe fragment

PubMed Central

Wang, Qingxiang; Gao, Feng; Ni, Jiancong; Liao, Xiaolei; Zhang, Xuan; Lin, Zhenyu

2016-01-01

An ultrasensitive DNA biosensor has been developed through in-situ labeling of electroactive melamine-Cu2+ complex (Mel-Cu2+) on the end of hairpin-like probe using gold nanoparticles (AuNPs) as the signal amplification platform. The 3′-thiolated hairpin-like probe was first immobilized to the gold electrode surface by the Au-S bond. The AuNPs were then tethered on the free 5′-end of the immobilized probe via the special affinity between Au and the modified -NH2. Followed by, the Mel and Cu2+ were assembled on the AuNPs surface through Au-N bond and Cu2+-N bond, respectively. Due to the surface area and electrocatalytic effects of the AuNPs, the loading amount and electron transfer kinetic of the Mel-Cu2+ were enhanced greatly, resulting in significantly enhanced electrochemical response of the developed biosensor. Compared with the synthesis process of conventional electroactive probe DNA accomplished by homogeneous method, the method presented in this work is more reagent- and time-saving. The proposed biosensor showed high selectivity, wide linear range and low detection limit. This novel strategy could also be extended to the other bioanalysis platforms such as immunosensors and aptasensors. PMID:26931160

Electrostatic interaction between an enzyme and electrodes in the electric double layer examined in a view of direct electron transfer-type bioelectrocatalysis.

PubMed

Sugimoto, Yu; Kitazumi, Yuki; Tsujimura, Seiya; Shirai, Osamu; Yamamoto, Masahiro; Kano, Kenji

2015-01-15

Effects of the electrode poential on the activity of an adsorbed enzyme has been examined by using copper efflux oxidase (CueO) as a model enzyme and by monitoring direct electron transfer (DET)-type bioelectrocatalysis of oxygen reduction. CueO adsorbed on bare Au electrodes at around the point of zero charge (E(pzc)) shows the highest DET activity, and the activity decreases as the adsorption potential (E(ad); at which the enzyme adsorbs) is far from E(pzc). We propose a model to explain the phenomena in which the electrostatic interaction between the enzyme and electrodes in the electric double layer affects the orientation and the stability of the adsorbed enzyme. The self-assembled monolayer of butanethiol on Au electrodes decreases the electric field in the outside of the inner Helmholtz plane and drastically diminishes the E(ad) dependence of the DET activity of CueO. When CueO is adsorbed on bare Au electrodes under open circuit potential and then is held at hold potentials (E(ho)) more positive than E(pzc), the DET activity of the CueO rapidly decreases with the hold time. The strong electric field with positive surface charge density on the metallic electrode (σ(M)) leads to fatal denaturation of the adsorbed CueO. Such denaturation effect is not so serious at E(ho)

Tungsten oxide-Au nanosized film composites for glucose oxidation and sensing in neutral medium

PubMed Central

Gougis, Maxime; Ma, Dongling; Mohamedi, Mohamed

2015-01-01

In this work, we report for the first time the use of tungsten oxide (WOx) as catalyst support for Au toward the direct electrooxidation of glucose. The nanostructured WOx/Au electrodes were synthesized by means of laser-ablation technique. Both micro-Raman spectroscopy and transmission electron microscopy showed that the produced WOx thin film is amorphous and made of ultrafine particles of subnanometer size. X-ray diffraction and X-ray photoelectron spectroscopy revealed that only metallic Au was present at the surface of the WOx/Au composite, suggesting that the WOx support did not alter the electronic structure of Au. The direct electrocatalytic oxidation of glucose in neutral medium such as phosphate buffered saline (pH 7.2) solution has been investigated with cyclic voltammetry, chronoamperometry, and square-wave voltammetry. Sensitivity as high as 65.7 μA cm−2 mM−1 up to 10 mM of glucose and a low detection limit of 10 μM were obtained with square-wave voltammetry. This interesting analytical performance makes the laser-fabricated WOx/Au electrode potentially promising for implantable glucose fuel cells and biomedical analysis as the evaluation of glucose concentration in biological fluids. Finally, owing to its unique capabilities proven in this work, it is anticipated that the laser-ablation technique will develop as a fabrication tool for chip miniature-sized sensors in the near future. PMID:25931820

Hydrogen peroxide sensing using ultrathin platinum-coated gold nanoparticles with core@shell structure.

PubMed

Li, Yongxin; Lu, Qiufang; Wu, Shengnan; Wang, Lun; Shi, Xianming

2013-03-15

Ultrathin platinum-coated gold (Pt@Au) nanoparticles with core@shell structure have been developed by under-potential deposition (UPD) redox replacement technique. A single UPD Cu replacement with Pt(2+) produced a uniform Pt monolayer on the surface of gold nanoparticles, which are immobilized on glassy carbon electrode (GCE) surface based on electrostatic interaction. The ultrathin Pt@Au nanoparticles were confirmed by cyclic voltammetry and X-ray photoelectron spectroscopy (XPS). Voltammetry and amperometric methodologies were used to evaluate the electrocatalytic activity of the Pt@Au nanoparticles modified electrode towards the reduction of hydrogen peroxide under the physiological condition. The present results show that ultrathin Pt coating greatly enhances the electrocatalytic activity towards the reduction of hydrogen peroxide, which can be utilized to fabricate the hydrogen peroxide sensor. Chronoamperometric experiments showed that at an applied potential of 0.08 V (vs. Ag/AgCl), the current reduction of hydrogen peroxide was linear to its concentration in the range of 1-450 μΜ, and the detection limit was found to be 0.18 μM (signal-to-noise ratio, S/N=3). Copyright © 2012 Elsevier B.V. All rights reserved.

Nanoscale Structural Changes Upon Electrooxidation of Au(111) as Probed by Potentiodynamic Scanning Tunneling Microscopy

DTIC Science & Technology

1994-02-01

electrochemical formation and removal of oxide films is of broadbased practical as well as fundamental importance. Studies of noble metals, such as gold and...atomic level. At the current state of development of STM, monocrystalline gold electrodes provide efficacious choices of systems, partly in view of...several in-situ STM studies have focussed on the surface morphological changes attending oxidation and rereduction of single-crystal gold electrodes

Voltammetric determination of the Escherichia coli DNA using a screen-printed carbon electrode modified with polyaniline and gold nanoparticles.

PubMed

Shoaie, Nahid; Forouzandeh, Mehdi; Omidfar, Kobra

2018-03-12

The authors describe an electrochemical assay for fast detection of Escherichia coli (E. coli). It is based on a dual signal amplification strategy and the use of a screen-printed carbon electrode (SPCE) whose surface was modified with a polyaniline (PANI) film and gold nanoparticles (AuNPs) via cyclic voltammetry (CV). In the next step, avidin was covalently immobilized on the PANI/AuNP composite on the SPCE surface. Subsequently, the biotinylated DNA capture probe was immobilized onto the PANI/AuNP/avidin-modified SPCE by biotin-avidin interaction. Then, DNA of E.coli, digoxigenin-labeled DNA detector probe and anti-digoxigenin-labeled horseradish peroxidase (HRP) were placed on the electrode. 3,3',5,5'-Tetramethylbenzidine (TMB) and H 2 O 2 solution were added and the CV electrochemical signal was generated at a potential of -0.1 V (vs. Ag/AgCl) and a scan rate 50 mV.s -1 . The assay can detect 4 × 10 6 to 4 CFU of E. coli without DNA amplification. The biosensor is highly specific over other pathogens including Klebsiella pneumoniae, Proteus mirabilis, Enterococcus faecalis, Staphylococcus haemolyticus and Pseudomonas aeruginosa. It can be concluded that this genosensor has an excellent potential for rapid and accurate diagnosis of E.coli inflicted infections. Graphical Abstract Schematic of an electrochemical E. coli genosensor based on sandwich assay on a polyaniline/gold nanoparticle-modified screen printed carbon electrode (SPCE). The biosensor can detect 4 × 10 6 to 4 CFU of E. coli without DNA amplification.

Cyto-sensing in electrochemical lab-on-paper cyto-device for in-situ evaluation of multi-glycan expressions on cancer cells.

PubMed

Su, Min; Ge, Lei; Kong, Qingkun; Zheng, Xiaoxiao; Ge, Shenguang; Li, Nianqiang; Yu, Jinghua; Yan, Mei

2015-01-15

A novel electrochemical lab-on-paper cyto-device (ELPCD) was fabricated to demonstrate sensitive and specific cancer cell detection as well as in-situ monitoring of multi-glycans on living cancer cells. In this ELPCD, aptamers modified three-dimensional macroporous Au-paper electrode (Au-PE) was employed as the working electrode for specific and efficient cancer cell capture. Using a sandwich format, sensitive and reproducible cell detection was achieved in this ELPCD on the basis of the electrochemical signal amplification of the Au-PE and the horseradish peroxidase-lectin electrochemical probe. The ELPCD displayed excellent analytical performance for the detection of four K562 cells with a wide linear calibration range from 550 to 2.0×10(7) cells mL(-1). Then, this ELPCD was successfully applied to determine cell-surface multi-glycans in parallel and in-situ monitor multi-glycans expression on living cells in response to drug treatment through in-electrode 3D cell culture. The proposed method provides promising application in decipherment of the glycomic codes as well as clinical diagnosis and treatment in early process of cancer. Copyright © 2014 Elsevier B.V. All rights reserved.

Amperometric detection of catechol using tyrosinase modified electrodes enhanced by the layer-by-layer assembly of gold nanocubes and polyelectrolytes.

PubMed

Karim, Md Nurul; Lee, Ji Eun; Lee, Hye Jin

2014-11-15

A novel amperometric biosensor for catechol was developed using the layer-by-layer (LbL) self-assembly of positively charged hexadecyltrimethylammonium stabilized gold nanocubes (AuNCs), negatively charged poly(sodium 4-styrenesulfonate) and tyrosinase on a screen printed carbon electrode (SPCE). A carboxylic acid terminated alkanethiol assembled on electrochemically deposited Au nanoparticles on a SPCE was used as a platform for LbL assembly. Each SPCE sensor surface was terminated with tyrosinase and the electrocatalytic response due to the tyrosinase reaction with catechol was measured using cyclic voltammetry and square wave voltammetry (SWV). The effect of introducing AuNCs into the LbL assembly to further enhance the catechol detection performance was then investigated by comparing the SWV results to those from biosensors created using both the tyrosinase modified LbL assembly in the absence of NCs and the covalent attachment of tyrosinase. A wide dynamic range from 10nM to 80 µM of catechol with an excellent sensitivity of 13.72 A/M and a detection limit of 0.4 nM were both achieved alongside a good selectivity and reproducibility for the AuNC-modified electrodes. As a demonstration, the optimized biosensor design was applied to determine catechol concentrations in tea samples. Copyright © 2014 Elsevier B.V. All rights reserved.

Tuning of platinum nano-particles by Au usage in their binary alloy for direct ethanol fuel cell: Controlled synthesis, electrode kinetics and mechanistic interpretation

NASA Astrophysics Data System (ADS)

Dutta, Abhijit; Mondal, Achintya; Datta, Jayati

2015-06-01

Understanding of the electrode-kinetics and mechanism of ethanol oxidation reaction (EOR) is of considerable interest for optimizing electro-catalysis in direct ethanol fuel cell (DEFC). This work attempts to design Pt based electro-catalyst on carbon support, tuned with gold nano-particles (NPs), for their use in DEFC operating in alkaline medium. The platinum-gold alloyed NPs are synthesized at desired compositions and size (2-10 nm) by controlled borohydride reduction method and successfully characterized by XRD, TEM, EDS and XPS techniques. The kinetic parameters along with the activation energies for the EOR are evaluated over the temperature range 20-80 °C and the oxidation reaction products estimated through ion chromatographic analysis. Compared to single Pt/C catalyst, the over potential of EOR is reduced by ca. 500 mV, at the onset during the reaction, for PtAu/C alloy with only 23% Pt content demonstrating the ability of Au and/or its surface oxides providing oxygen species at much lower potentials compared to Pt. Furthermore, a considerable increase in the peak power density (>191%) is observed in an in-house fabricated direct ethanol anion exchange membrane fuel cell, DE(AEM)FC using the best performing Au covered Pt electrode (23% Pt) compared to the monometallic Pt catalyst.

Fabrication of an electrochemical nanoaptasensor based on AuNPs for ultrasensitive determination of cocaine in serum sample.

PubMed

Roushani, Mahmoud; Shahdost-Fard, Faezeh

2016-04-01

Herein we describe an ultrasensitive electrochemical nanoaptasensor for the detection of one of the most dangerous narcotic drugs available, cocaine. The nanoaptasensor was constructed by the covalent attachment of a 5'-NH2-3'-gold nanoparticles terminated aptamer on the surface of a glassy carbon electrode which was deposited with gold nanoparticles (AuNPs/GCE). It is worth noting that the interaction of the cysteamine stable self-assembled monolayer on the AuNPs/GCE surface and the covalent attachment of terephthalaldehyde via amide coupling with the amine groups in the cysteamine and aptamer, respectively, resulted in the covalent attachment of the aptamer to AuNPs/GCE. The presence of gold nanoparticles both on surface of the glassy carbon electrode and in the end of the aptamer, can provide advantages such as increase of active surface area, high acceleration of the electron transfer and improved electrochemical signal, respectively. The decrease in the peak current of [Fe(CN)6](3-/4-) as the probe redox with increase of cocaine concentration, in differential pulse voltammetry as the measuring technique, from 5 pM up to 5 nM was linear and an unprecedented detection limit of 0.5pM was yielded. Furthermore, the effect of some common analgesic drugs as the potential interferents were investigated and also, to evaluate practical application of the proposed nanoaptasensor human blood serum sample as a real sample was used. Simple preparation, low operation cost, speed and validity are the decisive factors of this method motivating its application to biosensing investigation. Copyright © 2016 Elsevier B.V. All rights reserved.

Ethanol electrooxidation in alkaline medium on electrochemically synthesized Co(OH)2/Au composite

NASA Astrophysics Data System (ADS)

Babu, Sreejith P.; Elumalai, Perumal

2017-01-01

Gold (Au), cobalt hydroxide (Co(OH)2) and different Co(OH)2/Au compositions were electro-deposited onto stainless steel by a potentiodynamic method from the respective metal-ion solutions. The deposits were characterized by x-ray diffraction (XRD), scanning electron microscope (SEM) and Fourier transformed infra-red spectroscopy (FT-IR). The XRD and IR data confirmed that the deposits were Au, α-Co(OH)2 or Co(OH)2/Au composites. The SEM observations confirmed that the morphology of the Au was spherical, while the α-Co(OH)2 was flakey with pores. The morphology of the Co(OH)2/Au composites consisted of highly agglomerated Au grains distributed on the Co(OH)2 matrix. The electrocatalytic activity of each of the Au, Co(OH)2 and Co(OH)2/Au-composite electrodes towards ethanol electrooxidation in an alkaline medium was investigated by cyclic voltammetry and chronoamperometry. It turned out that the Co(OH)2/Au-composite electrodes exhibited superior catalytic activity for ethanol electrooxidation compared with the pristine Au or Co(OH)2 electrodes. A peak current density as high as 25 mA cm-2 was exhibited by the Co(OH)2/ Au composite while the Au and Co(OH)2 showed only 0.9 and 13 mA cm-2, respectively. The enhanced conductivity of the Co(OH)2/Au matrix due to the presence of Au, as well as the combined catalytic activity, seemed to be responsible for the superior performance of the Co(OH)2/Au-composite electrodes.

Electrochemical DNA sensor for Neisseria meningitidis detection.

PubMed

Patel, Manoj K; Solanki, Pratima R; Kumar, Ashok; Khare, Shashi; Gupta, Sunil; Malhotra, Bansi D

2010-08-15

Meningitis sensor based on nucleic acid probe of Neisseria meningitidis has been fabricated by immobilization of 5'-thiol end labeled single stranded deoxyribonucleic acid probe (ssDNA-SH) onto gold (Au) coated glass electrode. This ssDNA-SH/Au electrode hybridized with the genomic DNA (G-dsDNA/Au) and amplified DNA (PCR-dsDNA/Au) has been characterized using atomic force microscopy (AFM), Fourier transforms infrared spectroscopy (FT-IR) and electrochemical techniques. The ssDNA-SH/Au electrode can specifically detect upto 10-60 ng/microl of G-dsDNA-SH/Au and PCR-dsDNA-SH/Au of meningitis within 60s of hybridization time at 25 degrees C by cyclic voltammetry (CV) using methylene blue (MB) as electro-active DNA hybridization indicator. The values of sensitivities of the G-dsDNA-SH/Au and PCR-dsDNA-SH/Au electrodes have been determined as 0.0115 microA/ng cm(-2) and 0.0056 microA/ng cm(-2), respectively with regression coefficient (R) as 0.999. This DNA bioelectrode is stable for about 4 months when stored at 4 degrees C. Copyright 2010 Elsevier B.V. All rights reserved.

Green synthesis of gold nanoparticles for trace level detection of a hazardous pollutant (nitrobenzene) causing Methemoglobinaemia.

PubMed

Emmanuel, R; Karuppiah, Chelladurai; Chen, Shen-Ming; Palanisamy, Selvakumar; Padmavathy, S; Prakash, P

2014-08-30

The present study involves a green synthesis of gold nanoparticles (Au-NPs) using Acacia nilotica twig bark extract at room temperature and trace level detection of one of the hazardous materials, viz. nitrobenzene (NB) that causes Methemoglobinaemia. The synthesis protocol demonstrates that the bioreduction of chloroauric acid leads to the formation of Au-NPs within 10min, suggesting a higher reaction rate than any other chemical methods involved. The obtained Au-NPs have been characterized by UV-vis spectroscopy, X-ray diffraction, transmission electron microscopy, Energy-Dispersive X-ray Spectroscopy and Fourier Transform Infrared Spectroscopy. The electrochemical detection of NB has been investigated at the green synthesized Au-NPs modified glassy carbon electrode by using differential pulse voltammetry (DPV). The Au-NPs modified electrode exhibits excellent reduction ability toward NB compared to unmodified electrode. The developed NB sensor at Au-NPs modified electrode displays a wide linear response from 0.1 to 600μM with high sensitivity of 1.01μAμM(-1)cm(-2) and low limit of detection of 0.016μM. The modified electrode shows exceptional selectivity in the presence of ions, phenolic and biologically coactive compounds. In addition, the Au-NPs modified electrode exhibits an outstanding recovery results toward NB in various real water samples. Copyright © 2014 Elsevier B.V. All rights reserved.

Rhombic Coulomb diamonds in a single-electron transistor based on an Au nanoparticle chemically anchored at both ends.

PubMed

Azuma, Yasuo; Onuma, Yuto; Sakamoto, Masanori; Teranishi, Toshiharu; Majima, Yutaka

2016-02-28

Rhombic Coulomb diamonds are clearly observed in a chemically anchored Au nanoparticle single-electron transistor. The stability diagrams show stable Coulomb blockade phenomena and agree with the theoretical curve calculated using the orthodox model. The resistances and capacitances of the double-barrier tunneling junctions between the source electrode and the Au core (R1 and C1, respectively), and those between the Au core and the drain electrode (R2 and C2, respectively), are evaluated as 4.5 MΩ, 1.4 aF, 4.8 MΩ, and 1.3 aF, respectively. This is determined by fitting the theoretical curve against the experimental Coulomb staircases. Two-methylene-group short octanedithiols (C8S2) in a C8S2/hexanethiol (C6S) mixed self-assembled monolayer is concluded to chemically anchor the core of the Au nanoparticle at both ends between the electroless-Au-plated nanogap electrodes even when the Au nanoparticle is protected by decanethiol (C10S). This is because the R1 value is identical to that of R2 and corresponds to the tunneling resistances of the octanedithiol chemically bonded with the Au core and the Au electrodes. The dependence of the Coulomb diamond shapes on the tunneling resistance ratio (R1/R2) is also discussed, especially in the case of the rhombic Coulomb diamonds. Rhombic Coulomb diamonds result from chemical anchoring of the core of the Au nanoparticle at both ends between the electroless-Au-plated nanogap electrodes.

Electrochemical impedance immunosensor based on gold nanoparticles and aryl diazonium salt functionalized gold electrodes for the detection of antibody.

PubMed

Liu, Guozhen; Liu, Jingquan; Davis, Thomas P; Gooding, J Justin

2011-04-15

Electrodes modified with passivating organic layers have been shown to, here and previously, to exhibit good Faradaic electrochemistry upon attachment of gold nanoparticles (AuNP). Due to their low background capacitances these constructs have good potential in electrochemical sensing. Herein is reported the application of these electrode constructs for impedance based immunosensing. The immunosensor was constructed by modifying a gold electrode with 4-thiophenol (4-TP) passivating layers by diazonium salt chemistry. Subsequently, the attachment of AuNP and then a biotin derivative as a model epitope to detect anti-biotin IgG were carried out. The interfacial properties of the modified electrodes were evaluated in the presence of Fe(CN)(6)(4-/3-) redox couple as a probe by cyclic voltammetry and electrochemical impedance spectroscopy. The impedance change, due to the specific immuno-interaction at the immunosensor surface was utilized to detect anti-biotin IgG. The increase in charge-transfer resistance (R(ct)) was linearly proportional to the concentration of anti-biotin IgG in the range of 5-500 ng mL(-1), with a detection limit of 5 ng mL(-1). Copyright © 2011 Elsevier B.V. All rights reserved.

Novel electrochemical aptasensor for ultrasensitive detection of sulfadimidine based on covalently linked multi-walled carbon nanotubes and in situ synthesized gold nanoparticle composites.

PubMed

He, Baoshan; Du, Gengan

2018-05-01

In the current study, a sensitive electrochemical sensing strategy based on aptamer (APT) for detection of sulfadimidine (SM 2 ) was developed. A bare gold electrode (AuE) was first modified with 2-aminoethanethiol (2-AET) through self-assembly, used as linker for the subsequent immobilization of multi-walled carbon nanotubes and gold nanoparticle composites (MWCNTs/AuNPs). Then, the thiolated APT was assembled onto the electrode via sulfur-gold affinity. When SM 2 existed, the APT combined with SM 2 and formed a complex structure. The specific binding of SM 2 and APT increased the impedance, leading to hard electron transfer between the electrode surface and the redox probe [Fe(CN) 6 ] 3-/4- and producing a significant reduction of the signal. The SM 2 concentration could be reflected by the current difference of the peak currents before and after target binding. Under optimized conditions, the linear dynamic range is from 0.1 to 50 ng mL -1 , with a detection limit of 0.055 ng mL -1 . The sensor exhibited desirable selectivity against other sulfonamides and performs successfully when analyzing SM 2 in pork samples. Graphical abstract A new electrochemical biosensor for ultrasensitive detection of sulfadimidine (SM 2 ) by using a gold electrode modified with MWCNTs/AuNPs for signal amplification and aptamer (APT) for selectivity improvement.

Amperometric immunosensor for α-fetoprotein antigen in human serum based on co-immobilizing dinuclear copper complex and gold nanoparticle doped chitosan film

NASA Astrophysics Data System (ADS)

Gan, Ning; Meng, Ling Hua; Wang, Feng

2009-09-01

A sensitive amperometric immunosensor for α-fetoprotein (AFP), a tumor marker for the diagnosis of hepatocellular carcinoma (HCC), was constructed, The immunosensor is prepared by co-immobilizing [Cu2(phen)2Cl2] (μ-Cl)2 (CuL), nano-Au/Chitosan(Chit) composite, horseradish peroxidase (HRP) and AFP antibody(anti-AFP) on a glassy carbon electrode (GCE). Firstly, CuL was irreversibly absorb on GCE electrode through π-π stacking interaction; then nano-Au/Chit composite was immobilized onto the electrode because of its excellent membrane-forming ability, finally HRP and anti-AFP was adsorbed onto the surface of the gold nanoparticles to construct GCE | CuL/nanoAu-chit/HRP/anti-AFP immunosensor. The preparation procedure of the electrode was characterized by electrochemical and spectroscopy method. The results showed that this immunosensor exhibited an excellent electrocatalytic response to the reduction of hydrogen peroxide (H2O2) without the aid of an electron mediator, offers a high-sensitivity (1710 nA · ng-1 · ml-1) for the detection of AFP and has good correlation for detection of AFP in the range of 0.2 to 120.0 ng/ml with a detection limit of 0.05 ng/ml. The biosensor showed high selectivity as well as good stability and reproductivity.

A non-enzymatic sensor for hydrogen peroxide based on polyaniline, multiwalled carbon nanotubes and gold nanoparticles modified Au electrode.

PubMed

Narang, Jagriti; Chauhan, Nidhi; Pundir, C S

2011-11-07

We describe the construction of a polyaniline (PANI), multiwalled carbon nanotubes (MWCNTs) and gold nanoparticles (AuNPs) modified Au electrode for determination of hydrogen peroxide without using peroxidase (HRP). The AuNPs/MWCNT/PANI composite film deposited on Au electrode was characterized by Scanning Electron Microscopy (SEM) and electrochemical methods. Cyclic voltammetric (CV) studies of the electrode at different stages of construction demonstrated that the modified electrode had enhanced electrochemical oxidation of H(2)O(2), which offers a number of attractive features to develop amperometric sensors based on split of H(2)O(2). The amperometric response to H(2)O(2) showed a linear relationship in the range from 3.0 μM to 600.0 μM with a detection limit of 0.3 μM (S/N = 3) and with high sensitivity of 3.3 mA μM(-1). The sensor gave accurate and satisfactory results, when employed for determination of H(2)O(2) in milk and urine.

Enhanced performance of a glucose/O(2) biofuel cell assembled with laccase-covalently immobilized three-dimensional macroporous gold film-based biocathode and bacterial surface displayed glucose dehydrogenase-based bioanode.

PubMed

Hou, Chuantao; Yang, Dapeng; Liang, Bo; Liu, Aihua

2014-06-17

The power output and stability of enzyme-based biofuel cells (BFCs) is greatly dependent on the properties of both the biocathode and bioanode, which may be adapted for portable power production. In this paper, a novel highly uniform three-dimensional (3D) macroporous gold (MP-Au) film was prepared by heating the gold "supraspheres", which were synthesized by a bottom-up protein templating approach, and followed by modification of laccase on the MP-Au film by covalent immobilization. The as-prepared laccase/MP-Au biocathode exihibited an onset potential of 0.62 V versus saturated calomel electrode (SCE, or 0.86 V vs NHE, normal hydrogen electrode) toward O2 reduction and a high catalytic current of 0.61 mAcm(-2). On the other hand, mutated glucose dehydrogenase (GDH) surface displayed bacteria (GDH-bacteria) were used to improve the stability of the glucose oxidation at the bioanode. The as-assembled membraneless glucose/O2 fuel cell showed a high power output of 55.8 ± 2.0 μW cm(-2) and open circuit potential of 0.80 V, contributing to the improved electrocatalysis toward O2 reduction at the laccase/MP-Au biocathode. Moreover, the BFC retained 84% of its maximal power density even after continuous operation for 55 h because of the high stability of the bacterial surface displayed GDH mutant toward glucose oxidation. Our findings may be promising for the development of more efficient glucose BFC for portable battery or self-powered device applications.

Electroless deposition of Au nanoparticles on reduced graphene oxide/polyimide film for electrochemical detection of hydroquinone and catechol

NASA Astrophysics Data System (ADS)

Shen, Xuan; Xia, Xiaohong; Du, Yongling; Wang, Chunming

2017-09-01

An electrochemical sensor for determination of hydroquinone (HQ) and catechol (CC) was developed using Au nanoparticles (AuNPs) fabricated on reduced graphene oxide/polyimide (PI/RGO) film by electroless deposition. The electrochemical behaviors of HQ and CC at PI/RGO-AuNPs electrode were investigated by cyclic voltammetry (CV) and differential pulse voltammetry (DPV). Under the optimized condition, the current responses at PI/RGO-AuNPs electrode were linear over ranges from 1 to 654 mol/L for HQ and from 2 to 1289 mol/L for CC, with the detection limits of 0.09 and 0.2 mol/L, respectively. The proposed electrode exhibited good reproducibility, stability and selectivity. In addition, the proposed electrode was successfully applied in the determination of HQ and CC in tap water and the Yellow River samples.

Crystallographic orientation and electrode nature are key factors for electric current generation by Geobacter sulfurreducens.

PubMed

Maestro, Beatriz; Ortiz, Juan M; Schrott, Germán; Busalmen, Juan P; Climent, Víctor; Feliu, Juan M

2014-08-01

We have investigated the influence of electrode material and crystallographic structure on electron transfer and biofilm formation of Geobacter sulfurreducens. Single-crystal gold-Au(110), Au(111), Au(210)-and platinum-Pt(100), Pt(110), Pt(111), Pt(210)-electrodes were tested and compared to graphite rods. G. sulfurreducens electrochemically interacts with all these materials with different attachment kinetics and final current production, although redox species involved in the electron transfer to the anode are virtually the same in all cases. Initial bacterial colonization was fastest on graphite up to the monolayer level, whereas gold electrodes led to higher final current densities. Crystal geometry was shown to have an important influence, with Au(210) sustaining a current density of up to 1442±101μAcm(-2) at the steady state, over Au(111) with 961±94μAcm(-2) and Au(110) with 944±89μAcm(-2). On the other hand, the platinum electrodes displayed the lowest performances, including Pt(210). Our results indicate that both crystal geometry and electrode material are key parameters for the efficient interaction of bacteria with the substrate and should be considered for the design of novel materials and microbial devices to optimize energy production. Copyright © 2014 Elsevier B.V. All rights reserved.

Dithiocarbamate Self-Assembled Monolayers as Efficient Surface Modifiers for Low Work Function Noble Metals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Meyer, Dominik; Schäfer, Tobias; Schulz, Philip

2016-09-06

Tuning the work function of the electrode is one of the crucial steps to improve charge extraction in organic electronic devices. Here, we show that N,N-dialkyl dithiocarbamates (DTC) can be effectively employed to produce low work function noble metal electrodes. Work functions between 3.1 and 3.5 eV are observed for all metals investigated (Cu, Ag, and Au). Ultraviolet photoemission spectroscopy (UPS) reveals a maximum decrease in work function by 2.1 eV as compared to the bare metal surface. Electronic structure calculations elucidate how the complex interplay between intrinsic dipoles and dipoles induced by bond formation generates such large work functionmore » shifts. Subsequently, we quantify the improvement in contact resistance of organic thin film transistor devices with DTC coated source and drain electrodes. These findings demonstrate that DTC molecules can be employed as universal surface modifiers to produce stable electrodes for electron injection in high performance hybrid organic optoelectronics.« less

Effect of dissolved LiCl on the ionic liquid-Au(111) interface: an in situ STM study

NASA Astrophysics Data System (ADS)

Borisenko, Natalia; Atkin, Rob; Lahiri, Abhishek; Zein El Abedin, Sherif; Endres, Frank

2014-07-01

The structure of the electrolyte/electrode interface plays a significant role in electrochemical processes. To date, most studies are focusing on understanding the interfacial structure in pure ionic liquids. In this paper in situ scanning tunnelling microscopy (STM) has been employed to elucidate the structure of the charged Au(111)-ionic liquid (1-butyl-1-methylpyrrolidinium tris(pentafluoroethyl)trifluorophosphate, [Py1,4]FAP) interface in the presence of 0.1 M LiCl. The addition of the Li salt to the ionic liquid has a strong influence on the interfacial structure. In the first STM scan in situ measurements reveal that Au(111) undergoes the (22 \\times \\surd 3) ‘herringbone’ reconstruction in a certain potential regime, and there is strong evidence that the gold surface dissolves at negative electrode potentials in [Py1,4]FAP containing LiCl. Bulk deposition of Li is obtained at -2.9 V in the second STM scan.

In vitro extracellular recording and stimulation performance of nanoporous gold-modified multi-electrode arrays.

PubMed

Kim, Yong Hee; Kim, Gook Hwa; Kim, Ah Young; Han, Young Hwan; Chung, Myung-Ae; Jung, Sang-Don

2015-12-01

Nanoporous gold (Au) structures can reduce the impedance and enhance the charge injection capability of multi-electrode arrays (MEAs) used for interfacing neuronal networks. Even though there are various nanoporous Au preparation techniques, fabrication of MEA based on low-cost electro-codeposition of Ag:Au has not been performed. In this work, we have modified a Au MEA via the electro-codeposition of Ag:Au alloy, followed by the chemical etching of Ag, and report on the in vitro extracellular recording and stimulation performance of the nanoporous Au-modified MEA. Ag:Au alloy was electro-codeposited on a bilayer lift-off resist sputter-deposition passivated Au MEA followed by chemical etching of Ag to form a porous Au structure. The porous Au structure was analyzed by scanning electron microscopy and tunneling electron microscopy and found to have an interconnected nanoporous Au structure. The impedance value of the nanoporous Au-modified MEA is 15.4 ± 0.55 kΩ at 1 kHz, accompanied by the base noise V rms of 2.4 ± 0.3 μV. The charge injection limit of the nanoporous Au-modified electrode estimated from voltage transient measurement is approximately 1 mC cm(-2), which is comparable to roughened platinum and carbon nanotube electrodes. The charge injection capability of the nanoporous Au-modified MEA was confirmed by observing stimulus-induced spikes at above 0.2 V. The nanoporous Au-modified MEA showed mechanical durability upon ultrasonic treatment for up to an hour. Electro-codeposition of Ag:Au alloy combined with chemical etching Ag is a low-cost process for fabricating nanoporous Au-modified MEA suitable for establishing the stimulus-response relationship of cultured neuronal networks.

In vitro extracellular recording and stimulation performance of nanoporous gold-modified multi-electrode arrays

NASA Astrophysics Data System (ADS)

Kim, Yong Hee; Kim, Gook Hwa; Kim, Ah Young; Han, Young Hwan; Chung, Myung-Ae; Jung, Sang-Don

2015-12-01

Objective. Nanoporous gold (Au) structures can reduce the impedance and enhance the charge injection capability of multi-electrode arrays (MEAs) used for interfacing neuronal networks. Even though there are various nanoporous Au preparation techniques, fabrication of MEA based on low-cost electro-codeposition of Ag:Au has not been performed. In this work, we have modified a Au MEA via the electro-codeposition of Ag:Au alloy, followed by the chemical etching of Ag, and report on the in vitro extracellular recording and stimulation performance of the nanoporous Au-modified MEA. Approach. Ag:Au alloy was electro-codeposited on a bilayer lift-off resist sputter-deposition passivated Au MEA followed by chemical etching of Ag to form a porous Au structure. Main results. The porous Au structure was analyzed by scanning electron microscopy and tunneling electron microscopy and found to have an interconnected nanoporous Au structure. The impedance value of the nanoporous Au-modified MEA is 15.4 ± 0.55 kΩ at 1 kHz, accompanied by the base noise V rms of 2.4 ± 0.3 μV. The charge injection limit of the nanoporous Au-modified electrode estimated from voltage transient measurement is approximately 1 mC cm-2, which is comparable to roughened platinum and carbon nanotube electrodes. The charge injection capability of the nanoporous Au-modified MEA was confirmed by observing stimulus-induced spikes at above 0.2 V. The nanoporous Au-modified MEA showed mechanical durability upon ultrasonic treatment for up to an hour. Significance. Electro-codeposition of Ag:Au alloy combined with chemical etching Ag is a low-cost process for fabricating nanoporous Au-modified MEA suitable for establishing the stimulus-response relationship of cultured neuronal networks.

Chitosan coated on the layers' glucose oxidase immobilized on cysteamine/Au electrode for use as glucose biosensor.

PubMed

Zhang, Yawen; Li, Yunqiu; Wu, Wenjian; Jiang, Yuren; Hu, Biru

2014-10-15

A glucose biosensor was developed via direct immobilization of glucose oxidase (GOD) by self-assembled cysteamine monolayer on Au electrode surface followed by coating chitosan on the surface of electrode. In this work, chitosan film was coated on the surface of GOD as a protection film to ensure the stability and biocompatibility of the constructed glucose biosensor. The different application ranges of sensors were fabricated by immobilizing varied layers of GOD. The modified surface film was characterized by a scanning electron microscope (SEM) and the fabrication process of the biosensor was confirmed through electrochemical impedance spectroscopy (EIS) of ferrocyanide. The performance of cyclic voltammetry (CV) in the absence and presence of 25 mM glucose and ferrocenemethanol showed a diffusion-controlled electrode process and reflected the different maximum currents between the different GOD layers. With the developed glucose biosensor, the detection limits of the two linear responses are 49.96 μM and 316.8 μM with the sensitivities of 8.91 μA mM(-1)cm(-2) and 2.93 μA mM(-1)cm(-2), respectively. In addition, good stability (up to 30 days) of the developed biosensor was observed. The advantages of this new method for sensors construction was convenient and different width ranges of detection can be obtained by modified varied layers of GOD. The sensor with two layers of enzyme displayed two current linear responses of glucose. The present work provided a simplicity and novelty method for producing biosensors, which may help design enzyme reactors and biosensors in the future. Copyright © 2014 Elsevier B.V. All rights reserved.

Diamond nanoparticles as a way to improve electron transfer in sol-gel L-lactate biosensing platforms.

PubMed

Briones, M; Casero, E; Vázquez, L; Pariente, F; Lorenzo, E; Petit-Domínguez, M D

2016-02-18

In the present work, we have included for the first time diamond nanoparticles (DNPs) in a sol-gel matrix derived from (3-mercaptopropyl)-trimethoxysilane (MPTS) in order to improve electron transfer in a lactate oxidase (LOx) based electrochemical biosensing platform. Firstly, an exhaustive AFM study, including topographical, surface potential (KFM) and capacitance gradient (CG) measurements, of each step involved in the biosensing platform development was performed. The platform is based on gold electrodes (Au) modified with the sol-gel matrix (Au/MPTS) in which diamond nanoparticles (Au/MPTS/DNPs) and lactate oxidase (Au/MPTS/DNPs/LOx) have been included. For the sake of comparison, we have also characterized a gold electrode directly modified with DNPs (Au/DNPs). Secondly, the electrochemical behavior of a redox mediator (hydroxymethyl-ferrocene, HMF) was evaluated at the platforms mentioned above. The response of Au/MPTS/DNPs/LOx towards lactate was obtained. A linear concentration range from 0.053 mM to 1.6 mM, a sensitivity of 2.6 μA mM(-1) and a detection limit of 16 μM were obtained. These analytical properties are comparable to other biosensors, presenting also as advantages that DNPs are inexpensive, environment-friendly and easy-handled nanomaterials. Finally, the developed biosensor was applied for lactate determination in wine samples. Copyright © 2016 Elsevier B.V. All rights reserved.

Nanoporous Au-based chronocoulometric aptasensor for amplified detection of Pb(2+) using DNAzyme modified with Au nanoparticles.

PubMed

Zhang, Chen; Lai, Cui; Zeng, Guangming; Huang, Danlian; Tang, Lin; Yang, Chunping; Zhou, Yaoyu; Qin, Lei; Cheng, Min

2016-07-15

The authors herein described an amplified detection strategy employing nanoporous Au (NPG) and gold nanoparticles (AuNPs) to detect Pb(2+) ions in aqueous solution. The thiol modified Pb(2+)-specific DNAzyme was self-assembled onto the surface of the NPG modified electrode for hybridizing with the AuNPs labeled oligonucleotide and for forming the DNA double helix structure. Electrochemical signal, redox charge of hexaammineruthenium(III) chloride (RuHex), was measured by chronocoulometry. Taking advantage of amplification effects of the NPG electrode for increasing the reaction sites of capture probe and DNA-AuNPs complexes for bringing about the adsorption of large numbers of RuHex molecules, this electrochemical sensor could detect Pb(2+) quantitatively, in the range of 0.05-100nM, with a limit of detection as low as 0.012nM. Selectivity measurements revealed that the sensor was specific for Pb(2+) even with interference by high concentrations of other metal ions. This sensor was also used to detect Pb(2+) ions from samples of tap water, river water, and landfill leachate samples spiked with Pb(2+) ions, and the results showed good agreement with the found values determined by an atomic fluorescence spectrometer. This simple aptasensor represented a promising potential for on-site detecting Pb(2+) in drinking water. Copyright © 2016 Elsevier B.V. All rights reserved.

Selective Electrocatalytic Degradation of Odorous Mercaptans Derived from S-Au Bond Recongnition on a Dendritic Gold/Boron-Doped Diamond Composite Electrode.

PubMed

Chai, Shouning; Wang, Yujing; Zhang, Ya-Nan; Liu, Meichuan; Wang, Yanbin; Zhao, Guohua

2017-07-18

To improve selectivity of electrocatalytic degradation of toxic, odorous mercaptans, the fractal-structured dendritic Au/BDD (boron-doped diamond) anode with molecular recognition is fabricated through a facile replacement method. SEM and TEM characterizations show that the gold dendrites are single crystals and have high population of the Au (111) facet. The distinctive structure endows the electrode with advantages of low resistivity, high active surface area, and prominent electrocatalytic activity. To evaluate selectivity, the dendritic Au/BDD is applied in degrading two groups of synthetic wastewater containing thiophenol/2-mercaptobenzimidazole (targets) and phenol/2-hydroxybenzimidazole (interferences), respectively. Results show that targets removals reach 91%/94%, while interferences removals are only 58%/48% in a short time. The corresponding degradation kinetic constants of targets are 3.25 times and 4.1 times that of interferences in the same group, demonstrating modification of dendritic gold on BDD could effectively enhance electrocatalytic target-selectivity. XPS and EXAFS further reveal that the selective electrocatalytic degradation derives from preferential recognition and fast adsorption to thiophenol depending on strong Au-S bond. The efficient, selective degradation is attributed to the synergetic effects between accumulative behavior and outstanding electrochemical performances. This work provides a new strategy for selective electrochemical degradation of contaminants for actual wastewater treatment.

An ultra-sensitive Au nanoparticles functionalized DNA biosensor for electrochemical sensing of mercury ions.

PubMed

Zhang, Yanyan; Zhang, Cong; Ma, Rui; Du, Xin; Dong, Wenhao; Chen, Yuan; Chen, Qiang

2017-06-01

The present work describes an effective strategy to fabricate a highly sensitive and selective DNA-biosensor for the determination of mercury ions (Hg 2+ ). The DNA 1 was modified onto the surface of Au electrode by the interaction between sulfydryl group and Au electrode. DNA probe is complementary with DNA 1. In the presence of Hg 2+ , the electrochemical signal increases owing to that Hg 2+ -mediated thymine bases induce the conformation of DNA probe to change from line to hairpin and less DNA probes adsorb into DNA 1. Taking advantage of its reduction property, methylene blue is considered as the signal indicating molecule. For improving the sensitivity of the biosensor, Au nanoparticles (Au NPs) modified reporter DNA 3 is used to adsorb DNA 1. Electrochemical behaviors of the biosensor were evaluated by electrochemical impedance spectroscopy and cyclic voltammetry. Several important parameters which could affect the property of the biosensor were studied and optimized. Under the optimal conditions, the biosensor exhibits wide linear range, high sensitivity and low detection limit. Besides, it displays superior selectivity and excellent stability. The biosensor was also applied for water sample detection with satisfactory result. The novel strategy of fabricating biosensor provides a potential platform for fabricating a variety of metal ions biosensors. Copyright © 2017 Elsevier B.V. All rights reserved.

Synergetic enhancement of gold nanoparticles and 2-mercaptobenzothiazole as highly-sensitive sensing strategy for tetrabromobisphenol A

NASA Astrophysics Data System (ADS)

Chen, Xuerong; Ji, Liudi; Zhou, Yikai; Wu, Kangbing

2016-05-01

Various gold nanoparticles (AuNPs) were in-situ prepared on the electrode surface through electrochemical reduction under different potentials such as -0.60, -0.50, -0.40, -0.30 and -0.20 V. The reduction potentials heavily affect the surface morphology and electrochemical activity of AuNPs such as effective area and catalytic ability, as confirmed using atomic force microscopy and electrochemical impedance spectroscopy. The electrochemical behaviors of tetrabromobisphenol A (TBBPA), a widely-existed pollutant with severe adverse health effects, were studied. The oxidation activity of TBBPA enhances obviously on the surface of AuNPs, and the signal improvements of TBBPA show difference on the prepared AuNPs. Interestingly, the existence of 2-mercaptobenzothiazole (MBT) further improves the oxidation signals of TBBPA on AuNPs. The synergetic enhancement effects of AuNPs and MBT were studied using cyclic voltammetry and chronocoulometry. The numerous nano-scaled gold particles together with the strong hydrophobic interaction between TBBPA and the assembled MBT on AuNPs jointly provide highly-effective accumulation for TBBPA. As a result, a sensitive and simple electrochemical method was developed for the direct determination of TBBPA, with detection limit of 0.12 μg L-1 (0.22 nM). The practical applications in water samples manifest that this new sensing system is accurate and feasible.

Electric-field noise from carbon-adatom diffusion on a Au(110) surface: First-principles calculations and experiments

NASA Astrophysics Data System (ADS)

Kim, E.; Safavi-Naini, A.; Hite, D. A.; McKay, K. S.; Pappas, D. P.; Weck, P. F.; Sadeghpour, H. R.

2017-03-01

The decoherence of trapped-ion quantum gates due to heating of their motional modes is a fundamental science and engineering problem. This heating is attributed to electric-field noise arising from the trap-electrode surfaces. In this work, we investigate the source of this noise by focusing on the diffusion of carbon-containing adsorbates on the surface of Au(110). We show by density functional theory, based on detailed scanning probe microscopy, how the carbon adatom diffusion on the gold surface changes the energy landscape and how the adatom dipole moment varies with the diffusive motion. A simple model for the diffusion noise, which varies quadratically with the variation of the dipole moment, predicts a noise spectrum, in accordance with the measured values.

Development of a Sensitive Electrochemical Enzymatic Reaction-Based Cholesterol Biosensor Using Nano-Sized Carbon Interdigitated Electrodes Decorated with Gold Nanoparticles

PubMed Central

Sharma, Deepti; Lee, Jongmin; Seo, Junyoung; Shin, Heungjoo

2017-01-01

We developed a versatile and highly sensitive biosensor platform. The platform is based on electrochemical-enzymatic redox cycling induced by selective enzyme immobilization on nano-sized carbon interdigitated electrodes (IDEs) decorated with gold nanoparticles (AuNPs). Without resorting to sophisticated nanofabrication technologies, we used batch wafer-level carbon microelectromechanical systems (C-MEMS) processes to fabricate 3D carbon IDEs reproducibly, simply, and cost effectively. In addition, AuNPs were selectively electrodeposited on specific carbon nanoelectrodes; the high surface-to-volume ratio and fast electron transfer ability of AuNPs enhanced the electrochemical signal across these carbon IDEs. Gold nanoparticle characteristics such as size and morphology were reproducibly controlled by modulating the step-potential and time period in the electrodeposition processes. To detect cholesterol selectively using AuNP/carbon IDEs, cholesterol oxidase (ChOx) was selectively immobilized via the electrochemical reduction of the diazonium cation. The sensitivity of the AuNP/carbon IDE-based biosensor was ensured by efficient amplification of the redox mediators, ferricyanide and ferrocyanide, between selectively immobilized enzyme sites and both of the combs of AuNP/carbon IDEs. The presented AuNP/carbon IDE-based cholesterol biosensor exhibited a wide sensing range (0.005–10 mM) and high sensitivity (~993.91 µA mM−1 cm−2; limit of detection (LOD) ~1.28 µM). In addition, the proposed cholesterol biosensor was found to be highly selective for the cholesterol detection. PMID:28914766

Heparin molecularly imprinted polymer thin flm on gold electrode by plasma-induced graft polymerization for label-free biosensor.

PubMed

Orihara, Kouhei; Hikichi, Atsushi; Arita, Tomohiko; Muguruma, Hitoshi; Yoshimi, Yasuo

2018-03-20

Heparin, a highly sulfated glycosaminoglycan, is an important biomaterial having biological and therapeutic functionalities such as anticoagulation, regeneration, and protein stabilization. This study addresses a label-free quartz crystal microbalance (QCM) biosensor for heparin detection based on a macromolecularly imprinted polymer (MIP) as an artificial recognition element. We demonstrate the novel strategy for MIP in the form of thin film on a gold (Au) electrode with the plasma-induced graft polymerization (PIP) technique. The procedure of PIP is as follows: (i) Hexamethyldisiloxane plasma-polymerized thin film (PPF) as a pre-coating scaffold of active species for PIP (post-polymerization) is deposited on an Au electrode. (ii) The PPF/Au electrode is soaked in an water solution containing heparin (template), (2-(methacryloxy)-ethyl)trimethylammonium chloride acrylamide (functional monomer), acrylamide, and N,N-methylenebisacrylamide (crosslinker). Double bonds of monomer and crosslinker attacked by residually active species in pre-coating PPF cause radical chain reaction. Consequently, a growing polymer network of 20 nm thickness of PIP-MIP thin film is formed and grafted on the PPF/Au surface. (iii) The PIP-MIP/PPF/Au is washed by sodium chloride solution so as to remove the template. Non-imprinted polymer (NIP) is carried out like the same procedure without a template. The AFM, XPS, and QCM measurements show that the PIP process facilitates macromolecularly surface imprinting of template heparin where the template is easily removed and is rapidly rebound to PIP-MIP without a diffusional barrier. The heparin-PIP-MIP specifically binds to heparin compared with heparin analog chondroitin sulfate C (selective factor: 4.0) and a detectable range of heparin in the presence of CS (0.1 wt%) was 0.001-0.1 wt%. The PIP-NIP does not show selectivity between them. The evaluated binding kinetics are association (k a  = 350 ± 100 M -1  s -1 ), dissociation (k d  = (5.0 ± 2.0) × 10 -4  s -1 ), and binding (K D  = 1.3 ± 0.6 μM) constants, demonstrating that the PIP-MIP as a synthetic antibody can be applied to analytical chemistry. Copyright © 2018 Elsevier B.V. All rights reserved.

Gold nanoparticle decorated multi-walled carbon nanotubes as counter electrode for dye sensitized solar cells.

PubMed

Kaniyoor, Adarsh; Ramaprabhu, Sundara

2012-11-01

A novel counter electrode material for dye sensitized solar cells (DSSCs) composed of nanostructured Au particles decorated on functionalized multi-walled carbon nanotubes (f-MWNTs) is demonstrated for the first time. MWNTs synthesized by catalytic chemical vapor deposition technique are purified and functionalized by treating with concentrated acids. Au nanoparticles are decorated on f-MWNTs by a rapid and facile microwave assisted polyol reduction method. The materials are characterized by X-ray diffractometry, Fourier transform infra red spectroscopy and electron microscopy. The DSSC fabricated with Au/f-MWNTs based counter electrode shows enhanced power conversion efficiency (eta) of 4.9% under AM 1.5G simulated solar radiation. In comparison, the reference DSSCs fabricated with f-MWNTs and Pt counter electrodes show eta of 2.1% and 4.5%. This high performance of Au/f-MWNTs counter electrode is investigated using electrochemical impedance spectroscopy and cyclic voltammetry studies.

Spray-painted binder-free SnSe electrodes for high-performance energy-storage devices.

PubMed

Wang, Xianfu; Liu, Bin; Xiang, Qingyi; Wang, Qiufan; Hou, Xiaojuan; Chen, Di; Shen, Guozhen

2014-01-01

SnSe nanocrystal electrodes on three-dimensional (3D) carbon fabric and Au-coated polyethylene terephthalate (PET) wafer have been prepared by a simple spray-painting process and were further investigated as binder-free active-electrodes for Lithium-ion batteries (LIBs) and flexible stacked all-solid-state supercapacitors. The as-painted SnSe nanocrystals/carbon fabric electrodes exhibit an outstanding capacity of 676 mAh g(-1) after 80 cycles at a current density of 200 mA g(-1) and a considerable high-rate capability in lithium storage because of the excellent ion transport from the electrolyte to the active materials and the efficient charge transport between current collector and electrode materials. The binder-free electrodes also provide a larger electrochemical active surface compared with electrodes containing binders, which leads to the enhanced capacities of energy-storage devices. A flexible stacked all-solid-state supercapacitor based on the SnSe nanocrystals on Au-coated PET wafers shows high capacitance reversibility with little performance degradation at different current densities after 2200 charge-discharge cycles and even when bent. This allows for many potential applications in facile, cost-effective, spray-paintable, and flexible energy-storage devices. The results indicate that the fabrication of binder-free electrodes by a spray painting process is an interesting direction for the preparation of high-performance energy-storage devices. Copyright © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A multifunctional hemin@metal-organic framework and its application to construct an electrochemical aptasensor for thrombin detection

NASA Astrophysics Data System (ADS)

Xie, Shunbi; Ye, Jiawei; Yuan, Yali; Chai, Yaqin; Yuan, Ruo

2015-10-01

A new type of multifunctional metal-organic framework (MOF) has been synthesized by encapsulating hemin into the nano-sized Fe-MIL-88 MOFs (hemin@MOFs) and first applied in an electrochemical aptasensor to detect thrombin (TB) with the aid of an enzyme for signal amplification. The gold nanoparticle functionalized hemin@MOFs (Au/hemin@MOFs) have not only simultaneously served as redox mediators and solid electrocatalysts, but have also been utilized as an ideal loading platform to immobilize a large number of biomolecules. In this aptasensor, Au/hemin@MOFs conjugated with glucose oxidase (GOD) and thrombin binding aptamer (TBA II) were used as the secondary aptamer bioconjugates (Au/hemin@MOF-TBA II-GOD bioconjugates), and TB was sandwiched between Au/hemin@MOF-TBA II-GOD bioconjugates and the amino-terminated TBA I which was self-assembled on the gold nanoparticle (AuNP) modified electrode. The GOD could oxidize glucose into gluconic acid accompanied by the generation of H2O2. The generated H2O2 on the electrode surface was further electrocatalyzed by hemin@MOFs to amplify the electrochemical signal of hemin contained in hemin@MOFs. Therefore, the synthesized hemin@MOFs represented a new paradigm for multifunctional materials since it combined three different functions including serving as catalysts, redox mediators and loading platforms within a single material. With such an ingenious design, a wide linear range of 0.0001 nM to 30 nM was acquired with a relatively low detection limit of 0.068 pM for TB detection.A new type of multifunctional metal-organic framework (MOF) has been synthesized by encapsulating hemin into the nano-sized Fe-MIL-88 MOFs (hemin@MOFs) and first applied in an electrochemical aptasensor to detect thrombin (TB) with the aid of an enzyme for signal amplification. The gold nanoparticle functionalized hemin@MOFs (Au/hemin@MOFs) have not only simultaneously served as redox mediators and solid electrocatalysts, but have also been utilized as an ideal loading platform to immobilize a large number of biomolecules. In this aptasensor, Au/hemin@MOFs conjugated with glucose oxidase (GOD) and thrombin binding aptamer (TBA II) were used as the secondary aptamer bioconjugates (Au/hemin@MOF-TBA II-GOD bioconjugates), and TB was sandwiched between Au/hemin@MOF-TBA II-GOD bioconjugates and the amino-terminated TBA I which was self-assembled on the gold nanoparticle (AuNP) modified electrode. The GOD could oxidize glucose into gluconic acid accompanied by the generation of H2O2. The generated H2O2 on the electrode surface was further electrocatalyzed by hemin@MOFs to amplify the electrochemical signal of hemin contained in hemin@MOFs. Therefore, the synthesized hemin@MOFs represented a new paradigm for multifunctional materials since it combined three different functions including serving as catalysts, redox mediators and loading platforms within a single material. With such an ingenious design, a wide linear range of 0.0001 nM to 30 nM was acquired with a relatively low detection limit of 0.068 pM for TB detection. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr04532k

Ultra-sensitive film sensor based on Al2O3-Au nanoparticles supported on PDDA-functionalized graphene for the determination of acetaminophen.

PubMed

Li, Jianbo; Sun, Weiyan; Wang, Xiaojiao; Duan, Huimin; Wang, Yanhui; Sun, Yuanling; Ding, Chaofan; Luo, Chuannan

2016-08-01

An electrochemical sensor of acetaminophen based on poly(diallyldimethylammonium chloride) (PDDA)-functionalized reduced graphene-loaded Al2O3-Au nanoparticles coated onto glassy carbon electrode (Al2O3-Au/PDDA/reduced graphene oxide (rGO)/glass carbon electrode (GCE)) were prepared by layer self-assembly technique. The as-prepared electrode-modified materials were characterized by scanning electron microscopy, X-ray powder diffraction, and Fourier transform infrared spectroscopy. The electrocatalytic performances of Al2O3-Au/PDDA/rGO-modified glassy carbon electrode toward the acetaminophen were investigated by cyclic voltammetry and differential pulse voltammetry. The modified electrodes of graphene oxide (GO)/GCE, PDDA/rGO/GCE, and Al2O3-Au/PDDA/rGO/GCE were constructed for comparison and learning the catalytic mechanism. The research showed Al2O3-Au/PDDA/rGO/GCE having good electrochemical performance, attributing to the synergetic effect that comes from the special nanocomposite structure and physicochemical properties of Al2O3-Au nanoparticles and graphene. A low detection limit of 6 nM (S/N = 3) and a wide linear detection range from 0.02 to 200 μM (R (2) = 0.9970) was obtained. The preparation of sensor was successfully applied for the detection of acetaminophen in commercial pharmaceutical pills. Graphical abstract Schematic diagram of synthesis of Al2O3-Au/PDDA/rGO/GCE.

Sensing CA 15-3 in point-of-care by electropolymerizing O-phenylenediamine (oPDA) on Au-screen printed electrodes.

PubMed

Gomes, Rui S; Moreira, Felismina T C; Fernandes, Ruben; Sales, M Goreti F

2018-01-01

This work presents an alternative device for cancer screening in liquid biopsies. It combines a biomimetic film (i) with electrochemical detection (ii). The biomimetic film (i) was obtained by electro-polymerizing amine-substituted benzene rings around a CA 15-3 target. This protein target was previously adsorbed on a gold (Au) support and incubated in charged monomers (4-Styrenesulfonate sodium and 3-Hydroxytyraminium chloride). The protein was further eliminated by enzymatic activity, leaving behind vacant sites for subsequent rebinding. Electrochemical detection (ii) was achieved on an Au working electrode, designed on commercial screen-printed electrodes. Raman spectroscopy, atomic force microscopy and ellipsometric readings were used to follow the chemical modification of the Au surface. The ability of the material to rebind CA15-3 was monitored by electrochemical techniques. The device displayed linear responses to CA15-3 ranging from 0.25 to 10.00 U/mL, with detection limits of 0.05 U/mL. Accurate results were obtained by applying the sensor to the analysis of CA15-3 in PBS buffer and in serum samples. This biosensing device displayed successful features for the detection of CA 15-3 and constitutes a promising tool for breast cancer screening procedures in point-of-care applications. Moreover, its scale-up seems feasible as it contains a plastic antibody assembled in situ, in less than 1 minute, and the analysis of serum takes less than 30 minutes.

Electrochemical sensor based on gold nanoparticles fabricated molecularly imprinted polymer film at chitosan-platinum nanoparticles/graphene-gold nanoparticles double nanocomposites modified electrode for detection of erythromycin.

