A novel method for extracting nucleic acids from dried blood spots for ultrasensitive detection of low-density Plasmodium falciparum and Plasmodium vivax infections.

PubMed

Zainabadi, Kayvan; Adams, Matthew; Han, Zay Yar; Lwin, Hnin Wai; Han, Kay Thwe; Ouattara, Amed; Thura, Si; Plowe, Christopher V; Nyunt, Myaing M

2017-09-18

Greater Mekong Subregion countries are committed to eliminating Plasmodium falciparum malaria by 2025. Current elimination interventions target infections at parasite densities that can be detected by standard microscopy or rapid diagnostic tests (RDTs). More sensitive detection methods have been developed to detect lower density "asymptomatic" infections that may represent an important transmission reservoir. These ultrasensitive polymerase chain reaction (usPCR) tests have been used to identify target populations for mass drug administration (MDA). To date, malaria usPCR tests have used either venous or capillary blood sampling, which entails complex sample collection, processing and shipping requirements. An ultrasensitive method performed on standard dried blood spots (DBS) would greatly facilitate the molecular surveillance studies needed for targeting elimination interventions. A highly sensitive method for detecting Plasmodium falciparum and P. vivax 18S ribosomal RNA from DBS was developed by empirically optimizing nucleic acid extraction conditions. The limit of detection (LoD) was determined using spiked DBS samples that were dried and stored under simulated field conditions. Further, to assess its utility for routine molecular surveillance, two cross-sectional surveys were performed in Myanmar during the wet and dry seasons. The lower LoD of the DBS-based ultrasensitive assay was 20 parasites/mL for DBS collected on Whatman 3MM filter paper and 23 parasites/mL for Whatman 903 Protein Saver cards-equivalent to 1 parasite per 50 µL DBS. This is about 5000-fold more sensitive than standard RDTs and similar to the LoD of ≤16-22 parasites/mL reported for other ultrasensitive methods based on whole blood. In two cross-sectional surveys in Myanmar, nearly identical prevalence estimates were obtained from contemporaneous DBS samples and capillary blood samples collected during the wet and dry season. The DBS-based ultrasensitive method described in this study shows equal sensitivity as previously described methods based on whole blood, both in its limit of detection and prevalence estimates in two field surveys. The reduced cost and complexity of this method will allow for the scale-up of surveillance studies to target MDA and other malaria elimination interventions, and help lead to a better understanding of the epidemiology of low-density malaria infections.

Silver nanoclusters-assisted ion-exchange reaction with CdTe quantum dots for photoelectrochemical detection of adenosine by target-triggering multiple-cycle amplification strategy.

PubMed

Zhao, Yang; Tan, Lu; Gao, Xiaoshan; Jie, Guifen; Huang, Tingyu

2018-07-01

Herein, we successfully devised a novel photoelectrochemical (PEC) platform for ultrasensitive detection of adenosine by target-triggering cascade multiple cycle amplification based on the silver nanoparticles-assisted ion-exchange reaction with CdTe quantum dots (QDs). In the presence of target adenosine, DNA s1 is released from the aptamer and then hybridizes with hairpin DNA (HP1), which could initiate the cycling cleavage process under the reaction of nicking endonuclease. Then the product (DNA b) of cycle I could act as the "DNA trigger" of cycle II to further generate a large number of DNA s1, which again go back to cycle I, thus a cascade multiple DNA cycle amplification was carried out to produce abundant DNA c. These DNA c fragments with the cytosine (C)-rich loop were captured by magnetic beads, and numerous silver nanoclusters (Ag NCs) were synthesized by AgNO 3 and sodium borohydride. The dissolved AgNCs released numerous silver ions which could induce ion exchange reaction with the CdTe QDs, thus resulting in greatly amplified change of photocurrent for target detection. The detection linear range for adenosine was 1.0 fM ~10 nM with the detection limit of 0.5 fM. The present PEC strategy combining cascade multiple DNA cycle amplification and AgNCs-induced ion-exchange reaction with QDs provides new insight into rapid, and ultrasensitive PEC detection of different biomolecules, which showed great potential for detecting trace amounts in bioanalysis and clinical biomedicine. Copyright © 2018 Elsevier B.V. All rights reserved.

Magneto-mechanical detection of nucleic acids and telomerase activity in cancer cells.

PubMed

Weizmann, Yossi; Patolsky, Fernando; Lioubashevski, Oleg; Willner, Itamar

2004-02-04

The ultra-sensitive magneto-mechanical detection of DNA, single-base-mismatches in nucleic acids, and the assay of telomerase activity are accomplished by monitoring the magnetically induced deflection of a cantilever functionalized with magnetic beads associated with the biosensing interface. The analyzed M13phi DNA hybridized with the nucleic acid-functionalized magnetic beads is replicated in the presence of dNTPs that include biotin-labeled dUTP. The resulting beads are attached to an avidin-coated cantilever, and the modified cantilever is deflected by an external magnetic field. Similarly, telomerization of nucleic acid-modified magnetic beads in the presence of dNTPs, biotin-labeled dUTP, and telomerase from cancer cell extracts and the subsequent association of the magnetic beads to the cantilever surface results in the lever deflection by an external magnetic field. M13phi DNA is sensed with a sensitivity limit of 7.1 x 10(-20) M by the magneto-mechanical detection method.

Cadmium Sulphide-Reduced Graphene Oxide-Modified Photoelectrode-Based Photoelectrochemical Sensing Platform for Copper(II) Ions

PubMed Central

Ibrahim, I; Lim, H. N; Huang, N. M; Pandikumar, A

2016-01-01

A photoelectrochemical (PEC) sensor with excellent sensitivity and detection toward copper (II) ions (Cu2+) was developed using a cadmium sulphide-reduced graphene oxide (CdS-rGO) nanocomposite on an indium tin oxide (ITO) surface, with triethanolamine (TEA) used as the sacrificial electron donor. The CdS nanoparticles were initially synthesized via the aerosol-assisted chemical vapor deposition (AACVD) method using cadmium acetate and thiourea as the precursors to Cd2+ and S2-, respectively. Graphene oxide (GO) was then dip-coated onto the CdS electrode and sintered under an argon gas flow (50 mL/min) for the reduction process. The nanostructured CdS was adhered securely to the ITO by a continuous network of rGO that also acted as an avenue to intensify the transfer of electrons from the conduction band of CdS. The photoelectrochemical results indicated that the ITO/CdS-rGO photoelectrode could facilitate broad UV-visible light absorption, which would lead to a higher and steady-state photocurrent response in the presence of TEA in 0.1 M KCl. The photocurrent decreased with an increase in the concentration of Cu2+ ions. The photoelectrode response for Cu2+ ion detection had a linear range of 0.5–120 μM, with a limit of detection (LoD) of 16 nM. The proposed PEC sensor displayed ultra-sensitivity and good selectivity toward Cu2+ ion detection. PMID:27176635

Photoelectrochemical sensitive detection of insulin based on CdS/polydopamine co-sensitized WO3 nanorod and signal amplification of carbon nanotubes@polydopamine.

PubMed

Wang, Rongyu; Ma, Hongmin; Zhang, Yong; Wang, Qi; Yang, Zhongping; Du, Bin; Wu, Dan; Wei, Qin

2017-10-15

An ultrasensitive photoelectrochemical sandwich immunosensor was designed for detection of insulin based on WO 3 /CdS/polydopamine (WO 3 /CdS/PDA) co-sensitized and PDA@carbon nanotubes (PDA@CNT) conjugates for signal amplification. The CdS nanoparticles were first deposited on the WO 3 nanorods via sequential chemical bath deposition to form the WO 3 /CdS structure to enhance photocurrent. Then equipped with PDA to form the WO 3 /CdS/PDA photosensitive structure. The PDA was used not only to reduce the toxicity of CdS but also adsorb insulin primary antibodies (Ab 1 ). Meanwhile, insulin secondary antibodies (Ab 2 ) were decorated by PDA@CNT conjugates for signal amplification and further enhance photocurrent. Different photocurrent intensities were obtained by the photoelectrochemical workstation at applied bias of 0V due to the different amount of the PDA@CNT conjugates introduced by the different concentrations of insulin. A good linear relationship was obtained between the increased photocurrent and insulin concentrations range from 0.01ngmL -1 to 50ngmL -1 . And a detection limit of 2.8pgmL -1 was obtained. The proposed sensor was applied to the determination of the insulin in human serum sample, and satisfactory results were obtained. The sensor presented good specificity, reproducibility and stability, thus it might find application in the clinical diagnosis of insulin or other biomarkers in the near future. Copyright © 2017 Elsevier B.V. All rights reserved.

Effect of annealing on the sub-bandgap, defects and trapping states of ZnO nanostructures

NASA Astrophysics Data System (ADS)

Wahyuono, Ruri Agung; Hermann-Westendorf, Felix; Dellith, Andrea; Schmidt, Christa; Dellith, Jan; Plentz, Jonathan; Schulz, Martin; Presselt, Martin; Seyring, Martin; Rettenmeyer, Markus; Dietzek, Benjamin

2017-02-01

Annealing treatment was applied to different mesoporous ZnO nanostructures prepared by wet chemical synthesis, i.e. nanoflowers (NFs), spherical aggregates (SPs), and nanorods (NRs). The sub-bandgap, defect properties as well as the trapping state characteristics after annealing were characterized spectroscopically, including ultrasensitive photothermal deflection spectroscopy (PDS), photoluminescence and photo-electrochemical methods. The comprehensive experimental analysis reveals that annealing alters both the bandgap and the sub-bandgap. The defect concentration and the density of surface traps in the ZnO nanostructures are suppressed upon annealing as deduced from photoluminescence and open-circuit voltage decay analysis. The photo-electrochemical investigations reveal that the surface traps dominate the near conduction band edge of ZnO and, hence, lead to high recombination rates when used in DSSCs. The density of bulk traps in ZnO SPs is higher than that in ZnO NFs and ZnO NRs and promote lower recombination loss between photoinjected electrons with the electrolyte-oxidized species on the surface. The highest power conversion efficiency of ZnO NFs-, ZnO SPs-, and ZnO NRs-based DSSC obtained in our system is 2.0, 4.5, and 1.8%, respectively.

Peptide-Based Photoelectrochemical Cytosensor Using a Hollow-TiO2/EG/ZnIn2S4 Cosensitized Structure for Ultrasensitive Detection of Early Apoptotic Cells and Drug Evaluation.

PubMed

Wu, Rong; Fan, Gao-Chao; Jiang, Li-Ping; Zhu, Jun-Jie

2018-02-07

The ability to rapidly detect apoptotic cells and accurately evaluate therapeutic effects is significant in cancer research. To address this target, a biocompatible, ultrasensitive photoelectrochemical (PEC) cytosensing platform was developed based on electrochemically reduced graphene (EG)/ZnIn 2 S 4 cosensitized TiO 2 coupled with specific recognition between apoptotic cells and phosphatidylserine-binding peptide (PSBP). In this strategy, the HL-60 cells were selected as a model and C005, nilotinib, and imatinib were selected as apoptosis inducers to show cytosensing performances. In particular, a TiO 2 photoactive substrate was designed as hollow spheres to enhance the PEC performance. Graphene was electrodeposited on the hollow TiO 2 -modified electrode to accelerate electron transfer and increase conductivity, followed by in situ growth of ZnIn 2 S 4 nanocrystals as photosensitizers via successive ionic layer adsorption and reaction method, forming a TiO 2 /EG/ZnIn 2 S 4 cosensitized structure that was used as a PEC matrix to immobilize PSBP for the recognition of early apoptotic cells. The detection of apoptotic cells was based on steric hindrance originating from apoptotic cell capture to induce an obvious decrease in the photocurrent signal. The ultrahigh sensitivity of the cytosensor resulted from enhanced PEC performance, bioactivity, and high binding affinity between PSBP and apoptotic cells. Compared with other assays, incorporate toxic elements were avoided, such as Cd, Ru, and Te, which ensured normal cell growth and are appropriate for cell analysis. The designed PEC cytosensor showed a low detection limit of apoptotic cells (as low as three cells), a wide linear range from 1 × 10 3 to 5 × 10 7 cells/mL, and an accurate evaluation of therapeutic effects. It also exhibited good specificity, reproducibility, and stability.

Optical nano-biosensing interface via nucleic acid amplification strategy: construction and application.

PubMed

Zhou, Hong; Liu, Jing; Xu, Jing-Juan; Zhang, Shu-Sheng; Chen, Hong-Yuan

2018-03-21

Modern optical detection technology plays a critical role in current clinical detection due to its high sensitivity and accuracy. However, higher requirements such as extremely high detection sensitivity have been put forward due to the clinical needs for the early finding and diagnosing of malignant tumors which are significant for tumor therapy. The technology of isothermal amplification with nucleic acids opens up avenues for meeting this requirement. Recent reports have shown that a nucleic acid amplification-assisted modern optical sensing interface has achieved satisfactory sensitivity and accuracy, high speed and specificity. Compared with isothermal amplification technology designed to work completely in a solution system, solid biosensing interfaces demonstrated better performances in stability and sensitivity due to their ease of separation from the reaction mixture and the better signal transduction on these optical nano-biosensing interfaces. Also the flexibility and designability during the construction of these nano-biosensing interfaces provided a promising research topic for the ultrasensitive detection of cancer diseases. In this review, we describe the construction of the burgeoning number of optical nano-biosensing interfaces assisted by a nucleic acid amplification strategy, and provide insightful views on: (1) approaches to the smart fabrication of an optical nano-biosensing interface, (2) biosensing mechanisms via the nucleic acid amplification method, (3) the newest strategies and future perspectives.

Plasmonic ELISA for the ultrasensitive detection of disease biomarkers with the naked eye

NASA Astrophysics Data System (ADS)

de La Rica, Roberto; Stevens, Molly M.

2012-12-01

In resource-constrained countries, affordable methodologies for the detection of disease biomarkers at ultralow concentrations can potentially improve the standard of living. However, current strategies for ultrasensitive detection often require sophisticated instruments that may not be available in laboratories with fewer resources. Here, we circumvent this problem by introducing a signal generation mechanism for biosensing that enables the detection of a few molecules of analyte with the naked eye. The enzyme label of an enzyme-linked immunosorbent assay (ELISA) controls the growth of gold nanoparticles and generates coloured solutions with distinct tonality when the analyte is present. Prostate specific antigen (PSA) and HIV-1 capsid antigen p24 were detected in whole serum at the ultralow concentration of 1 × 10-18 g ml-1. p24 was also detected with the naked eye in the sera of HIV-infected patients showing viral loads undetectable by a gold standard nucleic acid-based test.

Carbon nanotube-based labels for highly sensitive colorimetric and aggregation-based visual detection of nucleic acids

NASA Astrophysics Data System (ADS)

Lee, Ai Cheng; Ye, Jian-Shan; Ngin Tan, Swee; Poenar, Daniel P.; Sheu, Fwu-Shan; Kiat Heng, Chew; Meng Lim, Tit

2007-11-01

A novel carbon nanotube (CNT) derived label capable of dramatic signal amplification of nucleic acid detection and direct visual detection of target hybridization has been developed. Highly sensitive colorimetric detection of human acute lymphocytic leukemia (ALL) related oncogene sequences amplified by the novel CNT-based label was demonstrated. Atomic force microscope (AFM) images confirmed that a monolayer of horseradish peroxidase and detection probe molecules was immobilized along the carboxylated CNT carrier. The resulting CNT labels significantly enhanced the nucleic acid assay sensitivity by at least 1000 times compared to that of conventional labels used in enzyme-linked oligosorbent assay (ELOSA). An excellent detection limit of 1 × 10-12 M (60 × 10-18 mol in 60 µl) and a four-order wide dynamic range of target concentration were achieved. Hybridizations using these labels were coupled to a concentration-dependent formation of visible dark aggregates. Targets can thus be detected simply with visual inspection, eliminating the need for expensive and sophisticated detection systems. The approach holds promise for ultrasensitive and low cost visual inspection and colorimetric nucleic acid detection in point-of-care and early disease diagnostic application.

Blue-light photoelectrochemical sensor based on nickel tetra-amined phthalocyanine-graphene oxide covalent compound for ultrasensitive detection of erythromycin.

PubMed

Peng, Jinyun; Huang, Qing; Zhuge, Wenfeng; Liu, Yuxia; Zhang, Cuizong; Yang, Wei; Xiang, Gang

2018-05-30

In this study, we developed a novel photoelectrochemical (PEC) sensor for the highly sensitive detection of erythromycin by functionalising graphene oxide (GO) with nickel tetra-amined phthalocyanine (NiTAPc) through covalent bonding, which resulted in the formation of NiTAPc-Gr. The fabricated sensor showed a higher PEC efficiency under blue light, exhibiting a peak wavelength of 456 nm, as compared to that of the monomer. Further, the NiTAPc-Gr/indium tin oxide (ITO) sensor exhibited a photocurrent that was 50-fold higher than that for a GO/ITO sensor under the same conditions. Under optimal conditions, the NiTAPc-Gr PEC sensor showed a linear response for erythromycin concentrations ranging from 0.40 to 120.00 μmol L -1 , with the minimum limit for detection being 0.08 μmol L -1 . Thus, the NiTAPc-Gr sensor exhibited superior performance and excellent PEC characteristics, high stability, and good reproducibility with respect to the sensing of erythromycin. Moreover, it is convenient to use, fast, small, and cheap to produce. Hence, it should find wide use in the analysis of erythromycin in real-world applications. Copyright © 2018 Elsevier B.V. All rights reserved.

CdS quantum dots modified CuO inverse opal electrodes for ultrasensitive electrochemical and photoelectrochemical biosensor

PubMed Central

Xia, Lei; Xu, Lin; Song, Jian; Xu, Ru; Liu, Dali; Dong, Biao; Song, Hongwei

2015-01-01

The CuO inverse opal photonic crystals (IOPCs) were synthesized by the sol-gel method and modified with CdS quantum dots by successive ionic layer adsorption and reaction (SILAR). CdS QDs modified CuO IOPCs FTO electrodes of different SILAR cycles were fabricated and their electrochemical properties were studied by cyclic voltammetry (CV) and chronoamperometry (I–t). Structure and morphology of the samples were characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), high-resolution TEM (HRTEM), Energy-dispersive X-ray analysis (EDX) and X-ray diffraction pattern (XRD). The result indicated that the structure of IOPCs and loading of CdS QDs could greatly improve the electrochemical properties. Three SILAR cycles of CdS QDs sensitization was the optimum condition for preparing electrodes, it exhibited a sensitivity of 4345 μA mM-1 cm-2 to glucose with a 0.15 μM detection limit (S/N= 3) and a linear range from 0.15 μM to 0.5 mM under a working potential of +0.7 V. It also showed strong stability, good reproducibility, excellent selectivity and fast amperometric response. This work provides a promising approach for realizing excellent photoelectrochemical nonenzymatic glucose biosensor of similar composite structure. PMID:26042520

Autonomous replication of nucleic acids by polymerization/nicking enzyme/DNAzyme cascades for the amplified detection of DNA and the aptamer-cocaine complex.

PubMed

Wang, Fuan; Freage, Lina; Orbach, Ron; Willner, Itamar

2013-09-03

The progressive development of amplified DNA sensors and aptasensors using replication/nicking enzymes/DNAzyme machineries is described. The sensing platforms are based on the tailoring of a DNA template on which the recognition of the target DNA or the formation of the aptamer-substrate complex trigger on the autonomous isothermal replication/nicking processes and the displacement of a Mg(2+)-dependent DNAzyme that catalyzes the generation of a fluorophore-labeled nucleic acid acting as readout signal for the analyses. Three different DNA sensing configurations are described, where in the ultimate configuration the target sequence is incorporated into a nucleic acid blocker structure associated with the sensing template. The target-triggered isothermal autonomous replication/nicking process on the modified template results in the formation of the Mg(2+)-dependent DNAzyme tethered to a free strand consisting of the target sequence. This activates additional template units for the nucleic acid self-replication process, resulting in the ultrasensitive detection of the target DNA (detection limit 1 aM). Similarly, amplified aptamer-based sensing platforms for cocaine are developed along these concepts. The modification of the cocaine-detection template by the addition of a nucleic acid sequence that enables the autonomous secondary coupled activation of a polymerization/nicking machinery and DNAzyme generation path leads to an improved analysis of cocaine (detection limit 10 nM).

Ultrasensitive electrochemical detection of nucleic acids by template enhanced hybridization followed with rolling circle amplification.

PubMed

Ji, Hanxu; Yan, Feng; Lei, Jianping; Ju, Huangxian

2012-08-21

An ultrasensitive protocol for electrochemical detection of DNA is designed with quantum dots (QDs) as a signal tag by combining the template enhanced hybridization process (TEHP) and rolling circle amplification (RCA). Upon the recognition of the molecular beacon (MB) to target DNA, the MB hybridizes with assistants and target DNA to form a ternary ''Y-junction''. The target DNA can be dissociated from the structure under the reaction of nicking endonuclease to initiate the next hybridization process. The template enhanced MB fragments further act as the primers of the RCA reaction to produce thousands of repeated oligonucleotide sequences, which can bind with oligonucleotide functionalized QDs. The attached signal tags can be easily read out by square-wave voltammetry after dissolving with acid. Because of the cascade signal amplification and the specific TEHP and RCA reaction, this newly designed protocol provides an ultrasensitive electrochemical detection of DNA down to the attomolar level (11 aM) with a linear range of 6 orders of magnitude (from 1 × 10(-17) to 1 × 10(-11) M) and can discriminate mismatched DNA from perfect matched target DNA with high selectivity. The high sensitivity and specificity make this method a great potential for early diagnosis in gene-related diseases.

Exonuclease III-assisted cascade signal amplification strategy for label-free and ultrasensitive electrochemical detection of nucleic acids.

PubMed

Xiong, Erhu; Yan, Xiaoxia; Zhang, Xiaohua; Liu, Yunqing; Zhou, Jiawan; Chen, Jinhua

2017-01-15

In this work, a simple, signal-on and label-free electrochemical biosensor for ultrasensitive DNA detection is reported on the basis of an autocatalytic and exonuclease III (Exo III)-assisted cascade signal amplification strategy. In the presence of target DNA (T-DNA), the hybridization between the 3'-protruding DNA fragment of hairpin DNA probe (HP1) and T-DNA triggered the Exo III cleavage process, accompanied by the releasing of T-DNA and autonomous generation of new DNA fragment which was used for the successive hybridization with the another hairpin DNA (HP2) on the electrode. After the Exo III cleavage process, numerous quadruplex-forming oligomers which caged in HP2 were liberated on the electrode surface and folded into G-quadruplex-hemin complexes with the help of K + and hemin to give a remarkable electrochemical response. As a result, a low detection limit of 4.83fM with an excellent selectivity toward T-DNA was achieved. The developed electrochemical biosensor should be further extended for the detection of a wide spectrum of analytes and has great potential for the development of ultrasensitive biosensing platform for early diagnosis in gene-related diseases. Copyright © 2016 Elsevier B.V. All rights reserved.

High-volume extraction of nucleic acids by magnetic bead technology for ultrasensitive detection of bacteria in blood components.

PubMed

Störmer, Melanie; Kleesiek, Knut; Dreier, Jens

2007-01-01

Nucleic acid isolation, the most technically demanding and laborious procedure performed in molecular diagnostics, harbors the potential for improvements in automation. A recent development is the use of magnetic beads covered with nucleic acid-binding matrices. We adapted this technology with a broad-range 23S rRNA real-time reverse transcription (RT)-PCR assay for fast and sensitive detection of bacterial contamination of blood products. We investigated different protocols for an automated high-volume extraction method based on magnetic-separation technology for the extraction of bacterial nucleic acids from platelet concentrates (PCs). We added 2 model bacteria, Staphylococcus epidermidis and Escherichia coli, to a single pool of apheresis-derived, single-donor platelets and assayed the PCs by real-time RT-PCR analysis with an improved primer-probe system and locked nucleic acid technology. Co-amplification of human beta(2)-microglobulin mRNA served as an internal control (IC). We used probit analysis to calculate the minimum concentration of bacteria that would be detected with 95% confidence. For automated magnetic bead-based extraction technology with the real-time RT-PCR, the 95% detection limit was 29 x 10(3) colony-forming units (CFU)/L for S. epidermidis and 22 x 10(3) CFU/L for E. coli. No false-positive results occurred, either due to nucleic acid contamination of reagents or externally during testing of 1030 PCs. High-volume nucleic acid extraction improved the detection limit of the assay. The improvement of the primer-probe system and the integration of an IC make the RT-PCR assay appropriate for bacteria screening of platelets.

A novel nonenzymatic cascade amplification for ultrasensitive photoelectrochemical DNA sensing based on target driven to initiate cyclic assembly of hairpins.

PubMed

Wen, Guangming; Dong, Wenxia; Liu, Bin; Li, Zhongping; Fan, Lifang

2018-05-29

A novel cascade photoelectrochemical (PEC) signal amplification biosensing tactics was developed for DNA detection based on a target-driven DNA association to induce cyclic hairpin assembly. In the circulatory system there are two ssDNA (A and B) and two hairpins (C and D). The hybridization of these ssDNA led to the formation of an A-target-B structure. The close proximity of their toehold and branch-migration regions was able to induce the cyclic hairpin assembly. Afterwards, the assembly result further causes the separation of a double-stranded probe DNA (Q:F) to switch the PEC signal via toehold-mediated strand replacement. As such, the signal stranded DNA-CdS QDs (F) as the signal tag was released in the presence of the target DNA. The signal DNA-CdS QDs was then coated to F-doped tin oxide (FTO) electrode leading to the "signal-on" PEC signal. The designed biosensing strategy showed a low detection limit of 21.3 pM for target DNA and a broad linear range from 50 pM to 100 nM. This signal amplification PEC sensing method exhibited a potential application to detect protein molecules, RNA or metal ions via changing the sequence of A and B recognition. Copyright © 2018 Elsevier B.V. All rights reserved.

Electrochemical detection of leukemia oncogenes using enzyme-loaded carbon nanotube labels

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

Lee, Ai Cheng; Du, Dan; Chen, Baowei

2014-09-07

Here we describe an ultrasensitive electrochemical nucleic acids assay amplified by carbon nanotubes (CNTs)-based labels for the detection of human acute lymphocytic leukemia (ALL) related p185 BCR-ABL fusion transcript. The carboxylated CNTs were functionalized with horseradish peroxidase (HRP) molecules and target-specific detection probes (DP) via diimide-activated amidation, and used to label and amplify target hybridization signal. The activity of captured HRP was monitored by square-wave voltammetry measuring the electroactive enzymatic product in the presence of 2-aminophenol and hydrogen peroxide substrate solution. The effect of DP and HRP loading of the CNT-based labels on its signal-to-noise ratio of electrochemical detection wasmore » studied systematically for the first time. Under optimized conditions, the signal-amplified assay achieved a detection limit of 83 fM targets oligonuecleotides and a 4-order wide dynamic range of target concentration. The resulting assay allowed a robust discrimination between the perfect match and a three-base mismatch sequence. When subjected to full-length (491 bp) DNA oncogene, the approach demonstrated a detection limit of approximately 33 pg of the target gene. The high sensitivity and specificity of assay enabled PCR-free detection of target transcripts in as little as 65 ng of mRNA extracted from positive ALL cell lines SUP-B15, in comparison to those obtained from negative cell lines HL-60. The approach holds promise for simple, low cost and ultrasensitive electrochemical nucleic acids detection in portable devices, point-of-care and early disease diagnostic applications.« less

Ultrasensitive detection of nucleic acids and proteins using quartz crystal microbalance and surface plasmon resonance sensors based on target-triggering multiple signal amplification strategy.

PubMed

Sun, Wenbo; Song, Weiling; Guo, Xiaoyan; Wang, Zonghua

2017-07-25

In this study, quartz crystal microbalance (QCM) and surface plasmon resonance (SPR) sensors were combined with template enhanced hybridization processes (TEHP), rolling circle amplification (RCA) and biocatalytic precipitation (BCP) for ultrasensitive detection of DNA and protein. The DNA complementary to the aptamer was released by the specific binding of the aptamer to the target protein and then hybridized with the capture probe and the assistant DNA to form a ternary "Y" junction structure. The initiation chain was generated by the template-enhanced hybridization process which leaded to the rolling circle amplification reaction, and a large number of repeating unit sequences were formed. Hybridized with the enzyme-labeled probes, the biocatalytic precipitation reaction was further carried out, resulting in a large amount of insoluble precipitates and amplifying the detection signal. Under the optimum conditions, detection limits as low as 43 aM for target DNA and 53 aM for lysozyme were achieved. In addition, this method also showed good selectivity and sensitivity in human serum. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrasensitive Direct Quantification of Nucleobase Modifications in DNA by Surface-Enhanced Raman Scattering: The Case of Cytosine.

PubMed

Morla-Folch, Judit; Xie, Hai-nan; Gisbert-Quilis, Patricia; Gómez-de Pedro, Sara; Pazos-Perez, Nicolas; Alvarez-Puebla, Ramon A; Guerrini, Luca

2015-11-09

Recognition of chemical modifications in canonical nucleobases of nucleic acids is of key importance since such modified variants act as different genetic encoders, introducing variability in the biological information contained in DNA. Herein, we demonstrate the feasibility of direct SERS in combination with chemometrics and microfluidics for the identification and relative quantification of 4 different cytosine modifications in both single- and double-stranded DNA. The minute amount of DNA required per measurement, in the sub-nanogram regime, removes the necessity of pre-amplification or enrichment steps (which are also potential sources of artificial DNA damages). These findings show great potentials for the development of fast, low-cost and high-throughput screening analytical devices capable of detecting known and unknown modifications in nucleic acids (DNA and RNA) opening new windows of activity in several fields such as biology, medicine and forensic sciences. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Reading Out Single-Molecule Digital RNA and DNA Isothermal Amplification in Nanoliter Volumes with Unmodified Camera Phones

PubMed Central

2016-01-01

Digital single-molecule technologies are expanding diagnostic capabilities, enabling the ultrasensitive quantification of targets, such as viral load in HIV and hepatitis C infections, by directly counting single molecules. Replacing fluorescent readout with a robust visual readout that can be captured by any unmodified cell phone camera will facilitate the global distribution of diagnostic tests, including in limited-resource settings where the need is greatest. This paper describes a methodology for developing a visual readout system for digital single-molecule amplification of RNA and DNA by (i) selecting colorimetric amplification-indicator dyes that are compatible with the spectral sensitivity of standard mobile phones, and (ii) identifying an optimal ratiometric image-process for a selected dye to achieve a readout that is robust to lighting conditions and camera hardware and provides unambiguous quantitative results, even for colorblind users. We also include an analysis of the limitations of this methodology, and provide a microfluidic approach that can be applied to expand dynamic range and improve reaction performance, allowing ultrasensitive, quantitative measurements at volumes as low as 5 nL. We validate this methodology using SlipChip-based digital single-molecule isothermal amplification with λDNA as a model and hepatitis C viral RNA as a clinically relevant target. The innovative combination of isothermal amplification chemistry in the presence of a judiciously chosen indicator dye and ratiometric image processing with SlipChip technology allowed the sequence-specific visual readout of single nucleic acid molecules in nanoliter volumes with an unmodified cell phone camera. When paired with devices that integrate sample preparation and nucleic acid amplification, this hardware-agnostic approach will increase the affordability and the distribution of quantitative diagnostic and environmental tests. PMID:26900709

Ultrasensitive HIV-1 p24 Assay Detects Single Infected Cells and Differences in Reservoir Induction by Latency Reversal Agents.

PubMed

Passaes, Caroline Pereira Bittencourt; Bruel, Timothée; Decalf, Jérémie; David, Annie; Angin, Mathieu; Monceaux, Valerie; Muller-Trutwin, Michaela; Noel, Nicolas; Bourdic, Katia; Lambotte, Olivier; Albert, Matthew L; Duffy, Darragh; Schwartz, Olivier; Sáez-Cirión, Asier

2017-03-15

The existence of HIV reservoirs in infected individuals under combined antiretroviral therapy (cART) represents a major obstacle toward cure. Viral reservoirs are assessed by quantification of HIV nucleic acids, a method which does not discriminate between infectious and defective viruses, or by viral outgrowth assays, which require large numbers of cells and long-term cultures. Here, we used an ultrasensitive p24 digital assay, which we report to be 1,000-fold more sensitive than classical enzyme-linked immunosorbent assays (ELISAs) in the quantification of HIV-1 Gag p24 production in samples from HIV-infected individuals. Results from ultrasensitive p24 assays were compared to those from conventional viral RNA reverse transcription-quantitative PCR (RT-qPCR)-based assays and from outgrowth assay readout by flow cytometry. Using serial dilutions and flow-based single-cell sorting, we show that viral proteins produced by a single infected cell can be detected by the ultrasensitive p24 assay. This unique sensitivity allowed the early (as soon as day 1 in 43% of cases) and more efficient detection and quantification of p24 in phytohemagglutinin-L (PHA)-stimulated CD4 + T cells from individuals under effective cART. When seven different classes of latency reversal agents (LRA) in resting CD4 + T cells from HIV-infected individuals were tested, the ultrasensitive p24 assay revealed differences in the extent of HIV reactivation. Of note, HIV RNA production was infrequently accompanied by p24 protein production (19%). Among the drugs tested, prostratin showed a superior capacity in inducing viral protein production. In summary, the ultrasensitive p24 assay allows the detection and quantification of p24 produced by single infected CD4 + T cells and provides a unique tool to assess early reactivation of infectious virus from reservoirs in HIV-infected individuals. IMPORTANCE The persistence of HIV reservoirs in infected individuals under effective antiretroviral treatment represents a major obstacle toward cure. Different methods to estimate HIV reservoirs exist, but there is currently no optimal assay to measure HIV reservoirs in HIV eradication interventions. In the present study, we report an ultrasensitive digital ELISA platform for quantification of the HIV-1 protein p24. This method was employed to assess the early reactivation of infectious virus from reservoirs in HIV-1-infected individuals. We found that viral proteins produced by a single infected cell can be detected by an ultrasensitive p24 assay. This unprecedented resolution showed major advantages in comparison to other techniques currently used to assess viral replication in reactivation studies. In addition, such a highly sensitive assay allows discrimination of drug-induced reactivation of productive HIV based on protein expression. The present study heralds new opportunities to evaluate the HIV reservoir and the efficacy of drugs used to target it. Copyright © 2017 American Society for Microbiology.

An ultrasensitive SiO2-encapsulated alloyed CdZnSeS quantum dot-molecular beacon nanobiosensor for norovirus.

PubMed

Adegoke, Oluwasesan; Seo, Min-Woong; Kato, Tatsuya; Kawahito, Shoji; Park, Enoch Y

2016-12-15

Ultrasensitive, rapid and selective diagnostic probes are urgently needed to overcome the limitations of traditional probes for norovirus (NV). Here, we report the detection of NV genogroup II via nucleic acid hybridization technology using a quantum dot (QD)-conjugated molecular beacon (MB) probe. To boost the sensitivity of the MB assay system, an ultrasensitive QD fluorophore with unique optical properties was synthesized, characterized and exploited as a fluorescence signal generator. Alloyed thioglycolic (TGA)-capped CdZnSeS QDs with a high photoluminescence (PL) quantum yield (QY) value of 92% were synthesized, and a modified silanization method was employed to encapsulate the thiol-capped QDs in a silica layer. The resulting highly luminescent alloyed SiO2-coated CdZnSeS QDs had a remarkable PL QY value of 98%. Transmission electron microscopy and dynamic light scattering confirmed the monodispersity of the alloyed nanocrystals, and zeta potential analysis confirmed their colloidal stability. Powder X-ray diffraction and PL lifetime measurements confirmed the surface modification of the QDs. The alloyed TGA-capped and SiO2-coated CdZnSeS QD-conjugated MB bioprobes detected extremely low concentrations of NV RNA. Ultrasensitive detection of low concentrations of NV RNA with a limit of detection (LOD) of 8.2copies/mL in human serum and a LOD of 9.3 copies/mL in buffer was achieved using the SiO2-coated CdZnSeS QD-MB probes, an increase in sensitivity of 3-fold compared with the detection limit for NV RNA using TGA-capped CdZnSeS QD-MBs. The additional merits of our detection system are rapidity, specificity and improved sensitivity over conventional molecular test probes. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

Ultrasensitive Visual Detection of HIV DNA Biomarkers via a Multi-amplification Nanoplatform.

PubMed

Long, Yuyin; Zhou, Cuisong; Wang, Congmin; Cai, Honglian; Yin, Cuiyun; Yang, Qiufang; Xiao, Dan

2016-04-01

Methodologies to detect disease biomarkers at ultralow concentrations can potentially improve the standard of living. A facile and label-free multi-amplification strategy is proposed for the ultrasensitive visual detection of HIV DNA biomarkers in real physiological media. This multi-amplification strategy not only exhibits a signficantly low detection limit down to 4.8 pM but also provides a label-free, cost-effective and facile technique for visualizing a few molecules of nucleic acid analyte with the naked eye. Importantly, the biosensor is capable of discriminating single-based mismatch lower than 5.0 nM in human serum samples. Moreover, the visual sensing platform exhibits excellent specificity, acceptable reusability and a long-term stability. All these advantages could be attributed to the nanofibrous sensing platform that 1) has a high surface-area-to-volume provided by electrospun nanofibrous membrane, and 2) combines glucose oxidase (GOx) biocatalysis, DNAzyme-catalyzed colorimetric reaction and catalytic hairpin assembly (CHA) recycling amplification together. This multi-amplification nanoplatform promises label-free and visual single-based mismatch DNA monitoring with high sensitivity and specificity, suggesting wide applications that range from virus detection to genetic disease diagnosis.

Biomimetic nanochannels based biosensor for ultrasensitive and label-free detection of nucleic acids.

PubMed

Sun, Zhongyue; Liao, Tangbin; Zhang, Yulin; Shu, Jing; Zhang, Hong; Zhang, Guo-Jun

2016-12-15

A very simple sensing device based on biomimetic nanochannels has been developed for label-free, ultrasensitive and highly sequence-specific detection of DNA. Probe DNA was modified on the inner wall of the nanochannel surface by layer-by-layer (LBL) assembly. After probe DNA immobilization, DNA detection was realized by monitoring the rectified ion current when hybridization occurred. Due to three dimensional (3D) nanoscale environment of the nanochannel, this special geometry dramatically increased the surface area of the nanochannel for immobilization of probe molecules on the inner-surface and enlarged contact area between probes and target-molecules. Thus, the unique sensor reached a reliable detection limit of 10 fM for target DNA. In addition, this DNA sensor could discriminate complementary DNA (c-DNA) from non-complementary DNA (nc-DNA), two-base mismatched DNA (2bm-DNA) and one-base mismatched DNA (1bm-DNA) with high specificity. Moreover, the nanochannel-based biosensor was also able to detect target DNA even in an interfering environment and serum samples. This approach will provide a novel biosensing platform for detection and discrimination of disease-related molecular targets and unknown sequence DNA. Copyright © 2016 Elsevier B.V. All rights reserved.

Single-Nanoparticle Photoelectrochemistry at a Nanoparticulate TiO2 -Filmed Ultramicroelectrode.

PubMed

Peng, Yue-Yi; Ma, Hui; Ma, Wei; Long, Yi-Tao; Tian, He

2018-03-26

An ultrasensitive photoelectrochemical method for achieving real-time detection of single nanoparticle collision events is presented. Using a micrometer-thick nanoparticulate TiO 2 -filmed Au ultra-microelectrode (TiO 2 @Au UME), a sub-millisecond photocurrent transient was observed for an individual N719-tagged TiO 2 (N719@TiO 2 ) nanoparticle and is due to the instantaneous collision process. Owing to a trap-limited electron diffusion process as the rate-limiting step, a random three-dimensional diffusion model was developed to simulate electron transport dynamics in TiO 2 film. The combination of theoretical simulation and high-resolution photocurrent measurement allow electron-transfer information of a single N719@TiO 2 nanoparticle to be quantified at single-molecule accuracy and the electron diffusivity and the electron-collection efficiency of TiO 2 @Au UME to be estimated. This method provides a test for studies of photoinduced electron transfer at the single-nanoparticle level. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Nucleic Acids for Ultra-Sensitive Protein Detection

PubMed Central

Janssen, Kris P. F.; Knez, Karel; Spasic, Dragana; Lammertyn, Jeroen

2013-01-01

Major advancements in molecular biology and clinical diagnostics cannot be brought about strictly through the use of genomics based methods. Improved methods for protein detection and proteomic screening are an absolute necessity to complement to wealth of information offered by novel, high-throughput sequencing technologies. Only then will it be possible to advance insights into clinical processes and to characterize the importance of specific protein biomarkers for disease detection or the realization of “personalized medicine”. Currently however, large-scale proteomic information is still not as easily obtained as its genomic counterpart, mainly because traditional antibody-based technologies struggle to meet the stringent sensitivity and throughput requirements that are required whereas mass-spectrometry based methods might be burdened by significant costs involved. However, recent years have seen the development of new biodetection strategies linking nucleic acids with existing antibody technology or replacing antibodies with oligonucleotide recognition elements altogether. These advancements have unlocked many new strategies to lower detection limits and dramatically increase throughput of protein detection assays. In this review, an overview of these new strategies will be given. PMID:23337338

Integrated Circuits for Rapid Sample Processing and Electrochemical Detection of Biomarkers

NASA Astrophysics Data System (ADS)

Besant, Justin

The trade-off between speed and sensitivity of detection is a fundamental challenge in the design of point-of-care diagnostics. As the relevant molecules in many diseases exist natively at extremely low levels, many gold-standard diagnostic tests are designed with high sensitivity at the expense of long incubations needed to amplify the target analytes. The central aim of this thesis is to design new strategies to detect biologically relevant analytes with both high speed and sensitivity. The response time of a biosensor is limited by the ability of the target analyte to accumulate to detectable levels at the sensor surface. We overcome this limitation by designing a range of integrated devices to optimize the flux of the analyte to the sensor by increasing the effective analyte concentration, shortening the required diffusion distance, and confining the analyte in close proximity to the sensor. We couple these devices with novel ultrasensitive electrochemical transduction strategies to convert rare analytes into a detectable signal. We showcase the clinical utility of these approaches with several applications including cancer diagnosis, bacterial identification, and antibiotic susceptibility profiling. We design and optimize a device to isolate rare cancer cells from the bloodstream with near 100% efficiency and 10 000-fold specificity. We analyse pathogen specific nucleic acids by lysing bacteria in close proximity to an electrochemical sensor and find that this approach has 10-fold higher sensitivity than standard lysis in bulk solution. We design an electronic chip to readout the antibiotic susceptibility profile with an hour-long incubation by concentrating bacteria into nanoliter chambers with integrated electrodes. Finally, we report a strategy for ultrasensitive visual readout of nucleic acids as low as 100 fM within 10 minutes using an amplification cascade. The strategies presented could guide the development of fast, sensitive and low-cost diagnostics for diseases not previously detectable at the point-of-care.

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.

Visible-light driven photoelectrochemical immunosensor for insulin detection based on MWCNTs@SnS2@CdS nanocomposites.

PubMed

Liu, Yixin; Zhang, Yifeng; Wu, Dan; Fan, Dawei; Pang, Xuehui; Zhang, Yong; Ma, Hongmin; Sun, Xu; Wei, Qin

2016-12-15

In this work, a label-free photoelectrochemical (PEC) immunosensor was developed for ultrasensitive detection of insulin based on MWCNTs@SnS2@CdS nanocomposites. As graphene-like 2D nanomaterial, SnS2 nanosheets loaded on the conducting framework of multi-walled carbon nanotubes (MWCNTs) were adopted for the construction of immunosensor for the first time, providing a favorable substrate for in-situ growth of CdS nanocrystal that had suitable band structure matching well with SnS2. The well-matched band structure of these two metal sulfides effectively inhibited the recombination of photogenerated electron-hole pairs, thus improving the photo-to-current conversion efficiency. Besides, the introduction of MWCNTs facilitated electron transfer across the surface of electrodes, leading to a further increment of photocurrent. The as constructed label-free PEC immunosensor based on MWCNTs@SnS2@CdS nanocomposites exhibited excellent PEC performance for the detection of insulin. The concentrations of insulin could be directly detected based on the decrement of photocurrent that was brought by the increased steric hindrances due to the formation of antigen-antibody immunocomplexes. Under the optimal conditions, the PEC immunosensor had a sensitive response to insulin in a linear range of 0.1pgmL(-1) to 5ngmL(-1) with a detection limit of 0.03pgmL(-1). Meanwhile, good stability and selectivity were achieved as well. The design and fabrication of this PEC immunosensor based on MWCNTs@SnS2@CdS nanocomposites not only provided an ideal platform for the detection of insulin, but also opened up a new avenue for the development of immunosensor for some other biomarkers analysis. Copyright © 2016 Elsevier B.V. All rights reserved.

Target-triggering multiple-cycle signal amplification strategy for ultrasensitive detection of DNA based on QCM and SPR.

PubMed

Song, Weiling; Yin, Wenshuo; Sun, Wenbo; Guo, Xiaoyan; He, Peng; Yang, Xiaoyan; Zhang, Xiaoru

2018-04-24

Detection of ultralow concentrations of nucleic acid sequences is a central challenge in the early diagnosis of genetic diseases. Herein, we developed a target-triggering cascade multiple cycle amplification for ultrasensitive DNA detection using quartz crystal microbalance (QCM) and surface plasmon resonance (SPR). It was based on the exonuclease Ⅲ (Exo Ⅲ)-assisted signal amplification and the hybridization chain reaction (HCR). The streptavidin-coated Au-NPs (Au-NPs-SA) were assembled on the HCR products as recognition element. Upon sensing of target DNA, the duplex DNA probe triggered the Exo Ⅲ cleavage process, accompanied by generating a new secondary target DNA and releasing target DNA. The released target DNA and the secondary target DNA were recycled. Simultaneously, numerous single strands were liberated and acted as the trigger of HCR to generate further signal amplification, resulting in the immobilization of abundant Au-NPs-SA on the gold substrate. The QCM sensor results were found to be comparable to that achieved using a SPR sensor platform. This method exhibited a high sensitivity toward target DNA with a detection limit of 0.70 fM. The high sensitivity and specificity make this method a great potential for detecting DNA with trace amounts in bioanalysis and clinical biomedicine. Copyright © 2018 Elsevier Inc. All rights reserved.

Hybrid nanosensor for colorimetric and ultrasensitive detection of nuclease contaminations

NASA Astrophysics Data System (ADS)

Cecere, Paola; Valentini, Paola; Pompa, Pier Paolo

2016-04-01

Nucleases are ubiquitous enzymes that degrade DNA or RNA, thus they can prejudice the good outcome of molecular biology experiments involving nucleic acids. We propose a colorimetric test for the naked-eye detection of nuclease contaminations. The system uses an hybrid nanosensor, based on gold nanoparticles functionalized with DNA probes. Our assay is rapid, instrument-free, simple and low-cost. Moreover, it reaches sensitivity equal or better than those of commercial kits, and presents a lot of advantageous aspects. Therefore, it is very competitive, with a real market potential. This test will be relevant in routine process monitoring in scientific laboratories, and in quality control in clinical laboratories and industrial processes, allowing the simultaneous detection of nucleases with different substrate specificities and large-scale screening.

Vertically aligned carbon nanofiber electrode arrays for nucleic acid detection

NASA Astrophysics Data System (ADS)

Arumugam, Prabhu U.; Yu, Edmond; Riviere, Roger; Meyyappan, M.

2010-10-01

We present electrochemical detection of DNA targets that corresponds to Escherichia coli O157:H7 16S rRNA gene using a nanoelectrode array consisting of vertically aligned carbon nanofiber (VACNF) electrodes. Parylene C is used as gap filling 'matrix' material to avoid high temperature processing in electrode construction. This easy to deposit film of several micron heights provides a conformal coating between the high aspect ratio VACNFs with negligible pin-holes. The low background currents show the potential of this approach for ultra-sensitive detection. Consistent and reproducible electrochemical-signals are achieved using a simple electrode preparation. This simple, reliable and low-cost approach is a forward step in developing practical sensors for applications like pathogen detection, early cancer diagnosis and environmental monitoring.

Carbon nanostructure-based field-effect transistors for label-free chemical/biological sensors.

PubMed

Hu, PingAn; Zhang, Jia; Li, Le; Wang, Zhenlong; O'Neill, William; Estrela, Pedro

2010-01-01

Over the past decade, electrical detection of chemical and biological species using novel nanostructure-based devices has attracted significant attention for chemical, genomics, biomedical diagnostics, and drug discovery applications. The use of nanostructured devices in chemical/biological sensors in place of conventional sensing technologies has advantages of high sensitivity, low decreased energy consumption and potentially highly miniaturized integration. Owing to their particular structure, excellent electrical properties and high chemical stability, carbon nanotube and graphene based electrical devices have been widely developed for high performance label-free chemical/biological sensors. Here, we review the latest developments of carbon nanostructure-based transistor sensors in ultrasensitive detection of chemical/biological entities, such as poisonous gases, nucleic acids, proteins and cells.

A cascade autocatalytic strand displacement amplification and hybridization chain reaction event for label-free and ultrasensitive electrochemical nucleic acid biosensing.

PubMed

Chen, Zhiqiang; Liu, Ying; Xin, Chen; Zhao, Jikuan; Liu, Shufeng

2018-08-15

Herein, an autocatalytic strand displacement amplification (ASDA) strategy was proposed for the first time, which was further ingeniously coupled with hybridization chain reaction (HCR) event for the isothermal, label-free and multiple amplification toward nucleic acid detection. During the ASDA module, the target recognition opens the immobilized hairpin probe (IP) and initiates the annealing of the auxiliary DNA strand (AS) with the opened IP for the successive polymerization and nicking reaction in the presence of DNA polymerase and nicking endonuclease. This induces the target recycling and generation of a large amount of intermediate DNA sequences, which can be used as target analogy to execute the autocatalytic strand displacement amplification. Simultaneously, the introduced AS strand can propagate the HCR between two hairpins (H1 and H2) to form a linear DNA concatamer with cytosine (C)-rich loop region, which can facilitate the in-situ synthesis of silver nanoclusters (AgNCs) as electrochemical tags for further amplification toward target responses. With current cascade ASDA and HCR strategy, the detection of target DNA could be achieved with a low detection limit of about 0.16 fM and a good selectivity. The developed biosensor also exhibits the distinct advantages of flexibility and simplicity in probe design and biosensor fabrication, and label-free electrochemical detection, thus opens a promising avenue for the detection of nucleic acid with low abundance in bioanalysis and clinical biomedicine. Copyright © 2018 Elsevier B.V. All rights reserved.

Sensitive and inexpensive digital DNA analysis by microfluidic enrichment of rolling circle amplified single-molecules.

PubMed

Kühnemund, Malte; Hernández-Neuta, Iván; Sharif, Mohd Istiaq; Cornaglia, Matteo; Gijs, Martin A M; Nilsson, Mats

2017-05-05

Single molecule quantification assays provide the ultimate sensitivity and precision for molecular analysis. However, most digital analysis techniques, i.e. droplet PCR, require sophisticated and expensive instrumentation for molecule compartmentalization, amplification and analysis. Rolling circle amplification (RCA) provides a simpler means for digital analysis. Nevertheless, the sensitivity of RCA assays has until now been limited by inefficient detection methods. We have developed a simple microfluidic strategy for enrichment of RCA products into a single field of view of a low magnification fluorescent sensor, enabling ultra-sensitive digital quantification of nucleic acids over a dynamic range from 1.2 aM to 190 fM. We prove the broad applicability of our analysis platform by demonstrating 5-plex detection of as little as ∼1 pg (∼300 genome copies) of pathogenic DNA with simultaneous antibiotic resistance marker detection, and the analysis of rare oncogene mutations. Our method is simpler, more cost-effective and faster than other digital analysis techniques and provides the means to implement digital analysis in any laboratory equipped with a standard fluorescent microscope. © The Author(s) 2017. Published by Oxford University Press on behalf of Nucleic Acids Research.

Design of nuclease-based target recycling signal amplification in aptasensors.

PubMed

Yan, Mengmeng; Bai, Wenhui; Zhu, Chao; Huang, Yafei; Yan, Jiao; Chen, Ailiang

2016-03-15

Compared with conventional antibody-based immunoassay methods, aptasensors based on nucleic acid aptamer have made at least two significant breakthroughs. One is that aptamers are more easily used for developing various simple and rapid homogeneous detection methods by "sample in signal out" without multi-step washing. The other is that aptamers are more easily employed for developing highly sensitive detection methods by using various nucleic acid-based signal amplification approaches. As many substances playing regulatory roles in physiology or pathology exist at an extremely low concentration and many chemical contaminants occur in trace amounts in food or environment, aptasensors for signal amplification contribute greatly to detection of such targets. Among the signal amplification approaches in highly sensitive aptasensors, the nuclease-based target recycling signal amplification has recently become a research focus because it shows easy design, simple operation, and rapid reaction and can be easily developed for homogenous assay. In this review, we summarized recent advances in the development of various nuclease-based target recycling signal amplification with the aim to provide a general guide for the design of aptamer-based ultrasensitive biosensing assays. Copyright © 2015 Elsevier B.V. All rights reserved.

Ultrasensitive FRET-based DNA sensor using PNA/DNA hybridization.

PubMed

Yang, Lan-Hee; Ahn, Dong June; Koo, Eunhae

2016-12-01

In the diagnosis of genetic diseases, rapid and highly sensitive DNA detection is crucial. Therefore, many strategies for detecting target DNA have been developed, including electrical, optical, and mechanical methods. Herein, a highly sensitive FRET based sensor was developed by using PNA (Peptide Nucleic Acid) probe and QD, in which red color QDs are hybridized with capture probes, reporter probes and target DNAs by EDC-NHS coupling. The hybridized probe with target DNA gives off fluorescent signal due to the energy transfer from QD to Cy5 dye in the reporter probe. Compared to the conventional DNA sensor using DNA probes, the DNA sensor using PNA probes shows higher FRET factor and efficiency due to the higher reactivity between PNA and target DNA. In addition, to elicit the effect of the distance between the donor and the acceptor, we have investigated two types of the reporter probes having Cy5 dyes attached at the different positions of the reporter probes. Results show that the shorter the distance between QDs and Cy5s, the stronger the signal intensity. Furthermore, based on the fluorescence microscopy images using microcapillary chips, the FRET signal is enhanced to be up to 276% times stronger than the signal obtained using the cuvette by the fluorescence spectrometer. These results suggest that the PNA probe system conjugated with QDs can be used as ultrasensitive DNA nanosensors. Copyright © 2016. Published by Elsevier B.V.

Ultrasensitive Faraday cage-type electrochemiluminescence assay for femtomolar miRNA-141 via graphene oxide and hybridization chain reaction-assisted cascade amplification.

PubMed

Lu, Jing; Wu, Lin; Hu, Yufang; Wang, Sui; Guo, Zhiyong

2018-06-30

In this study, a novel electrochemiluminescence (ECL) biosensor for sensitive detection of femtomolar miRNA-141 was constructed on the basis of Faraday cage-type strategy via graphene oxide (GO) and hybridization chain reaction (HCR)-assisted cascade amplification. A capture probe (CP) was immobilized on Fe 3 O 4 @SiO 2 @Au nanoparticles as capture unit, which could catch the miRNA-141, and the immobilization of the signal unit (Ru(phen) 3 2+ -HCR/GO) was allowed via nucleic acid hybridization. The prepared biosensor exhibited two advantages for signal amplification: firstly, GO could lap on the electrode surface directly, extending Outer Helmholtz Plane (OHP) of the sensor due to the large surface area and good electronic transport property; secondly, HCR-assisted cascade amplification was designed by anchoring all HCR products on the GO surface, then embedding Ru(phen) 3 2+ as a signal readout pathway. All these signal molecules could take part in electrochemical reactions, thus further enhancing the ECL signal drastically. Therefore, the proposed sensor constructed by integrating HCR with Faraday cage-type strategy displayed an ultrasensitive detection platform for the miRNA-141 with a low detection limit of 0.03 fM. In addition, this proposed biosensor provides a universal platform for analysis of other microRNAs. Copyright © 2018 Elsevier B.V. All rights reserved.

Microwave-Accelerated Method for Ultra-Rapid Extraction of Neisseria gonorrhoeae DNA for Downstream Detection

PubMed Central

Melendez, Johan H.; Santaus, Tonya M.; Brinsley, Gregory; Kiang, Daniel; Mali, Buddha; Hardick, Justin; Gaydos, Charlotte A.; Geddes, Chris D.

2016-01-01

Nucleic acid-based detection of gonorrhea infections typically require a two-step process involving isolation of the nucleic acid, followed by the detection of the genomic target often involving PCR-based approaches. In an effort to improve on current detection approaches, we have developed a unique two-step microwave-accelerated approach for rapid extraction and detection of Neisseria gonorrhoeae (GC) DNA. Our approach is based on the use of highly-focused microwave radiation to rapidly lyse bacterial cells, release, and subsequently fragment microbial DNA. The DNA target is then detected by a process known as microwave-accelerated metal-enhanced fluorescence (MAMEF), an ultra-sensitive direct DNA detection analytical technique. In the present study, we show that highly focused microwaves at 2.45 GHz, using 12.3 mm gold film equilateral triangles, are able to rapidly lyse both bacteria cells and fragment DNA in a time- and microwave power-dependent manner. Detection of the extracted DNA can be performed by MAMEF, without the need for DNA amplification in less than 10 minutes total time or by other PCR-based approaches. Collectively, the use of a microwave-accelerated method for the release and detection of DNA represents a significant step forward towards the development of a point-of-care (POC) platform for detection of gonorrhea infections. PMID:27325503

Ultrasensitive quantum dots-based DNA detection and hybridization kinetics analysis with evanescent wave biosensing platform.

PubMed

Long, Feng; Wu, Shuxu; He, Miao; Tong, Tiezheng; Shi, Hanchang

2011-01-15

Ultrasensitive DNA detection was achieved using a new biosensing platform based on quantum dots (QDs) and total internal reflection fluorescence, which featured an exceptional detection limit of 3.2 amol of bound target DNA. The reusable sensor surface was produced by covalently immobilizing streptavidin onto a self-assembled alkanethiol monolayer of fiber optic probe through a heterobifunctional reagent. Streptavidin served as a versatile binding element for biotinylated single-strand DNA (ssDNA). The ssDNA-coated fiber probe was evaluated as a nucleic acid biosensor through a DNA-DNA hybridization assay for a 30-mer ssDNA, which were the segments of the uidA gene of Escherichia coli and labeled by QDs using avidin-biotin interaction. Several negative control tests revealed the absence of significant non-specific binding. It also showed that bound target DNA could easily be eluted from the sensor surface using SDS solution (pH 1.9) without any significant loss of performance after more than 30 assay cycles. A quantitative measurement of DNA binding kinetics was achieved with high accuracy, indicating an association rate of 1.38×10(6) M(-1) s(-1) and a dissociation rate of 4.67×10(-3) s(-1). The proposed biosensing platform provides a simple, cheap, fast, and robust solution for many potential applications including clinical diagnosis, pathology, and genetics. Copyright © 2010 Elsevier B.V. All rights reserved.

Ternary Surface Monolayers for Ultrasensitive (Zeptomole) Amperometric Detection of Nucleic-Acid Hybridization without Signal Amplification

PubMed Central

Wu, Jie; Campuzano, Susana; Halford, Colin; Haake, David A.; Wang, Joseph

2010-01-01

A ternary surface monolayer, consisting of co-assembled thiolated capture probe (SHCP) mercaptohexanol (MCH) and dithiothreitol (DTT), is shown to offer dramatic improvements in the signal-to-noise characteristics of electrochemical DNA hybridization biosensors based on common self-assembled monolayers (SAMs). Remarkably low detection limits down to 40 zmole (in 4 μL samples) as well as only 1 CFU E. coli per sensor are thus obtained without any additional amplification step in connection to the commonly used horseradish peroxidase/3,3′,5,5′-tetramethylbenzidine (HRP/TMB) system. Such dramatic improvements in the detection limits (compared to common binary alkanethiol interfaces and to most electrochemical DNA sensing strategies without target or signal amplification) are attributed primarily to the remarkably higher resistance to non-specific adsorption. This reflects the highly compact layer (with lower pinhole density) produced by the coupling of the cyclic- and linear-configuration ‘backfillers’ that leads to a remarkably low background noise even in the presence of complex sample matrices. A wide range of surface compositions have been investigated and the ternary mixed monolayer has been systematically optimized. Detailed impedance spectroscopy and cyclic voltammetric studies shed useful insights into the surface coverage. The impressive sensitivity and high specificity of the simple developed methodology indicate great promise for a wide range of nucleic acid testing, including clinical diagnostics, biothreat detection, food safety and forensic analysis. PMID:20883023

Ternary surface monolayers for ultrasensitive (zeptomole) amperometric detection of nucleic acid hybridization without signal amplification.

PubMed

Wu, Jie; Campuzano, Susana; Halford, Colin; Haake, David A; Wang, Joseph

2010-11-01

A ternary surface monolayer, consisting of coassembled thiolated capture probe, mercaptohexanol and dithiothreitol, is shown to offer dramatic improvements in the signal-to-noise characteristics of electrochemical DNA hybridization biosensors based on common self-assembled monolayers. Remarkably low detection limits down to 40 zmol (in 4 μL samples) as well as only 1 CFU Escherichia coli per sensor are thus obtained without any additional amplification step in connection to the commonly used horseradish peroxidase/3,3',5,5'-tetramethylbenzidine system. Such dramatic improvements in the detection limits (compared to those of common binary alkanethiol interfaces and to those of most electrochemical DNA sensing strategies without target or signal amplification) are attributed primarily to the remarkably higher resistance to nonspecific adsorption. This reflects the highly compact layer (with lower pinhole density) produced by the coupling of the cyclic- and linear-configuration "backfillers" that leads to a remarkably low background noise even in the presence of complex sample matrixes. A wide range of surface compositions have been investigated, and the ternary mixed monolayer has been systematically optimized. Detailed impedance spectroscopy and cyclic voltammetric studies shed useful insights into the surface coverage. The impressive sensitivity and high specificity of the simple developed methodology indicate great promise for a wide range of nucleic acid testing, including clinical diagnostics, biothreat detection, food safety, and forensic analysis.

Microwave-accelerated method for ultra-rapid extraction of Neisseria gonorrhoeae DNA for downstream detection.

PubMed

Melendez, Johan H; Santaus, Tonya M; Brinsley, Gregory; Kiang, Daniel; Mali, Buddha; Hardick, Justin; Gaydos, Charlotte A; Geddes, Chris D

2016-10-01

Nucleic acid-based detection of gonorrhea infections typically require a two-step process involving isolation of the nucleic acid, followed by detection of the genomic target often involving polymerase chain reaction (PCR)-based approaches. In an effort to improve on current detection approaches, we have developed a unique two-step microwave-accelerated approach for rapid extraction and detection of Neisseria gonorrhoeae (gonorrhea, GC) DNA. Our approach is based on the use of highly focused microwave radiation to rapidly lyse bacterial cells, release, and subsequently fragment microbial DNA. The DNA target is then detected by a process known as microwave-accelerated metal-enhanced fluorescence (MAMEF), an ultra-sensitive direct DNA detection analytical technique. In the current study, we show that highly focused microwaves at 2.45 GHz, using 12.3-mm gold film equilateral triangles, are able to rapidly lyse both bacteria cells and fragment DNA in a time- and microwave power-dependent manner. Detection of the extracted DNA can be performed by MAMEF, without the need for DNA amplification, in less than 10 min total time or by other PCR-based approaches. Collectively, the use of a microwave-accelerated method for the release and detection of DNA represents a significant step forward toward the development of a point-of-care (POC) platform for detection of gonorrhea infections. Copyright © 2016 Elsevier Inc. All rights reserved.

Ultrasensitivity in signaling cascades revisited: Linking local and global ultrasensitivity estimations.

PubMed

Altszyler, Edgar; Ventura, Alejandra C; Colman-Lerner, Alejandro; Chernomoretz, Ariel

2017-01-01

Ultrasensitive response motifs, capable of converting graded stimuli into binary responses, are well-conserved in signal transduction networks. Although it has been shown that a cascade arrangement of multiple ultrasensitive modules can enhance the system's ultrasensitivity, how a given combination of layers affects a cascade's ultrasensitivity remains an open question for the general case. Here, we introduce a methodology that allows us to determine the presence of sequestration effects and to quantify the relative contribution of each module to the overall cascade's ultrasensitivity. The proposed analysis framework provides a natural link between global and local ultrasensitivity descriptors and it is particularly well-suited to characterize and understand mathematical models used to study real biological systems. As a case study, we have considered three mathematical models introduced by O'Shaughnessy et al. to study a tunable synthetic MAPK cascade, and we show how our methodology can help modelers better understand alternative models.

Ultrasensitivity in signaling cascades revisited: Linking local and global ultrasensitivity estimations

PubMed Central

Altszyler, Edgar; Ventura, Alejandra C.; Colman-Lerner, Alejandro; Chernomoretz, Ariel

2017-01-01

Ultrasensitive response motifs, capable of converting graded stimuli into binary responses, are well-conserved in signal transduction networks. Although it has been shown that a cascade arrangement of multiple ultrasensitive modules can enhance the system’s ultrasensitivity, how a given combination of layers affects a cascade’s ultrasensitivity remains an open question for the general case. Here, we introduce a methodology that allows us to determine the presence of sequestration effects and to quantify the relative contribution of each module to the overall cascade’s ultrasensitivity. The proposed analysis framework provides a natural link between global and local ultrasensitivity descriptors and it is particularly well-suited to characterize and understand mathematical models used to study real biological systems. As a case study, we have considered three mathematical models introduced by O’Shaughnessy et al. to study a tunable synthetic MAPK cascade, and we show how our methodology can help modelers better understand alternative models. PMID:28662096

Ultrasensitive Genotypic Detection of Antiviral Resistance in Hepatitis B Virus Clinical Isolates▿ †

PubMed Central

Fang, Jie; Wichroski, Michael J.; Levine, Steven M.; Baldick, Carl J.; Mazzucco, Charles E.; Walsh, Ann W.; Kienzle, Bernadette K.; Rose, Ronald E.; Pokornowski, Kevin A.; Colonno, Richard J.; Tenney, Daniel J.

2009-01-01

Amino acid substitutions that confer reduced susceptibility to antivirals arise spontaneously through error-prone viral polymerases and are selected as a result of antiviral therapy. Resistance substitutions first emerge in a fraction of the circulating virus population, below the limit of detection by nucleotide sequencing of either the population or limited sets of cloned isolates. These variants can expand under drug pressure to dominate the circulating virus population. To enhance detection of these viruses in clinical samples, we established a highly sensitive quantitative, real-time allele-specific PCR assay for hepatitis B virus (HBV) DNA. Sensitivity was accomplished using a high-fidelity DNA polymerase and oligonucleotide primers containing locked nucleic acid bases. Quantitative measurement of resistant and wild-type variants was accomplished using sequence-matched standards. Detection methodology that was not reliant on hybridization probes, and assay modifications, minimized the effect of patient-specific sequence polymorphisms. The method was validated using samples from patients chronically infected with HBV through parallel sequencing of large numbers of cloned isolates. Viruses with resistance to lamivudine and other l-nucleoside analogs and entecavir, involving 17 different nucleotide substitutions, were reliably detected at levels at or below 0.1% of the total population. The method worked across HBV genotypes. Longitudinal analysis of patient samples showed earlier emergence of resistance on therapy than was seen with sequencing methodologies, including some cases of resistance that existed prior to treatment. In summary, we established and validated an ultrasensitive method for measuring resistant HBV variants in clinical specimens, which enabled earlier, quantitative measurement of resistance to therapy. PMID:19433559

Tris(hydroxymethyl)aminomethane photooxidation on titania based photoanodes and its implication for photoelectrochemical biofuel cells

NASA Astrophysics Data System (ADS)

Filipiak, Marcin S.; Zloczewska, Adrianna; Grzeskowiak, Piotr; Lynch, Robert; Jönsson-Niedziolka, Martin

2015-09-01

In many photoelectrochemical biofuel cells tris(hydroxymethyl)aminomethane (TRIS) is used a buffer. We show that TRIS can be readily photooxidised on titania electrodes. Combining a titania nanotube photoanode in a TRIS buffer with an air-breathing enzymatic biocathode we construct a relatively efficient photoelectrochemical biofuel cell using the TRIS buffer as fuel. This shows both the prospect of using air-breathing bio-cathodes in this kind of cells, but more importantly, shows the need for caution when using TRIS as buffer in photoelectrochemical applications.

