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Sample records for one-pot multicomponent coupling

  1. Titanium-catalyzed multicomponent couplings: efficient one-pot syntheses of nitrogen heterocycles.

    PubMed

    Odom, Aaron L; McDaniel, Tanner J

    2015-11-17

    Nitrogen-based heterocycles are important frameworks for pharmaceuticals, natural products, organic dyes for solar cells, and many other applications. Catalysis for the formation of heterocyclic scaffolds, like many C-C and C-N bond-forming reactions, has focused on the use of rare, late transition metals like palladium and gold. Our group is interested in the use of Earth-abundant catalysts based on titanium to generate heterocycles using multicomponent coupling strategies, often in one-pot reactions. To be of maximal utility, the catalysts need to be easily prepared from inexpensive reagents, and that has been one guiding principle in the research. For this purpose, a series of easily prepared pyrrole-based ligands has been developed. Titanium imido complexes are known to catalyze the hydroamination of alkynes, and this reaction has been used to advantage in the production of α,β-unsaturated imines from 1,3-enynes and pyrroles from 1,4-diynes. Likewise, catalyst design can be used to find complexes applicable to hydrohydrazination, coupling of a hydrazine and alkyne, which is a method for the production of hydrazones. Many of the hydrazones synthesized are converted to indoles through Fischer cyclization by addition of a Lewis acid. However, more complex products are available in a single catalytic cycle through coupling of isonitriles, primary amines, and alkynes to give tautomers of 1,3-diimines, iminoamination (IA). The products of IA are useful intermediates for the one-pot synthesis of pyrazoles, pyrimidines, isoxazoles, quinolines, and 2-amino-3-cyanopyridines. The regioselectivity of the reactions is elucidated in some detail for some of these heterocycles. The 2-amino-3-cyanopyridines are synthesized through isolable intermediates, 1,2-dihydro-2-iminopyridines, which undergo Dimroth rearrangement driven by aromatization of the pyridine ring; the proposed mechanism of the reaction is discussed. The IA-based heterocyclic syntheses can be accomplished

  2. One-Pot Multicomponent Coupling Methods for the Synthesis of Diastereo- and Enantioenriched (Z)-Trisubstituted Allylic Alcohols

    PubMed Central

    Kerrigan, Michael H.; Jeon, Sang-Jin; Chen, Young K.; Salvi, Luca; Carroll, Patrick J.; Walsh, Patrick J.

    2009-01-01

    (Z)-Trisubstituted allylic alcohols are widespread structural motifs in natural products and biologically active compounds but are difficult to directly prepare. Introduced herein is a general one-pot multicomponent coupling method for the synthesis of (Z)-α,α,β-trisubstituted allylic alcohols. (Z)-Trisubstituted vinylzinc reagents are formed in situ by initial hydroboration of 1-bromo-1-alkynes. Addition of dialkylzinc reagents induces a 1,2-metallate rearrangement that is followed by a boron-to-zinc transmetallation. The resulting vinylzinc reagents add to a variety of prochiral aldehydes to produce racemic (Z)-trisubstituted allylic alcohols. When enantioenriched aldehyde substrates are employed (Z)-trisubstituted allylic alcohols are isolated with high dr (>20:1 in many cases). For example, vinylation of enantioenriched benzyl protected α- and β-hydroxy propanal derivatives furnished the expected anti-Felkin addition products via chelation control. Surprisingly, silyl protected α-hydroxy aldehydes also afford anti-Felkin addition products. A protocol for the catalytic asymmetric addition of (Z)-trisubstituted vinylzinc reagents to prochiral aldehydes with a (−)-MIB-based catalyst has also been developed. Several additives were investigated as inhibitors of the Lewis acidic alkylzinc halide byproducts, which promote the background reaction to form the racemate. α-Ethyl and α-cyclohexyl (Z)-trisubstituted allylic alcohols can now be synthesized with excellent levels of enantioselectivity in the presence of diamine inhibitors. PMID:19476375

  3. Interrupted oligomerization revisited: simple and efficient one-pot multicomponent approach to versatile synthetic intermediates.

    PubMed

    Valiulin, Roman A; Halliburton, Logan M; Kutateladze, Andrei G

    2007-09-27

    A novel multicomponent reaction allowing for a one-pot formation of three carbon-carbon bonds has been developed. It is based on in situ generation and anionic dimerization of methylenedithiane and produces a versatile synthetic equivalent of 4-hydroxy-1,3-alkanediones which, among other things, offers expeditious one-pot access to 3(2H)-furanones.

  4. Recent developments on ultrasound-assisted one-pot multicomponent synthesis of biologically relevant heterocycles.

    PubMed

    Banerjee, Bubun

    2017-03-01

    Heterocycles are the backbone of organic compounds. Specially, N- &O-containing heterocycles represent privileged structural subunits well distributed in naturally occurring compounds with immense biological activities. Multicomponent reactions (MCRs) are becoming valuable tool for synthesizing structurally diverse molecular entities. On the other hand, the last decade has seen a tremendous outburst in modifying chemical processes to make them sustainable for the betterment of our environment. The application of ultrasound in organic synthesis is fulfilling some of the goals of 'green and sustainable chemistry' as it has some advantages over the traditional thermal methods in terms of reaction rates, yields, purity of the products, product selectivity, etc. Therefore the synthesis of biologically relevant heterocycles using one-pot multi-component technique coupled with the application of ultrasound is one of the thrusting areas in the 21st Century among the organic chemists. The present review deals with the "up to date" developments on ultrasound assisted one-pot multi-component synthesis of biologically relevant heterocycles reported so far.

  5. Novel isocyanide-based one-pot multicomponent syntheses of tetrahydrobenzo[b][1,4]oxazepine and malonamide derivatives.

    PubMed

    Shaabani, Ahmad; Mofakham, Hamid; Maleki, Ali; Hajishaabanha, Fatemeh

    2010-09-13

    In this work, a novel one-pot multicomponent reaction of 2-aminophenols, Meldrum's acid, and isocyanides leads to the synthesis of tetrahydrobenzo[b][1,4]oxazepine or malonamide derivatives using 1 or 2 equiv of 2-aminophenols, respectively, in good to excellent yields at ambient temperature.

  6. Studies of one-pot double couplings on dibromoquinolines

    PubMed Central

    Piala, Alexander; Mayi, Diyar; Handy, Scott T.

    2011-01-01

    In a series of studies, the regioselectivity of Suzuki couplings of dibromoquinolines has been investigated. In general, it is much harder to achieve high levels of regioselectivity in these systems compared to many of the other dibromoheteroaromatics that have been studied. Useful levels of selectivity could be achieved for both a 5,7-dibromoquinoline as well as 3,4-dibromoquinoline. Double Suzuki couplings could also be achieved on these two compounds. PMID:21811345

  7. Novel multicomponent one-pot synthesis of tetrahydro-1H-1,5-benzodiazepine-2-carboxamide derivatives.

    PubMed

    Shaabani, Ahmad; Maleki, Ali; Mofakham, Hamid

    2008-01-01

    A new approach to the design of multicomponent reactions is introduced. As a result, the novel one-pot synthesis of 2,3,4,5-tetrahydro-1 H-1,5-benzodiazepine-2-carboxamide derivatives using an aromatic diamine, a linear or cyclic ketone, an isocyanide, and water in the presence of a catalytic amount of p-toluenesulfonic acid at ambient temperature in high yields is described.

  8. Tunable catalytic activity of solid solution metal-organic frameworks in one-pot multicomponent reactions.

    PubMed

    Aguirre-Díaz, Lina María; Gándara, Felipe; Iglesias, Marta; Snejko, Natalia; Gutiérrez-Puebla, Enrique; Monge, M Ángeles

    2015-05-20

    The aim of this research is to establish how metal-organic frameworks (MOFs) composed of more than one metal in equivalent crystallographic sites (solid solution MOFs) exhibit catalytic activity, which is tunable by virtue of the metal ions ratio. New MOFs with general formula [InxGa1-x(O2C2H4)0.5(hfipbb)] were prepared by the combination of Ga and In. They are isostructural with their monometal counterparts, synthesized with Al, Ga, and In. Differences in their behavior as heterogeneous catalysts in the three-component, one pot Strecker reaction illustrate the potential of solid solution MOFs to provide the ability to address the various stages involved in the reaction mechanism.

  9. Synthesis of unnatural amino acids via microwave-assisted regio-selective one-pot multi-component reactions of sulfamidates

    EPA Science Inventory

    Synthesis of triazole-based unnatural amino acids, triazole bisaminoacids and β-amino triazole has been described via stereo and regioselective one-pot multi-component reaction of sulfamidates, sodium azide, and alkynes under MW irradiation conditions. The developed method is app...

  10. PEG-mediated one-pot multicomponent reactions for the efficient synthesis of functionalized dihydropyridines and their functional group dependent DNA cleavage activity.

    PubMed

    Pal, Suman; Singh, Vandana; Das, Prolay; Choudhury, Lokman H

    2013-06-01

    Polyethylene glycol (PEG) has been found to be an inexpensive, non-toxic and useful medium for the one pot synthesis of highly functionalized dihydropyridines using multicomponent reactions (MCRs) at room temperature under catalyst free conditions. The notable features of this protocol are: mild reaction condition, applicability to wide range of substrates, reusability of the PEG and good yields. The interaction of the synthesized compounds with pUC19 plasmid DNA was also analyzed. Some of the synthesized compounds showed interesting functional group dependent nuclease activity for plasmid DNA cleavage under physiological conditions.

  11. Trypsin-catalyzed multicomponent reaction: A novel and efficient one-pot synthesis of thiazole-2-imine derivatives.

    PubMed

    Zhou, Junbin; Huang, Xingtian; Zhang, Zhuan; Song, Ping; Li, Yiqun

    2017-01-10

    The first Trypsin from porcine pancreas catalyzed a novel one-pot three-component reaction of α-bromoketone, primary alkylamines, and phenylisothiocyanate for the synthesis of thiazole-imine derivatives with high yields (up to 98%) in a short time under mild conditions. The results revealed that Trypsin exhibited excellent catalytic activity and great tolerance for broad substrates. This Trypsin-catalyzed three component convergent method provides a novel strategy for the synthesis of thiazole-2-imine derivatives and expands the promiscuous functions of enzymes in organic synthesis.

  12. Orthogonal dual thiol–chloroacetyl and thiol–ene couplings for the sequential one-pot assembly of heteroglycoclusters

    PubMed Central

    Fiore, Michele; Daskhan, Gour Chand; Thomas, Baptiste

    2014-01-01

    Summary We describe the first one-pot orthogonal strategy to prepare well-defined cyclopeptide-based heteroglycoclusters (hGCs) from glycosyl thiols. Both thiol–chloroactetyl coupling (TCC) and thiol–ene coupling (TEC) have been used to decorate cyclopeptides regioselectively with diverse combination of sugars. We demonstrate that the reaction sequence starting with TCC can be performed one-pot whereas the reverse sequence requires a purification step after the TEC reaction. The versatility of this orthogonal strategy has been demonstrated through the synthesis of diverse hGCs displaying alternating binary combinations of α-D-Man or β-D-GlcNAc, thus providing rapid access to attractive heteroglycosylated platforms for diverse biological applications. PMID:25161711

  13. Copper-mediated cross-coupling-cyclization-oxidation: a one-pot reaction to construct polysubstituted pyrroles.

    PubMed

    Liu, Pei; Liu, Jin-ling; Wang, Heng-shan; Pan, Ying-ming; Liang, Hong; Chen, Zhen-Feng

    2014-05-14

    A novel and efficient procedure for the synthesis of polysubstituted pyrroles has been developed in this work. The polysubsituted pyrroles were synthesized directly from terminal alkenes, amines and β-keto esters through cross-coupling-cyclization-oxidation in the presence of a catalytic amount of cuprous chloride. This method provides a one-pot synthesis route from terminal alkenes to polysubstituted pyrroles for the first time and opens a new area in cuprous catalysis.

  14. Nano-ZnO Catalyzed Multicomponent One-Pot Synthesis of Novel Spiro(indoline-pyranodioxine) Derivatives

    PubMed Central

    Sachdeva, Harshita; Saroj, Rekha; Dwivedi, Diksha

    2014-01-01

    A simple catalytic protocol for the synthesis of novel spiro[indoline-pyranodioxine] derivatives has been developed using ZnO nanoparticle as an efficient, green, and reusable catalyst. The derivatives are obtained in moderate to excellent yield by one-pot three-component reaction of an isatin, malononitrile/ethylcyanoacetate, and 2,2-dimethyl-1,3-dioxane-4,6-dione in absolute ethanol under conventional heating and microwave irradiation. The catalyst was recovered by filtration from the reaction mixture and reused during five consecutive runs without any apparent loss of activity for the same reaction. The mild reaction conditions and recyclability of the catalyst make it environmentally benign synthetic procedure. PMID:24683341

  15. A versatile approach to flavones via a one-pot Pd(II)-catalyzed dehydrogenation/oxidative boron-Heck coupling sequence of chromanones.