PubMed

Lian, Wenjing; Liu, Su; Yu, Jinghua; Xing, Xianrong; Li, Jie; Cui, Min; Huang, Jiadong

2012-01-01

A molecularly imprinted electrochemical sensor was fabricated based on gold electrode decorated by chitosan-platinum nanoparticles (CS-PtNPs) and graphene-gold nanoparticles (GR-AuNPs) nanocomposites for convenient and sensitive determination of erythromycin. The synergistic effects of CS-PtNPs and GR-AuNPs nanocomposites improved the electrochemical response and the sensitivity of the sensor. The molecularly imprinted polymers (MIPs) were prepared by HAuCl(4), 2-mercaptonicotinic acid (MNA) and erythromycin. Erythromycin and MNA were used as template molecule and functional monomer, respectively. They were first assembled on the surface of GR-AuNPs/CS-PtNPs/gold electrode by the formation of Au-S bonds and hydrogen-bonding interactions. Then the MIPs were formed by electropolymerization of HAuCl(4), MNA and erythromycin. The sensor was characterized by cyclic voltammetry (CV), scanning electron microscope (SEM), UV-visible (UV-vis) absorption speactra and amperometry. The linear range of the sensor was from 7.0 × 10(-8)mol/L-9.0 × 10(-5)mol/L, with the limit of detection (LOD) of 2.3 × 10(-8)mol/L (S/N=3). The sensor showed high selectivity, excellent stability and good reproducibility for the determination of erythromycin, and it was successfully applied to the detection of erythromycin in real spiked samples. Copyright © 2012 Elsevier B.V. All rights reserved.

Sensing CA 15-3 in point-of-care by electropolymerizing O-phenylenediamine (oPDA) on Au-screen printed electrodes

PubMed Central

Gomes, Rui S.; Moreira, Felismina T. C.; Fernandes, Ruben

2018-01-01

This work presents an alternative device for cancer screening in liquid biopsies. It combines a biomimetic film (i) with electrochemical detection (ii). The biomimetic film (i) was obtained by electro-polymerizing amine-substituted benzene rings around a CA 15–3 target. This protein target was previously adsorbed on a gold (Au) support and incubated in charged monomers (4-Styrenesulfonate sodium and 3-Hydroxytyraminium chloride). The protein was further eliminated by enzymatic activity, leaving behind vacant sites for subsequent rebinding. Electrochemical detection (ii) was achieved on an Au working electrode, designed on commercial screen-printed electrodes. Raman spectroscopy, atomic force microscopy and ellipsometric readings were used to follow the chemical modification of the Au surface. The ability of the material to rebind CA15-3 was monitored by electrochemical techniques. The device displayed linear responses to CA15-3 ranging from 0.25 to 10.00 U/mL, with detection limits of 0.05 U/mL. Accurate results were obtained by applying the sensor to the analysis of CA15-3 in PBS buffer and in serum samples. This biosensing device displayed successful features for the detection of CA 15–3 and constitutes a promising tool for breast cancer screening procedures in point-of-care applications. Moreover, its scale-up seems feasible as it contains a plastic antibody assembled in situ, in less than 1 minute, and the analysis of serum takes less than 30 minutes. PMID:29715330

Electrochemical immunosensor based on poly (3,4-ethylenedioxythiophene) modified with gold nanoparticle to detect aflatoxin B1.

PubMed

Sharma, Arati; Kumar, A; Khan, Raju

2017-07-01

Gold nanoparticles (Au-NPs) functionalized Poly (3,4-ethylenedioxythiophene) (PEDOT) bioelectrodes were fabricated layer by layer deposition on ITO electrode for detection of aflatoxin B 1 . The monoclonal anti-aflatoxin antibodies (Anti-AFB 1 ) were immobilized over the surface of PEDOT/Au-NPs/ITO using EDC/NHS coupling. The surface morphology and characteristics of the modified electrodes were investigated by scanning electron microscope and contact angle measurements. The electrochemical analysis of the fabricated immunoelectrode and the immobilization of the antibodies have been evaluated and confirmed by performing Cyclic Voltammetry (CV), Electrochemical Impedance Spectroscopy (EIS) and Fourier Transform Infrared Spectroscopy (FTIR). Decrease in the value of electron transfer resistance (R et ) and increase in the peak current values after incorporation of Au-NPs signifies the enhanced properties of PEDOT embedded Au-NPs. The heterogeneous rate constant (k s ) and transfer coefficient (α) have been determined by using Laviron's method. The fabricated immunosensor exhibits high sensitive amperometric response of 3.72μAngmL -1 towards AFB 1 concentration in a linear range of 1-25ngmL -1 with detection limit (LOD) of 0.0045ngmL -1 and limit of quantification (LOQ) of 0.0156ngmL -1 . The fabricated immunoelectrode shows a reproducibility of 96.13% and 94.5% towards real maize sample spiked with AFB 1 of concentration 30ngmL -1 and 50ngmL -1 , respectively. Copyright © 2017 Elsevier B.V. All rights reserved.

The photovoltaic performance of Ag2S quantum dots-sensitized solar cells using plasmonic Au nanoparticles/TiO2 working electrodes

NASA Astrophysics Data System (ADS)

Badawi, Ali; Mostafa, Nasser Y.; Al-Hosiny, Najm M.; Merazga, Amar; Albaradi, Ateyyah M.; Abdel-Wahab, F.; Atta, A. A.

2018-06-01

The photovoltaic performance of silver sulfide (Ag2S) quantum dots-sensitized solar cells (QDSSCs) using different concentrations (0, 0.05, 0.1, 0.3 and 0.5 wt.%) of plasmonic Au nanoparticles (NPs)/titania (TiO2) electrodes has been investigated. Ag2S quantum dots (QDs) were adsorbed onto the Au NPs/titania electrodes using the successive ionic layer adsorption and reaction (SILAR) deposition technique. The morphological properties of the Au NPs and the prepared titania electrodes were characterized using transmission electron microscope (TEM) and scanning electron microscope (SEM), respectively. The energy-dispersive X-ray (EDX) spectra of the bare titania and Ag2S QDs-sensitized titania electrodes were recorded. The optical properties of the prepared Ag2S QDs-sensitized titania electrodes were measured using a UV-visible spectrophotometer. The estimated energy band gap of Ag2S QDs-sensitized titania electrodes is 1.96 eV. The photovoltaic performance of the assembled Ag2S QDSSCs was measured under 100 mW/cm2 solar illumination. The optimal photovoltaic parameters were obtained as follows: open circuit voltage Voc = 0.50 V, current density Jsc = 3.18 mA/cm2, fill factor (FF) = 0.35 and energy conversion efficiency η = 0.55% for 0.3 wt.% of Au NPs/titania electrode. These results are attributed to the enhancement in the absorption and decrease in the electron-hole pairs recombination rate. The open circuit voltage decay (OCVD) measurements of the assembled Ag2S QDSSCs were measured. The calculated electron lifetime (τ) in Ag2S QDSSCs with Au NPs/titania electrodes is at least one order of magnitude more than that with bare titania electrode. The cut-on-cut-off cycles of the solar illumination measurements show the rapid sensitivity and good reproducibility of the assembled Ag2S QDSSCs.

Bendable solid-state supercapacitors with Au nanoparticle-embedded graphene hydrogel films

PubMed Central

Yang, Kyungwhan; Cho, Kyoungah; Yoon, Dae Sung; Kim, Sangsig

2017-01-01

In this study, we fabricate bendable solid-state supercapacitors with Au nanoparticle (NP)-embedded graphene hydrogel (GH) electrodes and investigate the influence of the Au NP embedment on the internal resistance and capacitive performance. Embedding the Au NPs into the GH electrodes results in a decrease of the internal resistance from 35 to 21 Ω, and a threefold reduction of the IR drop at a current density of 5 A/g when compared with GH electrodes without Au NPs. The Au NP-embedded GH supercapacitors (NP-GH SCs) exhibit excellent capacitive performances, with large specific capacitance (135 F/g) and high energy density (15.2 W·h/kg). Moreover, the NP-GH SCs exhibit comparable areal capacitance (168 mF/cm2) and operate under tensile/compressive bending. PMID:28074865

Electrochemical magnetoimmunosensing approach for the sensitive detection of H9N2 avian influenza virus particles.

PubMed

Zhou, Chuan-Hua; Shu, Yun; Hong, Zheng-Yuan; Pang, Dai-Wen; Zhang, Zhi-Ling

2013-09-01

A novel electrochemical magnetoimmunosensor for fast and ultrasensitive detection of H9N2 avian influenza virus particles (H9N2 AIV) was designed based on the combination of high-efficiency immunomagnetic separation, enzyme catalytic amplification, and the biotin-streptavidin system. The reusable, homemade magneto Au electrode (M-AuE) was designed and used for the direct sensing. Immunocomplex-coated magnetic beads (IMBs) were easily accumulated on the surface of the M-AuE to obtain the catalytically reduced electrochemical signal of H2 O2 after the immunoreaction. The transducer was regenerated through a simple washing procedure, which made it possible to detect all the samples on a single electrode with higher reproducibility. The magnetic-bead-based electrochemical immunosensor showed better analytical performance than the planar-electrode-based immunosensor with the same sandwich construction. Amounts as low as 10 pg mL(-1) H9N2 AIV could be detected even in samples of chicken dung. This electrochemical magnetoimmunosensor not only provides a simple platform for the detection of the virus with high sensitivity, selectivity, and reproducibility but also shows great potential in the early diagnosis of diseases. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Label-free capacitive immunosensor based on quartz crystal Au electrode for rapid and sensitive detection of Escherichia coli O157:H7.

PubMed

Li, Dujuan; Feng, Yangyang; Zhou, Ling; Ye, Zunzhong; Wang, Jianping; Ying, Yibin; Ruan, Chuanmin; Wang, Ronghui; Li, Yanbin

2011-02-14

A label-free capacitive immunosensor based on quartz crystal Au electrode was developed for rapid and sensitive detection of Escherichia coli O157:H7. The immunosensor was fabricated by immobilizing affinity-purified anti-E. coli O157:H7 antibodies onto self-assembled monolayers (SAMs) of 3-mercaptopropionic acid (MPA) on the surface of a quartz crystal Au electrode. Bacteria suspended in solution became attached to the immobilized antibodies when the immunosensor was tested in liquid samples. The change in capacitance caused by the bacteria was directly measured by an electrochemical detector. An equivalent circuit was introduced to simulate the capacitive immunosensor. The immunosensor was evaluated for E. coli O157:H7 detection in pure culture and inoculated food samples. The experimental results indicated that the capacitance change was linearly correlated with the cell concentration of E. coli O157:H7. The immunosensor was able to discriminate between cellular concentrations of 10(2)-10(5) cfu mL(-1) and has applications in detecting pathogens in food samples. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) were also employed to characterize the stepwise assembly of the immunosensor. Copyright © 2010 Elsevier B.V. All rights reserved.

The O2 reduction at the IFC modified O2 fuel cell electrode

NASA Technical Reports Server (NTRS)

Fielder, William L.; Singer, Joseph; Baldwin, Richard S.; Johnson, Richard E.

1992-01-01

The International Fuel Corporation (IFC) state of the art (SOA) O2 electrode (Au-10 percent Pt electrocatalyst by weight) is currently being used in the alkaline H2-O2 fuel cell in the NASA Space Shuttle. Recently, IFC modified O2 electrode, as a possible replacement for the SOA electrode. In the present study, O2 reduction data were obtained for the modified electrode at temperatures between 23.3 and 91.7 C. BET measurements gave an electrode BET surface area of about 2070 sq. cm/sq. cm of geometric surface area. The Tafel data could be fitted to two straight line regions. The slope for the lower region, designated as the 0.04 V/decade region, was temperature dependent, and the transfer coefficient was about 1.5. The 'apparent' energy of activation for this region was about 19 kcal/mol. An O2 reduction mechanism for this 0.04 region is presented. In the upper region, designated as the 0.08 V/decade region, diffusion may be the controlling process. Tafel data are presented to illustrate the increase in performance with increasing temperature.

Fully Printable Organic and Perovskite Solar Cells with Transfer-Printed Flexible Electrodes.

PubMed

Li, Xianqiang; Tang, Xiaohong; Ye, Tao; Wu, Dan; Wang, Hong; Wang, Xizu

2017-06-07

The perovskite solar cells (PSCs) and organic solar cells (OSCs) with high performance were fabricated with transfer-printed top metal electrodes. We have demonstrated that PSCs and OSCs with the top Au electrodes fabricated by using the transfer printing method have comparable or better performance than the devices with the top Au electrodes fabricated by using the conventional thermal evaporation method. The highest PCE of the PSCs and OSCs with the top electrodes fabricated using the transfer printing method achieved 13.72% and 2.35%, respectively. It has been investigated that fewer defects between the organic thin films and Au electrodes exist by using the transfer printing method which improved the device stability. After storing the PSCs and OSCs with the transfer-printed electrodes in a nitrogen environment for 97 and 103 days without encapsulation, the PSCs and OSCs still retained 71% and 91% of their original PCEs, respectively.

Selective AuCl3 doping of graphene for reducing contact resistance of graphene devices

NASA Astrophysics Data System (ADS)

Choi, Dong-Chul; Kim, Minwoo; Song, Young Jae; Hussain, Sajjad; Song, Woo-Seok; An, Ki-Seok; Jung, Jongwan

2018-01-01

Low contact resistance between metal-graphene contacts remains a well-known challenge for building high-performance two dimensional materials devices. In this study, CVD-grown graphene film was doped via AuCl3 solution selectively only to metal (Ti/Au) contact area to reduce the contact resistances without compromising the channel properties of graphene. With 10 mM-AuCl3 doping, doped graphene exhibited low contact resistivity of ∼897 Ω μm, which is lower than that (∼1774 Ω μm) of the raw graphene devices. The stability of the contact resistivity in atmospheric environment was evaluated. The contact resistivity increased by 13% after 60 days in an air environment, while the sheet resistance of doped graphene increased by 50% after 30 days. The improved stability of the contact resistivity of AuCl3-doped graphene could be attributed to the fact that the surface of doped-graphene is covered by Ti/Au electrode and the metal prevents the diffusion of AuCl3.

Sensitive electrochemical aptamer cytosensor for highly specific detection of cancer cells based on the hybrid nanoelectrocatalysts and enzyme for signal amplification.

PubMed

Sun, Duanping; Lu, Jing; Zhong, Yuwen; Yu, Yanyan; Wang, Yu; Zhang, Beibei; Chen, Zuanguang

2016-01-15

Human cancer is becoming a leading cause of death in the world and the development of a straightforward strategy for early detection of cancer is urgently required. Herein, a sandwich-type electrochemical aptamer cytosensor was developed for detection of human liver hepatocellular carcinoma cells (HepG2) based on the hybrid nanoelectrocatalysts and enzyme for signal amplification. The thiolated TLS11a aptamers were used as a selective bio-recognition element, attached to the gold nanoparticles (AuNPs) modified the glassy carbon electrode (GCE) surface. Meanwhile, the electrochemical nanoprobes were fabricated through the G-quadruplex/hemin/aptamer complexes and horseradish peroxidase (HRP) immobilized on the surfaces of Au@Pd core-shell nanoparticle-modified magnetic Fe3O4/MnO2 beads (Fe3O4/MnO2/Au@Pd). After the target cells were captured, the hybrid nanoprobes were further assembled to form an aptamer-cell-nanoprobes sandwich-like system on the electrode surface. Then, hybrid Fe3O4/MnO2/Au@Pd nanoelectrocatalysts, G-quadruplex/hemin HRP-mimicking DNAzymes and the natural HRP enzyme efficiently catalyzed the oxidation of hydroquinone (HQ) with H2O2, amplifying the electrochemical signals and improving the detection sensitivity. This electrochemical cytosensor delivered a wide detection range of 1×10(2)-1×10(7)cellsmL(-1), high sensitivity with a low detection limit of 15cellsmL(-1), good selectivity and repeatability. Finally, an electrochemical reductive desorption method was performed to break gold-thiol bond and desorb the components on the AuNPs/GCE for regenerating the cytosensor. These results have demonstrated that the electrochemical cytosensor has the potential to be a feasible tool for cost-effective cancer cell detection in early cancer diagnosis. Copyright © 2015 Elsevier B.V. All rights reserved.

A novel approach to construct a horseradish peroxidase|hydrophilic ionic liquids|Au nanoparticles dotted titanate nanotubes biosensor for amperometric sensing of hydrogen peroxide.

PubMed

Liu, Xiaoqiang; Feng, Heqing; Zhao, Ruoxia; Wang, Yanbing; Liu, Xiuhua

2012-01-15

The direct electrochemistry of horseradish peroxidase (HRP) on a novel sensing platform modified glassy carbon electrode (GCE) has been achieved. This sensing platform consists of Nafion, hydrophilic room-temperature ionic liquid (RTIL) and Au nanoparticles dotted titanate nanotubes (GNPs-TNTs). The composite of RTIL and GNPs-TNTs was immobilized on the electrode surface through the gelation of a small amount of HRP aqueous solution. The composite was characterized by transmission electron microscopy (TEM), powder X-ray diffraction (XRD) and infrared spectroscopy (IR). UV-Vis and IR spectroscopy demonstrated that HRP in the composite could retain its native secondary structure and biochemical activity. The HRP-immobilized electrode was investigated by cyclic voltammetry and chronoamperometry. The results from both techniques showed that the direct electron transfer between the nanocomposite modified electrodes and heme in HRP could be realized. The biosensor responded to H(2)O(2) in the linear range from 5×10(-6) to 1×10(-3) mol L(-1) with a detection limit of 2.1×10(-6) mol L(-1) (based on the S/N=3). Copyright © 2011 Elsevier B.V. All rights reserved.

An ultrasensitive electrochemical biosensor for polynucleotide kinase assay based on gold nanoparticle-mediated lambda exonuclease cleavage-induced signal amplification.

PubMed

Cui, Lin; Li, Yueying; Lu, Mengfei; Tang, Bo; Zhang, Chun-Yang

2018-01-15

Polynucleotide kinase (PNK) plays an essential role in cellular nucleic acid metabolism and the cellular response to DNA damage. However, conventional methods for PNK assay suffer from low sensitivity and involve multiple steps. Herein, we develop a simply electrochemical method for sensitive detection of PNK activity on the basis of Au nanoparticle (AuNP)-mediated lambda exonuclease cleavage-induced signal amplification. We use [Ru(NH 3 ) 6 ] 3+ as the electrochemically active indicator and design two DNA strands (i.e., strand 1 and strand 2) to sense PNK. The assembly of strand 2 on the AuNP surface leads to the formation of AuNP-strand 2 conjugates which can be subsequently immobilized on the gold electrode through the hybridization of strand 1 with strand 2 for the generation of a high electrochemical signal. The presence of PNK induces the phosphorylation of the strand 2-strand 1 hybrid and the subsequent cleavage of double-stranded DNA (dsDNA) by lambda exonuclease, resulting in the release of AuNP-strand 2 conjugates and [Ru(NH 3 ) 6 ] 3+ from the gold electrode surface and consequently the decrease of electrochemical signal. The PNK activity can be simply monitored by the measurement of [Ru(NH 3 ) 6 ] 3+ peak current signal. This assay is very sensitive with a detection limit of as low as 7.762 × 10 -4 UmL -1 and exhibits a large dynamic range from 0.001 to 10UmL -1 . Moreover, this method can be used to screen the PNK inhibitors, and it shows excellent performance in real sample analysis, thus holding great potential for further applications in biological researches and clinic diagnosis. Copyright © 2017 Elsevier B.V. All rights reserved.

One-pot preparation of PEDOT:PSS-reduced graphene decorated with Au nanoparticles for enzymatic electrochemical sensing of H2O2

NASA Astrophysics Data System (ADS)

Mercante, Luiza A.; Facure, Murilo H. M.; Sanfelice, Rafaela C.; Migliorini, Fernanda L.; Mattoso, Luiz H. C.; Correa, Daniel S.

2017-06-01

The development of novel graphene-based nanocomposites is a hotspot in materials science due to their unique optical, electronic, thermal, mechanical and catalytic properties for varied applications. The present work reports on the development of a graphene-based ternary nanocomposite of poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate), reduced graphene oxide and gold nanoparticles (PEDOT:PSS-rGO-AuNPs) for the detection of hydrogen peroxide (H2O2). The hybrid nanocomposite showed superior electrochemical properties and higher stability compared to each individual component as electrode materials, showing a synergistic effect between PEDOT, rGO and AuNPs. The nanocomposite was obtained via a facile one-step approach and was assembly with horseradish peroxidase (HRP). The PEDOT:PSS-rGO-AuNPs-HRP modified electrode has been used for the amperometric detection of H2O2 and exhibited a high sensitivity of up to 677 μA mM-1 cm-2, with a wide linear range from 5 to 400 μM and a low detection limit of 0.08 μM (S/N = 3). This developed enzymatic biosensor showed to be highly stable and unresponsive to potentially interfering substances, and it could be used for sensing H2O2 in real samples, including tap water and bovine milk samples. These enhanced sensing performance could be ascribed to the intimate contact of AuNPs onto the rough surface of the PEDOT:PSS-rGO nanocomposite, which has a high electrical conductivity and large surface area, providing it as an excellent substrate for the growth and support of nanoparticles. The method developed in this work opens up a general route to prepare a wide range of graphene-based hybrid nanocomposite films with multiple functions including sensing and biosensing.

A novel reduced graphene oxide/molybdenum disulfide/polyaniline nanocomposite-based electrochemical aptasensor for detection of aflatoxin B1.

PubMed

Geleta, Girma Selale; Zhao, Zhen; Wang, Zhenxin

2018-03-26

In this study, we developed a novel reduced graphene oxide/molybdenum disulfide/polyaniline@gold nanoparticles-based electrochemical aptasensor (termed as RGO/MoS2/PANI@AuNPs/Apt) for detection of aflatoxin B1 (AFB1). The RGO/MoS2/PANI nanocomposites were synthesized and characterized by multiple techniques, including scanning electron microscopy (SEM), transmission electron microscopy (TEM), infrared spectroscopy (FTIR), UV-visible spectroscopy, and X-ray photoelectron spectroscopy (XPS). A glassy carbon electrode (GCE) was then modified by the RGO/MoS2/PANI nanocomposites, coated with a chitosan (Cs) film, and followed by AuNPs attachment for immobilizing the AFB1 aptamers. In the presence of AFB1, the AFB1 binding-induced conformation change of the immobilized aptamer on the electrode surface results in the reduction of the electron transfer from a [Fe(CN)6]3-/4- redox couple in the solution to the GCE surface. Therefore, the aptamer-AFB1 binding event can be easily monitored by the peak current change of the RGO/MoS2/PANI@AuNPs/Apt through differential pulse voltammetry (DPV) measurement. Under the optimized conditions, the as-developed RGO/MoS2/PANI@AuNPs/Apt exhibits a wide linear range from 0.01 fg mL-1 to 1.0 fg mL-1 and a remarkably low detection limit (3σ) of 0.002 fg mL-1. The aptasensor also has good reproducibility as well as shows high selectivity against other fungal toxins, such as OTA and FB1. Moreover, the practicability of the RGO/MoS2/PANI@AuNPs/Apt was demonstrated by the analysis of AFB1 in the spiked wine samples.

Electric-field noise from carbon-adatom diusion on a Au(110) surface: first-principles calculations and experiments

NASA Astrophysics Data System (ADS)

Sadeghpour, Hossein; Kim, Eunja; Safavi-Naini, Arghavan; Weck, Philippe; Hite, Dustin; McKay, Kyle; Pappas, David

2017-04-01

The decoherence of trapped-ion quantum gates due to heating of their motional modes is a fundamental science and engineering challenge. Mitigating this noise, is fundamental to efficient and scalable operations in ion microtraps. To understand heating at the trap-electrode surfaces, we investigate the possible source of noise by focusing on the diffusion of carbon-containing adsorbates onto the Au(110) surface. Using density functional theory and detailed scanning probe microscopy, we show that the diffusive motion of carbon adatom on gold surface significantly affect the energy landscape and adatom dipole moment variation. A model for the diffusion noise, which varies quadratically with the variation of the dipole moment, qualitatively reproduces the measured noise spectrum, and the estimate of the noise spectral density is in accord with measured values.

Fast Response Polypyrrole Actuators with Auxiliary Electrodes

NASA Astrophysics Data System (ADS)

Zama, Tetsuji; Hara, Susumu; Takashima, Wataru; Kaneto, Keiichi

2005-11-01

Electrochemical polypyrrole (PPy) actuators, prepared electrochemically from a methyl benzoate solution of tetra-n-butylammonium trifluoromethanesulfonate (TBACF3SO3), have been studied to improve the response rate by two methods; 1) a PPy film attached with plural auxiliary electrodes of thin Au coils, 2) a PPy film equipped with a compliant Au electrode on one side of the film. With increasing the number of auxiliary electrodes for the first method, the film responded faster as if it were a shorter film. These results are due to the decrease in the IR voltage drop along the film from the electrodes and also due to the increased current to the whole film via plural electrodes. The PPy film with the Au thin layer (the second method) exhibited up to 8.8%/s strain rate, which was much faster than that (0.5%/s) without the auxiliary electrodes, keeping the maximum strain of 12--13%. The auxiliary electrodes improved not only the response speed of the PPy actuators but also the durability upon cycling electrochemically.

Interpenetrating polyaniline-gold electrodes for SERS and electrochemical measurements

NASA Astrophysics Data System (ADS)

West, R. M.; Semancik, S.

2016-11-01

Facile fabrication of nanostructured electrode arrays is critical for development of bimodal SERS and electrochemical biosensors. In this paper, the variation of applied potential at a polyaniline-coated Pt electrode is used to selectivity deposit Au on the polyaniline amine sites or on the underlying Pt electrode. By alternating the applied potential, the Au is grown simultaneously from the top and the bottom of the polyaniline film, leading to an interpenetrated, nanostructured polymer-metal composite extending from the Pt electrode to the electrolyte solution. The resulting films have unique pH-dependent electrochemical properties, e.g. they retain electrochemical activity in both acidic and neutral solutions, and they also include SERS-active nanostructures. By varying the concentration of chloroaurate used during deposition, Au nanoparticles, nanodendrites, or nanosheets can be selectively grown. For the films deposited under optimal conditions, using 5 mmol/L chloroaurate, the SERS enhancement factor for Rhodamine 6G was found to be as high as 1.1 × 106 with spot-to-spot and electrode-to-electrode relative standard deviations as low as 8% and 12%, respectively. The advantages of the reported PANI-Au composite electrodes lie in their facile fabrication, enabling the targeted deposition of tunable nanostructures on sensing arrays, and their ability to produce orthogonal optical and electrochemical analytical results.

Au-TiO2/Chit modified sensor for electrochemical detection of trace organophosphates insecticides.

PubMed

Qu, Yunhe; Min, Hong; Wei, Yinyin; Xiao, Fei; Shi, Guoyue; Li, Xiaohua; Jin, Litong

2008-08-15

In this paper, Au-TiO2/Chit modified electrode was prepared with Au-TiO2 nanocomposite (Au-TiO2) and Chitosan (Chit) as a conjunct. The Au-TiO2 nanocomposite and the films were characterized by electrochemical and spectroscopy methods. A set of experimental conditions was also optimized for the film's fabrication. The electrochemical and electrocatalytic behaviors of Au-TiO2/Chit modified electrode to trace organophosphates (OPs) insecticides such as parathion were discussed in this work. By differential pulse voltammetry (DPV) measurement, the current responses of Au-TiO2/Chit modified electrode were linear with parathion concentration ranging from 1.0 ng/ml to 7.0 x 10(3)ng/ml with the detection limit of 0.5 ng/ml. In order to evaluate the performance of the detection system, we also examined the real samples successfully in this work. It exhibited a sensitive, rapid and easy-to-use method for the fast determination of trace OPs insecticides.

Electrochemical, photoelectrochemical, and surface plasmon resonance detection of cocaine using supramolecular aptamer complexes and metallic or semiconductor nanoparticles.

PubMed

Golub, Eyal; Pelossof, Gilad; Freeman, Ronit; Zhang, Hong; Willner, Itamar

2009-11-15

Metallic or semiconductor nanoparticles (NPs) are used as labels for the electrochemical, photoelectrochemical, or surface plasmon resonance (SPR) detection of cocaine using a common aptasensor configuration. The aptasensors are based on the use of two anticocaine aptamer subunits, where one subunit is assembled on a Au support, acting as an electrode or a SPR-active surface, and the second aptamer subunit is labeled with Pt-NPs, CdS-NPs, or Au-NPs. In the different aptasensor configurations, the addition of cocaine results in the formation of supramolecular complexes between the NPs-labeled aptamer subunits and cocaine on the metallic surface, allowing the quantitative analysis of cocaine. The supramolecular Pt-NPs-aptamer subunits-cocaine complex allows the detection of cocaine by the electrocatalyzed reduction of H(2)O(2). The photocurrents generated by the CdS-NPs-labeled aptamer subunits-cocaine complex, in the presence of triethanol amine as a hole scavenger, allows the photoelectrochemical detection of cocaine. The supramolecular Au-NPs-aptamer subunits-cocaine complex generated on the Au support allows the SPR detection of cocaine through the reflectance changes stimulated by the electronic coupling between the localized plasmon of the Au-NPs and the surface plasmon wave. All aptasensor configurations enable the analysis of cocaine with a detection limit in the range of 10(-6) to 10(-5) M. The major advantage of the sensing platform is the lack of background interfering signals.

Self-Assembled Structures of Benzoic Acid on Au(111) Surface

NASA Astrophysics Data System (ADS)

Vu, Thu-Hien; Wandlowski, Thomas

2017-06-01

Electrochemical scanning tunneling microscopy combined with cyclic voltammetry were employed to explore the self-assembly of benzoic acid (BA) on a Au(111) substrate surface in a 0.1-M HClO4 solution. At the negatively charged surface, BA molecules form two highly ordered physisorbed adlayers with their phenyl rings parallel to the substrate surface. High-resolution scanning tunneling microscopy images reveal the packing arrangement and internal molecular structures. The striped pattern and zigzag structure of the BA adlayers are composed of parallel rows of dimers, in which two BA molecules are bound through a pair of O-H···O hydrogen bonds. Increasing the electrode potential further to positive charge densities of Au(111) leads to the desorption of the physisorbed hydrogen-bonded networks and the formation of a chemisorbed adlayer. BA molecules change their orientation from planar to upright fashion, which is accompanied by the deprotonation of the carboxyl group. Furthermore, potential-induced formation and dissolution of BA adlayers were also investigated. Structural transitions between the various types of ordered adlayers occur according to a nucleation and growth mechanism.

Electrochemical Biosensor Composed of Silver Ion-Mediated dsDNA on Au-Encapsulated Bi2 Se3 Nanoparticles for the Detection of H2 O2 Released from Breast Cancer Cells.

PubMed

Mohammadniaei, Mohsen; Yoon, Jinho; Lee, Taek; Bharate, Bapurao G; Jo, Jinhee; Lee, Donghyun; Choi, Jeong-Woo

2018-04-01

A newly developed electrochemical biosensor composed of a topological insulator (TI) and metallic DNA (mDNA) is fabricated. The bismuth selenide nanoparticle (Bi 2 Se 3 NP) is synthesized and sandwiched between the gold electrode and another Au-deposited thin layer (Bi 2 Se 3 @Au). Then, eight-silver-ion mediated double-stranded DNA (mDNA) is immobilized onto the substrate (Bi 2 Se 3 @Au-mDNA) for the further detection of hydrogen peroxide. The Bi 2 Se 3 NP acts as the electrochemical-signal booster, while unprecedentedly its encapsulation by the Au thin layer keeps the TI surface states protected, improves its electrochemical-signal stability and provides an excellent platform for the subsequent covalent immobilization of the mDNA through Au-thiol interaction. Electrochemical results show that the fabricated biosensor represents much higher Ag + redox current (≈10 times) than those electrodes prepared without Bi 2 Se 3 @Au. The characterization of the Bi 2 Se 3 @Au-mDNA film is confirmed by atomic force microscopy, scanning tunneling microscopy, and cyclic voltammetry. The proposed biosensor shows a dynamic range of 00.10 × 10 -6 m to 27.30 × 10 -6 m, very low detection limit (10 × 10 -9 m), unique current response (1.6 s), sound H 2 O 2 recovery in serum, and substantial capability to classify two breast cancer subtypes (MCF-7 and MDA-MB-231) based on their difference in the H 2 O 2 generation, offering potential applications in the biomedicine and pharmacology fields. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Production of gold nanoparticles by electrode-respiring Geobacter sulfurreducens biofilms

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tanzil, Abid H.; Sultana, Sujala T.; Saunders, Steven R.

2016-12-01

Current chemical syntheses of nanoparticles (NP) has had limited success due to the relatively high environmental cost caused by the use of harsh chemicals requiring necessary purification and size-selective fractionation. Therefore, biological approaches have received recent attention for their potential to overcome these obstacles as a benign synthetic approach. The intrinsic nature of biomolecules present in microorganisms has intrigued researchers to design bottom-up approaches to biosynthesize metal nanoparticles using microorganisms. Most of the literature work has focused on NP synthesis using planktonic cells while the use of biofilms are limited. The goal of this work was to synthesize gold nanoparticlesmore » (AuNPs) using electrode respiring Geobacter sulfurreducens biofilms. We found that most of the AuNPs are generated in the extracellular matrix of Geobacter biofilms with an average particle size of 20 nm. The formation of AuNPs was verified using TEM, FTIR and EDX. We also found that the extracellular substances extracted from electrode respiring G. sulfurreducens biofilms can reduce Au3+ to AuNPs. It appears that reducing sugars were involved in bioreduction and synthesis of AuNPs and amine groups acted as the major biomolecules involved in binding. This is first demonstration of AuNPs formation from the extracellular matrix of electrode respiring biofilms.« less

Block Copolymer Patterns as Templates for the Electrocatalyzed Deposition of Nanostructures on Electrodes and for the Generation of Surfaces of Controlled Wettability.

PubMed

Chandaluri, Chanchayya Gupta; Pelossof, Gilad; Tel-Vered, Ran; Shenhar, Roy; Willner, Itamar

2016-01-20

ITO electrodes modified with a nanopatterned film of polystyrene-block-poly(2-vinylpyridine), PS-b-P2VP, where the P2VP domains are quaternized with iodomethane, are used for selective deposition of redox-active materials. Electrochemical studies (cyclic voltammetry, Faradaic impedance measurements) indicate that the PS domains insulate the conductive surface toward redox labels in solution. In turn, the quaternized P2VP domains electrostatically attract negatively charged redox labels solubilized in the electrolyte solution, resulting in an effective electron transfer between the electrode and the redox label. This phenomenon is implemented for the selective deposition of the electroactive Prussian blue on the nanopatterned surface and for the electrochemical deposition of Au nanoparticles, modified with a monolayer of p-aminothiophenol/2-mercaptoethanesulfonic acid, on the quaternized P2VP domains. The patterned Prussian blue-modified surface enables controlling the wettability properties by the content of the electrochemically deposited Prussian blue. Controlled wettability is unattainable with the homopolymer-modified surface, attesting to the role of the nanopattern.

Graphene-bimetallic nanoparticle composites with enhanced electro-catalytic detection of bisphenol A

NASA Astrophysics Data System (ADS)

Pogacean, Florina; Biris, Alexandru R.; Socaci, Crina; Coros, Maria; Magerusan, Lidia; Rosu, Marcela-Corina; Lazar, Mihaela D.; Borodi, Gheorghe; Pruneanu, Stela

2016-12-01

This study brings for the first time novel knowledge about the synthesis by catalytic chemical vapor deposition with induction heating of graphene-bimetallic nanoparticle composites (Gr-AuCu and Gr-AgCu) and their morphological and structural characterization by transmission electron microscopy, Raman spectroscopy, and x-ray powder diffraction. Gold electrodes modified with the obtained materials exhibit an enhanced electro-catalytic effect towards one of the most encountered estrogenic disruptive chemicals, bisphenol A (BPA). The BPA behavior in varying pH solutions was investigated using the electrochemical quartz crystal microbalance, which allowed the accurate determination of the number of molecules involved in the oxidation process. The modified electrodes promote the oxidation of BPA at significantly lower potentials (0.66 V) compared to bare gold (0.78 V). In addition, the peak current density recorded with such electrodes greatly exceeded that obtained with bare gold (e.g. one order of magnitude larger, for a Au/Gr-AgCu electrode). The two modified electrodes have low detection limits, of 1.31 × 10-6 M and 1.91 × 10-6 M for Au/Gr-AgCu and Au/Gr-AuCu, respectively. The bare gold electrode has a higher detection limit of 5.1 × 10-6 M. The effect of interfering species (e.g. catechol and 3-nitrophenol) was also investigated. Their presence influenced not only the BPA peak potential, but also the peak current. With both modified electrodes, no peak currents were recorded below 3 × 10-5 M BPA.

Layered Metal Nanoparticle Structures on Electrodes for Sensing, Switchable Controlled Uptake/Release, and Photo-electrochemical Applications.

PubMed

Tel-Vered, Ran; Kahn, Jason S; Willner, Itamar

2016-01-06

Layered metal nanoparticle (NP) assemblies provide highly porous and conductive composites of unique electrical and optical (plasmonic) properties. Two methods to construct layered metal NP matrices are described, and these include the layer-by-layer deposition of NPs, or the electropolymerization of monolayer-functionalized NPs, specifically thioaniline-modified metal NPs. The layered NP composites are used as sensing matrices through the use of electrochemistry or surface plasmon resonance (SPR) as transduction signals. The crosslinking of the metal NP composites with molecular receptors, or the imprinting of molecular recognition sites into the electropolymerized NP matrices lead to selective and chiroselective sensing interfaces. Furthermore, the electrosynthesis of redox-active, imprinted, bis-aniline bridged Au NP composites yields electrochemically triggered "sponges" for the switchable uptake and release of electron-acceptor substrates, and results in conductive surfaces of electrochemically controlled wettability. Also, photosensitizer-relay-crosslinked Au NP composites, or electrochemically polymerized layered semiconductor quantum dot/metal NP matrices on electrodes, are demonstrated as functional nanostructures for photoelectrochemical applications. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cascaded Ga1-xAlxAs/GaAs solar cell with graded i-region

NASA Astrophysics Data System (ADS)

Mil'shtein, Sam; Halilov, Samed

2018-02-01

In current study we designed p-i-n junction with extended intrinsic layer, where linearly graded Alx Ga1-x As presents variable energy gap so needed for effective harvesting of sun radiation. The design realization involves two regions of compositional structure in the stacking direction. The top AlxGa1-xAs layer of 1 um total thickness has stoichiometric structure x=0.3-0.2d, where depth d runs from 0 to 1 um, topmost 200 nm of which is Be-doped. Bottom AlxGa1-xAs layer of 3 um total thickness has a variable composition of x=0.133-0.033d, d runs from 1 to 4 um, the very bottom of which with 10 nm thickness is Si-doped. On the top surface, there is a 50 nm layer of p+ doped GaAs as a spacer for growing AuGe/Ni anode electrode of 20% surface area, the bottom is coated with AuGe/Ni cathode electrode. The designed cell demonstrates 89% fill factor and 30% conversion efficiency without anti-reflection coating.

Using ruthenium polypyridyl functionalized ZnO mesocrystals and gold nanoparticle dotted graphene composite for biological recognition and electrochemiluminescence biosensing

NASA Astrophysics Data System (ADS)

Liu, Suli; Zhang, Jinxing; Tu, Wenwen; Bao, Jianchun; Dai, Zhihui

2014-01-01

Using ruthenium polypyridyl functionalized ZnO mesocrystals as bionanolabels, a universal biological recognition and biosensing platform based on gold nanoparticle (AuNP) dotted reduced graphene oxide (rGO) composite was developed. AuNP-rGO accelerated electron transfer between the detection probe and the electrode, and increased the surface area of the working electrode to load greater amounts of the capture antibodies. The large surface area of ZnO mesocrystals was beneficial for loading a high content ruthenium polypyridyl complex, leading to an enhanced electrochemiluminescence signal. Using α-fetoprotein (AFP) as a model, a simple and sensitive sandwich-type electrochemiluminescence biosensor with tripropylamine (TPrA) as a coreactant for detection of AFP was constructed. The designed biosensor provided a good linear range from 0.04 to 500 ng mL-1 with a low detection limit of 0.031 ng mL-1 at a S/N of 3 for AFP determination. The proposed biological recognition and biosensing platform extended the application of ruthenium polypyridyl functionalized ZnO mesocrystals, which provided a new promising prospect.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheng, Jue-Fei; School of Electronics and Information Engineering, Suzhou Vocational University, Suzhou 215104; Zhou, Liping, E-mail: zhoulp@suda.edu.cn, E-mail: leigao@suda.edu.cn

The electronic transport properties of benzene–porphyrin–benzene (BPB) molecules coupled to gold (Au) electrodes were investigated. By successively removing the front-end Au atoms, several BPB junctions with different molecule-electrode contact symmetries were constructed. The calculated current–voltage (I–V) curves depended strongly on the contact configurations between the BPB molecules and the Au electrodes. In particular, a significant low-voltage negative differential resistance effect appeared at −0.3 V in the junctions with pyramidal electrodes on both sides. Along with the breaking of this tip-contact symmetry, the low-bias negative differential resistance effect gradually disappeared. This tip-contact may be ideal for use in the design ofmore » future molecular devices because of its similarity with experimental processes.« less

A novel fabrication method for surface integration of metal structures into polymers (SIMSIP)

NASA Astrophysics Data System (ADS)

Carrion-Gonzalez, Hector

Recently developed flexible electronics applications require that the thin metal films embedded on elastomer substrates also be flexible. These electronic systems are radically different in terms of performance and functionality than conventional silicon-based devices. A key question is whether the metal deposited on flexible films can survive large strains without rupture. Cumbersome macro-fabrication methods have been developed for functional and bendable electronics (e.g., interconnects) encapsulated between layers of polymer films. However, future electronic applications may require electronic flexible devices to be in intimate contact with curved surfaces (e.g., retinal implants) and to be robust enough to withstand large and repeated mechanical deformations. In this research, a novel technique for surface integration of metal structures into polymers (SIMSIP) was developed. Surface embedding, as opposed to placing metal on polymers, provides better adherence while leaving the surface accessible for contacts. This was accomplished by first fabricating the micro-scale metal patterns on a quartz or Teflon mother substrate, and then embedding them to a flexible polyimide thin film. The technique was successfully used to embed micro-metal structures of gold (Au), silver (Ag), and copper (Cu) into polyimide films without affecting the functional properties of the either the metals or the polymers. Experimental results confirm the successful surface-embedding of metal structures as narrow as 0.6 microm wide for different geometries commonly used in circuit design. Although similar approaches exist in literature, the proposed methodology provides a simpler and more reliable way of producing flexible circuits/electronics that is also suitable for high volume manufacturing. In order to demonstrate the flexibility of metal interconnects fabricated using the SIMSIP technique, multiple Au electrodes (5 microm and 2.5 microm wide) were tested using the X-theta bending methodology. The X-theta bending test captures data on the electrical resistivity of micro Au electrodes fabricated using the proposed SIMSIP technique by bending them at different angles between 0o and 180o up to 50 times. The data shows that the electrical resistivity of the Au electrodes remains constant (<1% variation) despite the interconnects being repeatedly subjected to extreme tensile and compressive forces during the X-theta bending test. These results are significant from the perspective of flexible electronics and biotechnology applications since the fabricated thin films exhibit significant electrical stability, reliability and wear resistance. These surface-embedded, flexible, and mechanically stable metal interconnects will enable the further development of new electronic products with applications in biotechnology (e.g., e-skin), space exploration (e.g., satellites), and microelectronics (e.g., flat panel displays). The SIMSIP technique is also a suitable process for the nanofabrication of flexible electronic devices in applications that require intimate contact with bendable curved surfaces (e.g., retinal implants).

A SERS characterization of the stability of polythionates at the gold-electrolyte interface

NASA Astrophysics Data System (ADS)

Mirza, Jeff; Smith, Scott R.; Baron, Janet Y.; Choi, Yeonuk; Lipkowski, Jacek

2015-01-01

A gold nanorod (AuNR) array electrode was employed to record SERS spectra as a function of immersion time in electrolyte solutions of tetrathionate, trithionate, the [Au(S2O3)2]3- complex, sulfide and thiosulfate. The generalized two-dimensional correlation spectroscopy was employed to deconvolute broad bands in the SERS spectra. The results show that the polythionates, tetrathionate and trithionate, sulfide, and the [Au(S2O3)2]3- complex decompose to form cyclo-S8, polymeric and monoatomic sulfur at the gold surface. The relative amount of these different forms of sulfur in the film formed at the surface depends on the nature of the electrolyte species. The decomposition of tetrathionate leads predominantly to the formation of cyclo-S8. Comparable amounts of all three forms of sulfur are formed in the solution of the [Au(S2O3)2]3- complex. Monoatomic sulfur is formed predominantly at the gold surface in solutions of trithionate and thiosulfate. In contrast to the previous suggestions, the results of this study demonstrate that polythionates are not present in the passive layer during gold leaching from thiosulfate solutions at a prolonged leaching times.

Effect of Electrode Configuration on Nitric Oxide Gas Sensor Behavior.

PubMed

Cui, Ling; Murray, Erica P

2015-09-23

The influence of electrode configuration on the impedancemetric response of nitric oxide (NO) gas sensors was investigated for solid electrochemical cells [Au/yttria-stabilized zirconia (YSZ)/Au)]. Fabrication of the sensors was carried out at 1050 °C in order to establish a porous YSZ electrolyte that enabled gas diffusion. Two electrode configurations were studied where Au wire electrodes were either embedded within or wrapped around the YSZ electrolyte. The electrical response of the sensors was collected via impedance spectroscopy under various operating conditions where gas concentrations ranged from 0 to 100 ppm NO and 1%-18% O₂ at temperatures varying from 600 to 700 °C. Gas diffusion appeared to be a rate-limiting mechanism in sensors where the electrode configuration resulted in longer diffusion pathways. The temperature dependence of the NO sensors studied was independent of the electrode configuration. Analysis of the impedance data, along with equivalent circuit modeling indicated the electrode configuration of the sensor effected gas and ionic transport pathways, capacitance behavior, and NO sensitivity.

Elucidating Complex Surface Reconstructions with Atomic-Resolution Scanning Tunneling Microscopy: Au(100)-Aqueous Electrochemical Interface

DTIC Science & Technology

1992-05-01

that unusually high-quality STM data of this type 5-7can be obtained at ordered gold -aqueous interfaces. Reconstruction is seen 2 to be triggered on...all three low-index gold surfaces by altering the potential to values corresponding to small (10-15 pC cm-2 ) negative surface electronic 5-7 charges...connections. The former was platinum and the latter was a freshly electrooxidized gold wire. All electrode potentials quoted here, however, are

First Principles Calculations on the Diffusion of Cu, Ag and Au Atoms or Aggregates on the Bulk and Surface of Titania

DTIC Science & Technology

2011-04-01

filament. The filament may be composed of the metal electrode which is transported into the insulator or due to the formation of sub-oxides. During the...possibility that ionic transport and red-ox processes are at the basis of the resistive switching. The idea is that the oxidation of the active metal...oxide layer and subsequent discard at the inert metal counter-electrode. This mechanism should lead to the formation of metal dendrimers inside the

Effect of electrode material on characteristics of non-volatile resistive memory consisting of Ag{sub 2}S nanoparticles

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jang, Jaewon, E-mail: j1jang@knu.ac.kr

2016-07-15

In this study, Ag{sub 2}S nanoparticles are synthesized and used as the active material for two-terminal resistance switching memory devices. Sintered Ag{sub 2}S films are successfully crystallized on plastic substrates with synthesized Ag{sub 2}S nanoparticles, after a relatively low-temperature sintering process (200 °C). After the sintering process, the crystallite size is increased from 6.8 nm to 80.3 nm. The high ratio of surface atoms to inner atoms of nanoparticles reduces the melting point temperature, deciding the sintering process temperature. In order to investigate the resistance switching characteristics, metal/Ag{sub 2}S/metal structures are fabricated and tested. The effect of the electrode materialmore » on the non-volatile resistive memory characteristics is studied. The bottom electrochemically inert materials, such as Au and Pt, were critical for maintaining stable memory characteristics. By using Au and Pt inert bottom electrodes, we are able to significantly improve the memory endurance and retention to more than 10{sup 3} cycles and 10{sup 4} sec, respectively.« less

The improvement of low-resistance and high-transmission ohmic contact to p-GaN by Zn + implantation

NASA Astrophysics Data System (ADS)

Zhao, Shirong; Shi, Ying; Li, Hongjian; He, Qingyao

2010-05-01

The electrical and optical characteristics of Zn + ion-implanted Ni/Au ohmic contacts to p-GaN were investigated. After the preparation of Ni/Au electrode on the surface of p-GaN, the metal/ p-GaN contact interface was doped by 35 keV Zn + implantation with fluences of 5 × 10 15-5 × 10 16 cm -2. Subsequent rapid thermal annealing of the implanted samples were carried in air at 200-400 °C for 5 min. Obvious improvements of the electrode contact characteristics were observed, i.e. the decrease of specific contact resistance and the increase of light transmittance. The lowest specific contact resistance of 5.46 × 10 -5 Ω cm 2 was achieved by 1 × 10 16 cm -2 Zn + implantation. The transmission enhancement of the electrodes was found as the annealing temperature rises. Together with the morphology and structure analyses of the contacts by scanning and transmission electron microscope, the corresponding mechanism for such an improvement was discussed.

Electrochemical Sensor Coating Based on Electrophoretic Deposition of Au-Doped Self-Assembled Nanoparticles.

PubMed

Zhang, Rongli; Zhu, Ye; Huang, Jing; Xu, Sheng; Luo, Jing; Liu, Xiaoya

2018-02-14

The electrophoretic deposition (EPD) of self-assembled nanoparticles (NPs) on the surface of an electrode is a new strategy for preparing sensor coating. By simply changing the deposition conditions, the electrochemical response for an analyte of deposited NPs-based coating can be controlled. This advantage can decrease the difference between different batches of sensor coating and ensure the reproducibility of each sensor. This work investigated the effects of deposition conditions (including deposition voltage, pH value of suspension, and deposition time) on the structure and the electrochemical response for l-tryptophan of sensor coating formed from Au-doped poly(sodium γ-glutamate) with pendant dopamine units nanohybrids (Au/γ-PGA-DA NBs) via the EPD method. The structure and thickness of the deposited sensor coating were measured by atomic force microscopy, which demonstrated that the structure and thickness of coating can be affected by the deposition voltage, the pH value of the suspension, and the deposition time. The responsive current for l-tryptophan of the deposited sensor coating were measured by differential pulse voltammetry, which showed that the responsive current value was affected by the structure and thickness of the deposited coating. These arguments suggested that a rich design-space for tuning the electrochemical response for analyte and a source of variability in the structure of sensor coating can be provided by the deposition conditions. When Au/γ-PGA-DA NBs were deposited on the electrode surface and formed a continuous coating with particle morphology and thinner thickness, the deposited sensor coating exhibited optimal electrochemical response for l-tryptophan.

Synthesis of a novel Au nanoparticles decorated Ni-MOF/Ni/NiO nanocomposite and electrocatalytic performance for the detection of glucose in human serum.

PubMed

Chen, Jingyuan; Xu, Qin; Shu, Yun; Hu, Xiaoya

2018-07-01

A nonenzymatic glucose electrochemical sensor was constructed based on Au nanoparticles (AuNPs) decorated Ni metal-organic-framework (MOF)/Ni/NiO nanocomposite. Ni-MOF/Ni/NiO nanocomposite was synthesized by one-step calcination of Ni-MOF. Then AuNPs were loaded onto the Ni-based nanocomposites' surface through electrostatic adsorption. Through characterization by transmission electron microscopy (TEM), high resolution TEM (HRTEM) and energy disperse spectroscopy (EDS) mapping, it is found that the AuNPs were well distributed on the surface of Ni-based nanocomposite. Cyclic voltammetric (CV) study showed the electrocatalytic activity of Au-Ni nanocomposite was highly improved after loading AuNPs onto it. Amperometric study demonstrated that the Au-Ni nanocomposites modified glassy carbon electrode (GCE) exhibited a high sensitivity of 2133.5 mA M -1 cm -2 and a wide linear range (0.4-900 μM) toward the oxidation of glucose with a detection limit as low as 0.1 μM. Moreover, the reproducibility, selectivity and stability of the sensor all exhibited outstanding performance. We applied the as-fabricated high performance sensor to measure the glucose levels in human serum and obtained satisfactory results. It is believed that AuNPs decorated Ni MOF/Ni/NiO nanocomposite provides a new platform for developing highly performance electrochemical sensors in practical applications. Copyright © 2018 Elsevier B.V. All rights reserved.

Ultrasensitive luminol electrochemiluminescence for protein detection based on in situ generated hydrogen peroxide as coreactant with glucose oxidase anchored AuNPs@MWCNTs labeling.

PubMed

Cao, Yaling; Yuan, Ruo; Chai, Yaqin; Mao, Li; Niu, Huan; Liu, Huijing; Zhuo, Ying

2012-01-15

In this study, an ultrasensitive luminol electrochemiluminescence (ECL) immunosensor was constructed using carboxyl group functionalized multi-walled carbon nanotubes (MWCNTs) as platform and glucose oxidase (GOD) supported on Au nanoparticles (AuNPs) decorated MWCNTs (AuNPs@MWCNTs-GOD) as labels. Firstly, using poly(ethylenimine) (PEI) as linkage reagents, AuNPs@MWCNTs were prepared and introduced for binding of the secondary antibody (Ab(2)) and glucose oxidase (GOD) with high loading amount and good biological activity due to the improved surface area of AuNPs@MWCNTs and excellent biocompatibility of AuNPs. Then the GOD and Ab(2) labeled AuNPs@MWCNTs were linked to the electrode surface via sandwich immunoreactions. These localized GOD and AuNPs amplified luminol ECL signals dramatically, which was achieved by efficient catalysis of the GOD and AuNPs towards the oxidation of glucose to in situ generate improved amount of hydrogen peroxide (H(2)O(2)) as coreactant and the enhancement of AuNPs to the ECL reaction of luminol-H(2)O(2). The experimental results demonstrated that the proposed immunosensor exhibited sensitive and stable response for the detection of α-1-fetoprotein (AFP), ranging from 0.0001 to 80 ng mL(-1) with a limit of detection down to 0.03 pg mL(-1) (S/N=3). With excellent stability, sensitivity, selectivity and simplicity, the proposed luminol ECL immunosensor showed great potential in clinical applications. Copyright © 2011 Elsevier B.V. All rights reserved.

Surface diffusion of a carbon-adatom on Au(110) surfaces

NASA Astrophysics Data System (ADS)

Kim, E.; Safavi-Naini, A.; Hite, D. A.; McKay, K. S.; Pappas, D. P.; Weck, P. F.; Sadeghpour, H. R.

We have investigated the surface diffusion of carbon-adatom on gold surfaces using density functional theory and detailed scanning probe microscopy. The decoherence of trapped-ion quantum gates due to heating of their motional modes is a fundamental science and engineering problem. In an effort to understand heating at the trap-electrode surfaces, we investigate the possible source of noise by focusing on the diffusion of carbon-containing adsorbates onto the Au(110) surface. In this study, we show how the diffusive motion of carbon adatom on gold surface significantly affects the energy landscape and adatom dipole moment variation. A simple model for the diffusion noise, which varies quadratically with the variation of the dipole moment, qualitatively reproduces the measured noise spectrum, and the estimate of the noise spectral density is in accord with measured values. Sandia National Laboratories is a multiprogram laboratory operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Company, for the United States Department of Energy's NNSA under Contract DE-AC04-94AL85000.

Photocatalytically Renewable Micro-electrochemical Sensor for Real-Time Monitoring of Cells.

PubMed

Xu, Jia-Quan; Liu, Yan-Ling; Wang, Qian; Duo, Huan-Huan; Zhang, Xin-Wei; Li, Yu-Tao; Huang, Wei-Hua

2015-11-23

Electrode fouling and passivation is a substantial and inevitable limitation in electrochemical biosensing, and it is a great challenge to efficiently remove the contaminant without changing the surface structure and electrochemical performance. Herein, we propose a versatile and efficient strategy based on photocatalytic cleaning to construct renewable electrochemical sensors for cell analysis. This kind of sensor was fabricated by controllable assembly of reduced graphene oxide (RGO) and TiO2 to form a sandwiching RGO@TiO2 structure, followed by deposition of Au nanoparticles (NPs) onto the RGO shell. The Au NPs-RGO composite shell provides high electrochemical performance. Meanwhile, the encapsulated TiO2 ensures an excellent photocatalytic cleaning property. Application of this renewable microsensor for detection of nitric oxide (NO) release from cells demonstrates the great potential of this strategy in electrode regeneration and biosensing. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graphene-multiwall carbon nanotube-gold nanocluster composites modified electrode for the simultaneous determination of ascorbic acid, dopamine, and uric acid.

PubMed

Liu, Xiaofang; Wei, Shaping; Chen, Shihong; Yuan, Dehua; Zhang, Wen

2014-08-01

In this paper, graphene-multiwall carbon nanotube-gold nanocluster (GP-MWCNT-AuNC) composites were synthesized and used as modifier to fabricate a sensor for simultaneous detection of ascorbic acid (AA), dopamine (DA), and uric acid (UA). The electrochemical behavior of the sensor was investigated by electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV) and differential pulse voltammetry (DPV) techniques. The combination of GP, MWCNTs, and AuNCs endowed the electrode with a large surface area, good catalytic activity, and high selectivity and sensitivity. The linear response range for simultaneous detection of AA, DA, and UA at the sensor were 120-1,701, 2-213, and 0.7-88.3 μM, correspondingly, and the detection limits were 40, 0.67, and 0.23 μM (S/N=3), respectively. The proposed method offers a promise for simple, rapid, selective, and cost-effective analysis of small biomolecules.

Electro-oxidation of methanol on gold in alkaline media: Adsorption characteristics of reaction intermediates studied using time resolved electro-chemical impedance and surface plasmon resonance techniques

NASA Astrophysics Data System (ADS)

Assiongbon, K. A.; Roy, D.

2005-12-01

Electro-catalytic oxidation of methanol is the anode reaction in direct methanol fuel cells. We have studied the adsorption characteristics of the intermediate reactants of this multistep reaction on a gold film electrode in alkaline solutions by combining surface plasmon resonance (SPR) measurements with Fourier transform electro-chemical impedance spectroscopy (FT-EIS). Methanol oxidation in this system shows no significant effects of "site poisoning" by chemisorbed CO. Our results suggest that OH - chemisorbed onto Au acts as a stabilizing agent for the surface species of electro-active methanol. Double layer charging/discharging and adsorption/desorption of OH - show more pronounced effects than adsorption/oxidation of methanol in controlling the surface charge density of the Au substrate. These effects are manifested in both the EIS and the SPR data, and serve as key indicators of the surface reaction kinetics. The data presented here describe the important role of adsorbed OH - in electro-catalysis of methanol on Au, and demonstrate how SPR and FT-EIS can be combined for quantitative probing of catalytically active metal-solution interfaces.

How voltage drops are manifested by lithium ion configurations at interfaces and in thin films on battery electrodes

DOE PAGES

Leung, Kevin; Leenheer, Andrew Jay

2015-04-09

Battery electrode surfaces are generally coated with electronically insulating solid films of thickness 1-50 nm. Both electrons and Li + can move at the electrode–surface film interface in response to the voltage, which adds complexity to the “electric double layer” (EDL). We also apply Density Functional Theory (DFT) to investigate how the applied voltage is manifested as changes in the EDL at atomic length scales, including charge separation and interfacial dipole moments. Illustrating examples include Li 3PO 4, Li 2CO 3, and Li xMn 2O 4 thin films on Au(111) surfaces under ultrahigh vacuum conditions. Adsorbed organic solvent molecules canmore » strongly reduce voltages predicted in vacuum. We propose that manipulating surface dipoles, seldom discussed in battery studies, may be a viable strategy to improve electrode passivation. We also distinguish the computed potential governing electrons, which is the actual or instantaneous voltage, and the “lithium cohesive energy”-based voltage governing Li content widely reported in DFT calculations, which is a slower-responding self-consistency criterion at interfaces. Furthermore, this distinction is critical for a comprehensive description of electrochemical activities on electrode surfaces, including Li + insertion dynamics, parasitic electrolyte decomposition, and electrodeposition at overpotentials.« less

Electric-field noise from carbon-adatom diffusion on a Au(110) surface: First-principles calculations and experiments

DOE PAGES

Kim, E.; Safavi-Naini, A.; Hite, D. A.; ...