PCR-Free Detection of Genetically Modified Organisms Using Magnetic Capture Technology and Fluorescence Cross-Correlation Spectroscopy

PubMed Central

Zhou, Xiaoming; Xing, Da; Tang, Yonghong; Chen, Wei R.

2009-01-01

The safety of genetically modified organisms (GMOs) has attracted much attention recently. Polymerase chain reaction (PCR) amplification is a common method used in the identification of GMOs. However, a major disadvantage of PCR is the potential amplification of non-target DNA, causing false-positive identification. Thus, there remains a need for a simple, reliable and ultrasensitive method to identify and quantify GMO in crops. This report is to introduce a magnetic bead-based PCR-free method for rapid detection of GMOs using dual-color fluorescence cross-correlation spectroscopy (FCCS). The cauliflower mosaic virus 35S (CaMV35S) promoter commonly used in transgenic products was targeted. CaMV35S target was captured by a biotin-labeled nucleic acid probe and then purified using streptavidin-coated magnetic beads through biotin-streptavidin linkage. The purified target DNA fragment was hybridized with two nucleic acid probes labeled respectively by Rhodamine Green and Cy5 dyes. Finally, FCCS was used to detect and quantify the target DNA fragment through simultaneously detecting the fluorescence emissions from the two dyes. In our study, GMOs in genetically engineered soybeans and tomatoes were detected, using the magnetic bead-based PCR-free FCCS method. A detection limit of 50 pM GMOs target was achieved and PCR-free detection of GMOs from 5 µg genomic DNA with magnetic capture technology was accomplished. Also, the accuracy of GMO determination by the FCCS method is verified by spectrophotometry at 260 nm using PCR amplified target DNA fragment from GM tomato. The new method is rapid and effective as demonstrated in our experiments and can be easily extended to high-throughput and automatic screening format. We believe that the new magnetic bead-assisted FCCS detection technique will be a useful tool for PCR-free GMOs identification and other specific nucleic acids. PMID:19956680

Photoassisted electrolysis of water - Conversion of optical to chemical energy

NASA Technical Reports Server (NTRS)

Wrighton, M. S.; Bolts, J. M.; Kaiser, S. W.; Ellis, A. B.

1976-01-01

A description is given of devices, termed photoelectrochemical cells, which can, in principle, be used to directly convert light to fuels and/or electricity. The fundamental principles on which the photoelectrochemical cell is based are related to the observation that irradiation of a semiconductor electrode in an electrochemical cell can result in the flow of an electric current in the external circuit. Attention is given to the basic mechanisms involved, the energy conversion efficiency, the advantages of photoelectrochemical cells, and the results of investigations related to the study of energy conversion via photoelectrochemical cells.

Rapid single cell detection of Staphylococcus aureus by aptamer-conjugated gold nanoparticles

PubMed Central

Chang, Yi-Chung; Yang, Chia-Ying; Sun, Ruei-Lin; Cheng, Yi-Feng; Kao, Wei-Chen; Yang, Pan-Chyr

2013-01-01

Staphylococcus aureus is one of the most important human pathogens, causing more than 500,000 infections in the United States each year. Traditional methods for bacterial culture and identification take several days, wasting precious time for patients who are suffering severe bacterial infections. Numerous nucleic acid-based detection methods have been introduced to address this deficiency; however, the costs and requirement for expensive equipment may limit the widespread use of such technologies. Thus, there is an unmet demand of new platform technology to improve the bacterial detection and identification in clinical practice. In this study, we developed a rapid, ultra-sensitive, low cost, and non-polymerase chain reaction (PCR)-based method for bacterial identification. Using this method, which measures the resonance light-scattering signal of aptamer-conjugated gold nanoparticles, we successfully detected single S. aureus cell within 1.5 hours. This new platform technology may have potential to develop a rapid and sensitive bacterial testing at point-of-care. PMID:23689505

Rapid single cell detection of Staphylococcus aureus by aptamer-conjugated gold nanoparticles.

PubMed

Chang, Yi-Chung; Yang, Chia-Ying; Sun, Ruei-Lin; Cheng, Yi-Feng; Kao, Wei-Chen; Yang, Pan-Chyr

2013-01-01

Staphylococcus aureus is one of the most important human pathogens, causing more than 500,000 infections in the United States each year. Traditional methods for bacterial culture and identification take several days, wasting precious time for patients who are suffering severe bacterial infections. Numerous nucleic acid-based detection methods have been introduced to address this deficiency; however, the costs and requirement for expensive equipment may limit the widespread use of such technologies. Thus, there is an unmet demand of new platform technology to improve the bacterial detection and identification in clinical practice. In this study, we developed a rapid, ultra-sensitive, low cost, and non-polymerase chain reaction (PCR)-based method for bacterial identification. Using this method, which measures the resonance light-scattering signal of aptamer-conjugated gold nanoparticles, we successfully detected single S. aureus cell within 1.5 hours. This new platform technology may have potential to develop a rapid and sensitive bacterial testing at point-of-care.

An ultrasensitive universal detector based on neutralizer displacement

NASA Astrophysics Data System (ADS)

Das, Jagotamoy; Cederquist, Kristin B.; Zaragoza, Alexandre A.; Lee, Paul E.; Sargent, Edward H.; Kelley, Shana O.

2012-08-01

Diagnostic technologies that can provide the simultaneous detection of nucleic acids for gene expression, proteins for host response and small molecules for profiling the human metabolome will have a significant advantage in providing comprehensive patient monitoring. Molecular sensors that report changes in the electrostatics of a sensor's surface on analyte binding have shown unprecedented sensitivity in the detection of charged biomolecules, but do not lend themselves to the detection of small molecules, which do not carry significant charge. Here, we introduce the neutralizer displacement assay that allows charge-based sensing to be applied to any class of molecule irrespective of the analyte charge. The neutralizer displacement assay starts with an aptamer probe bound to a neutralizer. When analyte binding occurs the neutralizer is displaced, which results in a dramatic change in the surface charge for all types of analytes. We have tested the sensitivity, speed and specificity of this system in the detection of a panel of molecules: (deoxy)ribonucleic acid, ribonucleic acid, cocaine, adenosine triphosphate and thrombin.

Binding mechanism of PicoGreen to DNA characterized by magnetic tweezers and fluorescence spectroscopy.

PubMed

Wang, Ying; Schellenberg, Helene; Walhorn, Volker; Toensing, Katja; Anselmetti, Dario

2017-09-01

Fluorescent dyes are broadly used in many biotechnological applications to detect and visualize DNA molecules. However, their binding to DNA alters the structural and nanomechanical properties of DNA and, thus, interferes with associated biological processes. In this work we employed magnetic tweezers and fluorescence spectroscopy to investigate the binding of PicoGreen to DNA at room temperature in a concentration-dependent manner. PicoGreen is an ultrasensitive quinolinium nucleic acid stain exhibiting hardly any background signal from unbound dye molecules. By means of stretching and overwinding single, torsionally constrained, nick-free double-stranded DNA molecules, we acquired force-extension and supercoiling curves which allow quantifying DNA contour length, persistence length and other thermodynamical binding parameters, respectively. The results of our magnetic tweezers single-molecule binding study were well supported through analyzing the fluorescent spectra of stained DNA. On the basis of our work, we could identify a concentration-dependent bimodal binding behavior, where, apparently, PicoGreen associates to DNA as an intercalator and minor-groove binder simultaneously.

Electrochemical and photoelectrochemical oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and 2,5-diformylfuran

DOEpatents

Choi, Kyoung-Shin; Cha, Hyun Gil

2017-03-21

Electrochemical and photoelectrochemical cells for the oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and/or 2,5-diformylfuran are provided. Also provided are methods of using the cells to carry out the electrochemical and photoelectrochemical oxidation of 5-hydroxymethylfurfural to 2,5-furandicarboxylic acid and/or 2,5-diformylfuran.

Direct Mapping of Band Positions in Doped and Undoped Hematite during Photoelectrochemical Water Splitting

DOE PAGES

Shavorskiy, Andrey; Ye, Xiaofei; Karslgolu, Osman; ...

2017-10-30

Photoelectrochemical water splitting is a promising pathway for the direct conversion of renewable solar energy to easy to store and use chemical energy. The performance of a photoelectrochemical device is determined in large part by the heterogeneous interface between the photoanode and the electrolyte, which we here characterize directly under operating conditions using interface-specific probes. Utilizing X-ray photoelectron spectroscopy as a noncontact probe of local electrical potentials, we demonstrate direct measurements of the band alignment at the semiconductor/electrolyte interface of an operating hematite/KOH photoelectrochemical cell as a function of solar illumination, applied potential, and doping. Here, we provide evidence formore » the absence of in-gap states in this system, which is contrary to previous measurements using indirect methods, and give a comprehensive description of shifts in the band positions and limiting processes during the photoelectrochemical reaction.« less

Ultrasensitive Label-free Electronic Chip for DNA Analysis Using Carbon Nanotube Nanoelectrode Arrays

NASA Technical Reports Server (NTRS)

Li, Jun; Koehne, Jessica; Chen, Hua; Cassell, Alan; Ng, Hou Tee; Ye, Qi; Han, Jie; Meyyappan, M.

2004-01-01

There is a strong need for faster, cheaper, and simpler methods for nucleic acid analysis in today s clinical tests. Nanotechnologies can potentially provide solutions to these requirements by integrating nanomaterials with biofunctionalities. Dramatic improvement in the sensitivity and multiplexing can be achieved through the high-degree miniaturization. Here, we present our study in the development of an ultrasensitive label-free electronic chip for DNA/RNA analysis based on carbon nanotube nanoelectrode arrays. A reliable nanoelectrode array based on vertically aligned multi-walled carbon nanotubes (MWNTs) embedded in a SiO2 matrix is fabricated using a bottom-up approach. Characteristic nanoelectrode behavior is observed with a low-density MWNT nanoelectrode array in measuring both the bulk and surface immobilized redox species. The open-end of MWNTs are found to present similar properties as graphite edge-plane electrodes, with a wide potential window, flexible chemical functionalities, and good biocompatibility. A BRCA1 related oligonucleotide probe with 18 bases is covalently functionalized at the open ends of the MWNTs and specifically hybridized with an oligonucleotide target as well as a PCR amplicon. The guanine bases in the target molecules are employed as the signal moieties for the electrochemical measurements. Ru(bpy)3(2+) mediator is used to further amplify the guanine oxidation signal. This technique has been employed for direct electrochemical detection of label-free PCR amplicon through specific hybridization with the BRCAl probe. The detection limit is estimated to be less than approximately 1000 DNA molecules, approaching the limit of the sensitivity by laser-based fluorescence techniques in DNA microarray. This system provides a general electronic platform for rapid molecular diagnostics in applications requiring ultrahigh sensitivity, high-degree of miniaturization, simple sample preparation, and low- cost operation.

Ultrasensitive Quantification of Hepatitis B Virus A1762T/G1764A Mutant by a SimpleProbe PCR Using a Wild-Type-Selective PCR Blocker and a Primer-Blocker-Probe Partial-Overlap Approach ▿

PubMed Central

Nie, Hui; Evans, Alison A.; London, W. Thomas; Block, Timothy M.; Ren, Xiangdong David

2011-01-01

Hepatitis B virus (HBV) carrying the A1762T/G1764A double mutation in the basal core promoter (BCP) region is associated with HBe antigen seroconversion and increased risk of liver cirrhosis and hepatocellular carcinoma (HCC). Quantification of the mutant viruses may help in predicting the risk of HCC. However, the viral genome tends to have nucleotide polymorphism, which makes it difficult to design hybridization-based assays including real-time PCR. Ultrasensitive quantification of the mutant viruses at the early developmental stage is even more challenging, as the mutant is masked by excessive amounts of the wild-type (WT) viruses. In this study, we developed a selective inhibitory PCR (siPCR) using a locked nucleic acid-based PCR blocker to selectively inhibit the amplification of the WT viral DNA but not the mutant DNA. At the end of siPCR, the proportion of the mutant could be increased by about 10,000-fold, making the mutant more readily detectable by downstream applications such as real-time PCR and DNA sequencing. We also describe a primer-probe partial overlap approach which significantly simplified the melting curve patterns and minimized the influence of viral genome polymorphism on assay accuracy. Analysis of 62 patient samples showed a complete match of the melting curve patterns with the sequencing results. More than 97% of HBV BCP sequences in the GenBank database can be correctly identified by the melting curve analysis. The combination of siPCR and the SimpleProbe real-time PCR enabled mutant quantification in the presence of a 100,000-fold excess of the WT DNA. PMID:21562108

Photoelectrochemical detection of benzaldehyde in foodstuffs

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

LaCourse, W.R.; Krull, I.S.

Photoelectrochemical detection (PED) coupled with high performance liquid chromatography was used to quantitatively determine benzaldehyde in extracts, beverages, and foodstuffs. Photoelectrochemical detection is responsive to alkyl and aryl ketones and aldehydes and offers the advantages of 2-3 orders of magnitude linearity, 5-1-ng limits of detection, and a high degree of selectivity without chemical derivatization. This is the first application of the PED to sample analysis.

An Integrated Device View on Photo-Electrochemical Solar-Hydrogen Generation.

PubMed

Modestino, Miguel A; Haussener, Sophia

2015-01-01

Devices that directly capture and store solar energy have the potential to significantly increase the share of energy from intermittent renewable sources. Photo-electrochemical solar-hydrogen generators could become an important contributor, as these devices can convert solar energy into fuels that can be used throughout all sectors of energy. Rather than focusing on scientific achievement on the component level, this article reviews aspects of overall component integration in photo-electrochemical water-splitting devices that ultimately can lead to deployable devices. Throughout the article, three generalized categories of devices are considered with different levels of integration and spanning the range of complete integration by one-material photo-electrochemical approaches to complete decoupling by photovoltaics and electrolyzer devices. By using this generalized framework, we describe the physical aspects, device requirements, and practical implications involved with developing practical photo-electrochemical water-splitting devices. Aspects reviewed include macroscopic coupled multiphysics device models, physical device demonstrations, and economic and life cycle assessments, providing the grounds to draw conclusions on the overall technological outlook.

Surface Passivation of GaN Nanowires for Enhanced Photoelectrochemical Water-Splitting.

PubMed

Varadhan, Purushothaman; Fu, Hui-Chun; Priante, Davide; Retamal, Jose Ramon Duran; Zhao, Chao; Ebaid, Mohamed; Ng, Tien Khee; Ajia, Idirs; Mitra, Somak; Roqan, Iman S; Ooi, Boon S; He, Jr-Hau

2017-03-08

Hydrogen production via photoelectrochemical water-splitting is a key source of clean and sustainable energy. The use of one-dimensional nanostructures as photoelectrodes is desirable for photoelectrochemical water-splitting applications due to the ultralarge surface areas, lateral carrier extraction schemes, and superior light-harvesting capabilities. However, the unavoidable surface states of nanostructured materials create additional charge carrier trapping centers and energy barriers at the semiconductor-electrolyte interface, which severely reduce the solar-to-hydrogen conversion efficiency. In this work, we address the issue of surface states in GaN nanowire photoelectrodes by employing a simple and low-cost surface treatment method, which utilizes an organic thiol compound (i.e., 1,2-ethanedithiol). The surface-treated photocathode showed an enhanced photocurrent density of -31 mA/cm 2 at -0.2 V versus RHE with an incident photon-to-current conversion efficiency of 18.3%, whereas untreated nanowires yielded only 8.1% efficiency. Furthermore, the surface passivation provides enhanced photoelectrochemical stability as surface-treated nanowires retained ∼80% of their initial photocurrent value and produced 8000 μmol of gas molecules over 55 h at acidic conditions (pH ∼ 0), whereas the untreated nanowires demonstrated only <4 h of photoelectrochemical stability. These findings shed new light on the importance of surface passivation of nanostructured photoelectrodes for photoelectrochemical applications.

Photoelectrochemical response and corrosion behavior of CdS/TiO2 nanocomposite films in an aerated 0.5 M NaCl solution

NASA Astrophysics Data System (ADS)

Boonserm, Aleena; Kruehong, Chaiyaput; Seithtanabutara, Varinrumpai; Artnaseaw, Apichart; Kwakhong, Panomkorn

2017-10-01

This research aimed to investigate the photoelectrochemical response and corrosion behavior of CdS/TiO2 nanocomposite films using electrochemical measurements in an aerated 0.5 M NaCl solution under white light illumination. The CdS/TiO2 nanocomposite films were prepared by chemical bath deposition technique in a solution of cadmium and sulfide ions. The high resolution images of CdS/TiO2 nanocomposite films were provided by field emission scanning electron microscope. Theirs chemical identification and quantitative compositional information, crystallinity and actual chemical compounds formed were determined by energy dispersive spectroscopy, X-ray diffraction and X-ray photoelectron spectroscopy, respectively. The results indicated that the photoelectrochemical activity of the films depended strongly on CdS content. From the preparation of CdS/TiO2 nanocomposite films by 5, 10 and 15 dipping cycles in the chemical solutions, the best photoelectrochemical response was revealed by the 10 dipping cycles-prepared film. Galvanic couple testing demonstrated that the photoelectrochemical response of the film decreased continuously compared to that of anodized nanoporous TiO2 substrate which described by photocorrosion of CdS nanoparticles. In addition, chloride-ion attack also induced pitting corrosion leading to fluctuation and deterioration of photoelectrochemical response. CdO2 and Cd(OH)2 depositions were found as the main photocorrosion products on collapsed nanostructured-surface. The relevance between photoelectrochemical response and corrosion behavior of CdS/TiO2 nanocomposite film was discussed in detail.

Ultrasensitivity and sharp threshold theorems for multisite systems

NASA Astrophysics Data System (ADS)

Dougoud, M.; Mazza, C.; Vinckenbosch, L.

2017-02-01

This work studies the ultrasensitivity of multisite binding processes where ligand molecules can bind to several binding sites. It considers more particularly recent models involving complex chemical reactions in allosteric phosphorylation processes and for transcription factors and nucleosomes competing for binding on DNA. New statistics-based formulas for the Hill coefficient and the effective Hill coefficient are provided and necessary conditions for a system to be ultrasensitive are exhibited. It is first shown that the ultrasensitivity of binding processes can be approached using sharp-threshold theorems which have been developed in applied probability theory and statistical mechanics for studying sharp threshold phenomena in reliability theory, random graph theory and percolation theory. Special classes of binding process are then introduced and are described as density dependent birth and death process. New precise large deviation results for the steady state distribution of the process are obtained, which permits to show that switch-like ultrasensitive responses are strongly related to the multi-modality of the steady state distribution. Ultrasensitivity occurs if and only if the entropy of the dynamical system has more than one global minimum for some critical ligand concentration. In this case, the Hill coefficient is proportional to the number of binding sites, and the system is highly ultrasensitive. The classical effective Hill coefficient I is extended to a new cooperativity index I q , for which we recommend the computation of a broad range of values of q instead of just the standard one I  =  I 0.9 corresponding to the 10%-90% variation in the dose-response. It is shown that this single choice can sometimes mislead the conclusion by not detecting ultrasensitivity. This new approach allows a better understanding of multisite ultrasensitive systems and provides new tools for the design of such systems.

Z-Scheme NiTiO 3 /g-C 3 N 4 Heterojunctions with Enhanced Photoelectrochemical and Photocatalytic Performances under Visible LED Light Irradiation

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

Huang, Zhenyu; Zeng, Xiaoqiao; Li, Kai

Direct Z-scheme NiTiO3/g-C3N4 heterojunctions were successfully assembled by using simple calcination method and the photoelectrochemical and photocatalytic performance were investigated by light emitting diode (LED). The photoanode composed by the heterojunction with about 50 wt% NiTiO3 content exhibits the best photoelectrochemical activity with photoconversion efficiency up to 0.066%, which is 4.4 and 3.13 times larger than NiTiO3 or g-C3N4. The remarkably enhanced photoelectrochemical and photocatalytic activity of the heterojunction can be due to the efficiently photogenerated electron-hole separation by a Z-scheme mechanism.

Geological and technological evaluation of gold-bearing mineral material after photo-electrochemical activation leaching

NASA Astrophysics Data System (ADS)

Manzyrev, DV

2017-02-01

The paper reports the lab test results on simulation of heap leaching of unoxidized rebellious ore extracted from deep levels of Pogromnoe open pit mine, with different flowsheets and photo-electrochemically activated solutions. It has been found that pre-treatment of rebellious ore particles -10 mm in size by photo-electrochemically activated solutions at the stage preceding agglomeration with the use of rich cyanide solutions enhances gold recovery by 6%.

Photoelectrochemical determination of tert-butylhydroquinone in edible oil samples employing CdSe/ZnS quantum dots and LiTCNE.

PubMed

Monteiro, Thatyara Oliveira; Tanaka, Auro Atsushi; Damos, Flávio Santos; Luz, Rita de Cássia Silva

2017-07-15

A novel photoelectrochemical sensor was developed for determination of tert-butyl-hydroquinone (TBHQ) in edible vegetable oils, based on CdSe/ZnS core-shell quantum dots sensitized with lithium tetracyanoethylenide (LiTCNE). The CdSe/ZnS/LiTCNE photoelectrochemical sensor presented a TBHQ photocurrent about 13-fold higher and a charge transfer resistance 62-fold lower than observed for a CdSe/ZnS sensor. The photoelectrochemical sensor showed selectivity to TBHQ, with a high photocurrent for this antioxidant compared to the photocurrent responses for other phenolic antioxidants. The CdSe/ZnS/LiTCNE photoelectrochemical sensor presented a linear range from 0.6 to 250μmolL -1 , sensitivity of 0.012μALμmol -1 , and a limit of detection of 0.21μmolL -1 for TBHQ, under optimized experimental conditions. The sensor was successfully employed in the analysis of edible oil samples, with recoveries of between 98.25% and 99.83% achieved. Copyright © 2017 Elsevier Ltd. All rights reserved.

Photoelectrochemical CdSe/TiO2 nanotube array microsensor for high-resolution in-situ detection of dopamine.

PubMed

Qin, Caidie; Bai, Xue; Zhang, Yue; Gao, Kai

2018-05-03

A photoelectrochemical wire microelectrode was constructed based on the use of a TiO 2 nanotube array with electrochemically deposited CdSe semiconductor. A strongly amplified photocurrent is generated on the sensor surface. The microsensor has a response in the 0.05-20 μM dopamine (DA) concentration range and a 16.7 μM detection limit at a signal-to-noise ratio of 3. Sensitivity, recovery and reproducibility of the sensor were validated by detecting DA in spiked human urine, and satisfactory results were obtained. Graphical abstract Schematic of a sensitive photoelectrochemical microsensor based on CdSe modified TiO 2 nanotube array. The photoelectrochemical microsensor was successfully applied to the determination of dopamine in urine samples.

DNA nanosensor based on biocompatible graphene quantum dots and carbon nanotubes.

PubMed

Qian, Zhao Sheng; Shan, Xiao Yue; Chai, Lu Jing; Ma, Juan Juan; Chen, Jian Rong; Feng, Hui

2014-10-15

An ultrasensitive nanosensor based on fluorescence resonance energy transfer (FRET) between biocompatible graphene quantum dots and carbon nanotubes for DNA detection was reported. We take advantage of good biocompatibility and strong fluorescence of graphene quantum dots, base pairing specificity of DNA and unique fluorescence resonance energy transfer between graphene quantum dots and carbon nanotubes to achieve the analysis of low concentrations of DNA. Graphene quantum dots with high quantum yield up to 0.20 were prepared and served as the fluorophore of DNA probe. FRET process between graphene quantum dots-labeled probe and oxidized carbon nanotubes is easily achieved due to their efficient self-assembly through specific π-π interaction. This nanosensor can distinguish complementary and mismatched nucleic acid sequences with high sensitivity and good reproducibility. The detection method based on this nanosensor possesses a broad linear span of up to 133.0 nM and ultralow detection limit of 0.4 nM. The constructed nanosensor is expected to be highly biocompatible because of all its components with excellent biocompatibility. Copyright © 2014 Elsevier B.V. All rights reserved.

Sensitive and inexpensive digital DNA analysis by microfluidic enrichment of rolling circle amplified single-molecules

PubMed Central

Kühnemund, Malte; Hernández-Neuta, Iván; Sharif, Mohd Istiaq; Cornaglia, Matteo; Gijs, Martin A.M.

2017-01-01

Abstract Single molecule quantification assays provide the ultimate sensitivity and precision for molecular analysis. However, most digital analysis techniques, i.e. droplet PCR, require sophisticated and expensive instrumentation for molecule compartmentalization, amplification and analysis. Rolling circle amplification (RCA) provides a simpler means for digital analysis. Nevertheless, the sensitivity of RCA assays has until now been limited by inefficient detection methods. We have developed a simple microfluidic strategy for enrichment of RCA products into a single field of view of a low magnification fluorescent sensor, enabling ultra-sensitive digital quantification of nucleic acids over a dynamic range from 1.2 aM to 190 fM. We prove the broad applicability of our analysis platform by demonstrating 5-plex detection of as little as ∼1 pg (∼300 genome copies) of pathogenic DNA with simultaneous antibiotic resistance marker detection, and the analysis of rare oncogene mutations. Our method is simpler, more cost-effective and faster than other digital analysis techniques and provides the means to implement digital analysis in any laboratory equipped with a standard fluorescent microscope. PMID:28077562

Surface Interrogation Scanning Electrochemical Microscopy for a Photoelectrochemical Reaction: Water Oxidation on a Hematite Surface.

PubMed

Kim, Jae Young; Ahn, Hyun S; Bard, Allen J

2018-03-06

To understand the pathway of a photoelectrochemical (PEC) reaction, quantitative knowledge of reaction intermediates is important. We describe here surface interrogation scanning electrochemical microscopy for this purpose (PEC SI-SECM), where a light pulse to a photoactive semiconductor film at a given potential generates intermediates that are then analyzed by a tip generated titrant at known times after the light pulse. The improvements were demonstrated for photoelectrochemical water oxidation (oxygen evolution) reaction on a hematite surface. The density of photoactive sites, proposed to be Fe 4+ species, on a hematite surface was successfully quantified, and the photoelectrochemical water oxidation reaction dynamics were elucidated by time-dependent redox titration experiments. The new configuration of PEC SI-SECM should find expanded usage to understand and investigate more complicated PEC reactions with other materials.

Photoelectrochemical enzymatic biosensing of glucose using mesoporous TiO2

NASA Astrophysics Data System (ADS)

Chithralekha, P.; Kumar, V. T. Fidal; Chandra, T. S.; Roy, Somnath C.

2017-05-01

Mesoporous titania is prepared by sol-gel method. The enzymatic biosensing of glucose is done with mesoporous tiatania on ITO coated glass plates using photoelectrochemical method and mechanism of sensing is discussed.

Superlattice photoelectrodes for photoelectrochemical cells

DOEpatents

Nozik, A.J.

1985-07-03

The application of superlattice semiconductors as photoelectrodes in photoelectrochemical energy conversion processes is described. The invention is comprised of a multiple quantum well, or superlattice, semiconductor positioned on a plate and encapsulated in an insulation material, except the top surface, which is left exposed. An opening in insulation exposes a portion of the plate. When the photoelectrochemical cell is immersed in a liquid electrolyte and exposed to solar radiation, a redox reaction occurs, producing gases such as hydrogen and oxygen from a water electrolyte, which bubble off the cathode and anode portions of the cell. (LEW)

Superior photoelectrochemical properties of ZnO nanorods/poly(3-hexylthiophene) hybrid photoanodes

NASA Astrophysics Data System (ADS)

Majumder, T.; Hmar, J. J. L.; Dhar, S.; Mondal, S. P.

2017-06-01

Photoelectrochemical properties of ZnO nanorods (ZnO NRs) and poly(3-hexylthiophene) (P3HT) polymer hybrid photoanodes have been studied. The hybrid photoanodes demonstrated higher photoconversion efficiency, incident photon to current conversion efficiency (IPCE) and lower interfacial resistance compared to pristine ZnO nanorods and P3HT based electrodes. The origin of superior photoelectrochemical properties of ZnO/P3HT photoanodes has been explained using carrier transport mechanism at semiconductor/electrolyte junction. The stability of ZnO NRs/P3HT photoanode has been demonstrated.

Investigating rate-limiting barriers to nanoscale nonviral gene transfer with nanobiophotonics

NASA Astrophysics Data System (ADS)

Chen, Hunter H.

Nucleic acids are a novel class of therapeutics poised to address many unmet clinical needs. Safe and efficient delivery remains a significant challenge that has delayed the realization of the full therapeutic potential of nucleic acids. Nanoscale nonviral vectors offer an attractive alternative to viral vectors as natural and synthetic polymers or polypeptides may be rationally designed to meet the unique demands of individual applications. A mechanistic understanding of cellular barriers is necessary to develop guidelines for designing custom gene carriers which are expected to greatly impact this delivery challenge. The work herein focused on the relationships among nanocomplex stability, intracellular trafficking and unpacking kinetics, and DNA degradation. Ultrasensitive nanosensors based on QD-FRET were developed to characterize the biophysical properties of nanocomplexes and study these rate-limiting steps. Quantitative image analysis enabled the distributions of the subpopulation of condensed or released DNA to be determined within the major cellular compartments encountered during gene transfer. The steady state stability and unpacking kinetics within these compartments were found to impact transgene expression, elucidating multiple design strategies to achieve efficient gene transfer. To address enzymatic barriers, a novel two-step QD-FRET nanosensor was developed to analyze unpacking and DNA degradation simultaneously, which has not been accomplished previously. Bioresponsive strategies such as disulfide crosslinking and thermosensitivity were evaluated by QD-FRET and quantitative compartmental analysis as case studies to determine appropriate design specifications for thiolated polymers and thermoresponsive polypeptides. Relevant nanobiophotonic tools were developed as a platform to study major rate-limiting barriers to nanomedicine and demonstrated the feasibility of using mechanistic information gained from these tools to guide the rational design of gene carriers and achieve the desired properties that enable efficient gene transfer.

Dye-sensitized PS-b-P2VP-templated nickel oxide films for photoelectrochemical applications

PubMed Central

Massin, Julien; Bräutigam, Maximilian; Kaeffer, Nicolas; Queyriaux, Nicolas; Field, Martin J.; Schacher, Felix H.; Popp, Jürgen; Chavarot-Kerlidou, Murielle; Dietzek, Benjamin; Artero, Vincent

2015-01-01

Moving from homogeneous water-splitting photocatalytic systems to photoelectrochemical devices requires the preparation and evaluation of novel p-type transparent conductive photoelectrode substrates. We report here on the sensitization of polystyrene-block-poly-(2-vinylpyridine) (PS-b-P2VP) diblock copolymer-templated NiO films with an organic push–pull dye. The potential of these new templated NiO film preparations for photoelectrochemical applications is compared with NiO material templated by F108 triblock copolymers. We conclude that NiO films are promising materials for the construction of dye-sensitized photocathodes to be inserted into photoelectrochemical (PEC) cells. However, a combined effort at the interface between materials science and molecular chemistry, ideally funded within a Global Artificial Photosynthesis Project, is still needed to improve the overall performance of the photoelectrodes and progress towards economically viable PEC devices. PMID:26052420

Dye-sensitized PS-b-P2VP-templated nickel oxide films for photoelectrochemical applications.

PubMed

Massin, Julien; Bräutigam, Maximilian; Kaeffer, Nicolas; Queyriaux, Nicolas; Field, Martin J; Schacher, Felix H; Popp, Jürgen; Chavarot-Kerlidou, Murielle; Dietzek, Benjamin; Artero, Vincent

2015-06-06

Moving from homogeneous water-splitting photocatalytic systems to photoelectrochemical devices requires the preparation and evaluation of novel p-type transparent conductive photoelectrode substrates. We report here on the sensitization of polystyrene-block-poly-(2-vinylpyridine) (PS-b-P2VP) diblock copolymer-templated NiO films with an organic push-pull dye. The potential of these new templated NiO film preparations for photoelectrochemical applications is compared with NiO material templated by F108 triblock copolymers. We conclude that NiO films are promising materials for the construction of dye-sensitized photocathodes to be inserted into photoelectrochemical (PEC) cells. However, a combined effort at the interface between materials science and molecular chemistry, ideally funded within a Global Artificial Photosynthesis Project, is still needed to improve the overall performance of the photoelectrodes and progress towards economically viable PEC devices.

Metal-free hybrids of graphitic carbon nitride and nanodiamonds for photoelectrochemical and photocatalytic applications.

PubMed

Zhou, Li; Zhang, Huayang; Guo, Xiaochen; Sun, Hongqi; Liu, Shaomin; Tade, Moses O; Wang, Shaobin

2017-05-01

Graphitic carbon nitride (g-C 3 N 4 ) has been considered as a metal-free, cost-effective, eco-friendly and efficient catalyst for various photoelectrochemical applications. However, compared to conventional metal-based photocatalysts, its photocatalytic activity is still low because of the low mobility of carriers restricted by the polymer nature. Herein, a series of hybrids of g-C 3 N 4 (GCN) and nanodiamonds (NDs) were synthesized using a solvothermal method. The photoelectrochemical performance and photocatalytic efficiency of the GCN/NDs were investigated by means of the generation of photocurrent and photodegradation of methylene blue (MB) solutions under UV-visible light irradiations. In this study, the sample of GCN/ND-33% derived from 0.1g GCN and 0.05g NDs displayed the highest photocatalytic activity and the strongest photocurrent density. The mechanism of enhanced photoelectrochemical and photocatalytic performances was also discussed. Copyright © 2017 Elsevier Inc. All rights reserved.

Integrating a dual-silicon photoelectrochemical cell into a redox flow battery for unassisted photocharging.

PubMed

Liao, Shichao; Zong, Xu; Seger, Brian; Pedersen, Thomas; Yao, Tingting; Ding, Chunmei; Shi, Jingying; Chen, Jian; Li, Can

2016-05-04

Solar rechargeable flow cells (SRFCs) provide an attractive approach for in situ capture and storage of intermittent solar energy via photoelectrochemical regeneration of discharged redox species for electricity generation. However, overall SFRC performance is restricted by inefficient photoelectrochemical reactions. Here we report an efficient SRFC based on a dual-silicon photoelectrochemical cell and a quinone/bromine redox flow battery for in situ solar energy conversion and storage. Using narrow bandgap silicon for efficient photon collection and fast redox couples for rapid interface charge injection, our device shows an optimal solar-to-chemical conversion efficiency of ∼5.9% and an overall photon-chemical-electricity energy conversion efficiency of ∼3.2%, which, to our knowledge, outperforms previously reported SRFCs. The proposed SRFC can be self-photocharged to 0.8 V and delivers a discharge capacity of 730 mAh l(-1). Our work may guide future designs for highly efficient solar rechargeable devices.

Cross-Clade Ultrasensitive PCR-Based Assays To Measure HIV Persistence in Large-Cohort Studies

PubMed Central

Vandergeeten, Claire; Fromentin, Rémi; Merlini, Esther; Lawani, Mariam B.; DaFonseca, Sandrina; Bakeman, Wendy; McNulty, Amanda; Ramgopal, Moti; Michael, Nelson; Kim, Jerome H.; Ananworanich, Jintanat

2014-01-01

ABSTRACT A small pool of infected cells persists in HIV-infected individuals receiving antiretroviral therapy (ART). Here, we developed ultrasensitive assays to precisely measure the frequency of cells harboring total HIV DNA, integrated HIV DNA, and two long terminal repeat (2-LTR) circles. These assays are performed on cell lysates, which circumvents the labor-intensive step of DNA extraction, and rely on the coquantification of each HIV molecular form together with CD3 gene sequences to precisely measure cell input. Using primary isolates from HIV subtypes A, B, C, D, and CRF01_A/E, we demonstrate that these assays can efficiently quantify low target copy numbers from diverse HIV subtypes. We further used these assays to measure total HIV DNA, integrated HIV DNA, and 2-LTR circles in CD4+ T cells from HIV-infected subjects infected with subtype B. All samples obtained from ART-naive subjects were positive for the three HIV molecular forms (n = 15). Total HIV DNA, integrated HIV DNA, and 2-LTR circles were detected in, respectively, 100%, 94%, and 77% of the samples from individuals in which HIV was suppressed by ART. Higher levels of total HIV DNA and 2-LTR circles were detected in untreated subjects than individuals on ART (P = 0.0003 and P = 0.0004, respectively), while the frequency of CD4+ T cells harboring integrated HIV DNA did not differ between the two groups. These results demonstrate that these novel assays have the ability to quantify very low levels of HIV DNA of multiple HIV subtypes without the need for nucleic acid extraction, making them well suited for the monitoring of viral persistence in large populations of HIV-infected individuals. IMPORTANCE Since the discovery of viral reservoirs in HIV-infected subjects receiving suppressive ART, measuring the degree of viral persistence has been one of the greatest challenges in the field of HIV research. Here, we report the development and validation of ultrasensitive assays to measure HIV persistence in HIV-infected individuals from multiple geographical regions. These assays are relatively inexpensive, do not require DNA extraction, and can be completed in a single day. Therefore, they are perfectly adapted to monitor HIV persistence in large cohorts of HIV-infected individuals and, given their sensitivity, can be used to monitor the efficacy of therapeutic strategies aimed at interfering with HIV persistence after prolonged ART. PMID:25122785

Electrochemical and photoelectrochemical reduction of furfurals

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

Choi, Kyoung-Shin; Roylance, John James; Kubota, Stephen R.

Electrochemical cells and photoelectrochemical cells for the reduction of furfurals are provided. Also provided are methods of using the cells to carry out the reduction reactions. Using the cells and methods, furfurals can be converted into furan alcohols or linear ketones.

Ultrasensitive Detection of RNA and DNA Viruses Simultaneously Using Duplex UNDP-PCR Assay

PubMed Central

Wang, Zengguo; Zhang, Xiujuan; Zhao, Xiaomin; Du, Qian; Chang, Lingling; Tong, Dewen

2015-01-01

Mixed infection of multiple viruses is common in modern intensive pig rearing. However, there are no methods available to detect DNA and RNA viruses in the same reaction system in preclinical level. In this study, we aimed to develop a duplex ultrasensitive nanoparticle DNA probe-based PCR assay (duplex UNDP-PCR) that was able to simultaneously detect DNA and RNA viruses in the same reaction system. PCV2 and TGEV are selected as representatives of the two different types of viruses. PCV2 DNA and TGEV RNA were simultaneously released from the serum sample by boiling with lysis buffer, then magnetic beads and gold nanoparticles coated with single and/or duplex specific probes for TGEV and PCV2 were added to form a sandwich-like complex with nucleic acids released from viruses. After magnetic separation, DNA barcodes specific for PCV2 and TGEV were eluted using DTT and characterized by specific PCR assay for specific DNA barcodes subsequently. The duplex UNDP-PCR showed similar sensitivity as that of single UNDP-PCR and was able to detect 20 copies each of PCV2 and TGEV in the serum, showing approximately 250-fold more sensitivity than conventional duplex PCR/RT-PCR assays. No cross-reaction was observed with other viruses. The positive detection rate of single MMPs- and duplex MMPs-based duplex UNDP-PCR was identical, with 29.6% for PCV2, 9.3% for TGEV and 3.7% for PCV2 and TGEV mixed infection. This duplex UNDP-PCR assay could detect TGEV (RNA virus) and PCV2 (DNA virus) from large-scale serum samples simultaneously without the need for DNA/RNA extraction, purification and reverse transcription of RNA, and showed a significantly increased positive detection rate for PCV2 (29%) and TGEV (11.7%) preclinical infection than conventional duplex PCR/RT-PCR. Therefore, the established duplex UNDP-PCR is a rapid and economical detection method, exhibiting high sensitivity, specificity and reproducibility. PMID:26544710

Ultrasensitive Detection of RNA and DNA Viruses Simultaneously Using Duplex UNDP-PCR Assay.

PubMed

Huang, Yong; Xing, Na; Wang, Zengguo; Zhang, Xiujuan; Zhao, Xiaomin; Du, Qian; Chang, Lingling; Tong, Dewen

2015-01-01

Mixed infection of multiple viruses is common in modern intensive pig rearing. However, there are no methods available to detect DNA and RNA viruses in the same reaction system in preclinical level. In this study, we aimed to develop a duplex ultrasensitive nanoparticle DNA probe-based PCR assay (duplex UNDP-PCR) that was able to simultaneously detect DNA and RNA viruses in the same reaction system. PCV2 and TGEV are selected as representatives of the two different types of viruses. PCV2 DNA and TGEV RNA were simultaneously released from the serum sample by boiling with lysis buffer, then magnetic beads and gold nanoparticles coated with single and/or duplex specific probes for TGEV and PCV2 were added to form a sandwich-like complex with nucleic acids released from viruses. After magnetic separation, DNA barcodes specific for PCV2 and TGEV were eluted using DTT and characterized by specific PCR assay for specific DNA barcodes subsequently. The duplex UNDP-PCR showed similar sensitivity as that of single UNDP-PCR and was able to detect 20 copies each of PCV2 and TGEV in the serum, showing approximately 250-fold more sensitivity than conventional duplex PCR/RT-PCR assays. No cross-reaction was observed with other viruses. The positive detection rate of single MMPs- and duplex MMPs-based duplex UNDP-PCR was identical, with 29.6% for PCV2, 9.3% for TGEV and 3.7% for PCV2 and TGEV mixed infection. This duplex UNDP-PCR assay could detect TGEV (RNA virus) and PCV2 (DNA virus) from large-scale serum samples simultaneously without the need for DNA/RNA extraction, purification and reverse transcription of RNA, and showed a significantly increased positive detection rate for PCV2 (29%) and TGEV (11.7%) preclinical infection than conventional duplex PCR/RT-PCR. Therefore, the established duplex UNDP-PCR is a rapid and economical detection method, exhibiting high sensitivity, specificity and reproducibility.

A new approach to light up the application of semiconductor nanomaterials for photoelectrochemical biosensors: using self-operating photocathode as a highly selective enzyme sensor.

PubMed

Wang, Guang-Li; Liu, Kang-Li; Dong, Yu-Ming; Wu, Xiu-Ming; Li, Zai-Jun; Zhang, Chi

2014-12-15

Due to the intrinsic hole oxidation reaction occurred on the photoanode surface, currently developed photoelectrochemical biosensors suffer from the interference from coexisting reductive species (acting as electron donor) and a novel design strategy of photoelectrode for photoelectrochemical detection is urgently required. In this paper, a self-operating photocathode based on CdS quantum dots sensitized three-dimensional (3D) nanoporous NiO was designed and created, which showed highly selective and reversible response to dissolved oxygen (acting as electron acceptor) in the electrolyte solution. Using glucose oxidase (GOD) as a biocatalyst, a novel photoelectrochemical sensor for glucose was developed. The commonly encountered interferents such as H2O2, ascorbic acid (AA), cysteine (Cys), dopamine (DA), etc., almost had no effect for the cathodic photocurrent of the 3D NiO/CdS electrode, though these substances were proved to greatly influence the photocurrent of photoanodes, which indicated greatly improved selectivity of the method. The method was applied to detect glucose in real samples including serum and glucose injections with satisfactory results. This study could provide a new train of thought on designing of self-operating photocathode in photoelectrochemical sensing, promoting the application of semiconductor nanomaterials in photoelectrochemistry. Copyright © 2014 Elsevier B.V. All rights reserved.

Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoOx Catalyst.

PubMed

Kirner, Joel T; Finke, Richard G

2017-08-23

A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO x ) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO x ) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO 2 > SnO 2 ≫ WO 3 . Despite highest initial dye loading on TiO 2 films, photocurrent with hydroquinone (H 2 Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO 2 films, likely due to a higher driving force for charge injection into the more positive conduction band energy of SnO 2 . Dyeing conditions and SnO 2 film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λ max of the dye, and absorbed photon-to-current efficiency of 13% with H 2 Q, a 2-fold improvement over the previous thin-film architecture. A CoO x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO 2 , as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.

Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO x Catalyst

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

Kirner, Joel T.; Finke, Richard G.

A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO x) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO x) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO 2 > SnO 2 >> WO 3. Despite highest initial dye loading on TiO 2 films, photocurrent with hydroquinone (H 2Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO 2 films, likelymore » due to a higher driving force for charge injection into the more positive conduction band energy of SnO 2. Dyeing conditions and SnO 2 film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λmax of the dye, and absorbed photon-to-current efficiency of 13% with H 2Q, a 2-fold improvement over the previous thin-film architecture. A CoO x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO 2, as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are also discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.« less

Sensitization of Nanocrystalline Metal Oxides with a Phosphonate-Functionalized Perylene Diimide for Photoelectrochemical Water Oxidation with a CoO x Catalyst

DOE PAGES

Kirner, Joel T.; Finke, Richard G.

2017-07-20

A planar organic thin film composed of a perylene diimide dye (N,N'-bis(phosphonomethyl)-3,4,9,10-perylenediimide, PMPDI) with photoelectrochemically deposited cobalt oxide (CoO x) catalyst was previously shown to photoelectrochemically oxidize water (DOI: 10.1021/am405598w). Herein, the same PMPDI dye is studied for the sensitization of different nanostructured metal oxide (nano-MO x) films in a dye-sensitized photoelectrochemical cell architecture. Dye adsorption kinetics and saturation decreases in the order TiO 2 > SnO 2 >> WO 3. Despite highest initial dye loading on TiO 2 films, photocurrent with hydroquinone (H 2Q) sacrificial reductant in pH 7 aqueous solution is much higher on SnO 2 films, likelymore » due to a higher driving force for charge injection into the more positive conduction band energy of SnO 2. Dyeing conditions and SnO 2 film thickness were subsequently optimized to achieve light-harvesting efficiency >99% at the λmax of the dye, and absorbed photon-to-current efficiency of 13% with H 2Q, a 2-fold improvement over the previous thin-film architecture. A CoO x water-oxidation catalyst was photoelectrochemically deposited, allowing for photoelectrochemical water oxidation with a faradaic efficiency of 31 ± 7%, thus demonstrating the second example of a water-oxidizing, dye-sensitized photoelectrolysis cell composed entirely of earth-abundant materials. However, deposition of CoO x always results in lower photocurrent due to enhanced recombination between catalyst and photoinjected electrons in SnO 2, as confirmed by open-circuit photovoltage measurements. Possible future studies to enhance photoanode performance are also discussed, including alternative catalyst deposition strategies or structural derivatization of the perylene dye.« less

Photoelectrochemical Solar Cells.

ERIC Educational Resources Information Center

McDevitt, John T.

1984-01-01

This introduction to photoelectrochemical (PEC) cells reviews topics pertaining to solar energy conversion and demonstrates the ease with which a working PEC cell can be prepared with n-type silicon as the photoanode and a platinum counter electrode (both immersed in ethanolic ferrocene/ferricenium solutions). Experiments using the cell are…

Integrating a dual-silicon photoelectrochemical cell into a redox flow battery for unassisted photocharging

PubMed Central

Liao, Shichao; Zong, Xu; Seger, Brian; Pedersen, Thomas; Yao, Tingting; Ding, Chunmei; Shi, Jingying; Chen, Jian; Li, Can

2016-01-01

Solar rechargeable flow cells (SRFCs) provide an attractive approach for in situ capture and storage of intermittent solar energy via photoelectrochemical regeneration of discharged redox species for electricity generation. However, overall SFRC performance is restricted by inefficient photoelectrochemical reactions. Here we report an efficient SRFC based on a dual-silicon photoelectrochemical cell and a quinone/bromine redox flow battery for in situ solar energy conversion and storage. Using narrow bandgap silicon for efficient photon collection and fast redox couples for rapid interface charge injection, our device shows an optimal solar-to-chemical conversion efficiency of ∼5.9% and an overall photon–chemical–electricity energy conversion efficiency of ∼3.2%, which, to our knowledge, outperforms previously reported SRFCs. The proposed SRFC can be self-photocharged to 0.8 V and delivers a discharge capacity of 730 mAh l−1. Our work may guide future designs for highly efficient solar rechargeable devices. PMID:27142885

Boron-doped diamond semiconductor electrodes: Efficient photoelectrochemical CO2 reduction through surface modification

NASA Astrophysics Data System (ADS)

Roy, Nitish; Hirano, Yuiri; Kuriyama, Haruo; Sudhagar, Pitchaimuthu; Suzuki, Norihiro; Katsumata, Ken-Ichi; Nakata, Kazuya; Kondo, Takeshi; Yuasa, Makoto; Serizawa, Izumi; Takayama, Tomoaki; Kudo, Akihiko; Fujishima, Akira; Terashima, Chiaki

2016-11-01

Competitive hydrogen evolution and multiple proton-coupled electron transfer reactions limit photoelectrochemical CO2 reduction in aqueous electrolyte. Here, oxygen-terminated lightly boron-doped diamond (BDDL) thin films were synthesized as a semiconductor electron source to accelerate CO2 reduction. However, BDDL alone could not stabilize the intermediates of CO2 reduction, yielding a negligible amount of reduction products. Silver nanoparticles were then deposited on BDDL because of their selective electrochemical CO2 reduction ability. Excellent selectivity (estimated CO:H2 mass ratio of 318:1) and recyclability (stable for five cycles of 3 h each) for photoelectrochemical CO2 reduction were obtained for the optimum silver nanoparticle-modified BDDL electrode at -1.1 V vs. RHE under 222-nm irradiation. The high efficiency and stability of this catalyst are ascribed to the in situ photoactivation of the BDDL surface during the photoelectrochemical reaction. The present work reveals the potential of BDDL as a high-energy electron source for use with co-catalysts in photochemical conversion.

Unassisted photoelectrochemical water splitting exceeding 7% solar-to-hydrogen conversion efficiency using photon recycling

PubMed Central

Shi, Xinjian; Jeong, Hokyeong; Oh, Seung Jae; Ma, Ming; Zhang, Kan; Kwon, Jeong; Choi, In Taek; Choi, Il Yong; Kim, Hwan Kyu; Kim, Jong Kyu; Park, Jong Hyeok

2016-01-01

Various tandem cell configurations have been reported for highly efficient and spontaneous hydrogen production from photoelectrochemical solar water splitting. However, there is a contradiction between two main requirements of a front photoelectrode in a tandem cell configuration, namely, high transparency and high photocurrent density. Here we demonstrate a simple yet highly effective method to overcome this contradiction by incorporating a hybrid conductive distributed Bragg reflector on the back side of the transparent conducting substrate for the front photoelectrochemical electrode, which functions as both an optical filter and a conductive counter-electrode of the rear dye-sensitized solar cell. The hybrid conductive distributed Bragg reflectors were designed to be transparent to the long-wavelength part of the incident solar spectrum (λ>500 nm) for the rear solar cell, while reflecting the short-wavelength photons (λ<500 nm) which can then be absorbed by the front photoelectrochemical electrode for enhanced photocurrent generation. PMID:27324578

Ion implantation system and process for ultrasensitive determination of target isotopes

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

Farmer, III, Orville T.; Liezers, Martin

2016-09-13

A system and process are disclosed for ultrasensitive determination of target isotopes of analytical interest in a sample. Target isotopes may be implanted in an implant area on a high-purity substrate to pre-concentrate the target isotopes free of contaminants. A known quantity of a tracer isotope may also be implanted. Target isotopes and tracer isotopes may be determined in a mass spectrometer. The present invention provides ultrasensitive determination of target isotopes in the sample.

Photoelectrochemical fabrication of spectroscopic diffraction gratings, phase 2

NASA Technical Reports Server (NTRS)

Rauh, R. David; Carrabba, Michael M.; Li, Jianguo; Cartland, Robert F.; Hachey, John P.; Mathew, Sam

1990-01-01

This program was directed toward the production of Echelle diffraction gratings by a light-driven, electrochemical etching technique (photoelectrochemical etching). Etching is carried out in single crystal materials, and the differential rate of etching of the different crystallographic planes used to define the groove profiles. Etching of V-groove profiles was first discovered by us during the first phase of this project, which was initially conceived as a general exploration of photoelectrochemical etching techniques for grating fabrication. This highly controllable V-groove etching process was considered to be of high significance for producing low pitch Echelles, and provided the basis for a more extensive Phase 2 investigation.

Research Update: Photoelectrochemical water splitting and photocatalytic hydrogen production using ferrites (MFe2O4) under visible light irradiation

NASA Astrophysics Data System (ADS)

Dillert, Ralf; Taffa, Dereje H.; Wark, Michael; Bredow, Thomas; Bahnemann, Detlef W.

2015-10-01

The utilization of solar light for the photoelectrochemical and photocatalytic production of molecular hydrogen from water is a scientific and technical challenge. Semiconductors with suitable properties to promote solar-driven water splitting are a desideratum. A hitherto rarely investigated group of semiconductors are ferrites with the empirical formula MFe2O4 and related compounds. This contribution summarizes the published results of the experimental investigations on the photoelectrochemical and photocatalytic properties of these compounds. It will be shown that the potential of this group of compounds in regard to the production of solar hydrogen has not been fully explored yet.

Stretchable Electronic Sensors of Nanocomposite Network Films for Ultrasensitive Chemical Vapor Sensing.

PubMed

Yan, Hong; Zhong, Mengjuan; Lv, Ze; Wan, Pengbo

2017-11-01

A stretchable, transparent, and body-attachable chemical sensor is assembled from the stretchable nanocomposite network film for ultrasensitive chemical vapor sensing. The stretchable nanocomposite network film is fabricated by in situ preparation of polyaniline/MoS 2 (PANI/MoS 2 ) nanocomposite in MoS 2 suspension and simultaneously nanocomposite deposition onto prestrain elastomeric polydimethylsiloxane substrate. The assembled stretchable electronic sensor demonstrates ultrasensitive sensing performance as low as 50 ppb, robust sensing stability, and reliable stretchability for high-performance chemical vapor sensing. The ultrasensitive sensing performance of the stretchable electronic sensors could be ascribed to the synergistic sensing advantages of MoS 2 and PANI, higher specific surface area, the reliable sensing channels of interconnected network, and the effectively exposed sensing materials. It is expected to hold great promise for assembling various flexible stretchable chemical vapor sensors with ultrasensitive sensing performance, superior sensing stability, reliable stretchability, and robust portability to be potentially integrated into wearable electronics for real-time monitoring of environment safety and human healthcare. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Photoelectrochemical Cell of Hybrid Regioregular POLY(3-HEXYLTHIOPHENE-2,5-DIYL) and Molybdenum Disulfide Film

NASA Astrophysics Data System (ADS)

Abdelmola, Fatmaelzahraa M.; Ram, Manoj K.; Takshi, Arash; Stafanakos, Elias; Kumar, Ashok; Goswami, D. Yogi

The photoelectrochemical cell attracts attention worldwide due to conversion of optical energy into electricity, production of hydrogen through water splitting and use in photodetector and photo-sensor applications. We have been working on the photochemical cell based on regioregular polyhexylthiophenes hybrid-structured films for photoelectrochemical and photovoltaic applications. This paper discusses the hybrid film studies on regioregular poly(3-hexylthiophene-2,5-diyl) (P3HT) with 2D molybdenum disulfide (MoS2) for photoelectrochemical cell. The hybrid P3HT/MoS2 films deposited over indium tin oxide (ITO)-coated glass plate or n-type silicon substrates were characterized using FTIR, UV/vis, electrochemical and scanning electron microscopy (SEM) techniques. The optical measurements showed a higher absorption magnitude with low reflection properties of P3HT/MoS2 hybrid films revealing a superior photocurrent compared to both P3HT and MoS2 films. The P3HT/MoS2 hybrid-based photoelectrochemical cell yielded a short-circuit current (Isc) of 183.16μAṡcm-2, open-circuit voltage (Voc) of 0.92V, fill factor (FF) of 25% and power conversion efficiency (η) of 0.18% under the light intensity of 242Wṡm-2. The estimated power conversion efficiency and fill factor are comparable to organic-based photovoltaic devices.

Enhanced photoelectrochemical aptasensing platform based on exciton energy transfer between CdSeTe alloyed quantum dots and SiO2@Au nanocomposites.

PubMed

Fan, Gao-Chao; Zhu, Hua; Shen, Qingming; Han, Li; Zhao, Ming; Zhang, Jian-Rong; Zhu, Jun-Jie

2015-04-25

High-efficient exciton energy transfer between CdSeTe alloyed quantum dots and SiO2@Au nanocomposites was applied to develop an enhanced photoelectrochemical aptasensing platform with ultrahigh sensitivity, good selectivity, reproducibility and stability.

A fluorescent aptasensor for amplified label-free detection of adenosine triphosphate based on core-shell Ag@SiO2 nanoparticles.

PubMed

Song, Quanwei; Peng, Manshu; Wang, Le; He, Dacheng; Ouyang, Jin

2016-03-15

The novel, facile and universal aptamer-based methods for the highly sensitive and selective fluorescence detection of important biomolecules have attracted considerable interest. Here, we present a label-free aptasensor for adenosine triphosphate (ATP) detection in aqueous solutions by using an ultra-sensitive nucleic acid stain PicoGreen (PG) as a fluorescent indicator and core-shell Ag@SiO2 nanoparticles (NPs) as a metal-enhanced fluorescence (MEF) platform. In the presence of ATP, the complementary DNA (cDNA)/aptamer duplexes confined onto the Ag@SiO2 NPs surface can release their aptamers into the buffered solution, causing a significant reduction in fluorescence intensity. By virtue of the amplified fluorescence signal, this aptasensor toward ATP can achieve a detection limit of 14.2 nM with a wide linear range and exhibit a good assay performance in complex biological samples. This sensing approach is cost-effective and efficient because it avoids the fluorescence labeling process and the use of any enzymes. Hence, this method may offer an alternative tool for determining the concentrations of ATP in biochemical and biomedical research. Copyright © 2015 Elsevier B.V. All rights reserved.

A naked-eye colorimetric "PCR developer"

NASA Astrophysics Data System (ADS)

Valentini, Paola; Pompa, Pier Paolo

2016-04-01

Despite several advances in molecular biology and diagnostics, Polymerase Chain Reaction (PCR) is currently the gold standard for nucleic acids amplification and detection, due to its versatility, low-cost and universality, with estimated <10 billion reactions per year and a worldwide market of several billion dollars/year. Nevertheless, PCR still relies on the laborious, time-consuming, and multi-step gel electrophoresis-based detection, which includes gel casting, electrophoretic run, gel staining, and gel visualization. In this work, we propose a "PCR developer", namely a universal one-step, one-tube method, based on controlled aggregation of gold nanoparticles (AuNPs), to detect PCR products by naked eye in few minutes, with no need for any instrumentation. We demonstrated the specificity and sensitivity of the PCR developer on different model targets, suitable for a qualitative detection in real-world diagnostics (i.e., gene rearrangements, genetically modified organisms, and pathogens). The PCR developer proved to be highly specific and ultra-sensitive, discriminating down to few copies of HIV viral DNA, diluted in an excess of interfering human genomic DNA, which is a clinically relevant viral load. Hence, it could be a valuable tool for both academic research and clinical applications.

Target-responsive DNA-capped nanocontainer used for fabricating universal detector and performing logic operations

PubMed Central

Wu, Li; Ren, Jinsong; Qu, Xiaogang

2014-01-01

Nucleic acids have become a powerful tool in nanotechnology because of their controllable diverse conformational transitions and adaptable higher-order nanostructure. Using single-stranded DNA probes as the pore-caps for various target recognition, here we present an ultrasensitive universal electrochemical detection system based on graphene and mesoporous silica, and achieve sensitivity with all of the major classes of analytes and simultaneously realize DNA logic gate operations. The concept is based on the locking of the pores and preventing the signal-reporter molecules from escape by target-induced the conformational change of the tailored DNA caps. The coupling of ‘waking up’ gatekeeper with highly specific biochemical recognition is an innovative strategy for the detection of various targets, able to compete with classical methods which need expensive instrumentation and sophisticated experimental operations. The present study has introduced a new electrochemical signal amplification concept and also adds a new dimension to the function of graphene-mesoporous materials hybrids as multifunctional nanoscale logic devices. More importantly, the development of this approach would spur further advances in important areas, such as point-of-care diagnostics or detection of specific biological contaminations, and hold promise for use in field analysis. PMID:25249622

Strategically functionalized carbon nanotubes as the ultrasensitive electrochemical probe for picomolar detection of sildenafil citrate (Viagra).

PubMed

Gopalan, Anantha Iyengar; Lee, Kwang Pill; Komathi, Shanmugasundaram

2011-02-15

The present work demonstrates the utility of the functionalized carbon nanotubes, poly(4-aminobenzene sulfonic acid) (PABS) grafted multiwalled carbon nanotubes, MWNT-g-PABS, as an electrode modifier towards achieving ultrasensitive detection of a model drug, sildenafil citrate (SC). PABS units in MWNT-g-PABS interact with SC, pre-concentrate and accumulate at the surface. The electron transduction from SC to electrode is augmented via MWNT-g-PABS. As a result, the MWNT-g-PABS modified electrode exhibited ultrasensitive (57.7 μA/nM) and selective detection of SC with a detection limit of 4.7 pM. The present work provides scope towards targeting ultrasensitivity for the detection of biomolecules/drug through rational design and incorporation of appropriate chemical components to carbon nanotubes. Copyright © 2010 Elsevier B.V. All rights reserved.

Nano-enabled bioanalytical approaches to ultrasensitive detection of low abundance single nucleotide polymorphisms

PubMed Central

Lapitan Jr., Lorico D. S.; Guo, Yuan

2015-01-01

Single nucleotide polymorphisms (SNPs) constitute the most common types of genetic variations in the human genome. A number of SNPs have been linked to the development of life threatening diseases including cancer, cardiovascular diseases and neurodegenerative diseases. The ability for ultrasensitive and accurate detection of low abundant disease-related SNPs in bodily fluids (e.g. blood, serum, etc.) holds a significant value in the development of non-invasive future biodiagnostic tools. Over the past two decades, nanomaterials have been utilized in a myriad of biosensing applications due to their ability of detecting extremely low quantities of biologically important biomarkers with high sensitivity and accuracy. Of particular interest is the application of such technologies in the detection of SNPs. The use of various nanomaterials, coupled with different powerful signal amplification strategies, has paved the way for a new generation of ultrasensitive SNP biodiagnostic assays. Over the past few years, several ultrasensitive SNP biosensors capable of detecting specific targets down to the ultra-low regimes (ca. aM and below) and therefore holding great promises for early clinical diagnosis of diseases have been developed. This mini review will highlight some of the most recent, significant advances in nanomaterial-based ultrasensitive SNP sensing technologies capable of detecting specific targets on the attomolar (10–18 M) regime or below. In particular, the design of novel, powerful signal amplification strategies that hold the key to the ultrasensitivity is highlighted. PMID:25785914

Hydrogen production by photoelectrolytic decomposition of H2O using solar energy

NASA Technical Reports Server (NTRS)

Rauh, R. D.; Alkaitis, S. A.; Buzby, J. M.; Schiff, R.

1980-01-01

Photoelectrochemical systems for the efficient decomposition of water are discussed. Semiconducting d band oxides which would yield the combination of stability, low electron affinity, and moderate band gap essential for an efficient photoanode are sought. The materials PdO and Fe-xRhxO3 appear most likely. Oxygen evolution yields may also be improved by mediation of high energy oxidizing agents, such as CO3(-). Examination of several p type semiconductors as photocathodes revealed remarkable stability for p-GaAs, and also indicated p-CdTe as a stable H2 photoelectrode. Several potentially economical schemes for photoelectrochemical decomposition of water were examined, including photoelectrochemical diodes and two stage, four photon processes.

Research Update: Photoelectrochemical water splitting and photocatalytic hydrogen production using ferrites (MFe{sub 2}O{sub 4}) under visible light irradiation

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

Dillert, Ralf; Laboratorium für Nano- und Quantenengineering, Gottfried Wilhelm Leibniz Universität Hannover, Schneiderberg 39, 30167 Hannover; Taffa, Dereje H.

2015-10-01

The utilization of solar light for the photoelectrochemical and photocatalytic production of molecular hydrogen from water is a scientific and technical challenge. Semiconductors with suitable properties to promote solar-driven water splitting are a desideratum. A hitherto rarely investigated group of semiconductors are ferrites with the empirical formula MFe{sub 2}O{sub 4} and related compounds. This contribution summarizes the published results of the experimental investigations on the photoelectrochemical and photocatalytic properties of these compounds. It will be shown that the potential of this group of compounds in regard to the production of solar hydrogen has not been fully explored yet.

Integrated photoelectrochemical cell and system having a liquid electrolyte

DOEpatents

Deng, Xunming; Xu, Liwei

2010-07-06

An integrated photoelectrochemical (PEC) cell generates hydrogen and oxygen from water while being illuminated with radiation. The PEC cell employs a liquid electrolyte, a multi-junction photovoltaic electrode, and a thin ion-exchange membrane. A PEC system and a method of making such PEC cell and PEC system are also disclosed.

Photoelectrochemical generation of hydrogen and electricity from hydrazine hydrate using BiVO4 electrodes.

PubMed

Pilli, Satyananda Kishore; Summers, Kodi; Chidambaram, Dev

2015-06-07

This study demonstrates solar driven oxidation of hydrazine hydrate and the simultaneous production of hydrogen and electricity in photoelectrochemical cells and photofuel cells, respectively, using a visible light active molybdenum doped BiVO4 photoelectrode. The developed photoelectrodes exhibited tremendous efficiency towards anodic oxidation of hydrous hydrazine with continuous and stable hydrogen evolution at the Pt cathode under benign pH and zero bias conditions. Significantly, the photofuel cell containing hydrazine hydrate fuel has generated electricity with a high open circuit potential of 0.8 V. The presence of bicarbonate ions in the electrolyte has played a significant role in enhancing the kinetics of photoelectrochemical oxidation of hydrazine and improved the hydrogen and electricity generation efficiency thus avoiding the integration of an oxidation electrocatalyst. In addition, molybdenum doped BiVO4 as a possible photoelectrochemical hydrazine sensor has been investigated and the electrode photocurrent was found to be linearly dependent on the concentration of the hydrazine hydrate in the range of 20-90 mM with a correlation coefficient of 0.9936.

Photoelectrochemical Complexes of Fucoxanthin-Chlorophyll Protein for Bio-Photovoltaic Conversion with a High Open-Circuit Photovoltage.

PubMed

Zhang, Tianning; Liu, Cheng; Dong, Wenjing; Wang, Wenda; Sun, Yan; Chen, Xin; Yang, Chunhong; Dai, Ning

2017-12-05

Open-circuit photovoltage (V oc ) is among the critical parameters for achieving an efficient light-to-charge conversion in existing solar photovoltaic devices. Natural photosynthesis exploits light-harvesting chlorophyll (Chl) protein complexes to transfer sunlight energy efficiently. We describe the exploitation of photosynthetic fucoxanthin-chlorophyll protein (FCP) complexes for realizing photoelectrochemical cells with a high V oc . An antenna-dependent photocurrent response and a V oc up to 0.72 V are observed and demonstrated in the bio-photovoltaic devices fabricated with photosynthetic FCP complexes and TiO 2 nanostructures. Such high V oc is determined by fucoxanthin in FCP complexes, and is rarely found in photoelectrochemical cells with other natural light-harvesting antenna. We think that the FCP-based bio-photovoltaic conversion will provide an opportunity to fabricate environmental benign photoelectrochemical cells with high V oc , and also help improve the understanding of the essential physics behind the light-to-charge conversion in photosynthetic complexes. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Ultrasensitive detection enabled by nonlinear magnetization of nanomagnetic labels

DOE PAGES

Nikitin, M. P.; Orlov, A. V.; Sokolov, I. L.; ...

2018-01-01

The magnetically soft, disk-shaped particles reveal a strong nonlinearity of the magnetization process due to irreversible transitions from the spin vortex to single-domain configuration, enabling their ultrasensitive detection in high-background environments.

Ultra-sensitive transducer advances micro-measurement range

NASA Technical Reports Server (NTRS)

Rogallo, V. L.

1964-01-01

An ultrasensitive piezoelectric transducer, that converts minute mechanical forces into electrical impulses, measures the impact of micrometeoroids against space vehicles. It has uniform sensitivity over the entire target area and a high degree of stability.

Spectral sensitization of nanocrystalline solar cells

DOEpatents

Spitler, Mark T.; Ehret, Anne; Stuhl, Louis S.

2002-01-01

This invention relates to dye sensitized polycrystalline photoelectrochemical solar cells for use in energy transduction from light to electricity. It concerns the utility of highly absorbing organic chromophores as sensitizers in such cells and the degree to which they may be utilized alone and in combination to produce an efficient photoelectrochemical cell, e.g., a regenerative solar cell.