    PubMed

    Lee, Jun; Yu, Jihyun; Son, Seung Hwan; Heo, Jinyuk; Kim, Taelim; An, Ji-Young; Inn, Kyung-Soo; Kim, Nam-Jung

    2016-01-14

    A variety of flavones were expediently synthesized from readily accessible chromanones via a one-pot sequence involving Pd(II)-catalyzed dehydrogenation and oxidative boron-Heck coupling with arylboronic acid pinacol esters. In particular, the use of arylboronic acid pinacol esters was found to significantly improve the yield of the reaction.

  16. One-pot synthesis of thiazino[2,3,4-hi]indole derivatives through a tandem oxidative coupling/heteroannulation process.

    PubMed

    Mao, Xi; Tong, Tao; Fan, Senbao; Fang, Liting; Wu, Jingyi; Wang, Xiaoxia; Kang, Honglan; Lv, Xin

    2017-04-12

    A novel and expedient one-pot synthesis of thiazino[2,3,4-hi]indole derivatives from o-haloaryl enamines and o-bromothiophenols has been developed. The tandem oxidative coupling/heteroannulation reactions exhibit high selectivity and good efficiency. The polycyclic heterocyclic products obtained might be useful in medicinal chemistry and materials science.

  17. Palladium-catalyzed one-pot three- or four-component coupling of aryl iodides, alkynes, and amines through C-N bond cleavage: efficient synthesis of indole derivatives.

    PubMed

    Hao, Wei; Geng, Weizhi; Zhang, Wen-Xiong; Xi, Zhenfeng

    2014-02-24

    An efficient synthesis of N-substituted indole derivatives was realized by combining the Pd-catalyzed one-pot multicomponent coupling approach with cleavage of the C(sp(3))-N bonds. Three or four components of aryl iodides, alkynes, and amines were involved in this coupling process. The cyclopentadiene-phosphine ligand showed high efficiency. A variety of aryl iodides, including cyclic and acyclic tertiary amino aryl iodides, and substituted 1-bromo-2-iodobenzene derivatives could be used. Both symmetric and unsymmetric alkynes substituted with alkyl, aryl, or trimethylsilyl groups could be applied. Cyclic secondary amines such as piperidine, morpholine, 4-methylpiperidine, 1-methylpiperazine, 2-methylpiperidine, and acyclic amines including secondary and primary amines all showed good reactivity. Further application of the resulting indole derivatives was demonstrated by the synthesis of benzosilolo[2,3-b]indole.

  18. Combining click-multicomponent reaction: one-pot synthesis of triazolyl methoxy-phenyl indazolo[2,1-b]phthalazine-trione derivatives.

    PubMed

    Salehi, Peyman; MaGee, David I; Dabiri, Minoo; Torkian, Laleh; Donahue, Jordan

    2012-05-01

    [(1,2,3-Triazol-4-yl)methoxy-phenyl]-2H-indazolo[2,1-b]phthalazine-trione derivatives were synthesized in a simple and efficient method from the one-pot four-component condensation reaction of phthalhydrazide, aromatic propargyloxy aldehydes, active methylene compounds (dimedone and 1,3-cyclohexanedione), and azides in the presence of Cu(OAc)(2)/sodium ascorbate and p-toluenesulfonic acid as catalysts in good to excellent yields.

  19. A Research-Based Undergraduate Organic Laboratory Project: Investigation of a One-Pot, Multicomponent, Environmentally Friendly Prins-Friedel-Crafts-Type Reaction

    ERIC Educational Resources Information Center

    Dintzner, Matthew R.; Maresh, Justin J.; Kinzie, Charles R.; Arena, Anthony F.; Speltz, Thomas

    2012-01-01

    Students in the undergraduate organic laboratory synthesize tetrahydro-2-(4-nitrophenyl)-4-phenyl-2"H"-pyran via the Montmorillonite K10 clay-catalyzed reaction of p-nitrobenzaldehye with methanol, 3-buten-1-ol, and benzene. The synthesis comprises an environmentally friendly tandem Prins-Friedel-Crafts-type multicomponent reaction (MCR) and sets…

  20. One-pot synthesis of 4′-alkyl-4-cyanobiaryls on the basis of the terephthalonitrile dianion and neutral aromatic nitrile cross-coupling

    PubMed Central

    Peshkov, Roman Yu; Chunyan, Wang; Tretyakov, Evgeny V; Shteingarts, Vitalij D

    2016-01-01

    Summary A convenient one-pot approach to alkylcyanobiaryls is described. The method is based on biaryl cross-coupling between the sodium salt of the terephthalonitrile dianion and a neutral aromatic nitrile in liquid ammonia, and successive alkylation of the long-lived anionic intermediate with alkyl bromides. The reaction is compatible with benzonitriles that contain methyl, methoxy and phenyl groups, fluorine atoms, and a 1-cyanonaphthalene residue. The variety of ω-substituted alkyl bromides, including an extra bromine atom, a double bond, cyano and ester groups, as well as a 1,3-dioxane fragment are suitable as alkylation reagents. PMID:27559409

  1. One-pot multi-component synthesis of 1,4-dihydropyridines using Zn(2+) @KSF and evaluating their antibacterial and antioxidant activities.

    PubMed

    Mahmoodi, Nosrat O; Ramzanpour, Sahar; Ghanbari Pirbasti, Fateme

    2015-04-01

    New 5-aryl-10-(4-(4-methoxyphenyl)thiazole-2-yl)-9,10-dihydropyrido[2,3-d:5,6-d']dipyrimidinone-2,4,6,8-(1H,3H,5H,7H)-tetraones 6a-d were synthesized through one-pot four-component reaction of aldehydes, barbituric acid, and thiazole using Zn(2+) @KSF under reflux condition. The key features of this reaction are: incorporating four heterocyclic rings, using a heterogeneous and efficient catalyst, high yield, and easy-to-setup reaction. The structure of the products was confirmed by FT-IR, (1)H NMR, and (13)C NMR spectra. The antibacterial activities of compounds 6a-d were screened against Escherichia coli, Micrococcus luteus, Pseudomonas aeruginosa, and Staphylococcus aureus bacterial strains using the zone inhibition method. Also, the 2,2-diphenyl-2-picrylhydrazyl (DPPH) radical scavenging activities of compounds 6a-d were evaluated. All compounds showed good antioxidant capacity in comparison to ascorbic acid. The IC50 values of the antioxidant activity were calculated. The proposed mechanism for antioxidant activity is discussed.

  2. Rapid Synthesis of Thiophene-Based, Organic Dyes for Dye-Sensitized Solar Cells (DSSCs) by a One-Pot, Four-Component Coupling Approach.

    PubMed

    Matsumura, Keisuke; Yoshizaki, Soichi; Maitani, Masato M; Wada, Yuji; Ogomi, Yuhei; Hayase, Shuzi; Kaiho, Tatsuo; Fuse, Shinichiro; Tanaka, Hiroshi; Takahashi, Takashi

    2015-06-26

    This one-pot, four-component coupling approach (Suzuki-Miyaura coupling/C-H direct arylation/Knoevenagel condensation) was developed for the rapid synthesis of thiophene-based organic dyes for dye-sensitized solar cells (DSSCs). Seven thiophene-based, organic dyes of various donor structures with/without the use of a 3,4-ethylenedioxythiophene (EDOT) moiety were successfully synthesized in good yields based on a readily available thiophene boronic acid pinacol ester scaffold (one-pot, 3-step, 35-61%). Evaluation of the photovoltaic properties of the solar cells that were prepared using the synthesized dyes revealed that the introduction of an EDOT structure beside a cyanoacrylic acid moiety improved the short-circuit current (Jsc) while decreasing the fill factor (FF). The donor structure significantly influenced the open-circuit voltage (Voc), the FF, and the power conversion efficiency (PCE). The use of a n-hexyloxyphenyl amine donor, and our originally developed, rigid, and nonplanar donor, both promoted good cell performance (η=5.2-5.6%).

  3. One-pot hydrothermal synthesis of magnetically recoverable palladium/reduced graphene oxide nanocomposites and its catalytic applications in cross-coupling reactions.

    PubMed

    Fu, Wenzhi; Zhang, Zhuqing; Zhuang, Peiyuan; Shen, Jianfeng; Ye, Mingxin

    2017-07-01

    A facile, green, economical approach was designed to deposit palladium nanoparticles on magnetic reduced graphene oxide nanosheets (Pd-Fe3O4/rGO) via a one-pot hydrothermal synthesis method. The prepared Pd-Fe3O4/rGO nanocomposites were thoroughly characterized by Transmission electron microscopy, Scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray diffraction, and Raman spectroscopy. Importantly, the highly efficient catalytic property of the as-obtained Pd-Fe3O4/rGO catalyst was demonstrated for the Suzuki-Miyaura coupling reaction and Mizoroki-Heck coupling reaction. Significantly, the Suzuki-Miyaura coupling reactions could be efficiently performed in an environmentally friendly aqueous solution with no need for further additives. Besides, the nanocomposites could be conveniently separated from reaction system with an external permanent magnet for recycling and the inherent catalytic activity of the nanocomposites did not exacerbate after six repeated applications.

  4. Two-step one-pot synthesis of benzoannulated spiroacetals by Suzuki-Miyaura coupling/acid-catalyzed spiroacetalization.

    PubMed

    Butkevich, Alexey N; Corbu, Andrei; Meerpoel, Lieven; Stansfield, Ian; Angibaud, Patrick; Bonnet, Pascal; Cossy, Janine

    2012-10-05

    Substituted benzoannulated spiroacetals were prepared from (2-haloaryl)alkyl alcohols and dihydropyranyl or dihydrofuranyl pinacol boronates using a Suzuki-Miyaura coupling followed by an acid-catalyzed spirocyclization. Application of the reaction to a glycal boronate provides an approach to annulated spiroacetals in enantiopure form.

  5. Elucidation of the structure-property relationship of p-type organic semiconductors through rapid library construction via a one-pot, Suzuki-Miyaura coupling reaction.

    PubMed

    Fuse, Shinichiro; Matsumura, Keisuke; Wakamiya, Atsushi; Masui, Hisashi; Tanaka, Hiroshi; Yoshikawa, Susumu; Takahashi, Takashi

    2014-09-08

    The elucidation of the structure-property relationship is an important issue in the development of organic electronics. Combinatorial synthesis and the evaluation of systematically modified compounds is a powerful tool in the work of elucidating structure-property relationships. In this manuscript, D-π-A structure, 32 p-type organic semiconductors were rapidly synthesized via a one-pot, Suzuki-Miyaura coupling with subsequent Knoevenagel condensation. Evaluation of the solubility and photovoltaic properties of the prepared compounds revealed that the measured solubility was strongly correlated with the solubility parameter (SP), as reported by Fedors. In addition, the SPs were correlated with the Jsc of thin-film organic solar cells prepared using synthesized compounds. Among the evaluated photovoltaic properties of the solar cells, Jsc and Voc had strong correlations with the photoconversion efficiency (PCE).

  6. Synthesis of di-, tri-, and tetrasulfides through multifold carbon-sulfur cross-coupling reactions with indium tri(organothiolates) in a one-pot procedure.

    PubMed

    Lee, Phil Ho; Park, Youngchul; Park, Sangkyun; Lee, Euijae; Kim, Sunggak

    2011-02-04

    Pd-catalyzed multifold (2-, 3-, and 4-fold) carbon-sulfur cross-coupling reaction of indium tri(organothiolates) with polybromonated aromatic and heteroaromatic compounds was developed in a one-pot procedure. Both 2,5-dibromopyridine and 2,6-dibromopyridine reacted with indium tri(organothiolates) (0.68 equiv) in the presence of 4 mol % of Pd(OAc)(2), 4.2 mol % of Xantphos, and 1 equiv of diisopropylethylamine (DIPEA), producing disulfides in good to excellent yields. These results indicate that indium tri(organothiolates) transfer all three alkyl- or arylthio groups attached to indium metal to electrophilic coupling partners. Indium tri(organothiolates) derived from alkyl thiol having a low boiling point, such as n-propyl, isopropyl, and tert-butyl thiol, acted as good nucleophilic coupling partners. In addition, indium tri(arylthiolates) derived from aryl thiols possessing an electron-withdrawing or -donating group on the aromatic ring participated well in the Pd-catalyzed multifold carbon-sulfur cross-coupling reaction. 4,4'-Dibromo-1,1'-biphenyl, 9,10-dibromoanthracene, 2,4-dibromoanisole, 2,7-dibromo-9,9-dimethylfluorene, 3,4-dibromothiophene, 2,3-dibromothiophene, 2,2'-bithiophene, 1,3,5-tribromobenzene, and 1,2,4,5-tetrabromobenzene were converted smoothly to the corresponding di-, tri-, and tetrasulfides.

  7. Rhodium catalyzed oxidative coupling of salicylaldehydes with diazabicyclic olefins: a one pot strategy involving aldehyde C-H cleavage and π-allyl chemistry towards the synthesis of fused ring chromanones.