2017-03-01

The decoherence of trapped-ion quantum bits due to heating of their motional modes is a fundamental science and engineering problem. This heating is attributed to electric-field noise arising from processes on the trap-electrode surfaces. In this work, we address the source of this noise by focusing on the diffusion of carbon-containing adsorbates on the surface of Au(110). We show by detailed scanned probe microscopy and density functional theory how the carbon adatom diffusion on the gold surface changes the energy landscape, and how the adatom dipole moment varies with the diffusive motion. Lastly, a simple model for the diffusion noise,more » which varies quadratically with the variation of the dipole moment, qualitatively reproduces the measured noise spectrum, and the estimate of the noise spectral density is in accord with measured values.« less

Electric-field noise from carbon-adatom diffusion on a Au(110) surface: First-principles calculations and experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kim, E.; Safavi-Naini, A.; Hite, D. A.

The decoherence of trapped-ion quantum bits due to heating of their motional modes is a fundamental science and engineering problem. This heating is attributed to electric-field noise arising from processes on the trap-electrode surfaces. In this work, we address the source of this noise by focusing on the diffusion of carbon-containing adsorbates on the surface of Au(110). We show by detailed scanned probe microscopy and density functional theory how the carbon adatom diffusion on the gold surface changes the energy landscape, and how the adatom dipole moment varies with the diffusive motion. Lastly, a simple model for the diffusion noise,more » which varies quadratically with the variation of the dipole moment, qualitatively reproduces the measured noise spectrum, and the estimate of the noise spectral density is in accord with measured values.« less

Memory operations in Au nanoparticle single-electron transistors with floating gate electrodes

NASA Astrophysics Data System (ADS)

Azuma, Yasuo; Sakamoto, Masanori; Teranishi, Toshiharu; Majima, Yutaka

2016-11-01

Floating gate memory operations are demonstrated in a single-electron transistor (SET) fabricated by a chemical assembly using the Au nanogap electrodes and the chemisorbed Au nanoparticles. By applying pulse voltages to the control gate, phase shifts were clearly and stably observed both in the Coulomb oscillations and in the Coulomb diamonds. Writing and erasing operations on the floating gate memory were reproducibly observed, and the charges on the floating gate electrodes were maintained for at least 12 h. By considering the capacitance of the floating gate electrode, the number of electrons in the floating gate electrode was estimated as 260. Owing to the stability of the fabricated SET, these writing and erasing operations on the floating gate memory can be applied to reconfigurable SET circuits fabricated by a chemically assembled technique.

A comparative Study of Aptasensor Vs Immunosensor for Label-Free PSA Cancer Detection on GQDs-AuNRs Modified Screen-Printed Electrodes.

PubMed

Srivastava, Monika; Nirala, Narsingh R; Srivastava, S K; Prakash, Rajiv

2018-01-31

Label-free and sensitive detection of PSA (Prostate Specific Antigen) is still a big challenge in the arena of prostate cancer diagnosis in males. We present a comparative study for label-free PSA aptasensor and PSA immunosensor for the PSA-specific monoclonal antibody, based on graphene quantum dots-gold nanorods (GQDs-AuNRs) modified screen-printed electrodes. GQDs-AuNRs composite has been synthesized and used as an electro-active material, which shows fast electron transfer and catalytic property. Aptamer or anti-PSA has immobilized onto the surface of modified screen printed electrodes. Three techniques are used simultaneously, viz. cyclic voltammetry (CV), differential pulse voltammetry (DPV) and electrochemical impedence spectroscopy (EIS) to investigate the analytical performance of both PSA aptasensor and PSA immunosensor with its corresponding PSA antigen. Under optimum conditions, both sensors show comparable results with an almost same limit of detection (LOD) of 0.14 ng mL -1 . The results developed with aptasensor and anti-PSA is also checked through the detection of PSA in real samples with acceptable results. Our study suggests some advantages of aptasensor in terms of better stability, simplicity and cost effectiveness. Further our present work shows enormous potential of our developed sensors for real application using voltammetric and EIS techniques simultaneous to get reliable detection of the disease.

Design an aptasensor based on structure-switching aptamer on dendritic gold nanostructures/Fe3O4@SiO2/DABCO modified screen printed electrode for highly selective detection of epirubicin.

PubMed

Hashkavayi, Ayemeh Bagheri; Raoof, Jahan Bakhsh

2017-05-15

The present work describes a label free electrochemical aptasensor for selective detection of epirubicin. In this project, 5'-thiole terminated aptamer was self-assembled on carbon screen printed electrode, which modified with electrodeposited gold nanoparticles on magnetic double-charged diazoniabicyclo [2.2.2] octane dichloride silica hybrid (Fe 3 O 4 @SiO 2 /DABCO) by Au-S bond. The interactions of epirubicin with aptamer on the AuNPs/Fe 3 O 4 @SiO 2 /DABCO/SPE have been studied by cyclic voltammetry, linear sweep voltammetry and electrochemical impedance spectroscopy. Under optimized conditions, the peak current of epirubicin increased linearly with increasing epirubicin concentration, due to the switching in the aptamer conformation and formation of aptamer- epirubicin complex instead of aptamer on the modified electrode surface. The Apt/AuNPs/Fe 3 O 4 @SiO 2 /DABCO/SPE is sensitive, selective and has two linear range from 0.07µM to 1.0µM and 1.0µM to 21.0µM with a detection limit of 0.04µM. The applicability of the aptasensor was successfully assessed by determination of epirubicin in a human blood serum sample. Copyright © 2017 Elsevier B.V. All rights reserved.

Au nanoparticles/hollow molybdenum disulfide microcubes based biosensor for microRNA-21 detection coupled with duplex-specific nuclease and enzyme signal amplification.

PubMed

Shuai, Hong-Lei; Huang, Ke-Jing; Chen, Ying-Xu; Fang, Lin-Xia; Jia, Meng-Pei

2017-03-15

An ultrasensitive electrochemical biosensor for detecting microRNAs is fabricated based on hollow molybdenum disulfide (MoS 2 ) microcubes. Duplex-specific nuclease, enzyme and electrochemical-chemical-chemical redox cycling are used for signal amplification. Hollow MoS 2 microcubes constructed by ultrathin nanosheets are synthesized by a facile template-assisted strategy and used as supporting substrate. For biosensor assembling, biotinylated ssDNA capture probes are first immobilized on Au nanoparticles (AuNPs)/MoS 2 modified electrode in order to combine with streptavidin-conjugated alkaline phosphatase (SA-ALP). When capture probes hybridize with miRNAs, duplex-specific nuclease cleaves the formative duplexes. At the moment, the biotin group strips from the electrode surface and SA-ALP is incapacitated to attach onto electrode. Then, ascorbic acids induce the electrochemical-chemical-chemical redox cycling to produce electrochemical response in the presence of ferrocene methanol and tris (2-carboxyethyl) phosphine. Under optimum conditions, the proposed biosensor shows a good linear relationship between the current variation and logarithm of the microRNAs concentration ranging from 0.1fM to 0.1pM with a detection limit of 0.086fM (S/N=3). Furthermore, the biosensor is successfully applied to detect target miRNA-21 in human serum samples. Copyright © 2016 Elsevier B.V. All rights reserved.

Novel amperometric glucose biosensor based on MXene nanocomposite.

PubMed

Rakhi, R B; Nayak, Pranati; Xia, Chuan; Alshareef, Husam N

2016-11-10

A biosensor platform based on Au/MXene nanocomposite for sensitive enzymatic glucose detection is reported. The biosensor leverages the unique electrocatalytic properties and synergistic effects between Au nanoparticles and MXene sheets. An amperometric glucose biosensor is fabricated by the immobilization of glucose oxidase (GOx) enzyme on Nafion solubilized Au/ MXene nanocomposite over glassy carbon electrode (GCE). The biomediated Au nanoparticles play a significant role in facilitating the electron exchange between the electroactive center of GOx and the electrode. The GOx/Au/MXene/Nafion/GCE biosensor electrode displayed a linear amperometric response in the glucose concentration range from 0.1 to 18 mM with a relatively high sensitivity of 4.2 μAmM -1 cm -2 and a detection limit of 5.9 μM (S/N = 3). Furthermore, the biosensor exhibited excellent stability, reproducibility and repeatability. Therefore, the Au/MXene nanocomposite reported in this work is a potential candidate as an electrochemical transducer in electrochemical biosensors.

Novel amperometric glucose biosensor based on MXene nanocomposite

PubMed Central

Rakhi, R. B.; Nayuk, Pranati; Xia, Chuan; Alshareef, Husam N.

2016-01-01

A biosensor platform based on Au/MXene nanocomposite for sensitive enzymatic glucose detection is reported. The biosensor leverages the unique electrocatalytic properties and synergistic effects between Au nanoparticles and MXene sheets. An amperometric glucose biosensor is fabricated by the immobilization of glucose oxidase (GOx) enzyme on Nafion solubilized Au/ MXene nanocomposite over glassy carbon electrode (GCE). The biomediated Au nanoparticles play a significant role in facilitating the electron exchange between the electroactive center of GOx and the electrode. The GOx/Au/MXene/Nafion/GCE biosensor electrode displayed a linear amperometric response in the glucose concentration range from 0.1 to 18 mM with a relatively high sensitivity of 4.2 μAmM−1 cm−2 and a detection limit of 5.9 μM (S/N = 3). Furthermore, the biosensor exhibited excellent stability, reproducibility and repeatability. Therefore, the Au/MXene nanocomposite reported in this work is a potential candidate as an electrochemical transducer in electrochemical biosensors. PMID:27830757

Fabrication and Characterization of a Stabilized Thin Film Ag/AgCl Reference Electrode Modified with Self-Assembled Monolayer of Alkane Thiol Chains for Rapid Biosensing Applications.

PubMed

Rahman, Tanzilur; Ichiki, Takanori

2017-10-13

The fabrication of miniaturized electrical biosensing devices can enable the rapid on-chip detection of biomarkers such as miRNA molecules, which is highly important in early-stage cancer detection. The challenge in realizing such devices remains in the miniaturization of the reference electrodes, which is an integral part of electrical detection. Here, we report on a novel thin film Ag/AgCl reference electrode (RE) that has been fabricated on top of a Au-sputtered glass surface, which was coated with a self-assembled monolayer (SAM) of 6-mercepto-1-hexanol (MCH). The electrode showed very little measurement deviation (-1.5 mv) from a commercial Ag/AgCl reference electrode and exhibited a potential drift of only ± 0.2 mV/h. In addition, the integration of this SAM-modified microfabricated thin film RE enabled the rapid detection (<30 min) of miRNA (let-7a). The electrode can be integrated seamlessly into a microfluidic device, allowing the highly stable and fast measurement of surface potential and is expected to be very useful for the development of miniature electrical biosensors.

Modified Au nanoparticles-imprinted sol-gel, multiwall carbon nanotubes pencil graphite electrode used as a sensor for ranitidine determination.

PubMed

Rezaei, B; Lotfi-Forushani, H; Ensafi, A A

2014-04-01

A new, simple, and disposable molecularly imprinted electrochemical sensor for the determination of ranitidine was developed on pencil graphite electrode (PGE) via cyclic voltammetry (CV). The PGEs were coated with MWCNTs containing the carboxylic functional group (f-MWCNTs), imprinted with sol-gel and Au nanoparticle (AuNPs) layers (AuNP/MIP-sol-gel/f-MWCNT/PGE), respectively, to enhance the electrode's electrical transmission and sensitivity. The thin film of molecularly imprinted sol-gel polymers with specific binding sites for ranitidine was cast on modified PGE by electrochemical deposition. The AuNP/MIP-sol-gel/f-MWCNT/PGE thus developed was characterized by electrochemical impedance spectroscopy (EIS) and CV. The interaction between the imprinted sensor and the target molecule was also observed on the electrode by measuring the current response of 5.0mMK3[Fe(CN)6] solution as an electrochemical probe. The pick currents of ranitidine increased linearly with concentration in the ranges of 0.05 to 2.0μM, with a detection limit of (S/N=3) 0.02μM. Finally, the modified electrode was successfully employed to determine ranitidine in human urine samples. Copyright © 2014 Elsevier B.V. All rights reserved.

Space-confined fabrication of silver nanodendrites and their enhanced SERS activity

NASA Astrophysics Data System (ADS)

Wang, Shuqi; Xu, Li-Ping; Wen, Yongqiang; Du, Hongwu; Wang, Shutao; Zhang, Xueji

2013-05-01

Here we report a controllable method based on electrodeposition to fabricate Ag nanodendrites (NDs) on a microwell patterned electrode. The microwell patterns on the ITO electrode are fabricated via the microcontact printing technique. By varying the microwell size and electrodeposition time, the morphology of metal deposits on the microwell patterned ITO electrode can be tuned from boulders to dendrites. At the edge of the microwells, the current density was strengthened, which incurs rapid nucleation. The nucleus develops into dendrites because of Mullins-Sekerka instability. However, only boulders were observed at the center of microwells. By reducing the size of the microwells, only NDs were fabricated due to the edge effect. On the basis of understanding the underlying mechanism for dendritic growth in a confined space, our method is used for fabricating other noble metal (Au, Pt) nanodendrites. The controllable synthesis of Au and Pt NDs indicates the universality of this method. Compared with Ag film obtained from electron beam evaporation, the as-prepared Ag NDs exhibit highly enhanced surface-enhanced Raman scattering (SERS) sensitivity when they are used to detect rhodamine 6G (R6G). This approach provides a very controllable, reliable and general way for space-confined fabricating the noble metal nanodendrite arrays which show great promise in catalysis, sensing, biomedicine, electronic and magnetic devices.Here we report a controllable method based on electrodeposition to fabricate Ag nanodendrites (NDs) on a microwell patterned electrode. The microwell patterns on the ITO electrode are fabricated via the microcontact printing technique. By varying the microwell size and electrodeposition time, the morphology of metal deposits on the microwell patterned ITO electrode can be tuned from boulders to dendrites. At the edge of the microwells, the current density was strengthened, which incurs rapid nucleation. The nucleus develops into dendrites because of Mullins-Sekerka instability. However, only boulders were observed at the center of microwells. By reducing the size of the microwells, only NDs were fabricated due to the edge effect. On the basis of understanding the underlying mechanism for dendritic growth in a confined space, our method is used for fabricating other noble metal (Au, Pt) nanodendrites. The controllable synthesis of Au and Pt NDs indicates the universality of this method. Compared with Ag film obtained from electron beam evaporation, the as-prepared Ag NDs exhibit highly enhanced surface-enhanced Raman scattering (SERS) sensitivity when they are used to detect rhodamine 6G (R6G). This approach provides a very controllable, reliable and general way for space-confined fabricating the noble metal nanodendrite arrays which show great promise in catalysis, sensing, biomedicine, electronic and magnetic devices. Electronic supplementary information (ESI) available: SEM images. See DOI: 10.1039/c3nr00313b

Surface-enhanced molecularly imprinted electrochemiluminescence sensor based on Ru@SiO2 for ultrasensitive detection of fumonisin B1.

PubMed

Zhang, Wei; Xiong, Huiwen; Chen, Miaomiao; Zhang, Xiuhua; Wang, Shengfu

2017-10-15

A novel molecularly imprinted electrochemiluminescence (MIP-ECL) sensor based on Ru(bpy) 3 2+ -doped silica nanoparticles (Ru@SiO 2 NPs) is developed for highly sensitive detection of fumonisin B 1 (FB 1 ). Gold-nanoparticles (AuNPs), Ru@SiO 2 NPs with chitosan (CS) composites and a molecularly imprinted polymer (MIP) are assembled on a glassy carbon electrode (GCE) to fabricate an ECL platform step by step. AuNPs could greatly promote the ECL intensity and improve the analytical sensitivity according to the localized surface plasmon resonance (LSPR) and the electrochemical effect. In this surface-enhanced electrochemiluminescence (SEECL) system, AuNPs work as the LSPR source to improve the ECL intensity and Ru@SiO 2 NPs are used as ECL luminophores. In the phosphate buffer solution (PBS), the evident anodic ECL of Ru@SiO 2 on the above working electrode is observed in the presence of the template molecule fumonisin B 1 (FB 1 ), which could act as the coreactant of Ru@SiO 2 NPs due to the amino group of FB 1 . When the template molecules were eluted from the MIP, little coreactant was left, resulting in an apparent decrease of ECL signal. After the MIP-ECL sensor was incubated in FB 1 solution, the template molecules rebound to the MIP surface, leading to the enhancement of ECL signal again. On the basis of these results, a facile MIP-ECL sensor has been successfully fabricated, which exhibited a linear range from 0.001 to 100ngmL -1 with a detection limit of 0.35pgmL -1 for FB 1 . Moreover, the proposed MIP-ECL sensor displayed an excellent application in real samples. Copyright © 2017 Elsevier B.V. All rights reserved.

An ultrasensitive hollow-silica-based biosensor for pathogenic Escherichia coli DNA detection.

PubMed

Ariffin, Eda Yuhana; Lee, Yook Heng; Futra, Dedi; Tan, Ling Ling; Karim, Nurul Huda Abd; Ibrahim, Nik Nuraznida Nik; Ahmad, Asmat

2018-03-01

A novel electrochemical DNA biosensor for ultrasensitive and selective quantitation of Escherichia coli DNA based on aminated hollow silica spheres (HSiSs) has been successfully developed. The HSiSs were synthesized with facile sonication and heating techniques. The HSiSs have an inner and an outer surface for DNA immobilization sites after they have been functionalized with 3-aminopropyltriethoxysilane. From field emission scanning electron microscopy images, the presence of pores was confirmed in the functionalized HSiSs. Furthermore, Brunauer-Emmett-Teller (BET) analysis indicated that the HSiSs have four times more surface area than silica spheres that have no pores. These aminated HSiSs were deposited onto a screen-printed carbon paste electrode containing a layer of gold nanoparticles (AuNPs) to form a AuNP/HSiS hybrid sensor membrane matrix. Aminated DNA probes were grafted onto the AuNP/HSiS-modified screen-printed electrode via imine covalent bonds with use of glutaraldehyde cross-linker. The DNA hybridization reaction was studied by differential pulse voltammetry using an anthraquinone redox intercalator as the electroactive DNA hybridization label. The DNA biosensor demonstrated a linear response over a wide target sequence concentration range of 1.0×10 -12 -1.0×10 -2 μM, with a low detection limit of 8.17×10 -14 μM (R 2 = 0.99). The improved performance of the DNA biosensor appeared to be due to the hollow structure and rough surface morphology of the hollow silica particles, which greatly increased the total binding surface area for high DNA loading capacity. The HSiSs also facilitated molecule diffusion through the silica hollow structure, and substantially improved the overall DNA hybridization assay. Graphical abstract Step-by-step DNA biosensor fabrication based on aminated hollow silica spheres.

Determination of low levels of cadmium ions by the under potential deposition on a self-assembled monolayer on gold electrode.

PubMed

Noyhouzer, Tomer; Mandler, Daniel

2011-01-17

The electrochemical determination of low levels of Cd using a self-assembled monolayer (SAM) modified Au electrode is reported. Determination was based on the stripping of Cd, which was deposited by under potential deposition (UPD). A series of short alkanethiol SAMs bearing different end groups, i.e., sulfonate, carboxylate and ammonium, were examined. Lowest level of detection (ca. 50 ngL(-1)) was achieved with a 3-mercaptopropionic acid (MPA) monolayer using subtractive anodic square wave voltammetry (SASV). Additional surface methods, namely, reductive desorption and X-ray photoelectron spectroscopy, were applied to determine the interfacial structure of the electrodeposited Cd on the modified electrodes. We conclude that the deposited Cd forms a monoatomic layer, which bridges between the gold surface and the alkanethiol monolayer associating with both the gold and the sulfur atoms. Copyright © 2010 Elsevier B.V. All rights reserved.

Vertically aligned carbon nanotube probes for monitoring blood cholesterol

NASA Astrophysics Data System (ADS)

Roy, Somenath; Vedala, Harindra; Choi, Wonbong

2006-02-01

Detection of blood cholesterol is of great clinical significance. The amperometric detection technique was used for the enzymatic assay of total cholesterol. Multiwall carbon nanotubes (MWNTs), vertically aligned on a silicon platform, promote heterogeneous electron transfer between the enzyme and the working electrode. Surface modification of the MWNT with a biocompatible polymer, polyvinyl alcohol (PVA), converted the hydrophobic nanotube surface into a highly hydrophilic one, which facilitates efficient attachment of biomolecules. The fabricated working electrodes showed a linear relationship between cholesterol concentration and the output signal. The efficacy of the multiwall carbon nanotubes in promoting heterogeneous electron transfer was evident by distinct electrochemical peaks and higher signal-to-noise ratio as compared to the Au electrode with identical enzyme immobilization protocol. The selectivity of the cholesterol sensor in the presence of common interferents present in human blood, e.g. uric acid, ascorbic acid and glucose, is also reported.

Potential of Zero Charge and Its Temperature Derivative for Au(111) Electrode|Alkanethiol SAM|1.0 M Aqueous Electrolyte Solution Interfaces: Impact of Electrolyte Solution Ionic Strength and Its Effect on the Structure of the Modified Electrode|Electrolyte Solution Interface

DOE PAGES

Smalley, John F.

2017-04-06

In this study, we demonstrate how small and rapid temperature perturbations (produced by the indirect laser-induced temperature jump (ILIT) technique) of solid metal electrode|electrolyte solution interfaces may be used to determine the potential of zero (total) charge (E pzc) and its temperature derivativemore » $$\\left(\\frac{dEpzc}{dT}\\right)$$ of Au(111) electrode surfaces modified by alkanethiol self-assembled monolayers in contact with high ionic strength (i.e., 1.0 M) aqueous electrolyte solutions. The E pzc’s measured for two different types of SAMs (made from either HS(CH 2) n-1CH 3 (5 ≤ n ≤ 12, E pzc = -(0.99 ± 0.12) V vs SSCE) or HS(CH 2) nOH (3 ≤ n ≤ 16, E pzc = (0.46 ± 0.22) V vs SSCE)) are considerably different than those measured previously at much lower electrolyte solution ionic strengths. For mixed monolayers made from both HS(CH 2) n-1CH 3 and HS(CH 2) nFc (where Fc refers to ferrocene), the difference in Epzc decreases as a function of the surface concentration of the Fc moiety (i.e., [Fc]), and it completely disappears at a surprisingly small [Fc] (~4.0 × 10 –11 mol cm –2). These observations for the Au(111)|hydrophobic (neat and mixed) SAM|aqueous electrolyte solution interfaces, along with the surface potentials (g Sml(dip)) evaluated for the contacting electrolyte solution surfaces of these interfaces, are consistent with a structure for the water molecule components of these surfaces where there is a net orientation of the dipoles of these molecules. Accordingly, the negative (oxygen) ends of these molecules point toward the SAM surface. The positive values of g Sml(dip) evaluated for hydrophilic SAM (e.g., made from HS(CH 2) nOH)|aqueous electrolyte solution interfaces) also indicate that the structure of these interfaces is similar to that of the hydrophobic interfaces. However, g Sml(dip) decreases with increasing ionic strength for the hydrophilic interfaces, while it increases with increasing ionic strength for the hydrophobic interfaces. The data (and calculations) reported in the present work and other studies of hydrophobic (and hydrophilic)|aqueous solution interfaces are as yet insufficient to support a complete explanation for the effects of ionic strength observed in the present study. Nevertheless, an analysis based upon the value of $$\\left(\\frac{dEpzc}{dT}\\right)$$ (= (0.51 ± 0.12) mV/K, essentially the same for SAMs made from both HS(CH 2) n-1CH 3 and HS(CH 2) nOH), determined in the present study provides a further indication that upon formation of the SAM there is a partial charge transfer of electrons from the relevant gold atoms on the Au(111) surface to the sulfur atoms of the alkanethiols.« less

Enhanced electrocatalytic activity of the Au-electrodeposited Pt nanoparticles-coated conducting oxide for the quantum dot-sensitized solar cells

NASA Astrophysics Data System (ADS)

Yoon, Yeung-Pil; Kim, Jae-Hong; Kang, Soon-Hyung; Kim, Hyunsoo; Choi, Chel-Jong; Kim, Kyong-Kook; Ahn, Kwang-Soon

2014-08-01

Au was electrodeposited potentiostatically at 0.3 V for 5 min on nanoporous Pt nanoparticle-coated F-doped SnO2 (FTO/Pt) substrates. For comparison, Au-electrodeposited FTO (FTO/Au) and Au-uncoated FTO/Pt were prepared. FTO/Au showed large-sized Au clusters dispersed sparsely over FTO, which resulted in lower electrocatalytic activity than FTO/Pt. In contrast, FTO/Pt exhibited poor stability unlike FTO/Au due to poisoning by the adsorption of sulfur species. The Au-electrodeposited FTO/Pt (FTO/Pt/Au) consisted of small Au clusters deposited over the entire area of Pt due to the effective Au nucleation provided by nanoporous metallic Pt. FTO/Pt/Au exhibited enhanced electrocatalytic activity and excellent stability because the small Au particles well-dispersed over the nanoporous metallic Pt network provided numerous electrochemical reaction sites, and the Pt surface was not exposed to the electrolyte. When FTO/Pt/Au was used as the counter electrode (CE) of a quantum dot-sensitized solar cell, the significantly enhanced electrocatalytic activity of the FTO/Pt/Au CE facilitated the reduction reaction of Sn2- + 2e- (CE) → Sn-12- + S2- at the CE/electrolyte interface, resulting in a significantly hindered recombination reaction, Sn2- + 2e- (TiO2 in the photoanode) → Sn-12- + S2-, and significantly improved overall energy conversion efficiency.

Ultrasensitive electroanalytical tool for detecting, sizing, and evaluating the catalytic activity of platinum nanoparticles.

PubMed

Dasari, Radhika; Robinson, Donald A; Stevenson, Keith J

2013-01-16

Here we describe a very simple, reliable, low-cost electrochemical approach to detect single nanoparticles (NPs) and evaluate NP size distributions and catalytic activity in a fast and reproducible manner. Single NPs are detected through an increase in current caused by electrocatalytic oxidation of N(2)H(4) at the surface of the NP when it contacts a Hg-modified Pt ultramicroelectrode (Hg/Pt UME). Once the NP contacts the Hg/Pt UME, Hg poisons the Pt NP, deactivating the N(2)H(4) oxidation reaction. Hence, the current response is a "spike" that decays to the background current level rather than a stepwise "staircase" response as previously described for a Au UME. The use of Hg as an electrode material has several quantitative advantages including suppression of the background current by 2 orders of magnitude over a Au UME, increased signal-to-noise ratio for detection of individual collisions, precise integration of current transients to determine charge passed and NP size, reduction of surface-induced NP aggregation and electrode fouling processes, and reproducible and renewable electrodes for routine detection of catalytic NPs. The NP collision frequency was found to scale linearly with the NP concentration (0.016 to 0.024 pM(-1)s(-1)). NP size distributions of 4-24 nm as determined from the current-time transients correlated well with theory and TEM-derived size distributions.

Effects of Different Materials Used for Internal Floating Electrode on the Photovoltaic Properties of Tandem Type Organic Solar Cell

NASA Astrophysics Data System (ADS)

Triyana, Kuwat; Yasuda, Takeshi; Fujita, Katsuhiko; Tsutsui, Tetsuo

2004-04-01

Three thin heterojunctions sandwiched between indium tin oxide (ITO) and the top electrode as triple-heterojunction organic solar cells have been fabricated. Each heterojunction cell consists of CuPc as a donor layer and perilene tetracrboxylic-bis-benzimidazole (PTCBI) as an acceptor layer. Ultra thin (1 nm average thickness) layers of Ag or Au have been inserted between two heterojunctions as an internal electrode. Ag and Au were chosen as materials both for internal floating and top electrodes. Influences of different deposition sequences of the organic layer in each heterojunction cell and different electrode materials were also investigated. The optimum devices were obtained when the same material was used both as an internal electrode and a top electrode. When the deposition sequence of the heterojunction is PTCBI/CuPc, the most suitable electrode is Au and the ITO is negative relative to the top electrode. Meanwhile, Ag is suitable for an electrode when the deposition sequence is CuPc/PTCBI. In this second deposition sequence, the ITO is positive relative to the top electrode. The open circuit voltage (Voc) of both optimum devices is on the order of 1.35-1.5 V. These values are approximately three times higher than that in single-heterojunction organic solar cells.

A novel material screening platform for nanoporous gold-based neural electrodes

NASA Astrophysics Data System (ADS)

Chapman, Christopher Abbott Reece

Neural-electrical interfaces have emerged in the past decades as a promising modality to facilitate the understanding of the electropathophysiology of neurological disorders as well as the normal functioning of the central nervous system, and enable the treatment of neurological defects through electrical stimulation or electrically-controlled drug delivery. However, chronically implanted electrodes face a myriad of design challenges, including their coupling to neural tissue (biocompatibility), small form factor requirement, and their electrical properties (maintaining a low electrical impedance). Planar electrode materials such as planar platinum and gold experience a large increase in electrical impedance when electrode dimensions are reduced to increase spatial resolution of neural recordings. A decrease in electrode surface area reduces the total capacitance of the electrode double layer resulting in an increase in electrode impedance. This high impedance can reduce the signal amplitude and increase the thermal noise, resulting in degradation of signal-to-noise ratio. Conventionally, this increase in electrical impedance at small electrode dimensions has been mitigated by coatings with rough morphologies such as platinum black, conducting polymers, and titanium nitride. Porous surfaces have high effective surface area enabling low impedance at small electrode dimensions. However, achieving long-term stability of cellular coupling to the electrode surface has remained difficult. Designing electrodes that can physically couple with neurons successfully and maintain low impedance at small electrode dimensions necessitates consideration of novel electrode coatings, such as carbon nanotubes and gold nanopillars. Another promising material, and focus of this proposal, is thin film nanoporous gold (np-Au). Nanoporous gold is a promising material for addressing these limitations because of its inherently large effective surface area allows for lower impedances at small form factors, and its modifiable surface morphology can be used to control cell-electrode coupling. Additionally, thin film nanoporous gold is fabricated by traditional microfabrication methods, and thus can be directly adopted by the current state-of-the-art neural electrode fabrication processes. All these properties make thin film nanoporous gold a promising candidate for use in neural electrode surfaces. This dissertation seeks to characterize both the morphological and the electrical response of neural cells to thin film nanoporous gold morphologies using an in vitro electrode morphology screening platform. The specific aims for this proposal are to: (i) develop a electrode morphology library that displays varying topographies to study structure-property relationships of thin film nanoporous gold and cellular response, (ii) characterize neural cell response to identified nanoporous gold topographies that reduce adverse tissue response in vitro, and (iii) develop an electrophysiology platform to characterize neural coupling to each identified nanoporous gold topography.

Electrochemical DNA biosensor based on the BDD nanograss array electrode.

PubMed

Jin, Huali; Wei, Min; Wang, Jinshui

2013-04-10

The development of DNA biosensor has attracted considerable attention due to their potential applications, including gene analysis, clinical diagnostics, forensic study and more medical applications. Using electroactive daunomycin as an indicator, the hybridization detection was measured by differential pulse voltammetry in this study. Electrochemical DNA biosensor was developed based on the BDD film electrode (fBDD) and BDD nanograss array electrode (nBDD). In comparison with fBDD and AuNPs/CA/fBDD electrode, the lower semicircle diameter of electrochemical impedance spectroscopy obtained on nBDD and AuNPs/CA/nBDD electrode indicated that the presence of nanograss array improved the reactive site, reduced the interfacial resistance, and made the electron transfer easier. Using electroactive daunomycin as an indicator, the hybridization detection was measured by differential pulse voltammetry. The experimental results demonstrated that the prepared AuNPs/CA/nBDD electrode was suitable for DNA hybridization with favorable performance of faster response, higher sensitivity, lower detection limit and satisfactory selectivity, reproducibility and stability.

Electrochemical DNA biosensor based on the BDD nanograss array electrode

PubMed Central

2013-01-01

Background The development of DNA biosensor has attracted considerable attention due to their potential applications, including gene analysis, clinical diagnostics, forensic study and more medical applications. Using electroactive daunomycin as an indicator, the hybridization detection was measured by differential pulse voltammetry in this study. Results Electrochemical DNA biosensor was developed based on the BDD film electrode (fBDD) and BDD nanograss array electrode (nBDD). In comparison with fBDD and AuNPs/CA/fBDD electrode, the lower semicircle diameter of electrochemical impedance spectroscopy obtained on nBDD and AuNPs/CA/nBDD electrode indicated that the presence of nanograss array improved the reactive site, reduced the interfacial resistance, and made the electron transfer easier. Using electroactive daunomycin as an indicator, the hybridization detection was measured by differential pulse voltammetry. Conclusions The experimental results demonstrated that the prepared AuNPs/CA/nBDD electrode was suitable for DNA hybridization with favorable performance of faster response, higher sensitivity, lower detection limit and satisfactory selectivity, reproducibility and stability. PMID:23575250

Electrochemical synthesis of mesoporous Pt-Au binary alloys with tunable compositions for enhancement of electrochemical performance.

PubMed

Yamauchi, Yusuke; Tonegawa, Akihisa; Komatsu, Masaki; Wang, Hongjing; Wang, Liang; Nemoto, Yoshihiro; Suzuki, Norihiro; Kuroda, Kazuyuki

2012-03-21

Mesoporous Pt-Au binary alloys were electrochemically synthesized from lyotropic liquid crystals (LLCs) containing corresponding metal species. Two-dimensional exagonally ordered LLC templates were prepared on conductive substrates from diluted surfactant solutions including water, a nonionic surfactant, ethanol, and metal species by drop-coating. Electrochemical synthesis using such LLC templates enabled the preparation of ordered mesoporous Pt-Au binary alloys without phase segregation. The framework composition in the mesoporous Pt-Au alloy was controlled simply by changing the compositional ratios in the precursor solution. Mesoporous Pt-Au alloys with low Au content exhibited well-ordered 2D hexagonal mesostructures, reflecting those of the original templates. With increasing Au content, however, the mesostructural order gradually decreased, thereby reducing the electrochemically active surface area. Wide-angle X-ray diffraction profiles, X-ray photoelectron spectra, and elemental mapping showed that both Pt and Au were atomically distributed in the frameworks. The electrochemical stability of mesoporous Pt-Au alloys toward methanol oxidation was highly improved relative to that of nonporous Pt and mesoporous Pt films, suggesting that mesoporous Pt-Au alloy films are potentially applicable as electrocatalysts for direct methanol fuel cells. Also, mesoporous Pt-Au alloy electrodes showed a highly sensitive amperometric response for glucose molecules, which will be useful in next-generation enzyme-free glucose sensors.

Ultrasensitive cardiac troponin I antibody based nanohybrid sensor for rapid detection of human heart attack.

PubMed

Bhatnagar, Deepika; Kaur, Inderpreet; Kumar, Ashok

2017-02-01

An ultrasensitive cardiac troponin I antibody conjugated with graphene quantum dots (GQD) and polyamidoamine (PAMAM) nanohybrid modified gold electrode based sensor was developed for the rapid detection of heart attack (myocardial infarction) in human. Screen printed gold (Au) electrode was decorated with 4-aminothiophenol for amine functionalization of the Au surface. These amino groups were further coupled with carboxyl functionalities of GQD with EDC-NHS reaction. In order to enhance the sensitivity of the sensor, PAMAM dendrimer was successively embedded on GQD through carbodiimide coupling to provide ultra-high surface area for antibody immobilization. The activated cardiac troponin I (cTnI) monoclonal antibody was immobilized on PAMAM to form nanoprobe for sensing specific heart attack marker cTnI. Various concentrations of cardiac marker, cTnI were electrochemically measured using cyclic voltammetry (CV) and differential pulse voltammetry (DPV) in human blood serum. The modifications on sensor surface were characterized by FTIR and AFM techniques. The sensor is highly specific to cTnI and showed negligible response to non-specific antigens. The sensitivity of the sensor was 109.23μAcm -2 μg -1 and lower limit of detection of cTnI was found 20fgmL -1 . Copyright © 2016 Elsevier B.V. All rights reserved.

Electrodeposition of gold-platinum alloy nanoparticles on ionic liquid-chitosan composite film and its application in fabricating an amperometric cholesterol biosensor.

PubMed

Safavi, Afsaneh; Farjami, Fatemeh

2011-01-15

An electrodeposition method was applied to form gold-platinum (AuPt) alloy nanoparticles on the glassy carbon electrode (GCE) modified with a mixture of an ionic liquid (IL) and chitosan (Ch) (AuPt-Ch-IL/GCE). AuPt nanoparticles were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and electrochemical methods. AuPt-Ch-IL/GCE electrocatalyzed the reduction of H(2)O(2) and thus was suitable for the preparation of biosensors. Cholesterol oxidase (ChOx) was then, immobilized on the surface of the electrode by cross-linking ChOx and chitosan through addition of glutaraldehyde (ChOx/AuPt-Ch-IL/GCE). The fabricated biosensor exhibited two wide linear ranges of responses to cholesterol in the concentration ranges of 0.05-6.2 mM and 6.2-11.2 mM. The sensitivity of the biosensor was 90.7 μA mM(-1) cm(-2) and the limit of detection was 10 μM of cholesterol. The response time was less than 7 s. The Michaelis-Menten constant (K(m)) was found as 0.24 mM. The effect of the addition of 1 mM ascorbic acid and glucose was tested on the amperometric response of 0.5 mM cholesterol and no change in response current of cholesterol was observed. Copyright © 2010 Elsevier B.V. All rights reserved.

A new electrode design for ambipolar injection in organic semiconductors.

PubMed

Kanagasekaran, Thangavel; Shimotani, Hidekazu; Shimizu, Ryota; Hitosugi, Taro; Tanigaki, Katsumi

2017-10-17

Organic semiconductors have attracted much attention for low-cost, flexible and human-friendly optoelectronics. However, achieving high electron-injection efficiency is difficult from air-stable electrodes and cannot be equivalent to that of holes. Here, we present a novel concept of electrode composed of a bilayer of tetratetracontane (TTC) and polycrystalline organic semiconductors (pc-OSC) covered by a metal layer. Field-effect transistors of single-crystal organic semiconductors with the new electrodes of M/pc-OSC/TTC (M: Ca or Au) show both highly efficient electron and hole injection. Contact resistance for electron injection from Au/pc-OSC/TTC and hole injection from Ca/pc-OSC/TTC are comparable to those for electron injection from Ca and hole injection from Au, respectively. Furthermore, the highest field-effect mobilities of holes (22 cm 2  V -1  s -1 ) and electrons (5.0 cm 2  V -1  s -1 ) are observed in rubrene among field-effect transistors with electrodes so far proposed by employing Ca/pc-OSC/TTC and Au/pc-OSC/TTC electrodes for electron and hole injection, respectively.One of technological challenges building organic electronics is efficient injection of electrons at metal-semiconductor interfaces compared to that of holes. The authors show an air-stable electrode design with induced gap states, which support Fermi level pinning and thus ambipolar carrier injection.

Carbon nanostructured films modified by metal nanoparticles supported on filtering membranes for electroanalysis.

PubMed

Paramo, Erica; Palmero, Susana; Heras, Aranzazu; Colina, Alvaro

2018-02-01

A novel methodology to prepare sensors based on carbon nanostructures electrodes modified by metal nanoparticles is proposed. As a proof of concept, a novel bismuth nanoparticle/carbon nanofiber (Bi-NPs/CNF) electrode and a carbon nanotube (CNT)/gold nanoparticle (Au-NPs) have been developed. Bi-NPs/CNF films were prepared by 1) filtering a dispersion of CNFs on a polytetrafluorethylene (PTFE) filter, and 2) filtering a dispersion of Bi-NPs chemically synthesized through this CNF/PTFE film. Next the electrode is prepared by sticking the Bi-NPs/CNF/PTFE film on a PET substrate. In this work, Bi-NPs/CNF ratio was optimized using a Cd 2+ solution as a probe sample. The Cd anodic stripping peak intensity, registered by differential pulse anodic stripping voltammetry (DPASV), is selected as target signal. The voltammograms registered for Cd stripping with this Bi-NPs/CNF/PTFE electrode showed well-defined and highly reproducible electrochemical. The optimized Bi-NPs/CNF electrode exhibits a Cd 2+ detection limit of 53.57 ppb. To demonstrate the utility and versatility of this methodology, single walled carbon nanotubes (SWCNTs) and gold nanoparticles (Au-NPs) were selected to prepare a completely different electrode. Thus, the new Au-NPs/SWCNT/PTFE electrode was tested with a multiresponse technique. In this case, UV/Vis absorption spectroelectrochemistry experiments were carried out for studying dopamine, demonstrating the good performance of the Au-NPs/SWCNT electrode developed. Copyright © 2017 Elsevier B.V. All rights reserved.

Silver Makes Better Electrical Contacts to Thiol-Terminated Silanes than Gold.

PubMed

Li, Haixing; Su, Timothy A; Camarasa-Gómez, María; Hernangómez-Pérez, Daniel; Henn, Simon E; Pokorný, Vladislav; Caniglia, Caravaggio D; Inkpen, Michael S; Korytár, Richard; Steigerwald, Michael L; Nuckolls, Colin; Evers, Ferdinand; Venkataraman, Latha

2017-11-06

We report that the single-molecule junction conductance of thiol-terminated silanes with Ag electrodes are higher than the conductance of those formed with Au electrodes. These results are in contrast to the trends in the metal work function Φ(Ag)<Φ(Au). As such, a better alignment of the Au Fermi level to the molecular orbital of silane that mediates charge transport would be expected. This conductance trend is reversed when we replace the thiols with amines, highlighting the impact of metal-S covalent and metal-NH 2 dative bonds in controlling the molecular conductance. Density functional theory calculations elucidate the crucial role of the chemical linkers in determining the level alignment when molecules are attached to different metal contacts. We also demonstrate that conductance of thiol-terminated silanes with Pt electrodes is lower than the ones formed with Au and Ag electrodes, again in contrast to the trends in the metal work-functions. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

An amperometric enzyme electrode and its biofuel cell based on a glucose oxidase-poly(3-anilineboronic acid)-Pd nanoparticles bionanocomposite for glucose biosensing.

PubMed

Sun, Lingen; Ma, Yixuan; Zhang, Pei; Chao, Long; Huang, Ting; Xie, Qingji; Chen, Chao; Yao, Shouzhuo

2015-06-01

A new amperometric enzyme electrode and its biofuel cell were fabricated based on a glucose oxidase (GOx)-poly(3-anilineboronic acid) (PABA)-Pd nanoparticles (PdNPs) bionanocomposite for biosensing of glucose. Briefly, Pd was electroplated on a multiwalled carbon nanotubes (MWCNTs)-modified Au electrode, and the GOx-PABA-PdNPs bionanocomposite was prepared on the Pd(plate)/MWCNTs/Au electrode through the chemical oxidation of a GOx-3-anilineboronic acid adduct by Na2PdCl4, followed by electrode-modification with an outer-layer chitosan (CS) film. The thus-prepared CS/GOx-PABA-PdNPs/Pd(plate)/MWCNTs/Au electrode exhibited a linear amperometric response to glucose concentration from 2.0 μM to 4.5 mM with a sensitivity of 160 μA/mM/cm(2), sub-μM detection limit, and excellent operation/storage stability in the first-generation biosensing mode, as well as excellent analytical performance in the second-generation biosensing mode. The good recoveries of glucose obtained from spiked urine samples revealed the application potential of our amperometric enzyme electrode. In addition, a glucose/O2 biofuel cell was constructed using this enzyme electrode as the anode and a Pt/MWCNTs/Au electrode as the cathode, and this biofuel cell as a self-powered biosensing device showed a linear voltage response to glucose concentration from 100 μM to 13.5 mM with a sensitivity of 43.5 mV/mM/cm(2) and excellent operation/storage stability. Copyright © 2015 Elsevier B.V. All rights reserved.

Boronic Acid vs. Folic Acid: A Comparison of the bio-recognition performances by Impedimetric Cytosensors based on Ferrocene cored dendrimer.

PubMed

Dervisevic, Muamer; Şenel, Mehmet; Sagir, Tugba; Isik, Sevim

2017-05-15

A comparative study is reported where folic acid (FA) and boronic acid (BA) based cytosensors and their analytical performances in cancer cell detection were analyzed by using electrochemical impedance spectroscopy (EIS) method. Cytosensors were fabricated using self-assembled monolayer principle by modifying Au electrode with cysteamine (Cys) and immobilization of ferrocene cored polyamidiamine dendrimers second generation (Fc-PAMAM (G2)), after which electrodes were modified with FA and BA. Au/Fc-PAMAM(G2)/FA and Au/Fc-PAMAM(G2)/BA based cytosensors showed extremely good analytical performances in cancer cell detection with linear range of 1×10 2 to 1×10 6 cellsml -1 , detection limit of 20cellsml -1 with incubation time of 20min for FA based electrode, and for BA based electrode detection limit was 28cellsml -1 with incubation time of 10min. Next to excellent analytical performances, cytosensors showed high selectivity towards cancer cells which was demonstrated in selectivity study using human embryonic kidney 293 cells (HEK 293) as normal cells and Au/Fc-PAMAM(G2)/FA electrode showed two times better selectivity than BA modified electrode. These cytosensors are promising for future applications in cancer cell diagnosis. Copyright © 2017 Elsevier B.V. All rights reserved.

Fabrication of a novel aptasensor based on three-dimensional reduced graphene oxide/polyaniline/gold nanoparticle composite as a novel platform for high sensitive and specific cocaine detection.

PubMed

Hashemi, Pegah; Bagheri, Hasan; Afkhami, Abbas; Ardakani, Yalda Hosseinzadeh; Madrakian, Tayyebeh

2017-12-15

In the present research, we have developed a novel label free aptasensor based on screen printed carbon electrode (SPCE) modified with three-dimensional magnetic reduced graphene oxide(3D-MRGO)/polyaniline(PA)/gold nanoparticle(AuNP) nanocomposite for impedimetric determination of cocaine. To achieve this goal, a specific thiolated cocaine aptamer was immobilized onto the surface of synthesized nanocomposite. The signaling mechanism of the proposed aptasensor was based on increase in the [Fe(CN) 6 ] 3-/4- charge transfer resistance (R CT ) as an electrochemical probe in the presence of target analyte. In order to collect of 3D-MRGO/PA/AuNP/aptamer on the surface of working electrode easily, a new electrochemical cell was fabricated. The advantages of the new electrochemical cell configuration can be counted as reusing SPCE for several times, obtaining repeatable responses, reducing required volume of electrolyte and probe solution and making proposed method more user-friendly. Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FT-IR) were used for the characterization of synthesized nanocomposite and modified electrode surface. Under optimized condition, cocaine was determined in a linear concentration range from 0.09 to 85 nM with a detection limit of 0.029 nM by EIS. Also, in order to test applicability of the proposed aptasensor, it was applied to determine cocaine in urine and serum samples and satisfactory results were obtained. Copyright © 2017 Elsevier B.V. All rights reserved.

Observation of electrostatically released DNA from gold electrodes with controlled threshold voltages.

PubMed

Takeishi, Shunsaku; Rant, Ulrich; Fujiwara, Tsuyoshi; Buchholz, Karin; Usuki, Tatsuya; Arinaga, Kenji; Takemoto, Kazuya; Yamaguchi, Yoshitaka; Tornow, Marc; Fujita, Shozo; Abstreiter, Gerhard; Yokoyama, Naoki

2004-03-22

DNA oligo-nucleotides, localized at Au metal electrodes in aqueous solution, are found to be released when applying a negative bias voltage to the electrode. The release was confirmed by monitoring the intensity of the fluorescence of cyanine dyes (Cy3) linked to the 5' end of the DNA. The threshold voltage of the release changes depending on the kind of linker added to the DNA 3'-terminal. The amount of released DNA depends on the duration of the voltage pulse. Using this technique, we can retain DNA at Au electrodes or Au needles, and release the desired amount of DNA at a precise location in a target. The results suggest that DNA injection into living cells is possible with this method. (c) 2004 American Institute of Physics

Impedimetric Label-Free Immunosensor on Disposable Modified Screen-Printed Electrodes for Ochratoxin A

PubMed Central

Malvano, Francesca; Albanese, Donatella; Crescitelli, Alessio; Pilloton, Roberto; Esposito, Emanuela

2016-01-01

An impedimetric label-free immunosensor on disposable screen-printed carbon electrodes (SPCE) for quantitative determination of Ochratoxin A (OTA) has been developed. After modification of the SPCE surface with gold nanoparticles (AuNPs), the anti-OTA was immobilized on the working electrode through a cysteamine layer. After each coating step, the modified surfaces were characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The capacitance was chosen as the best parameter that describes the reproducible change in electrical properties of the electrode surface at different OTA concentrations and it was used to investigate the analytical parameters of the developed immunosensor. Under optimized conditions, the immunosensor showed a linear relationship between 0.3 and 20 ng/mL with a low detection limit of 0.25 ng/mL, making it suitable to control OTA content in many common food products. Lastly, the immunosensor was used to measure OTA in red wine samples and the results were compared with those registered with a competitive ELISA kit. The immunosensor was sensitive to OTA lower than 2 μg/kg, which represents the lower acceptable limit of OTA established by European legislation for common food products. PMID:27376339

Impedimetric Label-Free Immunosensor on Disposable Modified Screen-Printed Electrodes for Ochratoxin A.

PubMed

Malvano, Francesca; Albanese, Donatella; Crescitelli, Alessio; Pilloton, Roberto; Esposito, Emanuela

2016-06-30

An impedimetric label-free immunosensor on disposable screen-printed carbon electrodes (SPCE) for quantitative determination of Ochratoxin A (OTA) has been developed. After modification of the SPCE surface with gold nanoparticles (AuNPs), the anti-OTA was immobilized on the working electrode through a cysteamine layer. After each coating step, the modified surfaces were characterized by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). The capacitance was chosen as the best parameter that describes the reproducible change in electrical properties of the electrode surface at different OTA concentrations and it was used to investigate the analytical parameters of the developed immunosensor. Under optimized conditions, the immunosensor showed a linear relationship between 0.3 and 20 ng/mL with a low detection limit of 0.25 ng/mL, making it suitable to control OTA content in many common food products. Lastly, the immunosensor was used to measure OTA in red wine samples and the results were compared with those registered with a competitive ELISA kit. The immunosensor was sensitive to OTA lower than 2 μg/kg, which represents the lower acceptable limit of OTA established by European legislation for common food products.

Bio-inspired nanocatalysts for the oxygen reduction reaction.

PubMed

Grumelli, Doris; Wurster, Benjamin; Stepanow, Sebastian; Kern, Klaus

2013-01-01

Electrochemical conversions at fuel cell electrodes are complex processes. In particular, the oxygen reduction reaction has substantial overpotential limiting the electrical power output efficiency. Effective and inexpensive catalytic interfaces are therefore essential for increased performance. Taking inspiration from enzymes, earth-abundant metal centres embedded in organic environments present remarkable catalytic active sites. Here we show that these enzyme-inspired centres can be effectively mimicked in two-dimensional metal-organic coordination networks self-assembled on electrode surfaces. Networks consisting of trimesic acid and bis-pyridyl-bispyrimidine coordinating to single iron and manganese atoms on Au(111) effectively catalyse the oxygen reduction and reveal distinctive catalytic activity in alkaline media. These results demonstrate the potential of surface-engineered metal-organic networks for electrocatalytic conversions. Specifically designed coordination complexes at surfaces inspired by enzyme cofactors represent a new class of nanocatalysts with promising applications in electrocatalysis.

Comparison of GaP nanowires grown from Au and Sn vapor-liquid-solid catalysts as photoelectrode materials

NASA Astrophysics Data System (ADS)

Lee, Sudarat; Wen, Wen; Cheek, Quintin; Maldonado, Stephen

2018-01-01

Gallium phosphide (GaP) nanowire film electrodes have been prepared via solid sublimation of GaP powder using both gold (Au) and tin (Sn) nanoparticles as the vapor-liquid-solid (VLS) catalysts on Si(1 1 1) and GaP(1 1 1)B substrates. The resultant GaP nanowires are compared and contrasted in terms of structures and photoactivity in photoelectrochemical half cells. Raman spectra implicated a difference in the surface condition of the two types of nanowires. Complete wet etching removal of metallic VLS catalysts from the as-prepared GaP nanowires was possible with Sn catalysts but not with Au catalysts. The photoresponses of both Sn- and Au-seeded GaP nanowire films were collected and examined under 100 mW cm-2 white light illumination. Au-seeded nanowire films exhibited strong n-type characteristics when measured in nonaqueous electrolyte with ferrocene/ferricenium as the redox species while Sn-seeded nanowires showed behavior consistent with degenerate n-type doping.

Molecular Simulations of The Formation of Gold-Molecule-Gold Junctions

NASA Astrophysics Data System (ADS)

Wang, Huachuan

2013-03-01

We perform classical molecular simulations by combining grand canonical Monte Carlo (GCMC) sampling with molecular dynamics (MD) simulation to explore the dynamic gold nanojunctions in a Alkenedithiol (ADT) solvent. With the aid of a simple driving-spring model, which can reasonably represent the long-range elasticity of the gold electrode, the spring forces are obtained during the dynamic stretching procedure. A specific multi-time-scale double reversible reference system propagator (double-RESPA) algorithm has been designed for the metal-organic complex in MD simulations to identify the detailed metal-molecule bonding geometry at metal-molecule-metal interface. We investigate the variations of bonding sites of ADT molecules on gold nanojunctions at Au (111) surface at a constant chemical potential. Simulation results show that an Au-ADT-Au interface is formed on Au nanojunctions, bond-breaking intersection is at 1-1 bond of the monatomic chain of the cross-section, instead of at the Au-S bond. Breaking force is around 1.5 nN. These are consistent with the experimental measurements.

Au@MnO2 core-shell nanomesh electrodes for transparent flexible supercapacitors.

PubMed

Qiu, Tengfei; Luo, Bin; Giersig, Michael; Akinoglu, Eser Metin; Hao, Long; Wang, Xiangjun; Shi, Lin; Jin, Meihua; Zhi, Linjie

2014-10-29

A novel Au@MnO2 supercapacitor is presented. The sophisticated core-shell architecture combining an Au nanomesh core with a MnO2 shell on a flexible polymeric substrate is demonstrated as an electrode for high performance transparent flexible supercapacitors (TFSCs). Due to their unique structure, high areal/gravimetric capacitance and rate capability for TFSCs are achieved. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Mask-less deposition of Au-SnO2 nanocomposites on CMOS MEMS platform for ethanol detection.

PubMed

Santra, S; Sinha, A K; De Luca, A; Ali, S Z; Udrea, F; Guha, P K; Ray, S K; Gardner, J W

2016-03-29

Here we report on the mask-less deposition of Au-SnO2 nanocomposites with a silicon-on-insulator (SOI) complementary metal oxide semiconductor (CMOS) micro electro mechanical system (MEMS) platform through the use of dip pen nanolithography (DPN) to create a low-cost ethanol sensor. MEMS technology is used in order to achieve low power consumption, by the employment of a membrane structure formed using deep reactive ion etching technique. The device consists of an embedded tungsten micro-heater with gold interdigitated electrodes on top of the SOI membrane. The tungsten micro-heater is used to raise the membrane temperature up to its operating temperature and the electrodes are used to measure the resistance of the nanocomposite sensing layer. The CMOS MEMS devices have high electro-thermal efficiency, with 8.2 °C temperature increase per mW power of consumption. The sensing material (Au-SnO2 nanocomposite) was synthesised starting from SnO nanoplates, then Au nanoparticles were attached chemically to the surface of SnO nanoplates, finally the mixture was heated at 700 °C in an oven in air for 4 h. This composite material was sonicated for 2 h in terpineol to make a viscous homogeneous slurry and then 'written' directly across the electrode area using the DPN technique without any mask. The devices were characterised by exposure to ethanol vapour in humid air in the concentration range of 100-1000 ppm. The sensitivity varied from 1.2 to 0.27 ppm(-1) for 100-1000 ppm of ethanol at 10% relative humid air. Selectivity measurements showed that the sensors were selective towards ethanol when they were exposed to acetone and toluene.

Mask-less deposition of Au-SnO2 nanocomposites on CMOS MEMS platform for ethanol detection

NASA Astrophysics Data System (ADS)

Santra, S.; Sinha, A. K.; De Luca, A.; Ali, S. Z.; Udrea, F.; Guha, P. K.; Ray, S. K.; Gardner, J. W.

2016-03-01

Here we report on the mask-less deposition of Au-SnO2 nanocomposites with a silicon-on-insulator (SOI) complementary metal oxide semiconductor (CMOS) micro electro mechanical system (MEMS) platform through the use of dip pen nanolithography (DPN) to create a low-cost ethanol sensor. MEMS technology is used in order to achieve low power consumption, by the employment of a membrane structure formed using deep reactive ion etching technique. The device consists of an embedded tungsten micro-heater with gold interdigitated electrodes on top of the SOI membrane. The tungsten micro-heater is used to raise the membrane temperature up to its operating temperature and the electrodes are used to measure the resistance of the nanocomposite sensing layer. The CMOS MEMS devices have high electro-thermal efficiency, with 8.2 °C temperature increase per mW power of consumption. The sensing material (Au-SnO2 nanocomposite) was synthesised starting from SnO nanoplates, then Au nanoparticles were attached chemically to the surface of SnO nanoplates, finally the mixture was heated at 700 °C in an oven in air for 4 h. This composite material was sonicated for 2 h in terpineol to make a viscous homogeneous slurry and then ‘written’ directly across the electrode area using the DPN technique without any mask. The devices were characterised by exposure to ethanol vapour in humid air in the concentration range of 100-1000 ppm. The sensitivity varied from 1.2 to 0.27 ppm-1 for 100-1000 ppm of ethanol at 10% relative humid air. Selectivity measurements showed that the sensors were selective towards ethanol when they were exposed to acetone and toluene.

Three-Dimensional Conductive Nanocomposites Based on Multiwalled Carbon Nanotube Networks and PEDOT:PSS as a Flexible Transparent Electrode for Optoelectronics.

PubMed

Cho, Er-Chieh; Li, Chiu-Ping; Huang, Jui-Hsiung; Lee, Kuen-Chan; Huang, Jen-Hsien

2015-06-03

We have synthesized conductive nanocomposites composed of multiwalled carbon nanotubes (MWCNTs) and Au nanoparticles (NPs). The Au NPs with an average size of approximately 4.3 nm are uniformly anchored on the MWCNT. After being exposed to microwave (MW) plasma irradiation, the anchored Au NPs melt and fuse, leading to larger aggregates (34 nm) that can connect the MWCNT forming a three-dimensional conducting network. The formation of a continuous MWCNT network can produce more a conductive pathway, leading to lower sheet resistance. When the Au-MWCNT is dispersed in the highly conductive polymer, poly(ethylene dioxythiophene):polystyrenesulfonate ( PSS), we can obtain solution-processable composite formulations for the preparation of a flexible transparent electrode. The resulting Au-MWCNT/PEDOT:PSS hybrid films possess a sheet resistance of 51 Ω/sq with a transmittance of 86.2% at 550 nm. We also fabricate flexible organic solar cells and electrochromic devices to demonstrate the potential use of the as-prepared composite electrodes. Compared with the indium tin oxide-based devices, both the solar cells and electrochromic devices with the composites incorporated as a transparent electrode deliver comparable performance.