Cellulose nanofiber-templated three-dimension TiO 2 hierarchical nanowire network for photoelectrochemical photoanode

Treesearch

Zhaodong Li; Chunhua Yao; Fei Wang; Zhiyong Cai; Xudong Wang

2014-01-01

Three dimensional (3D) nanostructures with extremely large porosity possess a great promise for the development of high-performance energy harvesting storage devices. In this paper, we developed a high-density 3D TiO2 fiber-nanorod (NR) heterostructure for photoelectrochemical (PEC) water splitting. The hierarchical structure was synthesized on a...

Influence of deposition time on the surface morphology and photoelectrochemical properties of copper doped titania nanotubes prepared by electrodeposition

NASA Astrophysics Data System (ADS)

Mahmud, M. A.; Chin, L. Y.; Khusaimi, Z.; Zainal, Z.

2018-05-01

A great attention has focused on Cu doped titania nanotubes (Cu/TiNT) as a versatile advance material since it can be employed in various promising technological applications. The current study reported on the influence of various deposition times on the surface morphology and photoelectrochemical properties of Cu/TiNT via electrodeposition technique. Cu loaded on the TiNT surface was detected with prolonged deposition time. For photoelectrochemical (PEC) measurement, the highest responsive photocurrent density was obtained at 20 minutes with 54.3 µA/cm2. Too long duration (40 mins) resulted in poor performance of Cu/TiNT as only 22.6 µA/cm2 of photocurrent being generated.

A novel electrochemiluminescence strategy for ultrasensitive DNA assay using luminol functionalized gold nanoparticles multi-labeling and amplification of gold nanoparticles and biotin-streptavidin system.

PubMed

Chai, Ying; Tian, Dayong; Wang, Wei; Cui, Hua

2010-10-28

Luminol functionalized gold nanoparticles were used as labels for electrochemiluminescence signal amplification and an ultrasensitive, highly selective, convenient, low cost DNA detection strategy was developed.

The role of ultra-thin SiO2 layers in metal-insulator-semiconductor (MIS) photoelectrochemical devices (Presentation Recording)

NASA Astrophysics Data System (ADS)

Esposito, Daniel V.

2015-08-01

Solid-state junctions based on a metal-insulator-semiconductor (MIS) architecture are of great interest for a number of optoelectronic applications such as photovoltaics, photoelectrochemical cells, and photodetection. One major advantage of the MIS junction compared to the closely related metal-semiconductor junction, or Schottky junction, is that the thin insulating layer (1-3 nm thick) that separates the metal and semiconductor can significantly reduce the density of undesirable interfacial mid-gap states. The reduction in mid-gap states helps "un-pin" the junction, allowing for significantly higher built-in-voltages to be achieved. A second major advantage of the MIS junction is that the thin insulating layer can also protect the underlying semiconductor from corrosion in an electrochemical environment, making the MIS architecture well-suited for application in (photo)electrochemical applications. In this presentation, discontinuous Si-based MIS junctions immersed in electrolyte are explored for use as i.) photoelectrodes for solar-water splitting in photoelectrochemical cells (PECs) and ii.) position-sensitive photodetectors. The development and optimization of MIS photoelectrodes for both of these applications relies heavily on understanding how processing of the thin SiO2 layer impacts the properties of nano- and micro-scale MIS junctions, as well as the interactions of the insulating layer with the electrolyte. In this work, we systematically explore the effects of insulator thickness, synthesis method, and chemical treatment on the photoelectrochemical and electrochemical properties of these MIS devices. It is shown that electrolyte-induced inversion plays a critical role in determining the charge carrier dynamics within the MIS photoelectrodes for both applications.

Highly-efficient capillary photoelectrochemical water splitting using cellulose nanofiber-templated TiO 2 photoanodes

Treesearch

Zhaodong Li; Chunhua Yao; Yanhao Yu; Zhiyong Cai; Xudong Wang

2014-01-01

Among current endeavors to explore renewable energy technologies, photoelectrochemical (PEC) water splitting holds great promise for conversion of solar energy to chemical energy. [ 1–4 ] Light absorption, charge separation, and appropriate interfacial redox reactions are three key aspects that lead to highly efficient solar energy conversion. [ 5–10 ] Therefore,...

Macroscale Transformation Optics Enabled by Photoelectrochemical Etching.

PubMed

Barth, David S; Gladden, Christopher; Salandrino, Alessandro; O'Brien, Kevin; Ye, Ziliang; Mrejen, Michael; Wang, Yuan; Zhang, Xiang

2015-10-28

Photoelectrochemical etching of silicon can be used to form lateral refractive index gradients for transformation optical devices. This technique allows the fabrication of macroscale devices with large refractive index gradients. Patterned porous layers can also be lifted from the substrate and transferred to other materials, creating more possibilities for novel devices. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum-size-controlled photoelectrochemical etching of semiconductor nanostructures

DOEpatents

Fischer, Arthur J.; Tsao, Jeffrey Y.; Wierer, Jr., Jonathan J.; Xiao, Xiaoyin; Wang, George T.

2016-03-01

Quantum-size-controlled photoelectrochemical (QSC-PEC) etching provides a new route to the precision fabrication of epitaxial semiconductor nanostructures in the sub-10-nm size regime. For example, quantum dots (QDs) can be QSC-PEC-etched from epitaxial InGaN thin films using narrowband laser photoexcitation, and the QD sizes (and hence bandgaps and photoluminescence wavelengths) are determined by the photoexcitation wavelength.

Zinc oxide inverse opal electrodes modified by glucose oxidase for electrochemical and photoelectrochemical biosensor.

PubMed

Xia, Lei; Song, Jian; Xu, Ru; Liu, Dali; Dong, Biao; Xu, Lin; Song, Hongwei

2014-09-15

The ZnO inverse opal photonic crystals (IOPCs) were synthesized by the sol-gel method using the polymethylmethacrylate (PMMA) as a template. For glucose detection, glucose oxidase (GOD) was further immobilized on the inwall and surface of the IOPCs. The biosensing properties toward glucose of the Nafion/GOD/ZnO IOPCs modified FTO electrodes were carefully studied and the results indicated that the sensitivity of ZnO IOPCs modified electrode was 18 times than reference electrode due to the large surface area and uniform porous structure of ZnO IOPCs. Moreover, photoelectrochemical detection for glucose using the electrode was realized and the sensitivity approached to 52.4 µA mM(-1) cm(-2), which was about four times to electrochemical detection (14.1 µA mM(-1) cm(-2)). It indicated that photoelectrochemical detection can highly improve the sensor performance than conventional electrochemical method. It also exhibited an excellent anti-interference property and a good stability at the same time. This work provides a promising approach for realizing excellent photoelectrochemical biosensor of similar semiconductor photoelectric material. Copyright © 2014 Elsevier B.V. All rights reserved.

An Inexpensive Co-Intercalated Layered Double Hydroxide Composite with Electron Donor-Acceptor Character for Photoelectrochemical Water Splitting

PubMed Central

Zheng, Shufang; Lu, Jun; Yan, Dongpeng; Qin, Yumei; Li, Hailong; Evans, David G.; Duan, Xue

2015-01-01

In this paper, the inexpensive 4,4-diaminostilbene-2,2-disulfonate (DAS) and 4,4-dinitro-stilbene-2,2- disulfonate (DNS) anions with arbitrary molar ratios were successfully co-intercalated into Zn2Al-layered double hydroxides (LDHs). The DAS(50%)-DNS/LDHs composite exhibited the broad UV-visible light absorption and fluorescence quenching, which was a direct indication of photo-induced electron transfer (PET) process between the intercalated DAS (donor) and DNS (acceptor) anions. This was confirmed by the matched HOMO/LUMO energy levels alignment of the intercalated DAS and DNS anions, which was also compatible for water splitting. The DAS(50%)-DNS/LDHs composite was fabricated as the photoanode and Pt as the cathode. Under the UV-visible light illumination, the enhanced photo-generated current (4.67 mA/cm2 at 0.8 V vs. SCE) was generated in the external circuit, and the photoelectrochemical water split was realized. Furthermore, this photoelectrochemical water splitting performance had excellent crystalline, electrochemical and optical stability. Therefore, this novel inorganic/organic hybrid photoanode exhibited potential application prospect in photoelectrochemical water splitting. PMID:26174201

Cu2O-tipped ZnO nanorods with enhanced photoelectrochemical performance for CO2 photoreduction

NASA Astrophysics Data System (ADS)

Iqbal, Muzaffar; Wang, Yanjie; Hu, Haifeng; He, Meng; Hassan Shah, Aamir; Lin, Lin; Li, Pan; Shao, Kunjuan; Reda Woldu, Abebe; He, Tao

2018-06-01

The design of Cu2O-tipped ZnO nanorods is proposed here aiming at enhanced photoelectrochemical properties. The tip-selective deposition of Cu2O is confirmed by scanning transmission electron microscopy (STEM). The photoinduced charge behavior like charge generation, separation and transport has been thoroughly studied by UV-vis absorption analysis and different photoelectrochemical characterizations, including transient photocurrent, incident photon-to-current efficiency (IPCE), electrochemical impedance spectroscopy (EIS), intensity-modulated photocurrent spectroscopy (IMPS), and Mott-Schottky measurements. The photoelectrochemical characterizations clearly indicate that ZnO/Cu2O structures exhibit much higher performance than pristine ZnO, due to the formation of p-n junction, as well as the tip selective growth of Cu2O on ZnO. Photocatalytic CO2 reduction in aqueous solution under UV-visible light illumination shows that CO is the main product, and with the increase of the Cu2O content in the heterostructure, the CO yield increases. This work shows that Cu2O-tipped ZnO nanorods possess improved behavior of charge generation, separation and transport, which may work as a potential candidate for photocatalytic CO2 reduction.

Two-step electrodeposition to fabricate the p-n heterojunction of a Cu2O/BiVO4 photoanode for the enhancement of photoelectrochemical water splitting.

PubMed

Bai, Shouli; Liu, Jingchao; Cui, Meng; Luo, Ruixian; He, Jing; Chen, Aifan

2018-05-15

A Cu2O/BiVO4 p-n heterojunction based photoanode in photoelectrochemical (PEC) water splitting is fabricated by a two-step electrodeposition method on an FTO substrate followed by annealing treatment. The structures and properties of the samples are characterized by XRD, FESEM, HRTEM, XPS and UV-visible spectra. The photoelectrochemical activity of the photoanode in water oxidation has been investigated and measured in a three electrode quartz cell system; the obtained maximum photocurrent density of 1.72 mA cm-2 at 1.23 V vs. RHE is 4.5 times higher than that of pristine BiVO4 thin films (∼0.38 mA cm-2). The heterojunction based photoanode also exhibits a tremendous cathodic shift of the onset potential (∼420 mV) and enhancement in the IPCE value by more than 4-fold. The enhanced photoelectrochemical properties of the Cu2O/BiVO4 photoelectrode are attributed to the efficient separation of the photoexcited electron-hole pairs caused by the inner electronic field (IEF) of the p-n heterojunction.

Photoelectrochemical modulation of neuronal activity with free-standing coaxial silicon nanowires

NASA Astrophysics Data System (ADS)

Parameswaran, Ramya; Carvalho-de-Souza, João L.; Jiang, Yuanwen; Burke, Michael J.; Zimmerman, John F.; Koehler, Kelliann; Phillips, Andrew W.; Yi, Jaeseok; Adams, Erin J.; Bezanilla, Francisco; Tian, Bozhi

2018-02-01

Optical methods for modulating cellular behaviour are promising for both fundamental and clinical applications. However, most available methods are either mechanically invasive, require genetic manipulation of target cells or cannot provide subcellular specificity. Here, we address all these issues by showing optical neuromodulation with free-standing coaxial p-type/intrinsic/n-type silicon nanowires. We reveal the presence of atomic gold on the nanowire surfaces, likely due to gold diffusion during the material growth. To evaluate how surface gold impacts the photoelectrochemical properties of single nanowires, we used modified quartz pipettes from a patch clamp and recorded sustained cathodic photocurrents from single nanowires. We show that these currents can elicit action potentials in primary rat dorsal root ganglion neurons through a primarily atomic gold-enhanced photoelectrochemical process.

Ultrasensitive dual-channel detection of matrix metalloproteinase-2 in human serum using gold-quantum dot core-satellite nanoprobes.

PubMed

Zheng, Tingting; Zhang, Rui; Zhang, Qingfeng; Tan, Tingting; Zhang, Kui; Zhu, Jun-Jie; Wang, Hui

2013-09-18

We have developed a robust enzymatic peptide cleavage-based assay for the ultrasensitive dual-channel detection of matrix metalloproteinase-2 (MMP-2) in human serum using gold-quantum dot (Au-QD) core-satellite nanoprobes.

Ultrasensitive detection of oncogenic human papillomavirus in oropharyngeal tissue swabs.

PubMed

Isaac, Andre; Kostiuk, Morris; Zhang, Han; Lindsay, Cameron; Makki, Fawaz; O'Connell, Daniel A; Harris, Jeffrey R; Cote, David W J; Seikaly, Hadi; Biron, Vincent L

2017-01-14

The incidence of oropharyngeal squamous cell carcinoma (OPSCC) caused by oncogenic human papillomavirus (HPV) is rising worldwide. HPV-OPSCC is commonly diagnosed by RT-qPCR of HPV E6 and E7 oncoproteins or by p16 immunohistochemistry (IHC). Droplet digital PCR (ddPCR) has been recently reported as an ultra-sensitive and highly precise method of nucleic acid quantification for biomarker analysis. To validate the use of a minimally invasive assay for detection of oncogenic HPV based on oropharyngeal swabs using ddPCR. Secondary objectives were to compare the accuracy of ddPCR swabs to fresh tissue p16 IHC and RT-qPCR, and to compare the cost of ddPCR with p16 IHC. We prospectively included patients with p16 + oral cavity/oropharyngeal cancer (OC/OPSCC), and two control groups: p16 - OC/OPSCC patients, and healthy controls undergoing tonsillectomy. All underwent an oropharyngeal swab with ddPCR for quantitative detection of E6 and E7 mRNA. Surgical specimens had p16 IHC performed. Agreement between ddPCR and p16 IHC was determined for patients with p16 positive and negative OC/OPSCC as well as for healthy control patients. The sensitivity and specificity of ddPCR of oropharyngeal swabs were calculated against p16 IHC for OPSCC. 122 patients were included: 36 patients with p16 + OPSCC, 16 patients with p16 - OPSCC, 4 patients with p16 + OCSCC, 41 patients with p16 - OCSCC, and 25 healthy controls. The sensitivity and specificity of ddPCR of oropharyngeal swabs against p16 IHC were 92 and 98% respectively, using 20-50 times less RNA than that required for conventional RT-qPCR. Overall agreement between ddPCR of tissue swabs and p16 of tumor tissue was high at ĸ = 0.826 [0.662-0.989]. Oropharyngeal swabs analyzed by ddPCR is a quantitative, rapid, and effective method for minimally invasive oncogenic HPV detection. This assay represents the most sensitive and accurate mode of HPV detection in OPSCC without a tissue biopsy in the available literature.

Experimenting with Photoelectrochemical Cells in Drinking Straws: Practical Aids for Learning about Solar Energy in School or at Home

ERIC Educational Resources Information Center

Appleyard, S. J.

2008-01-01

Photoelectrochemical cells using dye-sensitized ZnO with a Cu[superscript 2+]/Fe[superscript 2+]/Fe[superscript 3+] electrolyte can be easily made at home or in a school classroom with household chemicals and other readily available materials. The cells, which are made with wire housed within plastic drinking straws, have open-circuit voltages of…

Investigation of Cadmium Selenide Photoelectrochemical Cells.

DTIC Science & Technology

1980-01-01

80-4 _INVESTIGATION OF C ADMIUM ,ELENIDE .PHOTOELECTROCHEMICAL CELLS by R.A. Sawchuk and D.R. Snelling Energy Systems Section AccsseionPar Energy ...cadmium selenide photo- anodes, a polysulphide redox’electrolyte and an in situ energy storage com- partment were evaluated at DREO. The...electron-hole recombination.- centers, and shorting to the nickel substrate. The concept of in situ energy storage was not successfully demonstrated. It is

Ultrasensitive Electrochemical Detection of mRNA Using Branched DNA Amplifiers

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

Mao, Xun; Liu, Guodong; Wang, Shengfu

2008-11-01

We describe here an ultrasensitive electrochemical detection of m RNA protocol without RNA purification and PCR amplification. The new m RNA electrical detection capability is coupled to the amplification feature of branched DNA (bDNA) technology and with the nagnetic beads based electrochemical bioassay.

Direct electrochemistry and electrocatalysis of a glucose oxidase-functionalized bioconjugate as a trace label for ultrasensitive detection of thrombin.

PubMed

Bai, Lijuan; Yuan, Ruo; Chai, Yaqin; Yuan, Yali; Wang, Yan; Xie, Shunbi

2012-11-18

For the first time, a glucose oxidase-functionalized bioconjugate was prepared and served as a new trace label through its direct electrochemistry and electrocatalysis in a sandwich-type electrochemical aptasensor for ultrasensitive detection of thrombin.

Evaluation and optimization of mass transport of redox species in silicon microwire-array photoelectrodes

PubMed Central

Xiang, Chengxiang; Meng, Andrew C.; Lewis, Nathan S.

2012-01-01

Physical integration of a Ag electrical contact internally into a metal/substrate/microstructured Si wire array/oxide/Ag/electrolyte photoelectrochemical solar cell has produced structures that display relatively low ohmic resistance losses, as well as highly efficient mass transport of redox species in the absence of forced convection. Even with front-side illumination, such wire-array based photoelectrochemical solar cells do not require a transparent conducting oxide top contact. In contact with a test electrolyte that contained 50 mM/5.0 mM of the cobaltocenium+/0 redox species in CH3CN–1.0 M LiClO4, when the counterelectrode was placed in the solution and separated from the photoelectrode, mass transport restrictions of redox species in the internal volume of the Si wire array photoelectrode produced low fill factors and limited the obtainable current densities to 17.6 mA cm-2 even under high illumination. In contrast, when the physically integrated internal Ag film served as the counter electrode, the redox couple species were regenerated inside the internal volume of the photoelectrode, especially in regions where depletion of the redox species due to mass transport limitations would have otherwise occurred. This behavior allowed the integrated assembly to operate as a two-terminal, stand-alone, photoelectrochemical solar cell. The current density vs. voltage behavior of the integrated photoelectrochemical solar cell produced short-circuit current densities in excess of 80 mA cm-2 at high light intensities, and resulted in relatively low losses due to concentration overpotentials at 1 Sun illumination. The integrated wire array-based device architecture also provides design guidance for tandem photoelectrochemical cells for solar-driven water splitting. PMID:22904185

Hot Hole Collection and Photoelectrochemical CO2 Reduction with Plasmonic Au/p-GaN Photocathodes.

PubMed

DuChene, Joseph S; Tagliabue, Giulia; Welch, Alex J; Cheng, Wen-Hui; Atwater, Harry A

2018-04-11

Harvesting nonequilibrium hot carriers from plasmonic-metal nanostructures offers unique opportunities for driving photochemical reactions at the nanoscale. Despite numerous examples of hot electron-driven processes, the realization of plasmonic systems capable of harvesting hot holes from metal nanostructures has eluded the nascent field of plasmonic photocatalysis. Here, we fabricate gold/p-type gallium nitride (Au/p-GaN) Schottky junctions tailored for photoelectrochemical studies of plasmon-induced hot-hole capture and conversion. Despite the presence of an interfacial Schottky barrier to hot-hole injection of more than 1 eV across the Au/p-GaN heterojunction, plasmonic Au/p-GaN photocathodes exhibit photoelectrochemical properties consistent with the injection of hot holes from Au nanoparticles into p-GaN upon plasmon excitation. The photocurrent action spectrum of the plasmonic photocathodes faithfully follows the surface plasmon resonance absorption spectrum of the Au nanoparticles and open-circuit voltage studies demonstrate a sustained photovoltage during plasmon excitation. Comparison with Ohmic Au/p-NiO heterojunctions confirms that the vast majority of hot holes generated via interband transitions in Au are sufficiently hot to inject above the 1.1 eV interfacial Schottky barrier at the Au/p-GaN heterojunction. We further investigated plasmon-driven photoelectrochemical CO 2 reduction with the Au/p-GaN photocathodes and observed improved selectivity for CO production over H 2 evolution in aqueous electrolytes. Taken together, our results offer experimental validation of photoexcited hot holes more than 1 eV below the Au Fermi level and demonstrate a photoelectrochemical platform for harvesting hot carriers to drive solar-to-fuel energy conversion.

Fabrication of A/R-TiO2 composite for enhanced photoelectrochemical performance: Solar hydrogen generation and dye degradation

NASA Astrophysics Data System (ADS)

Mahadik, Mahadeo A.; An, Gil Woo; David, Selvaraj; Choi, Sun Hee; Cho, Min; Jang, Jum Suk

2017-12-01

Anatase/rutile TiO2 nanorods composites were prepared by a facile hydrothermal method followed by dip coating method using titanium isopropoxide in acetic acid and ethanol solvent. The effects of the titanium isopropoxide precursor concentration, on the formation of dip coated anatase/rutile TiO2 nanorods composite were systematically explored. The growth of anatase on rutile TiO2 nanorods can be controlled by varying the titanium isopropoxide concentration. The morphological study reveals that anatase TiO2 nanograins formed on the surface of rutile TiO2 nanorod arrays through dip coating method. Photoelectrochemical analyses showed that the enhancement of the photocatalytic activities of the samples is affected by the anatase nanograins present on the rutile TiO2 nanorods, which can induce the separation of electrons and holes. To interpret the photoelectrochemical behaviors, the prepared photoelectrodes were applied in photoelectrochemical solar hydrogen generation and orange II dye degradation. The optimized photocurrent density of 1.8 mA cm-2 and the 625 μmol hydrogen generation was observed for 10 mM anatase/rutile TiO2 NRs composites. Additionally, 96% removal of the orange II dye was achieved within 5 h during oxidative degradation under solar light irradiation. One of the benefits of high specific surface area and the efficient photogenerated charge transport in the anatase/rutile TiO2 nanorod composite improves the photoelectrochemical hydrogen generation and orange dye degradation compared to the rutile TiO2. Thus, our strategy provides a promising, stable, and low cost alternative to existing photocatalysts and is expected to attract considerable attention for industrial applications.

Photoelectrochemical processes in polymer-tethered CdSe nanocrystals.

PubMed

Shallcross, R Clayton; D'Ambruoso, Gemma D; Pyun, Jeffrey; Armstrong, Neal R

2010-03-03

We demonstrate the electrochemical capture of CdSe semiconductor nanocrystals (NCs), with thiophene-terminated carboxylic acid capping ligands, at the surfaces of electrodeposited poly(thiophene) films (i) poly((diethyl)propylenedixoythiophene), P(Et)(2)ProDOT; (ii) poly(propylenedioxythiophene), PProDOT; and (iii) poly(ethylenedioxythiophene), PEDOT, coupled with the exploration of their photoelectrochemical properties. Host polymer films were created using a kinetically controlled electrodeposition protocol on activated indium-tin oxide electrodes (ITO), producing conformal films that facilitate high rates of electron transfer. ProDOT-terminated, ligand-capped CdSe-NCs were captured at the outer surface of the host polymer films using a unique pulse-potential step electrodeposition protocol, providing for nearly close-packed monolayers of the NCs at the host polymer/solution interface. These polymer-confined CdSe NCs were used as sensitizers in the photoelectrochemical reduction of methyl viologen (MV(+2)). High internal quantum efficiencies (IQEs) are estimated for photoelectrochemical sensitized MV(+2) reduction using CdSe NCs ranging from 3.1 to 7.0 nm diameters. Cathodic photocurrent at high MV(+2) concentrations are limited by the rate of hole-capture by the host polymer from photoexcited NCs. The rate of this hole-capture process is determined by (a) the onset potential for reductive dedoping of the host polymer film; (b) the concentration ratio of neutral to oxidized forms of the host polymer ([P(n)]/[P(ox)]); and (c) the NC diameter, which controls its valence band energy, E(VB). These relationships are consistent with control of photoinduced electron transfer by Marcus-like excess free energy relationships. Our electrochemical assembly methods provide an enabling route to the capture of functional NCs in conducting polymer hosts in both photoelectrochemical and photovoltaic energy conversion systems.

Chemically Modified Metal Oxide Nanostructure for Photoelectrochemical Water Splitting

NASA Astrophysics Data System (ADS)

Wang, Gongming

Hydrogen gas is chemical fuel with high energy density, and represents a clean, renewable and carbon-free burning fuel, which has the potential to solve the more and more urgent energy crisis in today's society. Inspired by natural photosynthesis, artificial photosynthesis to generate hydrogen energy has attracted a lot of attentions in the field of chemistry, physics and material. Photoelectrochemical water splitting based on semiconductors represents a green and low cost method to generate hydrogen fuel. However, the current overall efficiency of solar to hydrogen is quite low, due to some intrinsic limitations such as bandgap, diffusion distance, carrier lifetime and photostability of semiconductors. Although nanostructured semiconductors can improve their photoelectrochemical water splitting performance to some extent, by increasing electrolyte accessible area and shortening minority carrier diffusion distance, nanostructure engineering cannot change their intrinsic electronic properties. Recent development in chemically modified nanostructures such as surface catalyst decoration, element doping, plasmonic modification and interfacial hetero-junction design have led to significant advancement in the photoelectrochemical water splitting, by improving surface reaction kinetics and charge separation, transportation and collection efficiency. In this thesis, I will give a detailed discussion on the chemically modified metal oxide nanostructures for photoelectrocemical hydrogen generation, with a focus on the element doping, hydrogen treatment and catalyst modification. I have demonstrated nitrogen doping on ZnO and Ti doping on hematite can improve their photoelectrochemical performance. In addition, we found hydrogen treatment is a general and effective method to improve the photocatalytic performance, by increasing their carrier desities. Hydrogen treatment has been demonstrated on TiO2, WO3 and BiVO4. In the end, we also used electrochemical catalyt to modify these metal oxide photoelectrode for waste water treatment and chemical fuel generation.

Enhanced photoelectrochemical and photocatalytic activity of WO3-surface modified TiO2 thin film

NASA Astrophysics Data System (ADS)

Qamar, Mohammad; Drmosh, Qasem; Ahmed, Muhammad I.; Qamaruddin, Muhammad; Yamani, Zain H.

2015-02-01

Development of nanostructured photocatalysts for harnessing solar energy in energy-efficient and environmentally benign way remains an important area of research. Pure and WO3-surface modified thin films of TiO2 were prepared by magnetron sputtering on indium tin oxide glass, and photoelectrochemical and photocatalytic activities of these films were studied. TiO2 particles were <50 nm, while deposited WO3 particles were <20 nm in size. An enhancement in the photocurrent was observed when the TiO2 surface was modified WO3 nanoparticles. Effect of potential, WO3 amount, and radiations of different wavelengths on the photoelectrochemical activity of TiO2 electrodes was investigated. Photocatalytic activity of TiO2 and WO3-modified TiO2 for the decolorization of methyl orange was tested.

Nanostructured hematite thin films for photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Maabong, Kelebogile; Machatine, Augusto G. J.; Mwankemwa, Benard S.; Braun, Artur; Bora, Debajeet K.; Toth, Rita; Diale, Mmantsae

2018-04-01

Nanostructured hematite thin films prepared by dip coating technique were investigated for their photoelectrochemical activity for generation of hydrogen from water splitting. Structural, morphological and optical analyses of the doped/undoped films were performed by X-ray diffraction, high resolution field emission-scanning electron microscopy, UV-vis spectrophotometry and Raman spectroscopy. The photoelectrochemical measurements of the films showed enhanced photoresponse and cathodic shift of the onset potential upon Ti doping indicating improved transfer of photoholes at the semiconductor-electrolyte interface. Films doped with 1 at% Ti produced 0.72 mA/cm2 at 1.23 V vs RHE which is 2 times higher than current density for the pure film (0.30 mA/cm2, at 1.23 V vs RHE). Gas chromatography analysis of the films also showed enhanced hydrogen evolution at 1 at% Ti with respect to pure film.

DNA-engineered chiroplasmonic heteropyramids for ultrasensitive detection of mercuryion

USDA-ARS?s Scientific Manuscript database

In this study, plasmonic heteropyramids (HPs) made from two different sized gold nanoparticles (Au NPs) and five ssDNA sequences and their application for ultrasensitive detection of mercury ion (Hg2+) were demonstrated. Four ssDNA sequences were used as building blocks to form apyramidal DNA frame,...

A temperature-controlled photoelectrochemical cell for quantitative product analysis.

PubMed

Corson, Elizabeth R; Creel, Erin B; Kim, Youngsang; Urban, Jeffrey J; Kostecki, Robert; McCloskey, Bryan D

2018-05-01

In this study, we describe the design and operation of a temperature-controlled photoelectrochemical cell for analysis of gaseous and liquid products formed at an illuminated working electrode. This cell is specifically designed to quantitatively analyze photoelectrochemical processes that yield multiple gas and liquid products at low current densities and exhibit limiting reactant concentrations that prevent these processes from being studied in traditional single chamber electrolytic cells. The geometry of the cell presented in this paper enables front-illumination of the photoelectrode and maximizes the electrode surface area to electrolyte volume ratio to increase liquid product concentration and hence enhances ex situ spectroscopic sensitivity toward them. Gas is bubbled through the electrolyte in the working electrode chamber during operation to maintain a saturated reactant concentration and to continuously mix the electrolyte. Gaseous products are detected by an in-line gas chromatograph, and liquid products are analyzed ex situ by nuclear magnetic resonance. Cell performance was validated by examining carbon dioxide reduction on a silver foil electrode, showing comparable results both to those reported in the literature and identical experiments performed in a standard parallel-electrode electrochemical cell. To demonstrate a photoelectrochemical application of the cell, CO 2 reduction experiments were carried out on a plasmonic nanostructured silver photocathode and showed different product distributions under dark and illuminated conditions.

Solar-rechargeable battery based on photoelectrochemical water oxidation: Solar water battery

PubMed Central

Kim, Gonu; Oh, Misol; Park, Yiseul

2016-01-01

As an alternative to the photoelectrochemical water splitting for use in the fuel cells used to generate electrical power, this study set out to develop a solar energy rechargeable battery system based on photoelectrochemical water oxidation. We refer to this design as a “solar water battery”. The solar water battery integrates a photoelectrochemical cell and battery into a single device. It uses a water oxidation reaction to simultaneously convert and store solar energy. With the solar water battery, light striking the photoelectrode causes the water to be photo-oxidized, thus charging the battery. During the discharge process, the solar water battery reduces oxygen to water with a high coulombic efficiency (>90%) and a high average output voltage (0.6 V). Because the reduction potential of oxygen is more positive [E0 (O2/H2O) = 1.23 V vs. NHE] than common catholytes (e.g., iodide, sulfur), a high discharge voltage is produced. The solar water battery also exhibits a superior storage ability, maintaining 99% of its specific discharge capacitance after 10 h of storage, without any evidence of self-discharge. The optimization of the cell design and configuration, taking the presence of oxygen in the cell into account, was critical to achieving an efficient photocharge/discharge. PMID:27629362

Solar-rechargeable battery based on photoelectrochemical water oxidation: Solar water battery.

PubMed

Kim, Gonu; Oh, Misol; Park, Yiseul

2016-09-15

As an alternative to the photoelectrochemical water splitting for use in the fuel cells used to generate electrical power, this study set out to develop a solar energy rechargeable battery system based on photoelectrochemical water oxidation. We refer to this design as a "solar water battery". The solar water battery integrates a photoelectrochemical cell and battery into a single device. It uses a water oxidation reaction to simultaneously convert and store solar energy. With the solar water battery, light striking the photoelectrode causes the water to be photo-oxidized, thus charging the battery. During the discharge process, the solar water battery reduces oxygen to water with a high coulombic efficiency (>90%) and a high average output voltage (0.6 V). Because the reduction potential of oxygen is more positive [E(0) (O2/H2O) = 1.23 V vs. NHE] than common catholytes (e.g., iodide, sulfur), a high discharge voltage is produced. The solar water battery also exhibits a superior storage ability, maintaining 99% of its specific discharge capacitance after 10 h of storage, without any evidence of self-discharge. The optimization of the cell design and configuration, taking the presence of oxygen in the cell into account, was critical to achieving an efficient photocharge/discharge.

A temperature-controlled photoelectrochemical cell for quantitative product analysis

NASA Astrophysics Data System (ADS)

Corson, Elizabeth R.; Creel, Erin B.; Kim, Youngsang; Urban, Jeffrey J.; Kostecki, Robert; McCloskey, Bryan D.

2018-05-01

In this study, we describe the design and operation of a temperature-controlled photoelectrochemical cell for analysis of gaseous and liquid products formed at an illuminated working electrode. This cell is specifically designed to quantitatively analyze photoelectrochemical processes that yield multiple gas and liquid products at low current densities and exhibit limiting reactant concentrations that prevent these processes from being studied in traditional single chamber electrolytic cells. The geometry of the cell presented in this paper enables front-illumination of the photoelectrode and maximizes the electrode surface area to electrolyte volume ratio to increase liquid product concentration and hence enhances ex situ spectroscopic sensitivity toward them. Gas is bubbled through the electrolyte in the working electrode chamber during operation to maintain a saturated reactant concentration and to continuously mix the electrolyte. Gaseous products are detected by an in-line gas chromatograph, and liquid products are analyzed ex situ by nuclear magnetic resonance. Cell performance was validated by examining carbon dioxide reduction on a silver foil electrode, showing comparable results both to those reported in the literature and identical experiments performed in a standard parallel-electrode electrochemical cell. To demonstrate a photoelectrochemical application of the cell, CO2 reduction experiments were carried out on a plasmonic nanostructured silver photocathode and showed different product distributions under dark and illuminated conditions.

In situ Ni-doping during cathodic electrodeposition of hematite for excellent photoelectrochemical performance of nanostructured nickel oxide-hematite p-n junction photoanode

NASA Astrophysics Data System (ADS)

Phuan, Yi Wen; Ibrahim, Elyas; Chong, Meng Nan; Zhu, Tao; Lee, Byeong-Kyu; Ocon, Joey D.; Chan, Eng Seng

2017-01-01

Nanostructured nickel oxide-hematite (NiO/α-Fe2O3) p-n junction photoanodes synthesized from in situ doping of nickel (Ni) during cathodic electrodeposition of hematite were successfully demonstrated. A postulation model was proposed to explain the fundamental mechanism of Ni2+ ions involved, and the eventual formation of NiO on the subsurface region of hematite that enhanced the potential photoelectrochemical water oxidation process. Through this study, it was found that the measured photocurrent densities of the Ni-doped hematite photoanodes were highly dependent on the concentrations of Ni dopant used. The optimum Ni dopant at 25 M% demonstrated an excellent photoelectrochemical performance of 7-folds enhancement as compared to bare hematite photoanode. This was attributed to the increased electron donor density through the p-n junction and thus lowering the energetic barrier for water oxidation activity at the optimum Ni dopant concentration. Concurrently, the in situ Ni-doping of hematite has also lowered the photogenerated charge carrier transfer resistance as measured using the electrochemical impedance spectroscopy. It is expected that the fundamental understanding gained through this study is helpful for the rational design and construction of highly efficient photoanodes for application in photoelectrochemical process.

Simple Methods and Rational Design for Enhancing Aptamer Sensitivity and Specificity

PubMed Central

Kalra, Priya; Dhiman, Abhijeet; Cho, William C.; Bruno, John G.; Sharma, Tarun K.

2018-01-01

Aptamers are structured nucleic acid molecules that can bind to their targets with high affinity and specificity. However, conventional SELEX (Systematic Evolution of Ligands by EXponential enrichment) methods may not necessarily produce aptamers of desired affinity and specificity. Thus, to address these questions, this perspective is intended to suggest some approaches and tips along with novel selection methods to enhance evolution of aptamers. This perspective covers latest novel innovations as well as a broad range of well-established approaches to improve the individual binding parameters (aptamer affinity, avidity, specificity and/or selectivity) of aptamers during and/or post-SELEX. The advantages and limitations of individual aptamer selection methods and post-SELEX optimizations, along with rational approaches to overcome these limitations are elucidated in each case. Further the impact of chosen selection milieus, linker-systems, aptamer cocktails and detection modules utilized in conjunction with target-specific aptamers, on the overall assay performance are discussed in detail, each with its own advantages and limitations. The simple variations suggested are easily available for facile implementation during and/or post-SELEX to develop ultrasensitive and specific assays. Finally, success studies of established aptamer-based assays are discussed, highlighting how they utilized some of the suggested methodologies to develop commercially successful point-of-care diagnostic assays. PMID:29868605

Simple Methods and Rational Design for Enhancing Aptamer Sensitivity and Specificity.

PubMed

Kalra, Priya; Dhiman, Abhijeet; Cho, William C; Bruno, John G; Sharma, Tarun K

2018-01-01

Aptamers are structured nucleic acid molecules that can bind to their targets with high affinity and specificity. However, conventional SELEX (Systematic Evolution of Ligands by EXponential enrichment) methods may not necessarily produce aptamers of desired affinity and specificity. Thus, to address these questions, this perspective is intended to suggest some approaches and tips along with novel selection methods to enhance evolution of aptamers. This perspective covers latest novel innovations as well as a broad range of well-established approaches to improve the individual binding parameters (aptamer affinity, avidity, specificity and/or selectivity) of aptamers during and/or post-SELEX. The advantages and limitations of individual aptamer selection methods and post-SELEX optimizations, along with rational approaches to overcome these limitations are elucidated in each case. Further the impact of chosen selection milieus, linker-systems, aptamer cocktails and detection modules utilized in conjunction with target-specific aptamers, on the overall assay performance are discussed in detail, each with its own advantages and limitations. The simple variations suggested are easily available for facile implementation during and/or post-SELEX to develop ultrasensitive and specific assays. Finally, success studies of established aptamer-based assays are discussed, highlighting how they utilized some of the suggested methodologies to develop commercially successful point-of-care diagnostic assays.

DNA detection and single nucleotide mutation identification using SERS for molecular diagnostics and global health

NASA Astrophysics Data System (ADS)

Ngo, Hoan T.; Gandra, Naveen; Fales, Andrew M.; Taylor, Steve M.; Vo-Dinh, Tuan

2017-02-01

Nucleic acid-based molecular diagnostics at the point-of-care (POC) and in resource-limited settings is still a challenge. We present a sensitive yet simple DNA detection method with single nucleotide polymorphism (SNP) identification capability. The detection scheme involves sandwich hybridization of magnetic beads conjugated with capture probes, target sequences, and ultrabright surface-enhanced Raman Scattering (SERS) nanorattles conjugated with reporter probes. Upon hybridization, the sandwich probes are concentrated at the detection focus controlled by a magnetic system for SERS measurements. The ultrabright SERS nanorattles, consisting of a core and a shell with resonance Raman reporters loaded in the gap space between the core and the shell, serve as SERS tags for ultrasensitive signal detection. Specific DNA sequences of the malaria parasite Plasmodium falciparum and dengue virus 1 (DENV1) were used as the model marker system. Detection limit of approximately 100 attomoles was achieved. Single nucleotide polymorphism (SNP) discrimination of wild type malaria DNA and mutant malaria DNA, which confers resistance to artemisinin drugs, was also demonstrated. The results demonstrate the molecular diagnostic potential of the nanorattle-based method to both detect and genotype infectious pathogens. The method's simplicity makes it a suitable candidate for molecular diagnosis at the POC and in resource-limited settings.

Chemiluminescent labels released from long spacer arm-functionalized magnetic particles: a novel strategy for ultrasensitive and highly selective detection of pathogen infections.

PubMed

Yang, Haowen; Liang, Wenbiao; He, Nongyue; Deng, Yan; Li, Zhiyang

2015-01-14

Previously, the unique advantages provided by chemiluminescence (CL) and magnetic particles (MPs) have resulted in the development of many useful nucleic acid detection methods. CL is highly sensitive, but when applied to MPs, its intensity is limited by the inner filter-like effect arising from excess dark MPs. Herein, we describe a modified strategy whereby CL labels are released from MPs to eliminate this negative effect. This approach relies on (1) the magnetic capture of target molecules on long spacer arm-functionalized magnetic particles (LSA-MPs), (2) the conjugation of streptavidin-alkaline phosphatase (SA-AP) to biotinylated amplicons of target pathogens, (3) the release of CL labels (specifically, AP tags), and (4) the detection of the released labels. CL labels were released from LSA-MPs through LSA ultrasonication or DNA enzymolysis, which proved to be the superior method. In contrast to conventional MPs, LSA-MPs exhibited significantly improved CL detection, because of the introduction of LSA, which was made of water-soluble carboxymethylated β-1,3-glucan. Detection of hepatitis B virus with this technique revealed a low detection limit of 50 fM, high selectivity, and excellent reproducibility. Thus, this approach may hold great potential for early stage clinical diagnosis of infectious diseases.

Theoretical Investigation of Device Aspects of Semiconductor Superlattices.

DTIC Science & Technology

1983-09-01

n-i-p-i devices include bulk field effect transistors, ultrasensitive or ultrafast IR photodetectors , tunable light-emitting devices, and ultrafast...transistor4 ultrasensitive or ultrafast IR photodetectors , tunable light-emitt tg devices, and ultrafast optical modulators. Particularlylppealing...differential conductivity ( NDC ) ......................... 19 3.2.2. Spontaneous and stimulated FIR emission from interlayer transitions

Dual-sensing porphyrin-containing copolymer nanosensor as full-spectrum colorimeter and ultra-sensitive thermometer.

PubMed

Yan, Qiang; Yuan, Jinying; Kang, Yan; Cai, Zhinan; Zhou, Lilin; Yin, Yingwu

2010-04-28

A porphyrin-containing copolymer has dual-sensing in response to metal ions and temperature as a novel nanosensor. Triggered by ions, the sensor exhibits full-color tunable behavior as a cationic detector and colorimeter. Responding to temperature, the sensor displays an "isothermal" thermochromic point as an ultra-sensitive thermometer.

Evaluation of a novel ultra-sensitive nanoparticle probe-based assay for ricin detection.

PubMed

Yin, Hui-qiong; Jia, Min-xian; Shi, Li-jun; Liu, Jun; Wang, Rui; Lv, Mao-min; Ma, Yu-yuan; Zhao, Xiong; Zhang, Jin-gang

2014-01-01

A gold nanoparticle (GNP) probe-based assay (GNPA) modified from the bio-barcode assay (BCA) was developed for ultrasensitive detection of ricin, a potential biothreat agent. In the GNPA, a chain of ricin was captured by a GNP probe coated with polyclonal antibodies and single-stranded signal DNA. A magnetic microparticle (MMP) probe coated with ricin A chain monoclonal antibody was then added to form an immuno-complex. After being magnetically separated, the immuno-complex containing the single-stranded signal DNA was characterized by PCR and real-time PCR. A detection limit of 10(-2) fg/ml was determined for the ricin A chain; this is eight orders of magnitude more sensitive than that achieved with an ELISA and two orders more sensitive than that obtained with the BCA. The coefficients of variation (CV) of the intra- and inter-assay values ranged from 3.82-6.46%. The results here show that this novel assay is an ultrasensitive method for detection of ricin proteins and may be suitable for the ultrasensitive detection of other proteins.

Rolling chain amplification based signal-enhanced electrochemical aptasensor for ultrasensitive detection of ochratoxin A.

PubMed

Huang, Lin; Wu, Jingjing; Zheng, Lei; Qian, Haisheng; Xue, Feng; Wu, Yucheng; Pan, Daodong; Adeloju, Samuel B; Chen, Wei

2013-11-19

A novel electrochemical aptasensor is described for rapid and ultrasensitive detection of ochratoxin A (OTA) based on signal enhancement with rolling circle amplification (RCA). The primer for RCA was designed to compose of a two-part sequence, one part of the aptamer sequence directed against OTA while the other part was complementary to the capture probe on the electrode surface. In the presence of target OTA, the primer, originally hybridized with the RCA padlock, is replaced to combine with OTA. This induces the inhibition of RCA and decreases the OTA sensing signal obtained with the electrochemical aptasensor. Under the optimized conditions, ultrasensitive detection of OTA was achieved with a limit of detection (LOD) of 0.065 ppt (pg/mL), which is much lower than previously reported. The electrochemical aptasensor was also successfully applied to the determination of OTA in wine samples. This ultrasensitive electrochemical aptasensor is of great practical importance in food safety and could be widely extended to the detection of other toxins by replacing the sequence of the recognition aptamer.

Nanobody medicated immunoassay for ultrasensitive detection of cancer biomarker alpha-fetoprotein.

PubMed

Chen, Jing; He, Qing-hua; Xu, Yang; Fu, Jin-heng; Li, Yan-ping; Tu, Zhui; Wang, Dan; Shu, Mei; Qiu, Yu-lou; Yang, Hong-wei; Liu, Yuan-yuan

2016-01-15

Immunoassay for cancer biomarkers plays an important role in cancer prevention and early diagnosis. To the development of immunoassay, the quality and stability of applied antibody is one of the key points to obtain reliability and high sensitivity for immunoassay. The main purpose of this study was to develop a novel immunoassay for ultrasensitive detection of cancer biomarker alpha-fetoprotein (AFP) based on nanobody against AFP. Two nanobodies which bind to AFP were selected from a phage display nanobody library by biopanning strategy. The prepared nanobodies are clonable, thermally stable and applied in both sandwich enzyme linked immunoassay (ELISA) and immuno-PCR assay for ultrasensitive detection of AFP. The limit detection of sandwich ELISA setup with optimized nanobodies was 0.48ng mL(-1), and the half of saturation concentration (SC50) value was 6.68±0.56ng mL(-1). These nanobodies were also used to develop an immuno-PCR assay for ultrasensitive detection of AFP, its limit detection values was 0.005ng mL(-1), and the linear range was 0.01-10,000ng mL(-1). These established immunoassays based on nanobodies were highly specific to AFP and with negligible cross reactivity with other tested caner biomarkers. Furthermore, this novel concept of nanobodies mediated immunoassay may provide potential applications in a general method for the ultrasensitive detection of various cancer biomarkers. Copyright © 2015 Elsevier B.V. All rights reserved.

Capillary photoelectrode structures for photoelectrochemical and photocatalytic cells

DOEpatents

Wang, Xudong; Li, Zhaodong; Cai, Zhiyong; Yao, Chunhua

2017-05-02

Photocatalytic structures having a capillary-force based electrolyte delivery system are provided. Also provided are photoelectrochemical and photocatalytic cells incorporating the structures and methods for using the cells to generate hydrogen and/or oxygen from water. The photocatalytic structures use an electrolyte-transporting strip comprising a porous network of cellulose nanofibers to transport electrolyte from a body of the electrolyte to a porous photoelectrode or a porous photocatalytic substrate via capillary force.

Efficiency limits for photoelectrochemical water-splitting

DOE PAGES

Fountaine, Katherine T.; Lewerenz, Hans Joachim; Atwater, Harry A.

2016-12-02

Theoretical limiting efficiencies have a critical role in determining technological viability and expectations for device prototypes, as evidenced by the photovoltaics community’s focus on detailed balance. However, due to their multicomponent nature, photoelectrochemical devices do not have an equivalent analogue to detailed balance, and reported theoretical efficiency limits vary depending on the assumptions made. Here we introduce a unified framework for photoelectrochemical device performance through which all previous limiting efficiencies can be understood and contextualized. Ideal and experimentally realistic limiting efficiencies are presented, and then generalized using five representative parameters—semiconductor absorption fraction, external radiative efficiency, series resistance, shunt resistance andmore » catalytic exchange current density—to account for imperfect light absorption, charge transport and catalysis. Finally, we discuss the origin of deviations between the limits discussed herein and reported water-splitting efficiencies. This analysis provides insight into the primary factors that determine device performance and a powerful handle to improve device efficiency.« less

Photoelectrochemical water splitting in separate oxygen and hydrogen cells

NASA Astrophysics Data System (ADS)

Landman, Avigail; Dotan, Hen; Shter, Gennady E.; Wullenkord, Michael; Houaijia, Anis; Maljusch, Artjom; Grader, Gideon S.; Rothschild, Avner

2017-06-01

Solar water splitting provides a promising path for sustainable hydrogen production and solar energy storage. One of the greatest challenges towards large-scale utilization of this technology is reducing the hydrogen production cost. The conventional electrolyser architecture, where hydrogen and oxygen are co-produced in the same cell, gives rise to critical challenges in photoelectrochemical water splitting cells that directly convert solar energy and water to hydrogen. Here we overcome these challenges by separating the hydrogen and oxygen cells. The ion exchange in our cells is mediated by auxiliary electrodes, and the cells are connected to each other only by metal wires, enabling centralized hydrogen production. We demonstrate hydrogen generation in separate cells with solar-to-hydrogen conversion efficiency of 7.5%, which can readily surpass 10% using standard commercial components. A basic cost comparison shows that our approach is competitive with conventional photoelectrochemical systems, enabling safe and potentially affordable solar hydrogen production.

Manipulation of charge transfer and transport in plasmonic-ferroelectric hybrids for photoelectrochemical applications

PubMed Central

Wang, Zhijie; Cao, Dawei; Wen, Liaoyong; Xu, Rui; Obergfell, Manuel; Mi, Yan; Zhan, Zhibing; Nasori, Nasori; Demsar, Jure; Lei, Yong

2016-01-01

Utilizing plasmonic nanostructures for efficient and flexible conversion of solar energy into electricity or fuel presents a new paradigm in photovoltaics and photoelectrochemistry research. In a conventional photoelectrochemical cell, consisting of a plasmonic structure in contact with a semiconductor, the type of photoelectrochemical reaction is determined by the band bending at the semiconductor/electrolyte interface. The nature of the reaction is thus hard to tune. Here instead of using a semiconductor, we employed a ferroelectric material, Pb(Zr,Ti)O3 (PZT). By depositing gold nanoparticle arrays and PZT films on ITO substrates, and studying the photocurrent as well as the femtosecond transient absorbance in different configurations, we demonstrate an effective charge transfer between the nanoparticle array and PZT. Most importantly, we show that the photocurrent can be tuned by nearly an order of magnitude when changing the ferroelectric polarization in PZT, demonstrating a versatile and tunable system for energy harvesting. PMID:26753764

ZnO/CuO/M (M = Ag, Au) Hierarchical Nanostructure by Successive Photoreduction Process for Solar Hydrogen Generation.

PubMed

Kwon, Jinhyeong; Cho, Hyunmin; Jung, Jinwook; Lee, Habeom; Hong, Sukjoon; Yeo, Junyeob; Han, Seungyong; Ko, Seung Hwan

2018-05-12

To date, solar energy generation devices have been widely studied to meet a clean and sustainable energy source. Among them, water splitting photoelectrochemical cell is regarded as a promising energy generation way for splitting water molecules and generating hydrogen by sunlight. While many nanostructured metal oxides are considered as a candidate, most of them have an improper bandgap structure lowering energy transition efficiency. Herein, we introduce a novel wet-based, successive photoreduction process that can improve charge transfer efficiency by surface plasmon effect for a solar-driven water splitting device. The proposed process enables to fabricate ZnO/CuO/Ag or ZnO/CuO/Au hierarchical nanostructure, having an enhanced electrical, optical, photoelectrochemical property. The fabricated hierarchical nanostructures are demonstrated as a photocathode in the photoelectrochemical cell and characterized by using various analytic tools.

Band structure engineering of TiO2 nanowires by n-p codoping for enhanced visible-light photoelectrochemical water-splitting.

PubMed

Zhang, Daoyu; Yang, Minnan

2013-11-14

The advantages of one-dimensional nanostructures, such as excellent charge separation and charge transport, low charge carrier recombination losses and so on, render them the photocatalysts of choice for many applications that exploit solar energy. In this work, based on very recently synthesized ultrathin anatase TiO2 nanowires, we explore the possibility of these wires as photocatalysts for photoelectrochemical water-splitting via the mono-doping (C, N, V, and Cr) and n-p codoping (C&V, C&Cr, N&V, and N&Cr) schemes. Our first-principles calculations predict that the C&Cr and C&V codoped ANWs may be strong candidates for photoelectrochemical water-splitting, because they have a substantially reduced band gap of 2.49 eV, appropriate band edge positions, no carrier recombination centers, and enhanced optical absorption in the visible light region.

Enhancement in photo-electrochemical efficiency by reducing recombination rate in branched TiO2 nanotube array on functionalizing with ZnO micro crystals

NASA Astrophysics Data System (ADS)

Boda, Muzaffar Ahmad; Ashraf Shah, Mohammad

2018-06-01

In this study, branched TiO2 nanotube array were fabricated through electrochemical anodization process at constant voltage using third generation electrolyte. On account of morphological advantage, these nanotubes shows significant enhancement in photo-electrochemical property than compact or conventional titania nanotube array. However, their photo-electrochemical efficiency intensifies on coating with ZnO micro-crystals. ZnO coated branched TiO2 nanotube array shows a photocurrent density of 27.8 mA cm‑2 which is 1.55 times the photocurrent density (17.2 mA cm‑2) shown by bare branched titania nanotubes. The significant enhancement in photocurrent density shown by the resulting ZnO/TiO2 hybrid structure is attributed to suppression in electron–hole recombination phenomenon by offering smooth pathway to photo generated excitons on account of staggered band edge positions in individual semiconductors.

Optical and photoelectrochemical performance study based on n-ZnO nanorod arrays/p-CuAlO2 laminar films/Ni heterojunction

NASA Astrophysics Data System (ADS)

Ding, Juan; Yang, Haibin; Deng, Weiwen

2014-06-01

A novel ZnO nanorod arrays (NRs)/CuAlO2 laminar films heterojunction nanostructure was grown on the substrate of Ni plates using sol-gel synthesis for laminar films and subsequent hydrothermal reaction for nanorod arrays. The surface morphology, structure, optical and photoelectrochemical behaviors of this heterojunction were considered. Two significant absorption peaks of UV-vis spectra and a favorable forward current to reverse current ratio at applied voltage of -0.7 V to +2 V were observed in this heterojunction. Furthermore, the photoelectrochemical property was indicated that the highest photocurrent of 0.67 mA/cm2 was obtained under AM 1.5 illumination (vs Ag/AgCl). This heterojunction will play an important role in the optoelectronic fields and can be extended to other binary or ternary oxide compositions for optoelectronic applications.

Integrated Photoelectrochemical Solar Energy Conversion and Organic Redox Flow Battery Devices.

PubMed

Li, Wenjie; Fu, Hui-Chun; Li, Linsen; Cabán-Acevedo, Miguel; He, Jr-Hau; Jin, Song

2016-10-10

Building on regenerative photoelectrochemical solar cells and emerging electrochemical redox flow batteries (RFBs), more efficient, scalable, compact, and cost-effective hybrid energy conversion and storage devices could be realized. An integrated photoelectrochemical solar energy conversion and electrochemical storage device is developed by integrating regenerative silicon solar cells and 9,10-anthraquinone-2,7-disulfonic acid (AQDS)/1,2-benzoquinone-3,5-disulfonic acid (BQDS) RFBs. The device can be directly charged by solar light without external bias, and discharged like normal RFBs with an energy storage density of 1.15 Wh L -1 and a solar-to-output electricity efficiency (SOEE) of 1.7 % over many cycles. The concept exploits a previously undeveloped design connecting two major energy technologies and promises a general approach for storing solar energy electrochemically with high theoretical storage capacity and efficiency. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Enhanced photoelectrochemical and photocatalytic activity in visible-light-driven Ag/BiVO{sub 4} inverse opals

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

Fang, Liang, E-mail: lfang@suda.edu.cn, E-mail: dawei.cao@tu-ilmenau.de; Nan, Feng; Yang, Ying

2016-02-29

BiVO{sub 4} photonic crystal inverse opals (io-BiVO{sub 4}) with highly dispersed Ag nanoparticles (NPs) were prepared by the nanosphere lithography method combining the pulsed current deposition method. The incorporation of the Ag NPs can significantly improve the photoelectrochemical and photocatalytic activity of BiVO{sub 4} inverse opals in the visible light region. The photocurrent density of the Ag/io-BiVO{sub 4} sample is 4.7 times higher than that of the disordered sample without the Ag NPs, while the enhancement factor of the corresponding kinetic constant in photocatalytic experiment is approximately 3. The improved photoelectrochemical and photocatalytic activity is benefited from two reasons: onemore » is the enhanced light harvesting owing to the coupling between the slow light and localized surface plasmon resonance effect; the other is the efficient separation of charge carriers due to the Schottky barriers.« less

ZnO/CuO/M (M = Ag, Au) Hierarchical Nanostructure by Successive Photoreduction Process for Solar Hydrogen Generation

PubMed Central

Kwon, Jinhyeong; Cho, Hyunmin; Jung, Jinwook; Lee, Habeom; Han, Seungyong

2018-01-01

To date, solar energy generation devices have been widely studied to meet a clean and sustainable energy source. Among them, water splitting photoelectrochemical cell is regarded as a promising energy generation way for splitting water molecules and generating hydrogen by sunlight. While many nanostructured metal oxides are considered as a candidate, most of them have an improper bandgap structure lowering energy transition efficiency. Herein, we introduce a novel wet-based, successive photoreduction process that can improve charge transfer efficiency by surface plasmon effect for a solar-driven water splitting device. The proposed process enables to fabricate ZnO/CuO/Ag or ZnO/CuO/Au hierarchical nanostructure, having an enhanced electrical, optical, photoelectrochemical property. The fabricated hierarchical nanostructures are demonstrated as a photocathode in the photoelectrochemical cell and characterized by using various analytic tools. PMID:29757225

Band-offsets at BaTiO3/Cu2O heterojunction and enhanced photoelectrochemical response: theory and experiment(Conference Presentation)

NASA Astrophysics Data System (ADS)

Sharma, Dipika; Satsangi, Vibha R.; Dass Kaura, Sahab; Shrivastav, Rohit; Waghmare, Umesh V.

2016-10-01

Band-offsets at BaTiO3/Cu2O heterojunction and enhanced photoelectrochemical response: theory and experiment Dipika Sharmaa, Vibha R. Satsangib, Rohit Shrivastava, Umesh V. Waghmarec, Sahab Dassa aDepartment of Chemistry, Dayalbagh Educational Institute, Agra-282 110 (India) bDepartment of Physics and Computer Sciences, Dayalbagh Educational Institute, Agra-282 110 (India) cTheoretical Sciences Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur, Bangalore-560 064 (India) * Phone: +91-9219695960. Fax: +91-562-2801226. E-mail: drsahabdas@gmail.com. Study on photoelectrochemical activity of pristine BaTiO3, Cu2O and BaTiO3/Cu2O heterojunction has been carried out using DFT based band offsets and charge carriers effective mass calculations and their experimental verification. The results of DFT calculations show that BaTiO3 and Cu2O have staggered type band alignment after the heterojunction formation and high mobility of electrons in Cu2O as compared to the electrons in BaTiO3. Staggered type band edges alignment and high mobility of electrons and holes improved the separation of photo-generated charge carriers in BaTiO3/Cu2O heterojunction. To validate the theoretical results experiments were carried out on pristine BaTiO3, Cu2O and BaTiO3/Cu2O heterojunction with varying thickness of Cu2O. All samples were characterized by X- Ray Diffractometer, SEM and UV-Vis spectrometry. Nanostructured thin films of pristine BaTiO3, Cu2O and BaTiO3/Cu2O heterojunction were used as photoelectrode in the photoelectrochemical cell for water splitting reaction. Maximum photocurrent density of 1.44 mA/cm2 at 0.90 V/SCE was exhibited by 442 nm thick BaTiO3/Cu2O heterojunction photoelectrode Increased photocurrent density and enhanced photoconversion efficiency, exhibited by the heterojunction may be attributed to improved conductivity and enhanced separation of the photogenerated carriers at the BaTiO3/Cu2O interface. The experimental results and first-principles calculations compare well, thus suggesting that such calculations have the potential to be used in screening various metal oxide heterojunction before performing the experiments thereby saving precious chemicals, time and energy. Keywords: Photoelectrochemical, Water splitting, heterojunction, Cu2O, BaTiO3 References: [1] Surbhi Choudhary, et al. Nanostructured bilayered thin films in photoelectrochemical water splitting - A review: International Journal of Hydrogen Energy, (2012). [2] Dipika Sharma, Anuradha Verma, V.R. Satsangi, Rohit shrivastav, Sahab Dass Nanostructured SrTiO3 thin films sensitized by Cu2O for Photoelectrochemical Hydrogen Generation. International journal of Hydrogen Energy;42:,4230-4241, 2014.

Multiplex acute leukemia cytosensing using multifunctional hybrid electrochemical nanoprobes at a hierarchically nanoarchitectured electrode interface

NASA Astrophysics Data System (ADS)

Zheng, Tingting; Tan, Tingting; Zhang, Qingfeng; Fu, Jia-Ju; Wu, Jia-Jun; Zhang, Kui; Zhu, Jun-Jie; Wang, Hui

2013-10-01

We have developed a robust, nanobiotechnology-based electrochemical cytosensing approach with high sensitivity, selectivity, and reproducibility toward the simultaneous multiplex detection and classification of both acute myeloid leukemia and acute lymphocytic leukemia cells. The construction of the electrochemical cytosensor involves the hierarchical assembly of dual aptamer-functionalized, multilayered graphene-Au nanoparticle electrode interface and the utilization of hybrid electrochemical nanoprobes co-functionalized with redox tags, horseradish peroxidase, and cell-targeting nucleic acid aptamers. The hybrid nanoprobes are multifunctional, capable of specifically targeting the cells of interest, amplifying the electrochemical signals, and generating distinguishable signals for multiplex cytosensing. The as-assembled electrode interface not only greatly facilitates the interfacial electron transfer process due to its high conductivity and surface area but also exhibits excellent biocompatibility and specificity for cell recognition and adhesion. A superstructured sandwich-type sensor geometry is adopted for electrochemical cytosensing, with the cells of interest sandwiched between the nanoprobes and the electrode interface. Such an electrochemical sensing strategy allows for ultrasensitive, multiplex acute leukemia cytosensing with a detection limit as low as ~350 cells per mL and a wide linear response range from 5 × 102 to 1 × 107 cells per mL for HL-60 and CEM cells, with minimal cross-reactivity and interference from non-targeting cells. This electrochemical cytosensing approach holds great promise as a new point-of-care diagnostic tool for early detection and classification of human acute leukemia and may be readily expanded to multiplex cytosensing of other cancer cells.We have developed a robust, nanobiotechnology-based electrochemical cytosensing approach with high sensitivity, selectivity, and reproducibility toward the simultaneous multiplex detection and classification of both acute myeloid leukemia and acute lymphocytic leukemia cells. The construction of the electrochemical cytosensor involves the hierarchical assembly of dual aptamer-functionalized, multilayered graphene-Au nanoparticle electrode interface and the utilization of hybrid electrochemical nanoprobes co-functionalized with redox tags, horseradish peroxidase, and cell-targeting nucleic acid aptamers. The hybrid nanoprobes are multifunctional, capable of specifically targeting the cells of interest, amplifying the electrochemical signals, and generating distinguishable signals for multiplex cytosensing. The as-assembled electrode interface not only greatly facilitates the interfacial electron transfer process due to its high conductivity and surface area but also exhibits excellent biocompatibility and specificity for cell recognition and adhesion. A superstructured sandwich-type sensor geometry is adopted for electrochemical cytosensing, with the cells of interest sandwiched between the nanoprobes and the electrode interface. Such an electrochemical sensing strategy allows for ultrasensitive, multiplex acute leukemia cytosensing with a detection limit as low as ~350 cells per mL and a wide linear response range from 5 × 102 to 1 × 107 cells per mL for HL-60 and CEM cells, with minimal cross-reactivity and interference from non-targeting cells. This electrochemical cytosensing approach holds great promise as a new point-of-care diagnostic tool for early detection and classification of human acute leukemia and may be readily expanded to multiplex cytosensing of other cancer cells. Electronic supplementary information (ESI) available: Additional figures as noted in the text. See DOI: 10.1039/c3nr02903d

International Symposium on New Trends in Photoelectrochemistry Held in Altavilla Milicia (Pa), Italy on 22-26 September 1991. Extended Abstracts

DTIC Science & Technology

1991-09-01

Exchange Between Semiconductors and Molecules (Redox Ions)" F. Willig, Fritz - Haber Institut der Max-Planck Gesellschaft, Berlin GERMANY 8.00 p.m.: Dinner...Lecture "Photoelectrochemical Catalysis by Small Semiconducting Particles" H. Gerischer, Fritz - Haber Institut der Max-Planck- Gesellschaft, Berlin, GERMANY...examples of photoelectrochemical etching procedures with elemental, II-VI and III-V compound semiconducting electrodes will be discussed. 25 FRITZ - HABER

Photoelectrochemical etching measurement of defect density in GaN grown by nanoheteroepitaxy

NASA Astrophysics Data System (ADS)

Ferdous, M. S.; Sun, X. Y.; Wang, X.; Fairchild, M. N.; Hersee, S. D.

2006-05-01

The density of dislocations in n-type GaN was measured by photoelectrochemical etching. A 10× reduction in dislocation density was observed compared to planar GaN grown at the same time. Cross-sectional transmission electron microscopy studies indicate that defect reduction is due to the mutual cancellation of dislocations with equal and opposite Burger's vectors. The nanoheteroepitaxy sample exhibited significantly higher photoluminescence intensity and higher electron mobility than the planar reference sample.

Photoelectrochemical cell having photoanode with thin boron phosphide coating as a corrosion resistant layer

DOEpatents

Baughman, Richard J.; Ginley, David S.

1984-01-01

A surface prone to corrosion in corrosive environments is rendered anticorrosive by CVD growing a thin continuous film, e.g., having no detectable pinholes, thereon, of boron phosphide. In one embodiment, the film is semiconductive. In another aspect, the invention is an improved photoanode, and/or photoelectrochemical cell with a photoanode having a thin film of boron phosphide thereon rendering it anitcorrosive, and providing it with unexpectedly improved photoresponsive properties.

CdS/MoS2 heterojunction-based photoelectrochemical DNA biosensor via enhanced chemiluminescence excitation.

PubMed

Zang, Yang; Lei, Jianping; Hao, Qing; Ju, Huangxian

2016-03-15

This work developed a CdS/MoS2 heterojunction-based photoelectrochemical biosensor for sensitive detection of DNA under the enhanced chemiluminescence excitation of luminol catalyzed by hemin-DNA complex. The CdS/MoS2 photocathode was prepared by the stepwise assembly of MoS2 and CdS quantum dots (QDs) on indium tin oxide (ITO), and achieved about 280% increasing of photocurrent compared to pure CdS QDs electrode due to the formation of heterostructure. High photoconversion efficiency in the photoelectrochemical system was identified to be the rapid spatial charge separation of electron-hole pairs by the extension of electron transport time and electron lifetime. In the presence of target DNA, the catalytic hairpin assembly was triggered, and simultaneously the dual hemin-labeled DNA probe was introduced to capture DNA/CdS/MoS2 modified ITO electrode. Thus the chemiluminescence emission of luminol was enhanced via hemin-induced mimetic catalysis, leading to the physical light-free photoelectrochemical strategy. Under optimized conditions, the resulting photoelectrode was proportional to the logarithm of target DNA concentration in the range from 1 fM to 100 pM with a detection limit of 0.39 fM. Moreover, the cascade amplification biosensor demonstrated high selectivity, desirable stability and good reproducibility, showing great prospect in molecular diagnosis and bioanalysis. Copyright © 2015 Elsevier B.V. All rights reserved.

Morphology modulation of SrTiO3/TiO2 heterostructures for enhanced photoelectrochemical performance.

PubMed

Jiao, Zhengbo; Chen, Tao; Yu, Hongchao; Wang, Teng; Lu, Gongxuan; Bi, Yingpu

2014-04-01

Design and fabrication of nanoscale semiconductors with regulatable morphology or structure has attracted tremendous interest due to the dependency relationship between properties and architectures. Two types of SrTiO3/TiO2 nanocomposites with different morphologies and structures have been fabricated by controlling the kinetics of hydrothermal reactions. One is TiO2 nanotube arrays densely wrapped by SrTiO3 film and the other is SrTiO3 nanospheres distributed on the top region of TiO2 nanotube arrays, which has been firstly fabricated. It has been found that the photoelectrochemical performances of these heterostructures are crucially dominated by their architectures. Heterostructured SrTiO3/TiO2 nanotube arrays were fabricated by traditional method in the absence of NaOH and they exhibited higher photoelectrochemical performance than pure TiO2 nanotube arrays. However, the compact SrTiO3 coating film on the sidewalls of TiO2 nanotube arrays could inevitably destroy the tubular structures of TiO2 and thus go against the vectorial transport of electrons. Interestingly, when excess NaOH was added into the growth solution, SrTiO3 nanospheres would be rationally grafted on the top of TiO2 nanotube arrays, which could preserve the tubular structures of TiO2, and thus further improve the photoelectrochemical performance. Copyright © 2013 Elsevier Inc. All rights reserved.