    PubMed

    Jijy, E; Prakash, Praveen; Shimi, M; Pihko, Petri M; Joseph, Nayana; Radhakrishnan, K V

    2013-08-25

    An efficient one pot strategy for the synthesis of cyclopentene fused chromanone derivatives through the direct oxidative coupling of salicylaldehydes with bicyclic olefins in the presence of a rhodium-copper catalyst system is described. This is the first report on the ring opening-ring closing of bicyclic hydrazines via metal catalyzed oxidative coupling reaction.

  8. Enantio- and diastereoselective synthesis of piperidines by coupling of four components in a "one-pot" sequence involving diphenylprolinol silyl ether mediated Michael reaction.

    PubMed

    Urushima, Tatsuya; Sakamoto, Daisuke; Ishikawa, Hayato; Hayashi, Yujiro

    2010-10-15

    An efficient, asymmetric, four-component, one-pot synthesis of highly substituted piperidines with excellent diastereo- and enantioselectivity was established through the diphenylprolinol silyl ether mediated Michael reaction of aldehyde and nitroalkene, followed by the domino aza-Henry reaction/hemiaminalization reaction and a Lewis acid mediated allylation or cyanation reaction. All carbons of the piperidine ring are substituted with different groups, and its five contiguous stereocenters are completely controlled in both relative and absolute senses.

  9. One pot synthesis of exchange coupled Nd2Fe14B/alpha-Fe by pechini type sol-gel method.

    PubMed

    Hussain, Abid; Jadhav, Abhijit P; Baek, Yeon Kyung; Choi, Hul Jin; Lee, Jaeho; Kang, Young Soo

    2013-11-01

    In this work, a combination of nanoparticles of Nd2Fe14B hard magnetic phase and alpha-Fe soft magnetic phase were synthesized by one pot chemical synthesis technique using sol-gel method. A gel of Nd-Fe-B was prepared using NdCl3 x 6H2O, FeCl3 x 6H2O, H3BO3, citric acid, and ethylene glycol by pechini type sol-gel method. The gel was subsequently calcined and annealed to obtain the mixed oxide powders. The produced metal oxide particles were identified with XRD, SEM, TEM to obtain the crystal structure, shape and domain structure of them. The nanoparticles of mixed phase of Nd2Fe14B/alpha-Fe were obtained from these oxides by a process of reduction-diffusion in vacuum by employing CaH2 as reducing agent. During this process it was optimized by controlling temperature, reaction time and concentration of the reducing agent (CaH2). The phase formation of Nd2Fe14B was resulted by the direct diffusion of NdH2, Fe and B. The magnetic property of produced hard and soft phases was successfully identified with vibrating sample magnetometer (VSM). The mixed domains of the hard and soft phases were identified with selected area electron diffraction method (SAED) patterns.

  10. Facile one-pot synthesis of 4,5-disubstituted 1,2,3-(NH)-triazoles through Sonogashira coupling/1,3-dipolar cycloaddition of acid chlorides, terminal acetylenes, and sodium azide.

    PubMed

    Li, Jihui; Wang, Dong; Zhang, Yuanqing; Li, Jiting; Chen, Baohua

    2009-07-16

    A novel and efficient way of synthesizing 4,5-disubstituted-1,2,3-(NH)-triazoles through palladium-catalyzed and ultrasonic promoted Sonogashira coupling/1,3-dipolar cycloaddition of acid chlorides, terminal acetylenes, and sodium azide in one pot is developed. The reaction scope is quite general, and the methodology can produce excellent yields. The regioselective 1,4,5-trisubstituted-1,2,3-(NH)-triazoles can be made easily from 4,5-disubstituted-1,2,3-(NH)-triazoles.

  11. Chelation-assisted Pd-catalysed ortho-selective oxidative C-H/C-H cross-coupling of aromatic carboxylic acids with arenes and intramolecular Friedel-Crafts acylation: one-pot formation of fluorenones.

    PubMed

    Sun, Denan; Li, Bijin; Lan, Jingbo; Huang, Quan; You, Jingsong

    2016-03-04

    Pd-Catalysed ortho-selective oxidative C-H/C-H cross-coupling of aromatic carboxylic acids with arenes and subsequent intramolecular Friedel-Crafts acylation has been accomplished for the first time through a chelation-assisted C-H activation strategy. Starting from the readily available substrates, a variety of fluorenone derivatives are obtained in one pot. The direct use of naturally occurring carboxylic acid functionalities as directing groups avoids unnecessary steps for installation and removal of an extra directing group.

  12. Microwave-assisted combinatorial synthesis of hexa-substituted 1,4-dihydropyridines scaffolds using one-pot two-step multicomponent reaction followed by a S-alkylation.

    PubMed

    Li, Ming; Zuo, Zhengquan; Wen, Lirong; Wang, Shuwen

    2008-01-01

    A sequential one-pot two-step protocol for microwave-assisted synthesis of Hantzsch-type hexa-substituted 1,4-dihydropyridines has been developed. The three-component reactions of beta-aroylthioamides with aldehydes and acetonitrile derivatives produce the intermediates in situ followed by a S-alkylation to afford hexa-substituted 1,4-dihydropyridines. The reaction presumably proceeds via a Knoevenagel condensation-Michael addition-cyclocondensation-rearrangement-S N2 reaction sequence. Target compounds were obtained in high yields and simply purified by recrystallization. The novel method is complementary to the classical Hantzsch synthesis in that it is well-suited to the preparation of hexa-substituted 1,4-dihydropyridines.

  13. Successive copper(I)-catalyzed cross-couplings in one pot: a novel and efficient starting point for synthesis of carbapenems.

    PubMed

    Jiang, Biao; Tian, Hua; Huang, Zuo-Gang; Xu, Min

    2008-07-03

    An efficient approach for synthesizing a series of 2-sulfide carbapenems has been developed using two successive Cu(I)-catalyzed cross-couplings in a single pot. The method involves highly selective intramolecular coupling of lactam and dihaloalkene using 2,2'-bipyridine as a ligand, followed by intermolecular C-S formation in the presence of another ligand (1,10-phenanthroline, PPh 3) and mercaptan.

  14. Transition-metal-free cross-coupling of thioethers with aryl(cyano)iodonium triflates: a facile and efficient method for the one-pot synthesis of thiocyanates.

    PubMed

    Zhu, Dan; Chang, Denghu; Shi, Lei

    2015-04-28

    A novel transition-metal-free cross-coupling method for the one-step synthesis of thiocyanates via the C-S bond cleavage of readily available thioethers with aryl(cyano)-iodonium triflates as the cyanating agent is developed. This process features relatively broad substrate scopes, less-toxic hypervalent iodine reagents, mild operating conditions, excellent functional group compatibilities, and affords various thiocyanates in moderate to good yields.

  15. (15)N Double-labeled guanosine from inosine through ring-opening-ring-closing and one-pot Pd-catalyzed C-O and C-N cross-coupling reactions.

    PubMed

    Caner, Joaquim; Vilarrasa, Jaume

    2010-07-16

    [N,1-(15)N(2)]-Guanosine, or [1,NH(2)-(15)N(2)]-guanosine, and derivatives were prepared from tri-O-acetylinosine, via N-nitration and reaction with (15)NH(2)OH, followed by conversion of the (15)N-labeled 1-hydroxyinosine to the corresponding 2,6-dichloropurine riboside. The sequential one-pot C-O and C-N key couplings of this dichloro derivative with PhCH(2)OH and PhCO(15)NH(2) or (i)PrCO(15)NH(2) was achieved in good overall yields, with Pd(0)-Xantphos as the best choice of five different catalytic systems examined.

  16. One-pot syntheses of immunostimulatory glycolipids.

    PubMed

    Schombs, Matthew; Park, Francine E; Du, Wenjun; Kulkarni, Suvarn S; Gervay-Hague, Jacquelyn

    2010-08-06

    Glycolipids containing alpha-linked galactosyl and glucosyl moieties have been shown to possess unique immunostimulatory activity creating a need for access to diverse and anomerically pure sources of these compounds for immunological studies. To meet this demand, glycosyl iodides were enlisted in the synthesis of these biologically relevant glycoconjugates. In the first-generation protocol, per-O-benzyl galactosyl iodide was efficiently coupled with activated sphingosine acceptors, but fully functionalized ceramides were found to be unreactive. To overcome this obstacle, per-O-trimethylsilyl glycosyl iodides were investigated and shown to undergo highly efficient coupling with ceramide and glycerol ester acceptors. Contrary to what has been observed with other donors, we detected little difference between the reactivity of glucosyl and galactosyl iodides. The trimethylsilyl protecting groups play a dual role in activating the donor toward nucleophilic attack while at the same time providing transient protection: the silyl groups are readily removed upon methanolysis. All reactions proceeded with complete acceptor regioselectivity, eliminating the need for additional protecting group manipulations, and the desired alpha-anomers were formed exclusively. This three-step, one-pot synthetic platform provides rapid access to an important class of immunostimulatory molecules including the first reported synthesis of the glucosyl analogue of the bacterial antigen BbGL-II.

  17. Novel One-pot Fabrication of Lab-on-a-Bubble@Ag Substrate without Coupling-agent for Surface Enhanced Raman Scattering

    NASA Astrophysics Data System (ADS)

    Jiang, Jizhou; Ou-Yang, Lei; Zhu, Lihua; Zou, Jing; Tang, Heqing

    2014-02-01

    Through in-situ reduction of silver nitrate without using any coupling-agent, a substrate for surface-enhanced Raman scattering (SERS) was prepared by coating silver on hollow buoyant silica microspheres as a lab on a bubble (LoB). The silver coated LoBs (LoBs@Ag) floated on surface of a solution could provide a very convenient platform for the detection of target molecules in the solution. The LoBs@Ag substrate not only immobilized well-distributed Ag nanoparticles on the surface LoBs, but excluded the interference of coupling agents. This yielded high-resolution SERS spectra with excellent reproducibility. The adsorption of crystal violet (CV) on the LoBs@Ag substrate was investigated by means of SERS combined with density functional theory (DFT) calculations. The LoBs@Ag substrate exhibited a remarkable Raman enhancement effect for CV with an enhancement factor of 6.9 × 108 and wide adaptability from dye, pesticide to bio-molecules. On the basis of this substrate, a simple and sensitive SERS method was proposed for the determination of trace organic pollutants or bio-molecules.

  18. Novel One-pot Fabrication of Lab-on-a-Bubble@Ag Substrate without Coupling-agent for Surface Enhanced Raman Scattering

    PubMed Central

    Jiang, Jizhou; Ou-Yang, Lei; Zhu, Lihua; Zou, Jing; Tang, Heqing

    2014-01-01

    Through in-situ reduction of silver nitrate without using any coupling-agent, a substrate for surface-enhanced Raman scattering (SERS) was prepared by coating silver on hollow buoyant silica microspheres as a lab on a bubble (LoB). The silver coated LoBs (LoBs@Ag) floated on surface of a solution could provide a very convenient platform for the detection of target molecules in the solution. The LoBs@Ag substrate not only immobilized well-distributed Ag nanoparticles on the surface LoBs, but excluded the interference of coupling agents. This yielded high-resolution SERS spectra with excellent reproducibility. The adsorption of crystal violet (CV) on the LoBs@Ag substrate was investigated by means of SERS combined with density functional theory (DFT) calculations. The LoBs@Ag substrate exhibited a remarkable Raman enhancement effect for CV with an enhancement factor of 6.9 × 108 and wide adaptability from dye, pesticide to bio-molecules. On the basis of this substrate, a simple and sensitive SERS method was proposed for the determination of trace organic pollutants or bio-molecules. PMID:24487575

  19. One-pot synthesis of urchin-like FePd-Fe3O4 and their conversion into exchange-coupled L1(0)-FePd-Fe nanocomposite magnets.

    PubMed

    Yu, Yongsheng; Sun, Kewei; Tian, Yuan; Li, X-Z; Kramer, M J; Sellmyer, D J; Shield, J E; Sun, Shouheng

    2013-10-09

    We report a one-pot synthesis of urchin-like FePd-Fe3O4 nanocomposites, spherical clusters of FePd nanoparticles (NPs) with spikes of Fe3O4 nanorods (NRs), via controlled thermal decomposition of Fe(CO)5 and reduction of Pd(acac)2. The FePd NPs with sizes between 6 and 9 nm self-aggregate into 60 nm superparticles (SPs), and Fe3O4 NRs grow on the surface of these SPs. Reductive annealing at 500 °C converts the FePd-Fe3O4 into exchange-coupled nanocomposites L1(0)-FePd-Fe with their Hc tunable from 0.8 to 2.6 kOe and Ms controlled from 90 to 190 emu/g. The work provides a general approach to L1(0)-FePd-Fe nanocomposite magnets for understanding exchange coupling at the nanoscale. The concept may be extended to other magnetic nanocomposite systems and may help to build superstrong magnets for magnetic applications.