Simultaneous immobilization of glucose oxidase on the surface and cavity of hollow gold nanospheres as labels for highly sensitive electrochemical immunoassay of tumor marker.

PubMed

Song, Zhongju; Yuan, Ruo; Chai, Yaqin; Jiang, Wen; Su, Huilan; Che, Xin; Ran, Xiaoqi

2011-01-15

A novel tracer, glucose oxidase (GOD)-functionalized hollow gold nanospheres encapsulating glucose oxidase (Au(shell)@GOD), was designed to label the ferrocenemonocarboxylic-grafted secondary antibodies (Fc@Ab(2)) for highly sensitive detection of tumor marker using carboxyl group functionalized multiwall carbon nanotubes as platform. Initially, Au(shell)@GOD was synthesized specially by reverse micelle approach, and then the labeling of antibody and the preparation of GOD-functionalized Au(shell)@GOD were performed by one-pot assembly of Fc@Ab(2) and GOD on the surface of Au(shell)@GOD. The ferrocene used to label antibodies acted as a mediator of electron transfer between GOD and electrode surface. The high-content glucose oxidase in the tracer (on the surface and in the cavity) could significantly amplify the amperometric signal for sandwich-type immunoassay. Using carcinoembryonic antigen (CEA) as model analyte, the designed tracer showed linear range from 0.02 to 5.0 ng mL(-1) with the detection limit down to 6.7 pg mL(-1). The assay results of serum samples with the proposed method were in an acceptable agreement with the reference values. The new protocol showed acceptable stability and reproducibility, high sensitivity, and good precision, which could provide a promising potential for clinical screening and diagnosis of tumor disease. Copyright © 2010 Elsevier B.V. All rights reserved.

Design and fabrication of an electrochemical aptasensor using Au nanoparticles/carbon nanoparticles/cellulose nanofibers nanocomposite for rapid and sensitive detection of Staphylococcus aureus.

PubMed

Ranjbar, Saba; Shahrokhian, Saeed

2018-04-27

Since that pathogenic bacteria are major threats to human health, this paper describes the fabrication of an effective and durable sensing platform based on gold nanoparticles/carbon nanoparticles/cellulose nanofibers nanocomposite (AuNPs/CNPs/CNFs) at the surface of glassy carbon electrode for sensitive and selective detection of Staphylococcus aureus (S. aureus). The AuNPs/CNPs/CNFs nanocomposite with the high surface area, excellent conductivity, and good biocompatibility was used for self-assembled of the thiolated specific S. aureus aptamer as a sensing element. The surface morphology of AuNPs/CNPs/CNFs nanocomposite was characterized with field emission scanning electron microscopy (FESEM), energy dispersive spectroscopy (EDS), dynamic light scattering (DLS) and ultraviolet-visible (UV-Vis) spectrophotometric methods. Each aptasensor modification step was monitored with cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) techniques. The fabricated aptasensor exhibited a wide linear dynamic range (1.2 × 10 1 to 1.2 × 10 8 ) CFU mL -1 with a LOD of 1 CFU mL -1 and was be capable to accurate detection and determination of Staphylococcus aureus in human blood serum as a clinical sample with a complex matrix. Copyright © 2018 Elsevier B.V. All rights reserved.

Sensitive electrochemical sensing platform for microRNAs detection based on shortened multi-walled carbon nanotubes with high-loaded thionin.

PubMed

Deng, Keqin; Liu, Xinyan; Li, Chunxiang; Huang, Haowen

2018-05-31

The loading capacity of thionin (Thi) on shortened multi-walled carbon nanotubes (S-MWCNTs) and acidified multi-walled carbon nanotubes (A-MWCNTs) was compared. Two DNA probe fragments were designed for hybridization with microRNA-21 (miR-21), the microRNAs (miRNAs) model analyte. DNA probe 1 (P1) was assembled on Au nanoparticles (AuNPs) modified electrode. MiR-21 was captured by the pre-immobilized P1. A signal nanoprobe was synthesized by loading large amount of Thi on S-MWCNTs with covalently bonded probe 2 (P2). Owing to the large effective surface area of MWCNTs, fast electron shuttle of MWCNTs, high-loaded Thi on S-MWCNTs, and the increased conductivity from AuNPs, after signal probe hybridized with miR-21, it gave rise to a magnified current response on electrode. The increased electrochemical current enabled us to quantitatively detect miR-21. Expensive bioreagents and labeled target/detection DNA or miRNAs were avoided in this strategy. The operation complexity and assay cost were also reduced. Copyright © 2018 Elsevier B.V. All rights reserved.

Polyamidoamine dendrimers-assisted electrodeposition of gold-platinum bimetallic nanoflowers.

PubMed

Qian, Lei; Yang, Xiurong

2006-08-24

Novel Au-Pt bimetallic flower nanostructures fabricated on a polyamidoamine dendrimers-modified surface by electrodeposition are reported. These polyamidoamine dendrimers were stable, and they assisted the formation of Au-Pt bimetallic nanoflowers during the electrodeposition process. These nanoflowers were characterized by field-emitted scanning electron microscopy (FE-SEM), energy-dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), X-ray diffraction, and electrochemical methods. FE-SEM images showed that the bimetallic nanoflower included two parts: the "light" and the "pale" part. The two parts consisted of many small bimetallic nanoparticles, which was attributed to the progressive nucleation process. Moreover, the "light" part contained more bimetallic nanoparticles. The morphologies of bimetallic nanoflowers depended on the electrodeposition time and potential and the layer number of assembled dendrimers. The average size of nanoflowers increased with the increase in electrodeposition time. The layer number of assembled dendrimers obviously affected the size and morphologies of the "pale" parts of deposited nanoflowers. EDS and XPS indicated that the content of Au element was higher than that of Pt element in the nanoflowers. The bimetallic nanoflowers-modified electrode had electrochemical properties similar to those of bare gold and platinum electrodes. It also exhibited significant electrocatalytic activities toward oxygen reduction.

Analyzing the electrooxidation of ethylene glycol and glucose over platinum-modified gold electrocatalysts in alkaline electrolyte using in-situ infrared spectroscopy

NASA Astrophysics Data System (ADS)

Mahoney, Elizabeth G.; Sheng, Wenchao; Cheng, Mei; Lee, Kevin X.; Yan, Yushan; Chen, Jingguang G.

2016-02-01

Platinum modified gold (Pt/Au) catalysts are evaluated for the electrooxidation of ethylene glycol (EG) and glucose (Glc). The Pt/Au catalysts are synthesized on an Au disk and supported Au/C particles through the galvanic displacement of a copper monolayer with Pt. The Pt/Au catalysts are compared to monometallic Pt and Au catalysts for the oxidation of EG and Glc in alkaline electrolyte. The Pt/Au disk has an onset potential for these reactions that is similar to Pt and is lower than Au. The supported catalysts are less active toward the electrooxidation of EG and Glc than the corresponding disk electrodes, but the Pt/Au/C also has an onset potential similar to Pt/C. In-situ FTIR is used to analyze the C-C bond scission in both reactions on the surfaces of Pt, Au, and Pt/Au disks. While the Pt/Au disk is found to have a low onset potential for the oxidation of EG, it does not produce as much CO2 as bulk Pt. On the other hand, the FTIR results show that CO2 is produced for the oxidation of Glc on the Pt/Au disk. These results show promise for the possibility of decreasing the amount of Pt needed for the electrooxidation of polyol molecules.

The effect of gold nanoparticles modified electrode on the glucose sensing performance

NASA Astrophysics Data System (ADS)

Zulkifli, Zulfa Aiza; Ridhuan, Nur Syafinaz; Nor, Noorhashimah Mohamad; Zakaria, Nor Dyana; Razak, Khairunisak Abdul

2017-07-01

In this work, 20 nm, 30 nm, 40 nm, 50 nm and 60 nm colloidal gold nanoparticles (AuNPs) were synthesized using the seeding growth method. AuNPs produced had spherical shape with uniform size. The AuNPs also are well dispersed in colloidal form that was proven by low polydispersity index. The produced AuNPs were used to modify electrode for glucose sensor. The produced AuNPs were deposited on indium tin oxide substrate (ITO), followed by immobilization of glucose oxidase (GOx) on it. After that, Nafion was deposited on the GOx/AuNPs/ITO. Electrooxidation of glucose with AuNPs-modified electrode was examined by cyclic voltammeter (CV) in 15 mM glucose mixed with 0.01 M PBS. The optimum size of AuNPs was 30 nm with optical density 3.0. AuNPs were successfully immobilized with glucose oxidase (GOx) and proved to work well as a glucose sensor. Based on the high electrocatalytic activity of Nafion/GOx/AuNPs/ITO, the sensitivity of the glucose sensors was further examined by varying the concentration of glucose solution from 2 mM to 20 mM in 0.01 M phosphate buffer solution (PBS) solution. Good linear relationship was observed between the catalytic current and glucose concentration in the range of 2 mM to 20 mM. The sensitivity of the Nafion/GOx/AuNPs/ITO electrode calculated from the slope of linear square calibration was 0.909 µA mM-1 cm-2 that is comparable with other published work. The linear fitting to the experimental data gives R-square of 0.991 at 0.9 V and a detection limit of 2.03 mM. This detection range is sufficient to be medically useful in monitoring human blood glucose level in which the normal blood glucose level is in the range of 4.4 to 6.6 mM and diabetic blood glucose level is above 7 mM.

STM, SECPM, AFM and Electrochemistry on Single Crystalline Surfaces

PubMed Central

Wolfschmidt, Holger; Baier, Claudia; Gsell, Stefan; Fischer, Martin; Schreck, Matthias; Stimming, Ulrich

2010-01-01

Scanning probe microscopy (SPM) techniques have had a great impact on research fields of surface science and nanotechnology during the last decades. They are used to investigate surfaces with scanning ranges between several 100 μm down to atomic resolution. Depending on experimental conditions, and the interaction forces between probe and sample, different SPM techniques allow mapping of different surface properties. In this work, scanning tunneling microscopy (STM) in air and under electrochemical conditions (EC-STM), atomic force microscopy (AFM) in air and scanning electrochemical potential microscopy (SECPM) under electrochemical conditions, were used to study different single crystalline surfaces in electrochemistry. Especially SECPM offers potentially new insights into the solid-liquid interface by providing the possibility to image the potential distribution of the surface, with a resolution that is comparable to STM. In electrocatalysis, nanostructured catalysts supported on different electrode materials often show behavior different from their bulk electrodes. This was experimentally and theoretically shown for several combinations and recently on Pt on Au(111) towards fuel cell relevant reactions. For these investigations single crystals often provide accurate and well defined reference and support systems. We will show heteroepitaxially grown Ru, Ir and Rh single crystalline surface films and bulk Au single crystals with different orientations under electrochemical conditions. Image studies from all three different SPM methods will be presented and compared to electrochemical data obtained by cyclic voltammetry in acidic media. The quality of the single crystalline supports will be verified by the SPM images and the cyclic voltammograms. Furthermore, an outlook will be presented on how such supports can be used in electrocatalytic studies. PMID:28883327

Robust and Recyclable Substrate Template with an Ultrathin Nanoporous Counter Electrode for Organic-Hole-Conductor-Free Monolithic Perovskite Solar Cells.

PubMed

Li, Ming-Hsien; Yang, Yu-Syuan; Wang, Kuo-Chin; Chiang, Yu-Hsien; Shen, Po-Shen; Lai, Wei-Chih; Guo, Tzung-Fang; Chen, Peter

2017-12-06

A robust and recyclable monolithic substrate applying all-inorganic metal-oxide selective contact with a nanoporous (np) Au:NiO x counter electrode is successfully demonstrated for efficient perovskite solar cells, of which the perovskite active layer is deposited in the final step for device fabrication. Through annealing of the Ni/Au bilayer, the nanoporous NiO/Au electrode is formed in virtue of interconnected Au network embedded in oxidized Ni. By optimizing the annealing parameters and tuning the mesoscopic layer thickness (mp-TiO 2 and mp-Al 2 O 3 ), a decent power conversion efficiency (PCE) of 10.25% is delivered. With mp-TiO 2 /mp-Al 2 O 3 /np-Au:NiO x as a template, the original perovskite solar cell with 8.52% PCE can be rejuvenated by rinsing off the perovskite material with dimethylformamide and refilling with newly deposited perovskite. A renewed device using the recycled substrate once and twice, respectively, achieved a PCE of 8.17 and 7.72% that are comparable to original performance. This demonstrates that the novel device architecture is possible to recycle the expensive transparent conducting glass substrates together with all the electrode constituents. Deposition of stable multicomponent perovskite materials in the template also achieves an efficiency of 8.54%, which shows its versatility for various perovskite materials. The application of such a novel NiO/Au nanoporous electrode has promising potential for commercializing cost-effective, large scale, and robust perovskite solar cells.

Enhanced Output Power of PZT Nanogenerator by Controlling Surface Morphology of Electrode.

PubMed

Jung, Woo-Suk; Lee, Won-Hee; Ju, Byeong-Kwon; Yoon, Seok-Jin; Kang, Chong-Yun

2015-11-01

Piezoelectric power generation using Pb(Zr,Ti)O3(PZT) nanowires grown on Nb-doped SrTiO3(nb:STO) substrate has been demonstrated. The epitaxial PZT nanowires prepared by a hydrothermal method, with a diameter and length of approximately 300 nm and 7 μm, respecively, were vertically aligned on the substrate. An embossed Au top electrode was applied to maximize the effective power generation area for non-uniform PZT nanowires. The PZT nanogenerator produced output power density of 0.56 μW/cm2 with a voltage of 0.9 V and current of 75 nA. This research suggests that the morphology control of top electrode can be useful to improve the efficiency of piezoelectric power generation.

Soft actuator based on Kraton with GO/Ag/Pani composite electrodes for robotic applications

NASA Astrophysics Data System (ADS)

Khan, Ajahar; Kant Jain, Ravi; Banerjee, Priyabrata; Inamuddin; Asiri, Abdullah M.

2017-11-01

In this work, electrochemically-driven Kraton/graphene oxide/Ag/polyaniline (Kraton/GO/Ag/Pani) polymer composite based ionic polymer metal composite (IPMC) was fabricated as a soft actuator. Silver nanopowder with polyaniline coating used as an electrode material is a novel approach in the fabrication of IPMC, which gives new opportunities for development of the electrode on ionic polymer actuator surfaces directly without electroless plating of Pt or Au metal. The Kraton/GO/Ag/Pani membrane showed much higher water-uptake (WU), ion exchange capacity (IEC), proton conductivity than those of several reported IPMC membranes. The enhanced actuation performance indicates that the Kraton/GO/Ag/Pani is a better alternative to the highly expensive commercialized IPMC actuator.

Electrochemical immunosensor assay (EIA) for sensitive detection of E. coli O157:H7 with signal amplification on a SG-PEDOT-AuNPs electrode interface.

PubMed

Guo, Yuna; Wang, Yu; Liu, Su; Yu, Jinghua; Wang, Hongzhi; Cui, Min; Huang, Jiadong

2015-01-21

A novel electrochemical immunosensor assay (EIA) for highly sensitive and specific detection of Escherichia coli O157:H7 has been developed. This immunosensor is constructed by the assembly of capture antibody on SG-PEDOT-AuNPs composites modified glass carbon electrode. In the presence of target E. coli O157:H7, horseradish peroxidase (HRP)-labeled antibody is captured on the electrode surface to form a sandwich-type system via the specific identification. As a result, E. coli O157:H7 detection is realized by outputting a redox current from electro-reduction of hydrogen peroxide reaction catalyzed by HRP. In our assay, the combination of the unique properties of sulfonated graphene (SG) and gold nanoparticles (AuNPs) can not only accelerate electron transfer on electrode interface, but also provide an excellent scaffold for the conjugation of capture antibody that significantly improves the target capture efficiency and enhances the sensitivity of the biosensor. The results reveal the calibration plot obtained for E. coli O157:H7 is approximately linear from 7.8 × 10-7.8 × 10(6) colony-forming unit (cfu) mL(-1) with the limit of detection of 3.4 × 10 cfu mL(-1). In addition, the biosensor has been successfully applied to the quantitative assay of E. coli O157:H7 in synthetic samples (spring water and milk). Hence, the developed electrochemical-based immunosensor might provide a useful and practical tool for E. coli O157:H7 determination and related food safety analysis and clinical diagnosis.

Biocompatible Poly(catecholamine)-Film Electrode for Potentiometric Cell Sensing.

PubMed

Kajisa, Taira; Yanagimoto, Yoshiyuki; Saito, Akiko; Sakata, Toshiya

2018-02-23

Surface-coated poly(catecholamine) (pCA) films have attracted attention as biomaterial interfaces owing to their biocompatible and physicochemical characteristics. In this paper, we report that pCA-film-coated electrodes are useful for potentiometric biosensing devices. Four different types of pCA film, l-dopa, dopamine, norepinephrine, and epinephrine, with thicknesses in the range of 7-27 nm were electropolymerized by oxidation on Au electrodes by using cyclic voltammetry. By using the pCA-film electrodes, the pH responsivities were found to be 39.3-47.7 mV/pH within the pH range of 1.68 to 10.01 on the basis of the equilibrium reaction with hydrogen ions and the functional groups of the pCAs. The pCA films suppressed nonspecific signals generated by other ions (Na + , K + , Ca 2+ ) and proteins such as albumin. Thus, the pCA-film electrodes can be used in pH-sensitive and pH-selective biosensors. HeLa cells were cultivated on the surface of the pCA-film electrodes to monitor cellular activities. The surface potential of the pCA-film electrodes changed markedly because of cellular activity; therefore, the change in the hydrogen ion concentration around the cell/pCA-film interface could be monitored in real time. This was caused by carbon dioxide or lactic acid that is generated by cellular respiration and dissolves in the culture medium, resulting in the change of hydrogen concentration. pCA-film electrodes are suitable for use in biocompatible and pH-responsive biosensors, enabling the more selective detection of biological phenomena.

A novel signal-off electrochemiluminescence biosensor for the determination of glucose based on double nanoparticles.

PubMed

Liu, Linlin; Ma, Qiang; Li, Yang; Liu, ZiPing; Su, Xingguang

2015-01-15

In this work, a novel facile signal-off electrochemiluminescence (ECL) biosensor has been developed for the determination of glucose based on the integration of chitosan (CHIT), CdTe quantum dots (CdTe QDs) and Au nanoparticles (Au NPs) on the glassy carbon electrode (GCE). Chitosan displays high water permeability, hydrophilic property, strong hydrogel ability and good adhesion to load the double nanoparticles to the glassy carbon electrode surfaces. Au NPs are efficient glucose oxidase (GOx)-mimickess to catalytically oxidize glucose, similar to the natural process. Upon the addition of glucose, the Au NPs catalyzed glucose to produce gluconic acid and hydrogen peroxide (H2O2) based on the consumption of dissolved oxygen (O2), which resulted in a quenching effect on the ECL emission. Therefore, the determination of glucose could be achieved by monitoring the signal-off ECL biosensor. Under the optimum conditions, the ECL intensity of CdTe QDs and the concentration of glucose have a good linear relationship in the range of 0.01-10 mmol L(-1). The limit of detection for glucose was 5.28 μmol L(-1) (S/N=3). The biosensor showed good sensitivity, selectivity, reproducibility and stability. The proposed biosensor has been employed for the detection of glucose in human serum samples with satisfactory results. Copyright © 2014 Elsevier B.V. All rights reserved.

Amplified QCM biosensor for type IV collagenase based on collagenase-cleavage of gold nanoparticles functionalized peptide.

PubMed

Dong, Zong-Mu; Jin, Xin; Zhao, Guang-Chao

2018-05-30

The present study develops a rapid, simple and efficient method for the determination of type IV collagenase by using a specific peptide-modified quartz crystal microbalance (QCM). A small peptide (P1), contains a specific sequence (Pro-Gly) and a terminal cysteine, was synthetized and immobilized to the surface of QCM electrode via the reaction between Au and thiol of the cysteine. The peptide bond between proline and glycine can be specific hydrolyzed cleavage by type IV collagenase, which enabled the modified electrode with a high selectivity toward type IV collagenase. The cleaving process caused a frequency change of QCM to give a signal related to the concentration of type IV collagenase. The morphologies of the modified electrodes were characterized by scanning electron microscope (SEM) and the specific hydrolyzed cleavage process was monitored by QCM. When P1 was modified with gold nanoparticles (P1-Au NPs), the signal could be amplified to further enhance the sensitivity of the designed sensor due to the high-mass of the modified Au NPs. Compared the direct unamplified assay, the values obtained for the limit of detection for type IV collagenase was 0.96 ng mL -1 , yielding about 6.5 times of magnitude improvement in sensitivity. This signal enhanced peptide based QCM biosensor for type IV collagenase also showed good selectivity and sensitivity in complex matrix. Copyright © 2018 Elsevier B.V. All rights reserved.

Molecularly imprinted electrochemical biosensor based on Fe@Au nanoparticles involved in 2-aminoethanethiol functionalized multi-walled carbon nanotubes for sensitive determination of cefexime in human plasma.

PubMed

Yola, Mehmet Lütfi; Eren, Tanju; Atar, Necip

2014-10-15

The molecular imprinting technique depends on the molecular recognition. It is a polymerization method around the target molecule. Hence, this technique creates specific cavities in the cross-linked polymeric matrices. In present study, a sensitive imprinted electrochemical biosensor based on Fe@Au nanoparticles (Fe@AuNPs) involved in 2-aminoethanethiol (2-AET) functionalized multi-walled carbon nanotubes (f-MWCNs) modified glassy carbon (GC) electrode was developed for determination of cefexime (CEF). The results of X-ray photoelectron spectroscopy (XPS) and reflection-absorption infrared spectroscopy (RAIRS) confirmed the formation of the developed surfaces. CEF imprinted film was constructed by cyclic voltammetry (CV) for 9 cycles in the presence of 80 mM pyrrole in phosphate buffer solution (pH 6.0) containing 20mM CEF. The developed electrochemical biosensor was validated according to the International Conference on Harmonisation (ICH) guideline and found to be linear, sensitive, selective, precise and accurate. The linearity range and the detection limit were obtained as 1.0 × 10(-10)-1.0 × 10(-8)M and 2.2 × 10(-11)M, respectively. The developed CEF imprinted sensor was successfully applied to real samples such as human plasma. In addition, the stability and reproducibility of the prepared molecular imprinted electrode were investigated. The excellent long-term stability and reproducibility of the prepared CEF imprinted electrodes make them attractive in electrochemical sensors. Copyright © 2014 Elsevier B.V. All rights reserved.

AuNPs/CNOs/SWCNTs/chitosan-nanocomposite modified electrochemical sensor for the label-free detection of carcinoembryonic antigen.

PubMed

Rizwan, Mohammad; Elma, Syazwani; Lim, Syazana Abdullah; Ahmed, Minhaz Uddin

2018-06-01

In this work, a nanocomposite of gold nanoparticles (AuNPs), carbon nano-onions (CNOs), single-walled carbon nanotubes (SWCNTs) and chitosan (CS) (AuNPs/CNOs/SWCNTs/CS) was prepared for the development of highly sensitive electrochemical immunosensor for the detection of carcinoembryonic antigen (CEA), clinical tumor marker. Firstly, layer-by-layer fabrication of the CEA-immunosensors was studied using cyclic voltammetry (CV) and square wave voltammetry (SWV). By combining the advantages of large surface area and electronic properties of AuNPs, CNOs, SWCNTs, and film forming properties of CS, AuNPs/CNOs/SWCNTs/CS-nanocomposite-modified glassy carbon electrode showed a 200% increase in effective surface area and electronic conductivity. The calibration plot gave a negative linear relationship between log[concentration] of CEA and electrical current with a correlation coefficient of 0.9875. The CEA-immunosensor demonstrated a wide linear detection range of 100 fg mL -1 to 400 ng mL -1 with a low detection limit of 100 fg mL -1 . In addition to high sensitivity, reproducibility and large stability, CEA-immunosensor provided an excellent selectivity and resistant-to-interference in the presence of other antigens in serum and hence a potential to be used with real samples. Copyright © 2018 Elsevier B.V. All rights reserved.

Partially reduced graphene oxide-gold nanorods composite based bioelectrode of improved sensing performance.

PubMed

Nirala, Narsingh R; Abraham, Shiju; Kumar, Vinod; Pandey, Shobhit A; Yadav, Umakant; Srivastava, Monika; Srivastava, S K; Singh, Vidya Nand; Kayastha, Arvind M; Srivastava, Anchal; Saxena, Preeti S

2015-11-01

The present work proposes partially reduced graphene oxide-gold nanorods supported by chitosan (CH-prGO-AuNRs) as a potential bioelectrode material for enhanced glucose sensing. Developed on ITO substrate by immobilizing glucose oxidase on CH-prGO-AuNRs composite, these CH-prGO-AuNRs/ITO bioelectrodes demonstrate high sensitivity of 3.2 µA/(mg/dL)/cm(2) and linear range of 25-200 mg/dL with an ability to detect as low as 14.5 mg/dL. Further, these CH-prGO-AuNRs/ITO based electrodes attest synergistiacally enhanced sensing properties when compared to simple graphene oxide based CH-GO/ITO electrode. This is evident from one order higher electron transfer rate constant (Ks) value in case of CH-prGO-AuNRs modified electrode (12.4×10(-2) cm/s), in contrast to CH-GO/ITO electrode (6×10(-3) cm/s). Additionally, very low Km value [15.4 mg/dL(0.85 mM)] ensures better binding affinity of enzyme to substrate which is desirable for good biosensor stability and resistance to environmental interferences. Hence, with better loading capacity, kinetics and stability, the proposed CH-prGO-AuNRs composite shows tremendous potential to detect several bio-analytes in the coming future. Copyright © 2015 Elsevier B.V. All rights reserved.

Amperometric biosensors based on deposition of gold and platinum nanoparticles on polyvinylferrocene modified electrode for xanthine detection.

PubMed

Baş, Salih Zeki; Gülce, Handan; Yıldız, Salih; Gülce, Ahmet

2011-12-15

In this study, new xanthine biosensors, XO/Au/PVF/Pt and XO/Pt/PVF/Pt, based on electroless deposition of gold(Au) and platinum(Pt) nanoparticles on polyvinylferrocene(PVF) coated Pt electrode for detection of xanthine were presented. The amperometric responses of the enzyme electrodes were measured at the constant potential, which was due to the electrooxidation of enzymatically produced H(2)O(2). Compared with XO/PVF/Pt electrode, XO/Au/PVF/Pt and XO/Pt/PVF/Pt exhibited excellent electrocatalytic activity towards the oxidation of the analyte. Effect of Au and Pt nanoparticles was investigated by monitoring the response currents at the different deposition times and the different concentrations of KAuCl(4) and PtBr(2). Under the optimal conditions, the calibration curves of XO/Au/PVF/Pt and XO/Pt/PVF/Pt were obtained over the range of 2.5 × 10(-3) to 0.56 mM and 2.0 × 10(-3) to 0.66 mM, respectively. The detection limits were 7.5 × 10(-4)mM for XO/Au/PVF/Pt and 6.0 × 10(-4)mM for XO/Pt/PVF/Pt. The effects of interferents, the operational and the storage stabilities of the biosensors and the applicabilities of the proposed biosensors to the drug samples analysis were also evaluated. Copyright © 2011 Elsevier B.V. All rights reserved.

Highly selective determination of amitriptyline using Nafion-AuNPs@branched polyethyleneimine-derived carbon hollow spheres in pharmaceutical drugs and biological fluids.

PubMed

Zad, Zeinab Rezayati; Davarani, Saied Saeed Hosseiny; Taheri, Ali Reza; Bide, Yasamin

2016-12-15

In this paper, AuNPs@Polyethyleneimine-derived carbon hollow spheres were synthesized by a versatile and facile method in three steps and successfully developed and validated as Amitriptyline sensor using cyclic voltammetry (CV), chronoamperometry (CA) and differential pulse voltammetry (DPV) methods. The characterization of the electrode surface has been carried out by means of scanning electron microscopy (SEM), transmission electron microscopy (TEM), x-ray diffraction (XRD), x-ray photo-electron spectrum (XPS), electrochemical impedance spectroscopy (EIS) and chronocoulometry (CC). The obtained negatively charged modified electrode was highly selective to Amitriptyline and it was shown a wide linear range from 0.1 to 700μmolL(-1), with a lower detection limit of 0.034μmolL(-1) (n=5, S/N=3), revealing the high-sensitivity properties. The modified electrode is used to achieve the real-time quantitative detection of AMT for biological applications, and satisfactory results are obtained. Due to the advantages of the sensor, its selectivity, sensitivity and stability, it will have a bright future in the field of medical diagnosis. Copyright © 2016 Elsevier B.V. All rights reserved.

An electrochemical sulfite biosensor based on gold coated magnetic nanoparticles modified gold electrode.

PubMed

Rawal, Rachna; Chawla, Sheetal; Pundir, Chandra Shekhar

2012-01-15

A sulfite oxidase (SO(X)) (EC 1.8.3.1) purified from Syzygium cumini leaves was immobilized onto carboxylated gold coated magnetic nanoparticles (Fe(3)O(4)@GNPs) electrodeposited onto the surface of a gold (Au) electrode through N-ethyl-N'-(3-dimethylaminopropyl) carbodiimide (EDC)-N-hydroxy succinimide (NHS) chemistry. An amperometric sulfite biosensor was fabricated using SO(X)/Fe(3)O(4)@GNPs/Au electrode as working electrode, Ag/AgCl as standard and Pt wire as auxiliary electrode. The working electrode was characterized by Fourier Transform Infrared (FTIR) Spectroscopy, Cyclic Voltammetry (CV), Scanning Electron Microscopy (SEM) and Electrochemical Impedance Spectroscopy (EIS) before and after immobilization of SO(X). The biosensor showed optimum response within 2s when operated at 0.2V (vs. Ag/AgCl) in 0.1 M Tris-HCl buffer, pH 8.5 and at 35 °C. Linear range and detection limit were 0.50-1000 μM and 0.15 μM (S/N=3) respectively. Biosensor was evaluated with 96.46% recovery of added sulfite in red wine and 1.7% and 3.3% within and between batch coefficients of variation respectively. Biosensor measured sulfite level in red and white wines. There was good correlation (r=0.99) between red wines sulfite value by standard DTNB (5,5'-dithio-bis-(2-nitrobenzoic acid)) method and the present method. Enzyme electrode was used 300 times over a period of 4 months, when stored at 4 °C. Biosensor has advantages over earlier biosensors that it has excellent electrocatalysis towards sulfite, lower detection limit, higher storage stability and no interference by ascorbate, cysteine, fructose and ethanol. Copyright © 2011 Elsevier B.V. All rights reserved.

Enhanced peroxidase-like properties of Au@Pt DNs/NG/Cu2+ and application of sandwich-type electrochemical immunosensor for highly sensitive detection of CEA.

PubMed

Lv, Hui; Li, Yueyun; Zhang, Xiaobo; Gao, Zengqiang; Zhang, Chunyan; Zhang, Shuan; Dong, Yunhui

2018-07-30

Effective treatment of cancer depends upon the early detection of the tumor marker. Here, we report on the development of a new immunosensor for early detection of carcinoembryonic antigen (CEA). Cubic Au@Pt dendritic nanomaterials functionalized nitrogen-doped graphene loaded with copper ion (Au@Pt DNs/NG/Cu 2+ ) with enhanced peroxidase-like properties was synthesized as labels to effectively capture and immobilize secondary anti-CEA. The Au@Pt DNs with more active surface area could efficiently enhance electrocatalysis for reduction of hydrogen peroxide (H 2 O 2 ). Meanwhile, with good conductivity and large specific surface area, NG can immobilize a large amount of Au@Pt DNs. Furthermore, after adsorbed Cu 2+ can further promote the redox of H 2 O 2 and amplify the signal of the immunosensor. For the immobilization of primary antibodies, Au nanoparticles functionalized polydopamine (Au@PDA) were used as transducing materials to modify glassy carbon electrodes and enhance the electron transfer efficiently. Under optimal conditions, the immunosensor exhibited a satisfactory response to CEA with a limit detection of 0.167 pg/mL and linear detection range from 0.5 pg/mL to 50 ng/mL. Based on the high sensitivity and specificity of the immunosensor, we propose this multiple amplified biosensor for early detection of CEA. Copyright © 2018 Elsevier B.V. All rights reserved.

Selective determination of dopamine using quantum-sized gold nanoparticles protected with charge selective ligands

NASA Astrophysics Data System (ADS)

Kwak, Kyuju; Kumar, S. Senthil; Lee, Dongil

2012-06-01

We report here the selective determination of dopamine (DA) using quantum-sized gold nanoparticles coated with charge selective ligands. Glutathione protected gold nanoparticles (GS-Au25) were synthesized and immobilized into a sol-gel matrix via thiol linkers. The GS-Au25 modified sol-gel electrode was found to show excellent electrocatalytic activity towards the oxidation of DA but no activity towards the oxidation of ascorbic acid. The role of electrostatic charge in the selective electrocatalytic activity of GS-Au25 was verified by voltammetry of redox markers carrying opposite charges. The pH dependent sensitivity for the determination of DA further confirmed the charge screening effect of GS-Au25. Mechanistic investigation revealed that the selectivity is attained by the selective formation of an electrostatic complex between the negatively charged GS-Au25 and DA cation. The GS-Au25 modified sol-gel electrode also showed excellent selectivity for DA in the presence of an interferent, ascorbic acid.We report here the selective determination of dopamine (DA) using quantum-sized gold nanoparticles coated with charge selective ligands. Glutathione protected gold nanoparticles (GS-Au25) were synthesized and immobilized into a sol-gel matrix via thiol linkers. The GS-Au25 modified sol-gel electrode was found to show excellent electrocatalytic activity towards the oxidation of DA but no activity towards the oxidation of ascorbic acid. The role of electrostatic charge in the selective electrocatalytic activity of GS-Au25 was verified by voltammetry of redox markers carrying opposite charges. The pH dependent sensitivity for the determination of DA further confirmed the charge screening effect of GS-Au25. Mechanistic investigation revealed that the selectivity is attained by the selective formation of an electrostatic complex between the negatively charged GS-Au25 and DA cation. The GS-Au25 modified sol-gel electrode also showed excellent selectivity for DA in the presence of an interferent, ascorbic acid. Electronic supplementary information (ESI) available: TEM image of GS-Au25, SWV of GS-Au25 in solution, effect of scan rate on the CV of GS-Au25ME, CVs of DA and AA at the bare GCE and CVs of GS-Au25ME at different pHs. See DOI: 10.1039/c2nr30481c

Selective detection and recovery of gold at tannin-immobilized non-conducting electrode.

PubMed

Banu, Khaleda; Shimura, Takayoshi; Sadeghi, Saman

2015-01-01

A tannin-immobilized glassy carbon electrode (TIGC) was prepared via electrochemical oxidation of the naturally occurring polyphenolic mimosa tannin, which generated a non-conducting polymeric film (NCPF) on the electrode surface. The fouling of the electrode surface by the electropolymerized film was evaluated by monitoring the electrode response of ferricyanide ions as a redox marker. The NCPF was permselective to HAuCl4, and the electrochemical reduction of HAuCl4 to metallic gold at the TIGC electrode was evaluated by recording the reduction current during cyclic voltammetry measurement. In the mixed electrolyte containing HAuCl4 along with FeCl3 and/or CuCl2, the NCPF remained selective toward the electrochemical reduction of HAuCl4 into the metallic state. The chemical reduction of HAuCl4 into metallic gold was also observed when the NCPF was inserted into an acidic gold solution overnight. The adsorption capacity of Au(III) on tannin-immobilized carbon fiber was 29±1.45 mg g(-1) at 60°C. In the presence of excess Cu(II) and Fe(III), tannin-immobilized NCPF proved to be an excellent candidate for the selective detection and recovery of gold through both electrochemical and chemical processes. Copyright © 2014 Elsevier B.V. All rights reserved.

Fabrication of resistively-coupled single-electron device using an array of gold nanoparticles

NASA Astrophysics Data System (ADS)

Huong, Tran Thi Thu; Matsumoto, Kazuhiko; Moriya, Masataka; Shimada, Hiroshi; Kimura, Yasuo; Hirano-Iwata, Ayumi; Mizugaki, Yoshinao

2017-08-01

We demonstrated one type of single-electron device that exhibited electrical characteristics similar to those of resistively-coupled SE transistor (R-SET) at 77 K and room temperature (287 K). Three Au electrodes on an oxidized Si chip served as drain, source, and gate electrodes were formed using electron-beam lithography and evaporation techniques. A narrow (70-nm-wide) gate electrode was patterned using thermal evaporation, whereas wide (800-nm-wide) drain and source electrodes were made using shadow evaporation. Subsequently, aqueous solution of citric acid and 15-nm-diameter gold nanoparticles (Au NPs) and toluene solution of 3-nm-diameter Au NPs chemisorbed via decanethiol were dropped on the chip to make the connections between the electrodes. Current-voltage characteristics between the drain and source electrodes exhibited Coulomb blockade (CB) at both 77 and 287 K. Dependence of the CB region on the gate voltage was similar to that of an R-SET. Simulation results of the model based on the scanning electron microscopy image of the device could reproduce the characteristics like the R-SET.

Performance Enhancement of 3-Mercaptopropionic Acid-Capped CdSe Quantum-Dot Sensitized Solar Cells Incorporating Single-Walled Carbon Nanotubes.

PubMed

Yang, Jonghee; Park, Taehee; Lee, Jongtaek; Lee, Junyoung; Shin, Hokyeong; Yi, Whikun

2016-03-01

We fabricated a series of linker-assisted quantum-dot-sensitized solar cells based on the ex situ self-assembly of CdSe quantum dots (QDs) onto TiO2 electrode using sulfide/polysulfide (S(2-)/Sn(2-)) as an electrolyte and Au cathode. Our cell were combined with single-walled carbon nanotubes (SWNTs) by two techniques; One was mixing SWNTs with TiO2 electrode and the other was spraying SWNTs onto Au electrode. Absorption spectra were used to confirm the adsorption of QDs onto TiO2 electrode. Cell performance was measured on samples containing and not-containing SWNTs. Samples mixing SWNTs with TiO2 showed higher cell efficiency, on the while sample spraying SWNTs onto Au electrode showed lower efficiency compared with pristine sample (not-containing SWNTs). Electrochemical impedance spectroscopy analysis suggested that SWNTs can act as either barriers or excellent carrier transfers according their position and mixing method.

Colloidal Au and Au-alloy catalysts for direct borohydride fuel cells: Electrocatalysis and fuel cell performance

NASA Astrophysics Data System (ADS)

Atwan, Mohammed H.; Macdonald, Charles L. B.; Northwood, Derek O.; Gyenge, Elod L.

Supported colloidal Au and Au-alloys (Au-Pt and Au-Pd, 1:1 atomic ratio) on Vulcan XC-72 (with 20 wt% metal load) were prepared by the Bönneman method. The electrocatalytic activity of the colloidal metals with respect to borohydride electro-oxidation for fuel cell applications was investigated by voltammetry on static and rotating electrodes, chronoamperometry, chronopotentiometry and fuel cell experiments. The fundamental electrochemical techniques showed that alloying Au, a metal that leads to the maximum eight-electron oxidation of BH 4 -, with Pd or Pt, well-known catalysts of dehydrogenation reactions, improved the electrode kinetics of BH 4 - oxidation. Fuel cell experiments corroborated the kinetic studies. Using 5 mg cm -2 colloidal metal load on the anode, it was found that Au-Pt was the most active catalyst giving a cell voltage of 0.47 V at 100 mA cm -2 and 333 K, while under identical conditions the cell voltage using colloidal Au was 0.17 V.

Synergistic Enhancement of Electrocatalytic CO 2 Reduction with Gold Nanoparticles Embedded in Functional Graphene Nanoribbon Composite Electrodes

DOE PAGES

Rogers, Cameron; Perkins, Wade S.; Veber, Gregory; ...

2017-02-24

Regulating the complex environment accounting for the stability, selectivity, and activity of catalytic metal nanoparticle interfaces represents a challenge to heterogeneous catalyst design. Here in this paper, we demonstrate the intrinsic performance enhancement of a composite material composed of gold nanoparticles (AuNPs) embedded in a bottom-up synthesized graphene nanoribbon (GNR) matrix for the electrocatalytic reduction of CO 2. Electrochemical studies reveal that the structural and electronic properties of the GNR composite matrix increase the AuNP electrochemically active surface area (ECSA), lower the requisite CO 2 reduction overpotential by hundreds of millivolts (catalytic onset > -0.2 V versus reversible hydrogen electrodemore » (RHE)), increase the Faraday efficiency (>90%), markedly improve stability (catalytic performance sustained over >24 h), and increase the total catalytic output (>100-fold improvement over traditional amorphous carbon AuNP supports). The inherent structural and electronic tunability of bottom-up synthesized GNR-AuNP composites affords an unrivaled degree of control over the catalytic environment, providing a means for such profound effects as shifting the rate-determining step in the electrocatalytic reduction of CO 2 to CO, and thereby altering the electrocatalytic mechanism at the nanoparticle surface.« less

Au-modified three-dimensional In2O3 inverse opals: synthesis and improved performance for acetone sensing toward diagnosis of diabetes

NASA Astrophysics Data System (ADS)

Xing, Ruiqing; Li, Qingling; Xia, Lei; Song, Jian; Xu, Lin; Zhang, Jiahuan; Xie, Yi; Song, Hongwei

2015-07-01

Analyzing the volatile organic compounds (VOCs) in exhaled breath effectively is crucial to medical treatment, which can provide a fast and noninvasive way to diagnose disease. Well-designed materials with controlled structures have great influence on the sensing performance. In this work, the ordered three dimensional inverse opal (3DIO) macroporous In2O3 films with additional via-hole architectures were fabricated and different amounts of gold nanoparticles (Au NPs) were loaded on the In2O3 films aiming at enhancing their electrical responses. The gas sensing to acetone toward diabetes diagnosis in exhaled breath was performed with different Au/In2O3 electrodes. Representatively, the best 3DIO Au/In2O3 sensor can detect acetone effectively at 340 °C with response of 42.4 to 5 ppm, the actual detection limit is as low as 20 ppb, and it holds a dynamic response of 11 s and a good selectivity. Moreover, clinical tests proved that the as-prepared 3DIO Au/In2O3 IO sensor could distinguish acetone biomarkers in human breath clearly. The excellent gas sensing properties of the Au/In2O3 electrodes were attributed to the ``spillover effects'' between Au and In2O3 and the special 3DIO structure. This work indicates that 3DIO Au/In2O3 composite is a promising electrode material for actual application in the monitoring and detection of diabetes through exhaled breath.Analyzing the volatile organic compounds (VOCs) in exhaled breath effectively is crucial to medical treatment, which can provide a fast and noninvasive way to diagnose disease. Well-designed materials with controlled structures have great influence on the sensing performance. In this work, the ordered three dimensional inverse opal (3DIO) macroporous In2O3 films with additional via-hole architectures were fabricated and different amounts of gold nanoparticles (Au NPs) were loaded on the In2O3 films aiming at enhancing their electrical responses. The gas sensing to acetone toward diabetes diagnosis in exhaled breath was performed with different Au/In2O3 electrodes. Representatively, the best 3DIO Au/In2O3 sensor can detect acetone effectively at 340 °C with response of 42.4 to 5 ppm, the actual detection limit is as low as 20 ppb, and it holds a dynamic response of 11 s and a good selectivity. Moreover, clinical tests proved that the as-prepared 3DIO Au/In2O3 IO sensor could distinguish acetone biomarkers in human breath clearly. The excellent gas sensing properties of the Au/In2O3 electrodes were attributed to the ``spillover effects'' between Au and In2O3 and the special 3DIO structure. This work indicates that 3DIO Au/In2O3 composite is a promising electrode material for actual application in the monitoring and detection of diabetes through exhaled breath. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr02709h

Platinum-gold nanoclusters as catalyst for direct methanol fuel cells.

PubMed

Giorgi, L; Giorgi, R; Gagliardi, S; Serra, E; Alvisi, M; Signore, M A; Piscopiello, E

2011-10-01

Nanosized platinum-gold alloys clusters have been deposited on gas diffusion electrode by sputter deposition. The deposits were characterized by FE-SEM, TEM and XPS in order to verify the formation of alloy nanoparticles and to study the influence of deposition technique on the nanomorphology. The deposition by sputtering process allowed a uniform distribution of metal particles on porous surface of carbon supports. Typical island growth mode was observed with the formation of a dispersed metal nanoclusters (mean size about 5 nm). Cyclic voltammetry was used to determine the electrochemical active surface and the electrocatalytic performance of the PtAu electrocatalysts for methanol oxidation reaction. The data were re-calculated in the form of mass specific activity (MSA). The sputter-catalyzed electrodes showed higher performance and stability compared to commercial catalysts.

Mechanical and thermal behavior of ionic polymer metal composites: effects of electroded metals

NASA Astrophysics Data System (ADS)

Park, Il-Seok; Kim, Sang-Mun; Kim, Kwang J.

2007-08-01

In this study, we investigated the mechanical properties of various types of ionic polymer-metal composites (IPMCs) and Pt, Au, Pd, and Pt electroded ionic liquid (IL-Pt) IPMCs, by testing tensile modulus and dynamic mechanical behavior. The SEM was utilized to investigate the characteristics of the doped electroding layer, and the DSC was probed in order to look into the thermal behavior of various types of IPMCs. Au IPMCs, having a 5-7 µm-doped layer and nanosized Au particles (ca. 10 nm), showed the highest tensile strength (56 MPa) and modulus (602 MPa) in dried conditions. With regards to thermal behavior, Au IPMC had the highest Tg (153 °C) and Tm (263 °C) in both the DMA and DSC results. The fracture behavior of various types of IPMCs followed the behavior of the base material, Nafion™, which is represented as the semicrystalline polymer characteristic.

Human serum albumin-stabilized gold nanoclusters act as an electron transfer bridge supporting specific electrocatalysis of bilirubin useful for biosensing applications.

PubMed

Santhosh, Mallesh; Chinnadayyala, Somasekhar R; Singh, Naveen K; Goswami, Pranab

2016-10-01

Human serum albumin (HSA)-stabilized Au18 nanoclusters (AuNCs) were synthesized and chemically immobilized on an Indium tin oxide (ITO) plate. The assembly process was characterized by advanced electrochemical and spectroscopic techniques. The bare ITO electrode generated three irreversible oxidation peaks, whereas the HSA-AuNC-modified electrode produced a pair of redox peaks for bilirubin at a formal potential of 0.27V (vs. Ag/AgCl). However, the native HSA protein immobilized on the ITO electrode failed to produce any redox peak for bilirubin. The results indicate that the AuNCs present in HSA act as electron transfer bridge between bilirubin and the ITO plate. Docking studies of AuNC with HSA revealed that the best docked structure of the nanocluster is located around the vicinity of the bilirubin binding site, with an orientation that allows specific oxidation. When the HSA-AuNC-modified electrode was employed for the detection of bilirubin using chronoamperometry at 0.3V (vs. Ag/AgCl), a steady-state current response against bilirubin in the range of 0.2μM to 7μM, with a sensitivity of 0.34μAμM(-1) and limit of detection of 86.32nM at S/N 3, was obtained. The bioelectrode was successfully applied to measure the bilirubin content in spiked serum samples. The results indicate the feasibility of using HSA-AuNC as a biorecognition element for the detection of serum bilirubin levels using an electrochemical technique. Copyright © 2016 Elsevier B.V. All rights reserved.

Electrochemically assisted fabrication of size-exclusion films of organically modified silica and application to the voltammetry of phospholipids.

PubMed

Mehdi, B Layla; Rutkowska, Iwona A; Kulesza, Pawel J; Cox, James A

2013-06-01

Modification of electrodes with nm-scale organically modified silica films with pores diameters controlled at 10- and 50-nm is described. An oxidation catalyst, mixed-valence ruthenium oxide with cyano crosslinks or gold nanoparticles protected by dirhodium-substituted phosophomolybdate (AuNP-Rh 2 PMo 11 ), was immobilized in the pores. These systems comprise size-exclusion films at which the biological compounds, phosphatidylcholine and cardiolipin, were electrocatalytically oxidized without interference from surface-active concomitants such as bovine serum albumin. 10-nm pores were obtained by adding generation-4 poly(amidoamine) dendrimer, G4-PAMAM, to a (CH 3 ) 3 SiOCH 3 sol. 50-nm pores were obtained by modifying a glassy carbon electrode (GC) with a sub-monolayer film of aminopropyltriethoxylsilane, attaching 50-nm diameter poly(styrene sulfonate), PSS, spheres to the protonated amine, transferring this electrode to a (CH 3 ) 3 SiOCH 3 sol, and electrochemically generating hydronium at uncoated GC sites, which catalyzed ormosil growth around the PSS. Voltammetry of Fe(CN) 6 3- and Ru(NH 3 ) 6 3+ demonstrated the absence of residual charge after removal of the templating agents. With the 50-nm system, the pore structure was sufficiently defined to use layer-by-layer electrostatic assembly of AuNP-Rh 2 PMo 11 therein. Flow injection amperometry of phosphatidylcholine and cardiolipin demonstrated analytical utility of these electrodes.

A multifunctional hemin@metal-organic framework and its application to construct an electrochemical aptasensor for thrombin detection.

PubMed

Xie, Shunbi; Ye, Jiawei; Yuan, Yali; Chai, Yaqin; Yuan, Ruo

2015-11-21

A new type of multifunctional metal-organic framework (MOF) has been synthesized by encapsulating hemin into the nano-sized Fe-MIL-88 MOFs (hemin@MOFs) and first applied in an electrochemical aptasensor to detect thrombin (TB) with the aid of an enzyme for signal amplification. The gold nanoparticle functionalized hemin@MOFs (Au/hemin@MOFs) have not only simultaneously served as redox mediators and solid electrocatalysts, but have also been utilized as an ideal loading platform to immobilize a large number of biomolecules. In this aptasensor, Au/hemin@MOFs conjugated with glucose oxidase (GOD) and thrombin binding aptamer (TBA II) were used as the secondary aptamer bioconjugates (Au/hemin@MOF-TBA II-GOD bioconjugates), and TB was sandwiched between Au/hemin@MOF-TBA II-GOD bioconjugates and the amino-terminated TBA I which was self-assembled on the gold nanoparticle (AuNP) modified electrode. The GOD could oxidize glucose into gluconic acid accompanied by the generation of H2O2. The generated H2O2 on the electrode surface was further electrocatalyzed by hemin@MOFs to amplify the electrochemical signal of hemin contained in hemin@MOFs. Therefore, the synthesized hemin@MOFs represented a new paradigm for multifunctional materials since it combined three different functions including serving as catalysts, redox mediators and loading platforms within a single material. With such an ingenious design, a wide linear range of 0.0001 nM to 30 nM was acquired with a relatively low detection limit of 0.068 pM for TB detection.

In Situ Electrochemical Sensing and Real-Time Monitoring Live Cells Based on Freestanding Nanohybrid Paper Electrode Assembled from 3D Functionalized Graphene Framework.

PubMed

Zhang, Yan; Xiao, Jian; Lv, Qiying; Wang, Lu; Dong, Xulin; Asif, Muhammad; Ren, Jinghua; He, Wenshan; Sun, Yimin; Xiao, Fei; Wang, Shuai

2017-11-08

In this work, we develop a new type of freestanding nanohybrid paper electrode assembled from 3D ionic liquid (IL) functionalized graphene framework (GF) decorated by gold nanoflowers (AuNFs), and explore its practical application in in situ electrochemical sensing of live breast cell samples by real-time tracking biomarker H 2 O 2 released from cells. The AuNFs modified IL functionalized GF (AuNFs/IL-GF) was synthesized via a facile and efficient dopamine-assisted one-pot self-assembly strategy. The as-obtained nanohybrid assembly exhibits a typical 3D hierarchical porous structure, where the highly active electrocatalyst AuNFs are well dispersed on IL-GF scaffold. And the graft of hydrophilic IL molecules (i.e., 1-butyl-3-methylimidazolium tetrafluoroborate, BMIMBF 4 ) on graphene nanosheets not only avoids their agglomeration and disorder stacking during the self-assembly but also endows the integrated IL-GF monolithic material with unique hydrophilic properties, which enables it to be readily dispersed in aqueous solution and processed into freestanding paperlike material. Because of the unique structural properties and the combinational advantages of different components in the AuNFs/IL-GF composite, the resultant nanohybrid paper electrode exhibits good nonenzymatic electrochemical sensing performance toward H 2 O 2 . When used in real-time tracking H 2 O 2 secreted from different breast cells attached to the paper electrode without or with radiotherapy treatment, the proposed electrochemical sensor based on freestanding AuNFs/IL-GF paper electrode can distinguish the normal breast cell HBL-100 from the cancer breast cells MDA-MB-231 and MCF-7 cells, and assess the radiotherapy effects to different breast cancer cells, which opens a new horizon in real-time monitoring cancer cells by electrochemical sensing platform.

Organic nonvolatile resistive memory devices based on thermally deposited Au nanoparticle

NASA Astrophysics Data System (ADS)

Jin, Zhiwen; Liu, Guo; Wang, Jizheng

2013-05-01

Uniform Au nanoparticles (NPs) are formed by thermally depositing nominal 2-nm thick Au film on a 10-nm thick polyimide film formed on a Al electrode, and then covered by a thin polymer semiconductor film, which acts as an energy barrier for electrons to be injected from the other Al electrode (on top of polymer film) into the Au NPs, which are energetically electron traps in such a resistive random access memory (RRAM) device. The Au NPs based RRAM device exhibits estimated retention time of 104 s, cycle times of more than 100, and ON-OFF ratio of 102 to 103. The carrier transport properties are also analyzed by fitting the measured I-V curves with several conduction models.

Platinum nanoparticles decorated dendrite-like gold nanostructure on glassy carbon electrodes for enhancing electrocatalysis performance to glucose oxidation

NASA Astrophysics Data System (ADS)

Jia, Hongmei; Chang, Gang; Lei, Ming; He, Hanping; Liu, Xiong; Shu, Honghui; Xia, Tiantian; Su, Jie; He, Yunbin

2016-10-01

Platinum nanoparticles decorated dendrite-like gold nanostructure, bimetal composite materials on glassy carbon electrode (Pt/DGNs/GC) for enhancing electrocatalysis to glucose oxidation was designed and successfully fabricated by a facile two-step deposition method without any templates, surfactants, or stabilizers. Dendrite-like gold nanostructure was firstly deposited on the GC electrode via the potentiostatic method, and then platinum nanoparticles were decorated on the surface of gold substrate through chemical reduction deposition. X-ray diffraction (XRD), field-emission scanning electron microscope (FE-SEM), energy-dispersive X-ray spectroscopy (EDS) were applied to characterize the evolution of morphology and structure of the as-prepared Pt/DGNs/GC. Based on electrochemical measurements such as cyclic voltammetry, linear voltammetry and chronoamperometry, Pt/DGNs/GC exhibited significantly enhanced electrocatalytic performance to glucose oxidation compared those of pure dendrite-like Au nanoparticles in our previous report. Controlling chemical reduction deposition time, the amount of platinum nanoparticles on Au surface could be regulated, which further tuned electrocatalytic properties toward glucose oxidation. The dendrite-like gold surface partially covered by platinum nanoparticles dramatically enhanced the electrocatalytic performance for the oxidation of glucose because of excellent synergetic effects between gold and platinum species and the increased electrochemical active area from Pt nanoparticles loading. The non-enzymatic glucose biosensor based on Pt/DGNs/GC showed a rapid respond time (within 2 s), wide linear range (from 0.1 mM to 14 mM), low detection limit (0.01 mM), supernal sensitivity (275.44 μA cm-2 mM-1, R = 0.993), satisfactory reproducibility and good stability for glucose sensing. It was demonstrated that Pt/DGNs/GC could work as promising candidate for factual non-enzymatic glucose detection.

Influence of the solution pH in the 6-mercaptopurine self-assembled monolayer (6MP-SAM) on a Au(111) single-crystal electrode.

PubMed

Madueño, Rafael; García-Raya, Daniel; Viudez, Alfonso J; Sevilla, José M; Pineda, Teresa; Blázquez, Manuel

2007-10-23

Self-assembled monolayers (SAMs) of 6-mercaptopurine (6MP) have been prepared on a Au(111) single-crystal electrode by immersion of the metal surface in a 100 microM 6MP and 0.01 M HClO4 solution. The 6MP-SAM Au(111) single-crystal electrodes were transferred to the cell and allowed to equilibrate with the different aqueous working solutions before the electrochemical experiments. The influence of the solution pH was studied by cyclic voltammetry, double layer capacitance curves, and electrochemical impedance spectroscopy. The electrochemical behavior of the 6MP-SAM in acetic acid at pH 4 presents important differences in comparison to that obtained in 0.1 M KOH solutions. Cyclic voltammograms for the reductive desorption process in acid medium are broad and show some features that can be explained by a phase transition between a chemisorbed and a physisorbed state of the 6MP molecules. The low solubility of these molecules in acid medium could explain this phenomenon and the readsorption of the complete monolayer when the potential is scanned in the positive direction. The variation of the double-layer capacitance values in the potential range of monolayer stability with the pH suggests that the acid-base chemistry of the 6MP molecules is playing a role. This fact has been studied by following the variations of the electron-transfer rate constant of the highly charged redox probes as are Fe(CN)(6)-3/-4 and Ru(NH3)(6)+3/+2 as a function of solution pH. The apparent surface pKa value for the 6MP-SAM (pKa approximately 8) is explained by the total conversion of the different 6MP tautomers that exist in solution to the thiol species in the adsorbed state.

Efficient CH3NH3PbI3 perovskite/fullerene planar heterojunction hybrid solar cells with oxidized Ni/Au/Cu transparent electrode

NASA Astrophysics Data System (ADS)

Lai, Wei-Chih; Lin, Kun-Wei; Guo, Tzung-Fang; Chen, Peter; Liao, Yuan-Yu

2018-02-01

We demonstrated the performance of inverted CH3NH3PbI3 perovskite-based solar cells (SCs) with a thermally oxidized nickel/gold/copper (Ni/Au/Cu) trilayer transparent electrode. Oxidized Ni/Au/Cu is a high transparent layer and has less resistance than the oxidized Ni/Au layer. Like the oxidized Ni/Au layer, oxidized Ni and Cu in oxidized Ni/Au/Cu could perform as a hole transport layer of the perovskite-based SCs. It leads to improved perovskite SC performance on an open circuit voltage of 1.01 V, a short circuit current density of 14.36 mA/cm2, a fill factor of 76.7%, and a power conversion efficiency (η%) of 11.1%. The η% of perovskite SCs with oxidized Ni (10 nm)/Au (6 nm)/Cu (1 nm) improved by approximately 10% compared with that of perovskite SCs with oxidized Ni/Au.

Synthesis, characterization, and electrochemical behavior of Au@Pd core shell nanoparticles

NASA Astrophysics Data System (ADS)

Wicaksono, W. P.; Ivandini, T. A.

2017-04-01

Au@Pd core shell nanoparticles (Au@Pd CSNPs) were successfully synthesized using a seed-mediated growth method. Firstly, a pale pink gold seed solution was used to produce a pale purple gold nanoparticles (AuNPs) core solution. Then, three series of Pd shell thickness using 20μ, 100 μL, and 500 μL of PdCl2 produced purple, brown, and deep brown of Au@Pd CSNPs respectively. A strong absorbance UV-Visible spectrum with peaks at 285 nm and 535 nm was identified for AuNPs formation. The disappearance of the peak at 535 nm was indicated the Au@Pd CSNPs formation. The electrochemical properties were examined in phosphate buffer pH 7 using cyclic voltammetry technique with boron-doped diamond (BDD) as working electrode showed a couple oxidation and reduction peak of gold at 0.67 V and at 0.33 V, respectively. The Au@Pd CNPs will be used for modification of BDD electrodes.