A TiO2/FeMnP Core/Shell Nanorod Array Photoanode for Efficient Photoelectrochemical Oxygen Evolution.

PubMed

Schipper, Desmond E; Zhao, Zhenhuan; Leitner, Andrew P; Xie, Lixin; Qin, Fan; Alam, Md Kamrul; Chen, Shuo; Wang, Dezhi; Ren, Zhifeng; Wang, Zhiming; Bao, Jiming; Whitmire, Kenton H

2017-04-25

A variety of catalysts have recently been developed for electrocatalytic oxygen evolution, but very few of them can be readily integrated with semiconducting light absorbers for photoelectrochemical or photocatalytic water splitting. Here, we demonstrate an efficient core/shell photoanode with a highly active oxygen evolution electrocatalyst shell (FeMnP) and semiconductor core (rutile TiO 2 ) for photoelectrochemical oxygen evolution reaction. Metal-organic chemical vapor deposition from a single-source precursor was used to ensure good contact between the FeMnP and the TiO 2 . The TiO 2 /FeMnP core/shell photoanode reaches the theoretical photocurrent density for rutile TiO 2 of 1.8 mA cm -2 at 1.23 V vs reversible hydrogen electrode under simulated 100 mW cm -2 (1 sun) irradiation. The dramatic enhancement is a result of the synergistic effects of the high oxygen evolution reaction activity of FeMnP (delivering an overpotential of 300 mV with a Tafel slope of 65 mV dec -1 in 1 M KOH) and the conductive interlayer between the surface active sites and semiconductor core which boosts the interfacial charge transfer and photocarrier collection. The facile fabrication of the TiO 2 /FeMnP core/shell nanorod array photoanode offers a compelling strategy for preparing highly efficient photoelectrochemical solar energy conversion devices.

Particulate photocatalyst sheets for Z-scheme water splitting: advantages over powder suspension and photoelectrochemical systems and future challenges.

PubMed

Wang, Qian; Hisatomi, Takashi; Katayama, Masao; Takata, Tsuyoshi; Minegishi, Tsutomu; Kudo, Akihiko; Yamada, Taro; Domen, Kazunari

2017-04-28

Water splitting using semiconductor photocatalysts has been attracting growing interest as a means of solar energy based conversion of water to hydrogen, a clean and renewable fuel. Z-scheme photocatalytic water splitting based on the two-step excitation of an oxygen evolution photocatalyst (OEP) and a hydrogen evolution photocatalyst (HEP) is a promising approach toward the utilisation of visible light. In particular, a photocatalyst sheet system consisting of HEP and OEP particles embedded in a conductive layer has been recently proposed as a new means of obtaining efficient and scalable redox mediator-free Z-scheme solar water splitting. In this paper, we discuss the advantages and disadvantages of the photocatalyst sheet approach compared to conventional photocatalyst powder suspension and photoelectrochemical systems through an examination of the water splitting activity of Z-scheme systems based on SrTiO 3 :La,Rh as the HEP and BiVO 4 :Mo as the OEP. This photocatalyst sheet was found to split pure water much more efficiently than the powder suspension and photoelectrochemical systems, because the underlying metal layer efficiently transfers electrons from the OEP to the HEP. The photocatalyst sheet also outperformed a photoelectrochemical parallel cell during pure water splitting. The effects of H + /OH - concentration overpotentials and of the IR drop are reduced in the case of the photocatalyst sheet compared to photoelectrochemical systems, because the HEP and OEP are situated in close proximity to one another. Therefore, the photocatalyst sheet design is well-suited to efficient large-scale applications. Nevertheless, it is also noted that the photocatalytic activity of these sheets drops markedly with increasing background pressure because of reverse reactions involving molecular oxygen under illumination as well as delays in gas bubble desorption. It is shown that appropriate surface modifications allow the photocatalyst sheet to maintain its water splitting activity at elevated pressure. Accordingly, we conclude that the photocatalyst sheet system is a viable option for the realisation of efficient solar fuel production.

Signal Amplification by Glyco-qPCR for Ultrasensitive Detection of Carbohydrates: Applications in Glycobiology**

PubMed Central

Kwon, Seok Joon; Lee, Kyung Bok; Solakyildirim, Kemal; Masuko, Sayaka; Ly, Mellisa; Zhang, Fuming; Li, Lingyun; Dordick, Jonathan S.; Linhardt, Robert J.

2012-01-01

Tiny amounts of carbohydrates (ca. 1 zmol) can be detected quantitatively by a real-time method based on the conjugation of carbohydrates with DNA markers (see picture). The proposed method (glyco-qPCR) provides uniform, ultrasensitive detection of carbohydrates, which can be applied to glycobiology, as well as carbohydrate-based drug discovery. PMID:23073897

An ultra-sensitive monoclonal antibody-based fluorescent microsphere immunochromatographic test strip assay for detecting aflatoxin M1 in milk

USDA-ARS?s Scientific Manuscript database

A rapid lateral flow fluorescent microspheres immunochromatography test strip (FMs-ICTS) has been developed for the detection of aflatoxin M1 (AFM1) residues in milk. For this purpose, an ultra-sensitive anti-AFM1 monoclonal antibody (MAb) 1D3 was prepared and identified. The IC50 value of the MA...

CdS/CdSe quantum dot shell decorated vertical ZnO nanowire arrays by spin-coating-based SILAR for photoelectrochemical cells and quantum-dot-sensitized solar cells.

PubMed

Zhang, Ran; Luo, Qiu-Ping; Chen, Hong-Yan; Yu, Xiao-Yun; Kuang, Dai-Bin; Su, Cheng-Yong

2012-04-23

A CdS/CdSe composite shell is assembled onto the surface of ZnO nanowire arrays with a simple spin-coating-based successive ionic layer adsorption and reaction method. The as-prepared photoelectrode exhibit a high photocurrent density in photoelectrochemical cells and also generates good power conversion efficiency in quantum-dot-sensitized solar cells. Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Photoelectrochemical Properties of Graphene and Its Derivatives

PubMed Central

Adán-Más, Alberto; Wei, Di

2013-01-01

Graphene and its derivatives combine a numerous range of supreme properties that can be useful in many applications. The purpose of this review is to analyse the photoelectrochemical properties of pristine graphene, graphene oxide (GO) and reduced graphene oxide (rGO) and their impact on semiconductor catalysts/quantum dots. The mechanism that this group of materials follows to improve their performance will be cleared by explaining how those properties can be exploited in several applications such as photo-catalysts (degradation of pollutants) and photovoltaics (solar cells). PMID:28348339

Photo-electrochemical Oxidation of Organic C1 Molecules over WO3 Films in Aqueous Electrolyte: Competition Between Water Oxidation and C1 Oxidation.

PubMed

Reichert, Robert; Zambrzycki, Christian; Jusys, Zenonas; Behm, R Jürgen

2015-11-01

To better understand organic-molecule-assisted photo-electrochemical water splitting, photo-electrochemistry and on-line mass spectrometry measurements are used to investigate the photo-electrochemical oxidation of the C1 molecules methanol, formaldehyde, and formic acid over WO3 film anodes in aqueous solution and its competition with O2 evolution from water oxidation O2 (+) and CO2 (+) ion currents show that water oxidation is strongly suppressed by the organic species. Photo-electro-oxidation of formic acid is dominated by formation of CO2 , whereas incomplete oxidation of formaldehyde and methanol prevails, with the selectivity for CO2 formation increasing with increasing potential and light intensity. The mechanistic implications for the photo-electro-oxidation of the organic molecules and its competition with water oxidation, which could be derived from this novel approach, are discussed. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Efficient Suppression of Electron–Hole Recombination in Oxygen-Deficient Hydrogen-Treated TiO2 Nanowires for Photoelectrochemical Water Splitting

PubMed Central

2013-01-01

There is an increasing level of interest in the use of black TiO2 prepared by thermal hydrogen treatments (H:TiO2) due to the potential to enhance both the photocatalytic and the light-harvesting properties of TiO2. Here, we examine oxygen-deficient H:TiO2 nanotube arrays that have previously achieved very high solar-to-hydrogen (STH) efficiencies due to incident photon-to-current efficiency (IPCE) values of >90% for photoelectrochemical water splitting at only 0.4 V vs RHE under UV illumination. Our transient absorption (TA) mechanistic study provides strong evidence that the improved electrical properties of oxygen-deficient TiO2 enables remarkably efficient spatial separation of electron–hole pairs on the submicrosecond time scale at moderate applied bias, and this coupled to effective suppression of microsecond to seconds charge carrier recombination is the primary factor behind the dramatically improved photoelectrochemical activity. PMID:24376902

Cold sprayed WO3 and TiO2 electrodes for photoelectrochemical water and methanol oxidation in renewable energy applications.

PubMed

Haisch, Christoph; Schneider, Jenny; Fleisch, Manuel; Gutzmann, Henning; Klassen, Thomas; Bahnemann, Detlef W

2017-10-03

Films prepared by cold spray have potential applications as photoanodes in electrochemical water splitting and waste water purification. In the present study cold sprayed photoelectrodes produced with WO 3 (active under visible light illumination) and TiO 2 (active under UV illumination) on titanium metal substrates were investigated as photoanodes for the oxidation of water and methanol, respectively. Methanol was chosen as organic model pollutant in acidic electrolytes. Main advantages of the cold sprayed photoelectrodes are the improved metal-semiconductor junctions and the superior mechanical stability. Additionally, the cold spray method can be utilized as a large-scale electrode fabrication technique for photoelectrochemical applications. Incident photon to current efficiencies reveal that cold sprayed TiO 2 /WO 3 photoanodes exhibit the best photoelectrochemical properties with regard to the water and methanol oxidation reactions in comparison with the benchmark photocatalyst Aeroxide TiO 2 P25 due to more efficient harvesting of the total solar light irradiation related to their smaller band gap energies.

Visible light to electrical energy conversion using photoelectrochemical cells

NASA Technical Reports Server (NTRS)

Wrighton, Mark S. (Inventor); Ellis, Arthur B. (Inventor); Kaiser, Steven W. (Inventor)

1983-01-01

Sustained conversion of low energy visible or near i.r. light (>1.25 eV) to electrical energy has been obtained using wet photoelectrochemical cells where there are no net chemical changes in the system. Stabilization of n-type semi-conductor anodes of CdS, CdSe, CdTe, GaP, GaAs and InP to photoanodic dissolution is achieved by employing selected alkaline solutions of Na.sub.2 S, Na.sub.2 S/S, Na.sub.2 Se, Na.sub.2 Se/Se, Na.sub.2 Te and Na.sub.2 Te/Te as the electrolyte. The oxidation of (poly) sulfide, (poly)selenide or (poly)telluride species occurs at the irradiated anode, and reduction of polysulfide, polyselenide or polytelluride species occurs at the dark Pt cathode of the photoelectrochemical cell. Optical to electrical energy conversion efficiencies approaching 15% at selected frequencies have been observed in some cells. The wavelength for the onset of photocurrent corresponds to the band gap of the particular anode material used in the cell.

Target-aptamer binding triggered quadratic recycling amplification for highly specific and ultrasensitive detection of antibiotics at the attomole level.

PubMed

Wang, Hongzhi; Wang, Yu; Liu, Su; Yu, Jinghua; Xu, Wei; Guo, Yuna; Huang, Jiadong

2015-05-14

A novel electrochemical aptasensor for ultrasensitive detection of antibiotics by combining polymerase-assisted target recycling amplification with strand displacement amplification with the help of polymerase and nicking endonuclease has been reported. This work is the first time that target-aptamer binding triggered quadratic recycling amplification has been utilized for electrochemical detection of antibiotics.

A ligation DNAzyme-induced magnetic nanoparticles assembly for ultrasensitive detection of copper ions.

PubMed

Yin, Honghong; Kuang, Hua; Liu, Liqiang; Xu, Liguang; Ma, Wei; Wang, Libing; Xu, Chuanlai

2014-04-09

A novel biosensor for ultrasensitive detection of copper (Cu(2+)) was established based on the assembly of magnetic nanoparticles induced by the Cu(2+)-dependent ligation DNAzyme. With a low limit of detection of 2.8 nM and high specificity, this method has the potential to serve as a general platform for the detection of heavy metal ions.

Correction: One-step coelectrodeposition-assisted layer-by-layer assembly of gold nanoparticles and reduced graphene oxide and its self-healing three-dimensional nanohybrid for an ultrasensitive DNA sensor.

PubMed

Jayakumar, Kumarasamy; Camarada, María Belén; Dharuman, Venkataraman; Ju, Huangxian; Dey, Ramendra Sundar; Wen, Yangping

2018-02-01

Correction for 'One-step coelectrodeposition-assisted layer-by-layer assembly of gold nanoparticles and reduced graphene oxide and its self-healing three-dimensional nanohybrid for an ultrasensitive DNA sensor' by Jayakumar Kumarasamy, et al., Nanoscale, 2018, DOI: 10.1039/c7nr06952a.

Fe2 PO5 -Encapsulated Reverse Energetic ZnO/Fe2 O3 Heterojunction Nanowire for Enhanced Photoelectrochemical Oxidation of Water.

PubMed

Qin, Dong-Dong; He, Cai-Hua; Li, Yang; Trammel, Antonio C; Gu, Jing; Chen, Jing; Yan, Yong; Shan, Duo-Liang; Wang, Qiu-Hong; Quan, Jing-Jing; Tao, Chun-Lan; Lu, Xiao-Quan

2017-07-10

Zinc oxide is regarded as a promising candidate for application in photoelectrochemical water oxidation due to its higher electron mobility. However, its instability under alkaline conditions limits its application in a practical setting. Herein, we demonstrate an easily achieved wet-chemical route to chemically stabilize ZnO nanowires (NWs) by protecting them with a thin layer Fe 2 O 3 shell. This shell, in which the thickness can be tuned by varying reaction times, forms an intact interface with ZnO NWs, thus protecting ZnO from corrosion in a basic solution. The reverse energetic heterojunction nanowires are subsequently activated by introducing an amorphous iron phosphate, which substantially suppressed surface recombination as a passivation layer and improved photoelectrochemical performance as a potential catalyst. Compared with pure ZnO NWs (0.4 mA cm -2 ), a maximal photocurrent of 1.0 mA cm -2 is achieved with ZnO/Fe 2 O 3 core-shell NWs and 2.3 mA cm -2 was achieved for the PH 3 -treated NWs at 1.23 V versus RHE. The PH 3 low-temperature treatment creates a dual function, passivation and catalyst layer (Fe 2 PO 5 ), examined by X-ray photoelectron spectroscopy, TEM, photoelectrochemical characterization, and impedance measurements. Such a nano-composition design offers great promise to improve the overall performance of the photoanode material. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fast fabrication of long TiO2 nanotube array with high photoelectrochemical property on flexible stainless steel.

PubMed

Tao, Jie; Wu, Tao; Gao, Peng

2012-03-01

Oriented highly ordered long TiO2 nanotube array films with nanopore structure and high photoelectrochemical property were fabricated on flexible stainless steel substrate (50 microm) by anodization treatment of titanium thin films in a short time. The samples were characterized by means of field emission scanning electron microscopy (FESEM), X-ray diffraction (XRD) and photoelectrochemical methods, respectively. The results showed that Ti films deposited at the condition of 0.7 Pa Ar pressure and 96 W sputtering power at room temperature was uniform and dense with good homogeneity and high crystallinity. The voltage and the anodization time both played significant roles in the formation of TiO2 nanopore-nanotube array film. The optimal voltage was 60 V and the anodization time is less than 30 min by anodizing Ti films in ethylene glycerol containing 0.5% (w) NH4F and 3% (w) H2O. The growth rate of TiO2 nanotube array was as high as 340 nm/min. Moreover, the photocurrent-potential curves, photocurrent response curves and electrochemical impedance spectra results indicated that the TiO2 nanotube array film with the nanoporous structure exhibited a better photo-response ability and photoelectrochemical performance than the ordinary TiO2 nanotube array film. The reason is that the nanoporous structure on the surface of the nanotube array can separate the photo electron-hole pairs more efficiently and completely than the tubular structure.

Dye sensitized photoelectrochemical immunosensor for the tumor marker CEA by using a flower-like 3D architecture prepared from graphene oxide and MoS2.

PubMed

Song, Kaijing; Ding, Chuanmin; Zhang, Bing; Chang, Honghong; Zhao, Zhihuan; Wei, Wenlong; Wang, Junwen

2018-06-01

The authors describe a dye-sensitized photoelectrochemical immunoassay for the tumor marker carcinoembryonic antigen (CEA). The method employs the rhodamine dye Rh123 with red color and absorption maximum at 500 nm for spectral sensitization, and a 3D nanocomposite prepared from graphene oxide and MoS 2 acting as the photoelectric conversion layer. The nanocomposite with flower-like 3D architectures was characterized by transmission electron microscopy, scanning electron microscopy, X-ray powder diffraction, and UV-vis diffuse reflectometry. A photoelectrochemical sandwich immunoassay was developed that is based on the use of the nanocomposite and based on the specific binding of antibody and antigen, and by using a secondary antibody labeled with Rh123 and CdS (Ab 2 -Rh123@CdS). Under optimal conditions and at a typical working voltage of 0 V (vs. Hg/HgCl 2 ), the photocurrent increases linearly 10 pg mL -1 to 80 ng mL -1 CEA concentration range, with a 3.2 pg mL -1 detection limit. Graphical abstract Flower-like GO-MoS 2 complex with high efficiency of electron transport was synthesized to construct photoelectrochemical platform. The sandwich-type immunoassay was built on this platform based on specific binding of antigen and antibody. Carcinoembryonic antigen in sample was detected sensitively by using sensitization of rhodamine dye Rh123 as signal amplification strategy.

Titanium dioxide nanotube membranes for solar energy conversion: effect of deep and shallow dopants.

PubMed

Ding, Yuchen; Nagpal, Prashant

2017-04-12

Nanostructured titanium dioxide (TiO 2 ) has been intensively investigated as a material of choice for solar energy conversion in photocatalytic, photoelectrochemical, photovoltaic, and other photosensitized devices for converting light into chemical feedstocks or electricity. Towards management of light absorption in TiO 2 , while the nanotubular structure improves light absorption and simultaneous charge transfer to mitigate problems due to the indirect bandgap of the semiconductor, typically dopants are used to improve light absorption of incident solar irradiation in the wide bandgap of TiO 2 . While these dopants can be critical to the success of these solar energy conversion devices, their effect on photophysical and photoelectrochemical properties and detailed photokinetics are relatively under-studied. Here, we show the effect of deep and shallow metal dopants on the kinetics of photogenerated charged carriers in TiO 2 and the resulting effect on photocatalytic and photoelectrochemical processes using these nanotube membranes. We performed a detailed optical, electronic, voltammetry and electrochemical impedance study to understand the effect of shallow and deep metal dopants (using undoped and niobium- and copper-doped TiO 2 nanotubes) on light absorption, charge transport and charge transfer processes. Using wireless photocatalytic methylene blue degradation and carbon dioxide reduction, and wired photoelectrochemical device measurements, we elucidate the effect of different dopants on solar-to-fuel conversion efficiency and simultaneously describe the photokinetics using a model, to help design better energy conversion devices.

Ultrasensitivity of the Bacillus subtilis sporulation decision.

PubMed

Narula, Jatin; Devi, Seram N; Fujita, Masaya; Igoshin, Oleg A

2012-12-11

Starving Bacillus subtilis cells execute a gene expression program resulting in the formation of stress-resistant spores. Sporulation master regulator, Spo0A, is activated by a phosphorelay and controls the expression of a multitude of genes, including the forespore-specific sigma factor σ(F) and the mother cell-specific sigma factor σ(E). Identification of the system-level mechanism of the sporulation decision is hindered by a lack of direct control over Spo0A activity. This limitation can be overcome by using a synthetic system in which Spo0A activation is controlled by inducing expression of phosphorelay kinase KinA. This induction results in a switch-like increase in the number of sporulating cells at a threshold of KinA. Using a combination of mathematical modeling and single-cell microscopy, we investigate the origin and physiological significance of this ultrasensitive threshold. The results indicate that the phosphorelay is unable to achieve a sufficiently fast and ultrasensitive response via its positive feedback architecture, suggesting that the sporulation decision is made downstream. In contrast, activation of σ(F) in the forespore and of σ(E) in the mother cell compartments occurs via a cascade of coherent feed-forward loops, and thereby can produce fast and ultrasensitive responses as a result of KinA induction. Unlike σ(F) activation, σ(E) activation in the mother cell compartment only occurs above the KinA threshold, resulting in completion of sporulation. Thus, ultrasensitive σ(E) activation explains the KinA threshold for sporulation induction. We therefore infer that under uncertain conditions, cells initiate sporulation but postpone making the sporulation decision to average stochastic fluctuations and to achieve a robust population response.

Standardization and performance evaluation of "modified" and "ultrasensitive" versions of the Abbott RealTime HIV-1 assay, adapted to quantify minimal residual viremia.

PubMed

Amendola, Alessandra; Bloisi, Maria; Marsella, Patrizia; Sabatini, Rosella; Bibbò, Angela; Angeletti, Claudio; Capobianchi, Maria Rosaria

2011-09-01

Numerous studies investigating clinical significance of HIV-1 minimal residual viremia (MRV) suggest potential utility of assays more sensitive than those routinely used to monitor viral suppression. However currently available methods, based on different technologies, show great variation in detection limit and input plasma volume, and generally suffer from lack of standardization. In order to establish new tools suitable for routine quantification of minimal residual viremia in patients under virological suppression, some modifications were introduced into standard procedure of the Abbott RealTime HIV-1 assay leading to a "modified" and an "ultrasensitive" protocols. The following modifications were introduced: calibration curve extended towards low HIV-1 RNA concentration; 4 fold increased sample volume by concentrating starting material; reduced volume of internal control; adoption of "open-mode" software for quantification. Analytical performances were evaluated using the HIV-1 RNA Working Reagent 1 for NAT assays (NIBSC). Both tests were applied to clinical samples from virologically suppressed patients. The "modified" and the "ultrasensitive" configurations of the assay reached a limit of detection of 18.8 (95% CI: 11.1-51.0 cp/mL) and 4.8 cp/mL (95% CI: 2.6-9.1 cp/mL), respectively, with high precision and accuracy. In clinical samples from virologically suppressed patients, "modified" and "ultrasensitive" protocols allowed to detect and quantify HIV RNA in 12.7% and 46.6%, respectively, of samples resulted "not-detectable", and in 70.0% and 69.5%, respectively, of samples "detected <40 cp/mL" in the standard assay. The "modified" and "ultrasensitive" assays are precise and accurate, and easily adoptable in routine diagnostic laboratories for measuring MRV. Copyright © 2011 Elsevier B.V. All rights reserved.

Simple, multiplexed, PCR-based barcoding of DNA enables sensitive mutation detection in liquid biopsies using sequencing.

PubMed

Ståhlberg, Anders; Krzyzanowski, Paul M; Jackson, Jennifer B; Egyud, Matthew; Stein, Lincoln; Godfrey, Tony E

2016-06-20

Detection of cell-free DNA in liquid biopsies offers great potential for use in non-invasive prenatal testing and as a cancer biomarker. Fetal and tumor DNA fractions however can be extremely low in these samples and ultra-sensitive methods are required for their detection. Here, we report an extremely simple and fast method for introduction of barcodes into DNA libraries made from 5 ng of DNA. Barcoded adapter primers are designed with an oligonucleotide hairpin structure to protect the molecular barcodes during the first rounds of polymerase chain reaction (PCR) and prevent them from participating in mis-priming events. Our approach enables high-level multiplexing and next-generation sequencing library construction with flexible library content. We show that uniform libraries of 1-, 5-, 13- and 31-plex can be generated. Utilizing the barcodes to generate consensus reads for each original DNA molecule reduces background sequencing noise and allows detection of variant alleles below 0.1% frequency in clonal cell line DNA and in cell-free plasma DNA. Thus, our approach bridges the gap between the highly sensitive but specific capabilities of digital PCR, which only allows a limited number of variants to be analyzed, with the broad target capability of next-generation sequencing which traditionally lacks the sensitivity to detect rare variants. © The Author(s) 2016. Published by Oxford University Press on behalf of Nucleic Acids Research.

Recent advances in rapid and ultrasensitive biosensors for infectious agents: lesson from Bacillus anthracis diagnostic sensors.

PubMed

Kim, Joungmok; Yoon, Moon-Young

2010-06-01

Here, we review the cumulative efforts to develop rapid and ultrasensitive diagnostic systems, especially for the infectious agent, Bacillus anthracis, as a model system. This Minireview focuses on demonstrating the features of various probes for target molecule detection and recent methods of signal generation within the biosensors. Also, we discuss the possibility of using peptides as next-generation probe molecules.

In-electrode vs. on-electrode: ultrasensitive Faraday cage-type electrochemiluminescence immunoassay.

PubMed

Guo, Zhiyong; Sha, Yuhong; Hu, Yufang; Wang, Sui

2016-03-28

A new-concept of an "in-electrode" Faraday cage-type electrochemiluminescence immunoassay (ECLIA) method for the ultrasensitive detection of neurotensin (NT) was reported with capture antibody (Ab1)-nanoFe3O4@graphene (GO) and detector antibody (Ab2)&N-(4-aminobutyl)-N-ethylisoluminol (ABEI)@GO, which led to about 1000-fold improvement in sensitivity by extending the Helmholtz plane (OHP) of the proposed electrode assembly effectively.

Identifying ultrasensitive HGF dose-response functions in a 3D mammalian system for synthetic morphogenesis.

PubMed

Senthivel, Vivek Raj; Sturrock, Marc; Piedrafita, Gabriel; Isalan, Mark

2016-12-16

Nonlinear responses to signals are widespread natural phenomena that affect various cellular processes. Nonlinearity can be a desirable characteristic for engineering living organisms because it can lead to more switch-like responses, similar to those underlying the wiring in electronics. Steeper functions are described as ultrasensitive, and can be applied in synthetic biology by using various techniques including receptor decoys, multiple co-operative binding sites, and sequential positive feedbacks. Here, we explore the inherent non-linearity of a biological signaling system to identify functions that can potentially be exploited using cell genome engineering. For this, we performed genome-wide transcription profiling to identify genes with ultrasensitive response functions to Hepatocyte Growth Factor (HGF). We identified 3,527 genes that react to increasing concentrations of HGF, in Madin-Darby canine kidney (MDCK) cells, grown as cysts in 3D collagen cell culture. By fitting a generic Hill function to the dose-responses of these genes we obtained a measure of the ultrasensitivity of HGF-responsive genes, identifying a subset with higher apparent Hill coefficients (e.g. MMP1, TIMP1, SNORD75, SNORD86 and ERRFI1). The regulatory regions of these genes are potential candidates for future engineering of synthetic mammalian gene circuits requiring nonlinear responses to HGF signalling.

Interpretation of quantum yields exceeding unity in photoelectrochemical systems

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

Szklarczyk, M.; Allen, R.E.

1986-10-20

In photoelectrochemical systems involving light shining on a semiconductor interfaced with an electrolyte, the quantum yield as a function of photon frequency ..nu.. is observed to exhibit a peak at h..nu..roughly-equal2E/sub g/, where E/sub g/ is the band gap of the semiconductor. The maximum in this peak is sometimes found to exceed unity. We provide an interpretation involving surface states and inelastic electron-electron scattering. The theory indicates that the effect should be observable for p-type semiconductors, but not n-type.

A series of BCN nanosheets with enhanced photoelectrochemical performances

NASA Astrophysics Data System (ADS)

Li, Junqi; Lei, Nan; Hao, Hongjuan; Zhou, Jian

2017-03-01

A series of flake-like BCN compounds were produced by calcination at different reaction temperatures via thermal substitution of C atoms with B atoms of boric acid substructures in graphitic carbon nitrides (g-C3N4). The structural and optical properties of the samples were characterized by XRD, TEM, HRTEM, XPS and UV-vis absorption. The photoelectrochemical (PEC) performance of all samples were characterized through photocurrent and electrochemical impedance spectroscopy (EIS) measurement. The test results demonstrated that BCN nanosheets exhibited higher PEC performance with increasing substituted amount of boron.

Indium oxide thin film as potential photoanodes for corrosion protection of stainless steel under visible light

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

Zhang, Yan; Yu, Jianqiang, E-mail: jianqyu@qdu.edu.cn; Sun, Kai

Graphical abstract: If the conduction band potential of In{sub 2}O{sub 3} is more negative than the corrosion potential of stainless steel, photo-induced electrons will be transferred from In{sub 2}O{sub 3} to the steel, thus shifting the potential of the steel into a corrosion immunity region and preventing the steel from the corrosion. - Highlights: • Indium oxide performed novel application under visible light. • Indium oxide by sol–gel method behaved better photoelectrochemical properties. • Electrons were transferred to stainless steel from indium oxide once light on. - Abstract: This paper reports the photoelectrochemical cathodic protection of 304 stainless steel bymore » In{sub 2}O{sub 3} thin-film under visible-light. The films were fabricated with In{sub 2}O{sub 3} powders, synthesized by both sol–gel (In{sub 2}O{sub 3}-sg) and solid-state (In{sub 2}O{sub 3}-ss) processes. The photo-induced open circuit potential and the photo-to-current efficiency measurements suggested that In{sub 2}O{sub 3} could be a promising candidate material for photoelectrochemical cathodic protection of metallic alloys under visible light. Moreover, the polarization curve experimental results indicated that In{sub 2}O{sub 3}-sg thin-film can mitigate the corrosion potential of 304 stainless steel to much more negative values with a higher photocurrent density than the In{sub 2}O{sub 3}-ss film under visible-light illumination. All the results demonstrated that the In{sub 2}O{sub 3}-sg thin-film provides a better photoelectrochemical cathodic protection for 304 stainless steel than In{sub 2}O{sub 3}-ss thin-film under visible-light illumination. The higher photoelectrochemical efficiency is possibly due to the uniform thin films produced with the smaller particle size of In{sub 2}O{sub 3}-sg, which facilitates the transfer of the photo-induced electrons from bulk to the surface and suppresses the charge recombination of the electrons and holes.« less

Plasmon-Based Colorimetric Nanosensors for Ultrasensitive Molecular Diagnostics.

PubMed

Tang, Longhua; Li, Jinghong

2017-07-28

Colorimetric detection of target analytes with high specificity and sensitivity is of fundamental importance to clinical and personalized point-of-care diagnostics. Because of their extraordinary optical properties, plasmonic nanomaterials have been introduced into colorimetric sensing systems, which provide significantly improved sensitivity in various biosensing applications. Here we review the recent progress on these plasmonic nanoparticles-based colorimetric nanosensors for ultrasensitive molecular diagnostics. According to their different colorimetric signal generation mechanisms, these plasmonic nanosensors are classified into two categories: (1) interparticle distance-dependent colorimetric assay based on target-induced forming cross-linking assembly/aggregate of plasmonic nanoparticles; and (2) size/morphology-dependent colorimetric assay by target-controlled growth/etching of the plasmonic nanoparticles. The sensing fundamentals and cutting-edge applications will be provided for each of them, particularly focusing on signal generation and/or amplification mechanisms that realize ultrasensitive molecular detection. Finally, we also discuss the challenge and give our future perspective in this emerging field.

Furthur remarks on atmospheric probing by ultrasensitive radar

NASA Technical Reports Server (NTRS)

Atlas, D.

1969-01-01

This paper is supplementary to that of Hardy and Katz. It emphasizes the meteorological value of the various capabilities of ultrasensitive radar, highlights the points of agreement and disagreement, and focuses upon the directions of promising research. The theory of backscatter from a refractively turbulent region is said to be confirmed by the radar observations both with respect to magnitude and wavelength dependence. A reason for the apparent discrepancy between the results of some of the forwardscatter experiments and theory is suggested. Disagreement still exists with respect to the origin of clear air sea breeze echoes; the author does not agree with Hardy and Katz that they are due to insects. However, it is agreed that some unusually widespread echo displays on clear days are indeed due to insects. The meteorological value of ultrasensitive radars demonstrated by Hardy and Katz, here, and by others is so profound as to demand their use in remote atmospheric probing.

Ultrasensitive ROS-Responsive Coassemblies of Tellurium-Containing Molecules and Phospholipids.

PubMed

Wang, Lu; Fan, Fuqiang; Cao, Wei; Xu, Huaping

2015-07-29

Reactive oxygen species (ROS) play crucial roles in cell signaling and redox homeostasis and are strongly related to metabolic activities. The increase of the ROS concentration in organisms can result in several diseases, such as cardiovascular diseases and cancer. The concentration of ROS in biologically relevant conditions is typically as low as around tens of micromolars to 100 μM H2O2, which makes it necessary to develop ultrasensitive ROS-responsive systems. A general approach is reported here to fabricate an ultrasensitive ROS-responsive system via coassembly between tellurium-containing molecules and phospholipids, combining the ROS-responsiveness of tellurium and the biocompatibility of phospholipids. By using dynamic light scattering, transmission electron microscopy, scanning electron microscopy, and NMR spectra, coassembly behaviors and the responsiveness of the coassemblies have been investigated. These coassemblies can respond to 100 μM H2O2, which is a biologically relevant ROS concentration, and demonstrate reversible redox properties.

Cobalt oxide nanosheets wrapped onto nickel foam for non-enzymatic detection of glucose

NASA Astrophysics Data System (ADS)

Meng, Shangjun; Wu, Meiyan; Wang, Qian; Dai, Ziyang; Si, Weili; Huang, Wei; Dong, Xiaochen

2016-08-01

Ultra-sensitive and highly selective detection of glucose is essential for the clinical diagnosis of diabetes. In this paper, an ultra-sensitive glucose sensor was successfully fabricated based on cobalt oxide (Co3O4) nanosheets directly grown on nickel foam through a simple hydrothermal method. Characterizations indicated that the Co3O4 nanosheets are completely and uniformly wrapped onto the surface of nickel foam to form a three-dimensional heterostructure. The resulting self-standing electrochemical electrode presents a high performance for the non-enzymatic detection of glucose, including short response time (<10 s), ultra-sensitivity (12.97 mA mM-1 cm-2), excellent selectivity and low detection limit (0.058 μM, S/N = 3). These results indicate that Co3O4 nanosheets wrapped onto nickel foam are a low-cost, practical, and high performance electrochemical electrode for bio sensing.

Ultrasensitive sensing with three-dimensional terahertz metamaterial absorber

NASA Astrophysics Data System (ADS)

Tan, Siyu; Yan, Fengping; Wang, Wei; Zhou, Hong; Hou, Yafei

2018-05-01

Planar metasurfaces and metamaterial absorbers have shown great promise for label-free sensing applications at microwaves, optical and terahertz frequencies. The realization of high-quality-factor resonance in these structures is of significant interest to enhance the sensing sensitivities to detect minute frequency shifts. We propose and demonstrate in this manuscript an ultrasensitive terahertz metamaterial absorber sensor based on a three-dimensional split ring resonator absorber with a high quality factor of 60.09. The sensing performance of the proposed absorber sensor was systematically investigated through detailed numerical calculations and a maximum refractive index sensitivity of 34.40% RIU‑1 was obtained. Furthermore, the absorber sensor can maintain a high sensitivity for a wide range of incidence angles up to 60° under TM polarization incidence. These findings would improve the design flexibility of the absorber sensors and further open up new avenues to achieve ultrasensitive sensing in the terahertz regime.

Evaluation of a new ultrasensitive assay for cardiac troponin I.

PubMed

Casals, Gregori; Filella, Xavier; Bedini, Josep Lluis

2007-12-01

We evaluated the analytical and clinical performance of a new ultrasensitive cardiac troponin I assay (cTnI) on the ADVIA Centaur system (TnI-Ultra). The evaluation included the determination of detection limit, within-assay and between-assay variation and comparison with two other non-ultrasensitive methods. Moreover, cTnI was determined in 120 patients with acute chest pain with three methods. To evaluate the ability of the new method to detect MI earlier, it was assayed in 8 MI patients who first tested negative then positive by the other methods. The detection limit was 0.009 microg/L and imprecision was <10% at all concentrations evaluated. In comparison with two other methods, 10% of the anginas diagnosed were recategorized to MI. The ADVIA Centaur TnI-Ultra assay presented high reproducibility and high sensitivity. The use of the recommended lower cutpoint (0.044 microg/L) implied an increased and earlier identification of MI.

Identification of random nucleic acid sequence aberrations using dual capture probes which hybridize to different chromosome regions

DOEpatents

Lucas, J.N.; Straume, T.; Bogen, K.T.

1998-03-24

A method is provided for detecting nucleic acid sequence aberrations using two immobilization steps. According to the method, a nucleic acid sequence aberration is detected by detecting nucleic acid sequences having both a first nucleic acid sequence type (e.g., from a first chromosome) and a second nucleic acid sequence type (e.g., from a second chromosome), the presence of the first and the second nucleic acid sequence type on the same nucleic acid sequence indicating the presence of a nucleic acid sequence aberration. In the method, immobilization of a first hybridization probe is used to isolate a first set of nucleic acids in the sample which contain the first nucleic acid sequence type. Immobilization of a second hybridization probe is then used to isolate a second set of nucleic acids from within the first set of nucleic acids which contain the second nucleic acid sequence type. The second set of nucleic acids are then detected, their presence indicating the presence of a nucleic acid sequence aberration. 14 figs.

Identification of random nucleic acid sequence aberrations using dual capture probes which hybridize to different chromosome regions

DOEpatents

Lucas, Joe N.; Straume, Tore; Bogen, Kenneth T.

1998-01-01

A method is provided for detecting nucleic acid sequence aberrations using two immobilization steps. According to the method, a nucleic acid sequence aberration is detected by detecting nucleic acid sequences having both a first nucleic acid sequence type (e.g., from a first chromosome) and a second nucleic acid sequence type (e.g., from a second chromosome), the presence of the first and the second nucleic acid sequence type on the same nucleic acid sequence indicating the presence of a nucleic acid sequence aberration. In the method, immobilization of a first hybridization probe is used to isolate a first set of nucleic acids in the sample which contain the first nucleic acid sequence type. Immobilization of a second hybridization probe is then used to isolate a second set of nucleic acids from within the first set of nucleic acids which contain the second nucleic acid sequence type. The second set of nucleic acids are then detected, their presence indicating the presence of a nucleic acid sequence aberration.

Nanostructured hematite for photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Ling, Yichuan

Solar water splitting is an environmentally friendly reaction of producing hydrogen gas. Since Honda and Fujishima first demonstrated solar water splitting in 1972 by using semiconductor titanium dioxide (TiO2) as photoanode in a photoelectrochemical (PEC) cell, extensive efforts have been invested into improving the solar-to-hydrogen (STH) conversion efficiency and lower the production cost of photoelectrochemical devices. In the last few years, hematite (alpha-Fe2O3) nanostructures have been extensively studied as photoanodes for PEC water splitting. Although nanostructured hematite can improve its photoelectrochemical water splitting performance to some extent, by increasing active sites for water oxidation and shortening photogenerated hole path length to semiconductor/electrolyte interface, the photoactivity of pristine hematite nanostructures is still limited by a number of factors, such as poor electrical conductivities and slow oxygen evolution reaction kinetics. Previous studies have shown that tin (Sn) as an n-type dopant can substantially enhance the photoactivity of hematite photoanodes by modifying their optical and electrical properties. In this thesis, I will first demonstrate an unintentional Sn-doping method via high temperature annealing of hematite nanowires grown on fluorine-doped tin oxide (FTO) substrate to enhance the donor density. In addition to introducing extrinsic dopants into semiconductors, the carrier densities of hematite can also be enhanced by creating intrinsic defects. Oxygen vacancies function as shallow donors for a number of hematite. In this regard, I have investigated the influence of oxygen content on thermal decomposition of FeOOH to induce oxygen vacancies in hematite. In the end, I have studied low temperature activation of hematite nanostructures.

ZnO nanoflower-based photoelectrochemical DNAzyme sensor for the detection of Pb2+.

PubMed

Zhang, Bintian; Lu, Lili; Hu, Qichang; Huang, Feng; Lin, Zhang

2014-06-15

Lead contamination is now widespread, and exposure to lead may cause adverse effects on human beings. In this study, a photoelectrochemical sensor based on flower-like ZnO nanostructures was developed for Pb(2+) detection, using a Pb(2+)-dependent DNAzyme as the recognition unit and a double-strand DNA intercalator, Ru(bpy)2(dppz)(2+) (bpy=2,2'-bipyridine, dppz=dipyrido[3,2-a:2',3'-c] phenazine) as the photoelectrochemical signal reporter. The ZnO nanoflower was fabricated on an indium tin oxide (ITO) electrode by the convenient hydrothermal decomposition method. The morphology and photoelectrochemical property of the ZnO nanoflowers were characterized by SEM, XRD and photocurrent measurements. DNAzyme-substrate duplex was assembled on an ITO/ZnO electrode through electrostatic adsorption. In the presence of Pb(2+), RNA-cleavage activity of the DNAzyme was activated and its substrate strand was cleaved, resulting in the release of Ru(bpy)2(dppz)(2+) from the DNA film and the concomitant photocurrent decrease. The detection principle was verified by fluorescence measurements. Under the optimized conditions, a linear relationship between photocurrent and Pb(2+) concentration was obtained over the range of 0.5-20 nM, with a detection limit of 0.1 nM. Interference from other common metal ions was found negligible. Applicability of the sensor was demonstrated by analyzing lead level in human serum and Pb(2+) spiked water samples. This facile and economical sensor system showed high sensitivity and selectivity, thus can be potentially applied for on-site monitoring of lead contaminant. Copyright © 2014 Elsevier B.V. All rights reserved.

All-nanoparticle self-assembly ZnO/TiO₂ heterojunction thin films with remarkably enhanced photoelectrochemical activity.

PubMed

Yuan, Sujun; Mu, Jiuke; Mao, Ruiyi; Li, Yaogang; Zhang, Qinghong; Wang, Hongzhi

2014-04-23

The multilaminated ZnO/TiO2 heterojunction films were successfully deposited on conductive substrates including fluorine-doped tin oxide (FTO) glass and flexible indium tin oxide coated poly(ethylene terephthalate) via the layer-by-layer (LBL) self assembly method from the oxide colloids without using any polyelectrolytes. The positively charged ZnO nanoparticles and the negatively charged TiO2 nanoparticles were directly used as the components in the consecutive deposition process to prepare the heterojunction thin films by varying the thicknesses. Moreover, the crystal growth of both oxides could be efficiently inhibited by the good connection between ZnO and TiO2 nanoparticles even after calcination at 500 °C, especially for ZnO which was able to keep the crystallite size under 25 nm. The as-prepared films were used as the working electrodes in the three-electrode photoelectrochemical cells. Because the well-contacted nanoscale heterojunctions were formed during the LBL self-assembling process, the ZnO/TiO2 all-nanoparticle films deposited on both substrates showed remarkably enhanced photoelectrochemical properties compared to that of the well-established TiO2 LBL thin films with similar thicknesses. The photocurrent response collected from the ZnO/TiO2 electrode on the FTO glass substrate was about five times higher than that collected from the TiO2 electrode. Owing to the absence of the insulating layer of dried polyelectrolytes, the ZnO/TiO2 all-nanoparticle heterojunction films were expected to be used in the photoelectrochemical device before calcination.

Standalone anion- and co-doped titanium dioxide nanotubes for photocatalytic and photoelectrochemical solar-to-fuel conversion.

PubMed

Ding, Yuchen; Nagpal, Prashant

2016-10-14

Several strategies are currently being investigated for conversion of incident sunlight into renewable sources of energy, and photocatalytic or photoelectrochemical production of solar fuels can provide an important alternative. Titanium dioxide (TiO 2 ) has been heavily investigated as a material of choice due to its excellent optoelectronic properties and stability, and anion-doping proposed as a pathway to improve light absorption as well as improving the efficiency of oxygen production. While several studies have used morphological tuning, elemental doping, and surface engineering in TiO 2 to extend its absorption, there is a need to optimize simultaneously charge transport and improve interfacial chemical reaction kinetics. Here we show anion-doped (nitrogen, carbon) standalone TiO 2 nanotube membranes that absorb visible light for the water-splitting reaction, using both wireless (photocatalysis) and wired (photoelectrochemical) solar-to-fuel conversion (STFC) cells. Using simulated solar radiation, we show generation of hydrogen as a solar fuel using visible light photocatalysis. Furthermore, using a model we elucidate detailed photophysics and photoelectrochemical properties of these nanotubes, and explain the kinetics of photogenerated charge carriers following light absorption. We show that while visible light induces a superlinear photoresponse for catalytic reduction and may benefit from higher incident light intensity, ultraviolet light shows a linear photoresponse and saturation with higher light flux due to trapping of photogenerated charges (mainly electrons). These results can have important implications for design of other metal-oxide membranes for solar fuel generation, and appropriate design of dopants and induced energy levels in these photocatalysts.

Cathodic Electrodeposition of Ni-Mo on Semiconducting NiFe2 O4 for Photoelectrochemical Hydrogen Evolution in Alkaline Media.

PubMed

Wijten, Jochem H J; Jong, Ronald P H; Mul, Guido; Weckhuysen, Bert M

2018-04-25

Photocathodes for hydrogen evolution from water were made by electrodeposition of Ni-Mo layers on NiFe 2 O 4 substrates, deposited by spin coating on F:SnO 2 -glass. Analysis confirmed the formation of two separate layers, without significant reduction of NiFe 2 O 4 . Bare NiFe 2 O 4 was found to be unstable under alkaline conditions during (photo)electrochemistry. To improve the stability significantly, the deposition of a bifunctional Ni-Mo layer through a facile electrodeposition process was performed and the composite electrodes showed stable operation for at least 1 h. Moreover, photocurrents up to -2.1 mA cm -2 at -0.3 V vs. RHE were obtained for Ni-Mo/NiFe 2 O 4 under ambient conditions, showing that the new combination functions as both a stabilizing and catalytic layer for the photoelectrochemical evolution of hydrogen. The photoelectrochemical response of these composite electrodes decreased with increasing NiFe 2 O 4 layer thickness. Transient absorption spectroscopy showed that the lifetime of excited states is short and on the ns timescale. An increase in lifetime was observed for NiFe 2 O 4 of large layer thickness, likely explained by decreasing the defect density in the primary layer(s), as a result of repetitive annealing at elevated temperature. The photoelectrochemical and transient absorption spectroscopy results indicated that a short charge carrier lifetime limits the performance of Ni-Mo/NiFe 2 O 4 photocathodes. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

RGO modified Ni doped FeOOH for enhanced electrochemical and photoelectrochemical water oxidation

NASA Astrophysics Data System (ADS)

Zhang, Xiaofan; Zhang, Bingyan; Liu, Shuangshuang; Kang, Hongwei; Kong, Weiqian; Zhang, Shouren; Shen, Yan; Yang, Baocheng

2018-04-01

Ni,Fe-based (oxy)hydroxides have been one of the most active catalysts for the oxygen evolution reaction. In this article, reduced graphene oxide supported Ni doped FeOOH (RGO/Ni:FeOOH) was prepared for electrochemical and photoelectrochemical (PEC) water oxidation. The RGO/Ni:FeOOH exhibited a lower over-potential (260 mV at 10 mA cm-2) and smaller Tafel slope (32.3 mV dec-1) than that of the FeOOH and Ni:FeOOH. Such significant enhancement is attributed to Ni doping and RGO, which reduce the over-potential, improve the conductivity and enlarge surface areas. Besides, RGO/Ni:FeOOH decorated the TiO2 nanorods (NRs) was also fabricated for photoelectrochemical (PEC) water oxidation, which exhibited a higher photocurrent density and lower onset potential than that of TiO2 NRs the bare under illumination due to the synergistic effect of RGO and Ni:FeOOH. These results demonstrate the RGO/Ni:FeOOH has great promising as a co-catalyst to improve the PEC performance.

Revealing the semiconductor–catalyst interface in buried platinum black silicon photocathodes

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

Aguiar, Jeffery A.; Anderson, Nicholas C.; Neale, Nathan R.

2016-01-01

Nanoporous 'black' silicon semiconductors interfaced with buried platinum nanoparticle catalysts have exhibited stable activity for photoelectrochemical hydrogen evolution even after months of exposure to ambient conditions. The mechanism behind this stability has not been explained in detail, but is thought to involve a Pt/Si interface free from SiOx layer that would adversely affect interfacial charge transfer kinetics. In this paper, we resolve the chemical composition and structure of buried Pt/Si interfaces in black silicon photocathodes from a micron to sub-nanometer level using aberration corrected analytical scanning transmission electron microscopy. Through a controlled electrodeposition of copper on samples aged for onemore » month in ambient conditions, we demonstrate that the main active catalytic sites are the buried Pt nanoparticles located below the 400-800 nm thick nanoporous SiOx layer. Though hydrogen production performance degrades over 100 h under photoelectrochemical operating conditions, this burying strategy preserves an atomically clean catalyst/Si interface free of oxide or other phases under air exposure and provides an example of a potential method for stabilizing silicon photoelectrodes from oxidative degradation in photoelectrochemical applications.« less

Mesoscale modeling of photoelectrochemical devices: light absorption and carrier collection in monolithic, tandem, Si|WO3 microwires.

PubMed

Fountaine, Katherine T; Atwater, Harry A

2014-10-20

We analyze mesoscale light absorption and carrier collection in a tandem junction photoelectrochemical device using electromagnetic simulations. The tandem device consists of silicon (E(g,Si) = 1.1 eV) and tungsten oxide (E(g,WO3) = 2.6 eV) as photocathode and photoanode materials, respectively. Specifically, we investigated Si microwires with lengths of 100 µm, and diameters of 2 µm, with a 7 µm pitch, covered vertically with 50 µm of WO3 with a thickness of 1 µm. Many geometrical variants of this prototypical tandem device were explored. For conditions of illumination with the AM 1.5G spectra, the nominal design resulted in a short circuit current density, J(SC), of 1 mA/cm(2), which is limited by the WO3 absorption. Geometrical optimization of photoanode and photocathode shape and contact material selection, enabled a three-fold increase in short circuit current density relative to the initial design via enhanced WO3 light absorption. These findings validate the usefulness of a mesoscale analysis for ascertaining optimum optoelectronic performance in photoelectrochemical devices.

A new photoelectrochemical biosensors based on DNA conformational changes and isothermal circular strand-displacement polymerization reaction.

PubMed

Zhang, Xiaoru; Xu, Yunpeng; Zhao, Yanqing; Song, Weiling

2013-01-15

We report a strategy for the transduction of DNA hybridization into a readily detectable photoelectrochemical signal by means of a conformational change analogous to electrochemical DNA (E-DNA) approach. To demonstrate the effect of distance change for photosensitizer to the surface of electrode on the change of photocurrent, photosensitizer Ru(bpy)(2)(dcbpy)(2+) tagged DNA stem-loop structures were self-assembled onto a nanogold modified ITO electrode. Hybridization induced a large conformational change in DNA structure, which in turn significantly altered the electron-transfer tunneling distance between the electrode and photosensitizer. The resulting change in photocurrent was proportional to the concentration of DNA in the range of 1.0×10(-10)-8.0×10(-9)M. In order to improve the sensitivity of the photoelectrochemical biosensor, an amplified detection method based on isothermal strand displacement polymerization reaction was employed. With multiple rounds of isothermal strand replication, which led to strand displacement and constituted consecutive signal amplification, a detection limit of 9.4×10(-14)M target DNA was achieved. Copyright © 2012 Elsevier B.V. All rights reserved.

Tunable Syngas Production from CO2 and H2 O in an Aqueous Photoelectrochemical Cell.

PubMed

Chu, Sheng; Fan, Shizhao; Wang, Yongjie; Rossouw, David; Wang, Yichen; Botton, Gianluigi A; Mi, Zetian

2016-11-07

Syngas, the mixture of CO and H 2 , is a key feedstock to produce methanol and liquid fuels in industry, yet limited success has been made to develop clean syngas production using renewable solar energy. We demonstrated that syngas with a benchmark turnover number of 1330 and a desirable CO/H 2 ratio of 1:2 could be attained from photoelectrochemical CO 2 and H 2 O reduction in an aqueous medium by exploiting the synergistic co-catalytic effect between Cu and ZnO. The CO/H 2 ratio in the syngas products was tuned in a large range between 2:1 and 1:4 with a total unity Faradaic efficiency. Moreover, a high Faradaic efficiency of 70 % for CO was acheived at underpotential of 180 mV, which is the lowest potential ever reported in an aqueous photoelectrochemical cell. It was found that the combination of Cu and ZnO offered complementary chemical properties that lead to special reaction channels not seen in Cu, or ZnO alone. © 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

p-Type Doping of GaN Nanowires Characterized by Photoelectrochemical Measurements.

PubMed

Kamimura, Jumpei; Bogdanoff, Peter; Ramsteiner, Manfred; Corfdir, Pierre; Feix, Felix; Geelhaar, Lutz; Riechert, Henning

2017-03-08

GaN nanowires (NWs) doped with Mg as a p-type impurity were grown on Si(111) substrates by plasma-assisted molecular beam epitaxy. In a systematic series of experiments, the amount of Mg supplied during NW growth was varied. The incorporation of Mg into the NWs was confirmed by the observation of donor-acceptor pairs and acceptor-bound excitons in low-temperature photoluminescence spectroscopy. Quantitative information about the Mg concentrations was deduced from Raman scattering by local vibrational modes related to Mg. In order to study the type and density of charge carriers present in the NWs, we employed two photoelectrochemical techniques, open-circuit potential and Mott-Schottky measurements. Both methods showed the expected transition from n-type to p-type conductivity with increasing Mg doping level, and the latter characterization technique allowed us to quantify the charge carrier concentration. Beyond the quantitative information obtained for Mg doping of GaN NWs, our systematic and comprehensive investigation demonstrates the benefit of photoelectrochemical methods for the analysis of doping in semiconductor NWs in general.

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.

Different strategies for the detection of bioagents using electrochemical and photoelectrochemical genosensors

NASA Astrophysics Data System (ADS)

Voccia, Diego; Bettazi, Francesca; Palchetti, Ilaria

2015-10-01

In recent years various kinds of biosensors for the detection of pathogens have been developed. A genosensor consists in the immobilization, onto the surface of a chosen transducer, of an oligonucleotide with a specific base sequence called capture probe. The complementary sequence (the analytical target, i.e. a specific sequence of the DNA/RNA of the pathogen) present in the sample is recognized and captured by the probe through the hybridization reaction. The evaluation of the extent of the hybridization allows one to confirm whether the sample contains the complementary sequence of the probe or not. Electrochemical transducers have received considerable attention in connection with the detection of DNA hybridization. Moreover, recently, with the emergence of novel photoelectrochemically active species and new detection schemes, photoelectrochemistry has resulted in substantial progress in its analytical performance for biosensing applications. In this paper, some examples of electrochemical genosensors for multiplexed pathogen detection are shown. Moreover, the preliminary experiments towards the development of a photoelectrochemical genosensor using a TiO2 - nanocrystal-modified ITO electrode are discussed.

Photoinduced deposition of gold nanoparticles on TiO2-WO3 nanotube films as efficient photoanodes for solar water splitting

NASA Astrophysics Data System (ADS)

Momeni, Mohamad Mohsen; Ghayeb, Yousef

2016-06-01

Gold-modified TiO2-WO3 nanotubes with different amounts of gold were obtained by two methods; photoassisted deposition and one-step electrochemical anodizing method. The morphology, crystallinity and elemental composition were studied by FE-SEM, XRD and EDX. The photoelectrochemical performance was examined under Xe light illumination in 1 M NaOH electrolyte. Characterization of the as-prepared TiO2-WO3 samples indicated that sodium tungstate concentration in anodizing solution significantly influenced the morphology and photoelectrochemical activity of fabricated films. Also, photoelectrochemical characterizations show that the photocatalytic activity of Au/TiO2-WO3 nanotubes was improved as compared with that of bare TiO2-WO3 nanotubes. The experimental results showed that the photocatalytic activities of Au/TiO2-WO3 were significantly affected by the amount of Au nanoparticles. The amount of gold nanoparticles was effectively controlled by time of photoreduction of the chloroauric acid solution. These new photoanodes showed enhanced high photocurrent density with good stability and are a highly promising photoanodes for photocatalytic hydrogen production.

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

Todt, Michael A.; Isenberg, Allan E.; Nanayakkara, Sanjini U.

Semiconducting transition-metal dichalcogenide (TMD) nanoflake thin films are promising large-area electrodes for photo-electrochemical solar energy conversion applications. However, their energy conversion efficiencies are typically much lower than those of bulk electrodes. It is unclear to what extent this efficiency gap stems from differences among nanoflakes (e.g., area, thickness, and surface structural features). It is also unclear whether individual exfoliated nanoflakes can achieve energy conversion efficiencies similar to those of bulk crystals. Here, we use a single-nanoflake photo-electrochemical approach to show that there are both highly active and completely inactive nanoflakes within a film. For the exfoliated MoSe 2 samples studiedmore » herein, 7% of nanoflakes are highly active champions, whose photocurrent efficiency exceeds that of the bulk crystal. However, 66% of nanoflakes are inactive spectators, which are mostly responsible for the overall lower photocurrent efficiency compared to the bulk crystal. The photocurrent collection efficiency increases with nanoflake area and decreases more at perimeter edges than at interior step edges. These observations, which are hidden in ensemble-level measurements, reveal the underlying performance issues of exfoliated TMD electrodes for photo-electrochemical energy conversion applications.« less

A dye-sensitized photoelectrochemical tandem cell for light driven hydrogen production from water

DOE PAGES

Sherman, Benjamin D.; Sheridan, Matthew V.; Wee, Kyung -Ryang; ...

2016-12-02

Here, tandem junction photoelectrochemical water-splitting devices, whereby two light absorbing electrodes targeting separate portions of the solar spectrum generate the voltage required to convert water to oxygen and hydrogen, enable much higher possible efficiencies than single absorber systems. We report here on the development of a tandem system consisting of a dye-sensitized photoelectrochemical cell (DSPEC) wired in series with a dye-sensitized solar cell (DSC). The DSPEC photoanode incorporates a tris(bipyridine)ruthenium(II)-type chromophore and molecular ruthenium based water oxidation catalyst. The DSPEC was tested with two more-red absorbing DSC variations, one utilizing N719 dye with an I 3 –/I – redox mediatormore » solution and the other D35 dye with a tris(bipyridine)cobalt ([Co(bpy) 3] 3+/2+) based mediator. The tandem configuration consisting of the DSPEC and D35/[Co(bpy) 3] 3+/2+ based DSC gave the best overall performance and demonstrated the production of H 2 from H 2O with the only energy input from simulated solar illumination.« less

Photoelectrochemical Performance of TiO2/Ti Electrode for Organic Compounds

NASA Astrophysics Data System (ADS)

Maulidiyah, M.; Wijawan, I. B. P.; Wibowo, D.; Aladin, A.; Hamzah, B.; Nurdin, M.

2018-05-01

Photoelectrochemical performance of TiO2/Ti electrode was investigated by using organic compounds. The TiO2/Ti electrode was prepared by anodic oxidation at a potential bias of 25 V for 4 h then calcined for 450 °C to obtain the anatase polymorph. Subsequently, it was characterized by X-Ray Diffraction (XRD) and Scanning Electron Microscope-Energy Dispersive X-ray (SEM-EDX). The XRD pattern showed that TiO2 has anatase phase as confirmed by 2θ peaks at 37.93° 63.00°, and 83.00°. Using SEM-EDX data the TiO2 layer was formed on Ti plate with the composition of Ti (4.5 keV) and O (0.5 keV) elements. Furthermore, the photoelectrochemical sensing on the three organic compounds (ascorbic acid, glucose, and titan yellow) with the electrolyte addition showed that the linearity of TiO2/Ti electrode were 0.937, 0.968, and 0.938, meanwhile without the electrolyte were 0.998, 0.989, and 0.923, respectively.

The Ultrasensitivity of Living Polymers

NASA Astrophysics Data System (ADS)

O'Shaughnessy, Ben; Vavylonis, Dimitrios

2003-03-01

Synthetic and biological living polymers are self-assembling chains whose chain length distributions (CLDs) are dynamic. We show these dynamics are ultrasensitive: Even a small perturbation (e.g., temperature jump) nonlinearly distorts the CLD, eliminating or massively augmenting short chains. The origin is fast relaxation of mass variables (mean chain length, monomer concentration) which perturbs CLD shape variables before these can relax via slow chain growth rate fluctuations. Viscosity relaxation predictions agree with experiments on the best-studied synthetic system, α-methylstyrene.

Ultrasensitive, Biocompatible, Self-Calibrating, Multiparametric Temperature Sensors.

PubMed

Zhao, Haiguang; Vomiero, Alberto; Rosei, Federico

2015-11-18

Core-shell quantum dots serve as self-calibrating, ultrasensitive, multiparametric, near-infrared, and biocompatible temperature sensors. They allow temperature measurement with nanometer accuracy in the range 150-373 K, the broadest ever recorded for a nanothermometer, with sensitivities among the highest ever reported, which makes them essentially unique in the panorama of biocompatible nanothermometers with potential for in vivo biological thermal imaging and/or thermoablative therapy. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Comparability of AMH levels among commercially available immunoassays

PubMed Central

Su, H. Irene; Sammel, Mary D.; Homer, Michael V.; Bui, Kim; Haunschild, Carolyn; Stanczyk, Frank Z.

2015-01-01

Objective To compare AMH levels among three commercially available AMH immunoassays (AMH Gen II, Beckman Coulter; Ultrasensitive AMH, AnshLab; picoAMH, AnshLab) Design Cross-sectional Setting Academic reproductive endocrinology program Patients 90 newly diagnosed breast cancer patients prior to cancer treatment Interventions None Outcome 1) proportion of detectable AMH levels by immunoassay, 2) comparability among assays Results At a mean age of 38.1, the median (interquartile range) for AMH levels for the cohort were 0.92 [1.35] ng/mL for the Gen II assay, 1.68 [2.30] ng/mL for the Ultrasensitive and 1.5 [2.41] ng/mL for the picoAMH assays. Significantly higher proportions of detectable AMH levels were observed with the picoAMH kit (97%) compared to both Gen II (84%) and Ultrasensitive (92%) assays. Although AMH results were highly correlated among assays (r=0.92–0.99), Gen II AMH levels were consistently lower than both Ultrasensitive and picoAMH levels. Moreover, as AMH levels increased, the magnitude of difference grew larger between Gen II and each of the other two assays. Conclusions Measurement of AMH levels with the picoAMH kit maximized detection at very low levels, particularly in contrast to the Gen II kit. Conversion of AMH levels from different immunoassays using regression equations is potentially highly inaccurate. PMID:24726216

Sulfophenyl-Functionalized Reduced Graphene Oxide Networks on Electrospun 3D Scaffold for Ultrasensitive NO₂ Gas Sensor.

PubMed

Zou, Bin; Guo, Yunlong; Shen, Nannan; Xiao, Anshan; Li, Mingjun; Zhu, Liang; Wan, Pengbo; Sun, Xiaoming

2017-12-19

Ultrasensitive room temperature real-time NO₂ sensors are highly desirable due to potential threats on environmental security and personal respiratory. Traditional NO₂ gas sensors with highly operated temperatures (200-600 °C) and limited reversibility are mainly constructed from semiconducting oxide-deposited ceramic tubes or inter-finger probes. Herein, we report the functionalized graphene network film sensors assembled on an electrospun three-dimensional (3D) nanonetwork skeleton for ultrasensitive NO₂ sensing. The functional 3D scaffold was prepared by electrospinning interconnected polyacrylonitrile (PAN) nanofibers onto a nylon window screen to provide a 3D nanonetwork skeleton. Then, the sulfophenyl-functionalized reduced graphene oxide (SFRGO) was assembled on the electrospun 3D nanonetwork skeleton to form SFRGO network films. The assembled functionalized graphene network film sensors exhibit excellent NO₂ sensing performance (10 ppb to 20 ppm) at room temperature, reliable reversibility, good selectivity, and better sensing cycle stability. These improvements can be ascribed to the functionalization of graphene with electron-withdrawing sulfophenyl groups, the high surface-to-volume ratio, and the effective sensing channels from SFRGO wrapping onto the interconnected 3D scaffold. The SFRGO network-sensing film has the advantages of simple preparation, low cost, good processability, and ultrasensitive NO₂ sensing, all advantages that can be utilized for potential integration into smart windows and wearable electronic devices for real-time household gas sensors.

Design of In Situ Poled Ce(3+)-Doped Electrospun PVDF/Graphene Composite Nanofibers for Fabrication of Nanopressure Sensor and Ultrasensitive Acoustic Nanogenerator.

PubMed

Garain, Samiran; Jana, Santanu; Sinha, Tridib Kumar; Mandal, Dipankar

2016-02-01

We report an efficient, low-cost in situ poled fabrication strategy to construct a large area, highly sensitive, flexible pressure sensor by electrospun Ce(3+) doped PVDF/graphene composite nanofibers. The entire device fabrication process is scalable and enabling to large-area integration. It can able to detect imparting pressure as low as 2 Pa with high level of sensitivity. Furthermore, Ce(3+)-doped PVDF/graphene nanofiber based ultrasensitive pressure sensors can also be used as an effective nanogenerator as it generating an output voltage of 11 V with a current density ∼6 nA/cm(2) upon repetitive application of mechanical stress that could lit up 10 blue light emitting diodes (LEDs) instantaneously. Furthermore, to use it in environmental random vibrations (such as wind flow, water fall, transportation of vehicles, etc.), nanogenerator is integrated with musical vibration that exhibits to power up three blue LEDs instantly that promises as an ultrasensitive acoustic nanogenerator (ANG). The superior sensing properties in conjunction with mechanical flexibility, integrability, and robustness of nanofibers enabled real-time monitoring of sound waves as well as detection of different type of musical vibrations. Thus, ANG promises to use as an ultrasensitive pressure sensor, mechanical energy harvester, and effective power source for portable electronic and wearable devices.

Light-driven OR and XOR programmable chemical logic gates.

PubMed

Szaciłowski, Konrad; Macyk, Wojciech; Stochel, Grazyna

2006-04-12

Photoelectrodes made of nanocrystalline titanium dioxide modified with various pentacyanoferrates exhibit unique photoelectrochemical properties; photocurrent direction can be switched from anodic to cathodic and vice versa upon changes in photoelectrode potential and incident light wavelength (PhotoElectrochemical Photocurrent Switching, PEPS effect). At certain potentials, anodic photocurrent generated upon UV irradiation has the same intensity as the cathodic photocurrent generated upon visible irradiation. Under these conditions, simultaneous irradiation with UV and visible light results in compensation of anodic and cathodic photocurrents, and zero net photocurrent is observed. This process can be used for construction of unique light-driven chemical logic gates.

Photoelectrochemical cells including chalcogenophosphate photoelectrodes

NASA Technical Reports Server (NTRS)

Reichman, B.; Byvik, C. E. (Inventor)

1984-01-01

Photoelectrochemical cells employing chalcogenophosphate (MPX3) photoelectrodes are described where M is selected from the group of transition metal series of elements beginning with scandium (atomic number 21) through germanium (atomic number 32) yttrium (atomic number 39) through antimony (atomic number 51) and lanthanum (atomic number 57) through polonium (atomic number 84); P is phosphorus; and X is selected from the chalogenide series consisting of sulfur, selenium, and tellurium. These compounds have bandgaps in the desirable range from 2.0 eV to 2.2 eV for the photoelectrolysis of water and are stable when used as photoelectrodes for the same.

Solar energy conversion in a photoelectrochemical biofuel cell.

PubMed

Hambourger, Michael; Kodis, Gerdenis; Vaughn, Michael D; Moore, Gary F; Gust, Devens; Moore, Ana L; Moore, Thomas A

2009-12-07

A photoelectrochemical biofuel cell has been developed which incorporates aspects of both an enzymatic biofuel cell and a dye-sensitized solar cell. Photon absorption at a porphyrin-sensitized n-type semiconductor electrode gives rise to a charge-separated state. Electrons and holes are shuttled to appropriate cathodic and anodic catalysts, respectively, allowing the production of electricity, or a reduced fuel, via the photochemical oxidation of a biomass-derived substrate. The operation of this device is reviewed. The use of alternate anodic redox mediators provides insight regarding loss mechanisms in the device. Design strategies for enhanced performance are discussed.