  20. One-Pot Synthesis of Urchin-like FePd-Fe3O4 and Their Conversion into Exchange-Coupled L10-FePd-Fe Nanocomposite Magnets

    SciTech Connect

    Yu, Yongsheng; Sun, Kewei; Tian, Yuan; Li, X.-Z.; Kramer, Matthew J.; Sellymyer, D. J.; Shield, J. E.; Sun, Shouheng

    2013-09-16

    We report a one-pot synthesis of urchin-like FePd-Fe3O4 nanocomposites, spherical clusters of FePd nanoparticles (NPs) with spikes of Fe3O4 nanorods (NRs), via controlled thermal decomposition of Fe(CO)5 and reduction of Pd(acac)2. The FePd NPs with sizes between 6 and 9 nm self-aggregate into 60 nm superparticles (SPs), and Fe3O4 NRs grow on the surface of these SPs. Reductive annealing at 500 °C converts the FePd-Fe3O4 into exchange-coupled nanocomposites L1(0)-FePd-Fe with their Hc tunable from 0.8 to 2.6 kOe and Ms controlled from 90 to 190 emu/g. The work provides a general approach to L1(0)-FePd-Fe nanocomposite magnets for understanding exchange coupling at the nanoscale. The concept may be extended to other magnetic nanocomposite systems and may help to build superstrong magnets for magnetic applications.

  1. Rapid Synthesis of D-A'-π-A Dyes through a One-Pot Three-Component Suzuki-Miyaura Coupling and an Evaluation of their Photovoltaic Properties for Use in Dye-Sensitized Solar Cells.

    PubMed

    Irie, Shunsuke; Fuse, Shinichiro; Maitani, Masato M; Wada, Yuji; Ogomi, Yuhei; Hayase, Shuzi; Kaiho, Tatsuo; Masui, Hisashi; Tanaka, Hiroshi; Takahashi, Takashi

    2016-02-12

    Twenty-four D-A'-π-A dyes were rapidly synthesized through a one-pot three-component Suzuki-Miyaura coupling reaction, which was assisted by microwave irradiation. We measured the absorption spectra, electrochemical properties, and solar-cell performance of all the synthesized dyes. The D5 πA4 dye contained our originally designed rigid and nonplanar donor and exerted the highest efficiency at 5.4 %. The short-circuit current (Jsc ) was the most important parameter for the conversion efficiency (η) in the case of the organic D-A'-π-A dyes. Optimal ranges for the D-A'-π-A dyes were observed for high values of Jsc /λmax at λ=560-620 nm, an optical-absorption edge of λ=690-790 nm, and EHOMO and ELUMO values of <1.14 and -0.56 to -0.76 V, respectively.

  2. Sequential one-pot access to molecular diversity through aniline aqueous borylation.

    PubMed

    Erb, William; Albini, Mathieu; Rouden, Jacques; Blanchet, Jérôme

    2014-11-07

    On the basis of our recently reported aniline aqueous borylation, molecular diversity was achieved in a one-pot process by combining other reactions such as esterification, Suzuki-Miyaura coupling, hydrogenolysis, or Petasis borono-Mannich.

  3. Novel isocyanide-based three-component one-pot synthesis of cyanophenylamino-acetamide derivatives.

    PubMed

    Shaabani, Ahmad; Maleki, Ali; Mofakham, Hamid; Khavasi, Hamid Reza

    2008-01-01

    A one-pot multicomponent synthesis of a novel class of cyanophenylamino-acetamides through the conversion of primary amides to the corresponding nitriles, starting from simple and readily available inputs including 2-aminobenzamide, an aldehyde, and an isocyanide in the presence of p-toluenesulfonic acid as a catalyst, in excellent yields at room temperature in ethanol as a green reaction medium is described.

  4. Stereo- and regio-selective one-pot synthesis of triazole-based unnatural amino acids and β- amino triazoles

    EPA Science Inventory

    Synthesis of triazole based unnatural amino acids and β-amino triazole has been described via stereo and regioselective one-pot multi-component reaction of sulfamidates, sodium azide, and alkynes under MW conditions. The developed method is applicable to a broad substrate scope a...

  5. Synthesis of polyhydroxylated piperidine and pyrrolidine peptidomimetics via one-pot sequential lactam reduction/Joullié-Ugi reaction.

    PubMed

    Szcześniak, Piotr; Maziarz, Elżbieta; Stecko, Sebastian; Furman, Bartłomiej

    2015-04-03

    A direct approach to the synthesis of polyhydroxylated piperidine and pyrrolidine peptidomimetics is described. The presented strategy is based on one-pot reduction of sugar-derived lactams with Schwartz's reagent followed by a multicomponent Ugi-Joullié reaction.

  6. (2+1)-dimensional non-isospectral multi-component AKNS equations and its integrable couplings

    SciTech Connect

    Sun Yepeng

    2010-03-08

    (2+1)-dimensional non-isospectral multi-component AKNS equations are derived from an arbitrary order matrix spectral problem. As a reduction, (2+1)-dimensional non-isospectral multi-component Schroedinger equations are obtained. Moreover, new (2+1)-dimensional non-isospectral integrable couplings of the resulting AKNS equations are constructed by enlarging the associated matrix spectral problem.

  7. A palladium-catalysed multicomponent coupling approach to conjugated poly(1,3-dipoles) and polyheterocycles

    NASA Astrophysics Data System (ADS)

    Leitch, David C.; Kayser, Laure V.; Han, Zhi-Yong; Siamaki, Ali R.; Keyzer, Evan N.; Gefen, Ashley; Arndtsen, Bruce A.

    2015-06-01

    Conjugated polymers have emerged over the past several decades as key components for a range of applications, including semiconductors, molecular wires, sensors, light switchable transistors and OLEDs. Nevertheless, the construction of many such polymers, especially highly substituted variants, typically involves a multistep synthesis. This can limit the ability to both access and tune polymer structures for desired properties. Here we show an alternative approach to synthesize conjugated materials: a metal-catalysed multicomponent polymerization. This reaction assembles multiple monomer units into a new polymer containing reactive 1,3-dipoles, which can be modified using cycloaddition reactions. In addition to the synthetic ease of this approach, its modularity allows easy adaptation to incorporate a range of desired substituents, all via one-pot reactions.

  8. A palladium-catalysed multicomponent coupling approach to conjugated poly(1,3-dipoles) and polyheterocycles

    PubMed Central

    Leitch, David C.; Kayser, Laure V.; Han, Zhi-Yong; Siamaki, Ali R.; Keyzer, Evan N.; Gefen, Ashley; Arndtsen, Bruce A.

    2015-01-01

    Conjugated polymers have emerged over the past several decades as key components for a range of applications, including semiconductors, molecular wires, sensors, light switchable transistors and OLEDs. Nevertheless, the construction of many such polymers, especially highly substituted variants, typically involves a multistep synthesis. This can limit the ability to both access and tune polymer structures for desired properties. Here we show an alternative approach to synthesize conjugated materials: a metal-catalysed multicomponent polymerization. This reaction assembles multiple monomer units into a new polymer containing reactive 1,3-dipoles, which can be modified using cycloaddition reactions. In addition to the synthetic ease of this approach, its modularity allows easy adaptation to incorporate a range of desired substituents, all via one-pot reactions. PMID:26077769

  9. A facile one-pot route to cationic cellulose nanocrystals

    NASA Astrophysics Data System (ADS)

    Jasmani, Latifah; Eyley, Samuel; Wallbridge, Rachel; Thielemans, Wim

    2013-10-01

    Pyridinium-grafted-cellulose nanocrystals were prepared by a simple one-pot reaction using 4-(1-bromoethyl/bromomethyl)benzoic acid, pyridine and cellulose nanocrystals (CNCs). The grafting consists of an esterification reaction between 4-(1-bromoethyl/bromomethyl)benzoic acid and CNCs and a nucleophilic attack on the C-Br bond of 4-(1-bromoethyl/bromomethyl)benzoic acid by pyridine. This reaction simplifies existing cationization methods, which leads to a higher grafting density while retaining the CNC crystallinity.Pyridinium-grafted-cellulose nanocrystals were prepared by a simple one-pot reaction using 4-(1-bromoethyl/bromomethyl)benzoic acid, pyridine and cellulose nanocrystals (CNCs). The grafting consists of an esterification reaction between 4-(1-bromoethyl/bromomethyl)benzoic acid and CNCs and a nucleophilic attack on the C-Br bond of 4-(1-bromoethyl/bromomethyl)benzoic acid by pyridine. This reaction simplifies existing cationization methods, which leads to a higher grafting density while retaining the CNC crystallinity. Electronic supplementary information (ESI) available: Experimental description, FTIR, XPS and XRD spectra and detailed characterisation results of all compounds. See DOI: 10.1039/c3nr03456a

  10. Soliton dynamics to the multi-component complex coupled integrable dispersionless equation

    NASA Astrophysics Data System (ADS)

    Xu, Zong-Wei; Yu, Guo-Fu; Zhu, Zuo-Nong

    2016-11-01

    The generalized coupled integrable dispersionless (CID) equation describes the current-fed string in a certain external magnetic field. In this paper, we propose a multi-component complex CID equation. The integrability of the multi-component complex equation is confirmed by constructing Lax pairs. One-soliton and two-soliton solutions are investigated to exhibit rich evolution properties. Especially, similar as the multi-component short pulse equation and the first negative AKNS equation, periodic interaction, parallel solitons, elastic and inelastic interaction, energy re-distribution happen between two solitons. Multi-soliton solutions are given in terms of Pfaffian expression by virtue of Hirota's bilinear method.

  11. One-Pot Synthesis of Imidazole-4-Carboxylates by Microwave-Assisted 1,5-Electrocyclization of Azavinyl Azomethine Ylides

    PubMed Central

    Preti, Lisa; Attanasi, Orazio A.; Caselli, Emilia; Favi, Gianfranco; Ori, Claudia; Davoli, Paolo; Felluga, Fulvia

    2013-01-01

    Diversely functionalized imidazole-4-carboxylates were synthesized by microwave-assisted 1,5-eletrocyclization of 1,2-diaza-1,3-diene-derived azavinyl azomethine ylides. 1,2-Diaza-1,3-dienes were treated with primary aliphatic or aromatic amines and subjected to microwave irradiation in the presence of aldehydes. 3-Alkyl- and 3-arylimidazole-4-carboxylates were prepared in good yields through a one-pot multicomponent procedure. Modulation of the substituents at C-2, N-3 and C-5 was possible, and 2-unsubstituted imidazoles were obtained when paraformaldehyde was used. PMID:24273445

  12. Coupling Oxygen Consumption with Hydrocarbon Oxidation in Bacterial Multicomponent Monooxygenases.

    PubMed

    Wang, Weixue; Liang, Alexandria D; Lippard, Stephen J

    2015-09-15

    A fundamental goal in catalysis is the coupling of multiple reactions to yield a desired product. Enzymes have evolved elegant approaches to address this grand challenge. A salient example is the biological conversion of methane to methanol catalyzed by soluble methane monooxygenase (sMMO), a member of the bacterial multicomponent monooxygenase (BMM) superfamily. sMMO is a dynamic protein complex of three components: a hydroxylase, a reductase, and a regulatory protein. The active site, a carboxylate-rich non-heme diiron center, is buried inside the 251 kDa hydroxylase component. The enzyme processes four substrates: O2, protons, electrons, and methane. To couple O2 activation to methane oxidation, timely control of substrate access to the active site is critical. Recent studies of sMMO, as well as its homologues in the BMM superfamily, have begun to unravel the mechanism. The emerging and unifying picture reveals that each substrate gains access to the active site along a specific pathway through the hydroxylase. Electrons and protons are delivered via a three-amino-acid pore located adjacent to the diiron center; O2 migrates via a series of hydrophobic cavities; and hydrocarbon substrates reach the active site through a channel or linked set of cavities. The gating of these pathways mediates entry of each substrate to the diiron active site in a timed sequence and is coordinated by dynamic interactions with the other component proteins. The result is coupling of dioxygen consumption with hydrocarbon oxidation, avoiding unproductive oxidation of the reductant rather than the desired hydrocarbon. To initiate catalysis, the reductase delivers two electrons to the diiron(III) center by binding over the pore of the hydroxylase. The regulatory component then displaces the reductase, docking onto the same surface of the hydroxylase. Formation of the hydroxylase-regulatory component complex (i) induces conformational changes of pore residues that may bring protons to the

  13. Composite polymer nanoarchitectures from a one-pot hydrothermal route

    NASA Astrophysics Data System (ADS)

    Yu, Shirong; Chang, Ying; Yuan, Conghui; Wang, Shuang; Mao, Jie; Chen, Guorong; Luo, Weiang; Xu, Yiting; Dai, Lizong

    2015-11-01

    Exploitation of facile and versatile synthetic approaches to polymeric nanoarchitectures is of great interest in polymer science and engineering. Herein, we show that a simple hydrothermal route using double-solvents as reaction media has the ability to generate polymer nanospheres with tunable morphologies and components. In this one-pot approach, condensation polymerization of a resol precursor and radical polymerization of styrene are allowed to occur simultaneously under hydrothermal treatment. The synergistic self-organization of phenol-formaldehyde crosslinked networks and polystyrene chains leads to the formation of well-defined hollow nanospheres with adjustable shell thickness or even Janus particles comprising a solid hemisphere and a hollow hemisphere. Furthermore, control over the composition of the hollow polymer nanospheres can be easily achieved by introducing a third monomer into the hydrothermal system.