Performance assessment of polymer based electrodes for in vitro electrophysiological sensing: the role of the electrode impedance

NASA Astrophysics Data System (ADS)

Medeiros, Maria C. R.; Mestre, Ana L. G.; Inácio, Pedro M. C.; Santos, José M. L.; Araujo, Inês M.; Bragança, José; Biscarini, Fabio; Gomes, Henrique L.

2016-09-01

Conducting polymer electrodes based on poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) are used to record extracellular signals from autonomous cardiac contractile cells and glioma cell cultures. The performance of these conducting polymer electrodes is compared with Au electrodes. A small-signal impedance analysis shows that in the presence of an electrolyte, both Au and polymer electrodes establish high capacitive double-layers. However, the polymer/electrolyte interfacial resistance is 3 orders of magnitude lower than the resistance of the metal/electrolyte interface. The polymer low interfacial resistance minimizes the intrinsic thermal noise and increases the system sensitivity. However, when measurements are carried out in current mode a low interfacial resistance partially acts as a short circuit of the interfacial capacitance, this affects the signal shape.

Electrokinetic acceleration of DNA hybridization in microsystems.

PubMed

Lei, Kin Fong; Wang, Yun-Hsiang; Chen, Huai-Yi; Sun, Jia-Hong; Cheng, Ji-Yen

2015-06-01

In this work, electrokinetic acceleration of DNA hybridization was investigated by different combinations of frequencies and amplitudes of actuating electric signals. Because the frequencies from low to high can induce different kinds of electrokinetic forces, i.e., electroosmotic to electrothermal forces, this work provides an in-depth investigation of electrokinetic enhanced hybridization. Concentric circular Cr/Au microelectrodes of 350 µm in diameter were fabricated on a glass substrate and probe DNA was immobilized on the electrode surface. Target DNA labeled with fluorescent dyes suspending in solution was then applied to the electrode. Different electrokinetic forces were induced by the application of different electric signals to the circular microelectrodes. Local microfluidic vortexes were generated to increase the collision efficiency between the target DNA suspending in solution and probe DNA immobilized on the electrode surface. DNA hybridization on the electrode surface could be accelerated by the electrokinetic forces. The level of hybridization was represented by the fluorescent signal intensity ratio. Results revealed that such 5-min dynamic hybridization increased 4.5 fold of signal intensity ratio as compared to a 1-h static hybridization. Moreover, dynamic hybridization was found to have better differentiation ability between specific and non-specific target DNA. This study provides a strategy to accelerate DNA hybridization in microsystems. Copyright © 2015 Elsevier B.V. All rights reserved.

Chemical and Biological Sensors Based on Organic Electrochemical Transistors

NASA Astrophysics Data System (ADS)

Lin, Peng

Organic thin film transistors (OTFTs) have been explored for sensing applications for several decades due to their many advantages like easy fabrication, low cost, flexibility, and biocompatibility. Among these OTFTs, organic electrochemical transistors (OECTs) have attracted a great deal of interest in recent years since the devices can operate stably in aqueous environment with relatively low working voltages and are suitable for applications in chemical and biological sensing. In this thesis, ion-sensitive properties of OECTs based on poly(3,4- ethylenedioxythiophene):poly(styrene sulfonic acid) (PEDOT:PSS) have been systematically studied. It was found that the gate electrode played an important role on the ion-sensitive properties of OECTs. For the devices with Ag/AgCl gate electrode, Nernstian relationships between the shift of gate voltage and the concentrations of cations were obtained. For the devices with Pt and Au gate electrodes, the ion sensitivities were higher than that given by Nernst equation, which could be attributed to the interface between the metal gate electrode and the electrolyte. Moreover, OECTs based on PEDOT:PSS were integrated into flexible microfluidic systems. Then a novel label-free DNA sensor was developed, in which single-stranded DNA probes were immobilized on the surface of Au gate electrode. These devices successfully detected complementary DNA targets at concentrations as low as 1 nM. The detection limit was also extended to 10 pM by pulse-enhanced hybridization process of DNA. OECTs based on PEDOT:PSS were also exploited as cell-based biosensors. Human esophageal squamous epithelial cancer cell lines (KYSE30) and fibroblast cell lines (HFFI) were successfully grown on the surface of PEDOT:PSS film. Then the devices were used for in-vitro monitoring cell activities when the living cells were treated by trypsin and an anti-cancer drug, retinoic acid. It was found that the devices were sensitive to the change of surface charge and morphology of adherent cells. Finally, micro-dimensional OECT arrays were fabricated by photolithography. The fabrication process was mainly divided into three steps, i.e. fabrication of gold electrodes, fabrication of PEDOT:PSS films, and fabrication of PEG mirowells. Compared with macro-dimensional OECTs, micro-dimensional OECTs showed better electrical performance, such as faster response time and better stability in aqueous solution.

Enhanced chemiluminescence-based detection on gold substrate after electrografting of diazonium precursor-coated gold nanoparticles.

PubMed

Houmed Adabo, Ali; Zeggari, Rabah; Mohamed Saïd, Nasser; Bazzi, Rana; Elie-Caille, Céline; Marquette, Christophe; Martini, Matteo; Tillement, Olivier; Perriat, Pascal; Chaix, Carole; Boireau, Wilfrid; Roux, Stéphane

2016-04-01

Since it was demonstrated that nanostructured surfaces are more efficient for the detection based on the specific capture of analytes, there is a real need to develop strategies for grafting nanoparticles onto flat surfaces. Among the different routes for the functionalization of a surface, the reduction of diazonium salts appears very attractive for the covalent immobilization of nanoparticles because this method does not require a pre-treatment of the surface. For achieving this goal, gold nanoparticles coated by precursor of diazonium salts were synthesized by reduction of gold salt in presence of mercaptoaniline. These mercaptoaniline-coated gold nanoparticles (Au@MA) were successfully immobilized onto various conducting substrates (indium tin oxide (ITO), glassy carbon (GC) and gold electrodes with flat terraces) after addition of sodium nitrite at fixed potential. When applied onto the gold electrodes, such a grafting strategy led to an obvious enhancement of the luminescence of luminol used for the biodetection. Copyright © 2016 Elsevier Inc. All rights reserved.

N-doped graphene-carbon nanotube hybrid networks attaching with gold nanoparticles for glucose non-enzymatic sensor.

PubMed

Jeong, Hun; Nguyen, Dang Mao; Lee, Min Sang; Kim, Hong Gun; Ko, Sang Cheol; Kwac, Lee Ku

2018-09-01

Herein, we successfully developed a novel three dimensional (3D) opened networks based on nitrogen doped graphene‑carbon nanotubes attaching with gold nanoparticles (N-GR-CNTs/AuNPs) to apply for non-enzymatic glucose determination. It was demonstrated that the N-GR-CNTs/AuNPs modified electrode exhibited good behavior for glucose detection with a long linear range of 2 μM to 19.6 mM, high sensitivity of 0.9824 μA·mM -1 ·cm -2 , low detection limit of 500 nM, and negligible interference effect. The high performance of the N-GR-CNTs/AuNPs based sensor was assumed due to the outstanding catalytic activity of AuNPs well dispersing on N-GR-CNTs networks, which exhibited as a perfect supporting scaffold due to the enhanced electrical conductivity and large surface area. The obtained results indicated that the N-GR-CNTs/AuNPs hybrid is highly promising for sensitive and selective detection of glucose in sensor application. Copyright © 2018 Elsevier B.V. All rights reserved.

Horseradish peroxidase functionalized gold nanorods as a label for sensitive electrochemical detection of alpha-fetoprotein antigen.

PubMed

Guo, Jinjin; Han, Xiaowei; Wang, Junchun; Zhao, Junqing; Guo, Zilin; Zhang, Yuzhong

2015-12-15

In this study, a novel tracer, horseradish peroxidase (HRP) functionalized gold nanorods (Au NRs) nanocomposites (HRP-Au NRs), was designed to label the signal antibodies for sensitive electrochemical measurement of alpha-fetoprotein (AFP). The preparation of HRP-Au NRs nanocomposites and the labeling of secondary antibody (Ab2) were performed by one-pot assembly of HRP and Ab2 on the surface of Au NRs. The immunosensor was fabricated by assembling carbon nanotubes (CNTs), Au NRs, and capture antibodies (Ab1) on the glassy carbon electrode. In the presence of AFP antigen, the labels were captured on the surface of the Au NRs/CNTs via specific recognition of antigen-antibody, resulting in the signal intensity being clearly increased. Differential pulse voltammetry (DPV) was employed to record the response signal of the immunosensor in phosphate-buffered saline (PBS) containing hydrogen peroxide (H2O2) and 3,3',5,5'-tetramethylbenzidine (TMB). Under optimal conditions, the signal intensity was linearly related to the concentration of AFP in the range of 0.1-100 ng ml(-1), and the limit of detection was 30 pg ml(-1) (at signal/noise [S/N] = 3). Furthermore, the immunoassay method was evaluated using human serum samples, and the recovery obtained was within 99.0 and 102.7%, indicating that the immunosensor has potential clinical applications. Copyright © 2015 Elsevier Inc. All rights reserved.

Using reduced graphene oxide-Ca:CdSe nanocomposite to enhance photoelectrochemical activity of gold nanoparticles functionalized tungsten oxide for highly sensitive prostate specific antigen detection.

PubMed

Wang, Xueping; Xu, Rui; Sun, Xu; Wang, Yaoguang; Ren, Xiang; Du, Bin; Wu, Dan; Wei, Qin

2017-10-15

An ultrasensitive sandwich-type photoelectrochemical (PEC) immunosensor was constructed for the detection of prostate specific antigen (PSA). In this work, Au-nanoparticle-loaded tungsten oxide (WO 3 -Au) hybrid composites was applied as PEC sensing platform, while Ca ions doped CdSe equipped on the conducting framework of reduced graphene oxide (rGO-Ca:CdSe) nanocomposites were employed as the signal amplification probe. As for WO 3 -Au, massive Au nanoparticles were formed on the surface of WO 3 without any additional reducing agent, providing a novel nanocarriers for anchoring plenty of the primary antibodies due to the large specific surface area and good biocompatibility by chemical bonding between Au nanoparticles and -NH 2 of antibodies. Besides, the incorporation of the rGO and the doping of Ca ions could improve the conductivity and hinder the recombination of electron-hole pairs of CdSe nanoparticles effectively, thereby enhancing the photocurrent conversion efficiency. Based on the sandwich immunoreaction, the primary antibody was immobilized onto WO 3 -Au substrate, after the formed rGO-Ca:CdSe labels were captured onto the electrode surface via the specific antibody-antigen interaction, the photocurrent intensity could be further enhanced due to the sensitization effect. Under the optimal conditions, the proposed PEC immunosensor shows a linear relationship between photocurrent variation and the logarithm of PSA concentration in the wide range of 5pgmL -1 to 50ngmL -1 with a low detection limit of 2.6pgmL -1 (S/N=3). Moreover, it also presented good stability and acceptable specificity, indicating the potential applications in clinical diagnostics. Copyright © 2017 Elsevier B.V. All rights reserved.

Electrochemical sensing of sulphur dioxide: a comparison using dodecanethiol and citrate capped gold nanoclusters.

PubMed

Sathe, Bhaskar R; Risbud, Mandar S; Mulla, Imtiaz S; Pillai, Vijayamohanan K

2008-06-01

A comparison of cyclic voltammograms of dodecanethiol (DDT) capped Au nanoclusters (5.0 0.5 nm) and trisodium citrate (Cit) capped Au nanoclusters (approximately 10-15 nm) modified glassy carbon electrode shows a dramatic variation in the current when exposed to a small amount of sulphur dioxide. This is explained using the electrocatalytic properties of Au nanoclusters towards the oxidation of SO2, thus facilitating the fabrication of electrochemical sensors for the detection of SO2. The intrinsic redox changes observed for gold nanocluster-modified glassy carbon electrodes disappear on passing SO2, despite a dramatic current increase, which indeed scales up with the amount of dissolved SO2. Interestingly, a complete rejuvenation of the redox behavior of gold is also observed on subsequent removal of SO2 from the solution by passing pure nitrogen for 15 minutes. Further, these nanoclusters when characterized with X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) after SO2 passage reveal a variety of SO2 adsorption modes on gold surface. XP spectra also show a shift of 1.03 eV towards higher binding energy indicating a strong adsorption of SO2 gas, while FTIR gives conclusive evidence for the interaction of SO2 with gold nanoparticles.

Impedimetric Aptasensor for Ochratoxin A Determination Based on Au Nanoparticles Stabilized with Hyper-Branched Polymer

PubMed Central

Evtugyn, Gennady; Porfireva, Anna; Stepanova, Veronika; Kutyreva, Marianna; Gataulina, Alfiya; Ulakhovich, Nikolay; Evtugyn, Vladimir; Hianik, Tibor

2013-01-01

An impedimetric aptasensor for ochratoxin A (OTA) detection has been developed on the base of a gold electrode covered with a new modifier consisting of electropolymerized Neutral Red and a mixture of Au nanoparticles suspended in the dendrimeric polymer Botlorn H30®. Thiolated aptamer specific to OTA was covalently attached to Au nanoparticles via Au-S bonding. The interaction of the aptamer with OTA induced the conformational switch of the aptamer from linear to guanine quadruplex form followed by consolidation of the surface layer and an increase of the charge transfer resistance. The aptasensor makes it possible to detect from 0.1 to 100 nM of OTA (limit of detection: 0.02 nM) in the presence of at least 50 fold excess of ochratoxin B. The applicability of the aptasensor for real sample assay was confirmed by testing spiked beer samples. The recovery of 2 nM OTA was found to be 70% for light beer and 78% for dark beer. PMID:24287535

A double signal amplification platform for ultrasensitive and simultaneous detection of ascorbic acid, dopamine, uric acid and acetaminophen based on a nanocomposite of ferrocene thiolate stabilized Fe₃O₄@Au nanoparticles with graphene sheet.

PubMed

Liu, Meiling; Chen, Qiong; Lai, Cailang; Zhang, Youyu; Deng, Jianhui; Li, Haitao; Yao, Shouzhuo

2013-10-15

A double signal amplification platform for ultrasensitive and simultaneous detection of ascorbic acid (AA), dopamine (DA), uric acid (UA) and acetaminophen (AC) was fabricated by a nanocomposite of ferrocene thiolate stabilized Fe₃O₄@Au nanoparticles with graphene sheet. The platform was constructed by coating a newly synthesized phenylethynyl ferrocene thiolate (Fc-SAc) modified Fe₃O₄@Au NPs coupling with graphene sheet/chitosan (GS-chitosan) on a glassy carbon electrode (GCE) surface. The Fe₃O₄@Au-S-Fc/GS-chitosan modified GCE exhibits a synergistic catalytic and amplification effect toward AA, DA, UA and AC oxidation. The oxidation peak currents of the four compounds on the electrode were linearly dependent on AA, DA, UA and AC concentrations in the ranges of 4-400 μM, 0.5-50 μM, 1-300 μM and 0.3-250 μM in the individual detection of each component, respectively. By simultaneously changing the concentrations of AA, DA, UA and AC, their electrochemical oxidation peaks appeared at -0.03, 0.15, 0.24 and 0.35 V, and good linear current responses were obtained in the concentration ranges of 6-350, 0.5-50, 1-90 and 0.4-32 μM with the detection limits of 1, 0.1, 0.2 and 0.05 μM (S/N=3), respectively. Copyright © 2013 Elsevier B.V. All rights reserved.

Effects of V2O5/Au bi-layer electrodes on the top contact Pentacene-based organic thin film transistors

NASA Astrophysics Data System (ADS)

Borthakur, Tribeni; Sarma, Ranjit

2017-05-01

Top-contact Pentacene-based organic thin film transistors (OTFTs) with a thin layer of Vanadium Pent-oxide between Pentacene and Au layer are fabricated. Here we have found that the devices with V2O5/Au bi-layer source-drain electrode exhibit better field-effect mobility, high on-off ratio, low threshold voltage and low sub-threshold slope than the devices with Au only. The field-effect mobility, current on-off ratio, threshold voltage and sub-threshold slope of V2O5/Au bi-layer OTFT estimated from the device with 15 nm thick V2O5 layer is .77 cm2 v-1 s-1, 7.5×105, -2.9 V and .36 V/decade respectively.

Electrical immunosensor based on a submicron-gap interdigitated electrode and gold enhancement.

PubMed

Ahn, Junhyoung; Lee, Tae Han; Li, Taihua; Heo, Kwang; Hong, Seunghun; Ko, Jeongheon; Kim, Yongsam; Shin, Yong-Beom; Kim, Min-Gon

2011-08-15

We demonstrated that the detection of human interleukin 5 (IL5) with a higher sensitivity than the enzyme-linked immunosorbent assay (ELISA) was possible using mass-producible submicron-gap interdigitated electrodes (IDEs) combined with signal amplification by a gold nanoparticle (AuNP) and gold enhancement. IDEs, facing comb-shape electrodes, can act as simple and miniaturized devices for immunoassay. An IDE with a gap size of 400nm was fabricated by a stepper photolithography process and was applied for the immunoassay of human IL5. A biotinylated anti-human IL5 was immobilized on the streptavidin-modified IDE, and biotin-bovine serum albumin (BSA) and BSA were added sequentially to reduce non-specific binding between the streptavidin-immobilized IDE surface and other proteins. The immunoassay procedure included three main steps: the reaction of human IL5 to form antigen-antibody complexes, the binding of AuNP conjugation with an antibody against human IL5 for the sandwich immunoassay, and gold enhancement for electrical signal amplification. The measurement of electrical current at each step showed that the gold enhancement step was very critical in detection of the concentration of human IL5. Analysis by scanning electron microscope (SEM) showed that close to 1μm particles were formed from 10nm AuNP by the gold enhancement reaction using gold ions and hydroxylamine. Under optimized conditions, human IL5 could be analyzed at 1pgmL(-1) with a wide dynamic range (from 10(-3) to 100ngmL(-1) concentrations). Copyright © 2011 Elsevier B.V. All rights reserved.

Electrochemistry of Canis familiaris cytochrome P450 2D15 with gold nanoparticles: An alternative to animal testing in drug discovery.

PubMed

Rua, Francesco; Sadeghi, Sheila J; Castrignanò, Silvia; Valetti, Francesca; Gilardi, Gianfranco

2015-10-01

This work reports for the first time the direct electron transfer of the Canis familiaris cytochrome P450 2D15 on glassy carbon electrodes to provide an analytical tool as an alternative to P450 animal testing in the drug discovery process. Cytochrome P450 2D15, that corresponds to the human homologue P450 2D6, was recombinantly expressed in Escherichia coli and entrapped on glassy carbon electrodes (GC) either with the cationic polymer polydiallyldimethylammonium chloride (PDDA) or in the presence of gold nanoparticles (AuNPs). Reversible electrochemical signals of P450 2D15 were observed with calculated midpoint potentials (E1/2) of −191 ± 5 and −233 ± 4 mV vs. Ag/AgCl for GC/PDDA/2D15 and GC/AuNPs/2D15, respectively. These experiments were then followed by the electro-catalytic activity of the immobilized enzyme in the presence of metoprolol. The latter drug is a beta-blocker used for the treatment of hypertension and is a specific marker of the human P450 2D6 activity. Electrocatalysis data showed that only in the presence of AuNps the expected α-hydroxy-metoprolol product was present as shown by HPLC. The successful immobilization of the electroactive C. familiaris cytochrome P450 2D15 on electrode surfaces addresses the ever increasing demand of developing alternative in vitromethods for amore detailed study of animal P450 enzymes' metabolism, reducing the number of animals sacrificed in preclinical tests.

Synthesis of flower-like gold nanoparticles and their electrocatalytic activity towards the oxidation of methanol and the reduction of oxygen.

PubMed

Jena, Bikash Kumar; Raj, C Retna

2007-03-27

This article describes the synthesis of branched flower-like gold (Au) nanocrystals and their electrocatalytic activity toward the oxidation of methanol and the reduction of oxygen. Gold nanoflowers (GNFs) were obtained by a one-pot synthesis using N-2-hydroxyethylpiperazine-N-2-ethanesulphonic acid (HEPES) as a reducing/stabilizing agent. The GNFs have been characterized by UV-visible spectroscopy, transmission electron microscopy (TEM), X-ray diffraction (XRD), and electrochemical measurements. The UV-visible spectra show two bands corresponding to the transverse and longitudinal surface plasmon (SP) absorption at 532 and 720 nm, respectively, for the colloidal GNFs. The GNFs were self-assembled on a sol-gel-derived silicate network, which was preassembled on a polycrystalline Au electrode and used for electrocatalytic applications. The GNFs retain their morphology on the silicate network; the UV-visible diffuse reflectance spectra (DRS) of GNFs on the silicate network show longitudinal and transverse bands as in the case of colloidal GNFs. The GNFs show excellent electrocatalytic activity toward the oxidation of methanol and the reduction of oxygen. Oxidation of methanol in alkaline solution was observed at approximately 0.245 V, which is much less positive than that on an unmodified polycrystalline gold electrode. Reduction of oxygen to H2O2 and the further reduction of H2O2 to water in neutral pH were observed at less negative potentials on the GNFs electrode. The electrocatalytic activity of GNFs is significantly higher than that of the spherically shaped citrate-stabilized Au nanoparticles (SGNs).

Self-Assembly of Large Gold Nanoparticles for Surface-Enhanced Raman Spectroscopy.

PubMed

Yang, Guang; Nanda, Jagjit; Wang, Boya; Chen, Gang; Hallinan, Daniel T

2017-04-19

Performance of portable technologies from mobile phones to electric vehicles is currently limited by the energy density and lifetime of lithium batteries. Expanding the limits of battery technology requires in situ detection of trace components at electrode-electrolyte interphases. Surface-enhance Raman spectroscopy could satisfy this need if a robust and reproducible substrate were available. Gold nanoparticles (Au NPs) larger than 20 nm diameter are expected to greatly enhance Raman intensity if they can be assembled into ordered monolayers. A three-phase self-assembly method is presented that successfully results in ordered Au NP monolayers for particle diameters ranging from 13 to 90 nm. The monolayer structure and Raman enhancement factors (EFs) are reported for a model analyte, rhodamine, as well as the best performing polymer electrolyte salt, lithium bis(trifluoromethane)sulfonimide. Experimental EFs for the most part correlate with predictions based on monolayer geometry and with numerical simulations that identify local electromagnetic field enhancements. The EFs for the best performing Au NP monolayer are between 10 6 and 10 8 and give quantitative signal response when analyte concentration is changed.

Spectro-Electrochemical Examination of the Formation of Dimethyl Carbonate from CO and Methanol at Different Electrode Materials

PubMed Central

2017-01-01

In this work, we report a fundamental mechanistic study of the electrochemical oxidative carbonylation of methanol with CO for the synthesis of dimethyl carbonate on metallic electrodes at low overpotentials. For the first time, the reaction was shown to take place on the metallic catalysts without need of oxidized metals or additives. Moreover, in-situ spectroelectrochemical techniques were applied to this electrosynthesis reaction in order to reveal the reaction intermediates and to shed light into the reaction mechanism. Fourier transformed infrared spectroscopy was used with different electrode materials (Au, Pd, Pt, and Ag) to assess the effect of the electrode material on the reaction and the dependence of products and intermediates on the applied potentials. It was observed that the dimethyl carbonate is only formed when the electrode is able to decompose/oxidize MeOH to form (adsorbed) methoxy groups that can further react with CO to dimethyl carbonate. Furthermore, the electrode needs to adsorb CO not too strongly; otherwise, further reaction will be inhibited because of surface poisoning by CO. PMID:28929754

Au/ZnO hybrid nanocatalysts impregnated in N-doped graphene for simultaneous determination of ascorbic acid, acetaminophen and dopamine.

PubMed

Chen, Xianlan; Zhang, Guowei; Shi, Ling; Pan, Shanqing; Liu, Wei; Pan, Hiabo

2016-08-01

The formation of nitrogen-doped (N-doped) graphene uses hydrothermal method with urea as reducing agent and nitrogen source. The surface elemental composition of the catalyst was analyzed through XPS, which showed a high content of a total N species (7.12at.%), indicative of the effective N-doping, present in the form of pyridinic N, pyrrolic N and graphitic N groups. Moreover, Au nanoparticles deposited on ZnO nanocrystals surface, forming Au/ZnO hybrid nanocatalysts, undergo a super-hydrophobic to super-hydrophilic conversion. Herein, we present Au/ZnO hybrid nanocatalysts impregnated in N-doped graphene sheets through sonication technique of the Au/ZnO/N-doped graphene hybrid nanostructures. The as-prepared Au/ZnO/N-doped graphene hybrid nanostructure modified glassy carbon electrode (Au/ZnO/N-doped graphene/GCE) was first employed for the simultaneous determination of ascorbic acid (AA), dopamine (DA) and acetaminophen (AC). The oxidation over-potentials of AA, DA and AC decreased dramatically, and their oxidation peak currents increased significantly at Au/ZnO/N-doped graphene/GCE compared to those obtained at the N-doped graphene/GCE and bare CCE. The peak separations between AA and DA, DA and AC, and AC and AA are large up to 195, 198 and 393mV, respectively. The calibration curves for AA, DA and AC were obtained in the range of 30.00-13.00×10(3), 2.00-0.18×10(3) and 5.00-3.10×10(3)μM, respectively. The detection limits (S/N=3) were 5.00, 0.40 and 0.80μM for AA, DA and AC, respectively. Copyright © 2016 Elsevier B.V. All rights reserved.

Gold nanoparticle aerosols for rodent inhalation and translocation studies

NASA Astrophysics Data System (ADS)

Möller, Winfried; Gibson, Neil; Geiser, Marianne; Pokhrel, Suman; Wenk, Alexander; Takenaka, Shinji; Schmid, Otmar; Bulgheroni, Antonio; Simonelli, Federica; Kozempel, Jan; Holzwarth, Uwe; Wigge, Christoph; Eigeldinger-Berthou, Sylvie; Mädler, Lutz; Kreyling, Wolfgang G.

2013-04-01

The intensive use of nano-sized particles in many different applications necessitates studies on their risk assessment as there are still open questions on their safe handling and utilization. For reliable risk assessment, the interaction of nanoparticles (NP) with biological systems after various routes of exposure needs to be investigated using well-characterized NP. We report here on the generation of gold-NP (Au-NP) aerosols for inhalation studies with the spark ignition technique, and their characterization in terms of chemical composition, physical structure, morphology, and specific surface area, and on interaction with lung tissues and lung cells after 1 h inhalation by mice. The originally generated agglomerated Au-NP were converted into compact spherical Au-NP by thermal annealing at 600 °C, providing particles of similar mass, but different size and specific surface area. Since there are currently no translocation data available on inhaled Au-NP in the 10-50 nm diameter range, the emphasis was to generate NP as small as 20 nm for inhalation in rodents. For anticipated in vivo systemic translocation and dosimetry analyses, radiolabeled Au-NP were created by proton irradiating the gold electrodes of the spark generator, thus forming gamma ray emitting 195Au with 186 days half-life, allowing long-term biokinetic studies. The dissolution rate of 195Au from the NP was below detection limits. The highly concentrated, polydisperse Au-NP aerosol (1-2 × 107 NP/cm3) proved to be constant over several hours in terms of its count median mobility diameter, its geometric standard deviation and number concentration. After collection on filters particles can be re-suspended and used for instillation or ingestion studies.

A New-Type of Long-Range Restructuring of Ordered Metal Surfaces Induced by Lateral Adsorbate Interactions: Iodide on AU(110) Electrodes

DTIC Science & Technology

1994-02-01

separated by monoatomic steps. The direction of the (110) gold rows is evident in the atomic- resolution image of a uniform terrace, shown in Fig. 2A...distinguish between the average surface energy of a gold atom within a (110) terrace and at a monoatomic step (edge) site. The difference between these...having (3 x 2) symmetry (coverage - 0.67), is imaged instead of the substrate, with the iodide arranged in parallel close-packed rows in between the gold

Preparation of Janus Particles and Alternating Current Electrokinetic Measurements with a Rapidly Fabricated Indium Tin Oxide Electrode Array.

PubMed

Chen, Yu-Liang; Jiang, Hong-Ren

2017-06-23

This article provides a simple method to prepare partially or fully coated metallic particles and to perform the rapid fabrication of electrode arrays, which can facilitate electrical experiments in microfluidic devices. Janus particles are asymmetric particles that contain two different surface properties on their two sides. To prepare Janus particles, a monolayer of silica particles is prepared by a drying process. Gold (Au) is deposited on one side of each particle using a sputtering device. The fully coated metallic particles are completed after the second coating process. To analyze the electrical surface properties of Janus particles, alternating current (AC) electrokinetic measurements, such as dielectrophoresis (DEP) and electrorotation (EROT)- which require specifically designed electrode arrays in the experimental device- are performed. However, traditional methods to fabricate electrode arrays, such as the photolithographic technique, require a series of complicated procedures. Here, we introduce a flexible method to fabricate a designed electrode array. An indium tin oxide (ITO) glass is patterned by a fiber laser marking machine (1,064 nm, 20 W, 90 to 120 ns pulse-width, and 20 to 80 kHz pulse repetition frequency) to create a four-phase electrode array. To generate the four-phase electric field, the electrodes are connected to a 2-channel function generator and to two invertors. The phase shift between the adjacent electrodes is set at either 90° (for EROT) or 180° (for DEP). Representative results of AC electrokinetic measurements with a four-phase ITO electrode array are presented.

Investigating Catalytic Properties of Composite Nanoparticle Assemblies

DTIC Science & Technology

2001-11-01

electrode surfaces, were found to be catalytically active towards electrooxidation of CO and MeOH upon activation. The activation involved partial removal...to proceed under stirring at room temperature for 4 hours. producing a dark-brown solution of DT-encapsulated nanoparticles that was then cleaned in... ethanol or used in the heating treatment. Processing. Highly-monodispersed Au particles (5.3 ±0.3 nm) were prepared by thermally activated treatment of

Au-modified three-dimensional In₂O₃ inverse opals: synthesis and improved performance for acetone sensing toward diagnosis of diabetes.

PubMed

Xing, Ruiqing; Li, Qingling; Xia, Lei; Song, Jian; Xu, Lin; Zhang, Jiahuan; Xie, Yi; Song, Hongwei

2015-08-14

Analyzing the volatile organic compounds (VOCs) in exhaled breath effectively is crucial to medical treatment, which can provide a fast and noninvasive way to diagnose disease. Well-designed materials with controlled structures have great influence on the sensing performance. In this work, the ordered three dimensional inverse opal (3DIO) macroporous In2O3 films with additional via-hole architectures were fabricated and different amounts of gold nanoparticles (Au NPs) were loaded on the In2O3 films aiming at enhancing their electrical responses. The gas sensing to acetone toward diabetes diagnosis in exhaled breath was performed with different Au/In2O3 electrodes. Representatively, the best 3DIO Au/In2O3 sensor can detect acetone effectively at 340 °C with response of 42.4 to 5 ppm, the actual detection limit is as low as 20 ppb, and it holds a dynamic response of 11 s and a good selectivity. Moreover, clinical tests proved that the as-prepared 3DIO Au/In2O3 IO sensor could distinguish acetone biomarkers in human breath clearly. The excellent gas sensing properties of the Au/In2O3 electrodes were attributed to the "spillover effects" between Au and In2O3 and the special 3DIO structure. This work indicates that 3DIO Au/In2O3 composite is a promising electrode material for actual application in the monitoring and detection of diabetes through exhaled breath.

Effect of gold nanoparticles on the structure and electron-transfer characteristics of glucose oxidase redox polyelectrolyte-surfactant complexes.

PubMed

Cortez, M Lorena; Marmisollé, Waldemar; Pallarola, Diego; Pietrasanta, Lía I; Murgida, Daniel H; Ceolín, Marcelo; Azzaroni, Omar; Battaglini, Fernando

2014-10-06

Efficient electrical communication between redox proteins and electrodes is a critical issue in the operation and development of amperometric biosensors. The present study explores the advantages of a nanostructured redox-active polyelectrolyte-surfactant complex containing [Os(bpy)2Clpy](2+) (bpy=2,2'-bipyridine, py= pyridine) as the redox centers and gold nanoparticles (AuNPs) as nanodomains for boosting the electron-transfer propagation throughout the assembled film in the presence of glucose oxidase (GOx). Film structure was characterized by grazing-incidence small-angle X-ray scattering (GISAXS) and atomic force microscopy (AFM), GOx incorporation was followed by surface plasmon resonance (SPR) and quartz-crystal microbalance with dissipation (QCM-D), whereas Raman spectroelectrochemistry and electrochemical studies confirmed the ability of the entrapped gold nanoparticles to enhance the electron-transfer processes between the enzyme and the electrode surface. Our results show that nanocomposite films exhibit five-fold increase in current response to glucose compared with analogous supramolecular AuNP-free films. The introduction of colloidal gold promotes drastic mesostructural changes in the film, which in turn leads to a rigid, amorphous interfacial architecture where nanoparticles, redox centers, and GOx remain in close proximity, thus improving the electron-transfer process. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Bi-enzyme synergetic catalysis to in situ generate coreactant of peroxydisulfate solution for ultrasensitive electrochemiluminescence immunoassay.

PubMed

Wang, Haijun; Yuan, Ruo; Chai, Yaqin; Niu, Huan; Cao, Yaling; Liu, Huijing

2012-01-01

A novel electrochemiluminescence (ECL) immunosensor for ultrasensitive detection of α-1-fetoprotein (AFP) was designed based on the in situ bi-enzymatic reaction to generate coreactant of peroxydisulfate for signal amplification. In this work, AuNPs were electrodeposited on the glassy carbon electrode (GCE) surface, which promoted the electron transfer. Then, L-cysteine and another layer of AuNPs were, respectively assembled onto the modified electrode surface, which formed the multilayer films for amplifying the ECL signal of peroxydisulfate and immobilizing antibody. At last, glucose oxidase (GOD) and horseradish peroxidase (HRP) were employed to block the nonspecific binding sites. When proper amounts of glucose were added in the detection solution, GOD catalyzed the oxidation of glucose to generate H(2)O(2), which could be further catalyzed by HRP to generate O(2) for the signal amplification. The linear range for AFP detection was 0.001-100 ng mL(-1), with a low detection limit of 3.3 × 10(-4) ng mL(-1). The novel strategy has the advantages of simplicity, sensitivity, good selectivity and reproducibility which might hold a new promise for highly sensitive bioassays applied in clinical detection. Crown Copyright © 2012. Published by Elsevier B.V. All rights reserved.

Monolayers and multilayers of conjugated polymers as nanosized electronic components.

PubMed

Zotti, Gianni; Vercelli, Barbara; Berlin, Anna

2008-09-01

Conjugated polymers (CPs) are interesting materials for preparing devices based on nanoscopic molecular architectures because they exhibit electrical, electronic, magnetic, and optical properties similar to those of metals or semiconductors while maintaining the flexibility and ease of processing of polymers. The production of well-defined mono- and multilayers of CPs on electrodes with nanometer-scale, one-dimensional resolution remains, however, an important challenge. In this Account, we describe the preparation and conductive properties of nanometer-sized CP molecular structures formed on electrode surfaces--namely, self-assembled monolayer (SAM), brush-type, and self-assembled multilayer CPs--and in combination with gold nanoparticles (AuNPs). We have electrochemically polymerized SAMs of carboxyalkyl-functionalized terthiophenes aligned either perpendicular or parallel to the electrode surface. Anodic coupling of various pyrrole- and thiophene-based monomers in solution with the oligothiophene-based SAMs produced brush-like films. Microcontact printing of these SAMs produced patterns that, after heterocoupling, exhibited large height enhancements, as measured using atomic force microscopy (AFM). We have employed layer-by-layer self-assembly of water-soluble polythiophene-based polyelectrolytes to form self-assembled multilayers. The combination of isostructural polycationic and polyanionic polythiophenes produced layers of chains aligned parallel to the substrate plane. These stable, robust, and dense layers formed with high regularity on the preformed monolayers, with minimal interchain penetration. Infrared reflection/adsorption spectroscopy and X-ray diffraction analyses revealed unprecedented degrees of order. Deposition of soluble polypyrroles produced molecular layers that, when analyzed using a gold-coated AFM tip, formed gold-polymer-gold junctions that were either ohmic or rectifying, depending of the layer sequence. We also describe the electronic conduction of model alpha,omega-capped sexithiophenes featuring a range of electron donor/acceptor units and lengths of additional conjugation. The sexithiophene cores exhibit redox-type conductivity, developing at the neutral/cation and cation/dication levels with values depending the nature of the substitution and the redox system. Extending the conjugation beyond the sexithiophene frame introduces further oxidation processes displaying enhanced conductivity. Finally, we discuss the ability of CP-based monolayers to coordinate AuNPs. Although thiophene- and pyrrole-based oligomers aggregate toluene-soluble AuNPs, alkyl substitution inhibits the aggregation process through steric restraint. Consequently, we investigated the interactions between AuNPs and polypyrrole or polythiophene monolayers, including those formed from star-shaped molecules. The hindered aggregation provided by alkyl substituents allowed us to adsorb thiol-functionalized oligothiophenes and oligopyrroles directly onto preformed AuNPs. Novel materials incorporating AuNPs of the same size but bearing different conjugated ends or bridges have great promise for applications in electrocatalysis, electroanalysis, and organic electronics.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yoon, Yeung-Pil; Kim, Jae-Hong; Ahn, Kwang-Soon, E-mail: kstheory@ynu.ac.kr

Au was electrodeposited potentiostatically at 0.3 V for 5 min on nanoporous Pt nanoparticle-coated F-doped SnO{sub 2} (FTO/Pt) substrates. For comparison, Au-electrodeposited FTO (FTO/Au) and Au-uncoated FTO/Pt were prepared. FTO/Au showed large-sized Au clusters dispersed sparsely over FTO, which resulted in lower electrocatalytic activity than FTO/Pt. In contrast, FTO/Pt exhibited poor stability unlike FTO/Au due to poisoning by the adsorption of sulfur species. The Au-electrodeposited FTO/Pt (FTO/Pt/Au) consisted of small Au clusters deposited over the entire area of Pt due to the effective Au nucleation provided by nanoporous metallic Pt. FTO/Pt/Au exhibited enhanced electrocatalytic activity and excellent stability because the small Aumore » particles well-dispersed over the nanoporous metallic Pt network provided numerous electrochemical reaction sites, and the Pt surface was not exposed to the electrolyte. When FTO/Pt/Au was used as the counter electrode (CE) of a quantum dot-sensitized solar cell, the significantly enhanced electrocatalytic activity of the FTO/Pt/Au CE facilitated the reduction reaction of S{sub n}{sup 2− }+ 2e{sup −} (CE) → S{sub n−1}{sup 2−} + S{sup 2−} at the CE/electrolyte interface, resulting in a significantly hindered recombination reaction, S{sub n}{sup 2− }+ 2e{sup −} (TiO{sub 2} in the photoanode) → S{sub n-1}{sup 2−} + S{sup 2−}, and significantly improved overall energy conversion efficiency.« less

Evaluation parameters for the alkaline fuel cell oxygen electrode

NASA Technical Reports Server (NTRS)

Singer, J.; Srinivasan, V.

1985-01-01

Studies were made of Pt- and Au-catalyzed porous electrodes, designed for the cathode of the alkaline H2/O2 fuel cell, employing cyclic voltammetry and the floating half-cell method. The purpose was to obtain parameters from the cyclic voltammograms which could predict performance in the fuel cell. It was found that a satisfactory relationship between these two types of measurement could not be established; however, useful observations were made of relative performance of several types of carbon used as supports for noble metal catalysts and of some Au catalysts. The best half-cell performance with H2/O2 in a 35 percent KOH electrolyte at 80 C was given by unsupported fine particle Au on Teflon; this electrode is used in the Orbiter fuel cell.

Space-confined fabrication of silver nanodendrites and their enhanced SERS activity.

PubMed

Wang, Shuqi; Xu, Li-Ping; Wen, Yongqiang; Du, Hongwu; Wang, Shutao; Zhang, Xueji

2013-05-21

Here we report a controllable method based on electrodeposition to fabricate Ag nanodendrites (NDs) on a microwell patterned electrode. The microwell patterns on the ITO electrode are fabricated via the microcontact printing technique. By varying the microwell size and electrodeposition time, the morphology of metal deposits on the microwell patterned ITO electrode can be tuned from boulders to dendrites. At the edge of the microwells, the current density was strengthened, which incurs rapid nucleation. The nucleus develops into dendrites because of Mullins-Sekerka instability. However, only boulders were observed at the center of microwells. By reducing the size of the microwells, only NDs were fabricated due to the edge effect. On the basis of understanding the underlying mechanism for dendritic growth in a confined space, our method is used for fabricating other noble metal (Au, Pt) nanodendrites. The controllable synthesis of Au and Pt NDs indicates the universality of this method. Compared with Ag film obtained from electron beam evaporation, the as-prepared Ag NDs exhibit highly enhanced surface-enhanced Raman scattering (SERS) sensitivity when they are used to detect rhodamine 6G (R6G). This approach provides a very controllable, reliable and general way for space-confined fabricating the noble metal nanodendrite arrays which show great promise in catalysis, sensing, biomedicine, electronic and magnetic devices.

Electrochemical Sensing toward Trace As(III) Based on Mesoporous MnFe₂O₄/Au Hybrid Nanospheres Modified Glass Carbon Electrode.

PubMed

Zhou, Shaofeng; Han, Xiaojuan; Fan, Honglei; Liu, Yaqing

2016-06-22

Au nanoparticles decorated mesoporous MnFe₂O₄ nanocrystal clusters (MnFe₂O₄/Au hybrid nanospheres) were used for the electrochemical sensing of As(III) by square wave anodic stripping voltammetry (SWASV). Modified on a cheap glass carbon electrode, these MnFe₂O₄/Au hybrid nanospheres show favorable sensitivity (0.315 μA/ppb) and limit of detection (LOD) (3.37 ppb) toward As(III) under the optimized conditions in 0.1 M NaAc-HAc (pH 5.0) by depositing for 150 s at the deposition potential of -0.9 V. No obvious interference from Cd(II) and Hg(II) was recognized during the detection of As(III). Additionally, the developed electrode displayed good reproducibility, stability, and repeatability, and offered potential practical applicability for electrochemical detection of As(III) in real water samples. The present work provides a potential method for the design of new and cheap sensors in the application of electrochemical determination toward trace As(III) and other toxic metal ions.

Evaluation of MOSFET-type glucose sensor using platinum electrode with glucose oxidase

NASA Astrophysics Data System (ADS)

Ooe, Katsutoshi; Hamamoto, Yasutaro; Hirano, Yoshiaki

2005-02-01

As the population ages, health management will be one of the important issues. The development of a safe medical machine based on MEMS technologies for the human body will be the primary research project in the future. We have developed the glucose sensor, as one of the medical based devices, for use in the Health Monitoring System (HMS). HMS is the device that continuously monitors human health conditions. For example, blood is the monitoring target of HMS. The glucose sensor specifically detects the glucose levels of the blood and monitors the glucose concentration as the blood sugar level. This glucose sensor has a "separated Au electrode", which immobilizes GOx. In our previous work, GOx was immobilized onto Au electrode by the SAMs (Self-Assembled Monolayer) method, and the sensor, using this working electrode, detected the glucose concentration of an aqueous glucose solution. In this report, we used a Pt electrode, which immobilized GOx, as a working electrode. Au electrode, which was used previously, was dissolved by the application of current in the presence of chloride ions. Based on the above-mentioned fact, a new working electrode, which immobilized GOx, was produced using Pt, which did not possess such characteristics. These Pt working electrodes were produced using the covalent binding method and the cross-link method, and both the electrodes displayed a good sensing property. In addition, the electrode using glutaraldehyde (GA) and bovine serum albumin (BSA) as crosslinking agents was produced, and it displayed better characteristics as compared with those displayed by the electrode that used only GA. Based on the above-mentioned techniques, the improvement in performance of the sensor was confirmed.

A sensitive label-free electrochemical immunosensor for detection of cytokeratin 19 fragment antigen 21-1 based on 3D graphene with gold nanopaticle modified electrode.

PubMed

Zeng, Yan; Bao, Jing; Zhao, Yanan; Huo, Danqun; Chen, Mei; Yang, Mei; Fa, Huanbao; Hou, Changjun

2018-02-01

Previous studies have confirmed that cytokeratin 19 fragment antigen 21-1 (CYFRA 21-1) serves as a powerful biomarker in non-small cell lung cancer (NSCLC). Herein, we report for the first time a label-free electrochemical immunosensor for sensitive and selective detection of tumor marker CYFRA21-1. In this work, three-dimensional graphene @ gold nanoparticles (3D-G@Au) nanocomposite was modified on the glassy carbon electrode (GCE) surface to enhance the conductivity of immunosensor. The anti-CYFRA21-1 captured and fixed on the modified GCE through the cross-linking of chitosan (CS), glutaraldehyde (GA) and anti-CYFRA21-1. The differential pulse voltammetry (DPV) peak current change due to the specific interaction between anti-CYFRA21-1 and CYFRA21-1 on the modified electrode surface was utilized to detect CYFRA21-1. Under optimized conditions, the proposed electrochemical immunosensor was employed to detect CYFRA21-1 and exhibited a wide linear range of 0.25-800ngmL -1 and low detection limit of 100pgmL -1 (S/N = 3). Moreover, the recovery rates of serum samples were in the range from 95.2% to 108.7% and the developed immunosensor also shows a good correlation (less than 6.6%) with enzyme-linked immunosorbent assay (ELISA) in the detection of clinical serum samples. Therefore, it is expected that the proposed immunosensor based on a 3D-G@Au has great potential in clinical medical diagnosis of CYFRA21-1. Copyright © 2017 Elsevier B.V. All rights reserved.

Three-dimensionally ordered macroporous (3DOM) gold-nanoparticle-doped titanium dioxide (GTD) photonic crystals modified electrodes for hydrogen peroxide biosensor.

PubMed

Li, Jianlin; Han, Tao; Wei, Nannan; Du, Jiangyan; Zhao, Xiangwei

2009-12-15

Gold nanoparticles have been introduced into the wall framework of titanium dioxide photonic crystals by the colloidal crystal template technique. The three-dimensionally ordered macroporous gold-nanoparticle-doped titanium dioxide (3DOM GTD) film was modified on the indium-tin oxide (ITO) electrode surface and used for the hydrogen peroxide biosensor. The direct electron transfer and electrocatalysis of horseradish peroxidase (HRP) immobilized on this film have been investigated. The 3DOM GTD film could provide a good microenvironment for retaining the biological bioactivity, large internal area, and superior conductivity. The HRP/3DOM GTD/ITO electrode exhibited two couples of redox peaks corresponding to the HRP intercalated in the mesopores and adsorbed on the external surface of the film with the formal potential of -0.19 and -0.52V in 0.1M PBS (pH 7.4), respectively. The HRP intercalated in the mesopores showed a surface-controlled process with a single proton transfer. The direct electron transfer between the adsorbed HRP and the electrode is achieved without the aid of an electron mediator. The H(2)O(2) biosensor displayed a rapid eletrocatalytic response (less than 3s), a wide linear range from 0.5 microM to 1.4mM with a detection limit of 0.2 microM, high sensitivity (179.9 microAmM(-1)), good stability and reproducibility. Compared with the free-Au doped titanium dioxide photonic crystals modified electrode, the GTD modified electrode could greatly enhance the response current signal, linear detection range and higher sensitivity. The 3DOM GTD provided a new matrix for protein immobilization and direct transfer study and opened a way for low conductivity electrode biosensor.

Adsorption Behavior of TBPS in the Process of Cu Electrodeposition on an Au Film.

PubMed

Chen, Liang-Huei; Liu, Yung-Fang; Krug, Klaus; Lee, Yuh-Lang

2018-05-15

The adsorption behavior of an Cu electroplating additive, 3,3 thiobis-(1-propanesulfonic acid sodium salt) (TBPS) in a process of Cu deposition onto a single crystalline Au(111) surface is studied by an in-situ Surface-Enhanced Infrared Absorption Spectroscopy (SEIRAS). The SEIRAS spectra of the TBPS adlayer on a Cu film is investigated first and compared to that on an Au film. These results are utilized to evaluate the characteristics of TBPS adlayer on the electrode surface during the Cu deposition and stripping processes. The results show that the SEIRAS spectra of TBPS adsorbed on the Cu film resembles closely to that on the Au film, and the most pronounced peaks are symmetric S-O (ss-SO) and asymmetric S-O (as-SO) stretching modes. However, the as-SO band is sharper with a higher intensity on the Cu film. Since the ss-SO and as-SO peaks correspond to the molecular with upright and lie-down orientations, respectively, it implies that the TBPS molecules have higher ratio of lie-down orientation on the Cu film. In the Cu electrodeposition process, the cyclic voltammetry (CV) result shows that the presence of the TBPS in the HClO 4 solution can decrease the inhibition effect of HClO 4 to the Cu deposition. For the spectra measured at various potential during cathodic and anodic sweeping, an obvious change of the spectra occurs at ca. 0.6 V, the initiation of Cu underpotential deposition (Cu-UPD). For potentials higher and lower than 0.6 V, the spectra are similar, respectively, to those measured for the Au and Cu films. This result indicates that the TBPS molecules originally adsorbing on the Au film transfer to the surface of deposited Cu layer. This inference is also confirmed by the variation in wavenumber and peak intensity of ss-SO and as-SO peaks during the potential sweeping.

Sensitivity enhancement of capacitive tumor necrosis factor-α detection by deposition of nanoparticles on interdigitated electrode

NASA Astrophysics Data System (ADS)

Yagati, Ajay Kumar; Park, Jinsoo; Kim, Jungsuk; Ju, Heongkyu; Chang, Keun-A.; Cho, Sungbo

2016-06-01

An interdigitated electrodes (IDE) modified with gold nanoparticles (AuNPs) was fabricated to enhance the capacitive detection of tumor necrosis factor-α (TNF-α) and compared with a bare IDE. A TNF-α immunosensor was developed by covalently conjugating TNF-α antibodies with 3-mercaptopropionic acid by a carbodiimide/N-hydroxysuccinimide reaction on the AuNP/IDE. After the application of human serum samples containing various concentrations of TNF-α to the sensing electrode, changes in both the impedance spectrum and the electrode interfacial capacitance were measured. The capacitance changes were dependent on the TNF-α concentration in the range of 1 pg ml-1 to 10 ng ml-1, and the device had the calculated detection limit of 0.83 pg ml-1. The developed AuNP/IDE-based immunosensor was successfully used for the capacitive detection of the binding of TNF-α to its antibody, and was found to be feasible for the analysis of TNF-α in human blood serum.

Enhanced output-performance of piezoelectric poly(vinylidene fluoride trifluoroethylene) fibers-based nanogenerator with interdigital electrodes and well-ordered cylindrical cavities

NASA Astrophysics Data System (ADS)

Gui, Jinzheng; Zhu, Yezi; Zhang, Lingling; Shu, Xi; Liu, Wei; Guo, Shishang; Zhao, Xingzhong

2018-02-01

A piezoelectric nanogenerator based on poly(vinylidene fluoride trifluoroethylene) [P(VDF-TrFE)] nanofibers with an Au interdigital electrode (IDT)/P(VDF-TrFE) nanofiber film/well-ordered cylindrical cavity structure was prepared by combining Au IDTs with a rotary collector to obtain highly aligned P(VDF-TrFE) nanofiber arrays. The Au IDTs work not only as parallel electrodes to collect P(VDF-TrFE) nanofibers during electrospinning but also as charge-collecting electrodes in the nanogenerator. The well-ordered cylindrical cavities improve output performance by enhancing the deformation of P(VDF-TrFE) nanofiber films when subjected to external force. The nanogenerator performs well; as an example of application, we demonstrate energy harvesting from human walking, with a peak output voltage of 5 V and a peak short-circuit current of 1.2 μA. Such a device could have practical applications in wearable, self-powered devices.

Metallization of ultra-thin, non-thiol SAMs with flat-lying molecular units: Pd on 1, 4-dicyanobenzene.

PubMed

Eberle, Felix; Metzler, Martin; Kolb, Dieter M; Saitner, Marc; Wagner, Patrick; Boyen, Hans-Gerd

2010-09-10

Self-assembled monolayers of 1,4-dicyanobenzene on Au(111) electrodes are studied by cyclic voltammetry, in-situ STM and ex-situ XPS. High-resolution STM images reveal a long-range order of propeller-like assemblies each of which consists of three molecules, all lying flat on the gold substrate with the cyano groups oriented parallel to the metal surface. It is demonstrated that both functional groups can act as complexation sites for metal ions from solution. Surprisingly, such arrangements still allow the metal to be deposited on top of the molecules by electrochemical reduction despite the close vicinity to the Au surface. The latter is demonstrated by angle-resolved XPS which unequivocally shows that the metal indeed resides on top of the organic layer rather than underneath, despite the flat arrangement of the molecules.

Excessive Counterion Condensation on Immobilized ssDNA in Solutions of High Ionic Strength

PubMed Central

Rant, Ulrich; Arinaga, Kenji; Fujiwara, Tsuyoshi; Fujita, Shozo; Tornow, Marc; Yokoyama, Naoki; Abstreiter, Gerhard

2003-01-01

We present experiments on the bias-induced release of immobilized, single-stranded (ss) 24-mer oligonucleotides from Au-surfaces into electrolyte solutions of varying ionic strength. Desorption is evidenced by fluorescence measurements of dye-labeled ssDNA. Electrostatic interactions between adsorbed ssDNA and the Au-surface are investigated with respect to 1), a variation of the bias potential applied to the Au-electrode; and 2), the screening effect of the electrolyte solution. For the latter, the concentration of monovalent salt in solution is varied from 3 to 1600 mM. We find that the strength of electric interaction is predominantly determined by the effective charge of the ssDNA itself and that the release of DNA mainly occurs before the electrochemical double layer has been established at the electrolyte/Au interface. In agreement with Manning's condensation theory, the measured desorption efficiency (ηrel) stays constant over a wide range of salt concentrations; however, as the Debye length is reduced below a value comparable to the axial charge spacing of the DNA, ηrel decreases substantially. We assign this effect to excessive counterion condensation on the DNA in solutions of high ionic strength. In addition, the relative translational diffusion coefficient of ssDNA in solution is evaluated for different salt concentrations. PMID:14645075

Excessive counterion condensation on immobilized ssDNA in solutions of high ionic strength.

PubMed

Rant, Ulrich; Arinaga, Kenji; Fujiwara, Tsuyoshi; Fujita, Shozo; Tornow, Marc; Yokoyama, Naoki; Abstreiter, Gerhard

2003-12-01

We present experiments on the bias-induced release of immobilized, single-stranded (ss) 24-mer oligonucleotides from Au-surfaces into electrolyte solutions of varying ionic strength. Desorption is evidenced by fluorescence measurements of dye-labeled ssDNA. Electrostatic interactions between adsorbed ssDNA and the Au-surface are investigated with respect to 1), a variation of the bias potential applied to the Au-electrode; and 2), the screening effect of the electrolyte solution. For the latter, the concentration of monovalent salt in solution is varied from 3 to 1600 mM. We find that the strength of electric interaction is predominantly determined by the effective charge of the ssDNA itself and that the release of DNA mainly occurs before the electrochemical double layer has been established at the electrolyte/Au interface. In agreement with Manning's condensation theory, the measured desorption efficiency (etarel) stays constant over a wide range of salt concentrations; however, as the Debye length is reduced below a value comparable to the axial charge spacing of the DNA, etarel decreases substantially. We assign this effect to excessive counterion condensation on the DNA in solutions of high ionic strength. In addition, the relative translational diffusion coefficient of ssDNA in solution is evaluated for different salt concentrations.

Broadband light absorption enhancement in dye-sensitized solar cells with Au-Ag alloy popcorn nanoparticles

NASA Astrophysics Data System (ADS)

Xu, Qi; Liu, Fang; Liu, Yuxiang; Cui, Kaiyu; Feng, Xue; Zhang, Wei; Huang, Yidong

2013-07-01

In this paper, we present an investigation on the use of Au-Ag alloy popcorn-shaped nanoparticles (NPs) to realise the broadband optical absorption enhancement of dye-sensitized solar cells (DSCs). Both simulation and experimental results indicate that compared with regular plasmonic NPs, such as nano-spheres, irregular popcorn-shaped alloy NPs exhibit absorption enhancement over a broad wavelength range due to the excitation of localized surface plasmons (LSPs) at different wavelengths. The power conversion efficiency (PCE) of DSCs is enhanced by 16% from 5.26% to 6.09% by incorporating 2.38 wt% Au-Ag alloy popcorn NPs. Moreover, by adding a scattering layer on the exterior of the counter electrode, the popcorn NPs demonstrate an even stronger ability to increase the PCE by 32% from 5.94% to 7.85%, which results from the more efficient excitation of the LSP mode on the popcorn NPs.

Broadband light absorption enhancement in dye-sensitized solar cells with Au-Ag alloy popcorn nanoparticles.

PubMed

Xu, Qi; Liu, Fang; Liu, Yuxiang; Cui, Kaiyu; Feng, Xue; Zhang, Wei; Huang, Yidong

2013-01-01

In this paper, we present an investigation on the use of Au-Ag alloy popcorn-shaped nanoparticles (NPs) to realise the broadband optical absorption enhancement of dye-sensitized solar cells (DSCs). Both simulation and experimental results indicate that compared with regular plasmonic NPs, such as nano-spheres, irregular popcorn-shaped alloy NPs exhibit absorption enhancement over a broad wavelength range due to the excitation of localized surface plasmons (LSPs) at different wavelengths. The power conversion efficiency (PCE) of DSCs is enhanced by 16% from 5.26% to 6.09% by incorporating 2.38 wt% Au-Ag alloy popcorn NPs. Moreover, by adding a scattering layer on the exterior of the counter electrode, the popcorn NPs demonstrate an even stronger ability to increase the PCE by 32% from 5.94% to 7.85%, which results from the more efficient excitation of the LSP mode on the popcorn NPs.

Broadband light absorption enhancement in dye-sensitized solar cells with Au-Ag alloy popcorn nanoparticles

PubMed Central

Xu, Qi; Liu, Fang; Liu, Yuxiang; Cui, Kaiyu; Feng, Xue; Zhang, Wei; Huang, Yidong

2013-01-01

In this paper, we present an investigation on the use of Au-Ag alloy popcorn-shaped nanoparticles (NPs) to realise the broadband optical absorption enhancement of dye-sensitized solar cells (DSCs). Both simulation and experimental results indicate that compared with regular plasmonic NPs, such as nano-spheres, irregular popcorn-shaped alloy NPs exhibit absorption enhancement over a broad wavelength range due to the excitation of localized surface plasmons (LSPs) at different wavelengths. The power conversion efficiency (PCE) of DSCs is enhanced by 16% from 5.26% to 6.09% by incorporating 2.38 wt% Au-Ag alloy popcorn NPs. Moreover, by adding a scattering layer on the exterior of the counter electrode, the popcorn NPs demonstrate an even stronger ability to increase the PCE by 32% from 5.94% to 7.85%, which results from the more efficient excitation of the LSP mode on the popcorn NPs. PMID:23817586

Atomic scale deposition of Pt around Au nanoparticles to achieve much enhanced electrocatalysis of Pt

DOE PAGES

Xi, Zheng; Lv, Haifeng; Erdosy, Daniel P.; ...