Method for isolating chromosomal DNA in preparation for hybridization in suspension

DOEpatents

Lucas, Joe N.

2000-01-01

A method is provided for detecting nucleic acid sequence aberrations using two immobilization steps. According to the method, a nucleic acid sequence aberration is detected by detecting nucleic acid sequences having both a first nucleic acid sequence type (e.g., from a first chromosome) and a second nucleic acid sequence type (e.g., from a second chromosome), the presence of the first and the second nucleic acid sequence type on the same nucleic acid sequence indicating the presence of a nucleic acid sequence aberration. In the method, immobilization of a first hybridization probe is used to isolate a first set of nucleic acids in the sample which contain the first nucleic acid sequence type. Immobilization of a second hybridization probe is then used to isolate a second set of nucleic acids from within the first set of nucleic acids which contain the second nucleic acid sequence type. The second set of nucleic acids are then detected, their presence indicating the presence of a nucleic acid sequence aberration. Chromosomal DNA in a sample containing cell debris is prepared for hybridization in suspension by treating the mixture with RNase. The treated DNA can also be fixed prior to hybridization.

Quantitative and Cost Comparison of Ultrasensitive Human Immunodeficiency Virus Type 1 RNA Viral Load Assays: Bayer bDNA Quantiplex Versions 3.0 and 2.0 and Roche PCR Amplicor Monitor Version 1.5

PubMed Central

Elbeik, Tarek; Charlebois, Edwin; Nassos, Patricia; Kahn, James; Hecht, Frederick M.; Yajko, David; Ng, Valerie; Hadley, Keith

2000-01-01

Quantification of human immunodeficiency virus type 1 (HIV-1) RNA as a measure of viral load has greatly improved the monitoring of therapies for infected individuals. With the significant reductions in viral load now observed in individuals treated with highly active anti-retroviral therapy (HAART), viral load assays have been adapted to achieve greater sensitivity. Two commercially available ultrasensitive assays, the Bayer Quantiplex HIV-1 bDNA version 3.0 (bDNA 3.0) assay and the Roche Amplicor HIV-1 Monitor Ultrasensitive version 1.5 (Amplicor 1.5) assay, are now being used to monitor HIV-1-infected individuals. Both of these ultrasensitive assays have a reported lower limit of 50 HIV-1 RNA copies/ml and were developed from corresponding older generation assays with lower limits of 400 to 500 copies/ml. However, the comparability of viral load data generated by these ultrasensitive assays and the relative costs of labor, disposables, and biohazardous wastes were not determined in most cases. In this study, we used matched clinical plasma samples to compare the quantification of the newer bDNA 3.0 assay with that of the older bDNA 2.0 assay and to compare the quantification and costs of the bDNA 3.0 assay and the Amplicor 1.5 assay. We found that quantification by the bDNA 3.0 assay was approximately twofold higher than that by the bDNA 2.0 assay and was highly correlated to that by the Amplicor 1.5 assay. Moreover, cost analysis based on labor, disposables, and biohazardous wastes showed significant savings with the bDNA 3.0 assay as compared to the costs of the Amplicor 1.5 assay. PMID:10699005

Quantitative and cost comparison of ultrasensitive human immunodeficiency virus type 1 RNA viral load assays: Bayer bDNA quantiplex versions 3.0 and 2.0 and Roche PCR Amplicor monitor version 1.5.

PubMed

Elbeik, T; Charlebois, E; Nassos, P; Kahn, J; Hecht, F M; Yajko, D; Ng, V; Hadley, K

2000-03-01

Quantification of human immunodeficiency virus type 1 (HIV-1) RNA as a measure of viral load has greatly improved the monitoring of therapies for infected individuals. With the significant reductions in viral load now observed in individuals treated with highly active anti-retroviral therapy (HAART), viral load assays have been adapted to achieve greater sensitivity. Two commercially available ultrasensitive assays, the Bayer Quantiplex HIV-1 bDNA version 3.0 (bDNA 3.0) assay and the Roche Amplicor HIV-1 Monitor Ultrasensitive version 1.5 (Amplicor 1.5) assay, are now being used to monitor HIV-1-infected individuals. Both of these ultrasensitive assays have a reported lower limit of 50 HIV-1 RNA copies/ml and were developed from corresponding older generation assays with lower limits of 400 to 500 copies/ml. However, the comparability of viral load data generated by these ultrasensitive assays and the relative costs of labor, disposables, and biohazardous wastes were not determined in most cases. In this study, we used matched clinical plasma samples to compare the quantification of the newer bDNA 3.0 assay with that of the older bDNA 2.0 assay and to compare the quantification and costs of the bDNA 3.0 assay and the Amplicor 1.5 assay. We found that quantification by the bDNA 3.0 assay was approximately twofold higher than that by the bDNA 2.0 assay and was highly correlated to that by the Amplicor 1.5 assay. Moreover, cost analysis based on labor, disposables, and biohazardous wastes showed significant savings with the bDNA 3.0 assay as compared to the costs of the Amplicor 1.5 assay.

Ultrasensitive Hybridization-Based ELISA Method for the Determination of Phosphorodiamidate Morpholino Oligonucleotides in Biological samples.

PubMed

Burki, Umar; Straub, Volker

2017-01-01

Determining the concentration of oligonucleotide in biological samples such as tissue lysate and serum is essential for determining the biodistribution and pharmacokinetic profile, respectively. ELISA-based assays have shown far greater sensitivities compared to other methods such as HPLC and LC/MS. Here, we describe a novel ultrasensitive hybridization-based ELISA method for quantitating morpholino oligonucleotides in mouse tissue lysate and serum samples. The assay has a linear detection range of 5-250 pM (R2 > 0.99).

Converting environmentally hazardous materials into clean energy using a novel nanostructured photoelectrochemical fuel cell

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

Gan, Yong X., E-mail: yong.gan@utoledo.edu; Gan, Bo J.; Clark, Evan

2012-09-15

Highlights: ► A photoelectrochemical fuel cell has been made from TiO{sub 2} nanotubes. ► The fuel cell decomposes environmentally hazardous materials to produce electricity. ► Doping the anode with a transition metal oxide increases the visible light sensitivity. ► Loading the anode with a conducting polymer enhances the visible light absorption. -- Abstract: In this work, a novel photoelectrochemical fuel cell consisting of a titanium dioxide nanotube array photosensitive anode and a platinum cathode was made for decomposing environmentally hazardous materials to produce electricity and clean fuel. Titanium dioxide nanotubes (TiO{sub 2} NTs) were prepared via electrochemical oxidation of puremore » Ti in an ammonium fluoride and glycerol-containing solution. Scanning electron microscopy was used to analyze the morphology of the nanotubes. The average diameter, wall thickness and length of the as-prepared TiO{sub 2} NTs were determined. The photosensitive anode made from the highly ordered TiO{sub 2} NTs has good photo-catalytic property, as proven by the decomposition tests on urea, ammonia, sodium sulfide and automobile engine coolant under ultraviolet (UV) radiation. To improve the efficiency of the fuel cell, doping the TiO{sub 2} NTs with a transition metal oxide, NiO, was performed and the photosensitivity of the doped anode was tested under visible light irradiation. It is found that the NiO-doped anode is sensitive to visible light. Also found is that polyaniline-doped photosensitive anode can harvest photon energy in the visible light spectrum range much more efficiently than the NiO-doped one. It is concluded that the nanostructured photoelectrochemical fuel cell can generate electricity and clean fuel by decomposing hazardous materials under sunlight.« less

High density and ligand affinity confer ultrasensitive signal detection by a guanylyl cyclase chemoreceptor

PubMed Central

Pichlo, Magdalena; Bungert-Plümke, Stefanie; Weyand, Ingo; Seifert, Reinhard; Bönigk, Wolfgang; Strünker, Timo; Kashikar, Nachiket Dilip; Goodwin, Normann; Müller, Astrid; Körschen, Heinz G.; Collienne, Ursel; Pelzer, Patric; Van, Qui; Enderlein, Jörg; Klemm, Clementine; Krause, Eberhard; Trötschel, Christian; Poetsch, Ansgar; Kremmer, Elisabeth

2014-01-01

Guanylyl cyclases (GCs), which synthesize the messenger cyclic guanosine 3′,5′-monophosphate, control several sensory functions, such as phototransduction, chemosensation, and thermosensation, in many species from worms to mammals. The GC chemoreceptor in sea urchin sperm can decode chemoattractant concentrations with single-molecule sensitivity. The molecular and cellular underpinnings of such ultrasensitivity are not known for any eukaryotic chemoreceptor. In this paper, we show that an exquisitely high density of 3 × 105 GC chemoreceptors and subnanomolar ligand affinity provide a high ligand-capture efficacy and render sperm perfect absorbers. The GC activity is terminated within 150 ms by dephosphorylation steps of the receptor, which provides a means for precise control of the GC lifetime and which reduces “molecule noise.” Compared with other ultrasensitive sensory systems, the 10-fold signal amplification by the GC receptor is surprisingly low. The hallmarks of this signaling mechanism provide a blueprint for chemical sensing in small compartments, such as olfactory cilia, insect antennae, or even synaptic boutons. PMID:25135936

Self-Biased 215MHz Magnetoelectric NEMS Resonator for Ultra-Sensitive DC Magnetic Field Detection

NASA Astrophysics Data System (ADS)

Nan, Tianxiang; Hui, Yu; Rinaldi, Matteo; Sun, Nian X.

2013-06-01

High sensitivity magnetoelectric sensors with their electromechanical resonance frequencies < 200 kHz have been recently demonstrated using magnetostrictive/piezoelectric magnetoelectric heterostructures. In this work, we demonstrate a novel magnetoelectric nano-electromechanical systems (NEMS) resonator with an electromechanical resonance frequency of 215 MHz based on an AlN/(FeGaB/Al2O3) × 10 magnetoelectric heterostructure for detecting DC magnetic fields. This magnetoelectric NEMS resonator showed a high quality factor of 735, and strong magnetoelectric coupling with a large voltage tunable sensitivity. The admittance of the magnetoelectric NEMS resonator was very sensitive to DC magnetic fields at its electromechanical resonance, which led to a new detection mechanism for ultra-sensitive self-biased RF NEMS magnetoelectric sensor with a low limit of detection of DC magnetic fields of ~300 picoTelsa. The magnetic/piezoelectric heterostructure based RF NEMS magnetoelectric sensor is compact, power efficient and readily integrated with CMOS technology, which represents a new class of ultra-sensitive magnetometers for DC and low frequency AC magnetic fields.

Flexible suspended gate organic thin-film transistors for ultra-sensitive pressure detection

NASA Astrophysics Data System (ADS)

Zang, Yaping; Zhang, Fengjiao; Huang, Dazhen; Gao, Xike; di, Chong-An; Zhu, Daoben

2015-03-01

The utilization of organic devices as pressure-sensing elements in artificial intelligence and healthcare applications represents a fascinating opportunity for the next-generation electronic products. To satisfy the critical requirements of these promising applications, the low-cost construction of large-area ultra-sensitive organic pressure devices with outstanding flexibility is highly desired. Here we present flexible suspended gate organic thin-film transistors (SGOTFTs) as a model platform that enables ultra-sensitive pressure detection. More importantly, the unique device geometry of SGOTFTs allows the fine-tuning of their sensitivity by the suspended gate. An unprecedented sensitivity of 192 kPa-1, a low limit-of-detection pressure of <0.5 Pa and a short response time of 10 ms were successfully realized, allowing the real-time detection of acoustic waves. These excellent sensing properties of SGOTFTs, together with their advantages of facile large-area fabrication and versatility in detecting various pressure signals, make SGOTFTs a powerful strategy for spatial pressure mapping in practical applications.

A novel electrochemical biosensor for ultrasensitive and specific detection of DNA based on molecular beacon mediated circular strand displacement and rolling circle amplification.

PubMed

Cheng, Wei; Zhang, Wei; Yan, Yurong; Shen, Bo; Zhu, Dan; Lei, Pinhua; Ding, Shijia

2014-12-15

A novel electrochemical biosensing strategy was developed for ultrasensitive and specific detection of target DNA using a cascade signal amplification based on molecular beacon (MB) mediated circular strand displacement (CSD), rolling circle amplification (RCA), biotin-strepavidin system, and enzymatic amplification. The target DNA hybridized with the loop portion of MB probe immobilized on the gold electrode and triggered the CSD, leading to multiple biotin-tagged DNA duplex. Furthermore, via biotin-streptavidin interaction, the RCA was implemented, producing long massive tandem-repeat DNA sequences for binding numerous biotinylated detection probes. This enabled an ultrasensitive electrochemical readout by further employing the streptavidin-alkaline phosphatase. The proposed biosensor showed very high sensitivity and selectivity with a dynamic response range from 1 fM to 100 pM. The proposed strategy could have the potential for applying in clinical molecular diagnostics and environmental monitoring. Copyright © 2014 Elsevier B.V. All rights reserved.

Ultrasensitive Detection of Shigella Species in Blood and Stool.

PubMed

Luo, Jieling; Wang, Jiapeng; Mathew, Anup S; Yau, Siu-Tung

2016-02-16

A modified immunosensing system with voltage-controlled signal amplification was used to detect Shigella in stool and blood matrixes at the single-digit CFU level. Inactivated Shigella was spiked in these matrixes and detected directly. The detection was completed in 78 min. Detection limits of 21 CFU/mL and 18 CFU/mL were achieved in stool and blood, respectively, corresponding to 2-7 CFUs immobilized on the detecting electrode. The outcome of the detection of extremely low bacterium concentration, i.e., below 100 CFU/mL, blood samples show a random nature. An analysis of the detection probabilities indicates the correlation between the sample volume and the success of detection and suggests that sample volume is critical for ultrasensitive detection of bacteria. The calculated detection limit is qualitatively in agreement with the empirically determined detection limit. The demonstrated ultrasensitive detection of Shigella on the single-digit CFU level suggests the feasibility of the direct detection of the bacterium in the samples without performing a culture.

Advances in ultrasensitive mass spectrometry of organic molecules.

PubMed

Kandiah, Mathivathani; Urban, Pawel L

2013-06-21

Ultrasensitive mass spectrometric analysis of organic molecules is important for various branches of chemistry, and other fields including physics, earth and environmental sciences, archaeology, biomedicine, and materials science. It finds applications--as an enabling tool--in systems biology, biological imaging, clinical analysis, and forensics. Although there are a number of technical obstacles associated with the analysis of samples by mass spectrometry at ultratrace level (for example analyte losses during sample preparation, insufficient sensitivity, ion suppression), several noteworthy developments have been made over the years. They include: sensitive ion sources, loss-free interfaces, ion optics components, efficient mass analyzers and detectors, as well as "smart" sample preparation strategies. Some of the mass spectrometric methods published to date can achieve sensitivity which is by several orders of magnitude higher than that of alternative approaches. Femto- and attomole level limits of detection are nowadays common, while zepto- and yoctomole level limits of detection have also been reported. We envision that the ultrasensitive mass spectrometric assays will soon contribute to new discoveries in bioscience and other areas.

Luminescent Quantum Dots as Ultrasensitive Biological Labels

NASA Astrophysics Data System (ADS)

Nie, Shuming

2000-03-01

Highly luminescent semiconductor quantum dots have been covalently coupled to biological molecules for use in ultrasensitive biological detection. This new class of luminescent labels is considerably brighter and more resistant againt photobleaching in comparison with organic dyes. Quantum dots labeled with the protein transferrin undergo receptor-mediated endocytosis (RME) in cultured HeLa cells, and those dots that were conjugated to immunomolecules recognize specific antibodies or antigens. In addition, we show that DNA functionalized quantum dots can be used to target specific genes by hybridization. We expect that quantum dot bioconjugates will have a broad range of biological applications, such as ligand-receptor interactions, real-time monitoring of molecular trafficking inside living cells, multicolor fluorescence in-situ hybridization (FISH), high-sensitivity detection in miniaturized devices (e.g., DNA chips), and fluorescent tagging of combinatorial chemical libraries. A potential clinical application is the use of quantum dots for ultrasensitive viral RNA detection, in which as low as 100 copies of hepatitis C and HIV viruses per ml blood should be detected.

Tunable signal processing in synthetic MAP kinase cascades.

PubMed

O'Shaughnessy, Ellen C; Palani, Santhosh; Collins, James J; Sarkar, Casim A

2011-01-07

The flexibility of MAPK cascade responses enables regulation of a vast array of cell fate decisions, but elucidating the mechanisms underlying this plasticity is difficult in endogenous signaling networks. We constructed insulated mammalian MAPK cascades in yeast to explore how intrinsic and extrinsic perturbations affect the flexibility of these synthetic signaling modules. Contrary to biphasic dependence on scaffold concentration, we observe monotonic decreases in signal strength as scaffold concentration increases. We find that augmenting the concentration of sequential kinases can enhance ultrasensitivity and lower the activation threshold. Further, integrating negative regulation and concentration variation can decouple ultrasensitivity and threshold from the strength of the response. Computational analyses show that cascading can generate ultrasensitivity and that natural cascades with different kinase concentrations are innately biased toward their distinct activation profiles. This work demonstrates that tunable signal processing is inherent to minimal MAPK modules and elucidates principles for rational design of synthetic signaling systems. Copyright © 2011 Elsevier Inc. All rights reserved.

Optical fiber LPG biosensor integrated microfluidic chip for ultrasensitive glucose detection

PubMed Central

Yin, Ming-jie; Huang, Bobo; Gao, Shaorui; Zhang, A. Ping; Ye, Xuesong

2016-01-01

An optical fiber sensor integrated microfluidic chip is presented for ultrasensitive detection of glucose. A long-period grating (LPG) inscribed in a small-diameter single-mode fiber (SDSMF) is employed as an optical refractive-index (RI) sensor. With the layer-by-layer (LbL) self-assembly technique, poly (ethylenimine) (PEI) and poly (acrylic acid) (PAA) multilayer film is deposited on the SDSMF-LPG sensor for both supporting and signal enhancement, and then a glucose oxidase (GOD) layer is immobilized on the outer layer for glucose sensing. A microfluidic chip for glucose detection is fabricated after embedding the SDSMF-LPG biosensor into the microchannel of the chip. Experimental results reveal that the SDSMF-LPG biosensor based on such a hybrid sensing film can ultrasensitively detect glucose concentration as low as 1 nM. After integration into the microfluidic chip, the detection range of the sensor is extended from 2 µM to 10 µM, and the response time is remarkablely shortened from 6 minutes to 70 seconds. PMID:27231643

Flexible suspended gate organic thin-film transistors for ultra-sensitive pressure detection

PubMed Central

Zang, Yaping; Zhang, Fengjiao; Huang, Dazhen; Gao, Xike; Di, Chong-an; Zhu, Daoben

2015-01-01

The utilization of organic devices as pressure-sensing elements in artificial intelligence and healthcare applications represents a fascinating opportunity for the next-generation electronic products. To satisfy the critical requirements of these promising applications, the low-cost construction of large-area ultra-sensitive organic pressure devices with outstanding flexibility is highly desired. Here we present flexible suspended gate organic thin-film transistors (SGOTFTs) as a model platform that enables ultra-sensitive pressure detection. More importantly, the unique device geometry of SGOTFTs allows the fine-tuning of their sensitivity by the suspended gate. An unprecedented sensitivity of 192 kPa−1, a low limit-of-detection pressure of <0.5 Pa and a short response time of 10 ms were successfully realized, allowing the real-time detection of acoustic waves. These excellent sensing properties of SGOTFTs, together with their advantages of facile large-area fabrication and versatility in detecting various pressure signals, make SGOTFTs a powerful strategy for spatial pressure mapping in practical applications. PMID:25872157

Nucleic acid arrays and methods of synthesis

DOEpatents

Sabanayagam, Chandran R.; Sano, Takeshi; Misasi, John; Hatch, Anson; Cantor, Charles

2001-01-01

The present invention generally relates to high density nucleic acid arrays and methods of synthesizing nucleic acid sequences on a solid surface. Specifically, the present invention contemplates the use of stabilized nucleic acid primer sequences immobilized on solid surfaces, and circular nucleic acid sequence templates combined with the use of isothermal rolling circle amplification to thereby increase nucleic acid sequence concentrations in a sample or on an array of nucleic acid sequences.

Visible-light-driven photoelectrochemical and photocatalytic performances of Cr-doped SrTiO3/TiO2 heterostructured nanotube arrays.

PubMed

Jiao, Zhengbo; Chen, Tao; Xiong, Jinyan; Wang, Teng; Lu, Gongxuan; Ye, Jinhua; Bi, Yingpu

2013-01-01

Well-aligned TiO2 nanotube arrays have become of increasing significance because of their unique highly ordered array structure, high specific surface area, unidirectional charge transfer and transportation features. However, their poor visible light utilization as well as the high recombination rate of photoexcited electron-hole pairs greatly limited their practical applications. Herein, we demonstrate the fabrication of visible-light-responsive heterostructured Cr-doped SrTiO3/TiO2 nanotube arrays by a simple hydrothermal method, which facilitate efficient charge separation and thus improve the photoelectrochemical as well as photocatalytic performances.

Si-H induced synthesis of Si/Cu2O nanowire arrays for photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Zhang, Shaoyang; She, Guangwei; Li, Shengyang; Mu, Lixuan; Shi, Wensheng

2018-01-01

We report a facile and low-cost method to synthesize Si/Cu2O heterojunction nanowire arrays, without SiOx, at the Si/Cu2O interface. The reductive Si-H bonds on the surface of Si nanowires plays a key role in situ by reducing Cu(II) ions to Cu2O nanocubes and avoiding the SiOx interface layer. Different pH values would vary the electrochemical potential of reactions and as a result, different products would be formed. Utilized as a photoanode for water splitting, Si/Cu2O nanowire arrays exhibit good photoelectrochemical performance.

Self bleaching photoelectrochemical-electrochromic device

DOEpatents

Bechinger, Clemens S.; Gregg, Brian A.

2002-04-09

A photoelectrochemical-electrochromic device comprising a first transparent electrode and a second transparent electrode in parallel, spaced relation to each other. The first transparent electrode is electrically connected to the second transparent electrode. An electrochromic material is applied to the first transparent electrode and a nanoporous semiconductor film having a dye adsorbed therein is applied to the second transparent electrode. An electrolyte layer contacts the electrochromic material and the nanoporous semiconductor film. The electrolyte layer has a redox couple whereby upon application of light, the nanoporous semiconductor layer dye absorbs the light and the redox couple oxidizes producing an electric field across the device modulating the effective light transmittance through the device.

Superlattice photoelectrodes for photoelectrochemical cells

DOEpatents

Nozik, Arthur J.

1987-01-01

A superlattice or multiple-quantum-well semiconductor is used as a photoelectrode in a photoelectrochemical process for converting solar energy into useful fuels or chemicals. The quantum minibands of the superlattice or multiple-quantum-well semiconductor effectively capture hot-charge carriers at or near their discrete quantum energies and deliver them to drive a chemical reaction in an electrolyte. The hot-charge carries can be injected into the electrolyte at or near the various discrete multiple energy levels quantum minibands, or they can be equilibrated among themselves to a hot-carrier pool and then injected into the electrolyte at one average energy that is higher than the lowest quantum band gap in the semiconductor.

Photoelectrochemical cell

DOEpatents

Rauh, R. David; Boudreau, Robert A.

1983-06-14

A photoelectrochemical cell comprising a sealed container having a light-transmitting window for admitting light into the container across a light-admitting plane, an electrolyte in the container, a photoelectrode in the container having a light-absorbing surface arranged to receive light from the window and in contact with the electrolyte, the surface having a plurality of spaced portions oblique to the plane, each portion having dimensions at least an order of magnitude larger than the maximum wavelength of incident sunlight, the total surface area of the surface being larger than the area of the plane bounded by the container, and a counter electrode in the container in contact with the electrolyte.

A Hydrogen-Evolving Hybrid-Electrolyte Battery with Electrochemical/Photoelectrochemical Charging from Water Oxidation.

PubMed

Jin, Zhaoyu; Li, Panpan; Xiao, Dan

2017-02-08

Decoupled hydrogen and oxygen production were successfully embedded into an aqueous dual-electrolyte (acid-base) battery for simultaneous energy storage and conversion. A three-electrode configuration was adopted, involving an electrocatalytic hydrogen-evolving electrode as cathode, an alkaline battery-type or capacitor-type anode as shuttle, and a charging-assisting electrode for electro-/photoelectrochemically catalyzing water oxidation. The conceptual battery not only synergistically outputs electricity and chemical fuels with tremendous specific energy and power densities, but also supports various approaches to be charged by pure or solar-assisted electricity. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Investigations on photoelectrochemical performance of boron doped ZnO nanorods synthesized by facile hydrothermal technique

NASA Astrophysics Data System (ADS)

Sharma, Akash; Chakraborty, Mohua; Thangavel, R.

2018-05-01

Undoped and 10% Boron (B)-doped Zinc Oxide nanorods (ZnO NRs) on Tin doped Indium Oxide (ITO) coated glass substrates were synthesized using facile sol-gel, spin coating and hydrothermal method. The impact of adding Boron on the structural, optical properties, surface morphology and photoelectrochemical (PEC) performances of the ZnO NRs have been investigated. The XRD pattern confirmed the formation of pure hexagonal phase with space group P63mc (186). The same can also be clearly observed form the FESEM images. The UV-Vis study shows the narrowing in band gap from 3.22 eV to 3.19 eV with incorporation of Boron in ZnO matrix. The B-doped ZnO NRs sample shows an enhanced photocurrent density of 1.31 mA/cm2 at 0.5 V (vs. Ag/AgCl), which is more than 171% enhancement compared to bare ZnO NRs (0.483 mA/cm2) in 0.1 M Na2SO4 aqueous solution. The results clearly indicates that the boron doped ZnO NRs can be used as an efficient photoelectrode material for photoelectrochemical cell.

Advancing semiconductor-electrocatalyst systems: application of surface transformation films and nanosphere lithography.

PubMed

Brinkert, Katharina; Richter, Matthias H; Akay, Ömer; Giersig, Michael; Fountaine, Katherine T; Lewerenz, Hans-Joachim

2018-05-24

Photoelectrochemical (PEC) cells offer the possibility of carbon-neutral solar fuel production through artificial photosynthesis. The pursued design involves technologically advanced III-V semiconductor absorbers coupled via an interfacial film to an electrocatalyst layer. These systems have been prepared by in situ surface transformations in electrochemical environments. High activity nanostructured electrocatalysts are required for an efficiently operating cell, optimized in their optical and electrical properties. We demonstrate that shadow nanosphere lithography (SNL) is an auspicious tool to systematically create three-dimensional electrocatalyst nanostructures on the semiconductor photoelectrode through controlling their morphology and optical properties. First results are demonstrated by means of the photoelectrochemical production of hydrogen on p-type InP photocathodes where hitherto applied photoelectrodeposition and SNL-deposited Rh electrocatalysts are compared based on their J-V and spectroscopic behavior. We show that smaller polystyrene particle masks achieve higher defect nanostructures of rhodium on the photoelectrode which leads to a higher catalytic activity and larger short circuit currents. Structural analyses including HRSEM and the analysis of the photoelectrode surface composition by using photoelectron spectroscopy support and complement the photoelectrochemical observations. The optical performance is further compared to theoretical models of the nanostructured photoelectrodes on light scattering and propagation.

Electrolyte Concentration Effect of a Photoelectrochemical Cell Consisting of TiO 2 Nanotube Anode

DOE PAGES

Ren, Kai; Gan, Yong X.; Nikolaidis, Efstratios; ...

2013-01-01

The photoelectrochemical responses of a TiO 2 nanotube anode in ethylene glycol (EG), glycerol, ammonia, ethanol, urea, and Na 2 S electrolytes with different concentrations were investigated. The TiO 2 nanotube anode was highly efficient in photoelectrocatalysis in these solutions under UV light illumination. The photocurrent density is obviously affected by the concentration change. Na 2 S generated the highest photocurrent density at 0, 1, and 2 V bias voltages, but its concentration does not significantly affect the photocurrent density. Urea shows high open circuit voltage at proper concentration and low photocurrent at different concentrations. Externally applied bias voltage is alsomore » an important factor that changes the photoelectrochemical reaction process. In view of the open circuit voltage, EG, ammonia, and ethanol fuel cells show the trend that the open circuit voltage (OCV) increases with the increase of the concentration of the solutions. Glycerol has the highest OCV compared with others, and it deceases with the increase in the concentration because of the high viscosity. The OCV of the urea and Na 2 S solutions did not show obvious concentration effect.« less

Annealing effect of fluorine-doped SnO2/WO3 core-shell inverse opal nanoarchitecture for photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Cho, Seo Yoon; Kang, Soon Hyung; Yun, Gun; Balamurugan, Maheswari; Ahn, Kwang-Soon

2017-01-01

Fluorine-doped SnO2 inverse opal (FTO IO) was developed on a polystyrene bead template with a size of 350 nm (± 20 nm) by using the sol-gel-assisted spin-coating method. The resulting FTO IO film exhibited a pore diameter of 270 nm (± 5 nm), and a WO3 layer was electrodeposited with a constant charge of 400 mC/cm2, followed by a high-temperature annealing process (400, 475, and 550 °C) to increase the crystallinity of the IO films. The annealing temperature affected the morphology and the overall resistance of the thin film, thus significantly affecting the photoelectrochemical performance. In particular, the FTO/WO3 IO film annealed at 475 °C exhibited a photocurrent density of 2.9 mA/cm2 at 1.23 V versus normal hydrogen electrode, showing more than a three times higher photocurrent density in comparison with the other samples (550 °C), which is attributed to the large surface area and low resistance for the charge transport. Therefore, the annealing temperature significantly affects the morphological and the photoelectrochemical features of the FTO/WO3 IO films.

In situ synthesis of CdS/CdWO4/WO3 heterojunction films with enhanced photoelectrochemical properties

NASA Astrophysics Data System (ADS)

Zhan, Faqi; Li, Jie; Li, Wenzhang; Yang, Yahui; Liu, Wenhua; Li, Yaomin

2016-09-01

CdS/CdWO4/WO3 heterojunction films on fluorine-doped tin oxide (FTO) substrates are for the first time prepared as an efficient photoanode for photoelectrochemical (PEC) hydrogen generation by an in situ conversion process. The samples are characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), ultraviolet visible spectrometry (UV-vis) and X-ray photoelectron spectroscopy (XPS). The CdS hollow spheres (∼80 nm) sensitized WO3 plate film with a CdWO4 buffer-layer exhibits increased visible light absorption and a significantly improved photoelectrochemical performance. The photocurrent density at 0 V (vs. Ag/AgCl) of the CdS/CdWO4/WO3 anode is ∼3 times higher than that of the CdWO4/WO3 anode, and ∼9 times higher than that of pure WO3 under illumination. The highest incident-photon-to-current-efficiency (IPCE) value increased from 16% to 63% when the ternary heterojunction was formed. This study demonstrates that the synthesis of ternary composite photocatalysts by the in situ conversion process may be a promising approach to achieve high photoelectric conversion efficiency.

CuO-Functionalized Silicon Photoanodes for Photoelectrochemical Water Splitting Devices.

PubMed

Shi, Yuanyuan; Gimbert-Suriñach, Carolina; Han, Tingting; Berardi, Serena; Lanza, Mario; Llobet, Antoni

2016-01-13

One main difficulty for the technological development of photoelectrochemical (PEC) water splitting (WS) devices is the fabrication of active, stable and cost-effective photoelectrodes that ensure high performance. Here, we report the development of a CuO/Silicon based photoanode, which shows an onset potential for the water oxidation of 0.53 V vs SCE at pH 9, that is, an overpotential of 75 mV, and high stability above 10 h. These values account for a photovoltage of 420 mV due to the absorbed photons by silicon, as proven by comparing with analogous CuO/FTO electrodes that are not photoactive. The photoanodes have been fabricated by sputtering a thin film of Cu(0) on commercially available n-type Si wafers, followed by a photoelectrochemical treatment in basic pH conditions. The resulting CuO/Cu layer acts as (1) protective layer to avoid the corrosion of nSi, (2) p-type hole conducting layer for efficient charge separation and transportation, and (3) electrocatalyst to reduce the overpotential of the water oxidation reaction. The low cost, low toxicity, and good performance of CuO-based coatings can be an attractive solution to functionalize unstable materials for solar energy conversion.

Single-Nanoflake Photo-Electrochemistry Reveals Champion and Spectator Flakes in Exfoliated MoSe 2 Films

DOE PAGES

Todt, Michael A.; Isenberg, Allan E.; Nanayakkara, Sanjini U.; ...

2018-03-06

Semiconducting transition-metal dichalcogenide (TMD) nanoflake thin films are promising large-area electrodes for photo-electrochemical solar energy conversion applications. However, their energy conversion efficiencies are typically much lower than those of bulk electrodes. It is unclear to what extent this efficiency gap stems from differences among nanoflakes (e.g., area, thickness, and surface structural features). It is also unclear whether individual exfoliated nanoflakes can achieve energy conversion efficiencies similar to those of bulk crystals. Here, we use a single-nanoflake photo-electrochemical approach to show that there are both highly active and completely inactive nanoflakes within a film. For the exfoliated MoSe 2 samples studiedmore » herein, 7% of nanoflakes are highly active champions, whose photocurrent efficiency exceeds that of the bulk crystal. However, 66% of nanoflakes are inactive spectators, which are mostly responsible for the overall lower photocurrent efficiency compared to the bulk crystal. The photocurrent collection efficiency increases with nanoflake area and decreases more at perimeter edges than at interior step edges. These observations, which are hidden in ensemble-level measurements, reveal the underlying performance issues of exfoliated TMD electrodes for photo-electrochemical energy conversion applications.« less

Automated electrochemical synthesis and photoelectrochemical characterization of Zn1-xCo(x)O thin films for solar hydrogen production.

PubMed

Jaramillo, Thomas F; Baeck, Sung-Hyeon; Kleiman-Shwarsctein, Alan; Choi, Kyoung-Shin; Stucky, Galen D; McFarland, Eric W

2005-01-01

High-throughput electrochemical methods have been developed for the investigation of Zn1-xCo(x)O films for photoelectrochemical hydrogen production from water. A library of 120 samples containing 27 different compositions (0

Photoelectrochemical Water Splitting Properties of Ti-Ni-Si-O Nanostructures on Ti-Ni-Si Alloy

PubMed Central

Dong, Zhenbiao; Ning, Congqin

2017-01-01

Ti-Ni-Si-O nanostructures were successfully prepared on Ti-1Ni-5Si alloy foils via electrochemical anodization in ethylene glycol/glycerol solutions containing a small amount of water. The Ti-Ni-Si-O nanostructures were characterized by field-emission scanning electron microscopy (FE-SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), and diffuse reflectance absorption spectra. Furthermore, the photoelectrochemical water splitting properties of the Ti-Ni-Si-O nanostructure films were investigated. It was found that, after anodization, three different kinds of Ti-Ni-Si-O nanostructures formed in the α-Ti phase region, Ti2Ni phase region, and Ti5Si3 phase region of the alloy surface. Both the anatase and rutile phases of Ti-Ni-Si-O oxide appeared after annealing at 500 °C for 2 h. The photocurrent density obtained from the Ti-Ni-Si-O nanostructure photoanodes was 0.45 mA/cm2 at 0 V (vs. Ag/AgCl) in 1 M KOH solution. The above findings make it feasible to further explore excellent photoelectrochemical properties of the nanostructure-modified surface of Ti-Ni-Si ternary alloys. PMID:29088083

Photoelectrochemical Water Splitting Properties of Ti-Ni-Si-O Nanostructures on Ti-Ni-Si Alloy.

PubMed

Li, Ting; Ding, Dongyan; Dong, Zhenbiao; Ning, Congqin

2017-10-31

Ti-Ni-Si-O nanostructures were successfully prepared on Ti-1Ni-5Si alloy foils via electrochemical anodization in ethylene glycol/glycerol solutions containing a small amount of water. The Ti-Ni-Si-O nanostructures were characterized by field-emission scanning electron microscopy (FE-SEM), energy dispersive spectroscopy (EDS), X-ray diffraction (XRD), and diffuse reflectance absorption spectra. Furthermore, the photoelectrochemical water splitting properties of the Ti-Ni-Si-O nanostructure films were investigated. It was found that, after anodization, three different kinds of Ti-Ni-Si-O nanostructures formed in the α-Ti phase region, Ti₂Ni phase region, and Ti₅Si₃ phase region of the alloy surface. Both the anatase and rutile phases of Ti-Ni-Si-O oxide appeared after annealing at 500 °C for 2 h. The photocurrent density obtained from the Ti-Ni-Si-O nanostructure photoanodes was 0.45 mA/cm² at 0 V (vs. Ag/AgCl) in 1 M KOH solution. The above findings make it feasible to further explore excellent photoelectrochemical properties of the nanostructure-modified surface of Ti-Ni-Si ternary alloys.

Magnetic Field Effects on Photoelectrochemical Reactions of Porphyrin-Viologen Linked Compounds in an Ionic Liquid

NASA Astrophysics Data System (ADS)

Tahara, Hironobu; Yonemura, Hiroaki; Harada, Satoko; Yamada, Sunao

2011-08-01

Magnetic field effects (MFEs) on photoelectrochemical reactions of three porphyrin-viologen linked compounds with various methylene groups [ZnP(n)V (n=4,6,8)] were examined in 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM][BF4]) as an ionic liquid using a two-electrode cell. Stable anodic photocurrents are produced by irradiating ZnP(n)V (n=4,6,8) in [BMIM][BF4] with visible light, and the MFEs on photocurrents were clearly observed in ZnP(n)V (n=4,6,8). The MFEs on photocurrents increase with magnetic field for lower magnetic fields (B ≤200 mT) and are constant for higher magnetic fields (B > 200 mT). The magnitude of the MFEs in ZnP(n)V (n=6,8) are larger than that in ZnP(4)V. The MFEs can be explained by radical pair mechanism. The magnitude of the MFEs is larger than those in electrodes modified with ZnP(n)V (n=4,6,8) as Langmuir-Blodgett films. The results are most likely attributable to the properties of [BMIM][BF4] and the mechanism of photoelectrochemical reaction.

Electrochemical and photoelectrochemical nano-immunesensing using origami paper based method.

PubMed

Hasanzadeh, Mohammad; Shadjou, Nasrin

2016-04-01

Patterned paper has characteristics that lead to miniaturized assays that run by capillary action with small volumes of fluids. These methods suggest a path for the development of simple, inexpensive, and portable diagnostic assays that can be useful in remote settings, where simple immunoassays are becoming increasingly important for detecting disease and monitoring health. Incorporation of nanomaterials plays a major role in sensing probe immobilization and detection sensitivity of paper-based devices. Nanomaterial properties, such as increased surface area, have aided with signal amplification and lower detection limits. This review focuses on application of nanomaterials as signal amplification elements on origami paper-based electro-analytical devices for immune biomarkers detection with a brief introduction about various fabrication techniques and designs, biological and detection methods. In this review, we comprehensively summarize the selected latest research articles from 2013 to May 2015 on application of nanomaterials in various types of origami paper based electrochemical and photoelectrochemical immunosensors. The review breaks into two parts. The first part devotes to the development and applications of nanomaterials in electrochemical immunesensing. The second part provides an overview of recent origami paper based photoelectrochemical immunosensors. Copyright © 2015 Elsevier B.V. All rights reserved.

Comparability of antimüllerian hormone levels among commercially available immunoassays.

PubMed

Su, H Irene; Sammel, Mary D; Homer, Michael V; Bui, Kim; Haunschild, Carolyn; Stanczyk, Frank Z

2014-06-01

To compare antimüllerian hormone (AMH) levels among three commercially available AMH immunoassays: AMH Gen II (Beckman Coulter), Ultrasensitive AMH (Ansh Labs), and picoAMH (Ansh Labs). Cross-sectional. Academic reproductive endocrinology program. 90 newly diagnosed breast cancer patients before cancer treatment. None. Proportion of detectable AMH levels by immunoassay, and comparability among assays. At a mean age of 38.1 years, the median (interquartile range) AMH level for the cohort was 0.92 [1.35] ng/mL for the Gen II assay, 1.68 [2.30] ng/mL for the Ultrasensitive assay, and 1.52 [2.41] ng/mL for the picoAMH assay. Significantly higher proportions of detectable AMH levels were observed with the picoAMH kit (97%) compared with both the Gen II (84%) and Ultrasensitive (92%) assays. Although the AMH results were highly correlated among the assays (r = 0.92-0.99), the Gen II AMH levels were consistently lower than both Ultrasensitive and picoAMH levels. Moreover, as AMH levels increased, the magnitude of difference grew larger between Gen II and each of the other two assays. Measurement of AMH levels with the picoAMH kit maximized detection at very low levels, particularly in contrast with the Gen II kit. Conversion of AMH levels from different immunoassays using regression equations is potentially highly inaccurate. Copyright © 2014 American Society for Reproductive Medicine. Published by Elsevier Inc. All rights reserved.

Method for isolating nucleic acids

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

Hurt, Jr., Richard Ashley; Elias, Dwayne A.

The current disclosure provides methods and kits for isolating nucleic acid from an environmental sample. The current methods and compositions further provide methods for isolating nucleic acids by reducing adsorption of nucleic acids by charged ions and particles within an environmental sample. The methods of the current disclosure provide methods for isolating nucleic acids by releasing adsorbed nucleic acids from charged particles during the nucleic acid isolation process. The current disclosure facilitates the isolation of nucleic acids of sufficient quality and quantity to enable one of ordinary skill in the art to utilize or analyze the isolated nucleic acids formore » a wide variety of applications including, sequencing or species population analysis.« less

Composition for nucleic acid sequencing

DOEpatents

Korlach, Jonas [Ithaca, NY; Webb, Watt W [Ithaca, NY; Levene, Michael [Ithaca, NY; Turner, Stephen [Ithaca, NY; Craighead, Harold G [Ithaca, NY; Foquet, Mathieu [Ithaca, NY

2008-08-26

The present invention is directed to a method of sequencing a target nucleic acid molecule having a plurality of bases. In its principle, the temporal order of base additions during the polymerization reaction is measured on a molecule of nucleic acid, i.e. the activity of a nucleic acid polymerizing enzyme on the template nucleic acid molecule to be sequenced is followed in real time. The sequence is deduced by identifying which base is being incorporated into the growing complementary strand of the target nucleic acid by the catalytic activity of the nucleic acid polymerizing enzyme at each step in the sequence of base additions. A polymerase on the target nucleic acid molecule complex is provided in a position suitable to move along the target nucleic acid molecule and extend the oligonucleotide primer at an active site. A plurality of labelled types of nucleotide analogs are provided proximate to the active site, with each distinguishable type of nucleotide analog being complementary to a different nucleotide in the target nucleic acid sequence. The growing nucleic acid strand is extended by using the polymerase to add a nucleotide analog to the nucleic acid strand at the active site, where the nucleotide analog being added is complementary to the nucleotide of the target nucleic acid at the active site. The nucleotide analog added to the oligonucleotide primer as a result of the polymerizing step is identified. The steps of providing labelled nucleotide analogs, polymerizing the growing nucleic acid strand, and identifying the added nucleotide analog are repeated so that the nucleic acid strand is further extended and the sequence of the target nucleic acid is determined.

Method for sequencing nucleic acid molecules

DOEpatents

Korlach, Jonas; Webb, Watt W.; Levene, Michael; Turner, Stephen; Craighead, Harold G.; Foquet, Mathieu

2006-06-06

The present invention is directed to a method of sequencing a target nucleic acid molecule having a plurality of bases. In its principle, the temporal order of base additions during the polymerization reaction is measured on a molecule of nucleic acid, i.e. the activity of a nucleic acid polymerizing enzyme on the template nucleic acid molecule to be sequenced is followed in real time. The sequence is deduced by identifying which base is being incorporated into the growing complementary strand of the target nucleic acid by the catalytic activity of the nucleic acid polymerizing enzyme at each step in the sequence of base additions. A polymerase on the target nucleic acid molecule complex is provided in a position suitable to move along the target nucleic acid molecule and extend the oligonucleotide primer at an active site. A plurality of labelled types of nucleotide analogs are provided proximate to the active site, with each distinguishable type of nucleotide analog being complementary to a different nucleotide in the target nucleic acid sequence. The growing nucleic acid strand is extended by using the polymerase to add a nucleotide analog to the nucleic acid strand at the active site, where the nucleotide analog being added is complementary to the nucleotide of the target nucleic acid at the active site. The nucleotide analog added to the oligonucleotide primer as a result of the polymerizing step is identified. The steps of providing labelled nucleotide analogs, polymerizing the growing nucleic acid strand, and identifying the added nucleotide analog are repeated so that the nucleic acid strand is further extended and the sequence of the target nucleic acid is determined.

Method for sequencing nucleic acid molecules

DOEpatents

Korlach, Jonas; Webb, Watt W.; Levene, Michael; Turner, Stephen; Craighead, Harold G.; Foquet, Mathieu

2006-05-30

The present invention is directed to a method of sequencing a target nucleic acid molecule having a plurality of bases. In its principle, the temporal order of base additions during the polymerization reaction is measured on a molecule of nucleic acid, i.e. the activity of a nucleic acid polymerizing enzyme on the template nucleic acid molecule to be sequenced is followed in real time. The sequence is deduced by identifying which base is being incorporated into the growing complementary strand of the target nucleic acid by the catalytic activity of the nucleic acid polymerizing enzyme at each step in the sequence of base additions. A polymerase on the target nucleic acid molecule complex is provided in a position suitable to move along the target nucleic acid molecule and extend the oligonucleotide primer at an active site. A plurality of labelled types of nucleotide analogs are provided proximate to the active site, with each distinguishable type of nucleotide analog being complementary to a different nucleotide in the target nucleic acid sequence. The growing nucleic acid strand is extended by using the polymerase to add a nucleotide analog to the nucleic acid strand at the active site, where the nucleotide analog being added is complementary to the nucleotide of the target nucleic acid at the active site. The nucleotide analog added to the oligonucleotide primer as a result of the polymerizing step is identified. The steps of providing labelled nucleotide analogs, polymerizing the growing nucleic acid strand, and identifying the added nucleotide analog are repeated so that the nucleic acid strand is further extended and the sequence of the target nucleic acid is determined.

Use of the MagNA Pure LC Automated Nucleic Acid Extraction System followed by Real-Time Reverse Transcription-PCR for Ultrasensitive Quantitation of Hepatitis C Virus RNA

PubMed Central

Cook, Linda; Ng, Ka-Wing; Bagabag, Arthur; Corey, Lawrence; Jerome, Keith R.

2004-01-01

Hepatitis C virus (HCV) infection is an increasing health problem worldwide. Quantitative assays for HCV viral load are valuable in predicting response to therapy and for following treatment efficacy. Unfortunately, most quantitative tests for HCV RNA are limited by poor sensitivity. We have developed a convenient, highly sensitive real-time reverse transcription-PCR assay for HCV RNA. The assay amplifies a portion of the 5′ untranslated region of HCV, which is then quantitated using the TaqMan 7700 detection system. Extraction of viral RNA for our assay is fully automated with the MagNA Pure LC extraction system (Roche). Our assay has a 100% detection rate for samples containing 50 IU of HCV RNA/ml and is linear up to viral loads of at least 109 IU/ml. The assay detects genotypes 1a, 2a, and 3a with equal efficiency. Quantitative results by our assay correlate well with HCV viral load as determined by the Bayer VERSANT HCV RNA 3.0 bDNA assay. In clinical use, our assay is highly reproducible, with high and low control specimens showing a coefficient of variation for the logarithmic result of 2.8 and 7.0%, respectively. The combination of reproducibility, extreme sensitivity, and ease of performance makes this assay an attractive option for routine HCV viral load testing. PMID:15365000

A label-free colorimetric isothermal cascade amplification for the detection of disease-related nucleic acids based on double-hairpin molecular beacon.

PubMed

Wu, Dong; Xu, Huo; Shi, Haimei; Li, Weihong; Sun, Mengze; Wu, Zai-Sheng

2017-03-08

K-Ras mutations at codon 12 play an important role in an early step of carcinogenesis. Here, a label-free colorimetric isothermal cascade amplification for ultrasensitive and specific detection of K-Ras point mutation is developed based on a double-hairpin molecular beacon (DHMB). The biosensor consists of DHMB probe and a primer-incorporated polymerization template (PPT) designed partly complementary to DHMB. In the presence of polymerase, target DNA is designed to trigger strand displacement amplification (SDA) via promote the hybridization of PPT with DHMB and subsequently initiates cascade amplification process with the help of the nicking endonuclease. During the hybridization and enzymatic reaction, G-quadruplex/hemin DNAzymes are generated, catalyzing the oxidation of ABTS 2- by H 2 O 2 in the presence of hemin. Utilizing the proposed facile colorimetric scheme, the target DNA can be quantified down to 4 pM with the dynamic response range of 5 orders of magnitude, indicating the substantially improved detection capability. Even more strikingly, point mutation in K-ras gene can be readily observed by the naked eye without the need for the labeling or expensive equipment. Given the high-performance for K-Ras analysis, the enhanced signal transduction capability associated with double-hairpin structure of DHMB provides a novel rout to screen biomarkers, and the descripted colorimetric biosensor seems to hold great promise for diagnostic applications of genetic diseases. Copyright © 2016 Elsevier B.V. All rights reserved.

Method for identifying and quantifying nucleic acid sequence aberrations

DOEpatents

Lucas, Joe N.; Straume, Tore; Bogen, Kenneth T.

1998-01-01

A method for detecting nucleic acid sequence aberrations by detecting nucleic acid sequences having both a first and a second nucleic acid sequence type, the presence of the first and second sequence type on the same nucleic acid sequence indicating the presence of a nucleic acid sequence aberration. The method uses a first hybridization probe which includes a nucleic acid sequence that is complementary to a first sequence type and a first complexing agent capable of attaching to a second complexing agent and a second hybridization probe which includes a nucleic acid sequence that selectively hybridizes to the second nucleic acid sequence type over the first sequence type and includes a detectable marker for detecting the second hybridization probe.

Method for identifying and quantifying nucleic acid sequence aberrations

DOEpatents

Lucas, J.N.; Straume, T.; Bogen, K.T.

1998-07-21

A method is disclosed for detecting nucleic acid sequence aberrations by detecting nucleic acid sequences having both a first and a second nucleic acid sequence type, the presence of the first and second sequence type on the same nucleic acid sequence indicating the presence of a nucleic acid sequence aberration. The method uses a first hybridization probe which includes a nucleic acid sequence that is complementary to a first sequence type and a first complexing agent capable of attaching to a second complexing agent and a second hybridization probe which includes a nucleic acid sequence that selectively hybridizes to the second nucleic acid sequence type over the first sequence type and includes a detectable marker for detecting the second hybridization probe. 11 figs.

Replica amplification of nucleic acid arrays

DOEpatents

Church, George M.

2002-01-01

A method of producing a plurality of a nucleic acid array, comprising, in order, the steps of amplifying in situ nucleic acid molecules of a first randomly-patterned, immobilized nucleic acid array comprising a heterogeneous pool of nucleic acid molecules affixed to a support, transferring at least a subset of the nucleic acid molecules produced by such amplifying to a second support, and affixing the subset so transferred to the second support to form a second randomly-patterned, immobilized nucleic acid array, wherein the nucleic acid molecules of the second array occupy positions that correspond to those of the nucleic acid molecules from which they were amplified on the first array, so that the first array serves as a template to produce a plurality, is disclosed.

Nucleic acid analysis using terminal-phosphate-labeled nucleotides

DOEpatents

Korlach, Jonas [Ithaca, NY; Webb, Watt W [Ithaca, NY; Levene, Michael [Ithaca, NY; Turner, Stephen [Ithaca, NY; Craighead, Harold G [Ithaca, NY; Foquet, Mathieu [Ithaca, NY

2008-04-22

The present invention is directed to a method of sequencing a target nucleic acid molecule having a plurality of bases. In its principle, the temporal order of base additions during the polymerization reaction is measured on a molecule of nucleic acid, i.e. the activity of a nucleic acid polymerizing enzyme on the template nucleic acid molecule to be sequenced is followed in real time. The sequence is deduced by identifying which base is being incorporated into the growing complementary strand of the target nucleic acid by the catalytic activity of the nucleic acid polymerizing enzyme at each step in the sequence of base additions. A polymerase on the target nucleic acid molecule complex is provided in a position suitable to move along the target nucleic acid molecule and extend the oligonucleotide primer at an active site. A plurality of labelled types of nucleotide analogs are provided proximate to the active site, with each distinguishable type of nucleotide analog being complementary to a different nucleotide in the target nucleic acid sequence. The growing nucleic acid strand is extended by using the polymerase to add a nucleotide analog to the nucleic acid strand at the active site, where the nucleotide analog being added is complementary to the nucleotide of the target nucleic acid at the active site. The nucleotide analog added to the oligonucleotide primer as a result of the polymerizing step is identified. The steps of providing labelled nucleotide analogs, polymerizing the growing nucleic acid strand, and identifying the added nucleotide analog are repeated so that the nucleic acid strand is further extended and the sequence of the target nucleic acid is determined.

Method for nucleic acid hybridization using single-stranded DNA binding protein

DOEpatents

Tabor, Stanley; Richardson, Charles C.

1996-01-01

Method of nucleic acid hybridization for detecting the presence of a specific nucleic acid sequence in a population of different nucleic acid sequences using a nucleic acid probe. The nucleic acid probe hybridizes with the specific nucleic acid sequence but not with other nucleic acid sequences in the population. The method includes contacting a sample (potentially including the nucleic acid sequence) with the nucleic acid probe under hybridizing conditions in the presence of a single-stranded DNA binding protein provided in an amount which stimulates renaturation of a dilute solution (i.e., one in which the t.sub.1/2 of renaturation is longer than 3 weeks) of single-stranded DNA greater than 500 fold (i.e., to a t.sub.1/2 less than 60 min, preferably less than 5 min, and most preferably about 1 min.) in the absence of nucleotide triphosphates.

Quantum dot bioconjugates for ultrasensitive nonisotopic detection.

PubMed

Chan, W C; Nie, S

1998-09-25

Highly luminescent semiconductor quantum dots (zinc sulfide-capped cadmium selenide) have been covalently coupled to biomolecules for use in ultrasensitive biological detection. In comparison with organic dyes such as rhodamine, this class of luminescent labels is 20 times as bright, 100 times as stable against photobleaching, and one-third as wide in spectral linewidth. These nanometer-sized conjugates are water-soluble and biocompatible. Quantum dots that were labeled with the protein transferrin underwent receptor-mediated endocytosis in cultured HeLa cells, and those dots that were labeled with immunomolecules recognized specific antibodies or antigens.

Labeled nucleotide phosphate (NP) probes

DOEpatents

Korlach, Jonas [Ithaca, NY; Webb, Watt W [Ithaca, NY; Levene, Michael [Ithaca, NY; Turner, Stephen [Ithaca, NY; Craighead, Harold G [Ithaca, NY; Foquet, Mathieu [Ithaca, NY

2009-02-03

The present invention is directed to a method of sequencing a target nucleic acid molecule having a plurality of bases. In its principle, the temporal order of base additions during the polymerization reaction is measured on a molecule of nucleic acid, i.e. the activity of a nucleic acid polymerizing enzyme on the template nucleic acid molecule to be sequenced is followed in real time. The sequence is deduced by identifying which base is being incorporated into the growing complementary strand of the target nucleic acid by the catalytic activity of the nucleic acid polymerizing enzyme at each step in the sequence of base additions. A polymerase on the target nucleic acid molecule complex is provided in a position suitable to move along the target nucleic acid molecule and extend the oligonucleotide primer at an active site. A plurality of labelled types of nucleotide analogs are provided proximate to the active site, with each distinguishable type of nucleotide analog being complementary to a different nucleotide in the target nucleic acid sequence. The growing nucleic acid strand is extended by using the polymerase to add a nucleotide analog to the nucleic acid strand at the active site, where the nucleotide analog being added is complementary to the nucleotide of the target nucleic acid at the active site. The nucleotide analog added to the oligonucleotide primer as a result of the polymerizing step is identified. The steps of providing labelled nucleotide analogs, polymerizing the growing nucleic acid strand, and identifying the added nucleotide analog are repeated so that the nucleic acid strand is further extended and the sequence of the target nucleic acid is determined.

Nucleic acid tool enzymes-aided signal amplification strategy for biochemical analysis: status and challenges.

PubMed

Qing, Taiping; He, Dinggeng; He, Xiaoxiao; Wang, Kemin; Xu, Fengzhou; Wen, Li; Shangguan, Jingfang; Mao, Zhengui; Lei, Yanli

2016-04-01

Owing to their highly efficient catalytic effects and substrate specificity, the nucleic acid tool enzymes are applied as 'nano-tools' for manipulating different nucleic acid substrates both in the test-tube and in living organisms. In addition to the function as molecular scissors and molecular glue in genetic engineering, the application of nucleic acid tool enzymes in biochemical analysis has also been extensively developed in the past few decades. Used as amplifying labels for biorecognition events, the nucleic acid tool enzymes are mainly applied in nucleic acids amplification sensing, as well as the amplification sensing of biorelated variations of nucleic acids. With the introduction of aptamers, which can bind different target molecules, the nucleic acid tool enzymes-aided signal amplification strategies can also be used to sense non-nucleic targets (e.g., ions, small molecules, proteins, and cells). This review describes and discusses the amplification strategies of nucleic acid tool enzymes-aided biosensors for biochemical analysis applications. Various analytes, including nucleic acids, ions, small molecules, proteins, and cells, are reviewed briefly. This work also addresses the future trends and outlooks for signal amplification in nucleic acid tool enzymes-aided biosensors.

Formation mechanism of TiO2 nanotubes and their applications in photoelectrochemical water splitting and supercapacitors.

PubMed

Chen, Bo; Hou, Junbo; Lu, Kathy

2013-05-14

Structural observations of the transition of TiO2 nanopores into nanotubes by increasing the OH(-) concentration in the electrolyte challenge the validity of existing formation mechanisms of anodic TiO2 nanotubes. In this study, dehydration of titanium hydroxide in the cell wall is proposed as the mechanism that leads to the separation of neighboring nanotubes. Based on this understanding, bamboo-type TiO2 nanotubes with large surface area and excellent interconnectivity are achieved by cycling high and low applied potentials. After thermal treatment in a H2 atmosphere, the bamboo-type TiO2 nanotubes show large photoelectrochemical water splitting efficiency and supercapacitors performace.

Modelling heterogeneous interfaces for solar water splitting

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

Pham, Tuan Anh; Ping, Yuan; Galli, Giulia

2017-01-09

The generation of hydrogen from water and sunlight others a promising approach for producing scalable and sustainable carbon-free energy. The key of a successful solar-to-fuel technology is the design of efficient, long-lasting and low-cost photoelectrochemical cells, which are responsible for absorbing sunlight and driving water splitting reactions. To this end, a detailed understanding and control of heterogeneous interfaces between photoabsorbers, electrolytes and catalysts present in photoelectrochemical cells is essential. Here we review recent progress and open challenges in predicting physicochemical properties of heterogeneous interfaces for solar water splitting applications using first-principles-based approaches, and highlights the key role of these calculationsmore » in interpreting increasingly complex experiments.« less

100-Fold Enhancement of Charge Transport in Uniaxially Oriented Mesoporous Anatase TiO 2 Films

DOE PAGES

Li, Ke; Liu, Jie; Sheng, Xia; ...

2017-12-04

Mesoporous semiconductor films are of considerable interest for applications in photoelectrochemical devices, however, despite intensive research till now, their charge transport properties remain significantly lower than their single-crystal counterparts. Herein, we report a novel low-temperature template-free technique for growing high surface area mesoporous anatase TiO2 films with a preferred [001] crystalline-orientation on FTO-coated glass substrate. Compared to mesoporous films that comprised of randomly oriented crystallites, the uniaxial orientation enables a 100-fold increase in the rate of electron transport. The uniaxially oriented mesoporous anatase TiO2 films exhibit should greatly facilitate the development and application of photoelectrochemical and electrochemical devices.

Reactor process using metal oxide ceramic membranes

DOEpatents

Anderson, Marc A.

1994-01-01

A reaction vessel for use in photoelectrochemical reactions includes as its reactive surface a metal oxide porous ceramic membrane of a catalytic metal such as titanium. The reaction vessel includes a light source and a counter electrode. A provision for applying an electrical bias between the membrane and the counter electrode permits the Fermi levels of potential reaction to be favored so that certain reactions may be favored in the vessel. The electrical biasing is also useful for the cleaning of the catalytic membrane. Also disclosed is a method regenerating a porous metal oxide ceramic membrane used in a photoelectrochemical catalytic process by periodically removing the reactants and regenerating the membrane using a variety of chemical, thermal, and electrical techniques.

Influence of pH on the quantum-size-controlled photoelectrochemical etching of epitaxial InGaN quantum dots

DOE PAGES

Xiao, Xiaoyin; Lu, Ping; Fischer, Arthur J.; ...

2015-11-18

Illumination by a narrow-band laser has been shown to enable photoelectrochemical (PEC) etching of InGaN thin films into quantum dots with sizes controlled by the laser wavelength. Here, we investigate and elucidate the influence of solution pH on such quantum-size-controlled PEC etch process. We find that although a pH above 5 is often used for PEC etching of GaN-based materials, oxides (In 2O 3 and/or Ga 2O 3) form which interfere with quantum dot formation. Furthermore, at pH below 3, however, oxide-free QDs with self-terminated sizes can be successfully realized.

Ultrathin planar hematite film for solar photoelectrochemical water splitting

DOE PAGES

Liu, Dong; Bierman, David M.; Lenert, Andrej; ...

2015-10-08

Hematite holds promise for photoelectrochemical (PEC) water splitting due to its stability, low-cost, abundance and appropriate bandgap. However, it suffers from a mismatch between the hole diffusion length and light penetration length. We have theoretically designed and characterized an ultrathin planar hematite/silver nanohole array/silver substrate photoanode. Due to the supported destructive interference and surface plasmon resonance, photons are efficiently absorbed in an ultrathin hematite film. In conclusion, compared with ultrathin hematite photoanodes with nanophotonic structures, this photoanode has comparable photon absorption but with intrinsically lower recombination losses due to its planar structure and promises to exceed the state-of-the-art photocurrent ofmore » hematite photoanodes.« less

Synthesis and photoelectrochemical properties of a novel CuO/ZnO nanorod photocathode for solar hydrogen generation

NASA Astrophysics Data System (ADS)

Shaislamov, Ulugbek; Lee, Heon-Ju

2016-10-01

Here, we present a facile synthesis method and photoelectrochemical characterizations of a p-type CuO-nanorod array photoelectrode with ZnO nanorod branches. Vertically-aligned CuO nanorods were synthesized by using direct oxidation of metallic Cu nanorods grown on a Cu substrate by using a facile template-assisted electrodeposition method. The formed CuONR/ZnONB hierarchically-structured photoelectrode exhibited remarkable photoelectrodechemical performance and outstanding stability compared to the CuO NR photoelectrode without ZnO NR branches. Morphological, optical and electrochemical characterizations were carried out in order to examine the effects of ZnO nanorod branches on the stability and the overall electrochemical performance of the electrode.

Method of Identifying a Base in a Nucleic Acid

DOEpatents

Fodor, Stephen P. A.; Lipshutz, Robert J.; Huang, Xiaohua

1999-01-01

Devices and techniques for hybridization of nucleic acids and for determining the sequence of nucleic acids. Arrays of nucleic acids are formed by techniques, preferably high resolution, light-directed techniques. Positions of hybridization of a target nucleic acid are determined by, e.g., epifluorescence microscopy. Devices and techniques are proposed to determine the sequence of a target nucleic acid more efficiently and more quickly through such synthesis and detection techniques.

Identifying a base in a nucleic acid

DOEpatents

Fodor, Stephen P. A.; Lipshutz, Robert J.; Huang, Xiaohua

2005-02-08

Devices and techniques for hybridization of nucleic acids and for determining the sequence of nucleic acids. Arrays of nucleic acids are formed by techniques, preferably high resolution, light-directed techniques. Positions of hybridization of a target nucleic acid are determined by, e.g., epifluorescence microscopy. Devices and techniques are proposed to determine the sequence of a target nucleic acid more efficiently and more quickly through such synthesis and detection techniques.

Hybridization and sequencing of nucleic acids using base pair mismatches

DOEpatents

Fodor, Stephen P. A.; Lipshutz, Robert J.; Huang, Xiaohua

2001-01-01

Devices and techniques for hybridization of nucleic acids and for determining the sequence of nucleic acids. Arrays of nucleic acids are formed by techniques, preferably high resolution, light-directed techniques. Positions of hybridization of a target nucleic acid are determined by, e.g., epifluorescence microscopy. Devices and techniques are proposed to determine the sequence of a target nucleic acid more efficiently and more quickly through such synthesis and detection techniques.

Probe kit for identifying a base in a nucleic acid

DOEpatents

Fodor, Stephen P. A.; Lipshutz, Robert J.; Huang, Xiaohua

2001-01-01

Devices and techniques for hybridization of nucleic acids and for determining the sequence of nucleic acids. Arrays of nucleic acids are formed by techniques, preferably high resolution, light-directed techniques. Positions of hybridization of a target nucleic acid are determined by, e.g., epifluorescence microscopy. Devices and techniques are proposed to determine the sequence of a target nucleic acid more efficiently and more quickly through such synthesis and detection techniques.

Methods for Identifying Ligands that Target Nucleic Acid Molecules and Nucleic Acid Structural Motifs

NASA Technical Reports Server (NTRS)

Childs-Disney, Jessica L. (Inventor); Disney, Matthew D. (Inventor)

2017-01-01

Disclosed are methods for identifying a nucleic acid (e.g., RNA, DNA, etc.) motif which interacts with a ligand. The method includes providing a plurality of ligands immobilized on a support, wherein each particular ligand is immobilized at a discrete location on the support; contacting the plurality of immobilized ligands with a nucleic acid motif library under conditions effective for one or more members of the nucleic acid motif library to bind with the immobilized ligands; and identifying members of the nucleic acid motif library that are bound to a particular immobilized ligand. Also disclosed are methods for selecting, from a plurality of candidate ligands, one or more ligands that have increased likelihood of binding to a nucleic acid molecule comprising a particular nucleic acid motif, as well as methods for identifying a nucleic acid which interacts with a ligand.

Step-gate polysilicon nanowires field effect transistor compatible with CMOS technology for label-free DNA biosensor.

PubMed

Wenga, G; Jacques, E; Salaün, A-C; Rogel, R; Pichon, L; Geneste, F

2013-02-15

Currently, detection of DNA hybridization using fluorescence-based detection technique requires expensive optical systems and complex bioinformatics tools. Hence, the development of new low cost devices that enable direct and highly sensitive detection stimulates a lot of research efforts. Particularly, devices based on silicon nanowires are emerging as ultrasensitive electrical sensors for the direct detection of biological species thanks to their high surface to volume ratio. In this study, we propose innovative devices using step-gate polycrystalline silicon nanowire FET (poly-Si NW FETs), achieved with simple and low cost fabrication process, and used as ultrasensitive electronic sensor for DNA hybridization. The poly-SiNWs are synthesized using the sidewall spacer formation technique. The detailed fabrication procedure for a step-gate NWFET sensor is described in this paper. No-complementary and complementary DNA sequences were clearly discriminated and detection limit to 1 fM range is observed. This first result using this nano-device is promising for the development of low cost and ultrasensitive polysilicon nanowires based DNA sensors compatible with the CMOS technology. Copyright © 2012 Elsevier B.V. All rights reserved.

Rapid, On-Site, Ultrasensitive Melamine Quantitation Method for Protein Beverages Using Time-Resolved Fluorescence Detection Paper.

PubMed

Li, Guanghua; Wang, Du; Zhou, Aijun; Sun, Yimin; Zhang, Qi; Poapolathep, Amnart; Zhang, Li; Fan, Zhiyong; Zhang, Zhaowei; Li, Peiwu

2018-06-06

To ensure protein beverage safety and prevent illegal melamine use to artificially increase protein content, a rapid, on-site, ultrasensitive detection method for melamine must be developed because melamine is detrimental to human health. Herein, an ultrasensitive time-resolved fluorescence detection paper (TFDP) was developed to detect melamine in protein beverages within 15 min using a one-step sample preparation. The lower limits of detection were 0.89, 0.94, and 1.05 ng/mL, and the linear ranges were 2.67-150, 2.82-150, and 3.15-150 ng/mL (R 2 > 0.982) for peanut, walnut, and coconut beverages, respectively. The recovery rates were 85.86-110.60% with a coefficient of variation <7.80% in the spiking experiment. A high specificity was observed in the interferent experiment. When detecting real protein beverage samples, the TFDP and ultraperformance liquid chromatography-tandem mass spectrometer (UPLC-MS/MS) results were consistent. This method is a promising alternative for rapid, on-site detection of melamine in beverages.