  14. One-pot synthesis of (−)-Ambrox

    PubMed Central

    Yang, Shaoxiang; Tian, Hongyu; Sun, Baoguo; Liu, Yongguo; Hao, Yanfeng; Lv, Yanyu

    2016-01-01

    (−)-Ambrox is recognised as the prototype of all ambergris odorants. Widely used in perfumery, (−)-Ambrox is an important ingredient due to its unique scent and excellent fixative function. An environmentally friendly and practical preparation of (−)-Ambrox is still unavailable at present although a lot of attention has been paid to this hot research topic for many years. A one-pot synthesis of (−)-Ambrox was studied starting from (−)-sclareol through oxidation with hydrogen peroxide in the presence of a quaternary ammonium phosphomolybdate catalyst {[C5H5NC16H33] [H2PMo12O40]}, which gave the product a 20% overall yield. PMID:27581945

  15. Multi-catalysis reactions: direct organocatalytic sequential one-pot synthesis of highly functionalized cyclopenta[b]chromen-1-ones.

    PubMed

    Ramachary, Dhevalapally B; Reddy, Y Vijayendar; Kishor, Mamillapalli

    2008-11-21

    We have developed a new technology called multi-catalysis for the sequential one-pot synthesis of highly functionalized heterocycles. A practical and novel multi-component aniline-, self- and Brønsted acid-catalyzed selective process for the sequential one-pot synthesis of highly substituted 2-(2-hydroxy-aryl)-cyclopentane-1,3-diones, 3,9-dihydro-2H-cyclopenta[b]chromen-1-ones and 3,3-dimethyl-2,3,4,9-tetrahydro-xanthen-1-ones is reported. Direct combination of aniline- and self-catalyzed cascade olefination-hydrogenation (O-H) and Brønsted acid-catalyzed cascade oxy-Michael-dehydration (OM-DH) of 1,3-diones, salicylic aldehydes and organic-hydrides is developed in one-pot to furnish the highly functionalized 3,9-dihydro-2H-cyclopenta[b]chromen-1-ones and 3,3-dimethyl-2,3,4,9-tetrahydro-xanthen-1-ones with high yields.

  16. A Novel and Facile One-Pot Solvothermal Synthesis of PEDOT-PSS/Ni-Mn-Co-O Hybrid as an Advanced Supercapacitor Electrode Material.

    PubMed

    Yin, Chengjie; Yang, Chunming; Jiang, Min; Deng, Cuifen; Yang, Lishan; Li, Junhua; Qian, Dong

    2016-02-03

    In this work, a novel and facile one-pot method has been developed for the synthesis of a hybrid consisting of Ni-Mn-Co ternary oxide and poly(3,4-ethylenedioxythiophene)-polystyrenesulfonate (PEDOT-PSS/NMCO) with a hierarchical three-dimensional net structure via a solvothermal-coprecipitation coupled with oxidative polymerization route. Apart from the achievement of polymerization, coprecipitation, and solvothermal in one pot, the hydroxyl (OH(-)) ions generated from the oxidative polymerization of organic monomer by neutral KMnO4 solution were skillfully employed as precipitants for metal ions. As compared with the PEDOT-PSS/Ni-Mn binary oxide, PEDOT-PSS/Co-Mn binary oxide, and PEDOT-PSS/MnO2, PEDOT-PSS1.5/NMCO exhibits overwhelmingly superior supercapacitive performance, more specifically, a high specific capacitance of 1234.5 F g(-1) at a current density of 1 A g(-1), a good capacitance retention of 83.7% at a high current density of 5 A g(-1) after 1000 cycles, an energy density of 51.9 W h kg(-1) at a power density of 275 W kg(-1), and an energy density of 21.4 W h kg(-1) at an extremely elevated power density of 5500 W kg(-1). Noticeably, the energy density and power density of PEDOT-PSS/NMCO are by far higher than those of the existing analogues recently reported. The exceptional performance of PEDOT-PSS/NMCO benefits from its unique mesoporous architecture, which could provide a larger reaction surface area, faster ion and electron transfer ability, and good structural stability. The desirable integrated performance enables the multicomponent composite to be a promising electrode material for energy storage applications.

  17. An efficient one-pot four-segment condensation method for protein chemical synthesis.

    PubMed

    Tang, Shan; Si, Yan-Yan; Wang, Zhi-Peng; Mei, Kun-Rong; Chen, Xin; Cheng, Jing-Yuan; Zheng, Ji-Shen; Liu, Lei

    2015-05-04

    Successive peptide ligation using a one-pot method can improve the efficiency of protein chemical synthesis. Although one-pot three-segment ligation has enjoyed widespread application, a robust method for one-pot four-segment ligation had to date remained undeveloped. Herein we report a new one-pot multisegment peptide ligation method that can be used to condense up to four segments with operational simplicity and high efficiency. Its practicality is demonstrated by the one-pot four-segment synthesis of a plant protein, crambin, and a human chemokine, hCCL21.

  18. One-Pot Three-Component Condensation Synthesis and Structural Features of Organophosphorus-Sulfur Macrocycles.

    PubMed

    Hua, Guoxiong; Du, Junyi; Cordes, David B; Slawin, Alexandra M Z; Woollins, J Derek

    2016-05-20

    A new preparative route was developed to synthesize new phosphorus-sulfur [SP(═S)S moiety]-containing macrocycles via a one-pot and three-component domino reaction of four-membered ring thionation reagents such as 2,4-bis(4-methoxyphenyl)-1,3,2,4-dithiadiphosphetane 2,4-disulfide (LR, Lawesson's reagent) and 2,4-diferrocenyl-1,3,2,4-diathiadiphosphetane 2,4-disulfide (FcLR, a ferrocene analogue of Lawesson's reagent) and alkyldithiols(aryldithols) and dihaloalkanes in the presence of sodium hydride. Therefore, a series of 12- to 18-membered macrocycles incorporating two phosphorus and six sulfur atoms were synthesized. The synthesis features a novel application of the multicomponent reaction, providing an efficient route to the preparation of the new phosphorus-sulfur-containing macrocycles. Seven representative X-ray structures confirm the formation of these macrocycles and show the presence of a number of the intramolecular C-H···S hydrogen bonding, intermolecular C-H···S, C-H···Cl, and Cl···Cl short contacts and π-stacking interactions in their 3D network structures.

  19. Synthesis of task specific and reusable protic ionic liquids for one-pot multicomponent syntheses

    NASA Astrophysics Data System (ADS)

    Sardar, Sabahat; Wilfred, Cecilia Devi; Marc, Leveque Jean

    2016-11-01

    Protic ionic liquids (ILs) synthesized from 1-methylimidazole with 1,3-propane sultone and 1,4-butane sultone catalyzed Mannich reaction at 25 °C to afford Mannich bases in high yield (76%) and less time duration (20 min). Ionic liquids have been used as dual reagent i.e., as catalyst as well as solvent. Simple extraction by water separated ionic liquid from reaction mixture with 4 times recycling without any significant loss in activity.

  20. A Synthesis of "Dual Warhead" β-Aryl Ethenesulfonyl Fluorides and One-Pot Reaction to β-Sultams.

    PubMed

    Chinthakindi, Praveen K; Govender, Kimberleigh B; Kumar, A Sanjeeva; Kruger, Hendrik G; Govender, Thavendran; Naicker, Tricia; Arvidsson, Per I

    2017-02-03

    Herein, we report an operationally simple, ligand- and additive-free oxidative boron-Heck coupling that is compatible with the ethenesulfonyl fluoride functional group. The protocol proceeds at room temperature with chemoselectivity and E-isomer selectivity and offers facile access to a wide range of β-aryl/heteroaryl ethenesulfonyl fluorides from commercial boronic acids. Furthermore, we demonstrate a "one-pot click" reaction to directly transform the products to aryl-substituted β-sultams.

  1. One-pot synthesis of tetracyclic fused imidazo[1,2-a]pyridines via a three-component reaction.

    PubMed

    Yang, Bo; Tao, Chuanye; Shao, Taofeng; Gong, Jianxian; Che, Chao

    2016-01-01

    A novel three-component reaction has been developed to assemble biologically and pharmaceutically important tetracyclic fused imidazo[1,2-a]pyridines in a one-pot fashion utilizing readily available 2-aminopyridines, isatins and isocyanides. The three-component coupling proceeds through the Groebke-Blackburn-Bienaymé reaction followed by a retro-aza-ene reaction and subsequent nucleophilic reaction of the in-situ generated imidazo[1,2-a]pyridines bearing an isocyanate functional group.

  2. Chemoenzymatic one-pot synthesis in an aqueous medium: combination of metal-catalysed allylic alcohol isomerisation-asymmetric bioamination.

    PubMed

    Ríos-Lombardía, Nicolás; Vidal, Cristian; Cocina, María; Morís, Francisco; García-Álvarez, Joaquín; González-Sabín, Javier

    2015-07-11

    The ruthenium-catalysed isomerisation of allylic alcohols was coupled, for the first time, with asymmetric bioamination in a one-pot process in an aqueous medium. In the cases involving prochiral ketones, the ω-TA exhibited excellent enantioselectivity, identical to that observed in the single step. As a result, amines were obtained from allylic alcohols with high overall yields and excellent enantiomeric excesses.

  3. Transition metal-free one-pot synthesis of nitrogen-containing heterocycles.

    PubMed

    Kumari, Simpal; Kishore, Dharma; Paliwal, Sarvesh; Chauhan, Rajani; Dwivedi, Jaya; Mishra, Aakanksha

    2016-02-01

    One-pot heterocyclic synthesis is an exciting research area as it can open routes for the development of otherwise complex transformations in organic synthesis. Heterocyclic compounds show wide spectrum of applications in medicinal chemistry, chemical biology, and materials science. These heterocycles can be generated very efficiently through highly economical and viable routes using one-pot synthesis. In particular, the metal-free one-pot synthetic protocols are highly fascinating due to several advantages for the industrial production of heterocyclic frameworks. This comprehensive review is devoted to the transition metal-free one-pot synthesis of nitrogen-containing heterocycles from the period 2010-2013.

  4. A one-pot-three-step route to triazolotriazepinoindazolones from oxazolino-2H-indazoles.

    PubMed

    Conrad, Wayne E; Rodriguez, Kevin X; Nguyen, Huy H; Fettinger, James C; Haddadin, Makhluf J; Kurth, Mark J

    2012-08-03

    A one-pot-three-step method has been developed for the conversion of oxazolino-2H-indazoles into triazolotriazepinoindazolones with three points of diversity. Step one of this process involves a propargyl bromide-initiated ring opening of the oxazolino-2H-indazole (available by the Davis-Beirut reaction) to give an N(1)-(propargyl)-N(2)-(2-bromoethyl)-disubstituted indazolone, which then undergoes -CH(2)Br → -CH(2)N(3) displacement (step two) followed by an uncatalyzed intramolecular azide-alkyne 1,3-dipolar cycloaddition (step three) to form the target heterocycle. Employing 7-bromooxazolino-2H-indazole allows for further diversification through, for example, palladium-catalyzed coupling chemistry, as reported here.

  5. One-pot native chemical ligation by combination of two orthogonal thioester precursors.

    PubMed

    Asahina, Yuya; Kawakami, Toru; Hojo, Hironobu

    2017-02-09

    We developed a one-pot peptide ligation method using two orthogonal thioester precursors and a protecting group for the ligation reaction between Asp and Cys. Combination of the two precursors facilitated the one-pot operation and yielded the entire polypeptide. The usefulness of this method was successfully demonstrated by the total synthesis of histone H4.

  6. A One-Pot, Asymmetric Robinson Annulation in the Organic Chemistry Majors Laboratory

    ERIC Educational Resources Information Center

    Lazarski, Kiel E.; Rich, Alan A.; Mascarenhas, Cheryl M.

    2008-01-01

    The Robinson annulation is a topic of importance in the second-year organic curriculum. A one-pot, enantioselective Robinson annulation is described. The experiment is completed in two lab periods and is geared towards the second-year organic chemistry major. To our knowledge, this is the first example of a one-pot enantioselective Robinson…

  7. Carbohydrate-steroid conjugation by Ugi reaction: one-pot synthesis of triple sugar/pseudo-peptide/spirostane hybrids.