2017-05-07

Here, we report an electrochemical method to deposit atomic scale Pt on a 5 nm Au nanoparticle (NP) surface in N 2-saturated 0.5 M H 2SO 4. Furthermore, Pt is provided by the Pt wire counter electrode via one-step Pt wire oxidation, dissolution, and deposition realized by controlled electrochemical scanning. Scanning from 0.6–1.0 V (vs. RHE) for 10 000 cycles gives Au 98.2Pt 1.8, which serves as an excellent catalyst for the formic acid oxidation reaction, showing 41 times higher specific activity (20.19 mA cm -2) and 25 times higher mass activity (10.80 A mg Pt -1) with much bettermore » CO-tolerance and stability than commercial Pt. This work demonstrates a unique strategy to minimize the use of Pt as a catalyst for electrochemical reactions.« less

Atomic scale deposition of Pt around Au nanoparticles to achieve much enhanced electrocatalysis of Pt

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xi, Zheng; Lv, Haifeng; Erdosy, Daniel P.

Here, we report an electrochemical method to deposit atomic scale Pt on a 5 nm Au nanoparticle (NP) surface in N 2-saturated 0.5 M H 2SO 4. Furthermore, Pt is provided by the Pt wire counter electrode via one-step Pt wire oxidation, dissolution, and deposition realized by controlled electrochemical scanning. Scanning from 0.6–1.0 V (vs. RHE) for 10 000 cycles gives Au 98.2Pt 1.8, which serves as an excellent catalyst for the formic acid oxidation reaction, showing 41 times higher specific activity (20.19 mA cm -2) and 25 times higher mass activity (10.80 A mg Pt -1) with much bettermore » CO-tolerance and stability than commercial Pt. This work demonstrates a unique strategy to minimize the use of Pt as a catalyst for electrochemical reactions.« less

PDMS based multielectrode arrays for superior in-vitro retinal stimulation and recording.

PubMed

Biswas, Satarupa; Sikdar, Debdeep; Das, Debanjan; Mahadevappa, Manjunatha; Das, Soumen

2017-08-25

Understanding of the neural response to electrical stimulation requires simultaneous recording from the various neurons of retina. Electrodes form the physical interface with the neural or retinal tissue. Successful retinal stimulation and recording demands conformal integration of these electrodes with the soft tissue to ensure establishment of proper electrical connection with the excitable tissue. Mechanical impedance of polydimethylsiloxane (PDMS) being compliant with that of retinal tissue, offers excellent potential as a substrate for metal electrodes. In this paper, Cr/Au micro electrodes with 200 μm diameter were fabricated on rigid and flexible PDMS substrates under crack free condition. Spontaneous buckling of thin films over PDMS substrates improved electrode performance circumventing the fabrication issues faced over a buckled surface. Individual electrodes from the multielectrode arrays (MEAs) were examined with electrochemical impedance spectroscopy and cyclic voltammetry. Controlled fabrication process as described here generates buckles in the metal films leading to increased electrode surface area that increases the charge storage capacity and decreases the interface impedance of the metal electrodes. At 1 kHz, impedance was reduced from 490 ± 27 kΩ to 246 ± 19 kΩ and charge storage capacity was increased from 0.40 ± 0.87 mC/cm 2 to 2.1 ± 0.87 mC/cm 2 . Neural spikes recorded with PDMS based electrodes from isolated retina also contained less noise as indicated by signal to noise ratio analysis. The present study established that the use of PDMS as a substrate for MEAs can enhance the performance of any thin film metal electrodes without incorporation of any coating layers or nanomaterials.

A cost-effective nanoporous ultrathin film electrode based on nanoporous gold/IrO2 composite for proton exchange membrane water electrolysis

NASA Astrophysics Data System (ADS)

Zeng, Yachao; Guo, Xiaoqian; Shao, Zhigang; Yu, Hongmei; Song, Wei; Wang, Zhiqiang; Zhang, Hongjie; Yi, Baolian

2017-02-01

A cost-effective nanoporous ultrathin film (NPUF) electrode based on nanoporous gold (NPG)/IrO2 composite has been constructed for proton exchange membrane (PEM) water electrolysis. The electrode was fabricated by integrating IrO2 nanoparticles into NPG through a facile dealloying and thermal decomposition method. The NPUF electrode is featured in its 3D interconnected nanoporosity and ultrathin thickness. The nanoporous ultrathin architecture is binder-free and beneficial for improving electrochemical active surface area, enhancing mass transport and facilitating releasing of oxygen produced during water electrolysis. Serving as anode, a single cell performance of 1.728 V (@ 2 A cm-2) has been achieved by NPUF electrode with a loading of IrO2 and Au at 86.43 and 100.0 μg cm-2 respectively, the electrolysis voltage is 58 mV lower than that of conventional electrode with an Ir loading an order of magnitude higher. The electrolysis voltage kept relatively constant up to 300 h (@250 mA cm-2) during the course of durability test, manifesting that NPUF electrode is promising for gas evolution.

Electron transport in doped fullerene molecular junctions

NASA Astrophysics Data System (ADS)

Kaur, Milanpreet; Sawhney, Ravinder Singh; Engles, Derick

The effect of doping on the electron transport of molecular junctions is analyzed in this paper. The doped fullerene molecules are stringed to two semi-infinite gold electrodes and analyzed at equilibrium and nonequilibrium conditions of these device configurations. The contemplation is done using nonequilibrium Green’s function (NEGF)-density functional theory (DFT) to evaluate its density of states (DOS), transmission coefficient, molecular orbitals, electron density, charge transfer, current, and conductance. We conclude from the elucidated results that Au-C16Li4-Au and Au-C16Ne4-Au devices behave as an ordinary p-n junction diode and a Zener diode, respectively. Moreover, these doped fullerene molecules do not lose their metallic nature when sandwiched between the pair of gold electrodes.

Electrochemical Recovery of Gold from Waste Electric and Electronic Equipment Using Circulating Particulate Bed Reactor (CPBE)

NASA Astrophysics Data System (ADS)

Ravinder, T.; Ali, U. F. M.; Ridwan, F. M.; Ibrahim, N.; Azmi, N. H.

2017-06-01

The utilization of electrochemical process recovery involving low reactant concentrations of metal requires electrodes with high mass transport rates and specific surface areas. This is essential to increase cross-sectional current densities whilst optimizing the capital and operating costs. Experimental results demonstrated that Circulating Particulate Bed Reactor (CPBE) is suitable for the recovery of low concentrations of gold from aqueous chloride solution containing {{AuCl}}4- and {{AuCl}}2- of less than 0.5 mol m-3(< 102 g m-3). Elemental gold was successfully obtained on 0.5-1 mm gr particles in an electrochemical reactor incorporating a cation- permeable membrane and operated in bath recycle mode. Depletion to concentration < 5 × 10-3 mol m-3 (< 1 g m-3) appeared to be mass transport controlled at an applied potential of +0.20 V (SCE), specific electrical energy consumption (SEEC) of ca. 800-1300 kWh h (tonne Au)-1 for cell voltages (U) of 2.0-3.0 V, and fractional current efficiencies of ca. 0.95. However, atomic absorption and UV spectrophotometry established that as the ([{{AuCl}}4-+[{{AuCl}}2-]) concentration decayed, the [{{AuCl}}4-]:[{{AuCl}}2-] molar ratio changed. A multi-step mechanism for reduction of {{AuCl}}4- ions explained this behavior in terms of changing overpotentials for {{AuCl}}4- and {{AuCl}}2- reduction as total dissolved gold concentration decreased. In addition, SEM images confirmed that adherent and coherent Au deposits were achieved with CPBE for Au deposition under mass transport control at 0.20 V (SCE).

Double layer effects in electrocatalysis: The oxygen reduction reaction and ethanol oxidation reaction on Au(111), Pt(111) and Ir(111) in alkaline media containing Na and Li cations

DOE PAGES

Lopes, Pietro P.; Strmcnik, Dusan; Jirkovsky, Jakub S.; ...

2015-09-28

Oxygen reduction and ethanol oxidation reactions were studied on Au(111), Pt(111) and Ir(111) in alkaline solutions containing sodium and/or lithium cations. By keeping the same (111) surface orientation and exploring oxophilicity trends and non-covalent interactions between OH ad and alkali metal cations (AMC n+), we were able to gain deep insights into the multiple roles that OH ad plays in these important electrocatalytic reactions. Cyclic voltammetry experiments revealed that OH ad formation initiates at distinct electrode potentials, governed by the oxophilicity of the specific metal surface, with further OH ad adlayer stabilization by non-covalent alkali-cation interactions and affecting the formationmore » of a “true oxide” layer at higher electrode potentials. Although OH ad is a simple spectator for the ORR, it promotes the ethanol oxidation reaction (EOR) at lower potentials and act as spectator at high OHad coverages. By changing the alkali metal cation at the interface (Li +) on more oxophilic surfaces, it was possible to promote the EOR even more, relative to Na +, without changing the product distribution for the reaction. This cation effect suggests that OH ad—Li +(H 2O) x clusters can stabilize the ethoxide adlayer, thus improving the EOR activity. Finally, our results indicate the importance of the entire electrochemical interface in determining the electrocatalytic activity during reaction.« less

Highly Oxidizing Surface Radicals in Lunar Dust

NASA Astrophysics Data System (ADS)

Kulahci, I.; Freund, F. T.; Bose, M.; Loftus, D. J.

2007-12-01

Lunar rocks are generally believed to be very "dry" with little or no evidence for hydroxyl as indicators of traces of dissolved H2O. The absence of hydroxyl, however, is not a sure sign of the absence of dissolved H2O. The reason is that hydroxyl pairs in the structure of host minerals, O3X-OH HO-XO3, with X=Si4+, Al3+ etc., tend to undergo an electronic rearrangement (redox conversion) in the course of which two oxygen anions are oxidized from the 2- to the 1- valence, forming a peroxy link, O3X-OO-XO3, plus an H2 molecule. If the H2 molecules diffuse out (which they are expected to do from lunar rocks and lunar fines over the course of 4 Gyrs), the peroxy links remain as the only "memory" of a former solute H2O content. Hard UV causes peroxy links to dissociate. In the process an electron from a neighboring O2- jumps into the broken peroxy bond. This is equivalent to forming an O-, e.g. a defect electron in the oxygen anion sublattice. Such defect electrons, also known as positive holes or pholes for short, represent highly mobile charge carriers. When trapped at the surface of dust grains, these charge carriers turn into highly reactive, highly oxidizing O- radicals, which are of concern because of their toxicity when lunar dust is inhaled by astronauts. We propose a device to measure the UV-activation of peroxy links by dusting lunar fines onto a polyethylene base plate with Au electrodes sputtered onto both ends and an ammeter connecting the two electrodes. One end of the dust layer will be exposed to the ambient UV radiation, while the remainder will be shaded. During the lunar night no current is expected to flow between the two Au electrodes. During passage through the night-day terminator, a current is expected to flow between the Au electrodes carried by defect electrons activated in the irradiated portion of the dust layer. Such a current would be an indicator that lunar fines and, by implication, lunar rocks contain peroxy links as a memory of a former solute H2O content.

Shell-isolated nanoparticle-enhanced Raman spectroscopy: principle and applications (Presentation Recording)

NASA Astrophysics Data System (ADS)

Li, Jian-Feng; Tian, Zhong-Qun

2015-08-01

Surface-enhanced Raman spectroscopy (SERS) is a powerful technique that yields fingerprint vibrational information with ultra-high sensitivity. However, only roughened Ag, Au and Cu surfaces can generate strong SERS effect. The lack of materials and morphology generality has severely limited the breadth of SERS practical applications on surface science, electrochemistry and catalysis. Shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) was therefore invented to break the long-standing limitation of SERS. In SHINERS, Au@SiO2 core-shell nanoparticles were rationally designed. The gold core acts as plasmonic antenna and encapsulated by an ultra-thin, uniform and pinhole-free silica shell, can provide high electromagnetic field to enhance the Raman signals of probed molecules. The inert silica shell acts as tunneling barrier prevents the core from interacting with the environment. SHINERS has already been applied to a number of challenging systems, such as hydrogen and CO on Pt(hkl) and Rh(hkl), which can't be realized by traditional SERS. Combining with electrochemical methods, we has investigated the adsorption processes of pyridine at the Au(hkl) single crystal/solution interface, and in-situ monitored the surface electro-oxidation at Au(hkl) electrodes. These pioneering studies demonstrate convincingly the ability of SHINERS in exploring correlations between structure and reactivity as well as in monitoring intermediates at the interfaces. SHINERS was also explored from semiconductor surface for industry, to living bacteria for life science, and to pesticide residue detection for food safety. The concept of shell-isolated nanoparticle-enhancement is being applied to other spectroscopies such as infrared absorption, sum frequency generation and fluorescence. Jian-Feng Li et al., Nature, 2010, 464, 392-395.

Aptamer-based assay for monitoring genetic disorder phenylketonuria (PKU).

PubMed

Hasanzadeh, Mohammad; Zargami, Amir; Baghban, Hossein Navay; Mokhtarzadeh, Ahad; Shadjou, Nasrin; Mahboob, Soltanali

2018-05-16

The genetic disorder phenylketonuria (PKU) is the inability to metabolize phenylalanine because of a lack of the enzyme phenylalanine hydroxylase. Phenylalanine is used to biochemically form proteins, coded for by DNA. The development of an apta-assay for detection of l-Phenylalanine is presented in this work. A highly specific DNA-aptamer, selected to l-Phenylalanine was immobilized onto a gold nanostructure and electrochemical measurements were performed in a solution containing the phosphate buffer solution with physiological pH. We have constructed an aptamer immobilized gold nanostructure mediated, ultrasensitive electrochemical biosensor (Apt/AuNSs/Au electrode) for l-Phenylalanine detection without any additional signal amplification strategy. The aptamer assemble onto the AuNSs makes Apt/AuNSs/Au electrode an excellent platform for the l-Phenylalanine detection in physiological like condition. Differential pulse voltammetry were used for the quantitative l-Phenylalanine detection. The Apt/AuNSs/Au electrode offers an ultrasensitive and selective detection of l-Phenylalanine down to 0.23 μM level with a wide dynamic range from 0.72 μM-6 mM. The aptasensor exhibited excellent selectivity and stability. The real sample analysis was performed by spiking the unprocessed human serum samples with various concentration of l-Phenylalanine and obtained recovery within 2% error value. The sensor is found to be more sensitive than most of the literature reports. The simple and easy way of construction of this apta-assay provides an efficient and promising diagnosis of phenylketonuria. Copyright © 2018. Published by Elsevier B.V.

Ammonia gas sensors based on chemically reduced graphene oxide sheets self-assembled on Au electrodes

PubMed Central

2014-01-01

We present a useful ammonia gas sensor based on chemically reduced graphene oxide (rGO) sheets by self-assembly technique to create conductive networks between parallel Au electrodes. Negative graphene oxide (GO) sheets with large sizes (>10 μm) can be easily electrostatically attracted onto positive Au electrodes modified with cysteamine hydrochloride in aqueous solution. The assembled GO sheets on Au electrodes can be directly reduced into rGO sheets by hydrazine or pyrrole vapor and consequently provide the sensing devices based on self-assembled rGO sheets. Preliminary results, which have been presented on the detection of ammonia (NH3) gas using this facile and scalable fabrication method for practical devices, suggest that pyrrole-vapor-reduced rGO exhibits much better (more than 2.7 times with the concentration of NH3 at 50 ppm) response to NH3 than that of rGO reduced from hydrazine vapor. Furthermore, this novel gas sensor based on rGO reduced from pyrrole shows excellent responsive repeatability to NH3. Overall, the facile electrostatic self-assembly technique in aqueous solution facilitates device fabrication, the resultant self-assembled rGO-based sensing devices, with miniature, low-cost portable characteristics and outstanding sensing performances, which can ensure potential application in gas sensing fields. PMID:24917701

Zinc Oxide-Based Schottky Diode Prepared Using Radio-Frequency Magnetron Cosputtering System

NASA Astrophysics Data System (ADS)

Lai, Bo-Ting; Lee, Ching-Ting; Hong, Jhen-Dong; Yao, Shiau-Lu; Liu, Day-Shan

2010-08-01

The rectifying property of a zinc oxide (ZnO)-based Schottky diode prepared using a radio-frequency (rf) magnetron cosputtering system was improved by enhancing the cosputtered ZnO crystal quality, thereby optimizing the ohmic contact resistance and compensating the Schottky contact surface states. An undoped ZnO layer with a high c-axis orientation and a low internal residual stress was achieved using a postannealing treatment. A homogeneous n-type ZnO-indium tin oxide (ITO) cosputtered film was deposited onto the undoped ZnO layer to optimize the ohmic contact behavior to the Al electrode. The Schottky contact surface of the undoped ZnO layer to the Ni/Au electrode was passivated using an oxygen plasma treatment. Owing to the compensation of the native oxygen vacancies (VO) on the undoped ZnO surface, the leakage current markedly decreased and subsequently led to a quality Schottky diode performance with an ideality factor of 1.23 and a Schottky barrier height of 0.82 eV.

Wrinkled substrate and Indium Tin Oxide-free transparent electrode making organic solar cells thinner in active layer

NASA Astrophysics Data System (ADS)

Liu, Kong; Lu, Shudi; Yue, Shizhong; Ren, Kuankuan; Azam, Muhammad; Tan, Furui; Wang, Zhijie; Qu, Shengchun; Wang, Zhanguo

2016-11-01

To enable organic solar cells with a competent charge transport efficiency, reducing the thickness of active layer without sacrificing light absorption efficiency turns out to be of high feasibility. Herein, organic solar cells on wrinkled metal surface are designed. The purposely wrinkled Al/Au film with a smooth surface provides a unique scaffold for constructing thin organic photovoltaic devices by avoiding pinholes and defects around sharp edges in conventional nanostructures. The corresponding surface light trapping effect enables the thin active layer (PTB7-Th:PC71BM) with a high absorption efficiency. With the innovative MoO3/Ag/ZnS film as the top transparent electrode, the resulting Indium Tin Oxide-free wrinkled devices show a power conversion efficiency as 7.57% (50 nm active layer), higher than the planner counterparts. Thus, this paper provides a new methodology to improve the performance of organic solar cells by balancing the mutual restraint factors to a high level.

Preparation of indium tin oxide contact to n-CdZnTe gamma-ray detector

NASA Astrophysics Data System (ADS)

Li, Leqi; Xu, Yadong; Zhang, Binbin; Wang, Aoqiu; Dong, Jiangpeng; Yu, Hui; Jie, Wanqi

2018-03-01

The nonmetal electrode material Indium Tin Oxide (ITO) has advantages of excellent conductivity, higher adhesion, and interface stability, showing potential to replace the metallic contacts for fabrication of CdZnTe (CZT) X/γ-ray detectors. In this work, high quality ITO electrodes for n-type CZT crystals were prepared by magnetron sputtering under a sputtering power of 75 W and a sputtering pressure of 0.6 Pa. A low dark current of ˜1 nA is achieved for the 5 × 5 × 2 mm3 ITO/CZT/ITO planar device under 100 V bias. The characteristics of Schottky contact are presented in the room temperature I-V curves, which are similar to those of the Au contact detectors. Based on the thermoelectric emission theory, the contact barrier and resistance of ITO electrodes are evaluated to be 0.902-0.939 eV and 0.87-3.56 × 108 Ω, respectively, which are consistent with the values of the Au electrodes. The ITO/CZT/ITO structure detector exhibits a superior energy resolution of 6.5% illuminated by the uncollimated 241Am @59.5 keV γ-ray source, which is comparable to the CZT detector with Au electrodes.

Excitation mechanism in the photoisomerization of a surface-bound azobenzene derivative: Role of the metallic substrate.

PubMed

Hagen, Sebastian; Kate, Peter; Leyssner, Felix; Nandi, Dhananjay; Wolf, Martin; Tegeder, Petra

2008-10-28

Two-photon photoemission spectroscopy is employed to elucidate the electronic structure and the excitation mechanism in the photoinduced isomerization of the molecular switch tetra-tert-butyl-azobenzene (TBA) adsorbed on Au(111). Our results demonstrate that the optical excitation and the mechanism of molecular switching at a metal surface is completely different compared to the corresponding process for the free molecule. In contrast to direct (intramolecular) excitation operative in the isomerization in the liquid phase, the conformational change in the surface-bound TBA is driven by a substrate-mediated charge transfer process. We find that photoexcitation above a threshold hnu approximately 2.2 eV leads to hole formation in the Au d-band followed by a hole transfer to the highest occupied molecular orbital of TBA. This transiently formed positive ion resonance subsequently results in a conformational change. The photon energy dependent photoisomerization cross section exhibit an unusual shape for a photochemical reaction of an adsorbate on a metal surface. It shows a thresholdlike behavior below hnu approximately 2.2 eV and above hnu approximately 4.4 eV. These thresholds correspond to the minimum energy required to create single or multiple hot holes in the Au d-bands, respectively. This study provides important new insights into the use of light to control the structure and function of molecular switches in direct contact with metal electrodes.

Excitation mechanism in the photoisomerization of a surface-bound azobenzene derivative: Role of the metallic substrate

NASA Astrophysics Data System (ADS)

Hagen, Sebastian; Kate, Peter; Leyssner, Felix; Nandi, Dhananjay; Wolf, Martin; Tegeder, Petra

2008-10-01

Two-photon photoemission spectroscopy is employed to elucidate the electronic structure and the excitation mechanism in the photoinduced isomerization of the molecular switch tetra-tert-butyl-azobenzene (TBA) adsorbed on Au(111). Our results demonstrate that the optical excitation and the mechanism of molecular switching at a metal surface is completely different compared to the corresponding process for the free molecule. In contrast to direct (intramolecular) excitation operative in the isomerization in the liquid phase, the conformational change in the surface-bound TBA is driven by a substrate-mediated charge transfer process. We find that photoexcitation above a threshold hν ≈2.2 eV leads to hole formation in the Au d-band followed by a hole transfer to the highest occupied molecular orbital of TBA. This transiently formed positive ion resonance subsequently results in a conformational change. The photon energy dependent photoisomerization cross section exhibit an unusual shape for a photochemical reaction of an adsorbate on a metal surface. It shows a thresholdlike behavior below hν ≈2.2 eV and above hν ≈4.4 eV. These thresholds correspond to the minimum energy required to create single or multiple hot holes in the Au d-bands, respectively. This study provides important new insights into the use of light to control the structure and function of molecular switches in direct contact with metal electrodes.

Formation and Diffusion of Metal Impurities in Perovskite Solar Cell Material CH 3NH 3PbI 3 : Implications on Solar Cell Degradation and Choice of Electrode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ming, Wenmei; Yang, Dongwen; Li, Tianshu

Solar cells based on methylammonium lead triiodide (MAPbI 3) have shown remarkable progress in recent years and have demonstrated efficiencies greater than 20%. However, the long-term stability of MAPbI 3-based solar cells has yet to be achieved. Besides the well-known chemical and thermal instabilities, significant native ion migration in lead halide perovskites leads to current–voltage hysteresis and photoinduced phase segregation. Recently, it is further revealed that, despite having excellent chemical stability, the Au electrode can cause serious solar cell degradation due to Au diffusion into MAPbI 3. In addition to Au, many other metals have been used as electrodes inmore » MAPbI 3 solar cells. However, how the external metal impurities introduced by electrodes affect the long-term stability of MAPbI 3 solar cells has rarely been studied. A comprehensive study of formation energetics and diffusion dynamics of a number of noble and transition metal impurities (Au, Ag, Cu, Cr, Mo, W, Co, Ni, Pd) in MAPbI 3 based on first-principles calculations is reported herein. The results uncover important general trends of impurity formation and diffusion in MAPbI 3 and provide useful guidance for identifying the optimal metal electrodes that do not introduce electrically active impurity defects in MAPbI 3 while having low resistivities and suitable work functions for carrier extraction.« less

Formation and Diffusion of Metal Impurities in Perovskite Solar Cell Material CH3NH3PbI3: Implications on Solar Cell Degradation and Choice of Electrode.

PubMed

Ming, Wenmei; Yang, Dongwen; Li, Tianshu; Zhang, Lijun; Du, Mao-Hua

2018-02-01

Solar cells based on methylammonium lead triiodide (MAPbI 3 ) have shown remarkable progress in recent years and have demonstrated efficiencies greater than 20%. However, the long-term stability of MAPbI 3 -based solar cells has yet to be achieved. Besides the well-known chemical and thermal instabilities, significant native ion migration in lead halide perovskites leads to current-voltage hysteresis and photoinduced phase segregation. Recently, it is further revealed that, despite having excellent chemical stability, the Au electrode can cause serious solar cell degradation due to Au diffusion into MAPbI 3 . In addition to Au, many other metals have been used as electrodes in MAPbI 3 solar cells. However, how the external metal impurities introduced by electrodes affect the long-term stability of MAPbI 3 solar cells has rarely been studied. A comprehensive study of formation energetics and diffusion dynamics of a number of noble and transition metal impurities (Au, Ag, Cu, Cr, Mo, W, Co, Ni, Pd) in MAPbI 3 based on first-principles calculations is reported herein. The results uncover important general trends of impurity formation and diffusion in MAPbI 3 and provide useful guidance for identifying the optimal metal electrodes that do not introduce electrically active impurity defects in MAPbI 3 while having low resistivities and suitable work functions for carrier extraction.

Formation and Diffusion of Metal Impurities in Perovskite Solar Cell Material CH 3NH 3PbI 3 : Implications on Solar Cell Degradation and Choice of Electrode

DOE PAGES

Ming, Wenmei; Yang, Dongwen; Li, Tianshu; ...

2017-12-27

Solar cells based on methylammonium lead triiodide (MAPbI 3) have shown remarkable progress in recent years and have demonstrated efficiencies greater than 20%. However, the long-term stability of MAPbI 3-based solar cells has yet to be achieved. Besides the well-known chemical and thermal instabilities, significant native ion migration in lead halide perovskites leads to current–voltage hysteresis and photoinduced phase segregation. Recently, it is further revealed that, despite having excellent chemical stability, the Au electrode can cause serious solar cell degradation due to Au diffusion into MAPbI 3. In addition to Au, many other metals have been used as electrodes inmore » MAPbI 3 solar cells. However, how the external metal impurities introduced by electrodes affect the long-term stability of MAPbI 3 solar cells has rarely been studied. A comprehensive study of formation energetics and diffusion dynamics of a number of noble and transition metal impurities (Au, Ag, Cu, Cr, Mo, W, Co, Ni, Pd) in MAPbI 3 based on first-principles calculations is reported herein. The results uncover important general trends of impurity formation and diffusion in MAPbI 3 and provide useful guidance for identifying the optimal metal electrodes that do not introduce electrically active impurity defects in MAPbI 3 while having low resistivities and suitable work functions for carrier extraction.« less

Formation and Diffusion of Metal Impurities in Perovskite Solar Cell Material CH3NH3PbI3: Implications on Solar Cell Degradation and Choice of Electrode

PubMed Central

Ming, Wenmei; Yang, Dongwen; Li, Tianshu

2017-01-01

Abstract Solar cells based on methylammonium lead triiodide (MAPbI3) have shown remarkable progress in recent years and have demonstrated efficiencies greater than 20%. However, the long‐term stability of MAPbI3‐based solar cells has yet to be achieved. Besides the well‐known chemical and thermal instabilities, significant native ion migration in lead halide perovskites leads to current–voltage hysteresis and photoinduced phase segregation. Recently, it is further revealed that, despite having excellent chemical stability, the Au electrode can cause serious solar cell degradation due to Au diffusion into MAPbI3. In addition to Au, many other metals have been used as electrodes in MAPbI3 solar cells. However, how the external metal impurities introduced by electrodes affect the long‐term stability of MAPbI3 solar cells has rarely been studied. A comprehensive study of formation energetics and diffusion dynamics of a number of noble and transition metal impurities (Au, Ag, Cu, Cr, Mo, W, Co, Ni, Pd) in MAPbI3 based on first‐principles calculations is reported herein. The results uncover important general trends of impurity formation and diffusion in MAPbI3 and provide useful guidance for identifying the optimal metal electrodes that do not introduce electrically active impurity defects in MAPbI3 while having low resistivities and suitable work functions for carrier extraction. PMID:29610728

Enhancement of plasmon-induced charge separation efficiency by coupling silver nanocubes with a thin gold film

NASA Astrophysics Data System (ADS)

Akiyoshi, Kazutaka; Saito, Koichiro; Tatsuma, Tetsu

2016-10-01

Plasmon-induced charge separation (PICS), in which an energetic electron is injected from a plasmonic nanoparticle (NP) to a semiconductor on contact, is often inhibited by a protecting agent adsorbed on the NP. We addressed this issue for an Ag nanocube-TiO2 system by coating it with a thin Au layer or by inserting the Au layer between the nanocubes (NCs) and TiO2. Both of the electrodes exhibit much higher photocurrents due to PICS than the electrodes without the Au film or the Ag NCs. These photocurrent enhancements can be explained in terms of PICS with accelerated electron transfer, in which electron injection from the Ag NCs or Ag@Au core-shell NCs to TiO2 is promoted by the Au film, or PICS enhanced by a nanoantenna effect, in which the electron injection from the Au film to TiO2 is enhanced by optical near field generated by the Ag NC.

Tremella-like graphene-Au composites used for amperometric determination of dopamine.

PubMed

Li, Cong; Zhao, Jingyu; Yan, Xiaoyi; Gu, Yue; Liu, Weilu; Tang, Liu; Zheng, Bo; Li, Yaru; Chen, Ruixue; Zhang, Zhiquan

2015-03-21

Electrochemical detection of dopamine (DA) plays an important role in medical diagnosis. In this paper, tremella-like graphene-Au (t-GN-Au) composites were synthesized by a one-step hydrothermal method for selective detection of DA. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), Raman spectroscopy, and Fourier transform infrared (FTIR) spectroscopy were used to characterize as-prepared t-GN-Au composites. The t-GN-Au composites were directly used for the determination of DA via cyclic voltammetry (CV) and the chronoamperometry (CA) technique. CA measurement gave a wide linear range from 0.8 to 2000 μM, and the detection limit of 57 nM (S/N = 3) for DA. The mechanism and the heterogeneous electron transfer kinetics of the DA oxidation were discussed in the light of rotating disk electrode (RDE) experiments. Moreover, the modified electrode was applied to the determination of DA in human urine and serum samples.

Realization of MEMS-IC Vertical Integration Utilizing Smart Bumpless Bonding

NASA Astrophysics Data System (ADS)

Shiozaki, Masayoshi; Moriguchi, Makoto; Sasaki, Sho; Oba, Masatoshi

This paper reports fundamental technologies, properties, and new experimental results of SBB (Smart Bumpless Bonding) to realize MEMS-IC vertical integration. Although conventional bonding technologies have had difficulties integrating MEMS and its processing circuit because of their rough bonding surfaces, fragile structures, and thermal restriction, SBB technology realized the vertical integration without thermal treatment, any adhesive materials including bumps, and chemical mechanical polishing. The SBB technology bonds sealing parts for vacuum sealing and electrodes for electrical connection simultaneously as published in previous experimental study. The plasma CVD SiO2 is utilized to realize vacuum sealing as sealing material. And Au projection studs are formed on each electrode and connected electrically between two wafers by compressive plastic deformation and surface activation. In this paper, new experimental results including vacuum sealing properties, electrical improvement, IC bonding results on the described fundamental concept and properties are reported.

Electrochemiluminescence of luminol enhanced by the synergetic catalysis of hemin and silver nanoparticles for sensitive protein detection.

PubMed

Jiang, Xinya; Chai, Yaqin; Wang, Haijun; Yuan, Ruo

2014-04-15

A novel and ultrasensitive electrochemiluminescence (ECL) immunosensor, which was based on the amplifying ECL of luminol by hemin-reduced graphene oxide (hemin-rGO) and Ag nanoparticles (AgNPs) decorated reduced graphene oxide (Ag-rGO), was constructed for the detection of carcinoembryonic antigen (CEA). For this proposed sandwich-type ECL immunosensor, Au nanoparticles electrodeposited (DpAu) onto hemin-rGO (DpAu/hemin-rGO) constructed the base of the immunosensor. DpAu had outstanding electrical conductivity to promote the electron transfer at the electrode interface and had good biocompatibility to load large amounts of primary antibody (Ab1), which provided an excellent platform for this immunosensor. Moreover, AgNPs and glucose oxidase (GOD) functionalized graphene labeled secondary antibody (Ag-rGO-Ab2-GOD) was designed as the signal probe for the sandwiched immunosensor. Not only did the hemin-rGO improve the electron transfer of the electrode surface, but hemin also further amplified the ECL signal of luminol in the presence of hydrogen peroxide (H2O2). With the aid of Ag-rGO-Ab2-GOD, enhanced signal was obtained by in situ generation of H2O2 and catalysis of AgNPs to ECL reaction of the luminol-H2O2 system. The as-prepared ECL immunosensor exhibited excellent analytical property for the detection of CEA in the range from 0.1 pg mL(-1) to 160 ng mL(-1) with a detection limit of 0.03 pg mL(-1) (SN(-1)=3). © 2013 Published by Elsevier B.V.

Fabrication of Micro-Needle Electrodes for Bio-Signal Recording by a Magnetization-Induced Self-Assembly Method

PubMed Central

Chen, Keyun; Ren, Lei; Chen, Zhipeng; Pan, Chengfeng; Zhou, Wei; Jiang, Lelun

2016-01-01

Micro-needle electrodes (MEs) have attracted more and more attention for monitoring physiological electrical signals, including electrode-skin interface impedance (EII), electromyography (EMG) and electrocardiography (ECG) recording. A magnetization-induced self-assembling method (MSM) was developed to fabricate a microneedle array (MA). A MA coated with Ti/Au film was assembled as a ME. The fracture and insertion properties of ME were tested by experiments. The bio-signal recording performance of the ME was measured and compared with a typical commercial wet electrode (Ag/AgCl electrode). The results show that the MA self-assembled from the magnetic droplet array under the sum of gravitational surface tension and magnetic potential energies. The ME had good toughness and could easily pierce rabbit skin without being broken or buckling. When the compression force applied on the ME was larger than 2 N, ME could stably record EII, which was a lower value than that measured by Ag/AgCl electrodes. EMG signals collected by ME varied along with the contraction of biceps brachii muscle. ME could record static ECG signals with a larger amplitude and dynamic ECG signals with more distinguishable features in comparison with a Ag/AgCl electrode, therefore, ME is an alternative electrode for bio-signal monitoring in some specific situations. PMID:27657072

Gold nanoparticles hosted in a water-soluble silsesquioxane polymer applied as a catalytic material onto an electrochemical sensor for detection of nitrophenol isomers.

PubMed

Silva, Paulo Sérgio da; Gasparini, Bianca C; Magosso, Hérica A; Spinelli, Almir

2014-05-30

The water-soluble 3-n-propyl-4-picolinium silsesquioxane chloride (Si4Pic(+)Cl(-)) polymer was prepared, characterized and used as a stabilizing agent for the synthesis of gold nanoparticles (nAu). The ability of Si4Pic(+)Cl(-) to adsorb anionic metal complexes such as AuCl4(-) ions allowed well-dispersed nAu to be obtained with an average particle size of 4.5nm. The liquid suspension of nAu-Si4Pic(+)Cl(-) was deposited by the drop coating method onto a glassy carbon electrode (GCE) surface to build a sensor (nAu-Si4Pic(+)Cl(-)/GCE) which was used for the detection of o-nitrophenol (o-NP) and p-nitrophenol (p-NP). Under optimized experimental conditions the reduction peak current increased with increasing concentrations of both nitrophenol isomers in the range of 0.1-1.5μmolL(-1). The detection limits were 46nmolL(-1) and 55nmolL(-1) for o-NP and p-NP, respectively. These findings indicate that the nAu-Si4Pic(+)Cl(-) material is a very promising candidate to assemble electrochemical sensors for practical applications in the field of analytical chemistry. Copyright © 2014 Elsevier B.V. All rights reserved.

Carbon Dioxide Gas Sensors and Method of Manufacturing and Using Same

NASA Technical Reports Server (NTRS)

Hunter, Gary W. (Inventor); Xu, Jennifer C. (Inventor)

2014-01-01

A gas sensor comprises a substrate layer; a pair of interdigitated metal electrodes, said electrodes include upper surfaces, the electrodes selected from the group consisting of Pt, Pd, Au, Ir, Ag, Ru, Rh, In, Os, and their alloys. A first layer of solid electrolyte staying in between electrode fingers and partially on said upper surfaces of said electrodes, said first layer selected from NASICON, LISICON, KSICON and.beta.''-Alumina. A second layer of metal carbonate(s) as an auxiliary electrolyte engaging said upper surfaces of the electrodes and the first solid electrolyte. The metal carbonates selected from the group consisting of the following ions Na.sup.+, K.sup.+, Li.sup.+, Ag.sup.+, H.sup.+, Pb.sup.2+, Sr.sup.2+, Ba.sup.2+, and any combination thereof. An extra layer of metal oxide selected from the group consisting of SnO.sub.2, In.sub.2O.sub.3, TiO.sub.2, WO.sub.3, ZnO, Fe.sub.2O.sub.3, ITO, CdO, U.sub.3O.sub.8, Ta.sub.2O.sub.5, BaO, MoO.sub.2, MoO.sub.3, V.sub.2O.sub.5, Nb.sub.2O.sub.5, CuO, Cr.sub.2O.sub.3, La.sub.2O.sub.3, RuO.sub.3, RuO.sub.2, ReO.sub.2, ReO.sub.3, Ag.sub.2O, CoO, Cu.sub.2O, SnO, NiO, Pr.sub.2O.sub.3, BaO, PdO.sub.2, HfO.sub.3, HfO.sub.3 or other metal oxide and their mixtures residing above and in engagement with the second electrolyte to improve sensor performance and/or to reduce sensor heating power consumption.

Pd-Au@carbon dots nanocomposite: Facile synthesis and application as an ultrasensitive electrochemical biosensor for determination of colitoxin DNA in human serum.

PubMed

Huang, Qitong; Lin, Xiaofeng; Zhu, Jie-Ji; Tong, Qing-Xiao

2017-08-15

In this study, a green and fast method was developed to synthesize high-yield carbon dots (CDs) via one-pot microwave treatment of banana peels without using any other surface passivation agents. Then the as-prepared CDs was used as the reducing agent and stabilizer to synthesize a Pd-Au@CDs nanocomposite by a simple sequential reduction strategy. Finally, Pd-Au@CDs nanocomposite modified glassy carbon electrode (Pd-Au@CDs/GCE) was obtained as a biosensor for target DNA after being immobilized a single-stranded probe DNA by a carboxyl ammonia condensation reaction. Under the optimal conditions, the sensor could detect target DNA concentrations in the range from 5.0×10 -16 to 1.0×10 -1 °molL -1 . The detection limit (LD) was estimated to be 1.82×10 -17 molL -1 , which showed higher sensitivity than other electrochemical biosensors reported. In addition, the DNA sensor was also successfully applied to detect colitoxin DNA in human serum. Copyright © 2017 Elsevier B.V. All rights reserved.

Nanoparticle-wetted surfaces for relays and energy transmission contacts.

PubMed

Voevodin, Andrey A; Vaia, Richard A; Patton, Steven T; Diamanti, Steven; Pender, Mark; Yoonessi, Mitra; Brubaker, Jennifer; Hu, Jian-Jun; Sanders, Jeffrey H; Phillips, Benjamin S; MacCuspie, Robert I

2007-11-01

Submonolayer coatings of noble-metal nanoparticle liquids (NPLs) are shown to provide replenishable surfaces with robust asperities and metallic conductivity that extends the durability of electrical relays by 10 to 100 times (depending on the current driven through the contact) as compared to alternative approaches. NPLs are single-component materials consisting of a metal nanoparticle core (5-20 nm Au or Pt nanoparticles) surrounded by a covalently tethered ionic-liquid corona of 1.5 to 2 nm. Common relay failure modes, such as stiction, surface distortion, and contact shorting, are suppressed with the addition of a submonolayer of NPLs to the contact surfaces. This distribution of NPLs results in a force profile for a contact-retraction cycle that is distinct from bare Au contacts and thicker, multilayer coatings of NPLs. Postmortem examination reveals a substantial decrease in topological change of the electrode surface relative to bare contacts, as well as an indication of lateral migration of the nanoparticles from the periphery towards the contact. A general extension of this concept to dynamic physical interfaces experiencing impact, sliding, or rolling affords alternatives to increase reliability and reduced losses for transmittance of electrical and mechanical energy.

Fabrication and characterisation of ligand-functionalised ultrapure monodispersed metal nanoparticle nanoassemblies employing advanced gas deposition technique

NASA Astrophysics Data System (ADS)

Geremariam Welearegay, Tesfalem; Cindemir, Umut; Österlund, Lars; Ionescu, Radu

2018-02-01

Here, we report for the first time the fabrication of ligand-functionalised ultrapure monodispersed metal nanoparticles (Au, Cu, and Pt) from their pure metal precursors using the advanced gas deposition technique. The experimental conditions during nanoparticle formation were adjusted in order to obtain ultrafine isolated nanoparticles on different substrates. The morphology and surface analysis of the as-deposited metal nanoparticles were investigated using scanning electron microscopy, x-ray diffraction and Fourier transform infra-red spectroscopy, which demonstrated the formation of highly ordered pure crystalline nanoparticles with a relatively uniform size distribution of ∼10 nm (Au), ∼4 nm (Cu) and ∼3 nm (Pt), respectively. A broad range of organic ligands containing thiol or amine functional groups were attached to the nanoparticles to form continuous networks of nanoparticle-ligand nanoassemblies, which were characterised by scanning electron microscopy and x-ray photoelectron spectroscopy. The electrical resistance of the functional nanoassemblies deposited in the gap spacing of two microfabricated parallel Au electrodes patterned on silicon substrates ranged between tens of kΩ and tens of MΩ, which is suitable for use in many applications including (bio)chemical sensors, surface-enhanced Raman spectroscopy and molecular electronic rectifiers.

A Nano-Au/C-MWCNT based label free amperometric immunosensor for the detection of capsicum chlorosis virus in bell pepper.

PubMed

Sharma, Anshul; Kaushal, Ankur; Kulshrestha, Saurabh

2017-07-01

Accurate and on time diagnosis of plant viruses is an essential prerequisite for efficient control in field conditions. A number of diagnostic methods have been reported with the required level of sensitivity. Here, we propose a label free immunosensor for efficient and sensitive detection of capsicum chlorosis virus (CaCV) in bell pepper. Antigen was immobilized over the surface of gold nanoparticle/multi-walled carbon nanotube (Nano-Au/C-MWCNT) screen printed electrodes using 1-Ethyl-3-(3-dimethylaminopropyl)carbodiimide (EDC)/N-hydroxysuccinimide (NHS) cross linking chemistry followed by interaction with groundnut bud necrosis virus (GBNV)/CaCV specific polyclonal antibody. The electrochemical response was measured by cyclic voltammetry (CV), differential pulse voltammetry (DPV) using the redox indicator. Electrode surface characterization was done by performing scanning electron microscopy (SEM). Electrochemical studies showed positive results at different antigenic dilutions ranging from 10 -2 - 8x10 -5 . The sensitivity of the immunosensor developed has been compared with direct antigen coated enzyme-linked immunosorbent assay (DAC-ELISA) and the results showed that the immunosensor developed was 800-1000 times more sensitive, when compared to DAC-ELISA for CaCV detection. The immunosensor we have developed is economical and sensitive and could be used for immediate determination of the presence of virus in extracts from bell pepper leaves.

An efficient signal-on aptamer-based biosensor for adenosine triphosphate detection using graphene oxide both as an electrochemical and electrochemiluminescence signal indicator.

PubMed

Huang, Xiang; Li, Yuqin; Zhang, Xiaoshan; Zhang, Xin; Chen, Yaowen; Gao, Wenhua

2015-09-07

An efficient aptasensor was developed in which graphene oxide (GO) was employed as an indicator for both electrochemical impedance spectroscopy and electrochemiluminescence (ECL) signal generation. The aptasensor was fabricated by self-assembling the ECL probe of a thiolated adenosine triphosphate binding aptamer (ABA) tagged with a Ru complex (Ru(bpy)3(2+) derivatives) onto the surface of gold nanoparticle (AuNP) modified glassy carbon electrode (GCE). ABA immobilized onto AuNP modified GCE could strongly adsorb GO due to the strong π-π interaction between ABA and graphene oxide; ECL quenching of the Ru complex then takes place because of energy transfer and electron transfer, and a large increase of the electron transfer resistance (Ret) of the electrode. While in the presence of target adenosine triphosphate (ATP), the ABA prefers to form ABA-ATP bioaffinity complexes, which have weak affinity to graphene oxide and keep the graphene oxide away from the electrode surface, thus allowing the ECL signal enhancement, and in conjunction with the decrease of the Ret. Because of the high ECL quenching efficiency, unique structure, and electronic properties of graphene oxide, the Ret and ECL intensity versus the logarithm of ATP concentration was linear in the wide range from 10 pM to 10 nM with an ultra-low detection limit of 6.7 pM to 4.8 pM, respectively. The proposed aptasensor exhibited excellent reproducibility, stability, and outstanding selectivity, and ATP could be effectively distinguished from its analogues. More significantly, this efficient ECL aptasensor strategy based on GO acting both as an electrochemical and ECL signal indicator is general and can be easily extended to other biological binding events.

Integrated electrochemical gluconic acid biosensor based on self-assembled monolayer-modified gold electrodes. Application to the analysis of gluconic acid in musts and wines.

PubMed

Campuzano, S; Gamella, M; Serra, B; Reviejo, A J; Pingarrón, J M

2007-03-21

An integrated amperometric gluconic acid biosensor constructed using a gold electrode (AuE) modified with a self-assembled monolayer (SAM) of 3-mercaptopropionic acid (MPA) on which gluconate dehydrogenase (GADH, 0.84 U) and the mediator tetrathiafulvalene (TTF, 1.5 micromol) were coimmobilized by covering the electrode surface with a dialysis membrane is reported. The working conditions selected were Eapp=+0.15 V and 25+/-1 degrees C. The useful lifetime of one single TTF-GADH-MPA-AuE was surprisingly long. After 53 days of continuous use, the biosensor exhibited 86% of the original sensitivity. A linear calibration plot was obtained for gluconic acid over the 6.0x10(-7) to 2.0x10(-5) M concentration range, with a limit of detection of 1.9x10(-7) M. The effect of potential interferents (glucose, fructose, galactose, arabinose, and tartaric, citric, malic, ascorbic, gallic, and caffeic acids) on the biosensor response was evaluated. The behavior of the biosensor in a flow-injection system in connection with amperometric detection was tested. The analytical usefulness of the biosensor was evaluated by determining gluconic acid in wine and must samples, and the results obtained were validated by comparison with those provided by using a commercial enzyme test kit.

Chemically reduced graphene oxide-P25-Au nanocomposite materials and their photoelectrocatalytic and photocatalytic applications.

PubMed

Praveen, Raju; Ramaraj, Ramasamy

2016-10-05

Visible light active photocatalysts consisting of gold nanoparticle (Au NP) decorated chemically reduced graphene oxide-P25 nanocomposite materials (CRGO-P25-Au NCMs) were prepared through a one-pot chemical reduction method. The nanocomposite materials were characterized using diffuse reflectance spectroscopy (DRS), X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM) and electrochemical impedance spectroscopy (EIS) analyses. The performances of CRGO-P25-Au NCM modified ITO electrodes were evaluated towards the photoelectrochemical oxidation of methanol. The photoelectrode fabricated using CRGO-P25-Au NCM exhibited a higher photocurrent of 293 μA cm -2 compared to other control electrodes. The CRGO-P25-Au NCMs were also used for the photocatalytic reduction of highly toxic chromium(vi) ions to chromium(iii) ions in the presence of oxalic acid as a sacrificial electron donor. The results showed that around 75% of the Cr(vi) ions were photocatalytically reduced to Cr(iii) ions by the CRGO-P25-Au NCM within the light irradiation time of 1 h. In both applications, the enhanced catalytic activity of the CRGO-P25-Au NCM was attributed to the improved visible light absorption and the reduced charge recombination exerted by the interaction of CRGO and Au NPs with P25 and their synergistic effects.

Highly sensitive aptasensor based on synergetic catalysis activity of MoS2-Au-HE composite using cDNA-Au-GOD for signal amplification.

PubMed

Song, Hai-Yan; Kang, Tian-Fang; Lu, Li-Ping; Cheng, Shui-Yuan

2017-03-01

Single or few-layer nanosheets of MoS 2 (MoS 2 nanosheets) and a composite composed of MoS 2 nanosheets, Au nanoparticles (AuNPs) and hemin (HE) (denoted as MoS 2 -Au-HE) were prepared. The composites possessed high synergetic catalysis activity towards the electroreduction of hydrogen peroxide. Furthermore, glucose oxidase (GOD) and AuNPs were used as marker of the complementary DNA (cDNA) strand of kanamycin aptamer to prepare a conjugate (reffered as cDNA-Au-GOD) that was designed as the signal probe. Both cDNA-Au-GOD and MoS 2 -Au-HE were applied to fabricate aptasensor for kanamycin. MoS 2 -Au-HE acted as solid platform for kanamycin aptamer and signal transmitters. AuNPs were employed as the supporter of cDNA and GOD which catalyze dissolved oxygen to produce hydrogen peroxide in the presence of glucose. Then cathodic peak current of H 2 O 2 was recorded by differential pulse voltammetry (DPV). The electrochemical reduction of H 2 O 2 was catalyzed by MoS 2 -Au-HE that was modified onto the surface of a glassy carbon electrode (GCE). The cathodic peak current of H 2 O 2 was highly linearly decreased with an increase of kanamycin concentrations from 1.0ng/L to 1.0×10 5 ng/L, with a detection limit of 0.8ng/L. This aptasensor can be used to detect kanamycin in milk with high specificity, sensitivity and selectivity. Copyright © 2016 Elsevier B.V. All rights reserved.

The Vital Function of Fe3O4@Au nanocomposites for Hydrolase Biosensor Design and Its Application in Detection of Methyl Parathion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhao, Yuting; Zhang, Weiying; Lin, Yuehe

A nanocomposite of gold nanoparticles (AuNPs) decorating a magnetic Fe3O4 core was synthesized using cysteamine (SH–NH2) as linker, and characterized by TEM, XPS, UV and electrochemistry. Then a hydrolase biosensor, based on self-assembly of methyl parathion hydrolase (MPH) on the Fe3O4@Au nanocomposite, was developed for sensitive and selective detection of the organophosphorus pesticide (OP) methyl parathion. The magnetic nanocomposite provides an easy way to construct the enzyme biosensor by simply exerting an external magnetic field, and also provides a simple way to renew the electrode surface by removing the magnet. Unlike inhibition-based enzyme biosensors, the hydrolase is not poisoned bymore » OPs and thus is reusable for continuous measurement. AuNPs not only provide a large surface area, high loading efficiency and fast electron transfer, but also stabilize the enzyme through electrostatic interactions. The MPH biosensor shows rapid response and high selectivity for detection of methyl parathion, with a linear range from 0.5 to 1000 ng/mL and a detection limit of 0.1 ng/mL. It also shows acceptable reproducibility and stability. The simplicity and ease of operation of the proposed method has great potential for on-site detection of P–S containing pesticides and provides a promising strategy to construct a robust biosensor.« less

A cyclometalated iridium(III) complex used as a conductor for the electrochemical sensing of IFN-γ

NASA Astrophysics Data System (ADS)

Miao, Xiangmin; Ko, Chung-Nga; Vellaisamy, Kasipandi; Li, Zongbing; Yang, Guanjun; Leung, Chung-Hang; Ma, Dik-Lung

2017-02-01

A novel iridium(III) complex was prepared and used as a conductor for sensitive and enzyme-free electrochemical detection of interferon gamma (IFN-γ). This assay is based on a dual signal amplification mechanism involving positively charged gold nanoparticles ((+)AuNPs) and hybridization chain reaction (HCR). To construct the sensor, nafion (Nf) and (+)AuNPs composite membrane was first immobilized onto the electrode surface. Subsequently, a loop-stem structured capture probe (CP) containing a special IFN-γ interact strand was modified onto the (+)AuNP surface via the formation of Au-S bonds. Upon addition of IFN-γ, the loop-stem structure of CP was opened, and the newly exposed “sticky” region of CP then hybridized with DNA hairpin-1 (H1), which in turn opened its hairpin structure for hybridizing with DNA hairpin-2 (H2). Happen of HCR between H1 and H2 thus generated a polymeric duplex DNA (dsDNA) chain. Meanwhile, the iridium(III) complex could interact with the grooves of the dsDNA polymer, producing a strong current signal that was proportional to IFN-γ concentration. Thus, sensitive detection of IFN-γ could be realized with a detection limit down to 16.3 fM. Moreover, satisfied results were achieved by using this method for the detection of IFN-γ in human serum samples.

Functionalization of indium-tin-oxide electrodes by laser-nanostructured gold thin films for biosensing applications

NASA Astrophysics Data System (ADS)

Grochowska, Katarzyna; Siuzdak, Katarzyna; Karczewski, Jakub; Śliwiński, Gerard

2015-12-01

The production and properties of the indium-tin-oxide (ITO) electrodes functionalized by Au nanoparticle (NP) arrays of a relatively large area formed by pulsed laser nanostructuring of thin gold films are reported and discussed. The SEM inspection of modified electrodes reveals the presence of the nearly spherical and disc-shaped particles of dimensions in the range of 40-120 nm. The NP-array geometry can be controlled by selection of the laser processing conditions. It is shown that particle size and packing density of the array are important factors which determine the electrode performance. In the case of NP-modified electrodes the peak current corresponding to the glucose direct oxidation process shows rise with increasing glucose concentration markedly higher comparing to the reference Au disc electrode. The detection limit reaches 12 μM and linear response of the sensor is observed from 0.1 to 47 mM that covers the normal physiological range of the blood sugar detection.

13.2% efficiency Si nanowire/PEDOT:PSS hybrid solar cell using a transfer-imprinted Au mesh electrode

PubMed Central

Park, Kwang-Tae; Kim, Han-Jung; Park, Min-Joon; Jeong, Jun-Ho; Lee, Jihye; Choi, Dae-Geun; Lee, Jung-Ho; Choi, Jun-Hyuk

2015-01-01

In recent years, inorganic/organic hybrid solar cell concept has received growing attention for alternative energy solution because of the potential for facile and low-cost fabrication and high efficiency. Here, we report highly efficient hybrid solar cells based on silicon nanowires (SiNWs) and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) using transfer-imprinted metal mesh front electrodes. Such a structure increases the optical absorption and shortens the carrier transport distance, thus, it greatly increases the charge carrier collection efficiency. Compared with hybrid cells formed using indium tin oxide (ITO) electrodes, we find an increase in power conversion efficiency from 5.95% to 13.2%, which is attributed to improvements in both the electrical and optical properties of the Au mesh electrode. Our fabrication strategy for metal mesh electrode is suitable for the large-scale fabrication of flexible transparent electrodes, paving the way towards low-cost, high-efficiency, flexible solar cells. PMID:26174964

3D-nanostructured Au electrodes for the event-specific detection of MON810 transgenic maize.

PubMed

Fátima Barroso, M; Freitas, Maria; Oliveira, M Beatriz P P; de-Los-Santos-Álvarez, Noemí; Lobo-Castañón, María Jesús; Delerue-Matos, Cristina

2015-03-01

In the present work, the development of a genosensor for the event-specific detection of MON810 transgenic maize is proposed. Taking advantage of nanostructuration, a cost-effective three dimensional electrode was fabricated and a ternary monolayer containing a dithiol, a monothiol and the thiolated capture probe was optimized to minimize the unspecific signals. A sandwich format assay was selected as a way of precluding inefficient hybridization associated with stable secondary target structures. A comparison between the analytical performance of the Au nanostructured electrodes and commercially available screen-printed electrodes highlighted the superior performance of the nanostructured ones. Finally, the genosensor was effectively applied to detect the transgenic sequence in real samples, showing its potential for future quantitative analysis. Copyright © 2014 Elsevier B.V. All rights reserved.

The Au Cathode in the System Li2CO3-CO2-CO at 800 to 900 C

NASA Technical Reports Server (NTRS)

Hagedorn, Norman H.

1991-01-01

Gold is one of several metals being evaluated at NASA Lewis Research Center as positive electrode catalysts for an alkali metal/molten alkali metal carbonate/carbon dioxide electrochemical cell. Such a cell is proposed for CO2-rich planetary atmospheres such as those of Mars and Venus. Its application could be as a primary power supply, as a secondary power supply recharged either 'chemically' by replenishment of the alkali metal or electrochemically from a central station power source, or as a converter of carbon dioxide to oxygen via a complete electrochemical cycle. For the work being reported, lithium was assumed to be the alkali metal of choice for the negative electrode of the cell, and therefore molten lithium carbonate was the electrolyte used in the Au electrode experiments. Cathodic linear sweep voltammetry (LSV) was the primary analytical technique for evaluating the performance of the Au cathode. interest comprised the cell temperature and the total pressure and composition of the reactant gas. In the absence of operational difficulties, the effect of bubbling the reactant gas through the melt was also determined. On the basis of the variation of electrode performance with changes in these parameters, inferences have been made concerning the electrochemical and chemical processes at and near the electrode. The results of post-test micrographic analyses of the Au cathode are also presented. An attempt is then made to project from the experimental results to some relevant conclusions pertaining to a gold cathode in a practical alkali metal - carbon dioxide cell.

Dominance of Plasmonic Resonant Energy Transfer over Direct Electron Transfer in Substantially Enhanced Water Oxidation Activity of BiVO4 by Shape-Controlled Au Nanoparticles.