Ultrasensitive detection and characterization of molecules with infrared plasmonic metamaterials

PubMed Central

Cheng, Fei; Yang, Xiaodong; Gao, Jie

2015-01-01

Infrared vibrational spectroscopy is an effective technique which enables the direct probe of molecular fingerprints, and such detection can be further enhanced by the emerging engineered plasmonic metamaterials. Here we experimentally demonstrate ultrasensitive detection and characterization of polymer molecules based on an asymmetric infrared plasmonic metamaterial, and quantitatively analyze the molecule detection sensitivity and molecule-structure interactions. A sharp, non-radiative Fano resonance supported by the plasmonic metamaterial exhibits strongly enhanced near-field, and the resonance frequency is tailored to match the vibrational fingerprint of the target molecule. By utilizing the near-field nature of the plasmonic excitation, significantly enhanced absorption signal of molecules in the infrared spectroscopy are obtained, enabling ultrasensitive detection of only minute quantities of organic molecules. The enhancement of molecular absorption up to 105 fold is obtained, and sensitive detection of molecules at zeptomole levels (corresponding to a few tens of molecules within a unit cell) is achieved with high signal-to-noise ratio in our experiment. The demonstrated infrared plasmonic metamaterial sensing platform offers great potential for improving the specificity and sensitivity of label-free, biochemical detection. PMID:26388404

Ultrasensitive Inertial and Force Sensors with Diamagnetically Levitated Magnets

NASA Astrophysics Data System (ADS)

Prat-Camps, J.; Teo, C.; Rusconi, C. C.; Wieczorek, W.; Romero-Isart, O.

2017-09-01

We theoretically show that a magnet can be stably levitated on top of a punctured superconductor sheet in the Meissner state without applying any external field. The trapping potential created by such induced-only superconducting currents is characterized for magnetic spheres ranging from tens of nanometers to tens of millimeters. Such a diamagnetically levitated magnet is predicted to be extremely well isolated from the environment. We propose to use it as an ultrasensitive force and inertial sensor. A magnetomechanical readout of its displacement can be performed by using superconducting quantum interference devices. An analysis using current technology shows that force and acceleration sensitivities on the order of 10-23 N /√{Hz } (for a 100-nm magnet) and 10-14 g /√{Hz } (for a 10-mm magnet) might be within reach in a cryogenic environment. Such remarkable sensitivities, both in force and acceleration, can be used for a variety of purposes, from designing ultrasensitive inertial sensors for technological applications (e.g., gravimetry, avionics, and space industry), to scientific investigations on measuring Casimir forces of magnetic origin and gravitational physics.

Nonplasmonic Hot-Electron Photocurrents from Mn-Doped Quantum Dots in Photoelectrochemical Cells.

PubMed

Dong, Yitong; Rossi, Daniel; Parobek, David; Son, Dong Hee

2016-03-03

We report the measurement of the hot-electron current in a photoelectrochemical cell constructed from a glass/ITO/Al2 O3 (ITO=indium tin oxide) electrode coated with Mn-doped quantum dots, where hot electrons with a large excess kinetic energy were produced through upconversion of the excitons into hot electron hole pairs under photoexcitation at 3 eV. In our recent study (J. Am. Chem. Soc. 2015, 137, 5549), we demonstrated the generation of hot electrons in Mn-doped II-VI semiconductor quantum dots and their usefulness in photocatalytic H2 production reaction, taking advantage of the more efficient charge transfer of hot electrons compared with band-edge electrons. Here, we show that hot electrons produced in Mn-doped CdS/ZnS quantum dots possess sufficient kinetic energy to overcome the energy barrier from a 5.4-7.5 nm thick Al2 O3 layer producing a hot-electron current in photoelectrochemical cell. This work demonstrates the possibility of harvesting hot electrons not only at the interface of the doped quantum dot surface, but also far away from it, thus taking advantage of the capability of hot electrons for long-range electron transfer across a thick energy barrier. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Enhanced Photoelectrochemical Performance of Cuprous Oxide/Graphene Nanohybrids

PubMed Central

2017-01-01

Combination of an oxide semiconductor with a highly conductive nanocarbon framework (such as graphene or carbon nanotubes) is an attractive avenue to assemble efficient photoelectrodes for solar fuel generation. To fully exploit the possible synergies of the hybrid formation, however, precise knowledge of these systems is required to allow rational design and morphological engineering. In this paper, we present the controlled electrochemical deposition of nanocrystalline p-Cu2O on the surface of different graphene substrates. The developed synthetic protocol allowed tuning of the morphological features of the hybrids as deduced from electron microscopy. (Photo)electrochemical measurements (including photovoltammetry, electrochemical impedance spectroscopy, photocurrent transient analysis) demonstrated better performance for the 2D graphene containing photoelectrodes, compared to the bare Cu2O films, the enhanced performance being rooted in suppressed charge carrier recombination. To elucidate the precise role of graphene, comparative studies were performed with carbon nanotube (CNT) films and 3D graphene foams. These studies revealed, after allowing for the effect of increased surface area, that the 3D graphene substrate outperformed the other two nanocarbons. Its interconnected structure facilitated effective charge separation and transport, leading to better harvesting of the generated photoelectrons. These hybrid assemblies are shown to be potentially attractive candidates in photoelectrochemical energy conversion schemes, namely CO2 reduction. PMID:28460518

The high surface energy of NiO {110} facets incorporated into TiO2 hollow microspheres by etching Ti plate for enhanced photocatalytic and photoelectrochemical activity

NASA Astrophysics Data System (ADS)

Li, Jian; Cui, Hongzhi; Song, Xiaojie; Wei, Na; Tian, Jian

2017-02-01

We present a rational design for the controllable synthesis of NiO/TiO2 hollow microspheres (NTHMs) with Ti plate via a one-pot template-free synthesis strategy. Specifically, to enhance the formation of hollow microspheres, part of the titanium source is provided by the Ti plate. The hollow spherical NiO/TiO2 particles possess unique microstructural characteristics, namely, a higher specific surface area (∼65.82 m2 g-1), a larger mesoporous structure (∼7.79 nm), and hierarchical nanoarchitectures connected with mesopores within the shell (monodispersed size of ∼1 μm and shell thickness of ∼80 nm). In addition, as a cocatalyst for improved catalytic activity, the incorporated NiO nanoparticles with exposed high surface energy {110} facets displayed an outstanding performance. It has been proven that this facile nanostructure possesses remarkably high photoelectrochemical and photocatalytic activities. The main mechanism for enhancement of photocatalytic activity is attributed to the construction of p-n junctions with an inner electric field between TiO2 and NiO, which can dramatically enhance the separation efficiency of the photogenerated electron-hole pairs. This strategy could be applied to fabricate mixed metal oxide hollow microspheres toward the photoelectrochemical catalysis.

Present status of solid state photoelectrochemical solar cells and dye sensitized solar cells using PEO-based polymer electrolytes

NASA Astrophysics Data System (ADS)

Singh, Pramod Kumar; Nagarale, R. K.; Pandey, S. P.; Rhee, H. W.; Bhattacharya, Bhaskar

2011-06-01

Due to energy crises in the future, much effort is being directed towards alternate sources. Solar energy is accepted as a novel substitute for conventional sources of energy. Out of the long list of various types of solar cells available on the market, solid state photoelectrochemical solar cells (SSPECs) and dye sensitized solar cells (DSSCs) are proposed as an alternative to costly crystalline solar cell. This review provides a common platform for SSPECs and DSSCs using polymer electrolyte, particularly on polyethylene oxide (PEO)-based polymer electrolytes. Due to numerous advantageous properties of PEO, it is frequently used as an electrolyte in both SSPECs as well as DSSCs. In DSSCs, so far high efficiency (more than 11%) has been obtained only by using volatile liquid electrolyte, which suffers many disadvantages, such as corrosion, leakage and evaporation. The PEO-based solid polymer proves its importance and could be used to solve the problems stated above. The recent developments in SSPECs and DSSCs using modified PEO electrolytes by adding nano size inorganic fillers, blending with low molecular weight polymers and ionic liquid (IL) are discussed in detail. The role of ionic liquid in modifying the electrical, structural and photoelectrochemical properties of PEO polymer electrolytes is also described.

Enhanced photoelectrochemical response of plasmonic Au embedded BiVO4/Fe2O3 heterojunction.

PubMed

Verma, Anuradha; Srivastav, Anupam; Khan, Saif A; Rani Satsangi, Vibha; Shrivastav, Rohit; Kumar Avasthi, Devesh; Dass, Sahab

2017-06-14

The effect of embedding Au nanoparticles (NPs) in a BiVO 4 /Fe 2 O 3 heterojunction for photoelectrochemical water splitting is studied here for the first time. The present nanostructured heterojunction offers three major advantages over pristine BiVO 4 and Fe 2 O 3 : (i) the formation of a heterojunction between BiVO 4 and Fe 2 O 3 enhances the charge carrier separation and transfer, (ii) the layer of Fe 2 O 3 provides protection to BiVO 4 from photocorrosion and, (iii) the Au NPs possessing surface plasmon resonance (SPR) enhance the photoelectrochemical response by transferring energy to metal oxides by hot electron transfer (HET) and plasmon resonant energy transfer (PRET). The present study reveals that the heterojunction ITO/BiVO 4 /Fe 2 O 3 (with 32% v/v Au solution in both layers) gives the best performance and mitigates the limitations of both pristine Fe 2 O 3 and BiVO 4 . A thirteen-fold increment in applied bias photon-to-current conversion efficiency (ABPE) was observed at 1.24 V vs. RHE under the condition of 1 Sun illumination. Monochromatic incident photon-to-current conversion efficiency (IPCE) measurements indicated that an Au embedded heterojunction is more effective in harvesting visible light in comparison to a heterojunction without Au NPs.

A photoelectrochemical immunosensor for detection of α-fetoprotein based on Au-ZnO flower-rod heterostructures

NASA Astrophysics Data System (ADS)

Han, Zhizhong; Luo, Min; Chen, Li; Chen, Jinghua; Li, Chunyan

2017-04-01

In this work, a novel label free photoelectrochemical (PEC) immunosensor has been developed for the detection of α-fetoprotein (AFP). The immunosensor was based on Au-ZnO flower-rods (FRs) heterostructure, where Au nanoparticles (NPs) were firstly electrodeposited by cyclic voltammetry methods. Scanning electron microscopy (SEM), X-ray diffraction (XRD), Mott-Schottky plot (MS), UV-vis diffuse reflectance spectrum and fluorescence emission spectrum were used for the characterizations of Au-ZnO FRs. The results demonstrated that Au NPs not only obviously enhanced the visible light absorption of ZnO FRs due to surface plasmon resonance (SPR) but also improved the separation of photo-generated electron-hole pairs. Therefore, the photocurrent of Au-ZnO FRs was increased under simulated sunlight. The photocurrent was reduced after the specific antibody-antigen immune reaction. And the photocurrent decrement was linear with the logarithm of AFP antigen concentration in the range from 0.005 ng mL-1 to 50 ng mL-1 with a low detection limit of 0.56 pg mL-1 (S/N = 3). The PEC immunosensor also exhibited high anti-interference property and acceptable stability. This work would provide a promising photoelectrochemical strategy for the detection of other proteins in clinical diagnosis.

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 Photoelectrochemical Biosensor for Tyrosinase and Thrombin Detection

PubMed Central

Chen, Jiexia; Liu, Yifan; Zhao, Guang-Chao

2016-01-01

A novel photoelectrochemical biosensor for step-by-step assay of tyrosinase and thrombin was fabricated based on the specific interactions between the designed peptide and the target enzymes. A peptide chain with a special sequence which contains a positively charged lysine-labeled terminal, tyrosine at the other end and a cleavage site recognized by thrombin between them was designed. The designed peptide can be fixed on surface of the CdTe quantum dots (QDs)-modified indium-tin oxide (ITO) electrode through electrostatic attraction to construct the photoelectrochemical biosensor. The tyrosinase target can catalyze the oxidization of tyrosine by oxygen into ortho-benzoquinone residues, which results in a decrease in the sensor photocurrent. Subsequently, the cleavage site could be recognized and cut off by another thrombin target, restoring the sensor photocurrent. The decrease or increase of photocurrent in the sensor enables us to assay tyrosinase and thrombin. Thus, the detection of tyrosinase and thrombin can be achieved in the linear range from 2.6 to 32 μg/mL and from 4.5 to 100 μg/mL with detection limits of 1.5 μg/mL and 1.9 μg/mL, respectively. Most importantly, this strategy shall allow us to detect different classes of enzymes simultaneously by designing various enzyme-specific peptide substrates. PMID:26805846

Photoelectrochemical detection of alpha-fetoprotein based on ZnO inverse opals structure electrodes modified by Ag2S nanoparticles

PubMed Central

Jiang, Yandong; Liu, Dali; Yang, Yudan; Xu, Ru; Zhang, Tianxiang; Sheng, Kuang; Song, Hongwei

2016-01-01

In this work, a new photoelectrochemical biosensor based on Ag2S nanoparticles (NPs) modified macroporous ZnO inverse opals structure (IOs) was developed for sensitive and rapid detection of alpha fetal protein (AFP). Small size and uniformly dispersed Ag2S NPs were prepared using the Successive Ionic Layer Adsorption And Reaction (SILAR) method, which were adsorbed on ZnO IOs surface and frame work as matrix for immobilization of AFP. The composite structure of ZnO/Ag2S expanded the scope of light absorption to long wavelength, which can make full use of the light energy. Meanwhile, an effective matching of energy levels between the conduction bands of Ag2S and ZnO are beneficial to the photo-generated electrons transfer. The biosensors based on FTO (fluorine-doped tinoxide) ZnO/Ag2S electrode showed enough sensitivity and a wide linear range from 0.05 ng/mL to 200 ng/mL with a low detection limit of 8 pg/mL for the detection of AFP. It also exhibited high reproducibility, specificity and stability. The proposed method was potentially attractive for achieving excellent photoelectrochemical biosensor for detection of other proteins. PMID:27922086

Unravelling Photocarrier Dynamics beyond the Space Charge Region for Photoelectrochemical Water Splitting

DOE PAGES

Zhang, Wenrui; Yan, Danhua; Appavoo, Kannatassen; ...

2017-04-18

Semiconductor photoelectrodes for photoelectrochemical (PEC) water splitting require efficient carrier generation, separation, and transport at and beyond the space charge region (SCR) formed at the aqueous interface. The trade-off between photon collection and minority carrier delivery governs the photoelectrode design and implies maximum water splitting efficiency at an electrode thickness equivalent to the light absorption depth. Here, using planar ZnO thin films as a model system, we identify the photocarriers beyond the SCR as another significant source to substantially enhance the PEC performance. The high-quality ZnO films synthesized by pulsed laser deposition feature very few deep trap states and supportmore » a long photocarrier lifetime. Combined with photoelectrochemical characterization, ultrafast spectroscopy, and numerical calculations, it is revealed that engineering the exciton concentration gradient by film thickness facilitates the inward diffusion of photocarriers from the neighboring illuminated region to the SCR and, therefore, achieves a record high quantum efficiency over 80% at a thickness far beyond its light absorption depth and the SCR width. Furthermore, these results elucidate the important role of the photocarriers beyond SCR for the PEC process and provide new insight into exploring the full potential for efficient photoelectrode materials with large exciton diffusivity.« less

A novel photoelectrochemical biosensor for protein kinase activity assay based on phosphorylated graphite-like carbon nitride.

PubMed

Li, Xue; Zhou, Yunlei; Xu, Yan; Xu, Huijie; Wang, Minghui; Yin, Huanshun; Ai, Shiyun

2016-08-31

Protein kinases are general and significant regulators in the cell signaling pathway, and it is still greatly desired to achieve simple and quick kinase detection. Herein, we develop a simple and sensitive photoelectrochemical strategy for the detection of protein kinase activity based on the bond between phosphorylated peptide and phosphorylated graphite-like carbon nitride (P-g-C3N4) conjugates triggered by Zr(4+) ion coordination. Under optimal conditions, the increased photocurrent is proportional to the protein kinase A (PKA) concentration ranging from 0.05 to 50 U/mL with a detection limit of 0.077 U/mL. Moreover, this photoelectrochemical assay can be also applied to quantitative analysis of kinase inhibition. The results indicated that the IC50 value (inhibitor concentration producing 50% inhibitor) for ellagic acid was 9.1 μM. Moreover, the developed method is further applied to detect PKA activity in real samples, which contains serum from healthy person and gastric cancer patients and breast tissue from healthy person and breast cancer patients. Therefore, the established protocol provides a new and simple tool for assay of kinase activity and its inhibitors with low cost and high sensitivity. Copyright © 2016 Elsevier B.V. All rights reserved.

Method for analyzing nucleic acids by means of a substrate having a microchannel structure containing immobilized nucleic acid probes

DOEpatents

Ramsey, J. Michael; Foote, Robert S.

2003-12-09

A method and apparatus for analyzing nucleic acids includes immobilizing nucleic probes at specific sites within a microchannel structure and moving target nucleic acids into proximity to the probes in order to allow hybridization and fluorescence detection of specific target sequences.

Method for analyzing nucleic acids by means of a substrate having a microchannel structure containing immobilized nucleic acid probes

DOEpatents

Ramsey, J. Michael; Foote, Robert S.

2002-01-01

A method and apparatus for analyzing nucleic acids includes immobilizing nucleic probes at specific sites within a microchannel structure and moving target nucleic acids into proximity to the probes in order to allow hybridization and fluorescence detection of specific target sequences.

Oligonucleoside alkyl or arylphosphonate derivatives capable of crosslinking with or cleaving nucleic acids

DOEpatents

Miller, Paul S.; Ts'o, Paul O.P.

1999-06-15

A composition for inactivating a target nucleic acid which comprises an oligonucleoside alkyl or arylphosphonate analogue which is complementary to the sequence of the target nucleic acid and includes a functional group which reacts with the target nucleic acid to render the target nucleic acid inactive or nonfunctional.

Accelerated digestion of nucleic acids by pepsin from the stomach of chicken.

PubMed

Liu, Y; Zhang, Y; Guo, H; Wu, W; Dong, P; Liang, X

2016-10-01

Nucleic acids have become an important nutritional supplement in poultry feed; however, the digestion of nucleic acids in poultry is unclear. The objective of this study was to investigate the digestion of nucleic acids by chicken pepsin in vitro. The extracted pepsinogen from the stomach of the chicken was purified to homogeneity. Upon activation at pH 2.0, chicken pepsinogen was converted to its active form. Nucleic acids, including λ-DNA, salmon sperm DNA and single-strand DNA (ssDNA), can be used as substrates and digested into short-chain oligonucleotides by pepsin. Interestingly, the digestion of the nucleic acids was inhibited when pepsin was treated by alkaline solution (pH 8.0) or pepstatin A. Also, the digestion of the nucleic acids was not affected by the addition of haemoglobin or bovine serum albumin. The results suggested that nucleic acids could be digested by chicken pepsin. Thus pepsin may have a role in digesting nucleic acids in vivo. Nucleic acids added to poultry fed may be digested, starting from the stomach.

Liposome-coated mesoporous silica nanoparticles loaded with L-cysteine for photoelectrochemical immunoassay of aflatoxin B1.

PubMed

Lin, Youxiu; Zhou, Qian; Zeng, Yongyi; Tang, Dianping

2018-06-02

The authors describe a photoelectrochemical (PEC) immunoassay for determination of aflatoxin B 1 (AFB 1 ) in foodstuff. The competitive immunoreaction is carried out on a microplate coated with a capture antibody against AFB 1 using AFB 1 -bovine serum albumin (BSA)-liposome-coated mesoporous silica nanoparticles (MSN) loaded with L-cysteine as a support. The photocurrent is produced by a photoactive material consisting of cerium-doped Bi 2 MoO 6 . Initially, L-cysteine acting as the electron donor is gated in the pores by interaction between mesoporous silica and liposome. Thereafter, AFB 1 -BSA conjugates are covalently bound to the liposomes. Upon introduction of the analyte (AFB 1 ), the labeled AFB 1 -BSA complex competes with the analyte for the antibody deposited on the microplate. Accompanying with the immunocomplex, the liposomes on the MSNs are lysed upon addition of Triton X-100. This results in the opening of the pores and in a release of L-cysteine. Free cysteine then induces the electron-hole scavenger of the photoactive nanosheets to increase the photocurrent. The photocurrent (relative to background signal) increases with increasing AFB 1 concentration. Under optimum conditions, the photoactive nanosheets display good photoelectrochemical responses, and allow the detection of AFB 1 at a concentration as low as 0.1 pg·mL -1 within a linear response in the 0.3 pg·mL -1 to 10 ng·mL -1 concentration range. Accuracy was evaluated by analyzing naturally contaminated and spiked peanut samples by using a commercial AFB 1 ELISA kit as the reference, and well-matching results were obtained. Graphical abstract Schematic presentation of a photoelectrochemical immunoassay for AFB 1 . It is based on the use of Ce-doped Bi 2 MoO 6 nanosheets and of liposome-coated mesoporous silica nanoparticles loaded with L-cysteine.

Ultrasensitive biomolecular assays with amplifying nanowire FET biosensors

NASA Astrophysics Data System (ADS)

Chui, Chi On; Shin, Kyeong-Sik; Mao, Yufei

2013-09-01

In this paper, we review our recent development and validation of the ultrasensitive electronic biomolecular assays enabled by our novel amplifying nanowire field-effect transistor (nwFET) biosensors. Our semiconductor nwFET biosensor platform technology performs extreme proximity signal amplification in the electrical domain that requires neither labeling nor enzymes nor optics. We have designed and fabricated the biomolecular assay prototypes and developed the corresponding analytical procedures. We have also confirmed their analytical performance in quantitating key protein biomarker in human serum, demonstrating an ultralow limit of detection and concurrently high output current level for the first time.

Detection of nucleic acid sequences by invader-directed cleavage

DOEpatents

Brow, Mary Ann D.; Hall, Jeff Steven Grotelueschen; Lyamichev, Victor; Olive, David Michael; Prudent, James Robert

1999-01-01

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The 5' nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof. The present invention further relates to methods and devices for the separation of nucleic acid molecules based by charge.

Cleavage of nucleic acids

DOEpatents

Prudent, James R.; Hall, Jeff G.; Lyamichev, Victor L.; Brow, Mary Ann D.; Dahlberg, James E.

2007-12-11

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof.

Invasive cleavage of nucleic acids

DOEpatents

Prudent, James R.; Hall, Jeff G.; Lyamichev, Victor I.; Brow, Mary Ann D.; Dahlberg, James E.

1999-01-01

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof.

Invasive cleavage of nucleic acids

DOEpatents

Prudent, James R.; Hall, Jeff G.; Lyamichev, Victor I.; Brow, Mary Ann D.; Dahlberg, James E.

2002-01-01

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof.

Cleavage of nucleic acids

DOEpatents

Prudent, James R.; Hall, Jeff G.; Lyamichev, Victor I.; Brow; Mary Ann D.; Dahlberg, James E.

2010-11-09

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof.

Cleavage of nucleic acids

DOEpatents

Prudent, James R.; Hall, Jeff G.; Lyamichev, Victor I.; Brow, Mary Ann D.; Dahlberg, James E.

2000-01-01

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof.

Nucleic acid detection assays

DOEpatents

Prudent, James R.; Hall, Jeff G.; Lyamichev, Victor I.; Brow, Mary Ann; Dahlberg, James E.

2005-04-05

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof.

Oligonucleoside alkyl or arylphosphonate derivatives capable of crosslinking with or cleaving nucleic acids

DOEpatents

Miller, P.S.; Ts'o, P.O.P.

1999-06-15

A composition for inactivating a target nucleic acid which comprises an oligonucleoside alkyl or arylphosphonate analogue which is complementary to the sequence of the target nucleic acid is provided. It includes a functional group which reacts with the target nucleic acid to render the target nucleic acid inactive or nonfunctional. 16 figs.

Polymerase chain reaction system using magnetic beads for analyzing a sample that includes nucleic acid

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

Nasarabadi, Shanavaz

2011-01-11

A polymerase chain reaction system for analyzing a sample containing nucleic acid includes providing magnetic beads; providing a flow channel having a polymerase chain reaction chamber, a pre polymerase chain reaction magnet position adjacent the polymerase chain reaction chamber, and a post pre polymerase magnet position adjacent the polymerase chain reaction chamber. The nucleic acid is bound to the magnetic beads. The magnetic beads with the nucleic acid flow to the pre polymerase chain reaction magnet position in the flow channel. The magnetic beads and the nucleic acid are washed with ethanol. The nucleic acid in the polymerase chain reactionmore » chamber is amplified. The magnetic beads and the nucleic acid are separated into a waste stream containing the magnetic beads and a post polymerase chain reaction mix containing the nucleic acid. The reaction mix containing the nucleic acid flows to an analysis unit in the channel for analysis.« less

Solid phase sequencing of double-stranded nucleic acids

DOEpatents

Fu, Dong-Jing; Cantor, Charles R.; Koster, Hubert; Smith, Cassandra L.

2002-01-01

This invention relates to methods for detecting and sequencing of target double-stranded nucleic acid sequences, to nucleic acid probes and arrays of probes useful in these methods, and to kits and systems which contain these probes. Useful methods involve hybridizing the nucleic acids or nucleic acids which represent complementary or homologous sequences of the target to an array of nucleic acid probes. These probe comprise a single-stranded portion, an optional double-stranded portion and a variable sequence within the single-stranded portion. The molecular weights of the hybridized nucleic acids of the set can be determined by mass spectroscopy, and the sequence of the target determined from the molecular weights of the fragments. Nucleic acids whose sequences can be determined include nucleic acids in biological samples such as patient biopsies and environmental samples. Probes may be fixed to a solid support such as a hybridization chip to facilitate automated determination of molecular weights and identification of the target sequence.

Enhanced photoelectrochemical properties of TiO2 nanorod arrays decorated with CdS nanoparticles

PubMed Central

Xie, Zheng; Liu, Xiangxuan; Wang, Weipeng; Liu, Can; Li, Zhengcao; Zhang, Zhengjun

2014-01-01

TiO2 nanorod arrays (TiO2 NRAs) sensitized with CdS nanoparticles were fabricated via successive ion layer adsorption and reaction (SILAR), and TiO2 NRAs were obtained by oxidizing Ti NRAs obtained through oblique angle deposition. The TiO2 NRAs decorated with CdS nanoparticles exhibited excellent photoelectrochemical and photocatalytic properties under visible light, and the one decorated with 20 SILAR cycles CdS nanoparticles shows the best performance. This can be attributed to the enhanced separation of electrons and holes by forming heterojunctions of CdS nanoparticles and TiO2 NRAs. This provides a promising way to fabricate the material for solar energy conversion and wastewater degradation. PMID:27877718

Self-deposition of Pt nanoparticles on graphene woven fabrics for enhanced hybrid Schottky junctions and photoelectrochemical solar cells.

PubMed

Kang, Zhe; Tan, Xinyu; Li, Xiao; Xiao, Ting; Zhang, Li; Lao, Junchao; Li, Xinming; Cheng, Shan; Xie, Dan; Zhu, Hongwei

2016-01-21

In this study, we demonstrated a self-deposition method to deposit Pt nanoparticles (NPs) on graphene woven fabrics (GWF) to improve the performance of graphene-on-silicon solar cells. The deposition of Pt NPs increased the work function of GWF and reduced the sheet resistance of GWF, thereby improving the power conversion efficiency (PCE) of graphene-on-silicon solar cells. The PCE (>10%) was further enhanced via solid electrolyte coating of the hybrid Schottky junction in the photoelectrochemical solar cells. These results suggest that the combination of self-deposition of Pt NPs and solid-state electrolyte coating of graphene-on-silicon is a promising way to produce high performance graphene-on-semiconductor solar cells.

Numerical algorithms based on Galerkin methods for the modeling of reactive interfaces in photoelectrochemical (PEC) solar cells

NASA Astrophysics Data System (ADS)

Harmon, Michael; Gamba, Irene M.; Ren, Kui

2016-12-01

This work concerns the numerical solution of a coupled system of self-consistent reaction-drift-diffusion-Poisson equations that describes the macroscopic dynamics of charge transport in photoelectrochemical (PEC) solar cells with reactive semiconductor and electrolyte interfaces. We present three numerical algorithms, mainly based on a mixed finite element and a local discontinuous Galerkin method for spatial discretization, with carefully chosen numerical fluxes, and implicit-explicit time stepping techniques, for solving the time-dependent nonlinear systems of partial differential equations. We perform computational simulations under various model parameters to demonstrate the performance of the proposed numerical algorithms as well as the impact of these parameters on the solution to the model.

Solar-to-Chemical Energy Conversion with Photoelectrochemical Tandem Cells.

PubMed

Sivula, Kevin

2013-01-01

Efficiently and inexpensively converting solar energy into chemical fuels is an important goal towards a sustainable energy economy. An integrated tandem cell approach could reasonably convert over 20% of the sun's energy directly into chemical fuels like H2 via water splitting. Many different systems have been investigated using various combinations of photovoltaic cells and photoelectrodes, but in order to be economically competitive with the production of H2 from fossil fuels, a practical water splitting tandem cell must optimize cost, longevity and performance. In this short review, the practical aspects of solar fuel production are considered from the perspective of a semiconductor-based tandem cell and the latest advances with a very promising technology - metal oxide photoelectrochemical tandem cells - are presented.

Reactor process using metal oxide ceramic membranes

DOEpatents

Anderson, M.A.

1994-05-03

A reaction vessel for use in photoelectrochemical reactions includes as its reactive surface a metal oxide porous ceramic membrane of a catalytic metal such as titanium. The reaction vessel includes a light source and a counter electrode. A provision for applying an electrical bias between the membrane and the counter electrode permits the Fermi levels of potential reaction to be favored so that certain reactions may be favored in the vessel. The electrical biasing is also useful for the cleaning of the catalytic membrane. Also disclosed is a method regenerating a porous metal oxide ceramic membrane used in a photoelectrochemical catalytic process by periodically removing the reactants and regenerating the membrane using a variety of chemical, thermal, and electrical techniques. 2 figures.

Stable N-CuInSe.sub.2 /iodide-iodine photoelectrochemical cell

DOEpatents

Cahen, David; Chen, Yih W.

1985-01-01

In a photoelectrochemical solar cell, stable output and solar efficiency in excess of 10% are achieved with a photoanode of n-CuInSe.sub.2 electrode material and an iodine/iodide redox couple used in a liquid electrolyte. The photoanode is prepared by treating the electrode material by chemical etching, for example in Br.sub.2 /MeOH; heating the etched electrode material in air or oxygen; depositing a surface film coating of indium on the electrode material after the initial heating; and thereafter again heating the electrode material in air or oxygen to oxidize the indium. The electrolyte is treated by the addition of Cu.sup.+ or Cu.sup.2+ salts and In.sup.3+ salts.

Stable n-CuInSe/sub 2/iodide-iodine photoelectrochemical cell

DOEpatents

Cahen, D.; Chen, Y.W.

1984-09-20

In a photoelectrochemical solar cell, stable output and solar efficiency in excess of 10% are achieved with a photoanode of n-CuInSe/sub 2/ electrode material and an iodine/iodide redox couple used in a liquid electrolyte. The photoanode is prepared by treating the electrode material by chemical etching, for example in Br/sub 2//MeOH; heating the etched electrode material in air or oxygen; depositing a surface film coating of indium on the electrode material after the initial heating; and thereafter again heating the electrode material in air or oxygen to oxidize the indium. The electrolyte is treated by the addition of Cu/sup +/ or Cu/sup 2 +/ salts and in In/sup 3 +/ salts.

The "Rust" Challenge: On the Correlations between Electronic Structure, Excited State Dynamics, and Photoelectrochemical Performance of Hematite Photoanodes for Solar Water Splitting.

PubMed

Grave, Daniel A; Yatom, Natav; Ellis, David S; Toroker, Maytal Caspary; Rothschild, Avner

2018-03-05

In recent years, hematite's potential as a photoanode material for solar hydrogen production has ignited a renewed interest in its physical and interfacial properties, which continues to be an active field of research. Research on hematite photoanodes provides new insights on the correlations between electronic structure, transport properties, excited state dynamics, and charge transfer phenomena, and expands our knowledge on solar cell materials into correlated electron systems. This research news article presents a snapshot of selected theoretical and experimental developments linking the electronic structure to the photoelectrochemical performance, with particular focus on optoelectronic properties and charge carrier dynamics. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantitative detection of pathogens in centrifugal microfluidic disks

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

Koh, Chung-Yan; Schaff, Ulrich Y.; Sommer, Gregory Jon

A system and methods for detection of a nucleic acid including forming a plurality of nucleic acid detection complexes are described, each of the complexes including a nucleic acid analyte, a detection agent and a functionalized probe. The method further including binding the nucleic acid detection complexes to a plurality of functionalized particles in a fluid sample and separating the functionalized particles having the nucleic acid detection complexes bound thereto from the fluid sample using a density media. The nucleic acid analyte is detected by detecting the detection agent.

Method for promoting specific alignment of short oligonucleotides on nucleic acids

DOEpatents

Studier, F. William; Kieleczawa, Jan; Dunn, John J.

1996-01-01

Disclosed is a method for promoting specific alignment of short oligonucleotides on a nucleic acid polymer. The nucleic acid polymer is incubated in a solution containing a single-stranded DNA-binding protein and a plurality of oligonucleotides which are perfectly complementary to distinct but adjacent regions of a predetermined contiguous nucleotide sequence in the nucleic acid polymer. The plurality of oligonucleotides anneal to the nucleic acid polymer to form a contiguous region of double stranded nucleic acid. Specific application of the methods disclosed include priming DNA synthesis and template-directed ligation.

High processivity polymerases

DOEpatents

Shamoo, Yousif; Sun, Siyang

2014-06-10

Chimeric proteins comprising a sequence nonspecific single-stranded nucleic-acid-binding domain joined to a catalytic nucleic-acid-modifying domain are provided. Methods comprising contacting a nucleic acid molecule with a chimeric protein, as well as systems comprising a nucleic acid molecule, a chimeric protein, and an aqueous solution are also provided. The joining of sequence nonspecific single-stranded nucleic-acid-binding domain and a catalytic nucleic-acid-modifying domain in chimeric proteins, among other things, may prevent the separation of the two domains due to their weak association and thereby enhances processivity while maintaining fidelity.

One-step coelectrodeposition-assisted layer-by-layer assembly of gold nanoparticles and reduced graphene oxide and its self-healing three-dimensional nanohybrid for an ultrasensitive DNA sensor.

PubMed

Kumarasamy, Jayakumar; Camarada, María Belén; Venkatraman, Dharuman; Ju, Huangxian; Dey, Ramendra Sundar; Wen, Yangping

2018-01-18

A layer-by-layer (LBL) assembly was employed for preparing multilayer thin films with a controlled architecture and composition. In this study, we report the one-step coelectrodeposition-assisted LBL assembly of both gold nanoparticles (AuNPs) and reduced graphene oxide (rGO) on the surface of a glassy carbon electrode (GCE) for the ultrasensitive electrochemical impedance sensing of DNA hybridization. A self-healable nanohybrid thin film with a three-dimensional (3D) alternate-layered nanoarchitecture was obtained by the one-step simultaneous electro-reduction of both graphene oxide and gold chloride in a high acidic medium of H 2 SO 4 using cyclic voltammetry and was confirmed by different characterization techniques. The DNA bioelectrode was prepared by immobilizing the capture DNA onto the surface of the as-obtained self-healable AuNP/rGO/AuNP/GCE with a 3D LBL nanoarchitecture via gold-thiol interactions, which then served as an impedance sensing platform for the label-free ultrasensitive electrochemical detection of DNA hybridization over a wide range from 1.0 × 10 -9 to 1.0 × 10 -13 g ml -1 , a low limit of detection of 3.9 × 10 -14 g ml -1 (S/N = 3), ultrahigh sensitivity, and excellent selectivity. This study presents a promising electrochemical sensing platform for the label-free ultrasensitive detection of DNA hybridization with potential application in cancer diagnostics and the preparation of a self-healable nanohybrid thin film with a 3D alternate-layered nanoarchitecture via a one-step coelectrodeposition-assisted LBL assembly.

Magnetic Nanozyme-Linked Immunosorbent Assay for Ultrasensitive Influenza A Virus Detection.

PubMed

Oh, Sangjin; Kim, Jeonghyo; Tran, Van Tan; Lee, Dong Kyu; Ahmed, Syed Rahin; Hong, Jong Chul; Lee, Jaewook; Park, Enoch Y; Lee, Jaebeom

2018-04-18

Rapid and sensitive detection of influenza virus is of soaring importance to prevent further spread of infections and adequate clinical treatment. Herein, an ultrasensitive colorimetric assay called magnetic nano(e)zyme-linked immunosorbent assay (MagLISA) is suggested, in which silica-shelled magnetic nanobeads (MagNBs) and gold nanoparticles are combined to monitor influenza A virus up to femtogram per milliliter concentration. Two essential strategies for ultrasensitive sensing are designed, i.e., facile target separation by MagNBs and signal amplification by the enzymelike activity of gold nanozymes (AuNZs). The enzymelike activity was experimentally and computationally evaluated, where the catalyticity of AuNZ was tremendously stronger than that of normal biological enzymes. In the spiked test, a straightforward linearity was presented in the range of 5.0 × 10 -15 -5.0 × 10 -6 g·mL -1 in detecting the influenza virus A (New Caledonia/20/1999) (H1N1). The detection limit is up to 5.0 × 10 -12 g·mL -1 only by human eyes, as well as up to 44.2 × 10 -15 g·mL -1 by a microplate reader, which is the lowest record to monitor influenza virus using enzyme-linked immunosorbent assay-based technology as far as we know. Clinically isolated human serum samples were successfully observed at the detection limit of 2.6 PFU·mL -1 . This novel MagLISA demonstrates, therefore, a robust sensing platform possessing the advances of fathomable sample separation, enrichment, ultrasensitive readout, and anti-interference ability may reduce the spread of influenza virus and provide immediate clinical treatment.

Detection of nucleic acids by multiple sequential invasive cleavages

DOEpatents

Hall, Jeff G.; Lyamichev, Victor I.; Mast, Andrea L.; Brow, Mary Ann D.

1999-01-01

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof. The present invention further relates to methods and devices for the separation of nucleic acid molecules based on charge. The present invention also provides methods for the detection of non-target cleavage products via the formation of a complete and activated protein binding region. The invention further provides sensitive and specific methods for the detection of human cytomegalovirus nucleic acid in a sample.

Nucleic acid detection kits

DOEpatents

Hall, Jeff G.; Lyamichev, Victor I.; Mast, Andrea L.; Brow, Mary Ann; Kwiatkowski, Robert W.; Vavra, Stephanie H.

2005-03-29

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof. The present invention further relates to methods and devices for the separation of nucleic acid molecules based on charge. The present invention also provides methods for the detection of non-target cleavage products via the formation of a complete and activated protein binding region. The invention further provides sensitive and specific methods for the detection of nucleic acid from various viruses in a sample.

Detection of nucleic acids by multiple sequential invasive cleavages 02

DOEpatents

Hall, Jeff G.; Lyamichev, Victor I.; Mast, Andrea L.; Brow, Mary Ann D.

2002-01-01

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof. The present invention further relates to methods and devices for the separation of nucleic acid molecules based on charge. The present invention also provides methods for the detection of non-target cleavage products via the formation of a complete and activated protein binding region. The invention further provides sensitive and specific methods for the detection of human cytomegalovirus nucleic acid in a sample.

Detection of nucleic acids by multiple sequential invasive cleavages

DOEpatents

Hall, Jeff G; Lyamichev, Victor I; Mast, Andrea L; Brow, Mary Ann D

2012-10-16

The present invention relates to means for the detection and characterization of nucleic acid sequences, as well as variations in nucleic acid sequences. The present invention also relates to methods for forming a nucleic acid cleavage structure on a target sequence and cleaving the nucleic acid cleavage structure in a site-specific manner. The structure-specific nuclease activity of a variety of enzymes is used to cleave the target-dependent cleavage structure, thereby indicating the presence of specific nucleic acid sequences or specific variations thereof. The present invention further relates to methods and devices for the separation of nucleic acid molecules based on charge. The present invention also provides methods for the detection of non-target cleavage products via the formation of a complete and activated protein binding region. The invention further provides sensitive and specific methods for the detection of human cytomegalovirus nucleic acid in a sample.

Nucleic acid-binding polymers as anti-inflammatory agents

PubMed Central

Lee, Jaewoo; Sohn, Jang Wook; Zhang, Ying; Leong, Kam W.; Pisetsky, David; Sullenger, Bruce A.

2011-01-01

Dead and dying cells release nucleic acids. These extracellular RNAs and DNAs can be taken up by inflammatory cells and activate multiple nucleic acid-sensing toll-like receptors (TLR3, 7, 8, and 9). The inappropriate activation of these TLRs can engender a variety of inflammatory and autoimmune diseases. The redundancy of the TLR family encouraged us to seek materials that can neutralize the proinflammatory effects of any nucleic acid regardless of its sequence, structure or chemistry. Herein we demonstrate that certain nucleic acid-binding polymers can inhibit activation of all nucleic acid-sensing TLRs irrespective of whether they recognize ssRNA, dsRNA or hypomethylated DNA. Furthermore, systemic administration of such polymers can prevent fatal liver injury engendered by proinflammatory nucleic acids in an acute toxic shock model in mice. Therefore these polymers represent a novel class of anti-inflammatory agent that can act as molecular scavengers to neutralize the proinflammatory effects of various nucleic acids. PMID:21844380

Self-assembling multimeric nucleic acid constructs

DOEpatents

Cantor, Charles R.; Niemeyer, Christof M.; Smith, Cassandra L.; Sano, Takeshi; Hnatowich, Donald J.; Rusckowski, Mary

1999-10-12

The invention is directed to constructs and compositions containing multimeric forms of nucleic acid. Multimeric nucleic acids comprise single-stranded nucleic acids attached via biotin to streptavidin and bound with a functional group. These constructs can be utilized in vivo to treat or identify diseased tissue or cells. Repeated administrations of multimeric nucleic acid compositions produce a rapid and specific amplification of nucleic acid constructs and their attached functional groups. For treatment purposes, functional groups may be toxins, radioisotopes, genes or enzymes. Diagnostically, labeled multimeric constructs may be used to identify specific targets in vivo or in vitro. Multimeric nucleic acids may also be used in nanotechnology and to create self-assembling polymeric aggregates such as membranes of defined porosity, microcircuits and many other products.

Self-assembling multimeric nucleic acid constructs

DOEpatents

Cantor, Charles R.; Niemeyer, Christof M.; Smith, Cassandra L.; Sano, Takeshi; Hnatowich, Donald J.; Rusckowski, Mary

1996-01-01

The invention is directed to constructs and compositions containing multimeric forms of nucleic acid. Multimeric nucleic acids comprise single-stranded nucleic acids attached via biotin to streptavidin and bound with a functional group. These constructs can be utilized in vivo to treat or identify diseased tissue or cells. Repeated administrations of multimeric nucleic acid compositions produce a rapid and specific amplification of nucleic acid constructs and their attached functional groups. For treatment purposes, functional groups may be toxins, radioisotopes, genes or enzymes. Diagnostically, labeled multimeric constructs may be used to identify specific targets in vivo or in vitro. Multimeric nucleic acids may also be used in nanotechnology and to create self-assembling polymeric aggregates such as membranes of defined porosity, microcircuits and many other products.

Shaping up nucleic acid computation.

PubMed

Chen, Xi; Ellington, Andrew D

2010-08-01

Nucleic acid-based nanotechnology has always been perceived as novel, but has begun to move from theoretical demonstrations to practical applications. In particular, the large address spaces available to nucleic acids can be exploited to encode algorithms and/or act as circuits and thereby process molecular information. In this review we not only revisit several milestones in the field of nucleic acid-based computation, but also highlight how the prospects for nucleic acid computation go beyond just a large address space. Functional nucleic acid elements (aptamers, ribozymes, and deoxyribozymes) can serve as inputs and outputs to the environment, and can act as logical elements. Into the future, the chemical dynamics of nucleic acids may prove as useful as hybridization for computation. Copyright © 2010 Elsevier Ltd. All rights reserved.

Self-assembling multimeric nucleic acid constructs

DOEpatents

Cantor, C.R.; Niemeyer, C.M.; Smith, C.L.; Sano, Takeshi; Hnatowich, D.J.; Rusckowski, M.

1996-10-01

The invention is directed to constructs and compositions containing multimeric forms of nucleic acid. Multimeric nucleic acids comprise single-stranded nucleic acids attached via biotin to streptavidin and bound with a functional group. These constructs can be utilized in vivo to treat or identify diseased tissue or cells. Repeated administrations of multimeric nucleic acid compositions produce a rapid and specific amplification of nucleic acid constructs and their attached functional groups. For treatment purposes, functional groups may be toxins, radioisotopes, genes or enzymes. Diagnostically, labeled multimeric constructs may be used to identify specific targets in vivo or in vitro. Multimeric nucleic acids may also be used in nanotechnology and to create self-assembling polymeric aggregates such as membranes of defined porosity, microcircuits and many other products. 5 figs.

A preliminary result of three-dimensional microarray technology to gene analysis with endoscopic ultrasound-guided fine-needle aspiration specimens and pancreatic juices

PubMed Central

2010-01-01

Background Analysis of gene expression and gene mutation may add information to be different from ordinary pathological tissue diagnosis. Since samples obtained endoscopically are very small, it is desired that more sensitive technology is developed for gene analysis. We investigated whether gene expression and gene mutation analysis by newly developed ultra-sensitive three-dimensional (3D) microarray is possible using small amount samples from endoscopic ultrasound-guided fine-needle aspiration (EUS-FNA) specimens and pancreatic juices. Methods Small amount samples from 17 EUS-FNA specimens and 16 pancreatic juices were obtained. After nucleic acid extraction, the samples were amplified with labeling and analyzed by the 3D microarray. Results The analyzable rate with the microarray was 46% (6/13) in EUS-FNA specimens of RNAlater® storage, and RNA degradations were observed in all the samples of frozen storage. In pancreatic juices, the analyzable rate was 67% (4/6) in frozen storage samples and 20% (2/10) in RNAlater® storage. EUS-FNA specimens were classified into cancer and non-cancer by gene expression analysis and K-ras codon 12 mutations were also detected using the 3D microarray. Conclusions Gene analysis from small amount samples obtained endoscopically was possible by newly developed 3D microarray technology. High quality RNA from EUS-FNA samples were obtained and remained in good condition only using RNA stabilizer. In contrast, high quality RNA from pancreatic juice samples were obtained only in frozen storage without RNA stabilizer. PMID:20416107

A new class of fast-response and highly selective fluorescent probes for visualizing peroxynitrite in live cells, subcellular organelles, and kidney tissue of diabetic rats.

PubMed

Miao, Junfeng; Huo, Yingying; Liu, Qian; Li, Zhe; Shi, Heping; Shi, Yawei; Guo, Wei

2016-11-01

Peroxynitrite (ONOO(-)) is an extremely powerful oxidant in biological systems, and can react with a wide variety of molecular targets including proteins, lipids, and nucleic acids, eventually resulting in a series of disease states such as diabetes, Alzheimer's disease, cancer, arthritis, autoimmune, and other disorders. In this work, we present a new class of ONOO(-) fluorescent probes by exploiting the ONOO(-)-triggered N-oxidation and N-nitrosation reactions of aromatic tertiary amine for the first time. The as-obtained fluorescent probe A2 could detect ONOO(-) with quite fast fluorescence off-on response (within seconds), ultrasensitivity (detection limit: <2 nM), and excellent selectivity over a series of biologically relevant reactive oxygen species as well as metal cations. With the probe, the endogenous ONOO(-) in activated RAW264.7 murine macrophage, EA.hy926 endothelial cells after oxygen glucose deprivation and reoxygenation (OGD/RO), and kidney tissue of diabetic rats has been successfully visualized. Based on the molecular platform of A2, we further develop its mitochondria- and lysosome-targetable fluorescent probes Mito-A2 and Lyso-A2 by installing the corresponding targeting groups to alkoxy unit of A2, and confirm their abilities to image ONOO(-) in mitochondria and lysosomes, respectively, by co-localization assays. It is greatly expected that these probes can serve as useful imaging tools for clarifying the distribution and pathophysiological functions of ONOO(-) in cells, subcellular organelles, and animal tissues. Copyright © 2016 Elsevier Ltd. All rights reserved.

Nanoplasmonic biosensor: detection and amplification of dual bio-signatures of circulating tumor DNA.

PubMed

Nguyen, Anh H; Sim, Sang Jun

2015-05-15

Circulating tumor DNA (ctDNA) bearing tumor-specific mutation and methylation are promising biomarkers for noninvasive cancer assessment. However, existing methods for ctDNA detection are restricted to genetic mutations. Recently, nanoplasmonics has emerged as a platform for one-step dual detection with high sensitivity and specificity. Here we present a strategy for ultrasensitive detection of tumor-specific mutations (E542K and E545K) and methylation of ctDNA of PIK3CA gene based on localized surface plasmon resonance (LSPR) and the coupling plasmon mode of gold nanoparticles (AuNPs). Peptide nucleic acids (PNA) is used as a probe to capture and enrich the 69-bp PIK3CA ctDNA. The exposure of PNA-probed AuNPs to 200 fM ctDNA generates LSPR-peak shift of 4.3 nm, corresponding to the primary response. Immunogold colloids are exploited as methylation detectors and plasmon coupling based enhancement for secondary response. LSPR-peak shifted from 4.3 nm to 11.4 nm upon the immunogold colloids binding to two methylcytosines (mCpG), which is an approximately 107% increase, compared to that of the primary response. This enhancement leads to four times (~50 fM) improvement of sensitivity and because of two mCpG sites, ctDNA was detected. These results demonstrate that the sensor can simultaneously detect the hot-spot mutation and epigenetic changes on the ctDNA. Promisingly, other specific-tumor mutants and epigenetic changes can be detected at low concentration with this platform. Copyright © 2014 Elsevier B.V. All rights reserved.

Quantitative thermodynamic predication of interactions between nucleic acid and non-nucleic acid species using Microsoft excel.

PubMed

Zou, Jiaqi; Li, Na

2013-09-01

Proper design of nucleic acid sequences is crucial for many applications. We have previously established a thermodynamics-based quantitative model to help design aptamer-based nucleic acid probes by predicting equilibrium concentrations of all interacting species. To facilitate customization of this thermodynamic model for different applications, here we present a generic and easy-to-use platform to implement the algorithm of the model with Microsoft(®) Excel formulas and VBA (Visual Basic for Applications) macros. Two Excel spreadsheets have been developed: one for the applications involving only nucleic acid species, the other for the applications involving both nucleic acid and non-nucleic acid species. The spreadsheets take the nucleic acid sequences and the initial concentrations of all species as input, guide the user to retrieve the necessary thermodynamic constants, and finally calculate equilibrium concentrations for all species in various bound and unbound conformations. The validity of both spreadsheets has been verified by comparing the modeling results with the experimental results on nucleic acid sequences reported in the literature. This Excel-based platform described here will allow biomedical researchers to rationalize the sequence design of nucleic acid probes using the thermodynamics-based modeling even without relevant theoretical and computational skills. Copyright © 2013 Elsevier Ireland Ltd. All rights reserved.

An ultrasensitive strain sensor with a wide strain range based on graphene armour scales.

PubMed

Yang, Yi-Fan; Tao, Lu-Qi; Pang, Yu; Tian, He; Ju, Zhen-Yi; Wu, Xiao-Ming; Yang, Yi; Ren, Tian-Ling

2018-06-12

An ultrasensitive strain sensor with a wide strain range based on graphene armour scales is demonstrated in this paper. The sensor shows an ultra-high gauge factor (GF, up to 1054) and a wide strain range (ε = 26%), both of which present an advantage compared to most other flexible sensors. Moreover, the sensor is developed by a simple fabrication process. Due to the excellent performance, this strain sensor can meet the demands of subtle, large and complex human motion monitoring, which indicates its tremendous application potential in health monitoring, mechanical control, real-time motion monitoring and so on.

Ultra-sensitive near-infrared fiber-optic gas sensors enhanced by metal-organic frameworks

NASA Astrophysics Data System (ADS)

Chong, Xinyuan; Kim, Ki-Joong; Li, Erwen; Zhang, Yujing; Ohodnicki, Paul R.; Chang, Chih-Hung; Wang, Alan X.

2016-03-01

We demonstrate ultra-sensitive near-infrared (NIR) fiber-optic gas sensors enhanced by metalorganic framework (MOF) Cu-BTC (BTC=benzene-1,3,5- tricarboxylate), which is coated on a single-mode optical fiber. For the first time, we obtained high-resolution NIR spectroscopy of CO2 adsorbed in MOF without seeing any rotational side band. Real-time measurement showed different response time depending on the concentration of CO2, which is attributed to the complex adsorption and desorption mechanism of CO2 in Cu-BTC. The lowest detection limit of CO2 we achieved is 20 ppm with only 5-cm long Cu-BTC film.

Biomolecule detection based on Si single-electron transistors for practical use

NASA Astrophysics Data System (ADS)

Nakajima, Anri; Kudo, Takashi; Furuse, Sadaharu

2013-07-01

Experimental and theoretical analyses demonstrated that ultra-sensitive biomolecule detection can be achieved using a Si single-electron transistor (SET). A multi-island channel structure was used to enable room-temperature operation. Coulomb oscillation increases transconductance without increasing channel width, which increases detection sensitivity to a charged target. A biotin-modified SET biosensor was used to detect streptavidin at a dilute concentration. In addition, an antibody-functionalized SET biosensor was used for immunodetection of prostate-specific antigen, demonstrating its suitability for practical use. The feasibility of ultra-sensitive detection of biomolecules for practical use by using a SET biosensor was clearly proven through this systematic study.

Signal-on electrochemical detection of antibiotics at zeptomole level based on target-aptamer binding triggered multiple recycling amplification.

PubMed

Wang, Hongzhi; Wang, Yu; Liu, Su; Yu, Jinghua; Guo, Yuna; Xu, Ying; Huang, Jiadong

2016-06-15

In the work, a signal-on electrochemical DNA sensor based on multiple amplification for ultrasensitive detection of antibiotics has been reported. In the presence of target, the ingeniously designed hairpin probe (HP1) is opened and the polymerase-assisted target recycling amplification is triggered, resulting in autonomous generation of secondary target. It is worth noting that the produced secondary target could not only hybridize with other HP1, but also displace the Helper from the electrode. Consequently, methylene blue labeled HP2 forms a "close" probe structure, and the increase of signal is monitored. The increasing current provides an ultrasensitive electrochemical detection for antibiotics down to 1.3 fM. To our best knowledge, such work is the first report about multiple recycling amplification combing with signal-on sensing strategy, which has been utilized for quantitative determination of antibiotics. It would be further used as a general strategy associated with more analytical techniques toward the detection of a wide spectrum of analytes. Thus, it holds great potential for the development of ultrasensitive biosensing platform for the applications in bioanalysis, disease diagnostics, and clinical biomedicine. Copyright © 2016 Elsevier B.V. All rights reserved.

Ultrasensitive quantum dot fluorescence quenching assay for selective detection of mercury ions in drinking water.

PubMed

Ke, Jun; Li, Xinyong; Zhao, Qidong; Hou, Yang; Chen, Junhong

2014-07-09

Mercury is one of the most acutely toxic substances at trace level to human health and living thing. Developing a rapid, cheap and water soluble metal sensor for detecting mercury ions at ppb level remains a challenge. Herein, a metal sensor consisting of MPA coated Mn doped ZnSe/ZnS colloidal nanoparticles was utilized to ultrasensitively and selectively detect Hg(2+) ions with a low detection limit (0.1 nM) over a dynamic range from 0 to 20 nM. According to strong interaction between thiol(s) and mercury ions, mercaptopropionic acid (MPA) was used as a highly unique acceptor for mercury ions in the as-obtained ultrasensitive sensor. In the presence of mercury ions, colloidal nanoparticles rapidly agglomerated due to changes of surface chemical properties, which results in severe quenching of fluorescent intensity. Meanwhile, we find that the original ligands are separated from the surface of colloidal nanoparticles involving strongly chelation between mercury ion and thiol(s) proved by controlled IR analysis. The result shows that the QD-based metal ions sensor possesses satisfactory precision, high sensitivity and selectivity, and could be applied for the quantification analysis of real samples.

Self-Assembled Core-Satellite Gold Nanoparticle Networks for Ultrasensitive Detection of Chiral Molecules by Recognition Tunneling Current.

PubMed

Zhang, Yuanchao; Liu, Jingquan; Li, Da; Dai, Xing; Yan, Fuhua; Conlan, Xavier A; Zhou, Ruhong; Barrow, Colin J; He, Jin; Wang, Xin; Yang, Wenrong

2016-05-24

Chirality sensing is a very challenging task. Here, we report a method for ultrasensitive detection of chiral molecule l/d-carnitine based on changes in the recognition tunneling current across self-assembled core-satellite gold nanoparticle (GNP) networks. The recognition tunneling technique has been demonstrated to work at the single molecule level where the binding between the reader molecules and the analytes in a nanojunction. This process was observed to generate a unique and sensitive change in tunneling current, which can be used to identify the analytes of interest. The molecular recognition mechanism between amino acid l-cysteine and l/d-carnitine has been studied with the aid of SERS. The different binding strength between homo- or heterochiral pairs can be effectively probed by the copper ion replacement fracture. The device resistance was measured before and after the sequential exposures to l/d-carnitine and copper ions. The normalized resistance change was found to be extremely sensitive to the chirality of carnitine molecule. The results suggested that a GNP networks device optimized for recognition tunneling was successfully built and that such a device can be used for ultrasensitive detection of chiral molecules.

Template-free synthesis of porous ZnO/Ag microspheres as recyclable and ultra-sensitive SERS substrates

NASA Astrophysics Data System (ADS)

Liu, Yanjun; Xu, Chunxiang; Lu, Junfeng; Zhu, Zhu; Zhu, Qiuxiang; Manohari, A. Gowri; Shi, Zengliang

2018-01-01

The porous structured zinc oxide (ZnO) microspheres decorated with silver nanoparticles (Ag NPs) have been fabricated as surface-enhanced Raman scattering (SERS) substrate for ultra-sensitive, highly reproducible and stable biological/chemical sensing of various organic molecules. The ZnO microspheres were hydrothermally synthesized without any template, and the Ag NPs decorated on microspheres via photochemical reaction in situ, which provided stable Ag/ZnO contact to achieve a sensitive SERS response. It demonstrates a higher enhancement factor (EF) of 2.44 × 1011 and a lower detection limit of 10-11 M-10-12 M. This porous SERS substrate could also be self-cleaned through a photocatalytic process and then further recycled for the detection of same or different molecules, such as phenol red (PhR), dopamine (DA) and glucose (GLU) with ultra-low concentration and it possessed a sensitive response. The excellent performances are attributed to morphology of porous microspheres, hybrid structure of semiconductor/metal and corresponding localized field enhancement of surface plasmons. Therefore, it is expected to design the recyclable ultra-sensitive SERS sensors for the detection of biological molecules and organic pollutant monitoring.

Ultrasensitive Quantum Dot Fluorescence quenching Assay for Selective Detection of Mercury Ions in Drinking Water

PubMed Central

Ke, Jun; Li, Xinyong; Zhao, Qidong; Hou, Yang; Chen, Junhong

2014-01-01

Mercury is one of the most acutely toxic substances at trace level to human health and living thing. Developing a rapid, cheap and water soluble metal sensor for detecting mercury ions at ppb level remains a challenge. Herein, a metal sensor consisting of MPA coated Mn doped ZnSe/ZnS colloidal nanoparticles was utilized to ultrasensitively and selectively detect Hg2+ ions with a low detection limit (0.1 nM) over a dynamic range from 0 to 20 nM. According to strong interaction between thiol(s) and mercury ions, mercaptopropionic acid (MPA) was used as a highly unique acceptor for mercury ions in the as-obtained ultrasensitive sensor. In the presence of mercury ions, colloidal nanoparticles rapidly agglomerated due to changes of surface chemical properties, which results in severe quenching of fluorescent intensity. Meanwhile, we find that the original ligands are separated from the surface of colloidal nanoparticles involving strongly chelation between mercury ion and thiol(s) proved by controlled IR analysis. The result shows that the QD-based metal ions sensor possesses satisfactory precision, high sensitivity and selectivity, and could be applied for the quantification analysis of real samples. PMID:25005836

Ultrasensitive microfluidic solid-phase ELISA using an actuatable microwell-patterned PDMS chip.

PubMed

Wang, Tanyu; Zhang, Mohan; Dreher, Dakota D; Zeng, Yong

2013-11-07

Quantitative detection of low abundance proteins is of significant interest for biological and clinical applications. Here we report an integrated microfluidic solid-phase ELISA platform for rapid and ultrasensitive detection of proteins with a wide dynamic range. Compared to the existing microfluidic devices that perform affinity capture and enzyme-based optical detection in a constant channel volume, the key novelty of our design is two-fold. First, our system integrates a microwell-patterned assay chamber that can be pneumatically actuated to significantly reduce the volume of chemifluorescent reaction, markedly improving the sensitivity and speed of ELISA. Second, monolithic integration of on-chip pumps and the actuatable assay chamber allow programmable fluid delivery and effective mixing for rapid and sensitive immunoassays. Ultrasensitive microfluidic ELISA was demonstrated for insulin-like growth factor 1 receptor (IGF-1R) across at least five orders of magnitude with an extremely low detection limit of 21.8 aM. The microwell-based solid-phase ELISA strategy provides an expandable platform for developing the next-generation microfluidic immunoassay systems that integrate and automate digital and analog measurements to further improve the sensitivity, dynamic ranges, and reproducibility of proteomic analysis.

Enzyme-antibody dual labeled gold nanoparticles probe for ultrasensitive detection of κ-casein in bovine milk samples.

PubMed

Li, Y S; Zhou, Y; Meng, X Y; Zhang, Y Y; Liu, J Q; Zhang, Y; Wang, N N; Hu, P; Lu, S Y; Ren, H L; Liu, Z S

2014-11-15

A dual labeled probe was synthesized by coating gold nanoparticles (AuNPs) with anti-κ-CN monoclonal antibody (McAb) and horseradish peroxidase (HRP) enzyme on their surface. The McAb was used as detector and HRP was used as label for signal amplification catalytically oxidize the substrate. AuNPs were used as bridges between the McAb and HRP. Based on the probe, an immunoassay was developed for ultrasensitive detection of κ-CN in bovine milk samples. The assay has a linear response range within 4.2-560 ng mL(-1). The limit of detection (LOD) was 4.2 ng mL(-1) which was 10 times lower than that of traditional McAb-HRP based ELISA. The recoveries of κ-CN from three brand bovine milk samples were from 95.8% to 111.0% that had a good correlation (R(2)=0.998) with those obtained by official standard Kjeldahl method. For higher sensitivity and as simple as the traditional ELISA, the developed immunoassay could provide an alternative approach for ultrasensitive detection of κ-CN in bovine milk sample. Copyright © 2014 Elsevier B.V. All rights reserved.

Ultrasensitive and rapid detection of β-conglutin combining aptamers and isothermal recombinase polymerase amplification.

PubMed

Jauset-Rubio, Miriam; Sabaté Del Río, Jonathan; Mairal, Teresa; Svobodová, Markéta; El-Shahawi, Mohammad S; Bashammakh, Abdulaziz S; Alyoubi, Abdulrahman O; O'Sullivan, Ciara K

2017-01-01

Lupin is increasingly being used in a variety of food products due to its nutritional, functional and nutraceutical properties. However, several examples of severe and even fatal food-associated anaphylaxis due to lupin inhalation or ingestion have been reported, resulting in the lupin subunit β-conglutin, being defined as the Lup an 1 allergen by the International Union of Immunological Societies (IUIS) in 2008. Here, we report an innovative method termed aptamer-recombinase polymerase amplification (Apta-RPA) exploiting the affinity and specificity of a DNA aptamer selected against the anaphylactic β-conglutin allergen termed β-conglutin binding aptamer II (β-CBA II), facilitating ultrasensitive detection via isothermal amplification. Combining magnetic beads as the solid phase with Apta-RPA detection, the total assay time was reduced from 210 min to just 25 min, with a limit of detection of 3.5 × 10 -11  M, demonstrating a rapid and ultrasensitive generic methodology that can be used with any aptamer. Future work will focus on further simplification of the assay to a lateral flow format. Graphical Abstract Schematic representation of the rapid and novel bead-based Apta-RPA assay.

BiVO4 Photoanode with Exposed (040) Facets for Enhanced Photoelectrochemical Performance

NASA Astrophysics Data System (ADS)

Xia, Ligang; Li, Jinhua; Bai, Jing; Li, Linsen; Chen, Shuai; Zhou, Baoxue

2018-03-01

A BiVO4 photoanode with exposed (040) facets was prepared to enhance its photoelectrochemical performance. The exposure of the (040) crystal planes of the BiVO4 film was induced by adding NaCl to the precursor solution. The as-prepared BiVO4 photoanode exhibits higher solar-light absorption and charge-separation efficiency compared to those of an anode prepared without adding NaCl. To our knowledge, the photocurrent density (1.26 mA cm-2 at 1.23 V vs. RHE) of as-prepared BiVO4 photoanode is the highest according to the reports for bare BiVO4 films under simulated AM1.5G solar light, and the incident photon-to-current conversion efficiency is above 35% at 400 nm. The photoelectrochemical (PEC) water-splitting performance was also dramatically improved with a hydrogen evolution rate of 9.11 μmol cm-2 h-1, which is five times compared with the BiVO4 photoanode prepared without NaCl (1.82 μmol cm-2 h-1). Intensity-modulated photocurrent spectroscopy and transient photocurrent measurements show a higher charge-carrier-transfer rate for this photoanode. These results demonstrate a promising approach for the development of high-performance BiVO4 photoanodes which can be used for efficient PEC water splitting and degradation of organic pollutants. [Figure not available: see fulltext.

Discovery of Fe–Ce Oxide/BiVO 4 Photoanodes through Combinatorial Exploration of Ni–Fe–Co–Ce Oxide Coatings

DOE PAGES

Shinde, Aniketa; Guevarra, Dan; Liu, Guiji; ...

2016-08-23

An efficient photoanode is a prerequisite for a viable solar fuels technology. The challenges to realizing an efficient photoanode include the integration of a semiconductor light absorber and a metal oxide electrocatalyst to optimize corrosion protection, light trapping, hole transport, and photocarrier recombination sites. In order to efficiently explore metal oxide coatings, we employ a high throughput methodology wherein a uniform BiVO 4 film is coated with 858 unique metal oxide coatings covering a range of metal oxide loadings and the full (Ni-Fe-Co-Ce)Ox pseudo-quaternary composition space. Photoelectrochemical characterization of the photoanodes reveals that specific combinations of metal oxide composition andmore » loading provide up to a 13-fold increase in the maximum photoelectrochemical power generation for oxygen evolution in pH 13 electrolyte. Through mining of the high throughput data we identify composition regions that form improved interfaces with BiVO 4. Of particular note, integrated photoanodes with catalyst compositions in the range Fe (0.4-0.6)Ce (0.6-0.4)O x exhibit high interface quality and excellent photoelectrochemical power conversion. Furthermore, for scaled-up inkjet-printed electrodes and photoanodic electrodeposition of this composition on BiVO 4 we can confirm the discovery and the synthesis-independent interface improvement of (Fe-Ce)O x coatings on BiVO 4.« less

Sunlight-Driven Hydrogen Formation by Membrane-Supported Photoelectrochemical Water Splitting

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

Lewis, Nathan S.