    PubMed

    Rivera, Daniel G; Pérez-Labrada, Karell; Lambert, Liudmila; Dörner, Simon; Westermann, Bernhard; Wessjohann, Ludger A

    2012-10-01

    The one-pot synthesis of novel molecular chimeras incorporating sugar, pseudo-peptide, and steroidal moieties is described. For this, a new carbohydrate-steroid conjugation approach based on the Ugi four-component reaction was implemented for the ligation of glucose and chacotriose to spirostanic steroids. The approach proved wide substrate scope, as both mono and oligosaccharides functionalized with amino, carboxy, and isocyano groups were conjugated to steroidal substrates in an efficient, multicomponent manner. Two alternative strategies based on the hydrazoic acid variant of the Ugi reaction were employed for the synthesis of tetrazole-based chacotriose-diosgenin conjugates resembling naturally occurring spirostan saponins. This is the first time that triple sugar/pseudo-peptide/steroid hybrids are produced, thus opening up an avenue of opportunities for applications in drug discovery and biological chemistry.

  8. MICROWAVE-ACCELERATED MULTICOMPONENT REACTIONS UNDER SOLVENT-FREE CONDITIONS

    EPA Science Inventory

    The application of microwave-accelerated solventless synthetic protocols in multicomponent (MCC) reactions will be exemplified by several condensation and cyclization reactions including the rapid one-pot assembly of valuable heterocyclic compounds from in situ generated intermed...

  9. Preparation of nonsymmetrically substituted stilbenes in a one-pot two-step heck strategy using ethene as a reagent.

    PubMed

    Kormos, Chad M; Leadbeater, Nicholas E

    2008-05-16

    We present here a strategy for the preparation of nonsymmetrically substituted stilbenes using a one-pot two-step double Heck strategy. First a protocol is developed for the selective preparation of a range of styrenes using ethene as the alkene coupling partner. Then conditions are found for the effective coupling of the styrenes with aryl halides using a 1:1 stoichiometric ratio of the two components. The use of the microwave apparatus to perform the reactions offers a convenient method for synthesis as well as for safely, easily, and accurately loading vessels with gaseous reagents.

  10. Multi-component ground motion response spectra for coupled horizontal, vertical, angular accelerations, and tilt

    USGS Publications Warehouse

    Kalkan, E.; Graizer, V.

    2007-01-01

    Rotational and vertical components of ground motion are almost always ignored in design or in the assessment of structures despite the fact that vertical motion can be twice as much as the horizontal motion and may exceed 2g level, and rotational excitation may reach few degrees in the proximity of fault rupture. Coupling of different components of ground excitation may significantly amplify the seismic demand by introducing additional lateral forces and enhanced P-?? effects. In this paper, a governing equation of motion is postulated to compute the response of a SDOF oscillator under a multi-component excitation. The expanded equation includes secondary P-?? components associated with the combined impacts of tilt and vertical excitations in addition to the inertial forcing terms due to the angular and translational accelerations. The elastic and inelastic spectral ordinates traditionally generated considering the uniaxial input motion are compared at the end with the multi-component response spectra of coupled horizontal, vertical and tilting motions. The proposed multi-component response spectrum reflects kinematic characteristics of the ground motion that are not identifiable by the conventional spectrum itself, at least for the near-fault region where high intensity vertical shaking and rotational excitation are likely to occur.

  11. Combined Pd/C and Montmorillonite Catalysis for One-Pot Synthesis of Benzimidazoles

    PubMed Central

    Weires, Nicholas A.; Boster, Jared; Magolan, Jakob

    2013-01-01

    A series of nineteen benzimidazoles are prepared from ortho-nitroanilines via one-pot transfer hydrogenation, condensation, and dehydrogenation enabled by the concurrent use of two heterogeneous catalysts: montmorillonite-K10 and Pd/C. This strategy is further employed to accomplish a five-step, three-component synthesis of an antifungal benzimidazoquinazoline using a simple one-pot procedure. PMID:23525858

  12. One-Pot Benzo[b]phosphole Synthesis through Sequential Alkyne Arylmagnesiation, Electrophilic Trapping, and Intramolecular Phospha-Friedel-Crafts Cyclization.

    PubMed

    Wu, Bin; Chopra, Rena; Yoshikai, Naohiko

    2015-11-20

    A one-pot multicomponent synthesis of a benzo[b]phosphole derivative has been achieved by a sequence of transition-metal-catalyzed arylmagnesiation of an internal alkyne, electrophilic trapping of the resulting alkenylmagnesium species with a dichloroorganophosphine, and an intramolecular phospha-Friedel-Crafts reaction. With appropriate arylmagnesiation and P-C bond formation conditions, the present method allows for the modular and expedient preparation of benzophospholes bearing a variety of substituents on the phosphorus atom, the C2 and C3 atoms, and the "benzo" moiety.

  13. Tandem one-pot synthesis of flavans by recyclable silica-HClO4 catalyzed Knoevenagel condensation and [4 + 2]-Diels-Alder cycloaddition.

    PubMed

    Bharate, Sandip B; Mudududdla, Ramesh; Bharate, Jaideep B; Battini, Narsaiah; Battula, Satyanarayana; Yadav, Rammohan R; Singh, Baldev; Vishwakarma, Ram A

    2012-07-14

    An efficient one-pot multi-component synthesis of flavans using perchloric acid supported on silica as a recyclable heterogeneous catalyst has been described. This is the first report of direct one-step construction of a flavan skeleton from a phenolic precursor. The method involves a Knoevenagel-type condensation leading to in situ formation of transient O-quinone methide which further undergoes [4 + 2]-Diels-Alder cycloaddition with styrene to yield a flavan skeleton. The method provides easy access to a wide range of bio-active natural products viz. flavonoids, anthocyanins and catechins.

  14. A semi-discrete integrable multi-component coherently coupled nonlinear Schrödinger system

    NASA Astrophysics Data System (ADS)

    Zhao, Hai-qiong; Yuan, Jinyun

    2016-07-01

    A new integrable semi-discrete version is proposed for the multi-component coherently coupled nonlinear Schrödinger equation. The integrability of the semi-discrete system is confirmed by existence of Lax pair and infinite number of conservation laws. With the aid of gauge transformations, explicit formulas for N-fold Darboux transformations are derived whereby some physically important solutions of the system are presented. Furthermore, the theory of the semi-discrete system including Lax pair, Darboux transformations, exact solutions and infinite number of conservation laws are shown for their continuous counterparts in the continuous limit.

  15. Multi-Component Reactions in Heterocyclic Chemistry

    NASA Astrophysics Data System (ADS)

    Müller, Thomas J. J.; Orru, Romano V. A.; Chebanov, Valentin A.; Sakhno, Yana I.; Saraev, Vyacheslav E.; Muravyova, Elena A.; Andrushchenko, Anastasia Yu.; Desenko, Sergey M.; Akhmetova, V. R.; Khabibullina, G. R.; Rakhimova, E. B.; Vagapov, R. A.; Khairullina, R. R.; Niatshina, Z. T.; Murzakova, N. N.; Maslivets, Andrey N.; Voskressensky, Leonid G.; Danagulyan, Gevorg G.; Murtchyan, Armen D.; Tumanyan, Araksya K.; Banfi, Luca; Basso, Andrea; de Moliner, Fabio; Guanti, Giuseppe; Petricci, Elena; Riva, Renata; Taddei, Maurizio; Naimi-Jamal, M. Reza; Mashkouri, Sara; Sharifi, Ali; Przhevalski, Nikolai M.; Rozhkova, Elena N.; Tokmakov, Gennadii P.; Magedov, Igor V.; Armisheva, M. N.; Rassudihina, N. A.; Vahrin, M. I.; Gein, V. L.; Shaabani, Ahmad; Rezayan, Ali Hossein; Sarvary, Afshin; Heidary, Marjan; Ng, Seik Weng; Beliaev, Nikolai A.; Mokrushin, Vladimir S.; Paramonov, Igor V.; Ilyin, Alexey; Garkushenko, Anna K.; Dushek, Maria A.; Sagitullina, Galina P.; Sagitullin, Reva S.; Kysil, Volodymyr; Khvat, Alexander; Tsirulnikov, Sergey; Tkachenko, Sergey; Ivachtchenko, Alexandre; Gein, Vladimir L.; Panova, Olga S.; Ilyn, Alexey P.; Kravchenko, Dmitri V.; Potapov, Victor V.; Ivachtchenko, Alexandre V.; Vichegjanina, V. N.; Levandovskaya, E. B.; Gein, V. L.; Vahrin, M. I.; Vladimirov, I. N.; Zorina, A. A.; Nosova, N. V.; Gein, V. L.; Fedorova, O. V.; Vahrin, M. I.

    Multi-component and domino reactions are efficient and effective methods in the sustainable and diversity-oriented synthesis of heterocycles. In particular, transition metal-catalyzed multi-component sequences have recently gained considerable interest. Based upon the Sonogashira entry to alkynones, alkenones, and intermediate allenes, we have opened new avenues to the one-pot synthesis of numerous classes of heterocyclic frameworks in an MCR fashion. This methodological approach has now found various applications in one-pot syntheses of functional chromophores, pharmaceutically active compounds, and marine alkaloids and derivatives.

  16. Scalable, One-Pot, Microwave-Accelerated Tandem Synthesis of Unsymmetrical Urea Derivatives.

    PubMed

    Kulkarni, Abhijit R; Garai, Sumanta; Thakur, Ganesh A

    2017-01-20

    We report a facile, microwave-accelerated, one-pot tandem synthesis of unsymmetrical ureas via a Curtius rearrangement. In this method, one-pot microwave irradiation of commercially available (hetero)aromatic acids and amines in the presence of diphenylphosphoryl azide enabled extremely rapid (1-5 min) construction of an array of unsymmetrical ureas in good to excellent yields. We demonstrate the utility of our method in the efficient, gram-scale synthesis of key biologically active compounds targeting the cannabinoid 1 and α7 nicotinic acetylcholine receptors.

  17. Development of a one-pot assay for screening and identification of Mur pathway inhibitors in Mycobacterium tuberculosis

    PubMed Central

    Eniyan, Kandasamy; Kumar, Anuradha; Rayasam, Geetha Vani; Perdih, Andrej; Bajpai, Urmi

    2016-01-01

    The cell wall of Mycobacterium tuberculosis (Mtb) consists of peptidoglycan, arabinogalactan and mycolic acids. The cytoplasmic steps in the peptidoglycan biosynthetic pathway, catalyzed by the Mur (A-F) enzymes, involve the synthesis of UDP-n-acetylmuramyl pentapeptide, a key precursor molecule required for the formation of the peptidoglycan monomeric building blocks. Mur enzymes are indispensable for cell integrity and their lack of counterparts in eukaryotes suggests them to be promising Mtb drug targets. However, the caveat is that most of the current assays utilize a single Mur enzyme, thereby identifying inhibitors against only one of the enzymes. Here, we report development of a one-pot assay that reconstructs the entire Mtb Mur pathway in vitro and has the advantage of eliminating the requirement for nucleotide intermediates in the pathway as substrates. The MurA-MurF enzymes were purified and a one-pot assay was developed through optimization of successive coupled enzyme assays using UDP-n-acetylglucosamine as the initial sugar substrate. The assay is biochemically characterized and optimized for high-throughput screening of molecules that could disrupt multiple targets within the pathway. Furthermore, we have validated the assay by performing it to identify D-Cycloserine and furan-based benzene-derived compounds with known Mur ligase inhibition as inhibitors of Mtb MurE and MurF. PMID:27734910

  18. Mussel-inspired one-pot synthesis of a fluorescent and water-soluble polydopamine-polyethyleneimine copolymer.

    PubMed

    Zhao, Chenxu; Zuo, Fang; Liao, Zhijian; Qin, Zhenli; Du, Sinan; Zhao, Zhigang

    2015-05-01

    Inspired by the molecular mechanics of mussel adhesive formation, a novel water-soluble fluorescent macromolecule (polydopamine-polyethyleneimine (PDA-PEI)) is prepared by one-pot copolymerization of dopamine (DA) and PEI. In this method, DA is polymerized to form PDA, which is then coupled with PEI mainly through Michael addition. The fluorescence property of PDA-PEI is mainly attributed to the Michael addition of PEI on the 5,6-dihydroxyindole (DHI) units of PDA, where PEI can form hydrogen bonds with oxidative products such as DHI and force the DHI units to twist out of plane, resulting in a decrease in the intra- and intermolecular coupling of PDA. In addition, the influence of various metal cations on the fluorescence of the PDA-PEI copolymer is investigated. This work may facilitate the development of new strategies for controlling the emission characteristics of PDA.