PubMed

Lee, Mi Gyoung; Moon, Cheon Woo; Park, Hoonkee; Sohn, Woonbae; Kang, Sung Bum; Lee, Sanghan; Choi, Kyoung Jin; Jang, Ho Won

2017-10-01

The performance of plasmonic Au nanostructure/metal oxide heterointerface shows great promise in enhancing photoactivity, due to its ability to confine light to the small volume inside the semiconductor and modify the interfacial electronic band structure. While the shape control of Au nanoparticles (NPs) is crucial for moderate bandgap semiconductors, because plasmonic resonance by interband excitations overlaps above the absorption edge of semiconductors, its critical role in water splitting is still not fully understood. Here, first, the plasmonic effects of shape-controlled Au NPs on bismuth vanadate (BiVO 4 ) are studied, and a largely enhanced photoactivity of BiVO 4 is reported by introducing the octahedral Au NPs. The octahedral Au NP/BiVO 4 achieves 2.4 mA cm -2 at the 1.23 V versus reversible hydrogen electrode, which is the threefold enhancement compared to BiVO 4 . It is the highest value among the previously reported plasmonic Au NPs/BiVO 4 . Improved photoactivity is attributed to the localized surface plasmon resonance; direct electron transfer (DET), plasmonic resonant energy transfer (PRET). The PRET can be stressed over DET when considering the moderate bandgap semiconductor. Enhanced water oxidation induced by the shape-controlled Au NPs is applicable to moderate semiconductors, and shows a systematic study to explore new efficient plasmonic solar water splitting cells. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrathin efficient perovskite solar cells employing a periodic structure of a composite hole conductor for elevated plasmonic light harvesting and hole collection

NASA Astrophysics Data System (ADS)

Long, Mingzhu; Chen, Zefeng; Zhang, Tiankai; Xiao, Yubin; Zeng, Xiaoliang; Chen, Jian; Yan, Keyou; Xu, Jianbin

2016-03-01

We developed a molecule/polymer composite hole transporting material (HTM) with a periodic microstructure for morphology replication of a corrugated Au electrode, which in combination plays a dual role in the optical and electronic enhancement of high performance perovskite solar cells (PSCs). The electro-optics revealed that perovskite couldn't readily extinct the red light even though the thickness increased to 370 nm, but we found that the quasi periodic microstructure composite (PMC) HTM in combination with the conformal Au electrode could promote the absorption through the enhanced cavity effects, leading to comparable absorption even using much thinner perovskite (240 nm). We identified that the cavity was the combination of Fabry-Pérot interferometer and surface plasmonic resonance, with light harvesting enhancement through surface plasmon polariton or waveguide modes that propagate in the plane of the perovskite layer. On the other hand, the PMC HTM increased hole conductivity by one order of magnitude with respect to standard spiro-OMeTAD HTM due to molecular packing and self-assembly, embodying traceable hole mobility and density elevation up to 3 times, and thus the hysteresis was greatly avoided. Owing to dual optical and electronic enhancement, the PMC PSC afforded high efficiency PSC using as thin as 240 nm perovskite layer, delivering a Voc of 1.05 V, Jsc of 22.9 mA cm-2, FF of 0.736, and efficiency amounting to 17.7% PCE, the highest efficiency with ultrathin perovskite layer.We developed a molecule/polymer composite hole transporting material (HTM) with a periodic microstructure for morphology replication of a corrugated Au electrode, which in combination plays a dual role in the optical and electronic enhancement of high performance perovskite solar cells (PSCs). The electro-optics revealed that perovskite couldn't readily extinct the red light even though the thickness increased to 370 nm, but we found that the quasi periodic microstructure composite (PMC) HTM in combination with the conformal Au electrode could promote the absorption through the enhanced cavity effects, leading to comparable absorption even using much thinner perovskite (240 nm). We identified that the cavity was the combination of Fabry-Pérot interferometer and surface plasmonic resonance, with light harvesting enhancement through surface plasmon polariton or waveguide modes that propagate in the plane of the perovskite layer. On the other hand, the PMC HTM increased hole conductivity by one order of magnitude with respect to standard spiro-OMeTAD HTM due to molecular packing and self-assembly, embodying traceable hole mobility and density elevation up to 3 times, and thus the hysteresis was greatly avoided. Owing to dual optical and electronic enhancement, the PMC PSC afforded high efficiency PSC using as thin as 240 nm perovskite layer, delivering a Voc of 1.05 V, Jsc of 22.9 mA cm-2, FF of 0.736, and efficiency amounting to 17.7% PCE, the highest efficiency with ultrathin perovskite layer. Electronic supplementary information (ESI) available: XRD patterns corresponding to the perovskite; AFM images of 3D PMC HTM perovskite solar cells; performance statistics for 3D PMC HTM; ultraviolet photoelectron spectra (UPS) of HTMs on FTO. See DOI: 10.1039/c5nr05042a

Label-free peptide aptamer based impedimetric biosensor for highly sensitive detection of TNT with a ternary assembly layer.

PubMed

Li, Yanyan; Zhao, Manru; Wang, Haiyan

2017-11-01

We report a label-free peptide aptamer based biosensor for highly sensitive detection of TNT which was designed with a ternary assembly layer consisting of anti-TNT peptide aptamer (peptamer), dithiothreitol (DTT), and 6-mercaptohexanol (MCH), forming Au/peptamer-DTT/MCH. A linear relationship between the change in electron transfer resistance and the logarithm of the TNT concentration from 0.44 to 18.92 pM, with a detection limit of 0.15 pM, was obtained. In comparison, the detection limit of the aptasensor with a common binary assembly layer (Au/peptamer/MCH) was 0.15 nM. The remarkable improvement in the detection limit could be ascribed to the crucial role of the ternary assembly layer, providing an OH-richer hydrophilic environment and a highly compact surface layer with minimal surface defects, reducing the non-covalent binding (physisorption) of the peptamer and non-specific adsorption of TNT onto the electrode surface, leading to high sensitivity, and which can serve as a general sensing platform for the fabrication of other biosensors.

Alcohol oxidase protein mediated in-situ synthesized and stabilized gold nanoparticles for developing amperometric alcohol biosensor.

PubMed

Chinnadayyala, Somasekhar R; Santhosh, Mallesh; Singh, Naveen K; Goswami, Pranab

2015-07-15

A simple one step method for the alcohol oxidases (AOx) protein mediated synthesis of gold nano-particles (AuNPs) in alkaline (pH 8.5) condition with simultaneous stabilization of the nanoparticles on the AOx protein surface under native environment has been developed. The formation of the AOx conjugated AuNPs was confirmed by advanced analytical and spectroscopic techniques. The significant increase in zeta potential (ζ) value of -57mV for the synthesized AOx-AuNPs conjugate from the AOx (pI 4.5) protein (ζ, -30mV) implied good stability of the in-situ synthesized nano-conjugate. The AOx-AuNPs conjugate showed steady stability in alkaline (upto pH 8.5) and NaCl (up to 10(-1)M) solutions. The efficiency (Kcat/Km) of the AuNP conjugated AOx was increased by 18% from the free enzyme confirming the activating role of the surface stabilized AuNPs for the enzyme. The AuNPs-AOx conjugate was encapsulated with polyaniline (PANI) synthesized by oxidative polymerization of aniline using H2O2 generated in-situ from the AOx catalysed oxidation of alcohol. The PANI encapsulated AuNPs-AOx assembly was stabilized on a glassy carbon electrode (GCE) by chitosan-Nafion mixture and then utilized the fabricated bioelectrode for detection of alcohol amperometrically using H2O2 as redox indicator at +0.6V. The constructed biosensor showed high operational stability (6.3% loss after 25 measurements), wide linear detection range of 10µM-4.7mM (R(2)=0.9731), high sensitivity of 68.3±0.35µAmM(-1) and low detection limit of 7±0.027µM for ethanol. The fabricated bioelectrode was successfully used for the selective determination of alcohol in beverage samples. Copyright © 2015 Elsevier B.V. All rights reserved.

An electrochemical aptasensor for thrombin detection based on direct electrochemistry of glucose oxidase using a functionalized graphene hybrid for amplification.

PubMed

Bai, Lijuan; Yan, Bin; Chai, Yaqin; Yuan, Ruo; Yuan, Yali; Xie, Shunbi; Jiang, Liping; He, Ying

2013-11-07

In this work, we reported a new label-free electrochemical aptasensor for highly sensitive detection of thrombin using direct electron transfer of glucose oxidase (GOD) as a redox probe and a gold nanoparticle-polyaniline-graphene (Au-PANI-Gra) hybrid for amplification. The Au-PANI-Gra hybrid with large surface area provided a biocompatible sensing platform for the immobilization of GOD. GOD was encapsulated into the three-dimensional netlike (3-mercaptopropyl)trimethoxysilane (MPTS) to form the MPTS-GOD biocomposite, which not only retained the native functions and properties, but also exhibited tunable porosity, high thermal stability, and chemical inertness. With abundant thiol tail groups on MPTS, MPTS-GOD was able to chemisorb onto the surface of the Au-PANI-Gra modified electrode through the strong affinity of the Au-S bond. The electrochemical signal originated from GOD, avoiding the addition or labeling of other redox mediators. After immobilizing the thiolated thrombin binding aptamer through gold nanoparticles (AuNPs), GOD as a blocking reagent was employed to block the remaining active sites of the AuNPs and avoid the nonspecific adsorption. The proposed method avoided the labeling process of redox probes and increased the amount of electroactive GOD. The concentration of thrombin was monitored based on the decrease of current response through cyclic voltammetry (CV) in 0.1 M PBS (pH 7.4). With the excellent direct electron transfer of double layer GOD membranes, the resulting aptasensor exhibited high sensitivity for detection of thrombin with a wide linear range from 1.0 × 10(-12) to 3.0 × 10(-8) M. The proposed aptasensor also showed good stability, satisfactory reproducibility and high specificity, which provided a promising strategy for electrochemical aptamer-based detection of other biomolecules.

Characterization of opto-electrical enhancement of tandem photoelectrochemical cells by using photoconductive-AFM

NASA Astrophysics Data System (ADS)

Park, Sun-Young; Elbersen, Rick; Huskens, Jurriaan; Gardeniers, Han; Lee, Joo-Yul; Mul, Guido; Heo, Jinhee

2017-07-01

Solar-to-hydrogen conversion by water splitting in photoelectrochemical cells (PECs) is a promising approach to alleviate problems associated with intermittency in solar energy supply and demand. Several interfacial resistances in photoelectrodes limit the performance of such cells, while the properties of interfaces are not easy to analyze in situ. We applied photoconductive-AFM to analyze the performance of WO3/p+n Si photoanodes, containing an ultra-thin metal interface of either Au or Pt. The Au interface consisted of Au nanoparticles with well-ordered interspacing, while Pt was present in the form of a continuous film. Photoconductive-AFM data show that upon illumination significantly larger currents are measured for the WO3/p+n Si anode equipped with the Au interface, as compared to the WO3/p+n Si anode with the Pt interface, in agreement with the better performance of the former electrode in a photoelectrochemical cell. The remarkable performance of the Au-containing electrode is proposed to be the result of favorable electron-hole recombination rates induced by the Au nanoparticles in a plasmon resonance excited state.

Spin resolved electronic transport through N@C20 fullerene molecule between Au electrodes: A first principles study

NASA Astrophysics Data System (ADS)

Caliskan, Serkan

2018-05-01

Using first principles study, through Density Functional Theory combined with Non Equilibrium Green's Function Formalism, electronic properties of endohedral N@C20 fullerene molecule joining Au electrodes (Au-N@C20) was addressed in the presence of spin property. The electronic transport behavior across the Au-N@C20 molecular junction was investigated by spin resolved transmission, density of states, molecular orbitals, differential conductance and current-voltage (I-V) characteristics. Spin asymmetric variation was clearly observed in the results due to single N atom encapsulated in the C20 fullerene cage, where the N atom played an essential role in the electronic behavior of Au-N@C20. This N@C20 based molecular bridge, exhibiting a spin dependent I-V variation, revealed a metallic behavior within the bias range from -1 V to 1 V. The induced magnetic moment, spin polarization and other relevant quantities associated with the spin resolved transport were elucidated.

Electrodeposition of Au/Ag bimetallic dendrites assisted by Faradaic AC-electroosmosis flow

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ji, Jianlong; Li, Pengwei; Sang, Shengbo, E-mail: sbsang@tyut.edu.cn

2014-03-15

Au/Ag bimetallic dendrites were synthesized successfully from the corresponding aqueous solution via the AC electrodeposition method. Both of the morphologies and compositions could be tuned by the electrolyte concentration and AC frequency. The prepared bimetallic dendrites were characterized by scanning electron microscopy (SEM), energy dispersive X-ray spectrometer (EDS), transmission electron microscopy (TEM) and UV–vis spectroscopy. The underlying dendrite growth mechanism was then proposed in the context of the Directed Electrochemical Nanowires Assembly (DENA) models. Owing to the unscreened voltage dropping in the electrolyte bulk, electromigration dominates the species flux process, and cations tend to accumulate in areas with strong electricmore » field intensity, such as electrode edges. Moreover, Faradaic AC-electro-osmosis (ACEO) flow could increase the effective diffusion layer thickness in these areas during the electrochemical reaction, and leads to dendrite growth. Further Micro-Raman observations illustrated that the Au/Ag bimetallic dendrites exhibited pronounced surface-enhanced Raman scattering (SERS) activity, using 4-mercaptopyridine (4-MP) as model molecules.« less

Durable electrocatalytic-activity of Pt-Au/C cathode in PEMFCs.

PubMed

Selvaganesh, S Vinod; Selvarani, G; Sridhar, P; Pitchumani, S; Shukla, A K

2011-07-21

Longevity remains as one of the central issues in the successful commercialization of polymer electrolyte membrane fuel cells (PEMFCs) and primarily hinges on the durability of the cathode. Incorporation of gold (Au) to platinum (Pt) is known to ameliorate both the electrocatalytic activity and stability of cathode in relation to pristine Pt-cathodes that are currently being used in PEMFCs. In this study, an accelerated stress test (AST) is conducted to simulate prolonged fuel-cell operating conditions by potential cycling the carbon-supported Pt-Au (Pt-Au/C) cathode. The loss in performance of PEMFC with Pt-Au/C cathode is found to be ∼10% after 7000 accelerated potential-cycles as against ∼60% for Pt/C cathode under similar conditions. These data are in conformity with the electrochemical surface-area values. PEMFC with Pt-Au/C cathode can withstand >10,000 potential cycles with very little effect on its performance. X-ray diffraction and transmission electron microscopy studies on the catalyst before and after AST suggest that incorporating Au with Pt helps mitigate aggregation of Pt particles during prolonged fuel-cell operations while X-ray photoelectron spectroscopy reflects that the metallic nature of Pt is retained in the Pt-Au catalyst during AST in comparison to Pt/C that shows a major portion of Pt to be present as oxidic platinum. Field-emission scanning electron microscopy conducted on the membrane electrode assembly before and after AST suggests that incorporating Au with Pt helps mitigating deformations in the catalyst layer. This journal is © the Owner Societies 2011

Enhanced performances of dye-sensitized solar cells based on Au-TiO2 and Ag-TiO2 plasmonic hybrid nanocomposites

NASA Astrophysics Data System (ADS)

Ran, Huili; Fan, Jiajie; Zhang, Xiaoli; Mao, Jing; Shao, Guosheng

2018-02-01

Novel double-layer films were prepared and applied to dye-sensitized solar cells (DSSCs) using commercial TiO2 nanoparticles as a bonding underlayer and noble metal (Au and Ag) nanoparticles (NP) and nanowires (NW) incorporated to hybrid TiO2 composites, consisting of 3 dimensional (3D) hierarchical microspheres, 3D hollow spheres, 2 dimensional (2D) nanosheets and commercial P25 nanoparticles, as multifunctional light scattering overlayer. The influence of Au NP, Ag NP, Au NW, and Ag NW on of microstructures of the film electrodes and the photovoltaic (PV) performances of DSSCs was investigated. The result revealed that the ranges and intensity of sunlight absorption, the photo capture ability for dye molecules of the hybrid nanocomposite film electrodes, and the photoelectric conversion efficiency (PCE) of the cells were all significantly enhanced due to the plasmonic effect of the noble metal nanostructures. All composite DSSCs with noble metal nanostructures have higher PCE than the pure TiO2 solar cell. This is attributed the improved electron transport of the noble metal nanostructures, and the improvement of light absorption because of their local surface plasmon resonance (LSPR) effect. Under optical conditions, a PCE of 5.74% was obtained in the TiO2-AgNW DSSC, representing a 25.3% enhancement compared to a reference solar cell based on pure TiO2 film (4.58%). The main reason of the advancement is the improved electron transport of AgNW, the light absorption enhancement on account of the LSPR effect of AgNW, and increased light scattering due to the incorporation of the large one dimensional AgNWs within the photo-anode.

A sensitive electrochemical impedance immunosensor for determination of malachite green and leucomalachite green in the aqueous environment.

PubMed

Zhu, Dan; Li, Qiangqiang; Pang, Xiumei; Liu, Yue; Wang, Xue; Chen, Gang

2016-08-01

Application of malachite green (MG) and leucomalachite green (LMG) in fish farm water causes an environmental problem. This study proposes for the first time a sensitive and convenient electrochemical impedance spectroscopy (EIS) method for determining MG and LMG by a bovine serum albumin-decorated gold nanocluster (BSA-AuNC)/antibody composite film-based immunosensor. In order to improve the analytical performance, the glassy carbon electrode (GCE) was modified with 1, 4-phenylenediamine to form a stable layer, and then, BSA-AuNCs were covalently bound to the GCE. An adequate quantity of the polyclonal antibody of LMG was immobilized onto the surface of the BSA-AuNCs by the chemical reaction of EDC/NHS. The sensors can respond to the specific target based on specific covalent bonding. The experimental parameters, such as the pH, incubating concentration, and time, have been investigated and optimized. The calibration curve for LMG was linear in the range of 0.1~10.0 ng/mL with the limit of detection (LOD) 0.03 ng/mL. Furthermore, the sum of MG and LMG was detected in fish farm water by MG reduction. The recovery was between 89.7 % and 99.2 % in spiked samples. The EC sensor method was also compared with the ELISA method and validated by the LC-MS/MS method, which proves its great promise as a field instrument for the rapid monitoring of MG and LMG pollution. Graphical abstract 1, 4-Phenylenediamine and BSA-AuNC/antibody-decorated glassy carbon electrodes have been used for the impedimetric detection of the sum of malachite green and leucomalachite green via specific immuno-binding.

Simultaneous electrochemical detection of dopamine and uric acid over ceria supported three dimensional gold nanoclusters

NASA Astrophysics Data System (ADS)

Palanisamy, Sivakumar

2014-12-01

CeO2 is well known for being an active material to support the growth of Au nanoclusters (Au NCs). In this work, three dimensional (3D) Au NCs were deposited on three different shaped CeO2 nanostructures such as nanoparticles (NPs), nanorod arrays (NRAs) and nanoflowers (NFs) modified Ti substrate for electrochemical simultaneous detection of dopamine (DA) and uric acid (UA). The electrodeposition of 3D Au NCs were carried out via cyclic voltammetric (CV) method at over-potential, while CeO2 nanostructures were deposited by galvanostatic constant current method under the optimized conditions. The morphology and elemental composition analysis of 3D Au NCs with CeO2 nanostructures were characterized by SEM, XRD, XPS and EDAX measurements. The electrocatalytic activity of 3D Au NCs on different CeO2 supports were thoroughly investigated by using voltammetric and amperometric techniques. According to the obtained results, CeO2 NPs supported 3D Au NCs (3D Au NCs@CeO2 NPs) displayed strong signal for DA as compared to that of CeO2 NRAs (3D Au NCs@CeO2 NRAs) and CeO2 NFs supported 3D Au NCs (3D Au NCs@CeO2 NFs). In addition, the 3D Au NCs@CeO2 NPs electrode resulted in more sensitive and simultaneous detection of DA in the presence of excess UA. Thus, the 3D Au NCs@CeO2 NPs electrode can practically be applied for the detection of DA using biological samples.

Reducing the Schottky barrier between few-layer MoTe2 and gold

NASA Astrophysics Data System (ADS)

Qi, Dianyu; Wang, Qixing; Han, Cheng; Jiang, Jizhou; Zheng, Yujie; Chen, Wei; Zhang, Wenjing; Thye Shen Wee, Andrew

2017-12-01

Schottky barriers greatly influence the performance of optoelectronic devices. Schottky barriers can be reduced by harnessing the polymorphism of 2D metal transition dichalcogenides, since both semiconducting and metallic phases exist. However, high energy, high temperature or chemicals are normally required for phase transformation, or the processes are complex. In this work, stable low-resistance contacts between few layer MoTe2 flakes and gold electrodes are achieved by a simple thermal annealing treatment at low temperature (200-400 °C). The resulting Schottky barrier height of the annealed MoTe2/Au interface is low (~23 meV). A new Raman A g mode of the 1T‧ metallic phase of MoTe2 on gold electrode is observed, indicating that the low-resistance contact is due to the phase transition of 2H-MoTe2. The gold substrate plays an important role in the transformation, and a higher gold surface roughness increases the transformation rate. With this method, the mobility and ON-state current of the MoTe2 transistor increase by ~3-4 orders of magnitude, the photocurrent of vertically stacked graphene/MoTe2/Au device increases ~300%, and the response time decreases by ~20%.

Novel p-Type Conductive Semiconductor Nanocrystalline Film as the Back Electrode for High-Performance Thin Film Solar Cells.

PubMed

Zhang, Ming-Jian; Lin, Qinxian; Yang, Xiaoyang; Mei, Zongwei; Liang, Jun; Lin, Yuan; Pan, Feng

2016-02-10

Thin film solar cells, due to the low cost, high efficiency, long-term stability, and consumer applications, have been widely applied for harvesting green energy. All of these thin film solar cells generally adopt various metal thin films as the back electrode, like Mo, Au, Ni, Ag, Al, graphite, and so forth. When they contact with p-type layer, it always produces a Schottky contact with a high contact potential barrier, which greatly affects the cell performance. In this work, we report for the first time to find an appropriate p-type conductive semiconductor film, digenite Cu9S5 nanocrystalline film, as the back electrode for CdTe solar cells as the model device. Its low sheet resistance (16.6 Ω/sq) could compare to that of the commercial TCO films (6-30 Ω/sq), like FTO, ITO, and AZO. Different from the traditonal metal back electrode, it produces a successive gradient-doping region by the controllable Cu diffusion, which greatly reduces the contact potential barrier. Remarkably, it achieved a comparable power conversion efficiency (PCE, 11.3%) with the traditional metal back electrode (Cu/Au thin films, 11.4%) in CdTe cells and a higher PCE (13.8%) with the help of the Au assistant film. We believe it could also act as the back electrode for other thin film solar cells (α-Si, CuInS2, CIGSe, CZTS, etc.), for their performance improvement.

Efficient charge injection in p-type polymer field-effect transistors with low-cost molybdenum electrodes through V2O5 interlayer.

PubMed

Baeg, Kang-Jun; Bae, Gwang-Tae; Noh, Yong-Young

2013-06-26

Here we report high-performance polymer OFETs with a low-cost Mo source/drain electrode by efficient charge injection through the formation of a thermally deposited V2O5 thin film interlayer. A thermally deposited V2O5 interlayer is formed between a regioregular poly(3-hexylthiophene) (rr-P3HT) or a p-type polymer semiconductor containing dodecyl-substituted thienylenevinylene (TV) and dodecylthiophene (PC12TV12T) and the Mo source/drain electrode. The P3HT or PC12TV12T OFETs with the bare Mo electrode exhibited lower charge carrier mobility than those with Au owing to a large barrier height for hole injection (0.5-1.0 eV). By forming the V2O5 layer, the P3HT or PC12TV12T OFETs with V2O5 on the Mo electrode exhibited charge carrier mobility comparable to that of a pristine Au electrode. Best P3HT or PC12TV12T OFETs with 5 nm thick V2O5 on Mo electrode show the charge carrier mobility of 0.12 and 0.38 cm(2)/(V s), respectively. Ultraviolet photoelectron spectroscopy results exhibited the work-function of the Mo electrode progressively changed from 4.3 to 4.9 eV with an increase in V2O5 thickness from 0 to 5 nm, respectively. Interestingly, the V2O5-deposited Mo exhibits comparable Rc to Au, which mainly results from the decreased barrier height for hole carrier injection from the low-cost metal electrode to the frontier molecular orbital of the p-type polymer semiconductor after the incorporation of the transition metal oxide hole injection layer, such as V2O5. This enables the development of large-area, low-cost electronics with the Mo electrodes and V2O5 interlayer.

Pt skin on AuCu intermetallic substrate: a strategy to maximize Pt utilization for fuel cells.

PubMed

Wang, Gongwei; Huang, Bing; Xiao, Li; Ren, Zhandong; Chen, Hao; Wang, Deli; Abruña, Héctor D; Lu, Juntao; Zhuang, Lin

2014-07-09

The dependence on Pt catalysts has been a major issue of proton-exchange membrane (PEM) fuel cells. Strategies to maximize the Pt utilization in catalysts include two main approaches: to put Pt atoms only at the catalyst surface and to further enhance the surface-specific catalytic activity (SA) of Pt. Thus far there has been no practical design that combines these two features into one single catalyst. Here we report a combined computational and experimental study on the design and implementation of Pt-skin catalysts with significantly improved SA toward the oxygen reduction reaction (ORR). Through screening, using density functional theory (DFT) calculations, a Pt-skin structure on AuCu(111) substrate, consisting of 1.5 monolayers of Pt, is found to have an appropriately weakened oxygen affinity, in comparison to that on Pt(111), which would be ideal for ORR catalysis. Such a structure is then realized by substituting the Cu atoms in three surface layers of AuCu intermetallic nanoparticles (AuCu iNPs) with Pt. The resulting Pt-skinned catalyst (denoted as Pt(S)AuCu iNPs) has been characterized in depth using synchrotron XRD, XPS, HRTEM, and HAADF-STEM/EDX, such that the Pt-skin structure is unambiguously identified. The thickness of the Pt skin was determined to be less than two atomic layers. Finally the catalytic activity of Pt(S)AuCu iNPs toward the ORR was measured via rotating disk electrode (RDE) voltammetry through which it was established that the SA was more than 2 times that of a commercial Pt/C catalyst. Taking into account the ultralow Pt loading in Pt(S)AuCu iNPs, the mass-specific catalytic activity (MA) was determined to be 0.56 A/mg(Pt)@0.9 V, a value that is well beyond the DOE 2017 target for ORR catalysts (0.44 A/mg(Pt)@0.9 V). These findings provide a strategic design and a realizable approach to high-performance and Pt-efficient catalysts for fuel cells.

Rectified tunneling current response of bio-functionalized metal-bridge-metal junctions.

PubMed

Liu, Yaqing; Offenhäusser, Andreas; Mayer, Dirk

2010-01-15

Biomolecular bridged nanostructures allow direct electrical addressing of electroactive biomolecules, which is of interest for the development of bioelectronic and biosensing hybrid junctions. In the present paper, the electroactive biomolecule microperoxidase-11 (MP-11) was integrated into metal-bridge-metal (MBM) junctions assembled from a scanning tunneling microscope (STM) setup. Before immobilization of MP-11, the Au working electrode was first modified by a self-assembled monolayer of 1-undecanethiol (UDT). A symmetric and potential independent response of current-bias voltage (I(t)/V(b)) was observed for the Au (substrate)/UDT/Au (tip) junction. However, the I(t)/V(b) characteristics became potential dependent and asymmetrical after binding of MP-11 between the electrodes of the junction. The rectification ratio of the asymmetric current response varies with gate electrode modulation. A resonant tunneling process between metal electrode and MP-11 enhances the tunneling current and is responsible for the observed rectification. Our investigations demonstrated that functional building blocks of proteins can be reassembled into new conceptual devices with operation modes deviating from their native function, which could prove highly useful in the design of future biosensors and bioelectronic devices. Copyright 2009 Elsevier B.V. All rights reserved.

Electrical Characterization of 3D Au Microelectrodes for Use in Retinal Prostheses.

PubMed

Lee, Sangmin; Ahn, Jae Hyun; Seo, Jong-Mo; Chung, Hum; Cho, Dong-Il Dan

2015-06-17

In order to provide high-quality visual information to patients who have implanted retinal prosthetic devices, the number of microelectrodes should be large. As the number of microelectrodes is increased, the dimensions of each microelectrode must be decreased, which in turn results in an increased microelectrode interface impedance and decreased injection current dynamic range. In order to improve the trade-off envelope between the number of microelectrodes and the current injection characteristics, a 3D microelectrode structure can be used as an alternative. In this paper, the electrical characteristics of 2D and 3D Au microelectrodes were investigated. In order to examine the effects of the structural difference, 2D and 3D Au microelectrodes with different base areas but similar effective surface areas were fabricated and evaluated. Interface impedances were measured and similar dynamic ranges were obtained for both 2D and 3D Au microelectrodes. These results indicate that more electrodes can be implemented in the same area if 3D designs are used. Furthermore, the 3D Au microelectrodes showed substantially enhanced electrical durability characteristics against over-injected stimulation currents, withstanding electrical currents that are much larger than the limit measured for 2D microelectrodes of similar area. This enhanced electrical durability property of 3D Au microelectrodes is a new finding in microelectrode research, and makes 3D microelectrodes very desirable devices.

Catalytic behavior of a palladium doped binder free paper based cobalt electrode in electroreduction of hydrogen peroxide

NASA Astrophysics Data System (ADS)

Zhang, Dongming; Ye, Ke; Cao, Dianxue; Yin, Jinling; Cheng, Kui; Wang, Bin; Xu, Yang; Wang, Guiling

2015-01-01

A piece of flexible and conductive A4 paper is prepared by coating a layer of graphite with a normal 8B pencil. Then, Co nano-plates and Pd are assembled by a simple electrodeposition and chemical-reduction methods on the surface of the electrified paper, respectively. The as-prepared paper substrate/graphite-Co film-Pd (PG-CoPd) electrode is characterized by scanning electron microscopy equipped with energy dispersive X-ray spectrometer, transmission electron microscope and X-ray diffractometer. The catalytic activity of the PG-CoPd electrode for H2O2 electroreduction is investigated by means of cyclic voltammetry and chronoamperometry. The preparation process of the PG-CoPd electrode does not use any binder and it exhibits a three dimensional (3D) nano structure, high stability and good electric conductivity. The mass of the Pd in PG-CoPd is about 0.0535 mg cm-2 and the reduction current density reaches to -4.30 A cm-2 mg-1 in 1 mol dm-3 NaOH and 1.4 mol dm-3 H2O2 at -0.5 V, which is higher than our previous reports of Au/Pd modified Co electrode.

Au-embedded ZnO/NiO hybrid with excellent electrochemical performance as advanced electrode materials for supercapacitor.

PubMed

Zheng, Xin; Yan, Xiaoqin; Sun, Yihui; Bai, Zhiming; Zhang, Guangjie; Shen, Yanwei; Liang, Qijie; Zhang, Yue

2015-02-04

Here we design a nanostructure by embedding Au nanoparticles into ZnO/NiO core-shell composites as supercapacitors electrodes materials. This optimized hybrid electrodes exhibited an excellent electrochemical performance including a long-term cycling stability and a maximum specific areal capacitance of 4.1 F/cm(2) at a current density of 5 mA/cm(2), which is much higher than that of ZnO/NiO hierarchical materials (0.5 F/cm(2)). Such an enhanced property is attributed to the increased electro-electrolyte interfaces, short electron diffusion pathways and good electrical conductivity. Apart from this, electrons can be temporarily trapped and accumulated at the Fermi level (EF') because of the localized schottky barrier at Au/NiO interface in charge process until fill the gap between ZnO and NiO, so that additional electrons can be released during discharge. These results demonstrate that suitable interface engineering may open up new opportunities in the development of high-performance supercapacitors.

Synthesis and Microstructural Characterization of Manganese Oxide Electrodes for Application as Electrochemical Supercapacitors

NASA Astrophysics Data System (ADS)

Babakhani, Banafsheh

The aim of this thesis work was to synthesize Mn-based oxide electrodes with high surface area structures by anodic electrodeposition for application as electrochemical capacitors. Rod-like structures provide large surface areas leading to high specific capacitances. Since templated electrosynthesis of rods is not easy to use in practical applications, it is more desirable to form rod-like structures without using any templates. In this work, Mn oxide electrodes with rod-like structures (˜1.5 µm in diameter) were synthesized from a solution of 0.01 M Mn acetate under galvanostatic control without any templates, on Au coated Si substrates. The electrochemical properties of the synthesized nanocrystalline electrodes were investigated to determine the effect of morphology, chemistry and crystal structure on the corresponding electrochemical behavior of Mn oxide electrodes. Mn oxides prepared at different current densities showed a defective antifluoritetype crystal structure. The rod-like Mn oxide electrodes synthesized at low current densities (5 mAcm.2) exhibited a high specific capacitance due to their large surface areas. Also, specific capacity retention after 250 cycles in an aqueous solution of 0.5 M Na2SO4 at 100 mVs -1 was about 78% of the initial capacity (203 Fg-1 ). To improve the electrochemical capacitive behavior of Mn oxide electrodes, a sequential approach and a one-step method were adopted to synthesize Mn oxide/PEDOT electrodes through anodic deposition on Au coated Si substrates from aqueous solutions. In the former case, free standing Mn oxide rods (about 10 µm long and less than 1.5 µm in diameter) were first synthesized, then coated by electro-polymerization of a conducting polymer (PEDOT) giving coaxial rods. The one-step, co-electrodeposition method produced agglomerated Mn oxide/PEDOT particles. The electrochemical behavior of the deposits depended on the morphology and crystal structure of the fabricated electrodes, which were affected by the composition and pH of the electrolyte, temperature, current density and polymer deposition time. Mn oxide/PEDOT coaxial core/shell rods consisted of MnO2 with an antifluorite-type structure coated with amorphous PEDOT. The Mn oxide/PEDOT coaxial core/shell electrodes prepared by the sequential method showed significantly better specific capacity and redox performance properties relative to both uncoated Mn oxide rods and co- electrodeposited Mn oxide/PEDOT electrodes. The best specific capacitance for Mn oxide/PEDOT rods produced sequentially was ˜295 F g-1 with ˜92% retention after 250 cycles in 0.5 M Na2SO4 at 100 mV s-1. To further improve the electrochemical capacitive behavior of Mn oxide electrodes, Co-doped and Fe-doped Mn oxide electrodes with a rod-like morphology and antifluorite-type crystal structure were synthesized by anodic electrodeposition, on Au coated Si substrates, from dilute solutions of Mn acetate and Co sulphate and Mn acetate and Fe chloride. Also, Mn-Co oxide/PEDOT coaxial core/shell rods were synthesized by applying a shell of PEDOT on Mn-Co oxide electrodes. Mn-Co oxide/PEDOT electrodes consisted of MnO2, with partial Co 2+ and Co3+ ion substitution for Mn4+, and amorphous PEDOT. Mn-Fe oxide electrodes consisted of MnO2, with partial Fe2+ and Fe3+ ion substitution for Mn4+. Electrochemical analysis showed that the capacitance values for all deposits increased with increasing scan rate to 100 mVs -1, and then decreased after 100 mVs-1. The Mn-Co oxide/PEDOT electrodes showed improved specific capacity and electrochemical cyclability relative to uncoated Mn-Co oxides and Mn-Fe oxides. Mn-Co oxide/PEDOT electrodes with rod-like structures had high capacitances (up to 310 Fg -1) at a scan rate of 100 mVs-1 and maintained their capacitance after 500 cycles in 0.5 M Na2SO4 (91% retention). Capacitance reduction for the deposits was mainly due to the loss of Mn ions by dissolution in the electrolyte solution. To better understand the nucleation and growth mechanisms of Mn oxide electrodes, the effects of supersaturation ratio on the morphology and crystal structure of electrodeposited Mn oxide were studied. By changing deposition parameters, including deposition current density, electrolyte composition, pH and temperature, a series of nanocrystalline Mn oxide electrodes with various morphologies (continuous coatings, rod-like structures, aggregated rods and thin sheets) and an antifluorite-type crystal structure was obtained. Mn oxide thin sheets showed instantaneous nucleation and single crystalline growth; rods had a mix of instantaneous/progressive nucleation and polycrystalline growth and continuous coatings formed by progressive nucleation and polycrystalline growth. Electrochemical analysis revealed the best capacitance behaviour obtained for Mn oxide thin sheets followed by Mn oxide rods, with dimensions on the microscale, and then continuous coatings. The highest specific capacitance (˜230 Fg-1) and capacitance retention rates (˜88%) were obtained for Mn oxide thin sheets after 250 cycles in 0.5 M Na2 SO4 at 20 mVs-1.

Graphene-gold nanoparticle composite: application as a good scaffold for construction of glucose oxidase biosensor.

PubMed

Sabury, Sina; Kazemi, Sayed Habib; Sharif, Farhad

2015-04-01

In the present work we report a facile method for fabrication of glucose oxidase immobilized on the partially reduced graphene-gold nanocomposite (PRGO-AuNPs/GOx) as a novel biosensor for determination of glucose concentration. Scanning electron microscopy (SEM) and transmission electron microscopy (TEM) were used to study the morphology of PRGO and PRGO-AuNPs. Also, fast Fourier transformation infrared spectroscopy (FTIR) and UV-Vis spectroscopy were used to confirm formation of graphene and graphene-gold composite. Then, the electrochemical behavior of PRGO-AuNPs/GOx modified electrode was studied by cyclic voltammetry (CV). Our electrochemical studies, especially chronoamperometry (CA), showed that the PRGO-AuNPs/GOx modified electrode has excellent electrocatalytic activity towards the glucose. The limit of detection and sensitivity towards glucose were estimated as 0.06μM and 15.04mAmM(-1), respectively. Copyright © 2015 Elsevier B.V. All rights reserved.

The mechanical properties of ionic polymer-metal composites

NASA Astrophysics Data System (ADS)

Park, Il-Seok; Kim, Sang-Mun; Kim, Doyeon; Kim, Kwang J.

2007-04-01

In this study, we investigated the mechanical properties of various type ionic polymer-metal composites (IPMCs) and Pt, Au, Pd, and Pt electroded ionic liquid (IL-Pt) IPMCs, by testing tensile modulus and dynamic mechanical behavior. The SEM was utilized to investigate the characteristics of the doped electroding layer, and the DSC was probed in order to look into the thermal behavior of various types of IPMCs. Au IPMCs, having a 5~7 μm doped layer and nano-sized Au particles (ca. 10 nm), showed the highest tensile strength (56 MPa) and modulus (602 MPa) in a dried condition. In a thermal behavior, Au IPMC has the highest T g (153°C) and T m (263°C) in both the DMA and DSC results. The fracture behavior of various types IPMCs followed base material's behavior, Nafion TM, which is represented as the semicrystalline polymer characteristic.

Controlling the reproducibility of Coulomb blockade phenomena for gold nanoparticles on an organic monolayer/silicon system.

PubMed

Caillard, L; Sattayaporn, S; Lamic-Humblot, A-F; Casale, S; Campbell, P; Chabal, Y J; Pluchery, O

2015-02-13

Two types of highly ordered organic layers were prepared on silicon modified with an amine termination for binding gold nanoparticles (AuNPs). These two grafted organic monolayers (GOMs), consisting of alkyl chains with seven or 11 carbon atoms, were grafted on oxide-free Si(111) surfaces as tunnel barriers between the silicon electrode and the AuNPs. Three kinds of colloidal AuNPs were prepared by reducing HAuCl4 with three different reactants: citrate (Turkevich synthesis, diameter ∼16 nm), ascorbic acid (diameter ∼9 nm), or NaBH4 (Natan synthesis, diameter ∼7 nm). Scanning tunnel spectroscopy (STS) was performed in a UHV STM at 40 K, and Coulomb blockade behaviour was observed. The reproducibility of the Coulomb behavior was analysed as a function of several chemical and physical parameters: size, crystallinity of the AuNPs, influence of surrounding surfactant molecules, and quality of the GOM/Si interface (degree of oxidation after the full processing). Samples were characterized with scanning tunneling microscope, STS, atomic force microscope, Fourier transform infrared spectroscopy, x-ray photoelectron spectroscopy (XPS), and high resolution transmission electronic microscope. We show that the reproducibility in observing Coulomb behavior can be as high as ∼80% with the Natan synthesis of AuNPs and GOMs with short alkyl chains.

Layer-by-layer assembly of gold nanoparticles and cysteamine on gold electrode for immunosensing of human chorionic gonadotropin at picogram levels.

PubMed

Roushani, Mahmoud; Valipour, Akram; Valipour, Mehdi

2016-04-01

The development of an electrochemical immunosensor for the detection of human chorionic gonadotropin (hCG) is described with a limit of detection as low as 0.3 pg mL(-1) in phosphate buffer. In this immunosensor, cysteamine (Cys) and gold nanoparticles (AuNPs) were used to immobilize an anti-hCG monoclonal antibody onto a gold electrode (GE). The structure of AuNPs has been confirmed by EDS, SEM, and TEM analysis. Due to the large specific surface area and excellent electrical conductivity of AuNPs, electron transfer was promoted and the amount of hCG antibody was enhanced significantly. A systematic study on the effects of experimental parameters such as pH, incubation time in the hCG solution and urea solution used for experiments on the binding between the immobilized antibody and hCG has been carried out. Under optimal experimental parameters, differential pulse voltammetry (DPV) signal changes of the [Fe(CN)6](3-/4-) are used to detect hCG with two broad linear ranges: 0.001 to 0.2 and 0.2 to 60.7 ng mL(-1). The LOD value proves more sensitive in comparison with previously reported methods. The prepared immunosensor showed high sensitivity and stability. In addition, the immunosensor was successfully used for the determination of hCG in human serum. Copyright © 2015 Elsevier B.V. All rights reserved.

Silicon based nanogap device for studying electrical transport phenomena in molecule-nanoparticle hybrids.

PubMed

Strobel, Sebastian; Hernández, Rocío Murcia; Hansen, Allan G; Tornow, Marc

2008-09-17

We report the fabrication and characterization of vertical nanogap electrode devices using silicon-on-insulator substrates. Using only standard silicon microelectronic process technology, nanogaps down to 26 nm electrode separation were prepared. Transmission electron microscopy cross-sectional analysis revealed the well defined material architecture of the nanogap, comprising two electrodes of dissimilar geometrical shape. This asymmetry is directly reflected in transport measurements on molecule-nanoparticle hybrid systems formed by self-assembling a monolayer of mercaptohexanol on the electrode surface and the subsequent dielectrophoretic trapping of 30 nm diameter Au nanoparticles. The observed Coulomb staircase I-V characteristic measured at T = 4.2 K is in excellent agreement with theoretical modelling, whereby junction capacitances of the order of a few 10(-18) farad and asymmetric resistances of 30 and 300 MΩ, respectively, are also supported well by our independent estimates for the formed double barrier tunnelling system. We propose our nanoelectrode system for integrating novel functional electronic devices such as molecular junctions or nanoparticle hybrids into existing silicon microelectronic process technology.

Hydroxynaphthoquinone ultrathin films obtained by diazonium electroreduction: toward design of biosensitive electroactive interfaces.

PubMed

March, Gregory; Reisberg, Steeve; Piro, Benoit; Pham, Minh-Chau; Fave, Claire; Noel, Vincent

2010-05-01

Electroactive 2-(phenylsulfanyl)-8-hydroxy-1,4-naphthoquinone has been electrodeposited via the reduction of the corresponding diazonium salt on Au electrodes. Surface characterizations by X-ray photoelectron spectroscopy (XPS) and infrared reflection-absorption spectroscopy (IRRAS) reveal that the mechanism of film deposition follows an aryl radical formation and its immobilization on the electrode surface. Electrochemical study shows that the surface coverage can be finely tuned (thickness between one and four layers) by adjusting the potential and the deposition time. By managing the potential applied when reducing diazonium in potentiostatic mode, the formed layer could mediate or not charge transfer. This is the first time that the films obtained by diazonium process are demonstrated to act as mediators in the growth process. Hence, with potentials higher than the formal potential of quinone group, very thin and homogeneous layers are obtained, whereas thicker films are formed when more cathodic potentials than that of quinone are applied. The possibility to manage the charge-transfer kinetics, the thickness, and the homogeneity of electroactive deposits is interesting in the scope of designing electrochemical transducers.

The utilization of SiNWs/AuNPs-modified indium tin oxide (ITO) in fabrication of electrochemical DNA sensor.

PubMed

Rashid, Jahwarhar Izuan Abdul; Yusof, Nor Azah; Abdullah, Jaafar; Hashim, Uda; Hajian, Reza

2014-12-01

This work describes the incorporation of SiNWs/AuNPs composite as a sensing material for DNA detection on indium tin-oxide (ITO) coated glass slide. The morphology of SiNWs/AuNPs composite as the modifier layer on ITO was studied by scanning electron microscopy (SEM) and energy dispersive X-ray spectroscopy (EDX). The morphological studies clearly showed that SiNWs were successfully decorated with 20 nm-AuNPs using self-assembly monolayer (SAM) technique. The effective surface area for SiNWs/AuNPs-modified ITO enhanced about 10 times compared with bare ITO electrode. SiNWs/AuNPs nanocomposite was further explored as a matrix for DNA probe immobilization in detection of dengue virus as a bio-sensing model to evaluate its performance in electrochemical sensors. The hybridization of complementary DNA was monitored by differential pulse voltammetry (DPV) using methylene blue (MB) as the redox indicator. The fabricated biosensor was able to discriminate significantly complementary, non-complementary and single-base mismatch oligonucleotides. The electrochemical biosensor was sensitive to target DNA related to dengue virus in the range of 9.0-178.0 ng/ml with detection limit of 3.5 ng/ml. In addition, SiNWs/AuNPs-modified ITO, regenerated up to 8 times and its stability was up to 10 weeks at 4°C in silica gel. Copyright © 2014 Elsevier B.V. All rights reserved.

Enhanced electrocatalytic activity of graphene-gold nanoparticles hybrids for peroxynitrite electrochemical detection on hemin-based electrode.

PubMed

Wang, Beibei; Ji, Xueping; Ren, Jujie; Ni, Ruixing; Wang, Lin

2017-12-01

A simple, ultrasensitive peroxynitrite anion (ONOO - ) electrochemical sensing platform was developed by immobilizing hemin on a density controllable electrochemically reduced graphene oxide-Au nanoparticles (ERGO-AuNPs) nanohybrids. The ERGO-AuNPs in situ nanohybrids were produced onto a glass carbon electrode (GCE) by one-step electrodeposition, the density of which could be easily controlled by electrodeposited time. The morphology of ERGO-AuNPs nanohybrids was characterized by a scanning electron microscope (SEM). The ERGO-AuNPs nanohybrids showed a high electrocatalytic activity for immobilized-hemin, because the nanostructures hybrids could effectively promote electron transfer rate between hemin and the electrode. Due to nanohybrids-enhanced catalytic effect for hemin, they were firstly selected for use as a highly sensitive electrochemical platform for ONOO - detection. The resulted sensor showed a high electrocatalytic activity toward ONOO - oxidation, being free from the electroactive interferents, including nitrite, nitrate, dopamine and uric acid at an applied potential of 0.7V. The sensor exhibited a high sensitivity of 123.1nAμM -1 and a lower detection limit of 0.1μM, and a wide linear range of 2.4×10 -6 to 5.5×10 -5 M, which could be attributed to the synergy between ERGO and AuNPs in hybrids. The nanohybrids in situ preparation and ONOO - detection methods would be beneficial to developing other sensing interface and have promising applications in biological molecules analysis and clinical diagnostic. Copyright © 2017 Elsevier B.V. All rights reserved.

Plasmon-induced charge separation at two-dimensional gold semishell arrays on SiO2@TiO2 colloidal crystals

NASA Astrophysics Data System (ADS)

Wu, Ling; Nishi, Hiroyasu; Tatsuma, Tetsu

2015-10-01

Photoelectrodes based on plasmonic Au semishell (or halfshell) arrays are developed. A colloidal crystal consisting of SiO2@TiO2 core-shell particles is prepared on a TiO2-coated transparent electrode. A Au semishell (or halfshell) array is deposited by sputtering or evaporation on the colloidal crystal. An electrode with the semishell (or halfshell) array exhibits negative photopotential shifts and anodic photocurrents under visible light at 500-800 nm wavelengths in an aqueous electrolyte containing an electron donor. In particular, hydroquinone and ethanol are good electron donors. The photocurrents can be explained in terms of plasmon-induced charge separation at the Au-TiO2 interface.

Plasmon-induced charge separation at two-dimensional gold semishell arrays on SiO{sub 2}@TiO{sub 2} colloidal crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Ling; Nishi, Hiroyasu; Tatsuma, Tetsu, E-mail: tatsuma@iis.u-tokyo.ac.jp

2015-10-01

Photoelectrodes based on plasmonic Au semishell (or halfshell) arrays are developed. A colloidal crystal consisting of SiO{sub 2}@TiO{sub 2} core-shell particles is prepared on a TiO{sub 2}-coated transparent electrode. A Au semishell (or halfshell) array is deposited by sputtering or evaporation on the colloidal crystal. An electrode with the semishell (or halfshell) array exhibits negative photopotential shifts and anodic photocurrents under visible light at 500-800 nm wavelengths in an aqueous electrolyte containing an electron donor. In particular, hydroquinone and ethanol are good electron donors. The photocurrents can be explained in terms of plasmon-induced charge separation at the Au-TiO{sub 2} interface.

Controlling formation of single-molecule junctions by electrochemical reduction of diazonium terminal groups.

PubMed

Hines, Thomas; Díez-Pérez, Ismael; Nakamura, Hisao; Shimazaki, Tomomi; Asai, Yoshihiro; Tao, Nongjian

2013-03-06

We report controlling the formation of single-molecule junctions by means of electrochemically reducing two axialdiazonium terminal groups on a molecule, thereby producing direct Au-C covalent bonds in situ between the molecule and gold electrodes. We report a yield enhancement in molecular junction formation as the electrochemical potential of both junction electrodes approach the reduction potential of the diazonium terminal groups. Step length analysis shows that the molecular junction is significantly more stable, and can be pulled over a longer distance than a comparable junction created with amine anchoring bonds. The stability of the junction is explained by the calculated lower binding energy associated with the direct Au-C bond compared with the Au-N bond.

Novel electrode systems for amperometric sensing: the case of titanium

NASA Astrophysics Data System (ADS)

Terzi, F.; Pigani, L.; Zanardi, C.; Zanfrognini, B.; Ruggeri, S.; Maccaferri, G.; Seeber, R.

2014-10-01

After working for years on organic materials, e.g., polythiophenes and relevant composites with metal nanoparticles, we shifted our attention to unusual metals, chosen as candidates to effective amperometric sensing on the basis of the atomic structure and crystalline properties. The present contribution aims at proposing an electrode material rarely employed in electroanalysis, namely Ti. We have experimented that the peculiar nature of Ti leads to electrochemical behavior quite different with respect to the conventional electrode materials, including those based on TiO2 (nano)particles. Our work focuses on the determination of strong oxidizing species, namely H2O2 and HClO, and noble metal ions, namely Au(III). Strong oxidizing species are commodity chemicals employed in a number of different industrial processes, in which usually high concentration levels should be monitored. The procedures proposed have been successfully applied also in complex matrices, such as detergent samples. As to Au(III) determination, it also constitutes a crucial tool in order to increase the efficiency of hydrometallurgic processes and of the recovery of precious materials from electronic waste. Ti electrodes allow the determination of dissolved Au species in the presence of other metal ions. In any cases the electrodes exhibit reproducible and repeatable electrochemical responses, even in the presence of high concentration of organic fouling species typical of bio-sorption processes.

An amplified electrochemiluminescent aptasensor using Au nanoparticles capped by 3,4,9,10-perylene tetracarboxylic acid-thiosemicarbazide functionalized C60 nanocomposites as a signal enhancement tag

NASA Astrophysics Data System (ADS)

Ma, Meng-Nan; Zhang, Xia; Zhuo, Ying; Chai, Ya-Qin; Yuan, Ruo

2015-01-01

A novel electrochemiluminescent (ECL) signal tag of Au nanoparticles capped by 3,4,9,10-perylene tetracarboxylic acid-thiosemicarbazide functionalized C60 nanocomposites (AuNPs/TSC-PTC/C60NPs) was developed for thrombin (TB) aptasensor construction based on the peroxydisulfate/oxygen (S2O82-/O2) system. For signal tag fabrication, the C60 nanoparticles (C60NPs) were prepared and then coated with 3,4,9,10-perylene tetracarboxylic acid (PTCA) by π-π stacking interactions. Afterwards, thiosemicarbazide (TSC) was linked with PTCA functionalized C60NPs via amidation for further assembling Au nanoparticles (AuNPs). Finally, detection aptamer of thrombin (TBA 2) was labeled on the ECL signal amplification tag of AuNPs/TSC-PTC/C60NPs. Herein, TSC, with the active groups of -NH2 and -SH, was selected and introduced into the ECL S2O82-/O2 system for the first time, which could not only offer the active groups of -SH to absorb AuNPs for TBA 2 anchoring but also remarkably enhance the ECL signal of the S2O82-/O2 system by the formation of TSC-PTC/C60NPs for signal amplification. Meanwhile, the sensing interface of a glassy carbon electrode (GCE) was modified by AuNPs/graphene (AuNPs/GR) nanocomposites with the large specific surface area and the active sites, followed by immobilization of thiol-terminated thrombin capture aptamer (TBA 1). With the formation of the sandwich-type structure of TBA 1, TB, and TBA 2 signal probes, a desirable enhanced ECL signal was measured in the testing buffer of an S2O82-/O2 solution for detecting TB. The aptasensor exhibited a good linear relationship for TB detection in the range of 1 × 10-5-10 nM with a detection limit of 3.3 fM.A novel electrochemiluminescent (ECL) signal tag of Au nanoparticles capped by 3,4,9,10-perylene tetracarboxylic acid-thiosemicarbazide functionalized C60 nanocomposites (AuNPs/TSC-PTC/C60NPs) was developed for thrombin (TB) aptasensor construction based on the peroxydisulfate/oxygen (S2O82-/O2) system. For signal tag fabrication, the C60 nanoparticles (C60NPs) were prepared and then coated with 3,4,9,10-perylene tetracarboxylic acid (PTCA) by π-π stacking interactions. Afterwards, thiosemicarbazide (TSC) was linked with PTCA functionalized C60NPs via amidation for further assembling Au nanoparticles (AuNPs). Finally, detection aptamer of thrombin (TBA 2) was labeled on the ECL signal amplification tag of AuNPs/TSC-PTC/C60NPs. Herein, TSC, with the active groups of -NH2 and -SH, was selected and introduced into the ECL S2O82-/O2 system for the first time, which could not only offer the active groups of -SH to absorb AuNPs for TBA 2 anchoring but also remarkably enhance the ECL signal of the S2O82-/O2 system by the formation of TSC-PTC/C60NPs for signal amplification. Meanwhile, the sensing interface of a glassy carbon electrode (GCE) was modified by AuNPs/graphene (AuNPs/GR) nanocomposites with the large specific surface area and the active sites, followed by immobilization of thiol-terminated thrombin capture aptamer (TBA 1). With the formation of the sandwich-type structure of TBA 1, TB, and TBA 2 signal probes, a desirable enhanced ECL signal was measured in the testing buffer of an S2O82-/O2 solution for detecting TB. The aptasensor exhibited a good linear relationship for TB detection in the range of 1 × 10-5-10 nM with a detection limit of 3.3 fM. Electronic supplementary information (ESI) available. See DOI: 10.1039/c4nr05918b

Freestanding Gold/Graphene-Oxide/Manganese Oxide Microsupercapacitor Displaying High Areal Energy Density.

PubMed

Morag, Ahiud; Becker, James Y; Jelinek, Raz

2017-07-10

Microsupercapacitors are touted as one of the promising "next frontiers" in energy-storage research and applications. Despite their potential, significant challenges still exist in terms of physical properties and electrochemical performance, particularly attaining high energy density, stability, ease of synthesis, and feasibility of large-scale production. We present new freestanding microporous electrodes comprising self-assembled scaffold of gold and reduced graphene oxide (rGO) nanowires coated with MnO 2 . The electrodes exhibited excellent electrochemical characteristics, particularly superior high areal capacitance. Moreover, the freestanding Au/rGO scaffold also served as the current collector, obviating the need for an additional electrode support required in most reported supercapacitors, thus enabling low volume and weight devices with a high overall device specific energy. Stacked symmetrical solid-state supercapacitors were fabricated using the Au/rGO/MnO 2 electrodes in parallel configurations showing the advantage of using freestanding electrodes in the fabrication of low-volume devices. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fabrication of three-dimensional hybrid nanostructure-embedded ITO and its application as a transparent electrode for high-efficiency solution processable organic photovoltaic devices.

PubMed

Kim, Jeong Won; Jeon, Hwan-Jin; Lee, Chang-Lyoul; Ahn, Chi Won

2017-03-02

Well-aligned, high-resolution (10 nm), three-dimensional (3D) hybrid nanostructures consisting of patterned cylinders and Au islands were fabricated on ITO substrates using an ion bombardment process and a tilted deposition process. The fabricated 3D hybrid nanostructure-embedded ITO maintained its excellent electrical and optical properties after applying a surface-structuring process. The solution processable organic photovoltaic device (SP-OPV) employing a 3D hybrid nanostructure-embedded ITO as the anode displayed a 10% enhancement in the photovoltaic performance compared to the photovoltaic device prepared using a flat ITO electrode, due to the improved charge collection (extraction and transport) efficiency as well as light absorbance by the photo-active layer.

Electrochemical Characterization of O2 Plasma Functionalized Multi-Walled Carbon Nanotube Electrode for Legionella pneumophila DNA Sensor

NASA Astrophysics Data System (ADS)

Park, Eun Jin; Lee, Jun-Yong; Hyup Kim, Jun; Kug Kim, Sun; Lee, Cheol Jin; Min, Nam Ki

2010-08-01

An electrochemical DNA sensor for Legionella pneumophila detection was constructed using O2 plasma functionalized multi-walled carbon nanotube (MWCNT) film as a working electrode (WE). The cyclic voltammetry (CV) results revealed that the electrocatalytic activity of plasma functionalized MWCNT (pf-MWCNT) significantly changed depending on O2 plasma treatment time due to some oxygen containing functional groups on the pf-MWCNT surface. Scanning electron microscope (SEM) images and X-ray photoelectron spectroscopy (XPS) spectra were also presented the changes of their surface morphologies and oxygen composition before and after plasma treatment. From a comparison study, it was found that the pf-MWCNT WEs had higher electrocatalytic activity and more capability of probe DNA immobilization: therefore, electrochemical signal changes by probe DNA immobilization and hybridization on pf-MWCNT WEs were larger than on Au WEs. The pf-MWCNT based DNA sensor was able to detect a concentration range of 10 pM-100 nM of target DNA to detect L. pneumophila.

Graphene transparent electrode for enhanced optical power and thermal stability in GaN light-emitting diodes.

PubMed

Youn, Doo-Hyeb; Yu, Young-Jun; Choi, Hongkyw; Kim, Suck-Hwan; Choi, Sung-Yool; Choi, Choon-Gi

2013-02-22

We report an improvement of the optical power and thermal stability of GaN LEDs using a chemically doped graphene transparent conducting layer (TCL) and a low-resistance contact structure. In order to obtain low contact resistance between the TCL and p-GaN surface, a patterned graphene TCL with Cr/Au electrodes is suggested. A bi-layer patterning method of a graphene TCL was utilized to prevent the graphene from peeling off the p-GaN surface. To improve the work function and the sheet resistance of graphene, CVD (chemical vapor deposition) graphene was doped by a chemical treatment using a HNO(3) solution. The effect of the contact resistance on the power degradation of LEDs at a high injection current level was investigated. In addition, the enhancement of the optical power via an increase in the current spreading and a decrease in the potential barrier of the graphene TCL was investigated.

Graphene transparent electrode for enhanced optical power and thermal stability in GaN light-emitting diodes

NASA Astrophysics Data System (ADS)

Youn, Doo-Hyeb; Yu, Young-Jun; Choi, HongKyw; Kim, Suck-Hwan; Choi, Sung-Yool; Choi, Choon-Gi

2013-02-01

We report an improvement of the optical power and thermal stability of GaN LEDs using a chemically doped graphene transparent conducting layer (TCL) and a low-resistance contact structure. In order to obtain low contact resistance between the TCL and p-GaN surface, a patterned graphene TCL with Cr/Au electrodes is suggested. A bi-layer patterning method of a graphene TCL was utilized to prevent the graphene from peeling off the p-GaN surface. To improve the work function and the sheet resistance of graphene, CVD (chemical vapor deposition) graphene was doped by a chemical treatment using a HNO3 solution. The effect of the contact resistance on the power degradation of LEDs at a high injection current level was investigated. In addition, the enhancement of the optical power via an increase in the current spreading and a decrease in the potential barrier of the graphene TCL was investigated.

An electrochemiluminescent DNA sensor based on nano-gold enhancement and ferrocene quenching.