2014-03-26

This report describes the significant advances in the development of the polymer-supported photoelectrochemical water-splitting system that was proposed under DOE grant number DE-FG02-05ER15754. We developed Si microwire-array photoelectrodes, demonstrated control over the material and light-absorption properties of the microwire-array photoelectrodes, developed inexpensive processes for synthesizing the arrays, and doped the arrays p-type for use as photocathodes. We also developed techniques for depositing metal-nanoparticle catalysts of the hydrogen-evolution reaction (HER) on the wire arrays, investigated the stability and catalytic performance of the nanoparticles, and demonstrated that Ni-Mo alloys are promising earth-abundant catalysts of the HER. We also developed methods that allowmore » reuse of the single-crystalline Si substrates used for microwire growth and methods of embedding the microwire photocathodes in plastic to enable large-scale processing and deployment of the technology. Furthermore we developed techniques for controlling the structure of WO3 films, and demonstrated that structural control can improve the quantum yield of photoanodes. Thus, by the conclusion of this project, we demonstrated significant advances in the development of all components of a sunlight-driven membrane-supported photoelectrochemical water-splitting system. This final report provides descriptions of some of the scientific accomplishments that were achieved under the support of this project and also provides references to the peer-reviewed publications that resulted from this effort.« less

Nanoporous TiO2 and WO3 films by anodization of titanium and tungsten substrates: influence of process variables on morphology and photoelectrochemical response.

PubMed

de Tacconi, N R; Chenthamarakshan, C R; Yogeeswaran, G; Watcharenwong, A; de Zoysa, R S; Basit, N A; Rajeshwar, K

2006-12-21

The photoelectrochemical response of nanoporous films, obtained by anodization of Ti and W substrates in a variety of corrosive media and at preselected voltages in the range from 10 to 60 V, was studied. The as-deposited films were subjected to thermal anneal and characterized by scanning electron microscopy and X-ray diffraction. Along with the anodization media developed by previous authors, the effect of poly(ethylene glycol) (PEG 400) or D-mannitol as a modifier to the NH4F electrolyte and glycerol addition to the oxalic acid electrolyte was studied for TiO2 and WO3, respectively. In general, intermediate anodization voltages and film growth times yielded excellent-quality photoelectrochemical response for both TiO2 and WO3 as assessed by linear-sweep photovoltammetry and photoaction spectra. The photooxidation of water and formate species was used as reaction probes to assess the photoresponse quality of the nanoporous oxide semiconductor films. In the presence of formate as an electron donor, the incident photon to electron conversion efficiency (IPCE) ranged from approximately 130% to approximately 200% for both TiO2 and WO3 depending on the film preparation protocol. The best photoactive films were obtained from poly(ethylene glycol) (PEG 400) containing NH4F for TiO2 and from aqueous NaF for WO3.

Engineered photoproteins that give rise to photosynthetically-incompetent bacteria are effective as photovoltaic materials for biohybrid photoelectrochemical cells.

PubMed

Liu, Juntai; Friebe, Vincent M; Swainsbury, David J K; Crouch, Lucy I; Szabo, David A; Frese, Raoul N; Jones, Michael R

2018-04-17

Reaction centre/light harvesting proteins such as the RCLH1X complex from Rhodobacter sphaeroides carry out highly quantum-efficient conversion of solar energy through ultrafast energy transfer and charge separation, and these pigment-proteins have been incorporated into biohybrid photoelectrochemical cells for a variety of applications. In this work we demonstrate that, despite not being able to support normal photosynthetic growth of Rhodobacter sphaeroides, an engineered variant of this RCLH1X complex lacking the PufX protein and with an enlarged light harvesting antenna is unimpaired in its capacity for photocurrent generation in two types of bio-photoelectrochemical cells. Removal of PufX also did not impair the ability of the RCLH1 complex to act as an acceptor of energy from synthetic light harvesting quantum dots. Unexpectedly, the removal of PufX led to a marked improvement in the overall stability of the RCLH1 complex under heat stress. We conclude that PufX-deficient RCLH1 complexes are fully functional in solar energy conversion in a device setting and that their enhanced structural stability could make them a preferred choice over their native PufX-containing counterpart. Our findings on the competence of RCLH1 complexes for light energy conversion in vitro are discussed with reference to the reason why these PufX-deficient proteins are not capable of light energy conversion in vivo.

Synthesis and characterization of spray deposited CZTS thin films for photo-electrochemical application

NASA Astrophysics Data System (ADS)

Chavda, Arvind; Patel, Biren; Mukhopadhyay, Priyanka Marathey Indrajit; Ray, Abhijit

2018-05-01

Cu2ZnSnS4 (CZTS) is one of the most promising light absorber materials for photovoltaic and photo-electrochemical applications. We synthesized CZTS thin films on a F:SnO2 and soda lime glass substrates by very simple, cost effective and highly scalable spray pyrolysis technique. The films were post treated by rapid thermal processing route of sulfurization to enhance the stoichiometry and crystallinity of the film. The structural, morphological, optical and electrical properties of RTP sulfurized films were studied. The X-ray diffraction (XRD) pattern revealed the formation of tetragonal CZTS phase, which confirmed by Raman analysis with a major peak at 336 cm-1 without the presence of the principle vibration mode of any other secondary phases, such as Cu2SnS3, CuxS(x=1.8,2) etc. The sulfurized film exhibited increased crystallinity and better stoichiometry. The optical and electrical data reveal the direct optical band gap, bulk carrier concentration and resistivity of 1.5 eV, 2.28×1018 cm-3 and 1.21 Ω/cm2, respectively. Finally the photoactivity of CZTS thin films was tested by forming photoelectrochemical cell in 0.1M Na2S2O3 electrolyte (pH=7.72), showing a cathodic photocurrent of nearly 20 µA/cm2 at 0V RHE.

S-TiO2/S-reduced graphene oxide for enhanced photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Elbakkay, Mohamed H.; El Rouby, Waleed M. A.; El-Dek, S. I.; Farghali, Ahmed A.

2018-05-01

Sulfur-doped titanium oxide on the surface of sulfur-doped reduced graphene oxide nanocomposites (S-TiO2/S-RGO) were successfully synthesized for the first time through a simple low cost solvothermal reaction process. The sulfur doping was detected in both TiO2 matrix and carbon framework structure of reduced graphene oxide using X-ray photoelectron spectroscopy (XPS) and Energy-dispersive X-ray spectroscopy (EDX). Cross-sectional AFM analysis of S-RGO nanosheets reveals a thickness of 0.51 nm which is much thinner than those previously reported of heteroatom doped-RGO, confirming the single-layer feature. When the as-prepared (S-TiO2/S-RGO) nanocomposites are utilized as photoanodes for photoelectrochemical (PEC) water splitting, they exhibited an enhanced photoelectrochemical performance and long-term stability. The photocurrent density of S-TiO2/S-RGO(0.2) photoanode revealed 3.36 mA/cm2 at 1 V vs Ag/AgCl which is considered 3 times compared to bare synthesized TiO2. This improvement in the photocurrent density was attributed to the increased separation rate of photogenerated electrons and holes and efficient visible light harvesting as a result of the successful combination of the S-TiO2 and the S-RGO in the same nanocomposite photoanode. This promising result presents a new approach for the synthesis of high-efficient future metal-free photoelectrocatalysts.

Solar driven electrochromic photoelectrochemical fuel cells for simultaneous energy conversion, storage and self-powered sensing.

PubMed

Wang, Yanhu; Zhang, Lina; Cui, Kang; Xu, Caixia; Li, Hao; Liu, Hong; Yu, Jinghua

2018-02-15

One solar-driven electrochromic photoelectrochemical fuel cell (PFC) with highly efficient energy conversion and storage is easily constructed to achieve quantitative self-powered sensing. Layered bismuth oxyiodide-zinc oxide nanorod arrays (ZnO@BiOI NRA) with a core/shell p-n heterostructure are fabricated as the photoanode with electrochromic Prussian blue (PB) as the cathode. The core/shell p-n heterostructure for the ZnO@BiOI photoanode can effectively boost the photoelectrochemical (PEC) performance through the improvement of photon absorption and charge carrier separation. The optimal assembled PFC yields an open-circuit voltage (V OC ) of 0.48 V with the maximum power output density (P max ) as high as 155 μW cm -2 upon illumination. Benefitting from the interactive color-changing behavior of PB, the cathode not only exhibits cathodic catalytic activity in the PFC but also serves as an electrochromic display for self-powered sensing. The as-constructed PFC possesses multiple readable signal output nanochannels through the maximum power output density (P max ) of the PFC or the color change of PB. Meanwhile, the dual-signal-output makes the as-constructed self-powered sensor highly available in various operations demands with the enhanced reliability. With the advantages of high efficiency of PFCs, unique assay ability, and broad environmental suitability, the constructed self-powered platform shows broad application prospects as an integrated smart analytical device.

Discovery of Fe–Ce Oxide/BiVO 4 Photoanodes through Combinatorial Exploration of Ni–Fe–Co–Ce Oxide Coatings

DOE PAGES

Shinde, Aniketa; Guevarra, Dan; Liu, Guiji; ...

2016-08-23

An efficient photoanode is a prerequisite for a viable solar fuels technology. The challenges to realizing an efficient photoanode include the integration of a semiconductor light absorber and a metal oxide electrocatalyst to optimize corrosion protection, light trapping, hole transport, and photocarrier recombination sites. In order to efficiently explore metal oxide coatings, we employ a high throughput methodology wherein a uniform BiVO 4 film is coated with 858 unique metal oxide coatings covering a range of metal oxide loadings and the full (Ni-Fe-Co-Ce)O x pseudo-quaternary composition space. Photoelectrochemical characterization of the photoanodes reveals that specific combinations of metal oxide compositionmore » and loading provide up to a 13-fold increase in the maximum photoelectrochemical power generation for oxygen evolution in pH 13 electrolyte. Through mining of the high throughput data we identify composition regions that form improved interfaces with BiVO 4. Of particular note, integrated photoanodes with catalyst compositions in the range Fe (0.4-0.6)Ce (0.6-0.4)O x exhibit high interface quality and excellent photoelectrochemical power conversion. Furthermore, for scaled-up inkjet-printed electrodes and photoanodic electrodeposition of this composition on BiVO 4 we can confirm the discovery and the synthesis-independent interface improvement of (Fe-Ce)O x coatings on BiVO 4.« less

Photoelectrocatalytic oxidation of glucose at a ruthenium complex modified titanium dioxide electrode promoted by uric acid and ascorbic acid for photoelectrochemical fuel cells

NASA Astrophysics Data System (ADS)

Lu, Shuo-Jian; Ji, Shi-Bo; Liu, Jun-Chen; Li, Hong; Li, Wei-Shan

2015-01-01

The simultaneous presence of uric acid (UA) and ascorbic acid (AA) is first found to largely promote the photoelectrocatalytic oxidation of glucose (GLU) at an indium-tin oxide (ITO) or TiO2 nanoparticles/ITO electrode modified with [Ru(tatp)3]2+ (tatp = 1,4,8,9-tetra-aza-triphenylene) possessing good redox activity and nanoparticle size distribution. A well-defined electrocatalytic peak for GLU oxidation is shown at 0.265 V (vs. SCE) under approximate physiological conditions upon incorporation of UA and AA. The [Ru(tatp)3]2+/ITO electrode exhibits attractive amperometric oxidation responses towards GLU, UA and AA, while controlled potentiostatically at 0.3 V, 0.7 V and 1.0 V, respectively, indicating high sensitivity and excellent reproducibility. On basis of the photoelectrocatalysis of [Ru(tatp)3]2+/TiO2/ITO anode, a GLU concentration-dependent photoelectrochemical fuel cell vs. SCE is elaborately assembled. The proposed free-enzyme photoelectrochemical fuel cell employing 0.1 M GLU associated with 0.01 M UA and 0.01 M AA as fuel shows open-circuit photovoltage of 0.608 V, short-circuit photocurrent density of 124.5 μA cm-2 and maximum power density of 21.75 μW cm-2 at 0.455 V, fill factor of 0.32 and photoenergy conversion efficiency of 36.65%, respectively.

Surface modifications of chalcopyrite CuInS2 thin films for photochatodes in photoelectrochemical water splitting under sunlight irradiation

NASA Astrophysics Data System (ADS)

Gunawan; Haris, A.; Widiyandari, H.; Septina, W.; Ikeda, S.

2017-02-01

Copper chalcopyrite semiconductors include a wide range of compounds that are of interest for photoelectrochemical water splitting which enables them to be used as photochatodes for H2 generation. Among them, CuInS2 is one of the most important materials due to its optimum band gap energy for sunlight absorption. In the present study, we investigated the application of CuInS2 fabricated by electrodeposition as photochatodes for water splitting. Thin film of CuInS2 chalcopyrite was formed on Mo-coated glass substrate by stacked electrodeposition of copper and indium followed by sulfurization under H2S flow. The films worked as a H2 liberation electrode under cathodic polarization from a solution containing Na2SO4 after loading Pt deposits on the film. Introduction of an n-type CdS layer by chemical bath deposition on the CuInS2 surface before the Pt loading resulted appreciable improvements of H2 liberation efficiency and a higher photocurrent onset potential. Moreover, the use of In2S3 layer as an alternative n-type layer to the CdS significantly improved the H2 liberation performance: the CuInS2 film modified with In2S3 and Pt deposits worked as an efficient photocathode for photoelectrochemical water splitting.

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

Corbea, Javier Jesus Concepcion; Chen, Zoufeng; Jurss, Jonah Wesley

The present invention provides ruthenium or osmium complexes and their uses as a catalyst for catalytic water oxidation. Another aspect of the invention provides an electrode and photo-electrochemical cells for electrolysis of water molecules.

Nucleic Acid Immunity.

PubMed

Hartmann, G

2017-01-01

Organisms throughout biology need to maintain the integrity of their genome. From bacteria to vertebrates, life has established sophisticated mechanisms to detect and eliminate foreign genetic material or to restrict its function and replication. Tremendous progress has been made in the understanding of these mechanisms which keep foreign or unwanted nucleic acids from viruses or phages in check. Mechanisms reach from restriction-modification systems and CRISPR/Cas in bacteria and archaea to RNA interference and immune sensing of nucleic acids, altogether integral parts of a system which is now appreciated as nucleic acid immunity. With inherited receptors and acquired sequence information, nucleic acid immunity comprises innate and adaptive components. Effector functions include diverse nuclease systems, intrinsic activities to directly restrict the function of foreign nucleic acids (e.g., PKR, ADAR1, IFIT1), and extrinsic pathways to alert the immune system and to elicit cytotoxic immune responses. These effects act in concert to restrict viral replication and to eliminate virus-infected cells. The principles of nucleic acid immunity are highly relevant for human disease. Besides its essential contribution to antiviral defense and restriction of endogenous retroelements, dysregulation of nucleic acid immunity can also lead to erroneous detection and response to self nucleic acids then causing sterile inflammation and autoimmunity. Even mechanisms of nucleic acid immunity which are not established in vertebrates are relevant for human disease when they are present in pathogens such as bacteria, parasites, or helminths or in pathogen-transmitting organisms such as insects. This review aims to provide an overview of the diverse mechanisms of nucleic acid immunity which mostly have been looked at separately in the past and to integrate them under the framework nucleic acid immunity as a basic principle of life, the understanding of which has great potential to advance medicine. © 2017 Elsevier Inc. All rights reserved.

Universal nucleic acids sample preparation method for cells, spores and their mixture

DOEpatents

Bavykin, Sergei [Darien, IL

2011-01-18

The present invention relates to a method for extracting nucleic acids from biological samples. More specifically the invention relates to a universal method for extracting nucleic acids from unidentified biological samples. An advantage of the presently invented method is its ability to effectively and efficiently extract nucleic acids from a variety of different cell types including but not limited to prokaryotic or eukaryotic cells and/or recalcitrant organisms (i.e. spores). Unlike prior art methods which are focused on extracting nucleic acids from vegetative cell or spores, the present invention effectively extracts nucleic acids from spores, multiple cell types or mixtures thereof using a single method. Important that the invented method has demonstrated an ability to extract nucleic acids from spores and vegetative bacterial cells with similar levels effectiveness. The invented method employs a multi-step protocol which erodes the cell structure of the biological sample, isolates, labels, fragments nucleic acids and purifies labeled samples from the excess of dye.

Photoelectric performance of TiO2 nanotube array photoelectrodes sensitized with CdS0.54Se0.46 quantum dots

NASA Astrophysics Data System (ADS)

Gakhar, Ruchi; Smith, York R.; Misra, Mano; Chidambaram, Dev

2015-11-01

The photoelectrochemical performance of CdSSe quantum dots tethered to a framework of vertically oriented titania (TiO2) nanotubes was studied. The TiO2/CdSSe framework demonstrated improved charge transfer due to its unique band edge structure, thus validating the higher photocurrent generation. The composite film led to an 11-fold enhancement in comparison to the control TiO2 film, implying that the ternary quantum dots and the nanotubular structure of TiO2 work in tandem to promote charge separation and favorably impact photoelectrochemical performance. Further, the results also suggest that structural and optoelectronic properties of TiO2 films are significantly affected by the thicknesses of the CdSSe layer.

Harvesting Hydrogen Gas from Air Pollutants with an Unbiased Gas Phase Photoelectrochemical Cell.

PubMed

Verbruggen, Sammy W; Van Hal, Myrthe; Bosserez, Tom; Rongé, Jan; Hauchecorne, Birger; Martens, Johan A; Lenaerts, Silvia

2017-04-10

The concept of an all-gas-phase photoelectrochemical (PEC) cell producing hydrogen gas from volatile organic contaminated gas and light is presented. Without applying any external bias, organic contaminants are degraded and hydrogen gas is produced in separate electrode compartments. The system works most efficiently with organic pollutants in inert carrier gas. In the presence of oxygen, the cell performs less efficiently but still significant photocurrents are generated, showing the cell can be run on organic contaminated air. The purpose of this study is to demonstrate new application opportunities of PEC technology and to encourage further advancement toward PEC remediation of air pollution with the attractive feature of simultaneous energy recovery and pollution abatement. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Electrochemically hydrogenated TiO2 nanotubes with improved photoelectrochemical water splitting performance

PubMed Central

2013-01-01

One-dimensional anodic titanium oxide (ATO) nanotube arrays hold great potential as photoanode for photoelectrochemical (PEC) water splitting. In this work, we report a facile and eco-friendly electrochemical hydrogenation method to modify the electronic and PEC properties of ATO nanotube films. The hydrogenated ATO (ATO-H) electrodes present a significantly improved photocurrent of 0.65 mA/cm2 in comparison with that of pristine ATO nanotubes (0.29 mA/cm2) recorded under air mass 1.5 global illumination. The incident photon-to-current efficiency measurement suggests that the enhanced photocurrent of ATO-H nanotubes is mainly ascribed to the improved photoactivity in the UV region. We propose that the electrochemical hydrogenation induced surface oxygen vacancies contribute to the substantially enhanced electrical conductivity and photoactivity. PMID:24047205

Facile fabrication of Si-doped TiO2 nanotubes photoanode for enhanced photoelectrochemical hydrogen generation

NASA Astrophysics Data System (ADS)

Dong, Zhenbiao; Ding, Dongyan; Li, Ting; Ning, Congqin

2018-04-01

Photoelectrochemical (PEC) water splitting based doping modified one dimensional (1D) titanium dioxide (TiO2) nanostructures provide an efficient method for hydrogen generation. Here we first successfully fabricated 1D Si-doped TiO2 (Ti-Si-O) nanotube arrays through anodizing Ti-Si alloys with different Si amount, and reported the PEC properties for water splitting. The Ti-Si-O nanotube arrays fabricated on Ti-5 wt.% Si alloy and annealed at 600 °C possess higher PEC activity, yielding a higher photocurrent density of 0.83 mA/cm2 at 0 V vs. Ag/AgCl. The maximum photoconversion efficiency was 0.54%, which was 2.7 times the photoconversion efficiency of undoped TiO2.

In situ electrochemical and photo-electrochemical generation of the fenton reagent: a potentially important new water treatment technology.

PubMed

Peralta-Hernández, J M; Meas-Vong, Yunny; Rodríguez, Francisco J; Chapman, Thomas W; Maldonado, Manuel I; Godínez, Luis A

2006-05-01

In this work, the design and construction of an annular tube reactor for the electrochemical and photo-electrochemical in situ generation of H2O2 are described. By cathodic reduction of dissolved oxygen and the coupled oxidation of water at a UV-illuminated nanocrystalline-TiO2 semiconductor anode, it was found that the electrochemically generated H2O2 can be employed to readily oxidize the model compound Direct Yellow-52 in dilute acidic solution at high rates in the presence of small quantities of dissolved iron(II). Although, the model organic compound is chemically stable under UV radiation, its electrochemical oxidation rate increases substantially when the semiconductor anode is illuminated as compared to the same processes carried out in the dark.

Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells

PubMed Central

Swierk, John R.; Méndez-Hernández, Dalvin D.; McCool, Nicholas S.; Liddell, Paul; Terazono, Yuichi; Pahk, Ian; Tomlin, John J.; Oster, Nolan V.; Moore, Thomas A.; Moore, Ana L.; Gust, Devens; Mallouk, Thomas E.

2015-01-01

Solar fuel generation requires the efficient capture and conversion of visible light. In both natural and artificial systems, molecular sensitizers can be tuned to capture, convert, and transfer visible light energy. We demonstrate that a series of metal-free porphyrins can drive photoelectrochemical water splitting under broadband and red light (λ > 590 nm) illumination in a dye-sensitized TiO2 solar cell. We report the synthesis, spectral, and electrochemical properties of the sensitizers. Despite slow recombination of photoinjected electrons with oxidized porphyrins, photocurrents are low because of low injection yields and slow electron self-exchange between oxidized porphyrins. The free-base porphyrins are stable under conditions of water photoelectrolysis and in some cases photovoltages in excess of 1 V are observed. PMID:25583488

InP nanopore arrays for photoelectrochemical hydrogen generation.

PubMed

Li, Qiang; Zheng, Maojun; Zhang, Bin; Zhu, Changqing; Wang, Faze; Song, Jingnan; Zhong, Miao; Ma, Li; Shen, Wenzhong

2016-02-19

We report a facile and large-scale fabrication of highly ordered one-dimensional (1D) indium phosphide (InP) nanopore arrays (NPs) and their application as photoelectrodes for photoelectrochemical (PEC) hydrogen production. These InP NPs exhibit superior PEC performance due to their excellent light-trapping characteristics, high-quality 1D conducting channels and large surface areas. The photocurrent density of optimized InP NPs is 8.9 times higher than that of planar counterpart at an applied potential of +0.3 V versus RHE under AM 1.5G illumination (100 mW cm(-2)). In addition, the onset potential of InP NPs exhibits 105 mV of cathodic shift relative to planar control. The superior performance of the nanoporous samples is further explained by Mott-Schottky and electrochemical impedance spectroscopy ananlysis.

Real-time assays with molecular beacons and other fluorescent nucleic acid hybridization probes.

PubMed

Marras, Salvatore A E; Tyagi, Sanjay; Kramer, Fred Russell

2006-01-01

A number of formats for nucleic acid hybridization have been developed to identify DNA and RNA sequences that are involved in cellular processes and that aid in the diagnosis of genetic and infectious diseases. The introduction of hybridization probes with interactive fluorophore pairs has enabled the development of homogeneous hybridization assays for the direct identification of nucleic acids. A change in the fluorescence of these probes indicates the presence of a target nucleic acid, and there is no need to separate unbound probes from hybridized probes. The advantages of homogeneous hybridization assays are their speed and simplicity. In addition, homogeneous assays can be combined with nucleic acid amplification, enabling the detection of rare target nucleic acids. These assays can be followed in real time, providing quantitative determination of target nucleic acids over a broad range of concentrations.

Applications of synchrotron-based spectroscopic techniques in studying nucleic acids and nucleic acid-functionalized nanomaterials

PubMed Central

Wu, Peiwen; Yu, Yang; McGhee, Claire E.; Tan, Li Huey

2014-01-01

In this review, we summarize recent progresses in the application of synchrotron-based spectroscopic techniques for nucleic acid research that takes advantage of high-flux and high-brilliance electromagnetic radiation from synchrotron sources. The first section of the review focuses on the characterization of the structure and folding processes of nucleic acids using different types of synchrotron-based spectroscopies, such as X-ray absorption spectroscopy, X-ray emission spectroscopy, X-ray photoelectron spectroscopy, synchrotron radiation circular dichroism, X-ray footprinting and small-angle X-ray scattering. In the second section, the characterization of nucleic acid-based nanostructures, nucleic acid-functionalized nanomaterials and nucleic acid-lipid interactions using these spectroscopic techniques is summarized. Insights gained from these studies are described and future directions of this field are also discussed. PMID:25205057

Applications of synchrotron-based spectroscopic techniques in studying nucleic acids and nucleic acid-functionalized nanomaterials

DOE PAGES

Wu, Peiwen; Yu, Yang; McGhee, Claire E.; ...

2014-09-10

In this paper, we summarize recent progress in the application of synchrotron-based spectroscopic techniques for nucleic acid research that takes advantage of high-flux and high-brilliance electromagnetic radiation from synchrotron sources. The first section of the review focuses on the characterization of the structure and folding processes of nucleic acids using different types of synchrotron-based spectroscopies, such as X-ray absorption spectroscopy, X-ray emission spectroscopy, X-ray photoelectron spectroscopy, synchrotron radiation circular dichroism, X-ray footprinting and small-angle X-ray scattering. In the second section, the characterization of nucleic acid-based nanostructures, nucleic acid-functionalized nanomaterials and nucleic acid-lipid interactions using these spectroscopic techniques is summarized. Insightsmore » gained from these studies are described and future directions of this field are also discussed.« less

Method for nucleic acid isolation using supercritical fluids

DOEpatents

Nivens, David E.; Applegate, Bruce M.

1999-01-01

A method for detecting the presence of a microorganism in an environmental sample involves contacting the sample with a supercritical fluid to isolate nucleic acid from the microorganism, then detecting the presence of a particular sequence within the isolated nucleic acid. The nucleic acid may optionally be subjected to further purification.

21 CFR 866.3980 - Respiratory viral panel multiplex nucleic acid assay.

Code of Federal Regulations, 2010 CFR

2010-04-01

... 21 Food and Drugs 8 2010-04-01 2010-04-01 false Respiratory viral panel multiplex nucleic acid... § 866.3980 Respiratory viral panel multiplex nucleic acid assay. (a) Identification. A respiratory viral... simultaneously detect and identify multiple viral nucleic acids extracted from human respiratory specimens or...

21 CFR 866.3980 - Respiratory viral panel multiplex nucleic acid assay.

Code of Federal Regulations, 2014 CFR

2014-04-01

... 21 Food and Drugs 8 2014-04-01 2014-04-01 false Respiratory viral panel multiplex nucleic acid... § 866.3980 Respiratory viral panel multiplex nucleic acid assay. (a) Identification. A respiratory viral... simultaneously detect and identify multiple viral nucleic acids extracted from human respiratory specimens or...

21 CFR 866.3980 - Respiratory viral panel multiplex nucleic acid assay.

Code of Federal Regulations, 2011 CFR

2011-04-01

... 21 Food and Drugs 8 2011-04-01 2011-04-01 false Respiratory viral panel multiplex nucleic acid... § 866.3980 Respiratory viral panel multiplex nucleic acid assay. (a) Identification. A respiratory viral... simultaneously detect and identify multiple viral nucleic acids extracted from human respiratory specimens or...

21 CFR 866.3980 - Respiratory viral panel multiplex nucleic acid assay.

Code of Federal Regulations, 2013 CFR

2013-04-01

... 21 Food and Drugs 8 2013-04-01 2013-04-01 false Respiratory viral panel multiplex nucleic acid... § 866.3980 Respiratory viral panel multiplex nucleic acid assay. (a) Identification. A respiratory viral... simultaneously detect and identify multiple viral nucleic acids extracted from human respiratory specimens or...

21 CFR 866.3980 - Respiratory viral panel multiplex nucleic acid assay.

Code of Federal Regulations, 2012 CFR

2012-04-01

... 21 Food and Drugs 8 2012-04-01 2012-04-01 false Respiratory viral panel multiplex nucleic acid... § 866.3980 Respiratory viral panel multiplex nucleic acid assay. (a) Identification. A respiratory viral... simultaneously detect and identify multiple viral nucleic acids extracted from human respiratory specimens or...

Nanoplasmonic molecular ruler for nuclease activity and DNA footprinting

DOEpatents

Chen, Fanqing Frank; Liu, Gang L; Lee, Luke P

2013-10-29

This invention provides a nanoplasmonic molecular ruler, which can perform label-free and real-time monitoring of nucleic acid (e.g., DNA) length changes and perform nucleic acid footprinting. In various embodiments the ruler comprises a nucleic acid attached to a nanoparticle, such that changes in the nucleic acid length are detectable using surface plasmon resonance. The nanoplasmonic ruler provides a fast and convenient platform for mapping nucleic acid-protein interactions, for nuclease activity monitoring, and for other footprinting related methods.

Understanding Nucleic Acid–Ion Interactions

PubMed Central

Lipfert, Jan; Doniach, Sebastian; Das, Rhiju; Herschlag, Daniel

2015-01-01

Ions surround nucleic acids in what is referred to as an ion atmosphere. As a result, the folding and dynamics of RNA and DNA and their complexes with proteins and with each other cannot be understood without a reasonably sophisticated appreciation of these ions’ electrostatic interactions. However, the underlying behavior of the ion atmosphere follows physical rules that are distinct from the rules of site binding that biochemists are most familiar and comfortable with. The main goal of this review is to familiarize nucleic acid experimentalists with the physical concepts that underlie nucleic acid–ion interactions. Throughout, we provide practical strategies for interpreting and analyzing nucleic acid experiments that avoid pitfalls from oversimplified or incorrect models. We briefly review the status of theories that predict or simulate nucleic acid–ion interactions and experiments that test these theories. Finally, we describe opportunities for going beyond phenomenological fits to a next-generation, truly predictive understanding of nucleic acid–ion interactions. PMID:24606136

Lipid and polymeric carrier-mediated nucleic acid delivery

PubMed Central

Zhu, Lin; Mahato, Ram I

2010-01-01

Importance of the field Nucleic acids such as plasmid DNA, antisense oligonucleotide, and RNA interference (RNAi) molecules, have a great potential to be used as therapeutics for the treatment of various genetic and acquired diseases. To design a successful nucleic acid delivery system, the pharmacological effect of nucleic acids, the physiological condition of the subjects or sites, and the physicochemical properties of nucleic acid and carriers have to be thoroughly examined. Areas covered in this review The commonly used lipids, polymers and corresponding delivery systems are reviewed in terms of their characteristics, applications, advantages and limitations. What the reader will gain This article aims to provide an overview of biological barriers and strategies to overcome these barriers by properly designing effective synthetic carriers for nucleic acid delivery. Take home message A thorough understanding of biological barriers and the structure–activity relationship of lipid and polymeric carriers is the key for effective nucleic acid therapy. PMID:20836625

Electrophoretic Mobility Shift Assay (EMSA) for Detecting Protein-Nucleic Acid Interactions

PubMed Central

Hellman, Lance M.; Fried, Michael G.

2009-01-01

The gel electrophoresis mobility shift assay (EMSA) is used to detect protein complexes with nucleic acids. It is the core technology underlying a wide range of qualitative and quantitative analyses for the characterization of interacting systems. In the classical assay, solutions of protein and nucleic acid are combined and the resulting mixtures are subjected to electrophoresis under native conditions through polyacrylamide or agarose gel. After electrophoresis, the distribution of species containing nucleic acid is determined, usually by autoradiography of 32P-labeled nucleic acid. In general, protein-nucleic acid complexes migrate more slowly than the corresponding free nucleic acid. In this article, we identify the most important factors that determine the stabilities and electrophoretic mobilities of complexes under assay conditions. A representative protocol is provided and commonly used variants are discussed. Expected outcomes are briefly described. References to extensions of the method and a troubleshooting guide are provided. PMID:17703195

Solid phase sequencing of biopolymers

DOEpatents

Cantor, Charles; Koster, Hubert

2010-09-28

This invention relates to methods for detecting and sequencing target nucleic acid sequences, to mass modified nucleic acid probes and arrays of probes useful in these methods, and to kits and systems which contain these probes. Useful methods involve hybridizing the nucleic acids or nucleic acids which represent complementary or homologous sequences of the target to an array of nucleic acid probes. These probes comprise a single-stranded portion, an optional double-stranded portion and a variable sequence within the single-stranded portion. The molecular weights of the hybridized nucleic acids of the set can be determined by mass spectroscopy, and the sequence of the target determined from the molecular weights of the fragments. Nucleic acids whose sequences can be determined include DNA or RNA in biological samples such as patient biopsies and environmental samples. Probes may be fixed to a solid support such as a hybridization chip to facilitate automated molecular weight analysis and identification of the target sequence.

Method for nucleic acid isolation using supercritical fluids

DOEpatents

Nivens, D.E.; Applegate, B.M.

1999-07-13

A method is disclosed for detecting the presence of a microorganism in an environmental sample involves contacting the sample with a supercritical fluid to isolate nucleic acid from the microorganism, then detecting the presence of a particular sequence within the isolated nucleic acid. The nucleic acid may optionally be subjected to further purification. 4 figs.

Enhanced Photoelectrochemical Behavior of H-TiO2 Nanorods Hydrogenated by Controlled and Local Rapid Thermal Annealing

NASA Astrophysics Data System (ADS)

Wang, Xiaodan; Estradé, Sonia; Lin, Yuanjing; Yu, Feng; Lopez-Conesa, Lluis; Zhou, Hao; Gurram, Sanjeev Kumar; Peiró, Francesca; Fan, Zhiyong; Shen, Hao; Schaefer, Lothar; Braeuer, Guenter; Waag, Andreas

2017-05-01

Recently, colored H-doped TiO2 (H-TiO2) has demonstrated enhanced photoelectrochemical (PEC) performance due to its unique crystalline core—disordered shell nanostructures and consequent enhanced conduction behaviors between the core-shell homo-interfaces. Although various hydrogenation approaches to obtain H-TiO2 have been developed, such as high temperature hydrogen furnace tube annealing, high pressure hydrogen annealing, hydrogen-plasma assisted reaction, aluminum reduction and electrochemical reduction etc., there is still a lack of a hydrogenation approach in a controlled manner where all processing parameters (temperature, time and hydrogen flux) were precisely controlled in order to improve the PEC performance of H-TiO2 and understand the physical insight of enhanced PEC performance. Here, we report for the first time a controlled and local rapid thermal annealing (RTA) approach to prepare hydrogenated core-shell H-TiO2 nanorods grown on F:SnO2 (FTO) substrate in order to address the degradation issue of FTO in the typical TiO2 nanorods/FTO system observed in the conventional non-RTA treated approaches. Without the FTO degradation in the RTA approach, we systematically studied the intrinsic relationship between the annealing temperature, structural, optical, and photoelectrochemical properties in order to understand the role of the disordered shell on the improved photoelectrochemical behavior of H-TiO2 nanorods. Our investigation shows that the improvement of PEC performance could be attributed to (i) band gap narrowing from 3.0 to 2.9 eV; (ii) improved optical absorption in the visible range induced by the three-dimensional (3D) morphology and rough surface of the disordered shell; (iii) increased proper donor density; (iv) enhanced electron-hole separation and injection efficiency due to the formation of disordered shell after hydrogenation. The RTA approach developed here can be used as a suitable hydrogenation process for TiO2 nanorods/FTO system for important applications such as photocatalysis, hydrogen generation from water splitting and solar energy conversion.

Enhanced Photoelectrochemical Behavior of H-TiO2 Nanorods Hydrogenated by Controlled and Local Rapid Thermal Annealing.

PubMed

Wang, Xiaodan; Estradé, Sonia; Lin, Yuanjing; Yu, Feng; Lopez-Conesa, Lluis; Zhou, Hao; Gurram, Sanjeev Kumar; Peiró, Francesca; Fan, Zhiyong; Shen, Hao; Schaefer, Lothar; Braeuer, Guenter; Waag, Andreas

2017-12-01

Recently, colored H-doped TiO 2 (H-TiO 2 ) has demonstrated enhanced photoelectrochemical (PEC) performance due to its unique crystalline core-disordered shell nanostructures and consequent enhanced conduction behaviors between the core-shell homo-interfaces. Although various hydrogenation approaches to obtain H-TiO 2 have been developed, such as high temperature hydrogen furnace tube annealing, high pressure hydrogen annealing, hydrogen-plasma assisted reaction, aluminum reduction and electrochemical reduction etc., there is still a lack of a hydrogenation approach in a controlled manner where all processing parameters (temperature, time and hydrogen flux) were precisely controlled in order to improve the PEC performance of H-TiO 2 and understand the physical insight of enhanced PEC performance. Here, we report for the first time a controlled and local rapid thermal annealing (RTA) approach to prepare hydrogenated core-shell H-TiO 2 nanorods grown on F:SnO 2 (FTO) substrate in order to address the degradation issue of FTO in the typical TiO 2 nanorods/FTO system observed in the conventional non-RTA treated approaches. Without the FTO degradation in the RTA approach, we systematically studied the intrinsic relationship between the annealing temperature, structural, optical, and photoelectrochemical properties in order to understand the role of the disordered shell on the improved photoelectrochemical behavior of H-TiO 2 nanorods. Our investigation shows that the improvement of PEC performance could be attributed to (i) band gap narrowing from 3.0 to 2.9 eV; (ii) improved optical absorption in the visible range induced by the three-dimensional (3D) morphology and rough surface of the disordered shell; (iii) increased proper donor density; (iv) enhanced electron-hole separation and injection efficiency due to the formation of disordered shell after hydrogenation. The RTA approach developed here can be used as a suitable hydrogenation process for TiO 2 nanorods/FTO system for important applications such as photocatalysis, hydrogen generation from water splitting and solar energy conversion.

Refinement of Generalized Born Implicit Solvation Parameters for Nucleic Acids and their Complexes with Proteins

PubMed Central

Nguyen, Hai; Pérez, Alberto; Bermeo, Sherry; Simmerling, Carlos

2016-01-01

The Generalized Born (GB) implicit solvent model has undergone significant improvements in accuracy for modeling of proteins and small molecules. However, GB still remains a less widely explored option for nucleic acid simulations, in part because fast GB models are often unable to maintain stable nucleic acid structures, or they introduce structural bias in proteins, leading to difficulty in application of GB models in simulations of protein-nucleic acid complexes. Recently, GB-neck2 was developed to improve the behavior of protein simulations. In an effort to create a more accurate model for nucleic acids, a similar procedure to the development of GB-neck2 is described here for nucleic acids. The resulting parameter set significantly reduces absolute and relative energy error relative to Poisson Boltzmann for both nucleic acids and nucleic acid-protein complexes, when compared to its predecessor GB-neck model. This improvement in solvation energy calculation translates to increased structural stability for simulations of DNA and RNA duplexes, quadruplexes, and protein-nucleic acid complexes. The GB-neck2 model also enables successful folding of small DNA and RNA hairpins to near native structures as determined from comparison with experiment. The functional form and all required parameters are provided here and also implemented in the AMBER software. PMID:26574454

Cellular nucleic acid binding protein binds G-rich single-stranded nucleic acids and may function as a nucleic acid chaperone.

PubMed

Armas, Pablo; Nasif, Sofía; Calcaterra, Nora B

2008-02-15

Cellular nucleic acid binding protein (CNBP) is a small single-stranded nucleic acid binding protein made of seven Zn knuckles and an Arg-Gly rich box. CNBP is strikingly conserved among vertebrates and was reported to play broad-spectrum functions in eukaryotic cells biology. Neither its biological function nor its mechanisms of action were elucidated yet. The main goal of this work was to gain further insights into the CNBP biochemical and molecular features. We studied Bufo arenarum CNBP (bCNBP) binding to single-stranded nucleic acid probes representing the main reported CNBP putative targets. We report that, although bCNBP is able to bind RNA and single-stranded DNA (ssDNA) probes in vitro, it binds RNA as a preformed dimer whereas both monomer and dimer are able to bind to ssDNA. A systematic analysis of variant probes shows that the preferred bCNBP targets contain unpaired guanosine-rich stretches. These data expand the knowledge about CNBP binding stoichiometry and begins to dissect the main features of CNBP nucleic acid targets. Besides, we show that bCNBP presents a highly disordered predicted structure and promotes the annealing and melting of nucleic acids in vitro. These features are typical of proteins that function as nucleic acid chaperones. Based on these data, we propose that CNBP may function as a nucleic acid chaperone through binding, remodeling, and stabilizing nucleic acids secondary structures. This novel CNBP biochemical activity broadens the field of study about its biological function and may be the basis to understand the diverse ways in which CNBP controls gene expression. Copyright 2007 Wiley-Liss, Inc.

Note: optical optimization for ultrasensitive photon mapping with submolecular resolution by scanning tunneling microscope induced luminescence.

PubMed

Chen, L G; Zhang, C; Zhang, R; Zhang, X L; Dong, Z C

2013-06-01

We report the development of a custom scanning tunneling microscope equipped with photon collection and detection systems. The optical optimization includes the comprehensive design of aspherical lens for light collimation and condensing, the sophisticated piezo stages for in situ lens adjustment inside ultrahigh vacuum, and the fiber-free coupling of collected photons directly onto the ultrasensitive single-photon detectors. We also demonstrate submolecular photon mapping for the molecular islands of porphyrin on Ag(111) under small tunneling currents down to 10 pA and short exposure time down to 1.2 ms/pixel. A high quantum efficiency up to 10(-2) was also observed.

UltraSensitive Mycotoxin Detection by STING Sensors

PubMed Central

Actis, Paolo; Jejelowo, Olufisayo; Pourmand, Nader

2010-01-01

Signal Transduction by Ion Nano Gating (STING) technology is a label-free biosensor capable of identifying DNA and proteins. Based on a functionalized quartz nanopipette, the STING sensor includes specific recognition elements for analyte discrimination based on size, shape and charge density. A key feature of this technology is that it doesn't require any nanofabrication facility; each nanopipette can be easily, reproducibly, and inexpensively fabricated and tailored at the bench, thus reducing the cost and the turnaround time. Here, we show that STING sensors are capable of the ultrasensitive detection of HT-2 toxin with a detection limit of 100 fg/ml and compare the STING capabilities with respect to conventional sandwich assay techniques. PMID:20829024

Design of an ultrasensitive SPR biosensor based on a graphene-MoS2 hybrid structure with a MgF2 prism.

PubMed

Feng, Yuncai; Liu, Youwen; Teng, Jinghua

2018-05-10

We propose, to the best of our knowledge, a new configuration of a biosensor based on the graphene-MoS 2 hybrid structure by adopting the lower refractive index MgF 2 prism in order to improve the sensitivity and the figure of merit (FOM). We can obtain an ultrasensitive sensor with values of sensitivity and FOM as high as 540.8°/RIU and 145/RIU, respectively, by modulating the parameters in the configuration and comparatively choosing a different absentee layer material. The proposed structure is applicable in the realization of an integrated device for the surface plasmon resonance biosensor.

Artificial mismatch hybridization

DOEpatents

Guo, Zhen; Smith, Lloyd M.

1998-01-01

An improved nucleic acid hybridization process is provided which employs a modified oligonucleotide and improves the ability to discriminate a control nucleic acid target from a variant nucleic acid target containing a sequence variation. The modified probe contains at least one artificial mismatch relative to the control nucleic acid target in addition to any mismatch(es) arising from the sequence variation. The invention has direct and advantageous application to numerous existing hybridization methods, including, applications that employ, for example, the Polymerase Chain Reaction, allele-specific nucleic acid sequencing methods, and diagnostic hybridization methods.

Transgenic cells with increased plastoquinone levels and methods of use

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

Sayre, Richard T.; Subramanian, Sowmya; Cahoon, Edgar

Disclosed herein are transgenic cells expressing a heterologous nucleic acid encoding a prephenate dehydrogenase (PDH) protein, a heterologous nucleic acid encoding a homogentisate solanesyl transferase (HST) protein, a heterologous nucleic acid encoding a deoxyxylulose phosphate synthase (DXS) protein, or a combination of two or more thereof. In particular examples, the disclosed transgenic cells have increased plastoquinone levels. Also disclosed are methods of increasing cell growth rates or production of biomass by cultivating transgenic cells expressing a heterologous nucleic acid encoding a PDH protein, a heterologous nucleic acid encoding an HST protein, a heterologous nucleic acid encoding a DXS protein, ormore » a combination of two or more thereof under conditions sufficient to produce cell growth or biomass.« less

A novel ultrasensitive carboxymethyl chitosan-quantum dot-based fluorescence "turn on-off" nanosensor for lysozyme detection.

PubMed

Song, Yu; Li, Yang; Liu, Ziping; Liu, Linlin; Wang, Xinyan; Su, Xingguang; Ma, Qiang

2014-11-15

In this work, we developed an ultrasensitive "turn on-off" fluorescence nanosensor for lysozyme (Lyz) detection. The novel nanosensor was constructed with the carboxymethyl chitosan modified CdTe quantum dots (CMCS-QDs). Firstly, the CMCS-QDs were fabricated via the electrostatic interaction between amino groups in CMCS polymeric chains and carboxyl groups on the surface of QDs. In the fluorescence "turn-on" step, the strong binding ability between Zn(2+) and CMCS on the surface of QDs can enhance the photoluminescence intensity (PL) of QDs. In the following fluorescence "turn-off" step, the N-acetyl-glucosamine (NAG) section along the CMCS chains was hydrolyzed by Lyz. As a result, Zn(2+) was released from the surface of QDs, and the Lyz-QDs complexes were formed to quench the QDs PL. Under the optimal conditions, there was a good linear relationship between the PL of QDs and the Lyz concentration (0.1-1.2 ng/mL) with the detection limit of 0.031 ng/mL. The developed method was ultrasensitive, highly selective and fast. It has been successfully employed in the detection of Lyz in the serum with satisfactory results. Copyright © 2014 Elsevier B.V. All rights reserved.

High Surface Area MoS 2/Graphene Hybrid Aerogel for Ultrasensitive NO 2 Detection

DOE PAGES

Long, Hu; Harley-Trochimczyk, Anna; Pham, Thang; ...

2016-05-23

A MoS 2/graphene hybrid aerogel synthesized with two-dimensional MoS 2 sheets coating a high surface area graphene aerogel scaffold is characterized and used for ultrasensitive NO 2 detection. The combination of graphene and MoS 2 leads to improved sensing properties with the graphene scaffold providing high specific surface area and high electrical and thermal conductivity and the single to few-layer MoS2 sheets providing high sensitivity and selectivity to NO 2. The hybrid aerogel is integrated onto a low-power microheater platform to probe the gas sensing performance. At room temperature, the sensor exhibits an ultralow detection limit of 50 ppb NOmore » 2. By heating the material to 200 °C, the response and recovery times to reach 90% of the final signal decrease to <1 min, while retaining the low detection limit. The MoS 2/graphene hybrid also shows good selectivity for NO 2 against H 2 and CO, especially when compared to bare graphene aerogel. The unique structure of the hybrid aerogel is responsible for the ultrasensitive, selective, and fast NO 2 sensing. The improved sensing performance of this hybrid aerogel also suggests the possibility of other 2D material combinations for further sensing applications.« less

Ultrahigh-Sensitivity Piezoresistive Pressure Sensors for Detection of Tiny Pressure.

PubMed

Li, Hongwei; Wu, Kunjie; Xu, Zeyang; Wang, Zhongwu; Meng, Yancheng; Li, Liqiang

2018-06-20

High-sensitivity pressure sensors are crucial for the ultrasensitive touch technology and E-skin, especially at the tiny-pressure range below 100 Pa. However, it is highly challenging to substantially promote sensitivity beyond the current level at several to 200 kPa -1 and to improve the detection limit lower than 0.1 Pa, which is significant for the development of pressure sensors toward ultrasensitive and highly precise detection. Here, we develop an efficient strategy to greatly improve the sensitivity near to 2000 kPa -1 using short-channel coplanar device structure and sharp microstructure, which is systematically proposed for the first time and rationalized by the mathematic calculation and analysis. Significantly, benefiting from the ultrahigh sensitivity, the detection limit is improved to be as small as 0.075 Pa. The sensitivity and detection limit are both superior to the current levels and far surpass the function of human skin. Furthermore, the sensor shows fast response time (50 μs), excellent reproducibility and stability, and low power consumption. Remarkably, the sensor shows excellent detection capacity in the tiny-pressure range, including light-emitting diode switching with a pressure of 7 Pa, ringtone (2-20 Pa) recognition, and ultrasensitive (0.1 Pa) electronic glove. This work represents a performance and strategic progress in the field of pressure sensing.

Ultrasensitive and Highly Stable Resistive Pressure Sensors with Biomaterial-Incorporated Interfacial Layers for Wearable Health-Monitoring and Human-Machine Interfaces.

PubMed

Chang, Hochan; Kim, Sungwoong; Jin, Sumin; Lee, Seung-Woo; Yang, Gil-Tae; Lee, Ki-Young; Yi, Hyunjung

2018-01-10

Flexible piezoresistive sensors have huge potential for health monitoring, human-machine interfaces, prosthetic limbs, and intelligent robotics. A variety of nanomaterials and structural schemes have been proposed for realizing ultrasensitive flexible piezoresistive sensors. However, despite the success of recent efforts, high sensitivity within narrower pressure ranges and/or the challenging adhesion and stability issues still potentially limit their broad applications. Herein, we introduce a biomaterial-based scheme for the development of flexible pressure sensors that are ultrasensitive (resistance change by 5 orders) over a broad pressure range of 0.1-100 kPa, promptly responsive (20 ms), and yet highly stable. We show that employing biomaterial-incorporated conductive networks of single-walled carbon nanotubes as interfacial layers of contact-based resistive pressure sensors significantly enhances piezoresistive response via effective modulation of the interlayer resistance and provides stable interfaces for the pressure sensors. The developed flexible sensor is capable of real-time monitoring of wrist pulse waves under external medium pressure levels and providing pressure profiles applied by a thumb and a forefinger during object manipulation at a low voltage (1 V) and power consumption (<12 μW). This work provides a new insight into the material candidates and approaches for the development of wearable health-monitoring and human-machine interfaces.

Ultra-sensitive and selective Hg{sup 2+} detection based on fluorescent carbon dots

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

Liu, Ruihua; Li, Haitao; Kong, Weiqian

2013-07-15

Graphical abstract: Fluorescent carbon dots were efficiently synthesized by one-step sodium hydroxide-assisted reflux method from PEG and demonstrated to show high selectivity toward Hg2+ ions detection. - Highlights: • FCDs were synthesized by one-step sodium hydroxide-assisted reflux method from PEG. • The FCDs emit blue photoluminescence and have upconversion fluorescent property. • The FCDs show ultra-sensitive detective ability for Hg{sup 2+} ions. - Abstract: Fluorescent carbon dots (FCDs) were efficiently synthesized by one-step sodium hydroxide-assisted reflux method from poly(ethylene glycol) (PEG). The obtained FCDs exhibit excellent water-solubility and high stability. Under the UV irradiation, the FCDs could emit bright bluemore » photoluminescence, and also they were found to show excellent up-conversion fluorescence. It was further demonstrated that such FCDs can serve as effective fluorescent sensing platform for Hg{sup 2+} ions detection with ultra-sensitivity and selectivity. The sensing system achieved a limit of detection as low as 1 fM, which is much lower than all the previous reported sensing systems for Hg{sup 2+} ions detection. This FCDs sensing system has been successfully applied for the analysis of Hg{sup 2+} ions in water samples from river, lake, and tap water, showing good practical feasibility.« less

Efficient tungsten oxide/bismuth oxyiodide core/shell photoanode for photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Ma, Haipeng; Zhang, Jing; Liu, Zhifeng

2017-11-01

The novel WO3 nanorods (NRs)/BiOI core/shell structure composite is used as an efficient photoanode applied in photoelectrochemical (PEC) water splitting for the first time. It is synthesized via facile hydrothermal method and, successive ionic layer adsorption and reaction (SILAR) process. This facile synthesis route can achieve uniform WO3/BiOI core/shell composite nanostructures and obtain varied BiOI morphologies simultaneously. The WO3 NRs/BiOI-20 composite exhibits enhanced PEC activity compared to pristine WO3 with a photocurrent density of 0.79 mA cm-2 measured at 0.8 V vs. RHE under AM 1.5G. This excellent performance benefits from the broader absorption spectrum and suppressed electron-hole recombination. This novel core/shell composite may provide insight in developing more efficient solar driven photoelectrodes.

Hyperbranched TiO2-CdS nano-heterostructures for highly efficient photoelectrochemical photoanodes.

PubMed

Mezzetti, Alessandro; Balandeh, Mehrdad; Luo, Jingshan; Bellani, Sebastiano; Tacca, Alessandra; Divitini, Giorgio; Cheng, Chuanwei; Ducati, Caterina; Meda, Laura; Fan, Hongjin; Di Fonzo, Fabio

2018-08-17

Quasi-1D-hyperbranched TiO 2 nanostructures are grown via pulsed laser deposition and sensitized with thin layers of CdS to act as a highly efficient photoelectrochemical photoanode. The device properties are systematically investigated by optimizing the height of TiO 2 scaffold structure and thickness of the CdS sensitizing layer, achieving photocurrent values up to 6.6 mA cm -2 and reaching saturation with applied biases as low as 0.35 V RHE . The high internal conversion efficiency of these devices is to be found in the efficient charge generation and injection of the thin CdS photoactive film and in the enhanced charge transport properties of the hyperbranched TiO 2 scaffold. Hence, the proposed device represents a promising architecture for heterostructures capable of achieving high solar-to-hydrogen efficiency.

Photoelectrochemical hydrogen production from biomass derivatives and water.

PubMed

Lu, Xihong; Xie, Shilei; Yang, Hao; Tong, Yexiang; Ji, Hongbing

2014-11-21

Hydrogen, a clean energy carrier with high energy capacity, is a very promising candidate as a primary energy source for the future. Photoelectrochemical (PEC) hydrogen production from renewable biomass derivatives and water is one of the most promising approaches to producing green chemical fuel. Compared to water splitting, hydrogen production from renewable biomass derivatives and water through a PEC process is more efficient from the viewpoint of thermodynamics. Additionally, the carbon dioxide formed can be re-transformed into carbohydrates via photosynthesis in plants. In this review, we focus on the development of photoanodes and systems for PEC hydrogen production from water and renewable biomass derivatives, such as methanol, ethanol, glycerol and sugars. We also discuss the future challenges and opportunities for the design of the state-of-the-art photoanodes and PEC systems for hydrogen production from biomass derivatives and water.

Band edge engineering of oxide photoanodes for photoelectrochemical water splitting: Integration of subsurface dipoles with atomic-scale control

DOE PAGES

Hikita, Yasuyuki; Nishio, Kazunori; Seitz, Linsey C.; ...

2016-01-22

One of the crucial parameters dictating the efficiency of photoelectrochemical water-splitting is the semiconductor band edge alignment with respect to hydrogen and oxygen redox potentials. Despite the importance of metal oxides in their use as photoelectrodes, studies to control the band edge alignment in aqueous solution have been limited predominantly to compound semiconductors with modulation ranges limited to a few hundred mV. The ability to modulate the flat band potential of oxide photoanodes by as much as 1.3 V, using the insertion of subsurface electrostatic dipoles near a Nb-doped SrTiO 3/aqueous electrolyte interface is reported. Lastly, the tunable range achievedmore » far exceeds previous reports in any semiconductor/aqueous electrolyte system and suggests a general design strategy for highly efficient oxide photoelectrodes.« less

Nanochannels Photoelectrochemical Biosensor.

PubMed

Zhang, Nan; Ruan, Yi-Fan; Zhang, Li-Bin; Zhao, Wei-Wei; Xu, Jing-Juan; Chen, Hong-Yuan

2018-02-06

Nanochannels have brought new opportunities for biosensor development. Herein, we present the novel concept of a nanochannels photoelectrochemical (PEC) biosensor based on the integration of a unique Cu x O-nanopyramid-islands (NPIs) photocathode, an anodic aluminum oxide (AAO) membrane, and alkaline phosphatase (ALP) catalytic chemistry. The Cu x O-NPIs photocathode possesses good performance, and further assembly with AAO yields a designed architecture composed of vertically aligned, highly ordered nanoarrays on top of the Cu x O-NPIs film. After biocatalytic precipitation (BCP) was stimulated within the channels, the biosensor was used for the successful detection of ALP activity. This study has not only provided a novel paradigm for an unconventional nanochannels PEC biosensor, which can be used for general bioanalytical purposes, but also indicated that the new concept of nanochannel-semiconductor heterostructures is a step toward innovative biomedical applications.

Al decorated ZnO thin-film photoanode for SPR-enhanced photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Li, Hongxia; Li, Xin; Dong, Wei; Xi, Junhua; Wu, Xin

2018-06-01

Photoelectrochemical (PEC) water splitting has been considered to be a promising approach to ease the energy and environmental crisis. Herein, Al decorated ZnO thin films are successfully achieved through a facile dc magnetron-sputtering method followed with Al evaporation for further enhanced PEC performance. The Al/ZnO thin film with 60 s Al evaporating time exhibits the highest photocurrent density under AM1.5G and visible light irradiation, which are more than 5 and 3 times as the pure ZnO film, respectively. Such surface modification by Al not only enlarges the visible light absorption based on surface plasmonic resonance effect, but facilitates the charge separation and transportation at the electrode/electrolyte interface. Finally, a possible mechanism is proposed for the photocatalytic activity enhancement of Al/ZnO thin film photoanode.

Copper Phthalocyanine-Functionalized Graphitic Carbon Nitride: A Hybrid Heterostructure toward Photoelectrochemical and Photocatalytic Degradation Applications.

PubMed

Liu, Zhong-Guo; Wan, Jia-Yun; Yang, Ze; Wang, Shi-Quan; Wang, Hang-Xing

2016-07-05

In this work, alcian blue 8GX (AB), a copper(II) phthalocyanine derivative, was employed to functionalize graphitic carbon nitride (g-C3 N4 ) for the preparation of a highly efficient photocatalyst. The approach relies on a facile AB-assisted ethanol/water mixed-solvent exfoliation of bulk g-C3 N4 . The as-prepared g-C3 N4 /AB hybrid possesses significantly enhanced solution dispersibility and photoelectrochemical performance resulting from the synergistic effect between g-C3 N4 and AB, which involves the optimization of intimate interfacial contact, extension of light absorption range, and enhancement of charge-transfer efficiency. This synergy contributes enormously to the photocatalytic degradation of rhodamine 6G (R6G) under light irradiation. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fe doped BaTiO3 sensitized by Fe3O4 nanoparticles for improved photoelectrochemical response

NASA Astrophysics Data System (ADS)

Upadhyay, Rishibrind Kumar; Sharma, Dipika

2018-01-01

Nanostructured powders of pristine Fe3O4, BaTiO3, and Fe-BaTiO3 were synthesized using hydrothermal method and BaTiO3/Fe3O4 and Fe-BaTiO3/Fe3O4 composite sample were also prepared by mixing the appropriate amount of pristine powders. All samples were characterized using x-ray diffraction, SEM and UV-vis spectrometry. Photoelectrochemical properties were investigated in a three-electrode cell system. Maximum photocurrent density of 2.1 mA cm-2 at 0.95 V/SCE was observed for Fe-BaTiO3/Fe3O4 composite sample. Increased photocurrent density offered by composite may be attributed to improved conductivity and better separation of the photogenerated charge carriers at interface.

Smooth and selective photo-electrochemical etching of heavily doped GaN:Si using a mode-locked 355 nm microchip laser

NASA Astrophysics Data System (ADS)

Lee, SeungGeun; Mishkat-Ul-Masabih, Saadat; Leonard, John T.; Feezell, Daniel F.; Cohen, Daniel A.; Speck, James S.; Nakamura, Shuji; DenBaars, Steven P.

2017-01-01

We investigate the photo-electrochemical (PEC) etching of Si-doped GaN samples grown on nonpolar GaN substrates, using a KOH/K2S2O8 solution and illuminated by a Xe arc lamp or a Q-switched 355 nm laser. The etch rate with the arc lamp decreased as the doping concentration increased, and the etching stopped for concentrations above 7.7 × 1018 cm-3. The high peak intensity of the Q-switched laser extended the etchable concentration to 2.4 × 1019 cm-3, with an etch rate of 14 nm/min. Compositionally selective etching was demonstrated, with an RMS surface roughness of 1.6 nm after etching down to an n-Al0.20Ga0.80N etch stop layer.

Metal-free organic sensitizers for use in water-splitting dye-sensitized photoelectrochemical cells

DOE PAGES

Swierk, John R.; Méndez-Hernández, Dalvin D.; McCool, Nicholas S.; ...

2015-01-12

Solar fuel generation requires the efficient capture and conversion of visible light. In both natural and artificial systems, molecular sensitizers can be tuned to capture, convert, and transfer visible light energy. We demonstrate that a series of metal-free porphyrins can drive photoelectrochemical water splitting under broadband and red light (λ > 590 nm) illumination in a dye-sensitized TiO 2 solar cell. Here, we report the synthesis, spectral, and electrochemical properties of the sensitizers. Despite slow recombination of photoinjected electrons with oxidized porphyrins, photocurrents are low because of low injection yields and slow electron self-exchange between oxidized porphyrins. As a result,more » the free-base porphyrins are stable under conditions of water photoelectrolysis and in some cases photovoltages in excess of 1 V are observed.« less

Photoelectroreduction of Building-Block Chemicals.

PubMed

Chen, Fengjiao; Cui, Wei; Zhang, Jie; Wang, Yeyun; Zhou, Junhua; Hu, Yongpan; Li, Yanguang; Lee, Shuit-Tong

2017-06-12

Conventional photoelectrochemical cells utilize solar energy to drive the chemical conversion of water or CO 2 into useful chemical fuels. Such processes are confronted with general challenges, including the low intrinsic activities and inconvenient storage and transportation of their gaseous products. A photoelectrochemical approach is proposed to drive the reductive production of industrial building-block chemicals and demonstrate that succinic acid and glyoxylic acid can be readily synthesized on Si nanowire array photocathodes free of any cocatalyst and at room temperature. These photocathodes exhibit a positive onset potential, large saturation photocurrent density, high reaction selectivity, and excellent operation durability. They capitalize on the large photovoltage generated from the semiconductor/electrolyte junction to partially offset the required external bias, and thereby make this photoelectrosynthetic approach significantly more sustainable compared to traditional electrosynthesis. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Copper Oxide Nanograss for Efficient and Stable Photoelectrochemical Hydrogen Production by Water Splitting

NASA Astrophysics Data System (ADS)

Borkar, Rajnikant; Dahake, Rashmi; Rayalu, Sadhana; Bansiwal, Amit

2018-03-01

A biphasic copper oxide thin film of grass-like appendage morphology is synthesized by two-step electro-deposition method and later investigated for photoelectrochemical (PEC) water splitting for hydrogen production. Further, the thin film was characterized by UV-Visible spectroscopy, x-ray diffraction (XRD), Scanning electron microscopy (SEM) and PEC techniques. The XRD analysis confirms formation of biphasic copper oxide phases, and SEM reveals high surface area grass appendage-like morphology. These grass appendage structures exhibit a high cathodic photocurrent of - 1.44 mAcm-2 at an applied bias of - 0.7 (versus Ag/AgCl) resulting in incident to photon current efficiency (IPCE) of ˜ 10% at 400 nm. The improved light harvesting and charge transport properties of grass appendage structured biphasic copper oxides makes it a potential candidate for PEC water splitting for hydrogen production.

Engineered photoproteins that give rise to photosynthetically-incompetent bacteria are effective as photovoltaic materials for biohybrid photoelectrochemical cells

PubMed Central

Liu, Juntai; Friebe, Vincent M.; Swainsbury, David J. K.; Crouch, Lucy I.; Szabo, David A.; Frese, Raoul N.

2018-01-01

Reaction centre/light harvesting proteins such as the RCLH1X complex from Rhodobacter sphaeroides carry out highly quantum-efficient conversion of solar energy through ultrafast energy transfer and charge separation, and these pigment-proteins have been incorporated into biohybrid photoelectrochemical cells for a variety of applications. In this work we demonstrate that, despite not being able to support normal photosynthetic growth of Rhodobacter sphaeroides, an engineered variant of this RCLH1X complex lacking the PufX protein and with an enlarged light harvesting antenna is unimpaired in its capacity for photocurrent generation in two types of bio-photoelectrochemical cells. Removal of PufX also did not impair the ability of the RCLH1 complex to act as an acceptor of energy from synthetic light harvesting quantum dots. Unexpectedly, the removal of PufX led to a marked improvement in the overall stability of the RCLH1 complex under heat stress. We conclude that PufX-deficient RCLH1 complexes are fully functional in solar energy conversion in a device setting and that their enhanced structural stability could make them a preferred choice over their native PufX-containing counterpart. Our findings on the competence of RCLH1 complexes for light energy conversion in vitro are discussed with reference to the reason why these PufX-deficient proteins are not capable of light energy conversion in vivo. PMID:29364305

Dye-sensitized photoelectrochemical water oxidation through a buried junction.

PubMed

Xu, Pengtao; Huang, Tian; Huang, Jianbin; Yan, Yun; Mallouk, Thomas E

2018-06-18

Water oxidation has long been a challenge in artificial photosynthetic devices that convert solar energy into fuels. Water-splitting dye-sensitized photoelectrochemical cells (WS-DSPECs) provide a modular approach for integrating light-harvesting molecules with water-oxidation catalysts on metal-oxide electrodes. Despite recent progress in improving the efficiency of these devices by introducing good molecular water-oxidation catalysts, WS-DSPECs have poor stability, owing to the oxidation of molecular components at very positive electrode potentials. Here we demonstrate that a solid-state dye-sensitized solar cell (ss-DSSC) can be used as a buried junction for stable photoelectrochemical water splitting. A thin protecting layer of TiO 2 grown by atomic layer deposition (ALD) stabilizes the operation of the photoanode in aqueous solution, although as a solar cell there is a performance loss due to increased series resistance after the coating. With an electrodeposited iridium oxide layer, a photocurrent density of 1.43 mA cm -2 was observed in 0.1 M pH 6.7 phosphate solution at 1.23 V versus reversible hydrogen electrode, with good stability over 1 h. We measured an incident photon-to-current efficiency of 22% at 540 nm and a Faradaic efficiency of 43% for oxygen evolution. While the potential profile of the catalyst layer suggested otherwise, we confirmed the formation of a buried junction in the as-prepared photoelectrode. The buried junction design of ss-DSSs adds to our understanding of semiconductor-electrocatalyst junction behaviors in the presence of a poor semiconducting material.

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.

Gradient doping - a case study with Ti-Fe2O3 towards an improved photoelectrochemical response.

PubMed

Srivastav, Anupam; Verma, Anuradha; Banerjee, Anamika; Khan, Saif A; Gupta, Mukul; Satsangi, Vibha Rani; Shrivastav, Rohit; Dass, Sahab

2016-12-07

The present study investigates the effect of gradient doping on modifying the photoelectrochemical response of Ti-doped Fe 2 O 3 photoanodes for their use in sunlight based water splitting for hydrogen evolution. The deposition of a thin film over the ITO (tin doped indium oxide) substrate was carried out using a spray pyrolysis method. The concentration of dopant was varied from 0.5-8.0 at% and two sets of samples were also prepared with low to high (0.5-8%) and high to low (8-0.5%) dopant concentrations in the direction towards the substrate. The prepared thin films were characterized using X-ray Diffractometry (XRD), Scanning Electron Microscopy (SEM), Energy Dispersive X-ray (EDX) Spectroscopy, Secondary Ion Mass Spectroscopy (SIMS), X-ray Photoelectron Spectroscopy (XPS) and UV-visible Spectroscopy. The photoelectrochemical studies revealed that the deposition of dopant layers with a low to high concentration towards the substrate exhibited a highly improved photoresponse (200 times) in comparison to the pristine sample and a two fold enhancement in comparison to 2% Ti-doped Fe 2 O 3 . The improvement in the photoresponse has been attributed to the values of a high flat band potential, low resistance, high open circuit voltage, carrier separation efficiency, applied bias photon-to-current conversion efficiency (ABPE), and incident photon-to-current conversion efficiency (IPCE). A reduced charge transfer resistance has been demonstrated with Nyquist plots.

Photoelectrochemical performance of W-doped BiVO4 thin-films deposited by spray pyrolysis

NASA Astrophysics Data System (ADS)

Holland, Stephen K.; Dutter, Melissa R.; Lawrence, David J.; Reisner, Barbara A.; DeVore, Thomas C.