  19. PdCo/Pd-Hexacyanocobaltate Hybrid Nanoflowers: Cyanogel-Bridged One-Pot Synthesis and Their Enhanced Catalytic Performance

    PubMed Central

    Liu, Zhen-Yuan; Fu, Geng-Tao; Zhang, Lu; Yang, Xiao-Yu; Liu, Zhen-Qi; Sun, Dong-Mei; Xu, Lin; Tang, Ya-Wen

    2016-01-01

    Elaborate architectural manipulation of nanohybrids with multi-components into controllable 3D hierarchical structures is of great significance for both fundamental scientific interest and realization of various functionalities, yet remains a great challenge because different materials with distinct physical/chemical properties could hardly be incorporated simultaneously into the synthesis process. Here, we develop a novel one-pot cyanogel-bridged synthetic approach for the generation of 3D flower-like metal/Prussian blue analogue nanohybrids, namely PdCo/Pd-hexacyanocobaltate for the first time. The judicious introduction of polyethylene glycol (PEG) and the formation of cyanogel are prerequisite for the successful fabrication of such fascinating hierarchical nanostructures. Due to the unique 3D hierarchical structure and the synergistic effect between hybrid components, the as-prepared hybrid nanoflowers exhibit a remarkable catalytic activity and durability toward the reduction of Rhodamine B (RhB) by NaBH4. We expect that the obtained hybrid nanoflowers may hold great promises in water remediation field and beyond. Furthermore, the facile synthetic strategy presented here for synthesizing functional hybrid materials can be extendable for the synthesis of various functional hybrid nanomaterials owing to its versatility and feasibility. PMID:27573057

  20. PdCo/Pd-Hexacyanocobaltate Hybrid Nanoflowers: Cyanogel-Bridged One-Pot Synthesis and Their Enhanced Catalytic Performance

    NASA Astrophysics Data System (ADS)

    Liu, Zhen-Yuan; Fu, Geng-Tao; Zhang, Lu; Yang, Xiao-Yu; Liu, Zhen-Qi; Sun, Dong-Mei; Xu, Lin; Tang, Ya-Wen

    2016-08-01

    Elaborate architectural manipulation of nanohybrids with multi-components into controllable 3D hierarchical structures is of great significance for both fundamental scientific interest and realization of various functionalities, yet remains a great challenge because different materials with distinct physical/chemical properties could hardly be incorporated simultaneously into the synthesis process. Here, we develop a novel one-pot cyanogel-bridged synthetic approach for the generation of 3D flower-like metal/Prussian blue analogue nanohybrids, namely PdCo/Pd-hexacyanocobaltate for the first time. The judicious introduction of polyethylene glycol (PEG) and the formation of cyanogel are prerequisite for the successful fabrication of such fascinating hierarchical nanostructures. Due to the unique 3D hierarchical structure and the synergistic effect between hybrid components, the as-prepared hybrid nanoflowers exhibit a remarkable catalytic activity and durability toward the reduction of Rhodamine B (RhB) by NaBH4. We expect that the obtained hybrid nanoflowers may hold great promises in water remediation field and beyond. Furthermore, the facile synthetic strategy presented here for synthesizing functional hybrid materials can be extendable for the synthesis of various functional hybrid nanomaterials owing to its versatility and feasibility.

  1. Effects of interleaflet coupling on the morphologies of multicomponent lipid bilayer membranes

    NASA Astrophysics Data System (ADS)

    Funkhouser, Chloe M.; Mayer, Michael; Solis, Francisco J.; Thornton, K.

    2013-01-01

    We investigate dynamical and stationary compositional and surface morphologies in macroscopically phase-separating multicomponent lipid bilayer membranes using a computational model. We employ a phase-field method for the description of the coexisting phases and treat the two leaflets individually while including interleaflet interactions. The compositional evolution of the two leaflets is coupled to the shape evolution of the membrane via a Helfrich free energy with a composition-dependent spontaneous curvature. We investigate the effects of the interleaflet interaction on the dynamics and stationary states of a system favoring nonzero spontaneous curvatures. Morphological phase diagrams are mapped in composition space using three different interleaflet coupling strengths. We find that characteristics sensitive to the coupling strength include the time required to develop regions of fully separated phases, the prevalence of a stripe morphology, and the shifting of phase compositions to accommodate energetically favorable interactions across leaflets. Characteristics found to be robust with respect to coupling strength include (1) the stripe morphology is favored at nearly equal mixtures and (2) phase separation is prevented in systems where a pair of phases that preferentially interact across leaflets together occupy nearly all or none of the membrane.

  2. One-pot reductive mono-N-alkylation of aniline and nitroarene derivatives using aldehydes.

    PubMed

    Byun, Eunyoung; Hong, Bomi; De Castro, Kathlia A; Lim, Minkyung; Rhee, Hakjune

    2007-12-07

    One-pot reductive mono-N-alkylation of aniline and nitroarene derivatives using various aldehydes by Pd/C catalyst in aqueous 2-propanol solvent with ammonium formate as in situ hydrogen donor is illustrated. The reaction proceeded smoothly and selectively with excellent yield at room temperature. Our protocol presents a facile, economical, and environmentally benign alternative for reductive amination.

  3. One-Pot Synthesis of Rotationally Restricted, Conjugatable, BODIPY Derivatives from Phthalides.

    PubMed

    Del Río, Mayca; Lobo, Fernando; López, J Cristobal; Oliden, Ainhoa; Bañuelos, Jorge; López-Arbeloa, Iñigo; Garcia-Moreno, Inmaculada; Gómez, Ana M

    2017-01-20

    O-Ethylation of phthalides with Meerwein's reagent followed by reaction of the ensuing salts with pyrrole, results in the formation of 5-alkoxy-5-phenyl dipyrromethane derivatives, which function as ready precursors of ortho-substituted 8-aryl BODIPY derivatives by reaction with borontrifluoride etherate, an overall process that can be carried out in a one-pot operation.

  4. One-Pot Anti-Markovnikov Hydroamination of Unactivated Alkenes by Hydrozirconation and Amination

    PubMed Central

    Strom, Alexandra E.

    2013-01-01

    A one-pot hydroamination of alkenes is reported. The synthesis of primary and secondary amines from unactivated olefins was accomplished in the presence of a variety of functional groups. Hydrozirconation, followed by amination with nitrogen electrophiles, provides exclusive anti-Markovnikov selectivity, and most products are isolated in high yields without the use of column chromatography. PMID:23899320

  5. One pot direct synthesis of amides or oxazolines from carboxylic acids using Deoxo-Fluor reagent.

    PubMed

    Kangani, Cyrous O; Kelley, David E

    2005-12-19

    A mild and highly efficient one pot-one step condensation and/or condensation-cyclization of various acids to amides and/or oxazolines using Deoxo-Fluor reagents is described. Parallel syntheses of various free fatty acids with 2-amino-2, 2-dimethyl-1-propanol resulted with excellent yields.

  6. One pot synthesis of cyclohexanone oxime from nitrobenzene using a bifunctional catalyst.

    PubMed

    Rubio-Marqués, Paula; Hernández-Garrido, Juan Carlos; Leyva-Pérez, Antonio; Corma, Avelino

    2014-02-18

    Cyclohexanone oxime is formed from nitrobenzene with 97% yield in a one-pot reaction catalysed by palladium and gold nanoparticles on carbon. The reaction is carried out under hydrogen at 60 °C and the overall transformation involves a multi-step catalysed mechanism from which intermediates and catalytically active species have been identified.

  7. Diversity oriented one-pot three-component sequential synthesis of annulated benzothiazoloquinazolines

    PubMed Central

    2012-01-01

    Annulated benzothiazoloquinazolines have been synthesized by a diversity oriented simple and convenient synthesis involving one-pot three-component reaction of substituted 2-aminobenzothiazoles with α-tetralone and aromatic/heteroaromatic aldehydes in ethanol in the presence of catalytic amount of triethylamine. The synthesized compounds have been characterized by their elemental analyses and spectral data. PMID:22381142

  8. One-pot o-nitrobenzenesulfonylhydrazide (NBSH) formation-diimide alkene reduction protocol.

    PubMed

    Marsh, Barrie J; Carbery, David R

    2009-04-17

    A one-pot protocol for the formation of 2-nitrobenzenesulfonylhydrazide (NBSH) from commercial reagents and subsequent alkene reduction is presented. The transformation is operationally simple and generally efficient for effecting diimide alkene reductions. A range of 16 substrates have been reduced, highlighting the unique chemoselectivity of diimide as a reduction system.

  9. Gels and threads: mussel-inspired one-pot route to advanced responsive materials.

    PubMed

    Krogsgaard, M; Andersen, A; Birkedal, H

    2014-11-11

    An inexpensive one-pot route to self-healing hydrogels with pH-tunable modulus is presented. Hydrogels were formed by reacting tannic acid, trivalent metal ions and polyallylamine. Below pH 8 the hydrogels were supramolecular while above, covalent cross-linking strengthened the hydrogels. From concentrated mixtures, threads were spun, acting as water sensitive mechanical locks.

  10. Dienamine and Friedel-Crafts one-pot synthesis, and antitumor evaluation of diheteroarylalkanals.

    PubMed

    Frías, María; Padrón, José M; Alemán, José

    2015-05-26

    An asymmetric synthesis of diheteroarylalkanals through one-pot dienamine and Friedel-Crafts reaction is presented. The reaction tolerates a large variety of substituents at different positions of the starting aldehyde and also in the indole nucleophile, and a range of diheterocyclic alkanals can be achieved. Furthermore, we have studied the antiproliferative activity of these new compounds in representative cancer tumor cell lines.

  11. One-pot synthesis of responsive catalytic Au@PVP hybrid nanogels.

    PubMed

    Xiao, Chuanfu; Chen, Shoumin; Zhang, Laiying; Zhou, Shuiqin; Wu, Weitai

    2012-12-14

    Responsive catalytic hybrid nanogels with Au nanoparticle cores and a polyvinylpyrrolidone (PVP) based gel shell are prepared through a novel one-pot approach. The embedded Au nanoparticles demonstrate both a pH-modulated catalytic activity and anti-aggregation properties upon recycling.

  12. One-pot synthesis of novel 2,3-dihydro-1H-indazoles.

    PubMed

    Breton, Gary W; Lepore, Antonio J

    2011-11-16

    A copper(I)-mediated one-pot synthesis of 2,3-dihydro-1H-indazole heterocycles has been developed. This synthetic route provides the desired indazoles in moderate to good yields (55%-72%) which are substantially better than those achievable with an alternative two-step reaction sequence. The reaction is tolerant of functionality on the aromatic ring.

  13. One pot Click chemistry: A three component reaction for the synthesis of 2-mercaptobenzimidazole linked coumarinyl triazoles as anti-tubercular agents.

    PubMed

    Anand, Ashish; Kulkarni, Manohar V; Joshi, Shrinivas D; Dixit, Sheshagiri R

    2016-10-01

    2-Propargylthiobenzimidazole 1, 4-bromomethyl coumarins/1-aza-coumarins 2/3 and sodium azide have been reacted in one pot under Click chemistry conditions to give exclusively 1,4-disubstituted triazoles 5a-n. Anti-tubercular assays against M. tuberculosis (H37Rv) coupled with in silico molecular docking studies indicated that dimethyl substituents 5c and 5d showed promising activity with higher C-score values.

  14. Lewis acid-promoted reactions of zirconacyclopentadienes with isocyanates. A one-pot three-component synthesis of multiply-substituted iminocyclopentadienes from one isocyanate and two alkynes.

    PubMed

    Lu, Jiang; Mao, Guoliang; Zhang, Wenxiong; Xi, Zhenfeng

    2005-10-14

    Multiply-substituted iminocyclopentadienes were formed from Lewis acid-promoted reactions of zirconacyclopentadienes and isocyanates via a one-pot three-component coupling process; the C=O double bond of the RN=C=O moiety in the isocyanate was cleaved, and the isocyanates behaved formally as a one-carbon unit with Lewis acid-dependent and substituent-dependent reactions being realized.

  15. Amide-controlled, one-pot synthesis of tri-substituted purines generates structural diversity and analogues with trypanocidal activity.

    PubMed

    Pineda de las Infantas y Villatoro, Maria J; Unciti-Broceta, Juan D; Contreras-Montoya, Rafael; Garcia-Salcedo, Jose A; Gallo Mezo, Miguel A; Unciti-Broceta, Asier; Diaz-Mochon, Juan J

    2015-03-16

    A novel one-pot synthesis of tri-substituted purines and the discovery of purine analogues with trypanocidal activity are reported. The reaction is initiated by a metal-free oxidative coupling of primary alkoxides and diaminopyrimidines with Schiff base formation and subsequent annulation in the presence of large N,N-dimethylamides (e.g. N,N-dimethylpropanamide or larger). This synthetic route is in competition with a reaction previously-reported by our group, allowing the generation of a combinatorial library of tri-substituted purines by the simple modification of the amide and the alkoxide employed. Among the variety of structures generated, two purine analogues displayed trypanocidal activity against the protozoan parasite Trypanosoma brucei with IC50 < 5 μM, being each of those compounds obtained through each of the synthetic pathways.

  16. Synthesis and one-pot tethering of hydroxyl-capped phosphorylcholine onto cellulose membrane for improving hemocompatibility and antibiofouling property.