PubMed

Yao, Wu; Wang, Lun; Wang, Haiyan; Zhang, Xiaolei; Li, Ling; Zhang, Na; Pan, Le; Xing, Nannan

2013-02-15

An electrochemiluminescent DNA (ECL-DNA) sensor based on nano-gold signal enhancement (i.e. gold nanoparticles, GNP) and ferrocene signal quenching was investigated. The Au electrode was first modified with GNPs through electrodeposition method, followed by subsequent immobilization of single-stranded probe DNA labeled with ruthenium complex. The resulting sensor produced a higher ECL signal due to its higher density of self-assembled probe DNAs on the surface. Upon the hybridization of probe DNA with complementary target DNA labeled with ferrocene, ECL intensity decreased significantly due to spatial separation of ECL label from the electrode surface. As a result, the ECL signal was simultaneously quenched by ferrocene. The effects of both nano-gold electrodeposition time and ferrocene on the performance of ECL-DNA sensor were studied in detail and possible reasons for these effects were suggested as well. The reported ECL-DNA sensor showed great sensitivity and may provide an alternative approach for DNA detection in diagnostics and gene analysis. Copyright © 2012 Elsevier B.V. All rights reserved.

Template-assisted growth of transparent plasmonic nanowire electrodes

NASA Astrophysics Data System (ADS)

Caterina Giordano, Maria; Repetto, Diego; Mennucci, Carlo; Carrara, Angelica; Buatier de Mongeot, Francesco

2016-12-01

Self-organized nanowire arrays are confined by glancing-angle Au deposition on nanopatterned glass templates prepared by ion beam sputtering. The semi-transparent 1D nanowire arrays are extended over large cm2 areas and are endowed with excellent electrical conductivity competitive with the best transparent conductive oxides (sheet resistance in the range of 5-20 Ohm sq-1). In addition, the nanowires support localized surface plasmon (LSP) resonances, which are easily tunable into the visible and near infrared spectrum and are selectively excited with incident light polarized perpendicularly to the wires. Such substrates, thus, behave as multifunctional nanoelectrodes, which combine good optoelectronic performance with dichroic plasmonic excitation. The electrical percolation process of the Au nanoelectrodes was monitored in situ during growth at glancing angle, both on flat and nanopatterned glass templates. In the first case, we observed a universal scaling of the differential percolation rate, independently of the glancing deposition angle, while deviations from the universal scaling were observed when Au was confined on nanopatterned templates. In the latter case, the pronounced shadowing effect promotes the growth of locally connected 1D Au nanosticks on the ‘illuminated’ ripple ridges, thus, introducing strong anisotropies with respect to the case of a 2D percolating network.

Redox driven conductance changes for resistive memory

NASA Astrophysics Data System (ADS)

Shoute, Lian C. T.; Pekas, Nikola; Wu, Yiliang; McCreery, Richard L.

2011-03-01

The relationship between bias-induced redox reactions and resistance switching is considered for memory devices containing TiO2 or a conducting polymer in "molecular heterojunctions" consisting of thin (2-25 nm) films of covalently bonded molecules, polymers, and oxides. Raman spectroscopy was used to monitor changes in the oxidation state of polythiophene in Au/P3HT/SiO2/Au devices, and it was possible to directly determine the formation and stability of the conducting polaron state of P3HT by applied bias pulses [P3HT = poly(3-hexyl thiophene)]. Polaron formation was strongly dependent on junction composition, particularly on the interfaces between the polymer, oxide, and electrodes. In all cases, trace water was required for polaron formation, leading to the proposal that water reduction acts as a redox counter-reaction to polymer oxidation. Polaron stability was longest for the case of a direct contact between Au and SiO2, implying that catalytic water reduction at the Au surface generated hydroxide ions which stabilized the cationic polaron. The spectroscopic information about the dependence of polaron stability on device composition will be useful for designing and monitoring resistive switching memory based on conducting polymers, with or without TiO2 present.

A new method of making ohmic contacts to p-GaN

NASA Astrophysics Data System (ADS)

Hernández-Gutierrez, C. A.; Kudriavtsev, Yu.; Mota, Esteban; Hernández, A. G.; Escobosa-Echavarría, A.; Sánchez-Resendiz, V.; Casallas-Moreno, Y. L.; López-López, M.

2016-12-01

The structural, chemical, and electrical characteristics of In+ ion-implanted Au/Ni, Au/Nb and Au/W ohmic contacts to p-GaN were investigated. After the preparation of Ni, Nb and W electrode on the surface of p-GaN, the metal/p-GaN contact interface was implanted by 30 keV In+ ions with an implantation dose of 5 × 1015 ions/cm2 at room temperature to form a thin layer of InxGa1-xN located at the metal-semiconductor interface, achieved to reduce the specific contact resistance due to the improving quantum tunneling transport trough to the structure. The characterization was carried out by high-resolution X-ray diffraction, scanning electron microscopy, Raman spectroscopy, and secondary ion mass spectrometry to investigate the formation of ternary alloy, re-crystallization by rapid thermal annealing process after In+ implantation, and the redistribution of elements. The specific contact resistance was extracted by current-voltage (I-V) curves using transmission line method; the lowest specific contact resistance of 2.5 × 10-4 Ωcm2 was achieved for Au/Ni/p-InxGa1-xN/p-GaN ohmic contacts.

Solid-state voltammetry-based electrochemical immunosensor for Escherichia coli using graphene oxide-Ag nanoparticle composites as labels.

PubMed

Jiang, Xiaochun; Chen, Kun; Wang, Jing; Shao, Kang; Fu, Tao; Shao, Feng; Lu, Donglian; Liang, Jiangong; Foda, M Frahat; Han, Heyou

2013-06-21

A new electrochemical immunosensor based on solid-state voltammetry was fabricated for the detection of Escherichia coli (E. coli) by using graphene oxide-Ag nanoparticle composites (P-GO-Ag) as labels. To construct the platform, Au nanoparticles (AuNPs) were first self-assembled on an Au electrode surface through cysteamine and served as an effective matrix for antibody (Ab) attachment. Under a sandwich-type immunoassay format, the analyte and the probe (P-GO-Ag-Ab) were successively captured onto the immunosensor. Finally, the bonded AgNPs were detected through a solid-state redox process in 0.2 M of KCl solution. Combining the advantages of the high-loading capability of graphene oxide with promoted electron-transfer rate of AuNPs, this immunosensor produced a 26.92-fold signal enhancement compared with the unamplified protocol. Under the optimal conditions, the immunosensor exhibited a wide linear dependence on the logarithm of the concentration of E. coli ranging from 50 to 1.0 × 10(6) cfu mL(-1) with a detection limit of 10 cfu mL(-1). Moreover, as a practical application, the proposed immunosensor was used to monitor E. coli in lake water with satisfactory results.

Charge injection engineering of ambipolar field-effect transistors for high-performance organic complementary circuits.

PubMed

Baeg, Kang-Jun; Kim, Juhwan; Khim, Dongyoon; Caironi, Mario; Kim, Dong-Yu; You, In-Kyu; Quinn, Jordan R; Facchetti, Antonio; Noh, Yong-Young

2011-08-01

Ambipolar π-conjugated polymers may provide inexpensive large-area manufacturing of complementary integrated circuits (CICs) without requiring micro-patterning of the individual p- and n-channel semiconductors. However, current-generation ambipolar semiconductor-based CICs suffer from higher static power consumption, low operation frequencies, and degraded noise margins compared to complementary logics based on unipolar p- and n-channel organic field-effect transistors (OFETs). Here, we demonstrate a simple methodology to control charge injection and transport in ambipolar OFETs via engineering of the electrical contacts. Solution-processed caesium (Cs) salts, as electron-injection and hole-blocking layers at the interface between semiconductors and charge injection electrodes, significantly decrease the gold (Au) work function (∼4.1 eV) compared to that of a pristine Au electrode (∼4.7 eV). By controlling the electrode surface chemistry, excellent p-channel (hole mobility ∼0.1-0.6 cm(2)/(Vs)) and n-channel (electron mobility ∼0.1-0.3 cm(2)/(Vs)) OFET characteristics with the same semiconductor are demonstrated. Most importantly, in these OFETs the counterpart charge carrier currents are highly suppressed for depletion mode operation (I(off) < 70 nA when I(on) > 0.1-0.2 mA). Thus, high-performance, truly complementary inverters (high gain >50 and high noise margin >75% of ideal value) and ring oscillators (oscillation frequency ∼12 kHz) based on a solution-processed ambipolar polymer are demonstrated.

Electron Transfer Mechanism in Gold Surface Modified with Self-Assembly Monolayers from First Principles

NASA Astrophysics Data System (ADS)

Lima, Filipe C. D. A.; Iost, Rodrigo M.; Crespilho, Frank N.; Caldas, Marília J.; Calzolari, Arrigo; Petrilli, Helena M.

2013-03-01

We report the investigation of electron tunneling mechanism of peptide ferrocenyl-glycylcystamine self-assembled monolayers (SAMs) onto Au (111) electrode surfaces. Recent experimental investigations showed that electron transfer in peptides can occur across long distances by separating the donor from the acceptor. This mechanism can be further fostered by the presence of electron donor terminations of Fc terminal units on SAMs but the charge transfer mechanism is still not clear. We study the interaction of the peptide ferrocenyl-glycylcystamine on the Au (111) from first principles calculations to evaluate the electron transfer mechanism. For this purpose, we used the Kohn Sham (KS) scheme for the Density Functional Theory (DFT) as implemented in the Quantum-ESPRESSO suit of codes, using Vandebilt ultrasoft pseudopotentials and GGA-PBE exchange correlation functional to evaluate the ground-state atomic and electronic structure of the system. The analysis of KS orbital at the Fermi Energy showed high electronic density localized in Fc molecules and the observation of a minor contribution from the solvent and counter ion. Based on the results, we infer evidences of electron tunneling mechanism from the molecule to the Au(111). We acknowledge FAPESP for grant support. Also, LCCA/USP, RICE and CENAPAD for computational resources.

Versatile plasmonic-effects at the interface of inverted perovskite solar cells.

PubMed

Shalan, Ahmed Esmail; Oshikiri, Tomoya; Sawayanagi, Hiroki; Nakamura, Keisuke; Ueno, Kosei; Sun, Quan; Wu, Hui-Ping; Diau, Eric Wei-Guang; Misawa, Hiroaki

2017-01-19

Plasmonics is a highly promising approach to enhancing the light-harvesting properties of hybrid organic/inorganic perovskite solar cells. In the present work, our cells have a p-i-n inverted planar structure. An ultrathin NiO film with two different thicknesses of 5 and 10 nm prepared by a pulsed laser deposition process on an ITO substrate with a faceted and furrowed surface enabled the formation of a continuous and compact layer of well-crystallized CH 3 NH 3 PbI 3 via an anti-solvent chlorobenzene process. The coverage mechanism of the NiO film on the ITO was clearly demonstrated through the J-V and external quantum efficiency (EQE) curves. Moreover, the results demonstrated that the gold nanoislands (Au NIs) increased the power conversion efficiency to 5.1%, almost double that of the samples without Au NIs. This result is due to the excitation of surface plasmons, which is characterized by strong scattering and enhancement of the electric field in the vicinity of the Au NIs loaded at the interface between the NiO and perovskite films. Additionally, we observed an enhancement of the EQE at wavelengths shorter than the plasmon resonance peak. In the current state, we speculate that the plasmoelectric potential effect is considered to be a good explanation of the photocurrent enhancement at the off-resonance region. Our work provides good guidance for the design and fabrication of solar-energy-related devices employing NiO electrodes and plasmonic Au NIs.

Gold Nanoclusters@Ru(bpy)₃²⁺-Layered Double Hydroxide Ultrathin Film as a Cathodic Electrochemiluminescence Resonance Energy Transfer Probe.

PubMed

Yu, Yingchang; Lu, Chao; Zhang, Meining

2015-08-04

Herein, it is the first report that a cathodic electrochemiluminescence (ECL) resonance energy transfer (ERET) system is fabricated by layer-by-layer (LBL) electrostatic assembly of CoAl layered double hydroxide (LDH) nanosheets with a mixture of blue BSA-gold nanoclusters (AuNCs) and Ru(bpy)3(2+) (denoted as AuNCs@Ru) on an Au electrode. The possible ECL mechanism indicates that the appearance of CoAl-LDH nanosheets generates a long-range stacking order of the AuNCs@Ru on an Au electrode, facilitating the occurrence of the ERET between BSA-AuNC donors and Ru(bpy)3(2+) acceptors on the as-prepared AuNCs@Ru-LDH ultrathin films (UTFs). Furthermore, it is observed that the cathodic ECL intensity can be quenched efficiently in the presence of 6-mercaptopurine (6-MP) in a linear range of 2.5-100 nM with a detection limit of 1.0 nM. On the basis of these interesting phenomena, a facile cathodic ECL sensor has successfully distinguished 6-MP from other thiol-containing compounds (e.g., cysteine and glutathione) in human serum and urine samples. The proposed sensing scheme opens a way for employing the layered UTFs as a platform for the cathodic ECL of Ru(bpy)3(2+).

An impedimetric biosensor for detection of dengue serotype at picomolar concentration based on gold nanoparticles-polyaniline hybrid composites.

PubMed

Nascimento, Helena P O; Oliveira, Maria D L; de Melo, Celso P; Silva, Gilcelia J L; Cordeiro, Marli T; Andrade, Cesar A S

2011-09-01

In this work, we describe the preparation and characterization of a novel gold nanoparticles-polyaniline hybrid composite (AuNpPANI) with SH-terminal groups that, due to its ability of immobilizing dengue serotype-specific primers 1, 2 and 3 (ST1, ST2 and ST3), can be used for the development of biosensors. Electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV) were performed. CV and EIS results demonstrated that the AuNpPANI can immobilize ST1, ST2 and ST3, forming AuNpPANI-ST complexes. Well-defined cyclic voltammograms characteristic of a diffusion-limited redox process were observed both for the bare gold electrode and after these electrodes have been modified by the adsorption of AuNpPANI or AuNpPANI-ST. The AuNpPANI-ST(1-3) systems were able to recognize the dengue serotype of different patients at picomolar concentrations. Even when small volumes and low concentrations of the analyte were used, the CV and EIS results showed unequivocal evidence of an existing interaction between dengue serotype-specific primers and their complementary genomic DNA targets. Copyright © 2011 Elsevier B.V. All rights reserved.

Evaluation of Complexation Ability Using a Sensor Electrode Chip Equipped with a Wireless Screening System

PubMed Central

Isoda, Takaaki; Urushibara, Ikuko; Sato, Hikaru; Yamauchi, Noriyoshi

2012-01-01

We fabricated an electrode chip with a structure coated by an insulation layer that contains dispersed SiO2 adsorbent particles modified by an amino-group on a source-drain electrode. Voltage changes caused by chelate molecule adsorption onto electrode surfaces and by specific cation interactions were investigated. The detection of specific cations without the presence of chelate molecules on the free electrode was also examined. By comparing both sets of results the complexation ability of the studied chelate molecules onto the electrode was evaluated. Five pairs of source-drain electrodes(×8 arrays) were fabricated on a glass substrate of 20 × 30mm in size. The individual Au/Cr (1.0/0.1μm thickness) electrodes had widths of 50 μm and an inter-electrode interval of 100μm.The fabricated source-drain electrodes were further coated with an insulation layer comprising a porous SiO2 particle modified amino-group to adsorb the chelate molecules. The electrode chip was equipped with a handy-type sensor signal analyzer that was mounted on an amplifier circuit using a Miniship™ or a system in a packaged LSI device. For electrode surfaces containing different adsorbed chelate molecules an increase in the sensor voltage depended on a combination of host-guest reactions and generally decreased in the following order:5,10,15,20-tetrakis(N-methylpyridinium-4-yl)-21H,23H-porphine, tetrakis(p-toluenesulfonate) (TMPyP)as a Cu2+chelator and Cu2+>2-nitroso-5-[N-n-propyl-N-(3-sulfopropyl)amino]phenol(nitroso-PSAP) as an Fe2+chelator and Fe2+>4,7-diphenyl-1,10-phenanthrolinedisulfonic acid, disodium salt (BPDSA) as an Fe2+chelatorand Fe2+>3-[3-(2,4-dimethylphenylcarbamoyl)-2-hydroxynaphthalene-1-yl-azo]-4-hydroxybenzenesulfonic acid, sodium salt (XB-1) as a Mg2+chelator and Mg2+>2,9-dimethyl-4,7-diphenyl-1,10-phenanthrolinedisulfonic acid, disodium salt (BCIDSA) as a Cu2+chelator and Cu2+, respectively. In contrast, for the electrode surfaces with adsorbed O,O′-bis(2-aminoethyl)ethyleneglycol-N,N,N′,N′-tetraacetic acid (GEDTA) or O,O′-bis(2-aminophenyl)ethyleneglycol-N,N,N′,N′-tetraacetic acid, tetrapotassium salt, hydrate (BAPTA) as a Ca2+chelator no increase in the detection voltage was found for all the electrode tests conducted in the presence of Ca2+.To determine the differences in electrode detection, molecular orbital (MO) calculations of the chelate molecules and surface molecular modeling of the adsorbents were carried out. In accordance with frontier orbital theory, the lowest unoccupied MO (LUMO) of the chelate molecules can accept two lone pair electrons at the highest occupied MO (HOMO) of the amino group on the model surface structure of the SiO2 particle. As a result, a good correlation was obtained between the LUMO-HOMO difference and the ion response of all the electrodes tested. Based on the results obtained, the order of adsorbed chelate molecules on adsorption particles reflects the different metal ion detection abilities of the electrode chips. PMID:22969407

Molecular dynamics simulations of the formation of 1D spin-valves from stretched Au-Co and Pt-Co nanowires

NASA Astrophysics Data System (ADS)

Cortes-Huerto, R.; Sondon, T.; Saúl, A.

2014-11-01

We have performed molecular dynamics (MD) simulations of stretched Aux-Co1 - x and Ptx-Co1 - x nanowires to investigate the formation of bimetallic monoatomic wires between two electrodes. We have considered nanowires with two concentrations x = 0.2 and 0.8, aspect ratio of 13, a cross section of 1 nm2 and a wide range of temperatures (from 10 to 400 K). For the MD simulations we have used a semi-empirical interatomic potential based on the second moment approximation (SMA) of the density of states to the tight-binding Hamiltonian. For Au-Co alloys, Au atoms tends to migrate towards the narrowed region to form almost pure Au wires. In the PtCo case the formed chains usually consist of Pt enriched alternating structures. The most striking result is probably the Au0.2-Co0.8 alloy where pure monoatomic Au chains form between two Co electrodes constituting a potential 1D spin valve. Despite the known ease with which the 5d metals (Pt, Ir, and Au) form monoatomic chains (MACS), our results show that in the presence of Co (x = 0.2), the percentage of chain formation is higher than in the Pt and Au rich cases (x = 0.8).

Low contact resistance of the MWCNTs ohmic contact to p-GaN and its application for high power LED

NASA Astrophysics Data System (ADS)

Yokogawa, Toshiya; Miyake, Syota

2017-08-01

A low contact resistance electrode for p-GaN was obtained using the metallic multi-wall carbon nanotubes (MWCNTs) as the electrode material. The work function of the metallic MWCNTs was confirmed to be 4.84 eV as large as that of Au, Pd and Ni which are generally used for the p-GaN electrode material. Consequently the specific contact resistance was obtained to be as low as 2×10-3 Ωcm2 by optimizing the GaN surface treatment using hydrochloric acid because of the large work function of the MWCNTs. We also characterized the properties of LEDs using the MWCNTs ohmic contact for p-GaN. Low operation voltage and high optical output power was successfully obtained. Threshold voltage was about 2.7 V, and optical output power was about 0.8 W for the 1×1 mm2 size LED chip.

Novel nanostructured oxygen sensor

NASA Astrophysics Data System (ADS)

Boardman, Alan James

New government regulations and industry requirements for medical oxygen sensors require the development of alternate materials and process optimization of primary sensor components. Current oxygen sensors are not compliant with the Restriction of Hazardous Substances (RoHS) Directive. This work focused on two areas. First, was finding suitable readily available materials for the sensor anodes. Second was optimizing the processing of the sensor cathode membrane for reduced delamination. Oxygen sensors were made using tin (Sn) and bismuth (Bi) electrodes, potassium hydroxide (KOH) and acetic acid (CH3COOH) electrolytes with platinum (Pt) and gold (Au) reference electrodes. Bi electrodes were fabricated by casting and pressing processes. Electrochemical characterization of the Sn and Bi electrodes was performed by Cyclic Voltammetry (CV), Electrochemical Impedance Spectroscopy (EIS) and sensing characterization per BSEN ISO 21647:2009 at various oxygen percentages, 0%, 20.9% and 100% oxygen levels with an automated test apparatus. The Sn anode with both electrolyte solutions showed good oxygen sensing properties and performance in a sensor. This system shows promise for replacement of Pb electrodes as required by the RoHS Directive. The Bi anode with Au cathode in both KOH and CH3COOH electrolytes showed acceptable performance and oxygen sensing properties. The Bi anodes fabricated by separate manufacturing methods demonstrated effectiveness for use in medical oxygen sensors. Gold thin films were prepared by magnetron sputtering on Flouroethylene Polymer (FEP) films. The FEP substrate temperature ranged from -77°C to 50°C. X-Ray Diffraction (XRD) and 4-point resistivity characterized the effects of substrate temperature to Au thin film particle size. XRD peak broadening and resistivity measurements showed a strong correlation of particle size to FEP substrate temperature. Particle size at 50°C was 594A and the -77°C particle size was 2.4 x 103A. Substrate temperature exhibited a strong correlation to adhesion of the Au thin film to the FEP. Adhesion of the Au thin film with a FEP temperature of 50°C was rated a 3B per the ASTM D3359-02 peel test standard. At FEP substrate temperature of -77°C it was rated at 1B. The morphology of the deposited Au thin films was observed using optical microscopy and Scanning Electron Microscopy (SEM).

Enhanced peroxydisulfate electrochemiluminescence for dopamine biosensing based on Au nanoparticle decorated reduced graphene oxide.

PubMed

Yan, Yuting; Liu, Qian; Wang, Kun; Jiang, Ling; Yang, Xingwang; Qian, Jing; Dong, Xiaoya; Qiu, Baijing

2013-12-07

This work reports a novel strategy to amplify the electrochemiluminescence (ECL) signal of peroxydisulfate solution based on the Au nanoparticle decorated reduced graphene oxide (Au NP-RGO), and further an ECL biosensor for sensitive and selective detection of dopamine (DA) was constructed. Due to the synergistic amplification of Au NPs and RGO, the ECL signal of peroxydisulfate solution on the Au NP-RGO modified electrode was about 5-fold enhanced compared to that of the bare electrode with the ECL onset potential positively shifted from -1.2 V to -0.9 V. More interestingly, the ECL intensity of peroxydisulfate solution increased with the increase of DA concentration, based on which an ECL biosensor for DA determination was fabricated. The as-prepared solid-state ECL DA sensor showed a wide linear response of 0.02-40 μM with a detection limit of 6.7 nM (S/N = 3). Moreover, we expect this work would open up a new field in the application of peroxydisulfate solution ECL for highly sensitive bioassays.

Tuning the Morphology of Li2O2 by Noble and 3d metals: A Planar Model Electrode Study for Li-O2 Battery.

PubMed

Yang, Yao; Liu, Wei; Wu, Nian; Wang, Xiaochen; Zhang, Tao; Chen, Linfeng; Zeng, Rui; Wang, Yingming; Lu, Juntao; Fu, Lei; Xiao, Li; Zhuang, Lin

2017-06-14

In this work, a planar model electrode method has been used to investigate the structure-activity relationship of multiple noble and 3d metal catalysts for the cathode reaction of Li-O 2 battery. The result shows that the battery performance (discharge/charge overpotential) strongly depends not only on the type of catalysts but also on the morphology of the discharge product (Li 2 O 2 ). Specifically, according to electrochemical characterization and scanning electron microscopy (SEM) observation, noble metals (Pd, Pt, Ru, Ir, and Au) show excellent battery performance (smaller discharge/charge overpotential), with wormlike Li 2 O 2 particles with size less than 200 nm on their surfaces. On the other hand, 3d metals (Fe, Co, Ni, and Mn) offered poor battery performance (larger discharge/charge overpotential), with much larger Li 2 O 2 particles (1 μm to a few microns) on their surfaces after discharging. Further research shows that a "volcano plot" is found by correlating the discharging/charging plateau voltage with the adsorption energy of LiO 2 on different metals. The metals with better battery performance and worm-like-shaped Li 2 O 2 are closer to the top of the "volcano", indicating adsorption energy of LiO 2 is one of the key characters for the catalyst to reach a good performance for the oxygen electrode of Li-O 2 battery, and it has a strong influence on the morphology of the discharge product on the electrode surface.

The low-bias conducting mechanism of single-molecule junctions constructed with methylsulfide linker groups and gold electrodes

NASA Astrophysics Data System (ADS)

Wang, Minglang; Wang, Yongfeng; Sanvito, Stefano; Hou, Shimin

2017-08-01

The atomic structure and electronic transport properties of two types of molecular junctions, in which a series of saturated and conjugated molecules are symmetrically connected to gold electrodes through methylsulfide groups, are investigated using the non-equilibrium Green's function formalism combined with density functional theory. Our calculations show that the low-bias junction conductance is determined by the electronic tunneling between the two Au-S donor-acceptor bonds formed at the molecule-electrode interfaces. For alkanes with 4, 6, and 8 carbon atoms in the chain, the Au-S bonds moderately couple with the σ-type frontier molecular orbitals of the alkane backbone and thus prefer to be coplanar with the alkane backbone in the junction. This results in an exponential decrease of the junction conductance as a function of the number of methylene groups. In contrast, the Au-S bonds couple strongly with the π-type orbitals of the 1,4'-bis(methylsulfide)benzene and 4,4'-bis(methylsulfide)biphenyl molecules and thus tend to be perpendicular to the neighboring benzene rings, leading to the rather large junction conductance. Our findings contribute to the understanding of the low-bias conducting mechanism and facilitate the design of molecular electronic devices with methylsulfide groups and gold electrodes.

InGaN light-emitting diodes with highly transparent ZnO:Ga electrodes

NASA Astrophysics Data System (ADS)

Liu, H. Y.; Li, X.; Ni, X.; Avrutin, V.; Izyumskaya, N.; Özgür, Ü.; Morkoç, H.

2010-03-01

InGaN light-emitting diodes (LEDs) utilizing ZnO layers heavily doped with Ga (GZO) as transparent p-electrodes were fabricated and their characteristics were demonstrated to be superior to those of LEDs with metal Ni/Au electrodes. Highly conductive and highly transparent GZO films were grown on p-GaN contact layers of the LED structures by plasma-assisted molecular beam epitaxy under metal-rich conditions. The c and a lattice constants of GZO were found to be close to the bulk values, indicating small lattice distortion of GZO. The as-grown GZO films showed resistivities as low as 2.2-2.9×10-4 Ω cm. Upon rapid thermal annealing at the optimum temperature of 675 °C, the resistivity decreased reaching a value of ~1.9×10-4 Ω cm. Unlike the LEDs with Ni/Au contacts, the LEDs with GZO electrodes showed no filamentation and very uniform light emission at high current densities. The peak value of the relative external quantum efficiency for the LEDs with GZO contacts has substantial improvement compared with that for the LEDs with Ni/Au contacts. Under pulsed excitation mode, GZO-LEDs withstood current densities up to 5000 A/cm2.

An electrochemical immunosensor for brain natriuretic peptide prepared with screen-printed carbon electrodes nanostructured with gold nanoparticles grafted through aryl diazonium salt chemistry.

PubMed

Serafín, V; Torrente-Rodríguez, R M; González-Cortés, A; García de Frutos, P; Sabaté, M; Campuzano, S; Yáñez-Sedeño, P; Pingarrón, J M

2018-03-01

A sensitive amperometric immunosensor has been prepared by immobilization of capture antibodies onto gold nanoparticles (AuNPs) grafted on a screen-printed carbon electrode (SPCE) through aryl diazonium salt chemistry using 4-aminothiophenol (AuNPs-S-Phe-SPCE). The immunosensor was designed for the accurate determination of clinically relevant levels of B-type natriuretic peptide (BNP) in human serum samples. The nanostructured electrochemical platform resulted in an ordered layer of AuNPs onto SPCEs which combined the advantages of high conductivity and improved stability of immobilized biomolecules. The resulting disposable immunosensor used a sandwich type immunoassay involving a peroxidase-labeled detector antibody. The amperometric transduction was carried out at -0.20V (vs the Ag pseudo-reference electrode) upon the addition of hydroquinone (HQ) as electron transfer mediator and H 2 O 2 as the enzyme substrate. The nanostructured immunosensors show a storage stability of at least 25 days, a linear range between 0.014 and 15ngmL -1 , and a LOD of 4pgmL -1 , which is 100 times lower than the established cut-off value for heart failure (HF) diagnosis. The performance of the immunosensor is advantageously compared with that provided with immunosensors prepared by grafting SPCE with p-phenylendiamine (H 2 N-Phe-SPCE) and attaching AuNPs by immersion into an AuNPs suspension or by electrochemical deposition, as well as with immunosensors constructed using commercial AuNPs-modified SPCEs. The developed immunosensor was applied to the successful analysis of human serum from heart failure (HF) patients upon just a 10-times dilution as sample treatment. Copyright © 2017 Elsevier B.V. All rights reserved.

The effect of Au nanoparticles on the strain-dependent electrical properties of CVD graphene

NASA Astrophysics Data System (ADS)

Bai, Jing; Nan, Haiyan; Qi, Han; Bing, Dan; Du, Ruxia

2018-03-01

We conducted an experimental study of the effect of Au nanoparticles (NPs) on the strain-dependent electrical properties in chemical vapor deposition grown graphene. We used 5-nm thick Au NPs as an effective cover (and doping) layer for graphene, and found that Au NPs decrease electrical resistance by two orders of magnitude. In addition, the Au NPs suppress the effect of strain on resistance because the intrinsic topological cracks and grain boundaries in graphene are filled with Au nanoparticles. This method has a big potential to advance industrial production of large-area, high-quality electronic devices and graphene-based transparent electrodes.

A MoS₂-based system for efficient immobilization of hemoglobin and biosensing applications.

PubMed

Chao, Jie; Zou, Min; Zhang, Chi; Sun, Haofan; Pan, Dun; Pei, Hao; Su, Shao; Yuwen, Lihui; Fan, Chunhai; Wang, Lianhui

2015-07-10

A novel hydrogen peroxide (H2O2) and nitric oxide (NO) biosensor was fabricated by immobilizing hemoglobin (Hb) on a gold nanoparticle-decorated MoS2 nanosheet (AuNPs@MoS2) nanocomposite film modified glass carbon electrode. The AuNPs@MoS2 nanocomposite not only made the immobilized Hb keep its native biological activity but also facilitated the electron transfer between electrode and the electroactive center of Hb due to its excellent conductivity and biocompatibility. The direct electrochemistry and bioelectrocatalytic activity of Hb were investigated by cyclic voltammetry (CV). The modified electrode showed good electrocatalytic ability toward the reduction of H2O2 and NO. Under optimal conditions, the current response was linear with the concentration of H2O2 and NO in the range from 10 to 300 μM and 10 to 1100 μM with a detection limit of 4 and 5 μM, respectively. This MoS2-based biosensor was sensitive, reproducible and stable, indicating that AuNPs@MoS2 nanocomposite maybe a promising platform to construct electrochemical sensors for chemical and biological molecules detection.

In situ study of an oxidation reaction on a Pt/C electrode by ambient pressure hard X-ray photoelectron spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Takagi, Yasumasa, E-mail: ytakagi@ims.ac.jp; Uemura, Yohei; Yokoyama, Toshihiko

2014-09-29

We have constructed an ambient pressure X-ray photoelectron spectroscopy instrument that uses hard X-ray radiation at the high-performance undulator beamline BL36XU of SPring-8. The dependence of the Au 4f peak intensity from Au foil on the ambient N{sub 2} pressure was measured. At a photon energy of 7.94 keV, the Au 4f peak intensity maintained 40% at 3000 Pa compared with that at high vacuum. We designed a polymer electrolyte fuel cell that allows us to perform X-ray photoelectron spectroscopy measurements of an electrode under working conditions. The oxidized Pt peaks were observed in the Pt 3d{sub 5/2} level of Pt nanoparticlesmore » in the cathode, and the peaks clearly depended on the applied voltage between the anode and cathode. Our apparatus can be applied as a valuable in situ tool for the investigation of the electronic states and adsorbed species of polymer electrolyte fuel cell electrode catalysts under the reaction conditions.« less

One-Pot Green Synthesis of Graphene Nanosheets Encapsulated Gold Nanoparticles for Sensitive and Selective Detection of Dopamine

PubMed Central

Thirumalraj, Balamurugan; Rajkumar, Chellakannu; Chen, Shen-Ming; Palanisamy, Selvakumar

2017-01-01

We report a simple new approach for green preparation of gallic acid supported reduced graphene oxide encapsulated gold nanoparticles (GA-RGO/AuNPs) via one-pot hydrothermal method. The as-prepared composites were successfully characterized by using Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray powder diffraction techniques (XRD), scanning electron microscope (SEM), high resolution transmission electron microscopy (HRTEM) and elemental analysis. The GA-RGO/AuNPs modified electrode behaves as a hybrid electrode material for sensitive and selective detection of dopamine (DA) in presence of ascorbic acid (AA) and uric acid (UA). The GA-RGO/AuNPs modified electrode displays an excellent electrocatalytic activity towards the oxidation of DA and exhibits a wide linear response range over the DA concentrations from 0.01–100.3 μM with a detection limit (LOD) of 2.6 nM based on S/N = 3. In addition, the proposed sensor could be applied for the determination of DA in human serum and urine samples for practical analysis. PMID:28128225

One-Pot Green Synthesis of Graphene Nanosheets Encapsulated Gold Nanoparticles for Sensitive and Selective Detection of Dopamine

NASA Astrophysics Data System (ADS)

Thirumalraj, Balamurugan; Rajkumar, Chellakannu; Chen, Shen-Ming; Palanisamy, Selvakumar

2017-01-01

We report a simple new approach for green preparation of gallic acid supported reduced graphene oxide encapsulated gold nanoparticles (GA-RGO/AuNPs) via one-pot hydrothermal method. The as-prepared composites were successfully characterized by using Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray powder diffraction techniques (XRD), scanning electron microscope (SEM), high resolution transmission electron microscopy (HRTEM) and elemental analysis. The GA-RGO/AuNPs modified electrode behaves as a hybrid electrode material for sensitive and selective detection of dopamine (DA) in presence of ascorbic acid (AA) and uric acid (UA). The GA-RGO/AuNPs modified electrode displays an excellent electrocatalytic activity towards the oxidation of DA and exhibits a wide linear response range over the DA concentrations from 0.01-100.3 μM with a detection limit (LOD) of 2.6 nM based on S/N = 3. In addition, the proposed sensor could be applied for the determination of DA in human serum and urine samples for practical analysis.

Linker Dependent Bond Rupture Force Measurements in Single-Molecule Junctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frei M.; Hybertsen M.; Aradhya S.V.

We use a modified conducting atomic force microscope to simultaneously probe the conductance of a single-molecule junction and the force required to rupture the junction formed by alkanes terminated with four different chemical link groups which vary in binding strength and mechanism to the gold electrodes. Molecular junctions with amine, methylsulfide, and diphenylphosphine terminated molecules show clear conductance signatures and rupture at a force that is significantly smaller than the measured 1.4 nN force required to rupture the single-atomic gold contact. In contrast, measurements with a thiol terminated alkane which can bind covalently to the gold electrode show conductance andmore » force features unlike those of the other molecules studied. Specifically, the strong Au-S bond can cause structural rearrangements in the electrodes, which are accompanied by substantial conductance changes. Despite the strong Au-S bond and the evidence for disruption of the Au structure, the experiments show that on average these junctions also rupture at a smaller force than that measured for pristine single-atom gold contacts.« less

Glassy carbon electrodes sequentially modified by cysteamine-capped gold nanoparticles and poly(amidoamine) dendrimers generation 4.5 for detecting uric acid in human serum without ascorbic acid interference.

PubMed

Ramírez-Segovia, A S; Banda-Alemán, J A; Gutiérrez-Granados, S; Rodríguez, A; Rodríguez, F J; Godínez, Luis A; Bustos, E; Manríquez, J

2014-02-17

Glassy carbon electrodes (GCE) were sequentially modified by cysteamine-capped gold nanoparticles (AuNp@cysteamine) and PAMAM dendrimers generation 4.5 bearing 128-COOH peripheral groups (GCE/AuNp@cysteamine/PAMAM), in order to explore their capabilities as electrochemical detectors of uric acid (UA) in human serum samples at pH 2. The results showed that concentrations of UA detected by cyclic voltammetry with GCE/AuNp@cysteamine/PAMAM were comparable (deviation <±10%; limits of detection (LOD) and quantification (LOQ) were 1.7×10(-4) and 5.8×10(-4) mg dL(-1), respectively) to those concentrations obtained using the uricase-based enzymatic-colorimetric method. It was also observed that the presence of dendrimers in the GCE/AuNp@cysteamine/PAMAM system minimizes ascorbic acid (AA) interference during UA oxidation, thus improving the electrocatalytic activity of the gold nanoparticles. Copyright © 2013 Elsevier B.V. All rights reserved.

The spin-dependent electronic transport properties of M(dcdmp)2 (M = Cu, Au, Co, Ni) molecular devices based on zigzag graphene nanoribbon electrodes

NASA Astrophysics Data System (ADS)

Li, Dongde; Wu, Di; Zhang, Xiaojiao; Zeng, Bowen; Li, Mingjun; Duan, Haiming; Yang, Bingchu; Long, Mengqiu

2018-05-01

The spin-dependent electronic transport properties of M(dcdmp)2 (M = Cu, Au, Co, Ni; dcdmp = 2,3-dicyano-5,6-dimercaptopyrazyne) molecular devices based on zigzag graphene nanoribbon (ZGNR) electrodes were investigated by density functional theory combined nonequilibrium Green's function method (DFT-NEGF). Our results show that the spin-dependent transport properties of the M(dcdmp)2 molecular devices can be controlled by the spin configurations of the ZGNR electrodes, and the central 3d-transition metal atom can introduce a larger magnetism than that of the nonferrous metal one. Moreover, the perfect spin filtering effect, negative differential resistance, rectifying effect and magnetic resistance phenomena can be observed in our proposed M(dcdmp)2 molecular devices.

Efficient room temperature hydrogen sensor based on UV-activated ZnO nano-network

NASA Astrophysics Data System (ADS)

Kumar, Mohit; Kumar, Rahul; Rajamani, Saravanan; Ranwa, Sapana; Fanetti, Mattia; Valant, Matjaz; Kumar, Mahesh

2017-09-01

Room temperature hydrogen sensors were fabricated from Au embedded ZnO nano-networks using a 30 mW GaN ultraviolet LED. The Au-decorated ZnO nano-networks were deposited on a SiO2/Si substrate by a chemical vapour deposition process. X-ray diffraction (XRD) spectrum analysis revealed a hexagonal wurtzite structure of ZnO and presence of Au. The ZnO nanoparticles were interconnected, forming nano-network structures. Au nanoparticles were uniformly distributed on ZnO surfaces, as confirmed by FESEM imaging. Interdigitated electrodes (IDEs) were fabricated on the ZnO nano-networks using optical lithography. Sensor performances were measured with and without UV illumination, at room temperate, with concentrations of hydrogen varying from 5 ppm to 1%. The sensor response was found to be ˜21.5% under UV illumination and 0% without UV at room temperature for low hydrogen concentration of 5 ppm. The UV-photoactivated mode enhanced the adsorption of photo-induced O- and O2- ions, and the d-band electron transition from the Au nanoparticles to ZnO—which increased the chemisorbed reaction between hydrogen and oxygen. The sensor response was also measured at 150 °C (without UV illumination) and found to be ˜18% at 5 ppm. Energy efficient low cost hydrogen sensors can be designed and fabricated with the combination of GaN UV LEDs and ZnO nanostructures.

Parameters for Fabricating Nano-Au Colloids through the Electric Spark Discharge Method with Micro-Electrical Discharge Machining.

PubMed

Tseng, Kuo-Hsiung; Chung, Meng-Yun; Chang, Chaur-Yang

2017-06-02

In this study, the Electric Spark Discharge Method (ESDM) was employed with micro-electrical discharge machining (m-EDM) to create an electric arc that melted two electrodes in deionized water (DW) and fabricated nano-Au colloids through pulse discharges with a controlled on-off duration (T ON -T OFF ) and a total fabrication time of 1 min. A total of six on-off settings were tested under normal experimental conditions and without the addition of any chemical substances. Ultraviolet-visible spectroscopy (UV-Vis), Zetasizer Nano measurements, and scanning electron microscopy-energy dispersive X-ray (SEM-EDX) analyses suggested that the nano-Au colloid fabricated at 10-10 µs (10 µs on, 10 µs off) had higher concentration and suspension stability than products made at other T ON -T OFF settings. The surface plasmon resonance (SPR) of the colloid was 549 nm on the first day of fabrication and stabilized at 532 nm on the third day. As the T ON -T OFF period increased, the absorbance (i.e., concentration) of all nano-Au colloids decreased. Absorbance was highest at 10-10 µs. The SPR peaks stabilized at 532 nm across all T ON -T OFF periods. The Zeta potential at 10-10 µs was -36.6 mV, indicating that no nano-Au agglomeration occurred and that the particles had high suspension stability.

Parameters for Fabricating Nano-Au Colloids through the Electric Spark Discharge Method with Micro-Electrical Discharge Machining

PubMed Central

Tseng, Kuo-Hsiung; Chung, Meng-Yun; Chang, Chaur-Yang

2017-01-01

In this study, the Electric Spark Discharge Method (ESDM) was employed with micro-electrical discharge machining (m-EDM) to create an electric arc that melted two electrodes in deionized water (DW) and fabricated nano-Au colloids through pulse discharges with a controlled on–off duration (TON–TOFF) and a total fabrication time of 1 min. A total of six on–off settings were tested under normal experimental conditions and without the addition of any chemical substances. Ultraviolet–visible spectroscopy (UV–Vis), Zetasizer Nano measurements, and scanning electron microscopy–energy dispersive X-ray (SEM–EDX) analyses suggested that the nano-Au colloid fabricated at 10–10 µs (10 µs on, 10 µs off) had higher concentration and suspension stability than products made at other TON–TOFF settings. The surface plasmon resonance (SPR) of the colloid was 549 nm on the first day of fabrication and stabilized at 532 nm on the third day. As the TON–TOFF period increased, the absorbance (i.e., concentration) of all nano-Au colloids decreased. Absorbance was highest at 10–10 µs. The SPR peaks stabilized at 532 nm across all TON–TOFF periods. The Zeta potential at 10–10 µs was −36.6 mV, indicating that no nano-Au agglomeration occurred and that the particles had high suspension stability. PMID:28574476

Ultrasensitive Label-free Electrochemical Immunosensor based on Multifunctionalized Graphene Nanocomposites for the Detection of Alpha Fetoprotein

PubMed Central

Wang, Yaoguang; Zhang, Yong; Wu, Dan; Ma, Hongmin; Pang, Xuehui; Fan, Dawei; Wei, Qin; Du, Bin

2017-01-01

In this work, a novel label-free electrochemical immunosensor was developed for the quantitative detection of alpha fetoprotein (AFP). Multifunctionalized graphene nanocomposites (TB-Au-Fe3O4-rGO) were applied to modify the electrode to achieve the amplification of electrochemical signal. TB-Au-Fe3O4-rGO includes the advantages of graphene, ferroferric oxide nanoparticles (Fe3O4 NPs), gold nanoparticles (Au NPs) and toluidine blue (TB). As a kind of redox probe, TB can produce the electrochemical signal. Graphene owns large specific surface area, high electrical conductivity and good adsorption property to load a large number of TB. Fe3O4 NPs have good electrocatalytic performance towards the redox of TB. Au NPs have good biocompatibility to capture the antibodies. Due to the good electrochemical performance of TB-Au-Fe3O4-rGO, the effective and sensitive detection of AFP was achieved by the designed electrochemical immunosensor. Under optimal conditions, the designed immunosensor exhibited a wide linear range from 1.0 × 10−5 ng/mL to 10.0 ng/mL with a low detection limit of 2.7 fg/mL for AFP. It also displayed good electrochemical performance including good reproducibility, selectivity and stability, which would provide potential applications in the clinical diagnosis of other tumor markers. PMID:28186128

Photocatalytic properties of PbS/graphene oxide/polyaniline electrode for hydrogen generation.

PubMed

Shaban, Mohamed; Rabia, Mohamed; El-Sayed, Asmaa M Abd; Ahmed, Aya; Sayed, Somaya

2017-10-26

In this work, roll-graphene oxide (Ro-GO), polyaniline (PANI) nano/microparticles, and PbS nanoparticles were prepared by modified Hammer, oxidative polymerization, and chemical bath deposition methods, respectively. These nano/microstructures were characterized, optimized, and designed to form PbS/Ro-GO/PANI nano/microcomposite. Also, the ratios of PbS and Ro-GO were optimized, and the optimized composition of the used composite was 0.4 g PANI, 0.125 g Ro-GO, and 0.075 g PbS. The band gap values for PANI, PbS, Ro-GO, and PbS/Ro-GO/PANI rocomposite were 3, 1.13, 2.86, (1.16, 2) eV, respectively. Two photoelectrode assemblies, Au/PbS/Ro-GO/PANI and PbS/Ro-GO/PANI/ITO/glass were used for the photoelectrochemical (PEC) hydrogen generation. In the first assembly 45 nm- Au layer was sputtered on the surface of a disk of PbS/Ro-GO/PANI composite. For the second assembly, a disk of PbS/Ro-GO/PANI composite was glued on ITO glass using Ag-THF paste. The lifetime efficiency values were 64.2 and 43.4% for the first and second electrode for 2 h, respectively. Finally, the incident photon-to-current conversion efficiency (IPCE) and photon-to-current efficiency (ABPE) were calculated under monochromatic illumination conditions. The optimum IPCE efficiency at 390 nm was 9.4% and 16.17%, whereas ABPE % efficiency was 1.01% and 1.75% for Au/PbS/Ro-GO/PANI and PbS/Ro-GO/PANI/ITO/glass, respectively.

Electrochemical Fabrication of Nanostructures on Porous Silicon for Biochemical Sensing Platforms.

PubMed

Ko, Euna; Hwang, Joonki; Kim, Ji Hye; Lee, Joo Heon; Lee, Sung Hwan; Tran, Van-Khue; Chung, Woo Sung; Park, Chan Ho; Choo, Jaebum; Seong, Gi Hun

2016-01-01

We present a method for the electrochemical patterning of gold nanoparticles (AuNPs) or silver nanoparticles (AgNPs) on porous silicon, and explore their applications in: (1) the quantitative analysis of hydroxylamine as a chemical sensing electrode and (2) as a highly sensitive surface-enhanced Raman spectroscopy (SERS) substrate for Rhodamine 6G. For hydroxylamine detection, AuNPs-porous silicon can enhance the electrochemical oxidation of hydroxylamine. The current changed linearly for concentrations ranging from 100 μM to 1.32 mM (R(2) = 0.995), and the detection limit was determined to be as low as 55 μM. When used as SERS substrates, these materials also showed that nanoparticles decorated on porous silicon substrates have more SERS hot spots than those decorated on crystalline silicon substrates, resulting in a larger SERS signal. Moreover, AgNPs-porous silicon provided five-times higher signal compared to AuNPs-porous silicon. From these results, we expect that nanoparticles decorated on porous silicon substrates can be used in various types of biochemical sensing platforms.

Electron scattering effects at physisorbed hydrogen molecules on break-junction electrodes and nanowires formation in hydrogen environment

NASA Astrophysics Data System (ADS)

van der Maas, M.; Vasnyov, S.; Hendriksen, B. L. M.; Shklyarevskii, O. I.; Speller, S.

2012-06-01

Physisorption of hydrogen molecules on the surface of gold and other coinage metals has been studied using distance tunneling spectroscopy. We have observed that the distance dependence of the tunnel current (resistance) displays a strong N-shaped deviation from exponential behavior. Such deviations are difficult to explain within the Tersoff-Hamann approximation. We suggest the scattering of tunneling electrons by H2 molecules as an origin for the observed effect. We have found that this phenomenon is also common for strongly adsorbed organic molecules with a single anchoring group. Pulling Au, Cu and Pt nanowires at 22 K in hydrogen environment shows that the break-junction electrodes are still connected through hydrogen-metal monoatomic chains down to very low conductance values of 10-4-10-6 G0.

Gold nanoparticles embedded electropolymerized thin film of pyrimidine derivative on glassy carbon electrode for highly sensitive detection of l-cysteine.

PubMed

Kannan, Ayyadurai; Sevvel, Ranganathan

2017-09-01

This paper demonstrates the fabrication of novel gold nanoparticles incorporated poly (4-amino-6-hydroxy-2-mercaptopyrimidine) (Nano-Au/Poly-AHMP) film modified glassy carbon electrode and it is employed for highly sensitive detection of l-cysteine (CYS). The modified electrode was characterized by scanning electron microscope (SEM), cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS). SEM images of modified electrode revealed the homogeneous distribution of gold nanoparticles on poly (4-amino-6-hydroxy-2-mercaptopyrimidine) thin film modified glassy carbon electrode. The modified electrode was successfully utilized for highly selective and sensitive determination of l-cysteine at physiological pH7.0. The present electrochemical sensor successfully resolved the voltammetric signals of ascorbic acid (AA) and l-cysteine with peak separation of 0.510V. To the best of our knowledge, this is the first report of larger peak separation between AA and CYS. Wide linear concentration ranges (2μM-500μM), low detection limit (0.020μM), an excellent reproducibility and stability are achieved for cysteine sensing with this Nano-Au/Poly-AHMP/GCE. Copyright © 2017 Elsevier B.V. All rights reserved.

Phase Boundary Propagation in Li-Alloying Battery Electrodes Revealed by Liquid-Cell Transmission Electron Microscopy

DOE PAGES

Leenheer, Andrew J.; Jungjohann, Katherine L.; Zavadil, Kevin R.; ...

2016-05-31

Battery cycle life is directly influenced by the microstructural changes occurring in the electrodes during charge and discharge cycles. In this study, we image in situ the nanoscale phase evolution in negative electrode materials for Li-ion batteries using a fully enclosed liquid cell in a transmission electron microscope (TEM) to reveal early degradation that is not evident in the charge–discharge curves. To compare the electrochemical phase transformation behavior between three model materials, thin films of amorphous Si, crystalline Al, and crystalline Au were lithiated and delithiated at controlled rates while immersed in a commercial liquid electrolyte. This method allowed formore » the direct observation of lithiation mechanisms in nanoscale negative electrodes, revealing that a simplistic model of a surface-to-interior lithiation front is insufficient. For the crystalline films, a lithiation front spread laterally from a few initial nucleation points, with continued grain nucleation along the growing interface. The intermediate lithiated phases were identified using electron diffraction, and high-resolution postmortem imaging revealed the details of the final microstructure. Lastly, our results show that electrochemically induced solid–solid phase transformations can lead to highly concentrated stresses at the laterally propagating phase boundary which should be considered for future designs of nanostructured electrodes for Li-ion batteries.« less

DNA-templated synthesis of PtAu bimetallic nanoparticle/graphene nanocomposites and their application in glucose biosensor

PubMed Central

2014-01-01

In this paper, single-stranded DNA (ss-DNA) is demonstrated to functionalize graphene (GR) and to further guide the growth of PtAu bimetallic nanoparticles (PtAuNPs) on GR with high densities and dispersion. The obtained nanocomposites (PtAuNPs/ss-DNA/GR) were characterized by transmission electron microscopy (TEM), energy-dispersive X-ray spectrometer (EDS), and electrochemical techniques. Then, an enzyme nanoassembly was prepared by self-assembling glucose oxidase (GOD) on PtAuNP/ss-DNA/GR nanocomposites (GOD/PtAuNPs/ss-DNA/GR). The nanocomposites provided a suitable microenvironment for GOD to retain its biological activity. The direct and reversible electron transfer process between the active site of GOD and the modified electrode was realized without any extra electron mediator. Thus, the prepared GOD/PtAuNP/ss-DNA/GR electrode was proposed as a biosensor for the quantification of glucose. The effects of pH, applied potential, and temperature on the performance of the biosensor were discussed in detail and were optimized. Under optimal conditions, the biosensor showed a linearity with glucose concentration in the range of 1.0 to 1,800 μM with a detection limit of 0.3 μM (S/N = 3). The results demonstrate that the developed approach provides a promising strategy to improve the sensitivity and enzyme activity of electrochemical biosensors. PMID:24572068

Gold nanoparticles-immobilized, hierarchically ordered, porous TiO2 nanotubes for biosensing of glutathione

PubMed Central

Mers, SV Sheen; Kumar, Elumalai Thambuswamy Deva; Ganesh, V

2015-01-01

Glutathione (GSH) is vital for several functions of our human body such as neutralization of free radicals and reactive oxygen compounds, maintaining the active forms of vitamin C and E, regulation of nitric oxide cycle, iron metabolism, etc. It is also an endogenous antioxidant in most of the biological reactions. Given the importance of GSH, a simple strategy is proposed in this work to develop a biosensor for quantitative detection of GSH. This particular biosensor comprises of gold nanoparticles (Au NPs)-immobilized, hierarchically ordered titanium dioxide (TiO2) porous nanotubes. Hexagonally arranged, honeycomb-like nanoporous tubular TiO2 electrodes are prepared by using a simple electrochemical anodization process by applying a constant potential of 30 V for 24 hours using ethylene glycol consisting of ammonium fluoride as an electrolytic medium. Structural morphology and crystalline nature of such TiO2 nanotubes are analyzed using field emission scanning electron microscope (FESEM) and X-ray diffraction (XRD). Interestingly, nanocomposites of TiO2 with Au NPs is prepared in an effort to alter the intrinsic properties of TiO2, especially tuning of its band gap. Au NPs are prepared by a well-known Brust and Schiffrin method and are immobilized onto TiO2 electrodes which act as a perfect electrochemical sensing platform for GSH detection. Structural characterization and analysis of these modified electrodes are performed using FESEM, XRD, and UV-visible spectroscopic studies. GSH binding events on Au NPs-immobilized porous TiO2 electrodes are monitored by electrochemical techniques, namely, cyclic voltammetry (CV) and chronoamperometry (CA). Several parameters such as sensitivity, selectivity, stability, limit of detection, etc are investigated. In addition, Au NPs dispersed in aqueous medium are also explored for naked-eye detection of GSH using UV-visible spectroscopy in order to compare the performance of the proposed sensor. Our studies clearly indicate that these materials could potentially be used for GSH sensing applications. PMID:26491318

Polyamidoamine dendrimers-capped carbon dots/Au nanocrystal nanocomposites and its application for electrochemical immunosensor.

PubMed

Gao, Qi; Han, Jingman; Ma, Zhanfang

2013-11-15

In this work, polyamidoamine dendrimers capped-carbon dots (PAMAM-CDs) were fabricated by one-step microwave assisted pyrolysis of citric acid (CA) and PAMAM, where the formation of CDs and the surface passivation were accomplished simultaneously. The obtained graphitic PAMAM-CDs, with abundant amine groups, were employed as reducing and capping agents for the formation of PAMAM-CDs/Au nanocrystal nanocomposites. The resulting nanocomposites exhibited excellent conductivity, stability and biocompatibility on the surface of electrode and were designed as an immobilized matrix for sensitive immunosensing of alpha-fetoprotein (AFP). The proposed immunosensor showed a wide linear detection range from 100 fg mL(-1) to 100 ng mL(-1). The detection limit for AFP was 0.025 pg mL(-1). Importantly, the immunosensor was evaluated for the analysis of clinical serum samples, obtaining a good correlation with enzyme-linked immunosorbent assay (ELISA). The results indicated that the immunosensor provided a possible application for the detection of AFP in clinical diagnosis. Copyright © 2013 Elsevier B.V. All rights reserved.

A host-guest-recognition-based electrochemical aptasensor for thrombin detection.

PubMed

Fan, Hao; Li, Hui; Wang, Qingjiang; He, Pingang; Fang, Yuzhi

2012-05-15

A sensitive electrochemical aptasensor for thrombin detection is presented based on the host-guest recognition technique. In this sensing protocol, a 15 based thrombin aptamer (ab. TBA) was dually labeled with a thiol at its 3' end and a 4-((4-(dimethylamino)phenyl)azo) benzoic acid (dabcyl) at its 5' end, respectively, which was previously immobilized on one Au electrode surface by AuS bond and used as the thrombin probe during the protein sensing procedure. One special electrochemical marker was prepared by modifying CdS nanoparticle with β-cyclodextrins (ab. CdS-CDs), which employed as electrochemical signal provider and would conjunct with the thrombin probe modified electrode through the host-guest recognition of CDs to dabcyl. In the absence of thrombin, the probe adopted linear structure to conjunct with CdS-CDs. In present of thrombin, the TBA bond with thrombin and transformed into its special G-quarter structure, which forced CdS-CDs into the solution. Therefore, the target-TBA binding event can be sensitively transduced via detecting the electrochemical oxidation current signal of Cd of CdS nanoparticles in the solution. Using this method, as low as 4.6 pM thrombin had been detected. Copyright © 2012 Elsevier B.V. All rights reserved.

An electrochemical sensor for homocysteine detection using gold nanoparticle incorporated reduced graphene oxide.

PubMed

Rajaram, Rajendran; Mathiyarasu, Jayaraman

2018-05-30

In this work, we report a methodology for the quantification of Homocysteine (HcySH) at neutral pH (pH-7.0) using Au nanoparticles incorporated reduced graphene oxide (AuNP/rGO/GCE) modified glassy carbon electrode. The modified electrode was characterized using SEM and XRD techniques. The electrode exhibited a typical behavior against the standard redox probe [Fe(CN) 6 ] 3-/4- and resulted in 0.06 V peak to peak potential value. The modified electrode exhibited electrocatalytic activity towards electrochemical biosensing of HcySH, which is established using voltammetric studies. HcySH oxidation peak potential is observed at 0.12 V on AuNP/rGO/GCE which is 0.7 V cathodic than bare glassy carbon electrode (0.82 V). The large peak potential shift observed is reasoned as the interaction of SH group of HcySH with the gold nanoparticles and the electrocatalytic property of reduced graphene oxide that enhances the electrochemical detection at reduced overpotential. Further, successive addition of HcySH showed a linear increment in the sensitivity within the concentration range of 2-14 mM. From an amperometric protocol, the limit of detection is found as 6.9 μM with a sensitivity of 14.8 nA/μM. From a set of cyclic voltammetric measurements, it is observed that the electrode produces a linear signal on the concentration of HcySH in the presence of hydrogen peroxide. Thus it can be concluded that the matrix can detect HcySH even in the presence of hydrogen peroxide. Copyright © 2018 Elsevier B.V. All rights reserved.

In situ TEM study of the Li-Au reaction in an electrochemical liquid cell.

PubMed

Zeng, Zhiyuan; Liang, Wen-I; Chu, Ying-Hao; Zheng, Haimei

2014-01-01

We study the lithiation of a Au electrode in an electrochemical liquid cell using transmission electron microscopy (TEM). The commercial liquid electrolyte for lithium ion batteries (1 M lithium hexafluorophosphate LiPF6 dissolved in 1 : 1 (v/v) ethylene carbonate (EC) and diethyl carbonate (DEC)) was used. Three distinct types of morphology change during the reaction, including gradual dissolution, explosive reaction and local expansion/shrinkage, are observed. It is expected that significant stress is generated from lattice expansion during lithium-gold alloy formation. There is vigorous bubble formation from electrolyte decomposition, likely due to the catalytic effect of Au, while the bubble generation is less severe with titanium electrodes. There is an increase of current in response to electron beam irradiation, and electron beam effects on the observed electrochemical reaction are discussed.