2013-09-01

The effect of tungsten doping and hydrogen annealing treatments on the photoelectrochemical (PEC) performance of bismuth vanadate (BiVO4) photoanodes for solar water splitting was studied. Thin films of BiVO4 were deposited on ITO-coated glass slides by ultrasonic spray pyrolysis of an aqueous solution containing bismuth nitrate and vanadium oxysulfate. Tungsten doping was achieved by adding either silicotungstic acid (STA) or ammonium metatungstate (AMT) in the aqueous precursor. The 1.7 μm - 2.2 μm thick films exhibited a highly porous microstructure. Undoped films that were reduced at 375 ºC in 3% H2 exhibited the largest photocurrent densities under 0.1 W cm-2 AM1.5 illumination. This performance enhancement was believed to be due to the formation of oxygen vacancies, which are shallow electron donors, in the films. Films doped with 1% or 5% tungsten from either STA or AMT exhibited reduced photoelectrochemical performance and greater sample-to-sample performance variations. Powder X-ray diffraction data of the undoped films indicated that they were comprised primarily of the monoclinic scheelite phase while unidentified phases were also present. Scanning electron microscopy showed slightly different morphology characteristics for the Wdoped films. It is surmised that the addition of W in the deposition process promoted the morphology differences and the formation of different phases, thus reducing the PEC performance of the photoanode samples. Significant PEC performance variability was also observed among films deposited using the described process.

Increasing the open-circuit voltage of photoprotein-based photoelectrochemical cells by manipulation of the vacuum potential of the electrolytes.

PubMed

Tan, Swee Ching; Crouch, Lucy I; Mahajan, Sumeet; Jones, Michael R; Welland, Mark E

2012-10-23

The innately highly efficient light-powered separation of charge that underpins natural photosynthesis can be exploited for applications in photoelectrochemistry by coupling nanoscale protein photoreaction centers to man-made electrodes. Planar photoelectrochemical cells employing purple bacterial reaction centers have been constructed that produce a direct current under continuous illumination and an alternating current in response to discontinuous illumination. The present work explored the basis of the open-circuit voltage (V(OC)) produced by such cells with reaction center/antenna (RC-LH1) proteins as the photovoltaic component. It was established that an up to ~30-fold increase in V(OC) could be achieved by simple manipulation of the electrolyte connecting the protein to the counter electrode, with an approximately linear relationship being observed between the vacuum potential of the electrolyte and the resulting V(OC). We conclude that the V(OC) of such a cell is dependent on the potential difference between the electrolyte and the photo-oxidized bacteriochlorophylls in the reaction center. The steady-state short-circuit current (J(SC)) obtained under continuous illumination also varied with different electrolytes by a factor of ~6-fold. The findings demonstrate a simple way to boost the voltage output of such protein-based cells into the hundreds of millivolts range typical of dye-sensitized and polymer-blend solar cells, while maintaining or improving the J(SC). Possible strategies for further increasing the V(OC) of such protein-based photoelectrochemical cells through protein engineering are discussed.

Principles of nucleic acid hybridization and comparison with monoclonal antibody technology for the diagnosis of infectious diseases.

PubMed Central

Edberg, S. C.

1985-01-01

Until the 1980s the diagnosis of specific etiologic agents of infectious diseases rested with their isolation in vitro and identification by analysis of their phenotypic characteristics. In the 1970s the concept of a microbial species evolved from phenotypic analysis to nucleic acid homology. Currently, nucleic acid sequences specific for a given species are being isolated and amplified and utilized not only to identify the pathogen after it has been grown in vitro but also elucidate it directly in biological material. The procedures for making nucleic acid hybridization probes are analogous to the generation of monoclonal antibody tests. Currently, research and development are centered in choosing the particular nucleic acid to analyze, establishing the most efficient vector system for amplifying the nucleic acid, generating an efficient means of selecting the particular nucleic acid fragment specific for the microorganism, and in measuring the hybridization reaction. While immunological techniques have been utilized in the clinical laboratory for over thirty years, the means of detecting nucleic acid hybridization reactions are just beginning to be usable in the clinical diagnostic laboratory. Much of nucleic acid hybridization research is proprietary, and a particular challenge is to develop a means whereby information can be used for the progress of science as a whole when generated by private ownership. Images FIG. 4 PMID:3004048

Method of increasing conversion of a fatty acid to its corresponding dicarboxylic acid

DOEpatents

Craft, David L.; Wilson, C. Ron; Eirich, Dudley; Zhang, Yeyan

2004-09-14

A nucleic acid sequence including a CYP promoter operably linked to nucleic acid encoding a heterologous protein is provided to increase transcription of the nucleic acid. Expression vectors and host cells containing the nucleic acid sequence are also provided. The methods and compositions described herein are especially useful in the production of polycarboxylic acids by yeast cells.

Use of CYP52A2A promoter to increase gene expression in yeast

DOEpatents

Craft, David L.; Wilson, C. Ron; Eirich, Dudley; Zhang, Yeyan

2004-01-06

A nucleic acid sequence including a CYP promoter operably linked to nucleic acid encoding a heterologous protein is provided to increase transcription of the nucleic acid. Expression vectors and host cells containing the nucleic acid sequence are also provided. The methods and compositions described herein are especially useful in the production of polycarboxylic acids by yeast cells.

dbAMEPNI: a database of alanine mutagenic effects for protein–nucleic acid interactions

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

Liu, Ling; Xiong, Yi; Gao, Hongyun

Protein–nucleic acid interactions play essential roles in various biological activities such as gene regulation, transcription, DNA repair and DNA packaging. Understanding the effects of amino acid substitutions on protein–nucleic acid binding affinities can help elucidate the molecular mechanism of protein–nucleic acid recognition. Until now, no comprehensive and updated database of quantitative binding data on alanine mutagenic effects for protein–nucleic acid interactions is publicly accessible. Thus, we developed a new database of Alanine Mutagenic Effects for Protein-Nucleic Acid Interactions (dbAMEPNI). dbAMEPNI is a manually curated, literature-derived database, comprising over 577 alanine mutagenic data with experimentally determined binding affinities for protein–nucleic acidmore » complexes. Here, it contains several important parameters, such as dissociation constant (Kd), Gibbs free energy change (ΔΔG), experimental conditions and structural parameters of mutant residues. In addition, the database provides an extended dataset of 282 single alanine mutations with only qualitative data (or descriptive effects) of thermodynamic information.« less

Detection and isolation of nucleic acid sequences using competitive hybridization probes

DOEpatents

Lucas, Joe N.; Straume, Tore; Bogen, Kenneth T.

1997-01-01

A method for detecting a target nucleic acid sequence in a sample is provided using hybridization probes which competitively hybridize to a target nucleic acid. According to the method, a target nucleic acid sequence is hybridized to first and second hybridization probes which are complementary to overlapping portions of the target nucleic acid sequence, the first hybridization probe including a first complexing agent capable of forming a binding pair with a second complexing agent and the second hybridization probe including a detectable marker. The first complexing agent attached to the first hybridization probe is contacted with a second complexing agent, the second complexing agent being attached to a solid support such that when the first and second complexing agents are attached, target nucleic acid sequences hybridized to the first hybridization probe become immobilized on to the solid support. The immobilized target nucleic acids are then separated and detected by detecting the detectable marker attached to the second hybridization probe. A kit for performing the method is also provided.

dbAMEPNI: a database of alanine mutagenic effects for protein–nucleic acid interactions

DOE PAGES

Liu, Ling; Xiong, Yi; Gao, Hongyun; ...

2018-04-02

Protein–nucleic acid interactions play essential roles in various biological activities such as gene regulation, transcription, DNA repair and DNA packaging. Understanding the effects of amino acid substitutions on protein–nucleic acid binding affinities can help elucidate the molecular mechanism of protein–nucleic acid recognition. Until now, no comprehensive and updated database of quantitative binding data on alanine mutagenic effects for protein–nucleic acid interactions is publicly accessible. Thus, we developed a new database of Alanine Mutagenic Effects for Protein-Nucleic Acid Interactions (dbAMEPNI). dbAMEPNI is a manually curated, literature-derived database, comprising over 577 alanine mutagenic data with experimentally determined binding affinities for protein–nucleic acidmore » complexes. Here, it contains several important parameters, such as dissociation constant (Kd), Gibbs free energy change (ΔΔG), experimental conditions and structural parameters of mutant residues. In addition, the database provides an extended dataset of 282 single alanine mutations with only qualitative data (or descriptive effects) of thermodynamic information.« less

Introduction of structural affinity handles as a tool in selective nucleic acid separations

NASA Technical Reports Server (NTRS)

Willson, III, Richard Coale (Inventor); Cano, Luis Antonio (Inventor)

2011-01-01

The method is used for separating nucleic acids and other similar constructs. It involves selective introduction, enhancement, or stabilization of affinity handles such as single-strandedness in the undesired (or desired) nucleic acids as compared to the usual structure (e.g., double-strandedness) of the desired (or undesired) nucleic acids. The undesired (or desired) nucleic acids are separated from the desired (or undesired) nucleic acids due to capture by methods including but not limited to immobilized metal affinity chromatography, immobilized single-stranded DNA binding (SSB) protein, and immobilized oligonucleotides. The invention is useful to: remove contaminating genomic DNA from plasmid DNA; remove genomic DNA from plasmids, BACs, and similar constructs; selectively separate oligonucleotides and similar DNA fragments from their partner strands; purification of aptamers, (deoxy)-ribozymes and other highly structured nucleic acids; Separation of restriction fragments without using agarose gels; manufacture recombinant Taq polymerase or similar products that are sensitive to host genomic DNA contamination; and other applications.

Detection and isolation of nucleic acid sequences using competitive hybridization probes

DOEpatents

Lucas, J.N.; Straume, T.; Bogen, K.T.

1997-04-01

A method for detecting a target nucleic acid sequence in a sample is provided using hybridization probes which competitively hybridize to a target nucleic acid. According to the method, a target nucleic acid sequence is hybridized to first and second hybridization probes which are complementary to overlapping portions of the target nucleic acid sequence, the first hybridization probe including a first complexing agent capable of forming a binding pair with a second complexing agent and the second hybridization probe including a detectable marker. The first complexing agent attached to the first hybridization probe is contacted with a second complexing agent, the second complexing agent being attached to a solid support such that when the first and second complexing agents are attached, target nucleic acid sequences hybridized to the first hybridization probe become immobilized on to the solid support. The immobilized target nucleic acids are then separated and detected by detecting the detectable marker attached to the second hybridization probe. A kit for performing the method is also provided. 7 figs.

Nucleic Acid analysis by fourier transform ion cyclotron resonance mass spectrometry at the beginning of the twenty-first century.

PubMed

Frahm, J L; Muddiman, D C

2005-01-01

Mass spectrometers measure an intrinsic property (i.e., mass) of a molecule, which makes it an ideal platform for nucleic acid analysis. Importantly, the unparalleled capabilities of Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry further extend its usefulness for nucleic acid analysis. The beginning of the twenty-first century has been marked with notable advances in the field of FT-ICR mass spectrometry analysis of nucleic acids. Some of these accomplishments include fundamental studies of nucleic acid properties, improvements in sample clean up and preparation, better methods to obtain higher mass measurement accuracy, analysis of noncovalent complexes, tandem mass spectrometry, and characterization of peptide nucleic acids. This diverse range of studies will be presented herein.

Ultra-sensitive detection of leukemia by graphene

NASA Astrophysics Data System (ADS)

Akhavan, Omid; Ghaderi, Elham; Hashemi, Ehsan; Rahighi, Reza

2014-11-01

Graphene oxide nanoplatelets (GONPs) with extremely sharp edges (lateral dimensions ~20-200 nm and thicknesses <2 nm) were applied in extraction of the overexpressed guanine synthesized in the cytoplasm of leukemia cells. The blood serums containing the extracted guanine were used in differential pulse voltammetry (DPV) with reduced graphene oxide nanowall (rGONW) electrodes to develop fast and ultra-sensitive electrochemical detection of leukemia cells at leukemia fractions (LFs) of ~10-11 (as the lower detection limit). The stability of the DPV signals obtained by oxidation of the extracted guanine on the rGONWs was studied after 20 cycles. Without the guanine extraction, the DPV peaks relating to guanine oxidation of normal and abnormal cells overlapped at LFs <10-9, and consequently, the performance of rGONWs alone was limited at this level. As a benchmark, the DPV using glassy carbon electrodes was able to detect only LFs ~ 10-2. The ultra-sensitivity obtained by this combination method (guanine extraction by GONPs and then guanine oxidation by rGONWs) is five orders of magnitude better than the sensitivity of the best current technologies (e.g., specific mutations by polymerase chain reaction) which not only are expensive, but also require a few days for diagnosis.Graphene oxide nanoplatelets (GONPs) with extremely sharp edges (lateral dimensions ~20-200 nm and thicknesses <2 nm) were applied in extraction of the overexpressed guanine synthesized in the cytoplasm of leukemia cells. The blood serums containing the extracted guanine were used in differential pulse voltammetry (DPV) with reduced graphene oxide nanowall (rGONW) electrodes to develop fast and ultra-sensitive electrochemical detection of leukemia cells at leukemia fractions (LFs) of ~10-11 (as the lower detection limit). The stability of the DPV signals obtained by oxidation of the extracted guanine on the rGONWs was studied after 20 cycles. Without the guanine extraction, the DPV peaks relating to guanine oxidation of normal and abnormal cells overlapped at LFs <10-9, and consequently, the performance of rGONWs alone was limited at this level. As a benchmark, the DPV using glassy carbon electrodes was able to detect only LFs ~ 10-2. The ultra-sensitivity obtained by this combination method (guanine extraction by GONPs and then guanine oxidation by rGONWs) is five orders of magnitude better than the sensitivity of the best current technologies (e.g., specific mutations by polymerase chain reaction) which not only are expensive, but also require a few days for diagnosis. Electronic supplementary information (ESI) available. See DOI: 10.1039/C4NR04589K

Reactivity of Nucleic Acid Radicals

PubMed Central

Greenberg, Marc M.

2016-01-01

Nucleic acid oxidation plays a vital role in the etiology and treatment of diseases, as well as aging. Reagents that oxidize nucleic acids are also useful probes of the biopolymers’ structure and folding. Radiation scientists have contributed greatly to our understanding of nucleic acid oxidation using a variety of techniques. During the past two decades organic chemists have applied the tools of synthetic and mechanistic chemistry to independently generate and study the reactive intermediates produced by ionizing radiation and other nucleic acid damaging agents. This approach has facilitated resolving mechanistic controversies and lead to the discovery of new reactive processes. PMID:28529390

Carbon nanotube enhanced label-free detection of microRNAs based on hairpin probe triggered solid-phase rolling-circle amplification

NASA Astrophysics Data System (ADS)

Tian, Qianqian; Wang, Ying; Deng, Ruijie; Lin, Lei; Liu, Yang; Li, Jinghong

2014-12-01

The detection of microRNAs (miRNAs) is imperative for gaining a better understanding of the functions of these biomarkers and has great potential for the early diagnosis of human disease. High sensitivity and selectivity for miRNA detection brings new challenges. Herein, an ultrasensitive protocol for electrochemical detection of miRNA is designed through carbon nanotube (CNT) enhanced label-free detection based on hairpin probe triggered solid-phase rolling-circle amplification (RCA). Traditionally, RCA, widely applied for signal enhancement in the construction of a variety of biosensors, has an intrinsic limitation of ultrasensitive detection, as it is difficult to separate the enzymes, templates, and padlock DNAs from the RCA products in the homogeneous solution. We purposely designed a solid-phase RCA strategy, using CNTs as the solid substrate, integrated with a hairpin structured probe to recognize target miRNA. In the presence of miRNA the stem-loop structure will be unfolded, triggering the CNT based RCA process. Due to the efficient blocking effect originating from the polymeric RCA products, the label-free assay of miRNA exhibits an ultrasensitive detection limit of 1.2 fM. Furthermore, the protocol possesses excellent specificity for resolving lung cancer-related let-7 family members which have only one-nucleotide variations. The high sensitivity and selectivity give the method great potential for applications in online diagnostics and in situ detection in long-term development.The detection of microRNAs (miRNAs) is imperative for gaining a better understanding of the functions of these biomarkers and has great potential for the early diagnosis of human disease. High sensitivity and selectivity for miRNA detection brings new challenges. Herein, an ultrasensitive protocol for electrochemical detection of miRNA is designed through carbon nanotube (CNT) enhanced label-free detection based on hairpin probe triggered solid-phase rolling-circle amplification (RCA). Traditionally, RCA, widely applied for signal enhancement in the construction of a variety of biosensors, has an intrinsic limitation of ultrasensitive detection, as it is difficult to separate the enzymes, templates, and padlock DNAs from the RCA products in the homogeneous solution. We purposely designed a solid-phase RCA strategy, using CNTs as the solid substrate, integrated with a hairpin structured probe to recognize target miRNA. In the presence of miRNA the stem-loop structure will be unfolded, triggering the CNT based RCA process. Due to the efficient blocking effect originating from the polymeric RCA products, the label-free assay of miRNA exhibits an ultrasensitive detection limit of 1.2 fM. Furthermore, the protocol possesses excellent specificity for resolving lung cancer-related let-7 family members which have only one-nucleotide variations. The high sensitivity and selectivity give the method great potential for applications in online diagnostics and in situ detection in long-term development. Electronic supplementary information (ESI) available: Preparation of the chemically modified multi-walled carbon nanotubes (CNTs), characterization of the CNTs and modified CNTs, preparation of the circular probe, gel electrophoresis of the RCA products, and DNA probes as noted in the text. See DOI: 10.1039/c4nr05243a

Revealing Nucleic Acid Mutations Using Förster Resonance Energy Transfer-Based Probes

PubMed Central

Junager, Nina P. L.; Kongsted, Jacob; Astakhova, Kira

2016-01-01

Nucleic acid mutations are of tremendous importance in modern clinical work, biotechnology and in fundamental studies of nucleic acids. Therefore, rapid, cost-effective and reliable detection of mutations is an object of extensive research. Today, Förster resonance energy transfer (FRET) probes are among the most often used tools for the detection of nucleic acids and in particular, for the detection of mutations. However, multiple parameters must be taken into account in order to create efficient FRET probes that are sensitive to nucleic acid mutations. In this review; we focus on the design principles for such probes and available computational methods that allow for their rational design. Applications of advanced, rationally designed FRET probes range from new insights into cellular heterogeneity to gaining new knowledge of nucleic acid structures directly in living cells. PMID:27472344

RNA-guided transcriptional regulation

DOEpatents

Church, George M.; Mali, Prashant G.; Esvelt, Kevin M.

2016-02-23

Methods of modulating expression of a target nucleic acid in a cell are provided including introducing into the cell a first foreign nucleic acid encoding one or more RNAs complementary to DNA, wherein the DNA includes the target nucleic acid, introducing into the cell a second foreign nucleic acid encoding a nuclease-null Cas9 protein that binds to the DNA and is guided by the one or more RNAs, introducing into the cell a third foreign nucleic acid encoding a transcriptional regulator protein or domain, wherein the one or more RNAs, the nuclease-null Cas9 protein, and the transcriptional regulator protein or domain are expressed, wherein the one or more RNAs, the nuclease-null Cas9 protein and the transcriptional regulator protein or domain co-localize to the DNA and wherein the transcriptional regulator protein or domain regulates expression of the target nucleic acid.

Crystallization and X-ray diffraction analysis of an 'all-locked' nucleic acid duplex derived from a tRNA(Ser) microhelix.

PubMed

Behling, Katja; Eichert, André; Fürste, Jens P; Betzel, Christian; Erdmann, Volker A; Förster, Charlotte

2009-08-01

Modified nucleic acids are of great interest with respect to their nuclease resistance and enhanced thermostability. In therapeutical and diagnostic applications, such molecules can substitute for labile natural nucleic acids that are targeted against particular diseases or applied in gene therapy. The so-called 'locked nucleic acids' contain modified sugar moieties such as 2'-O,4'-C-methylene-bridged beta-D-ribofuranose and are known to be very stable nucleic acid derivatives. The structure of locked nucleic acids in single or multiple LNA-substituted natural nucleic acids and in LNA-DNA or LNA-RNA heteroduplexes has been well investigated, but the X-ray structure of an ;all-locked' nucleic acid double helix has not been described to date. Here, the crystallization and X-ray diffraction data analysis of an 'all-locked' nucleic acid helix, which was designed as an LNA originating from a tRNA(Ser) microhelix RNA structure, is presented. The crystals belonged to space group C2, with unit-cell parameters a = 77.91, b = 40.74, c = 30.06 A, beta = 91.02 degrees . A high-resolution and a low-resolution data set were recorded, with the high-resolution data showing diffraction to 1.9 A resolution. The crystals contained two double helices per asymmetric unit, with a Matthews coefficient of 2.48 A(3) Da(-1) and a solvent content of 66.49% for the merged data.

Nucleic acid-functionalized transition metal nanosheets for biosensing applications

PubMed Central

Mo, Liuting; Li, Juan; Liu, Qiaoling; Qiu, Liping; Tan, Weihong

2017-01-01

In clinical diagnostics, as well as food and environmental safety practices, biosensors are powerful tools for monitoring biological or biochemical processes. Two-dimensional (2D) transition metal nanomaterials, including transition metal chalcogenides (TMCs) and transition metal oxides (TMOs), are receiving growing interest for their use in biosensing applications based on such unique properties as high surface area and fluorescence quenching abilities. Meanwhile, nucleic acid probes based on Watson-Crick base-pairing rules are also being widely applied in biosensing based on their excellent recognition capability. In particular, the emergence of functional nucleic acids in the 1980s, especially aptamers, has substantially extended the recognition capability of nucleic acids to various targets, ranging from small organic molecules and metal ions to proteins and cells. Based on π-π stacking interaction between transition metal nanosheets and nucleic acids, biosensing systems can be easily assembled. Therefore, the combination of 2D transition metal nanomaterials and nucleic acids brings intriguing opportunities in bioanalysis and biomedicine. In this review, we summarize recent advances of nucleic acid-functionalized transition metal nanosheets in biosensing applications. The structure and properties of 2D transition metal nanomaterials are first discussed, emphasizing the interaction between transition metal nanosheets and nucleic acids. Then, the applications of nucleic acid-functionalized transition metal nanosheet-based biosensors are discussed in the context of different signal transducing mechanisms, including optical and electrochemical approaches. Finally, we provide our perspectives on the current challenges and opportunities in this promising field. PMID:27020066

Nucleic acid-functionalized transition metal nanosheets for biosensing applications.

PubMed

Mo, Liuting; Li, Juan; Liu, Qiaoling; Qiu, Liping; Tan, Weihong

2017-03-15

In clinical diagnostics, as well as food and environmental safety practices, biosensors are powerful tools for monitoring biological or biochemical processes. Two-dimensional (2D) transition metal nanomaterials, including transition metal chalcogenides (TMCs) and transition metal oxides (TMOs), are receiving growing interest for their use in biosensing applications based on such unique properties as high surface area and fluorescence quenching abilities. Meanwhile, nucleic acid probes based on Watson-Crick base-pairing rules are also being widely applied in biosensing based on their excellent recognition capability. In particular, the emergence of functional nucleic acids in the 1980s, especially aptamers, has substantially extended the recognition capability of nucleic acids to various targets, ranging from small organic molecules and metal ions to proteins and cells. Based on π-π stacking interaction between transition metal nanosheets and nucleic acids, biosensing systems can be easily assembled. Therefore, the combination of 2D transition metal nanomaterials and nucleic acids brings intriguing opportunities in bioanalysis and biomedicine. In this review, we summarize recent advances of nucleic acid-functionalized transition metal nanosheets in biosensing applications. The structure and properties of 2D transition metal nanomaterials are first discussed, emphasizing the interaction between transition metal nanosheets and nucleic acids. Then, the applications of nucleic acid-functionalized transition metal nanosheet-based biosensors are discussed in the context of different signal transducing mechanisms, including optical and electrochemical approaches. Finally, we provide our perspectives on the current challenges and opportunities in this promising field. Copyright © 2016 Elsevier B.V. All rights reserved.

Ultrasensitive dual-beam absorption and gain spectroscopy: applications for near-infrared and visible diode laser sensors

NASA Astrophysics Data System (ADS)

Allen, Mark G.; Carleton, Karen L.; Davis, Steven J.; Kessler, William J.; Otis, Charles E.; Palombo, Daniel A.; Sonnenfroh, David M.

1995-06-01

A dual-beam detection strategy with automatic balancing is described for ultrasensitive spectroscopy. Absorbances of 2 \\times 10-7 Hz-1/2 in free-space configurations and 5 \\times 10-6 Hz -1/2 in fiber-coupled configurations are demonstrated. With the dual-beam technique, atmospherically broadened absorption transitions may be resolved with InGaAsP, AlGaAs, and AlGaInP single-longitudinal-mode diode lasers. Applications to trace measurements of NO2 , O2, and H2O are described by the use of simple, inexpensive laser and detector systems. Small signal gain measurements on optically pumped I2 with a sensitivity of 10-5 are also reported.

Repeated Solid-state Dewetting of Thin Gold Films for Nanogap-rich Plasmonic Nanoislands.

PubMed

Kang, Minhee; Park, Sang-Gil; Jeong, Ki-Hun

2015-10-15

This work reports a facile wafer-level fabrication for nanogap-rich gold nanoislands for highly sensitive surface enhanced Raman scattering (SERS) by repeating solid-state thermal dewetting of thin gold film. The method provides enlarged gold nanoislands with small gap spacing, which increase the number of electromagnetic hotspots and thus enhance the extinction intensity as well as the tunability for plasmon resonance wavelength. The plasmonic nanoislands from repeated dewetting substantially increase SERS enhancement factor over one order-of-magnitude higher than those from a single-step dewetting process and they allow ultrasensitive SERS detection of a neurotransmitter with extremely low Raman activity. This simple method provides many opportunities for engineering plasmonics for ultrasensitive detection and highly efficient photon collection.

Repeated Solid-state Dewetting of Thin Gold Films for Nanogap-rich Plasmonic Nanoislands

PubMed Central

Kang, Minhee; Park, Sang-Gil; Jeong, Ki-Hun

2015-01-01

This work reports a facile wafer-level fabrication for nanogap-rich gold nanoislands for highly sensitive surface enhanced Raman scattering (SERS) by repeating solid-state thermal dewetting of thin gold film. The method provides enlarged gold nanoislands with small gap spacing, which increase the number of electromagnetic hotspots and thus enhance the extinction intensity as well as the tunability for plasmon resonance wavelength. The plasmonic nanoislands from repeated dewetting substantially increase SERS enhancement factor over one order-of-magnitude higher than those from a single-step dewetting process and they allow ultrasensitive SERS detection of a neurotransmitter with extremely low Raman activity. This simple method provides many opportunities for engineering plasmonics for ultrasensitive detection and highly efficient photon collection. PMID:26469768

Ultrasensitive aptamer-based protein detection via a dual amplified biocatalytic strategy

PubMed Central

Xiang, Yun; Zhang, Yuyong; Qian, Xiaoqing; Chai, Yaqin; Wang, Joseph; Yuan, Ruo

2010-01-01

We present an ultrasensitive aptasensor for electronic monitoring of proteins through a dual amplified strategy in this paper. The target protein thrombin is sandwiched between an electrode surface confined aptamer and an aptamer-enzyme-carbon nanotube bioconjugate. The analytical signal amplification is achieved by coupling the signal amplification nature of multiple enzymes with the biocatalytic signal enhancement of redox-recycling. Our novel dramatic signal amplification strategy, with a detection limit of 8.3 fM, shows about 4 orders of magnitude improvement in sensitivity for thrombin detection compared to other universal single enzyme-based assay. This makes our approach an attractive alternative to other common PCR-based signal amplification in ultralow level of protein detection. PMID:20452761

Proteomic analysis of single mammalian cells enabled by microfluidic nanodroplet sample preparation and ultrasensitive nanoLC-MS.

PubMed

Zhu, Ying; Clair, Geremy; Chrisler, William; Shen, Yufeng; Zhao, Rui; Shukla, Anil; Moore, Ronald; Misra, Ravi; Pryhuber, Gloria; Smith, Richard; Ansong, Charles; Kelly, Ryan T

2018-05-24

We report on the quantitative proteomic analysis of single mammalian cells. Fluorescence-activated cell sorting was employed to deposit cells into a newly developed nanodroplet sample processing chip, after which samples were analysed by ultrasensitive nanoLC-MS. An average of ~670 protein groups were confidently identified from single HeLa cells, which is a far greater level of proteome coverage for single cells than has been previously reported. We demonstrate that the single cell proteomics platform can be used to differentiate cell types from enzyme-dissociated human lung primary cells and identify specific protein markers for epithelial and mesenchymal cells. © 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Single Nanochannel-Aptamer-Based Biosensor for Ultrasensitive and Selective Cocaine Detection.

PubMed

Wang, Jian; Hou, Jue; Zhang, Huacheng; Tian, Ye; Jiang, Lei

2018-01-17

Ultrasensitive and selective detection of molecules at nano or sub-nanomolar level is very important for many areas such as early diagnosis and drug testing. Herein, we report a high-sensitive cocaine sensor based on a single nanochannel coupled with DNA aptamers. The single nanochannel-aptamer-based biosensor can recognize cocaine molecules with an excellent sensitivity and good selectivity. A linear relationship between target cocaine concentration and output ionic current is obtained in a wide concentration range of cocaine from 1 nM to 10 μM. The cocaine sensor also shows a detection limit down to 1 nM. This study provides a new avenue to develop new nanochannel-aptamer-based biosensors for rapid and ultratrace detection of a variety of illicit drugs.

Ultra-Sensitive Photoreceiver Boosts Data Transmission

NASA Technical Reports Server (NTRS)

2007-01-01

NASA depends on advanced, ultra-sensitive photoreceivers and photodetectors to provide high-data communications and pinpoint image-detection and -recognition capabilities from great distances. In 2003, Epitaxial Technologies LLC was awarded a Small Business Innovation Research (SBIR) contract from Goddard Space Flight Center to address needs for advanced sensor components. Epitaxial developed a photoreciever capable of single proton sensitivity that is also smaller, lighter, and requires less power than its predecessor. This receiver operates in several wavelength ranges; will allow data rate transmissions in the terabit range; and will enhance Earth-based missions for remote sensing of crops and other natural resources, including applications for fluorescence and phosphorescence detection. Widespread military and civilian applications are anticipated, especially through enhancing fiber optic communications, laser imaging, and laser communications.

Ultrasensitive Single Fluorescence-Labeled Probe-Mediated Single Universal Primer-Multiplex-Droplet Digital Polymerase Chain Reaction for High-Throughput Genetically Modified Organism Screening.

PubMed

Niu, Chenqi; Xu, Yuancong; Zhang, Chao; Zhu, Pengyu; Huang, Kunlun; Luo, Yunbo; Xu, Wentao

2018-05-01

As genetically modified (GM) technology develops and genetically modified organisms (GMOs) become more available, GMOs face increasing regulations and pressure to adhere to strict labeling guidelines. A singleplex detection method cannot perform the high-throughput analysis necessary for optimal GMO detection. Combining the advantages of multiplex detection and droplet digital polymerase chain reaction (ddPCR), a single universal primer-multiplex-ddPCR (SUP-M-ddPCR) strategy was proposed for accurate broad-spectrum screening and quantification. The SUP increases efficiency of the primers in PCR and plays an important role in establishing a high-throughput, multiplex detection method. Emerging ddPCR technology has been used for accurate quantification of nucleic acid molecules without a standard curve. Using maize as a reference point, four heterologous sequences ( 35S, NOS, NPTII, and PAT) were selected to evaluate the feasibility and applicability of this strategy. Surprisingly, these four genes cover more than 93% of the transgenic maize lines and serve as preliminary screening sequences. All screening probes were labeled with FAM fluorescence, which allows the signals from the samples with GMO content and those without to be easily differentiated. This fiveplex screening method is a new development in GMO screening. Utilizing an optimal amplification assay, the specificity, limit of detection (LOD), and limit of quantitation (LOQ) were validated. The LOD and LOQ of this GMO screening method were 0.1% and 0.01%, respectively, with a relative standard deviation (RSD) < 25%. This method could serve as an important tool for the detection of GM maize from different processed, commercially available products. Further, this screening method could be applied to other fields that require reliable and sensitive detection of DNA targets.

Compatible immuno-NASBA LOC device for quantitative detection of waterborne pathogens: design and validation.

PubMed

Zhao, Xinyan; Dong, Tao; Yang, Zhaochu; Pires, Nuno; Høivik, Nils

2012-02-07

Waterborne pathogens usually pose a global threat to animals and human beings. There has been a growing demand for convenient and sensitive tools to detect the potential emerging pathogens in water. In this study, a lab-on-a-chip (LOC) device based on the real-time immuno-NASBA (immuno-nucleic acid sequence-based amplification) assay was designed, fabricated and verified. The disposable immuno-NASBA chip is modelled on a 96-well ELISA microplate, which contains 43 reaction chambers inside the bionic channel networks. All valves are designed outside the chip and are reusable. The sample and reagent solutions were pushed into each chamber in turn, which was controlled by the valve system. Notably, the immuno-NASBA chip is completely compatible with common microplate readers in a biological laboratory, and can distinguish multiple waterborne pathogens in water samples quantitatively and simultaneously. The performance of the LOC device was demonstrated by detecting the presence of a synthetic peptide, ACTH (adrenocorticotropic hormone) and two common waterborne pathogens, Escherichia coli (E. coli) and rotavirus, in artificial samples. The results indicated that the LOC device has the potential to quantify traces of waterborne pathogens at femtomolar levels with high specificity, although the detection process was still subject to some factors, such as ribonuclease (RNase) contamination and non-specific adsorption. As an ultra-sensitive tool to quantify waterborne pathogens, the LOC device can be used to monitor water quality in the drinking water system. Furthermore, a series of compatible high-throughput LOC devices for monitoring waterborne pathogens could be derived from this prototype with the same design idea, which may render the complicated immuno-NASBA assays convenient to common users without special training.

Rapid Microarray Detection of DNA and Proteins in Microliter Volumes with SPR Imaging Measurements

PubMed Central

Seefeld, Ting Hu; Zhou, Wen-Juan; Corn, Robert M.

2011-01-01

A four chamber microfluidic biochip is fabricated for the rapid detection of multiple proteins and nucleic acids from microliter volume samples with the technique of surface plasmon resonance imaging (SPRI). The 18 mm × 18 mm biochip consists of four 3 μL microfluidic chambers attached to an SF10 glass substrate, each of which contains three individually addressable SPRI gold thin film microarray elements. The twelve element (4 × 3) SPRI microarray consists of gold thin film spots (1 mm2 area; 45 nm thickness) each in individually addressable 0.5 μL volume microchannels. Microarrays of single-stranded DNA and RNA (ssDNA and ssRNA respectively) are fabricated by either chemical and/or enzymatic attachment reactions in these microchannels; the SPRI microarrays are then used to detect femtomole amounts (nanomolar concentrations) of DNA and proteins (single stranded DNA binding protein and thrombin via aptamer-protein bioaffinity interactions). Microarrays of ssRNA microarray elements were also used for the ultrasensitive detection of zeptomole amounts (femtomolar concentrations) of DNA via the technique of RNase H-amplified SPRI. Enzymatic removal of ssRNA from the surface due to the hybridization adsorption of target ssDNA is detected as a reflectivity decrease in the SPR imaging measurements. The observed reflectivity loss was proportional to the log of the target ssDNA concentration with a detection limit of 10 fM or 30 zeptomoles (18,000 molecules). This enzymatic amplified ssDNA detection method is not limited by diffusion of ssDNA to the interface, and thus is extremely fast, requiring only 200 seconds in the microliter volume format. PMID:21488682

Simulation and fabrication of a new novel 3D injectable biosensor for high throughput genomics and proteomics in a lab-on-a-chip device.

PubMed

Esfandyarpour, Rahim; Esfandyarpour, Hesaam; Harris, James S; Davis, Ronald W

2013-11-22

Biosensors are used for the detection of biochemical molecules such as proteins and nucleic acids. Traditional techniques, such as enzyme-linked immuno-sorbent assay (ELISA), are sensitive but require several hours to yield a result and usually require the attachment of a fluorophore molecule to the target molecule. Micromachined biosensors that employ electrical detection are now being developed. Here we describe one such device, which is ultrasensitive, real-time, label free and localized. It is called the nanoneedle biosensor and shows promise to overcome some of the current limitations of biosensors. The key element of this device is a 10 nm wide annular gap at the end of the needle, which is the sensitive part of the sensor. The total diameter of the sensor is about 100 nm. Any change in the population of molecules in this gap results in a change of impedance across the gap. Single molecule detection should be possible because the sensory part of the sensor is in the range of bio-molecules of interest. To increase throughput we can flow the solution containing the target molecules over an array of such structures, each with its own integrated read-out circuitry to allow 'real-time' detection (i.e. several minutes) of label free molecules without sacrificing sensitivity. To fabricate the arrays we used electron beam lithography together with associated pattern transfer techniques. Preliminary measurements on individual needle structures in water are consistent with the design. Since the proposed sensor has a rigid nano-structure, this technology, once fully developed, could ultimately be used to directly monitor protein quantities within a single living cell, an application that would have significant utility for drug screening and studying various intracellular signaling pathways.

Insect Cell-Derived Cofactors Become Fully Functional after Proteinase K and Heat Treatment for High-Fidelity Amplification of Glycosylphosphatidylinositol-Anchored Recombinant Scrapie and BSE Prion Proteins

PubMed Central

Imamura, Morikazu; Kato, Nobuko; Okada, Hiroyuki; Yoshioka, Miyako; Iwamaru, Yoshifumi; Shimizu, Yoshihisa; Mohri, Shirou; Yokoyama, Takashi; Murayama, Yuichi

2013-01-01

The central event in prion infection is the conformational conversion of host-encoded cellular prion protein (PrPC) into the pathogenic isoform (PrPSc). Diverse mammalian species possess the cofactors required for in vitro replication of PrPSc by protein-misfolding cyclic amplification (PMCA), but lower organisms, such as bacteria, yeasts, and insects, reportedly lack the essential cofactors. Various cellular components, such as RNA, lipids, and other identified cofactor molecules, are commonly distributed in both eukaryotes and prokaryotes, but the reasons for the absence of cofactor activity in lower organisms remain to be elucidated. Previously, we reported that brain-derived factors were necessary for the in vitro replication of glycosylphosphatidylinositol-anchored baculovirus-derived recombinant PrP (Bac-PrP). Here, we demonstrate that following protease digestion and heat treatment, insect cell lysates had the functional cofactor activity required for Bac-PrP replication by PMCA. Mammalian PrPSc seeds and Bac-PrPSc generated by PMCA using Bac-PrP and insect cell-derived cofactors showed similar pathogenicity and produced very similar lesions in the brains of inoculated mice. These results suggested that the essential cofactors required for the high-fidelity replication of mammalian PrPSc were present in the insect cells but that the cofactor activity was masked or inhibited in the native state. We suggest that not only RNA, but also DNA, are the key components of PMCA, although other cellular factors were necessary for the expression of the cofactor activity of nucleic acids. PMCA using only insect cell-derived substances (iPMCA) was highly useful for the ultrasensitive detection of PrPSc of some prion strains. PMID:24367521

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.

Detection of human papillomavirus type 16 in oropharyngeal squamous cell carcinoma using droplet digital polymerase chain reaction.

PubMed

Biron, Vincent L; Kostiuk, Morris; Isaac, Andre; Puttagunta, Lakshmi; O'Connell, Daniel A; Harris, Jeffrey; Côté, David W J; Seikaly, Hadi

2016-05-15

The incidence of oropharyngeal squamous cell carcinoma caused by oncogenic HPV (HPV-OPSCC) is rising worldwide. HPV-OPSCC is commonly diagnosed by RT-qPCR of HPV-16 E6 and E7 oncoproteins or by cyclin-dependent kinase inhibitor 2A, multiple tumor suppressor 1 (p16) immunohistochemistry (IHC). Droplet digital PCR (ddPCR) has been recently reported as ultra-sensitive and highly precise method of nucleic acid quantification for biomarker analysis. We aimed to validate this method for the detection of HPV-16 E6 and E7 in HPV-OPSCC. Participants were recruited from January 2015-November 2015 at initial presentation to the University of Alberta Head and Neck Oncology Clinic. RNA was extracted, purified and quantified from prospectively collected participant tissues, and ddPCR was performed with fluorescent probes detecting HPV-16 E6 and E7. Results from ddPCR were compared with p16 IHC performed by clinical pathology as standard of care. Head and neck tissues were prospectively obtained from 68 participants including 29 patients with OPSCC, 29 patients with non-OPSCC and 10 patients without carcinoma. 79.2% of patients with OPSCC were p16 positive. The sensitivity and specificity of ddPCR HPV E6/E7 compared with p16 IHC in OPSCC was 91.3 and 100%, respectively. The amount of target RNA used was ≤1 ng, 20-50 times lower than reported by other for RT-qPCR HPV E6/E7. The ddPCR of HPV E6/E7 is a novel and highly specific method of detecting HPV-16 in OPSCC. Cancer 2016;122:1544-51. © 2016 American Cancer Society. © 2016 American Cancer Society.

Simulation and fabrication of a new novel 3D injectable biosensor for high throughput genomics and proteomics in a lab-on-a-chip device

NASA Astrophysics Data System (ADS)

Esfandyarpour, Rahim; Esfandyarpour, Hesaam; Harris, James S.; Davis, Ronald W.

2013-11-01

Biosensors are used for the detection of biochemical molecules such as proteins and nucleic acids. Traditional techniques, such as enzyme-linked immuno-sorbent assay (ELISA), are sensitive but require several hours to yield a result and usually require the attachment of a fluorophore molecule to the target molecule. Micromachined biosensors that employ electrical detection are now being developed. Here we describe one such device, which is ultrasensitive, real-time, label free and localized. It is called the nanoneedle biosensor and shows promise to overcome some of the current limitations of biosensors. The key element of this device is a 10 nm wide annular gap at the end of the needle, which is the sensitive part of the sensor. The total diameter of the sensor is about 100 nm. Any change in the population of molecules in this gap results in a change of impedance across the gap. Single molecule detection should be possible because the sensory part of the sensor is in the range of bio-molecules of interest. To increase throughput we can flow the solution containing the target molecules over an array of such structures, each with its own integrated read-out circuitry to allow ‘real-time’ detection (i.e. several minutes) of label free molecules without sacrificing sensitivity. To fabricate the arrays we used electron beam lithography together with associated pattern transfer techniques. Preliminary measurements on individual needle structures in water are consistent with the design. Since the proposed sensor has a rigid nano-structure, this technology, once fully developed, could ultimately be used to directly monitor protein quantities within a single living cell, an application that would have significant utility for drug screening and studying various intracellular signaling pathways.

Introductory Remarks

NASA Astrophysics Data System (ADS)

Lu, Yi; Li, Yingfu

The emergence of a large number of natural and artificial functional nucleic acids (FNAs; aptamers and nucleic acid enzymes, collectively termed functional nucleic acids in this book) has generated tremendous enthusiasm and new opportunities for molecular scientists from diverse disciplines to devise new concepts and applications. In this volume, we have assembled some leading experts to provide a timely account of recent progress in sensing and other analytical applications that explore functional nucleic acids.

Interactive fluorophore and quencher pairs for labeling fluorescent nucleic acid hybridization probes.

PubMed

Marras, Salvatore A E

2008-03-01

The use of fluorescent nucleic acid hybridization probes that generate a fluorescence signal only when they bind to their target enables real-time monitoring of nucleic acid amplification assays. Real-time nucleic acid amplification assays markedly improves the ability to obtain qualitative and quantitative results. Furthermore, these assays can be carried out in sealed tubes, eliminating carryover contamination. Fluorescent nucleic acid hybridization probes are available in a wide range of different fluorophore and quencher pairs. Multiple hybridization probes, each designed for the detection of a different nucleic acid sequence and each labeled with a differently colored fluorophore, can be added to the same nucleic acid amplification reaction, enabling the development of high-throughput multiplex assays. In order to develop robust, highly sensitive and specific real-time nucleic acid amplification assays it is important to carefully select the fluorophore and quencher labels of hybridization probes. Selection criteria are based on the type of hybridization probe used in the assay, the number of targets to be detected, and the type of apparatus available to perform the assay. This article provides an overview of different aspects of choosing appropriate labels for the different types of fluorescent hybridization probes used with different types of spectrofluorometric thermal cyclers currently available.

Nucleic Acid Extraction from Synthetic Mars Analog Soils for in situ Life Detection.

PubMed

Mojarro, Angel; Ruvkun, Gary; Zuber, Maria T; Carr, Christopher E

2017-08-01

Biological informational polymers such as nucleic acids have the potential to provide unambiguous evidence of life beyond Earth. To this end, we are developing an automated in situ life-detection instrument that integrates nucleic acid extraction and nanopore sequencing: the Search for Extra-Terrestrial Genomes (SETG) instrument. Our goal is to isolate and determine the sequence of nucleic acids from extant or preserved life on Mars, if, for example, there is common ancestry to life on Mars and Earth. As is true of metagenomic analysis of terrestrial environmental samples, the SETG instrument must isolate nucleic acids from crude samples and then determine the DNA sequence of the unknown nucleic acids. Our initial DNA extraction experiments resulted in low to undetectable amounts of DNA due to soil chemistry-dependent soil-DNA interactions, namely adsorption to mineral surfaces, binding to divalent/trivalent cations, destruction by iron redox cycling, and acidic conditions. Subsequently, we developed soil-specific extraction protocols that increase DNA yields through a combination of desalting, utilization of competitive binders, and promotion of anaerobic conditions. Our results suggest that a combination of desalting and utilizing competitive binders may establish a "universal" nucleic acid extraction protocol suitable for analyzing samples from diverse soils on Mars. Key Words: Life-detection instruments-Nucleic acids-Mars-Panspermia. Astrobiology 17, 747-760.

Self-assembling nucleic acid delivery vehicles via linear, water-soluble, cyclodextrin-containing polymers.

PubMed

Davis, M E; Pun, S H; Bellocq, N C; Reineke, T M; Popielarski, S R; Mishra, S; Heidel, J D

2004-01-01

Non-viral (synthetic) nucleic acid delivery systems have the potential to provide for the practical application of nucleic acid-based therapeutics. We have designed and prepared a tunable, non-viral nucleic acid delivery system that self-assembles with nucleic acids and centers around a new class of polymeric materials; namely, linear, water-soluble cyclodextrin-containing polymers. The relationships between polymer structure and gene delivery are illustrated, and the roles of the cyclodextrin moieties for minimizing toxicity and forming inclusion complexes in the self-assembly processes are highlighted. This vehicle is the first example of a polymer-based gene delivery system formed entirely by self-assembly.

Nucleic Acid-Induced Resistance to Viral Infection

PubMed Central

Takano, Kouichi; Warren, Joel; Jensen, Keith E.; Neal, Alan L.

1965-01-01

Takano, Kouichi (Chas. Pfizer & Co., Inc., Terre Haute, Ind.), Joel Warren, Keith E. Jensen, and Alan L. Neal. Nucleic acid resistance to viral infection. J. Bacteriol. 90:1542–1547. 1965.—Administration of nonviral nucleic acids to mice increased their resistance to a subsequent infection with influenza or encephalomyocarditis viruses. Injection of ribonucleic acid or deoxyribonucleic acid by peripheral routes did not modify susceptibility to intranasal infection. Lung tissue extracts from animals previously treated with yeast nucleic acid inhibited the growth of vaccinia and influenza viruses. The protective effect of exogenous nucleic acids persisted in mice for several days, but gradually diminished to undetectable levels. PMID:4285332

Prospects for nucleic acid-based therapeutics against hepatitis C virus.

PubMed

Lee, Chang Ho; Kim, Ji Hyun; Lee, Seong-Wook

2013-12-21

In this review, we discuss recent advances in nucleic acid-based therapeutic technologies that target hepatitis C virus (HCV) infection. Because the HCV genome is present exclusively in RNA form during replication, various nucleic acid-based therapeutic approaches targeting the HCV genome, such as ribozymes, aptamers, siRNAs, and antisense oligonucleotides, have been suggested as potential tools against HCV. Nucleic acids are potentially immunogenic and typically require a delivery tool to be utilized as therapeutics. These limitations have hampered the clinical development of nucleic acid-based therapeutics. However, despite these limitations, nucleic acid-based therapeutics has clinical value due to their great specificity, easy and large-scale synthesis with chemical methods, and pharmaceutical flexibility. Moreover, nucleic acid therapeutics are expected to broaden the range of targetable molecules essential for the HCV replication cycle, and therefore they may prove to be more effective than existing therapeutics, such as interferon-α and ribavirin combination therapy. This review focuses on the current status and future prospects of ribozymes, aptamers, siRNAs, and antisense oligonucleotides as therapeutic reagents against HCV.

Single-stranded nucleic acids promote SAMHD1 complex formation.

PubMed

Tüngler, Victoria; Staroske, Wolfgang; Kind, Barbara; Dobrick, Manuela; Kretschmer, Stefanie; Schmidt, Franziska; Krug, Claudia; Lorenz, Mike; Chara, Osvaldo; Schwille, Petra; Lee-Kirsch, Min Ae

2013-06-01

SAM domain and HD domain-containing protein 1 (SAMHD1) is a dGTP-dependent triphosphohydrolase that degrades deoxyribonucleoside triphosphates (dNTPs) thereby limiting the intracellular dNTP pool. Mutations in SAMHD1 cause Aicardi-Goutières syndrome (AGS), an inflammatory encephalopathy that mimics congenital viral infection and that phenotypically overlaps with the autoimmune disease systemic lupus erythematosus. Both disorders are characterized by activation of the antiviral cytokine interferon-α initiated by immune recognition of self nucleic acids. Here we provide first direct evidence that SAMHD1 associates with endogenous nucleic acids in situ. Using fluorescence cross-correlation spectroscopy, we demonstrate that SAMHD1 specifically interacts with ssRNA and ssDNA and establish that nucleic acid-binding and formation of SAMHD1 complexes are mutually dependent. Interaction with nucleic acids and complex formation do not require the SAM domain, but are dependent on the HD domain and the C-terminal region of SAMHD1. We finally demonstrate that mutations associated with AGS exhibit both impaired nucleic acid-binding and complex formation implicating that interaction with nucleic acids is an integral aspect of SAMHD1 function.

Portable nucleic acid thermocyclers.

PubMed

Almassian, David R; Cockrell, Lisa M; Nelson, William M

2013-11-21

A nucleic acid thermal cycler is considered to be portable if it is under ten pounds, easily carried by one individual, and battery powered. Nucleic acid amplification includes both polymerase chain reaction (e.g. PCR, RT-PCR) and isothermal amplification (e.g. RPA, HDA, LAMP, NASBA, RCA, ICAN, SMART, SDA). There are valuable applications for portable nucleic acid thermocyclers in fields that include clinical diagnostics, biothreat detection, and veterinary testing. A system that is portable allows for the distributed detection of targets at the point of care and a reduction of the time from sample to answer. The designer of a portable nucleic acid thermocycler must carefully consider both thermal control and the detection of amplification. In addition to thermal control and detection, the designer may consider the integration of a sample preparation subsystem with the nucleic acid thermocycler. There are a variety of technologies that can achieve accurate thermal control and the detection of nucleic acid amplification. Important evaluation criteria for each technology include maturity, power requirements, cost, sensitivity, speed, and manufacturability. Ultimately the needs of a particular market will lead to user requirements that drive the decision between available technologies.

Nucleic acid in-situ hybridization detection of infectious agents

NASA Astrophysics Data System (ADS)

Thompson, Curtis T.

2000-04-01

Limitations of traditional culture methods and newer polymerase chain reaction (PCR)-based methods for detection and speciation of infectious agents demonstrate the need for more rapid and better diagnostics. Nucleic acid hybridization is a detection technology that has gained wide acceptance in cancer and prenatal cytogenetics. Using a modification of the nucleic acid hybridization technique known as fluorescence in-situ hybridization, infectious agents can be detected in a variety of specimens with high sensitivity and specificity. The specimens derive from all types of human and animal sources including body fluids, tissue aspirates and biopsy material. Nucleic acid hybridization can be performed in less than one hour. The result can be interpreted either using traditional fluorescence microscopy or automated platforms such as micro arrays. This paper demonstrates proof of concept for nucleic acid hybridization detection of different infectious agents. Interpretation within a cytologic and histologic context is possible with fluorescence microscopic analysis, thereby providing confirmatory evidence of hybridization. With careful probe selection, nucleic acid hybridization promises to be a highly sensitive and specific practical diagnostic alternative to culture, traditional staining methods, immunohistochemistry and complicated nucleic acid amplification tests.

Biosensors: Viruses for ultrasensitive assays

NASA Astrophysics Data System (ADS)

Donath, Edwin

2009-04-01

A three-dimensional assay based on genetically engineered viral nanoparticles and nickel nanohairs can detect much lower levels of protein markers associated with heart attacks than conventional assays.

Formation of thin film like assembly of exfoliated C3N4 nanoflakes by solvent non-evaporative method using centrifuge

NASA Astrophysics Data System (ADS)

Tejasvi, Ravi; Basu, Suddhasatwa

2017-12-01

A simple method for depositing a thin film of nanomaterial on a substrate using centrifugation technique has been developed, whereby solvent evaporation is prevented and solvent reuse is possible. The centrifuge technique of deposition yields uniform, smooth thin film irrespective of substrate surface texture. The deposited TiO2/eC3N4 film studied, through field emission scanning electron microscope, atomic force microscope, and optical surface profilometer, shows variation in surface roughness on the basis of centrifugation speeds. Initially film coverage improves and surface roughness decreases with the increase in rpm of the centrifuge and the surface roughness slightly increases with further increase in rpm. The photoelectrochemical studies of TiO2/eC3N4 films suggest that the centrifuge technique forms better heterojunctions compared to that by spin coating technique leading to enhanced photoelectrochemical water splitting.

Carbon quantum dots coated BiVO{sub 4} inverse opals for enhanced photoelectrochemical hydrogen generation

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

Nan, Feng; Shen, Mingrong; Fang, Liang, E-mail: zhkang@suda.edu.cn, E-mail: lfang@suda.edu.cn

Carbon quantum dots (CQDs) coated BiVO{sub 4} inverse opal (io-BiVO{sub 4}) structure that shows dramatic improvement of photoelectrochemical hydrogen generation has been fabricated using electrodeposition with a template. The io-BiVO{sub 4} maximizes photon trapping through slow light effect, while maintaining adequate surface area for effective redox reactions. CQDs are then incorporated to the io-BiVO{sub 4} to further improve the photoconversion efficiency. Due to the strong visible light absorption property of CQDs and enhanced separation of the photoexcited electrons, the CQDs coated io-BiVO{sub 4} exhibit a maximum photo-to-hydrogen conversion efficiency of 0.35%, which is 6 times higher than that of themore » pure BiVO{sub 4} thin films. This work is a good example of designing composite photoelectrode by combining quantum dots and photonic crystal.« less

Enhanced photoelectrochemical water splitting of BiVO4 photonic crystal photoanode by decorating with MoS2 nanosheets

NASA Astrophysics Data System (ADS)

Nan, Feng; Cai, Tianyi; Ju, Sheng; Fang, Liang

2018-04-01

Bismuth vanadate (BiVO4) has been considered as one of the promising Photoelectrochemical (PEC) photoanode materials. However, the performances remain poorly rated due to inefficient carrier separation, short carrier diffusion length, and sluggish water oxidation kinetics. Herein, a photoanode consisting of MoS2 nanosheet coating on the three-dimensional ordered BiVO4 inverse opal is fabricated by a facile combination of nanosphere lithography and hydrothermal methods. By taking advantage of the photonic crystal and two-dimensional material, the optimized MoS2/BiVO4 inverse opal photoanode exhibits a 560% improvement of the photocurrent density and threefold enhancement of the incident photon-to-current efficiency than that of the pristine BiVO4 film photoanode. Systematic studies reveal that the excellent PEC activity should be attributed to enhanced light harvesting and charge separation efficiency.

Photoelectrochemical response of GaN, InGaN, and GaNP nanowire ensembles

NASA Astrophysics Data System (ADS)

Philipps, Jan M.; Hölzel, Sara; Hille, Pascal; Schörmann, Jörg; Chatterjee, Sangam; Buyanova, Irina A.; Eickhoff, Martin; Hofmann, Detlev M.

2018-05-01

The photoelectrochemical responses of GaN, GaNP, and InGaN nanowire ensembles are investigated by the electrical bias dependent photoluminescence, photocurrent, and spin trapping experiments. The results are explained in the frame of the surface band bending model. The model is sufficient for InGaN nanowires, but for GaN nanowires the electrochemical etching processes in the anodic regime have to be considered additionally. These processes lead to oxygen rich surface (GaxOy) conditions as evident from energy dispersive X-ray fluorescence. For the GaNP nanowires, a bias dependence of the carrier transfer to the electrolyte is not reflected in the photoluminescence response, which is tentatively ascribed to a different origin of radiative recombination in this material as compared to (In)GaN. The corresponding consequences for the applications of the materials for water splitting or pH-sensing will be discussed.

Multiple exciton generation for photoelectrochemical hydrogen evolution reactions with quantum yields exceeding 100%

DOE PAGES

Yan, Yong; Crisp, Ryan W.; Gu, Jing; ...

2017-04-03

Multiple exciton generation (MEG) in quantum dots (QDs) has the potential to greatly increase the power conversion efficiency in solar cells and in solar-fuel production. During the MEG process, two electron-hole pairs (excitons) are created from the absorption of one high-energy photon, bypassing hot-carrier cooling via phonon emission. Here we demonstrate that extra carriers produced via MEG can be used to drive a chemical reaction with quantum efficiency above 100%. We developed a lead sulfide (PbS) QD photoelectrochemical cell that is able to drive hydrogen evolution from aqueous Na 2S solution with a peak external quantum efficiency exceeding 100%. QDmore » photoelectrodes that were measured all demonstrated MEG when the incident photon energy was larger than 2.7 times the bandgap energy. Finally, our results demonstrate a new direction in exploring high-efficiency approaches to solar fuels.« less

Semiconductor-Based Photoelectrochemical Conversion of Carbon Dioxide: Stepping Towards Artificial Photosynthesis.

PubMed

Pang, Hong; Masuda, Takuya; Ye, Jinhua

2018-01-18

The photoelectrochemical (PEC) carbon dioxide reduction process stands out as a promising avenue for the conversion of solar energy into chemical feedstocks, among various methods available for carbon dioxide mitigation. Semiconductors derived from cheap and abundant elements are interesting candidates for catalysis. Whether employed as intrinsic semiconductors or hybridized with metallic cocatalysts, biocatalysts, and metal molecular complexes, semiconductor photocathodes exhibit good performance and low overpotential during carbon dioxide reduction. Apart from focusing on carbon dioxide reduction materials and chemistry, PEC cells towards standalone devices that use photohybrid electrodes or solar cells have also been a hot topic in recent research. An overview of the state-of-the-art progress in PEC carbon dioxide reduction is presented and a deep understanding of the catalysts of carbon dioxide reduction is also given. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hierarchical Cu2O foam/g-C3N4 photocathode for photoelectrochemical hydrogen production

NASA Astrophysics Data System (ADS)

Ma, Xinzhou; Zhang, Jingtao; Wang, Biao; Li, Qiuguo; Chu, Sheng

2018-01-01

Solar photoelectrochemical (PEC) hydrogen production is a promising way for solving energy and environment problems. Earth-abundant Cu2O is a potential light absorber for PEC hydrogen production. In this article, hierarchical porous Cu2O foams are prepared by thermal oxidation of the electrochemically deposited Cu foams. PEC performances of the Cu2O foams are systematically studied and discussed. Benefiting from their higher light harvesting and more efficient charge separation, the Cu2O foams demonstrate significantly enhanced photocurrents and photostability compared to their film counterparts. Moreover, by integrating g-C3N4, hierarchical Cu2O foam/g-C3N4 composites are prepared with further improved photocurrent and photostability, appearing to be potential photocathodes for solar PEC hydrogen production. This study may provide a new and useful insight for the development of Cu2O-based photocathodes for PEC hydrogen production.

Band structure engineering of semiconductors for enhanced photoelectrochemical water splitting: The case of TiO2

NASA Astrophysics Data System (ADS)

Yin, Wan-Jian; Tang, Houwen; Wei, Su-Huai; Al-Jassim, Mowafak M.; Turner, John; Yan, Yanfa

2010-07-01

Here, we propose general strategies for the rational design of semiconductors to simultaneously meet all of the requirements for a high-efficiency, solar-driven photoelectrochemical (PEC) water-splitting device. As a case study, we apply our strategies for engineering the popular semiconductor, anatase TiO2 . Previous attempts to modify known semiconductors such as TiO2 have often focused on a particular individual criterion such as band gap, neglecting the possible detrimental consequence to other important criteria. Density-functional theory calculations reveal that with appropriate donor-acceptor coincorporation alloys with anatase TiO2 hold great potential to satisfy all of the criteria for a viable PEC device. We predict that (Mo, 2N) and (W, 2N) are the best donor-acceptor combinations in the low-alloy concentration regime whereas (Nb, N) and (Ta, N) are the best choice of donor-acceptor pairs in the high-alloy concentration regime.

Enhanced photoelectrochemical water splitting by oxides heterojunction photocathode coupled with Ag.

PubMed

Lu, Xue; Liu, Zhifeng

2017-08-14

A novel one-dimensional Co 3 O 4 /CuO/Ag composite structure film was directly grown on indium tin oxide glass substrate by a simple hydrothermal method and electrodeposition method. The film was employed for the first time as a photocathode for photoelectrochemical (PEC) water splitting to generate hydrogen. The photocurrent density of the Co 3 O 4 /CuO/Ag composite structure achieved -5.13 mA cm -2 at -0.2 V vs. RHE, which is roughly 12.8 times that of 1D Co 3 O 4 nanowires and 3.31 times Co 3 O 4 /CuO heterojunction photocathodes. The enhanced PEC performance of this Co 3 O 4 /CuO/Ag composite structure ascribes increased light-harvesting and light-absorption, distensible photoresponse range, decreased interface charge transfer resistance, and improved photogenerated electron-hole pairs transfer and separation.

Efficient water reduction with gallium phosphide nanowires

PubMed Central

Standing, Anthony; Assali, Simone; Gao, Lu; Verheijen, Marcel A.; van Dam, Dick; Cui, Yingchao; Notten, Peter H. L.; Haverkort, Jos E. M.; Bakkers, Erik P. A. M.

2015-01-01

Photoelectrochemical hydrogen production from solar energy and water offers a clean and sustainable fuel option for the future. Planar III/V material systems have shown the highest efficiencies, but are expensive. By moving to the nanowire regime the demand on material quantity is reduced, and new materials can be uncovered, such as wurtzite gallium phosphide, featuring a direct bandgap. This is one of the few materials combining large solar light absorption and (close to) ideal band-edge positions for full water splitting. Here we report the photoelectrochemical reduction of water, on a p-type wurtzite gallium phosphide nanowire photocathode. By modifying geometry to reduce electrical resistance and enhance optical absorption, and modifying the surface with a multistep platinum deposition, high current densities and open circuit potentials were achieved. Our results demonstrate the capabilities of this material, even when used in such low quantities, as in nanowires. PMID:26183949

Scalable high-precision tuning of photonic resonators by resonant cavity-enhanced photoelectrochemical etching

PubMed Central

Gil-Santos, Eduardo; Baker, Christopher; Lemaître, Aristide; Gomez, Carmen; Leo, Giuseppe; Favero, Ivan

2017-01-01

Photonic lattices of mutually interacting indistinguishable cavities represent a cornerstone of collective phenomena in optics and could become important in advanced sensing or communication devices. The disorder induced by fabrication technologies has so far hindered the development of such resonant cavity architectures, while post-fabrication tuning methods have been limited by complexity and poor scalability. Here we present a new simple and scalable tuning method for ensembles of microphotonic and nanophotonic resonators, which enables their permanent collective spectral alignment. The method introduces an approach of cavity-enhanced photoelectrochemical etching in a fluid, a resonant process triggered by sub-bandgap light that allows for high selectivity and precision. The technique is presented on a gallium arsenide nanophotonic platform and illustrated by finely tuning one, two and up to five resonators. It opens the way to applications requiring large networks of identical resonators and their spectral referencing to external etalons. PMID:28117394

Ni-doped TiO2 nanotubes photoanode for enhanced photoelectrochemical water splitting

NASA Astrophysics Data System (ADS)

Dong, Zhenbiao; Ding, Dongyan; Li, Ting; Ning, Congqin

2018-06-01

Photoelectrochemical (PEC) water splitting hydrogen production provides a promising way for sustainable development. In this work, we prepared Ni-doped TiO2 (Ti-Ni-O) nanotubes through anodizing different Ti-Ni alloys and further annealing them at elevated temperatures, and reported their PEC water splitting performance. It was found that Ni doping could improve light absorption and facilitate separation of photo-excited electron-hole pair. The nanotubes fabricated on Ti-1 wt.% Ni alloy and annealed at 550 °C exhibited better PEC water splitting performance than those on Ti-10 wt.% Ni alloy. The photoconversion efficiency was 0.67%, which was 3.35 times the photoconversion efficiency of undoped TiO2. It demonstrated that it was feasible to fabricate high-performance Ti-Ni-O nanotubes on Ti-Ni alloys and used as photoanode for improving PEC water splitting.

Hydrogen and electricity production in a light-assisted microbial photoelectrochemical cell with CaFe2O4 photocathode

NASA Astrophysics Data System (ADS)

Chen, Qing-Yun; Zhang, Kai; Liu, Jian-Shan; Wang, Yun-Hai

2017-04-01

A microbial photoelectrochemical cell (MPEC) was designed with a p-type CaFe2O4 semiconductor as the photoelectrode for simultaneous hydrogen and electricity production under light illumination. The CaFe2O4 photoelectrode was synthesized by the sol-gel method and well characterized by x-ray diffraction, field emission scanning electron microscope, and UV-Vis-NIR spectrophotometer. The linear sweep voltammogram of the CaFe2O4 photoelectrode presented the cathodic photocurrent output. For the MPEC, with an external resistance of 2000 Ω, the maximum power density of 143 mW was obtained. Furthermore, with an external resistance of 100 Ω, the maximum hydrogen production rate of 6.7 μL·cm-2 could be achieved. The MPEC with CaFe2O4 photocathode was compared to MPEC with other photocathodes as well as photocatalytic water splitting technology.

Enhanced photoelectrochemical property of ZnO nanorods array synthesized on reduced graphene oxide for self-powered biosensing application.

PubMed

Kang, Zhuo; Gu, Yousong; Yan, Xiaoqin; Bai, Zhiming; Liu, Yichong; Liu, Shuo; Zhang, Xiaohui; Zhang, Zheng; Zhang, Xueji; Zhang, Yue

2015-02-15

We have realized the direct synthesis of ZnO nanorods (ZnO NRs) array on reduced graphene layer (rGO), and demonstrated the enhanced photoelectrochemical (PEC) property of the rGO/ZnO based photoanode under UV irradiation compared with the pristine ZnO NRs array. The introduction of the rGO layer resulted in a favorable energy band structure for electron migration, which finally led to the efficient photoinduced charge separation. Such nanostructure was subsequently employed for self-powered PEC biosensing of glutathione in the condition of 0 V bias, with a linear range from 10 to 200 µM, a detection limit of 2.17 µM, as well as excellent selectivity, reproducibility and stability. The results indicated the rGO/ZnO nanostructure is a competitive candidate in the PEC biosensing field. Copyright © 2014 Elsevier B.V. All rights reserved.

Influence of surface states of CuInS2 quantum dots in quantum dots sensitized photo-electrodes

NASA Astrophysics Data System (ADS)

Peng, Zhuoyin; Liu, Yueli; Wu, Lei; Zhao, Yinghan; Chen, Keqiang; Chen, Wen

2016-12-01

Surface states are significant factor for the enhancement of electrochemical performance in CuInS2 quantum dot sensitized photo-electrodes. DDT, OLA, MPA, and S2- ligand capped CuInS2 quantum dot sensitized photo-electrodes are prepared by thermolysis, solvethermal and ligand-exchange processes, respectively, and their optical properties and photoelectrochemical properties are investigated. The S2- ligand enhances the UV-vis absorption and electron-hole separation property as well as the excellent charge transfer performance of the photo-electrodes, which is attributed to the fact that the atomic S2- ligand for the interfacial region of quantum dots may improve the electron transfer rate. These S2--capped CuInS2 quantum dot sensitized photo-electrodes exhibit the excellent photoelectrochemical efficiency and IPCE peak value, which is higher than that of the samples with DDT, OLA and MPA ligands.