    PubMed

    Yuan, Jiang; Tong, Ling; Yi, Huaixiang; Wang, Bingxiang; Shen, Jian; Lin, Sicong

    2013-11-01

    Tethering of biomimetic phosphorylcholine derivative onto the surface of biomedical devices is an effective method for improving hemocompatibility and antibiofouling property. Herein, series of novel hydroxyl-capped phosphorylcholines (HOPC) with different carbon spacer lengths were first synthesized and characterized with element analysis (EA), Fourier transform infrared spectroscopy(FTIR), and nuclear magnetic resonance spectroscopy (NMR). Then, HOPC (n=5, 2a) was one-pot tethered onto cellulose membrane with hexamethylene diisocyanate (HDI) as a coupling agent. The existence of phosphorylcholine was demonstrated by water contact angle measurement, attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR), atomic force microscopy (AFM), and X-ray photoelectron spectroscopy (XPS). The hemocompatibility and antibiofouling property were evaluated by hemolytic test, platelet adhesion, protein adsorption, and Escherichia coli adhesion test. The results showed that cellulose membranes tethered with HOPC exhibited excellent hemocompatibility featured by low platelet adhesion and fibrinogen adsorption as well as antibiofouling property with bacterial adhesion resistance.

  17. Modeling multicomponent ionic transport in groundwater with IPhreeqc coupling: Electrostatic interactions and geochemical reactions in homogeneous and heterogeneous domains

    NASA Astrophysics Data System (ADS)

    Muniruzzaman, Muhammad; Rolle, Massimo

    2016-12-01

    The key role of small-scale processes like molecular diffusion and electrochemical migration has been increasingly recognized in multicomponent reactive transport in saturated porous media. In this study, we propose a two-dimensional multicomponent reactive transport model taking into account the electrostatic interactions during transport of charged ions in physically and chemically heterogeneous porous media. The modeling approach is based on the local charge balance and on the description of compound-specific and spatially variable diffusive/dispersive fluxes. The multicomponent ionic transport code is coupled with the geochemical code PHREEQC-3 by utilizing the IPhreeqc module, thus enabling to perform the geochemical calculations included in the PHREEQC's reaction package. The multicomponent reactive transport code is benchmarked with different 1-D and 2-D transport problems. Successively, conservative and reactive transport examples are presented to demonstrate the capability of the proposed model to simulate transport of charged species in heterogeneous porous media with spatially variable physical and chemical properties. The results reveal that the Coulombic cross-coupling between dispersive fluxes can significantly influence conservative as well as reactive transport of charged species both at the laboratory and at the field scale.

  18. Gold-silver-alloy nanoprobes for one-pot multiplex DNA detection

    NASA Astrophysics Data System (ADS)

    Doria, G.; Larguinho, M.; Dias, J. T.; Pereira, E.; Franco, R.; Baptista, P. V.

    2010-06-01

    A specific colorimetric DNA detection method based on oligonucleotide functionalized gold-silver-alloy nanoparticles (AuAg-alloy-nanoprobes) is presented. The AuAg-alloy-nanoprobes were then used for the specific detection of a DNA sequence from TP53—a gene involved in cancer development. The AuAg-alloy-nanoprobes were then used in combination with Au-nanoprobes for a one-pot dual-colour detection strategy that allowed for the simultaneous differential detection of two distinct target sequences. This system poses an unprecedented opportunity to explore the combined use of metal nanoparticles with different composition towards the development of a multiplex one-pot colorimetric assay for DNA detection.

  19. Compartmentalization of incompatible reagents within Pickering emulsion droplets for one-pot cascade reactions.

    PubMed

    Yang, Hengquan; Fu, Luman; Wei, Lijuan; Liang, Jifen; Binks, Bernard P

    2015-01-28

    It is a dream that future synthetic chemistry can mimic living systems to process multistep cascade reactions in a one-pot fashion. One of the key challenges is the mutual destruction of incompatible or opposing reagents, for example, acid and base, oxidants and reductants. A conceptually novel strategy is developed here to address this challenge. This strategy is based on a layered Pickering emulsion system, which is obtained through lamination of Pickering emulsions. In this working Pickering emulsion, the dispersed phase can separately compartmentalize the incompatible reagents to avoid their mutual destruction, while the continuous phase allows other reagent molecules to diffuse freely to access the compartmentalized reagents for chemical reactions. The compartmentalization effects and molecular transport ability of the Pickering emulsion were investigated. The deacetalization-reduction, deacetalization-Knoevenagel, deacetalization-Henry and diazotization-iodization cascade reactions demonstrate well the versatility and flexibility of our strategy in processing the one-pot cascade reactions involving mutually destructive reagents.

  20. One-pot modification of 5'-capped RNA based on methionine analogs.

    PubMed

    Muttach, Fabian; Rentmeister, Andrea

    2016-09-01

    This paper outlines chemically and enzymatically synthesized S-adenosylmethionine (AdoMet) analogs and their use in the site-specific modification of RNA by methyltransferases, enabling the facile attachment of clickable moieties to the nucleic acid. We then focus on methodological aspects of setting up a methyltransferase-based enzymatic cascade reaction starting from methionine analogs. This strategy is applied to the one-pot modification of the mRNA cap which is subsequently derivatized in copper-free and copper-catalyzed click reactions. We show that high transfer efficiencies to the cap are obtained using Se-propargyl-, hexenynyl- and azido-bearing methionine analogs. By switching to other methyltransferases our one-pot modification approach should be directly applicable to the regiospecific modification of other target molecules including nucleic acids, proteins and small molecules.

  1. One-pot lipase-catalyzed aldol reaction combination of in situ formed acetaldehyde.

    PubMed

    Wang, Na; Zhang, Wei; Zhou, Long-Hua; Deng, Qing-Feng; Xie, Zong-Bo; Yu, Xiao-Qi

    2013-12-01

    A facile tandem route to α,β-unsaturated aldehydes was developed by combining the two catalytic activities of the same enzyme in a one-pot strategy for the aldol reaction and in situ generation of acetaldehyde. Lipase from Mucor miehei was found to have conventional and promiscuous catalytic activities for the hydrolysis of vinyl acetate and aldol condensation with in situ formed acetaldehyde. The first reaction continuously provided material for the second reaction, which effectively reduced the volatilization loss, oxidation, and polymerization of acetaldehyde, as well as avoided a negative effect on the enzyme of excessive amounts of acetaldehyde. After optimizing the process, several substrates participated in the reaction and provided the target products in moderate to high yields using this single lipase-catalyzed one-pot biotransformation.

  2. Regioselective one-pot protection and protection-glycosylation of carbohydrates.

    PubMed

    Wang, Cheng-Chung; Zulueta, Medel Manuel L; Hung, Shang-Cheng

    2011-01-01

    Deciphering the roles and structure-activity relationships of carbohydrates in biological processes requires access to sugar molecules of confirmed structure and high purity. Chemical synthesis is one of the best ways to obtain such access. However, the synthesis of carbohydrates has long been impeded by two major challenges--the regioselective protection of the polyol moiety of each monosaccharide building block and the stereoselective glycosylation to produce oligosaccharides of desired length. Here, we review the development of the first regioselective protection-glycosylation and a revolutionary regioselective combinatorial one-pot protection of monosaccharides that can be used to differentiate the various hydroxy groups of monosaccharides with a vast array of orthogonal protective groups in one-pot procedures.

  3. Highly efficient non-precious metal electrocatalysts prepared from one-pot synthesized zeolitic imidazolate frameworks.

    PubMed

    Zhao, Dan; Shui, Jiang-Lan; Grabstanowicz, Lauren R; Chen, Chen; Commet, Sean M; Xu, Tao; Lu, Jun; Liu, Di-Jia

    2014-02-01

    A facile synthesis of non-PGM ORR electrocatalysts through thermolysis of one-pot synthesized ZIF is demonstrated. The electrocatalysts exhibit excellent activity, with a maximum volumetric current density of 88.1 A cm(-3) measured at 0.8 V in PEFC tests. This approach not only makes ZIFs-based electrocatalysts easy to scale up, but also paves the way for the tailored synthesis of electrocatalysts.

  4. Hcp cobalt nanocrystals with high magnetic anisotropy prepared by easy one-pot synthesis.

    PubMed

    Meziane, L; Salzemann, C; Aubert, C; Gérard, H; Petit, C; Petit, M

    2016-11-10

    Herein we describe the first synthesis of pure mono-disperse spherical hcp-nanocrystals ferromagnetic at room temperature. Our strategy, based on the simple combination of oleylamine and ClCo(PPh3)3, allows the one-pot synthesis of size-controlled hcp-nanocrystals. The size and shape of the nanocrystals can be tuned by varying the reaction time or the concentration.

  5. Enantioselective one-pot synthesis of 2-amino-4-(indol-3-yl)-4H-chromenes.

    PubMed

    Chen, Weiliang; Cai, Yunfei; Fu, Xuan; Liu, Xiaohua; Lin, Lili; Feng, Xiaoming

    2011-09-16

    An enantioselective one-pot synthesis of 2-amino-4-(indol-3-yl)-4H-chromenes via a Knoevenagel/Pinner/Friedel-Crafts reaction of salicylaldehyde, malononitrile, and indole is presented. Moderate to good yields (up to 89%) and high enantioselectivities (up to 90% ee) were obtained with an N,N'-dioxide-Zn(II) complex as the catalyst. This strategy provides an efficient and convenient method to access enantiomerically enriched 2-amino-4H-chromene derivatives.

  6. Regioselective One-Pot Synthesis of Triptycenes via Triple-Cycloadditions of Arynes to Ynolates.

    PubMed

    Umezu, Satoshi; Dos Passos Gomes, Gabriel; Yoshinaga, Tatsuro; Sakae, Mikei; Matsumoto, Kenji; Iwata, Takayuki; Alabugin, Igor; Shindo, Mitsuru

    2017-01-24

    We developed the novel one-pot synthetic method of substituted triptycenes by the reaction of ynolates and arynes. This four-step process involves three cycloadditions and electrocyclic ring opening of the strained Dewar anthracene. Each of the three related but structurally distinct classes of nucleophiles (ynolate, enolate, and anthracenolate) reacts with o-benzyne in the same predictable manner controlled by chelation and negative hyperconjugation. The resulting functionalized C3 -symmetrical triptycenes hold promise in the design of functional materials.

  7. One-Pot Strategy for Thiazoline Synthesis from Alkenes and Thioamides.

    PubMed

    Alom, Nur-E; Wu, Fan; Li, Wei

    2017-02-17

    A convenient synthesis of a privileged pharmaceutical motif, thiazoline is accomplished. This reaction utilizes simple and readily available alkene and thioamide substrates in an intermolecular fashion via a simple one-pot procedure. A wide range of functional groups is tolerated, and the thiazoline product has been further utilized for the synthesis of the corresponding β-aminothiol and thiazole from routine hydrolysis and oxidation protocols.

  8. One-pot synthesis of hypervalent iodine reagents for electrophilic trifluoromethylation.

    PubMed

    Matoušek, Václav; Pietrasiak, Ewa; Schwenk, Rino; Togni, Antonio

    2013-07-05

    Simplified syntheses suited for large scale preparations of the two hypervalent iodine reagents 1 and 2 for electrophilic trifluoromethylation are reported. In both cases, the stoichiometric oxidants sodium metaperiodate and tert-butyl hypochlorite have been replaced by trichloroisocyanuric acid. Reagent 1 is accessible in a one-pot procedure from 2-iodobenzoic acid in 72% yield. Reagent 2 was prepared via fluoroiodane 11 in a considerably shorter reaction time and with no need of an accurate temperature control.

  9. Facile one-pot synthesis of porphyrin based porous polymer networks (PPNs) as biomimetic catalysts

    SciTech Connect

    Zou, LF; Feng, DW; Liu, TF; Chen, YP; Fordham, S; Yuan, S; Tian, J; Zhou, HC

    2015-01-01

    Stable porphyrin based porous polymer networks, PPN-23 and PPN-24, have been synthesized through a facile one-pot approach by the aromatic substitution reactions of pyrrole and aldehydes. PPN-24(Fe) shows high catalytic efficiency as a biomimetic catalyst in the oxidation reaction of 2,2'-azino-bis(3-ethylbenzthiazoline-6-sulfonic acid) (ABTS) in the presence of H2O2.

  10. One-pot polyol synthesis of highly monodisperse short green silver nanorods.

    PubMed

    Patarroyo, Javier; Genç, Aziz; Arbiol, Jordi; Bastús, Neus G; Puntes, Victor

    2016-09-21

    Green silver nanorods (Ag NRs) of a low aspect ratio (2.8) have been produced in high yields via an optimized, simple, and robust one-pot polyol method in the presence of tannic acid, which favors the nucleation of decahedral seeds needed for the production of monodisperse Ag NRs. These Ag NRs were further used as sacrificial templates to produce Au hollow nanostructures via galvanic replacement reaction with HAuCl4 at room temperature.

  11. One-pot synthesis and characterization of subnanometre-size benzotriazolate protected copper clusters.

    PubMed

    Salorinne, Kirsi; Chen, Xi; Troff, Ralf W; Nissinen, Maija; Häkkinen, Hannu

    2012-07-21

    A simple one-pot method for the preparation of subnanometre-size benzotriazolate (BTA) protected copper clusters, Cu(n)BTA(m), is reported. The clusters were analyzed by optical and infrared spectroscopy, mass spectrometry and transmission electron microscopy together with computational methods. We suggest a structural motif where the copper core of the Cu(n)BTA(m) clusters is protected by BTA-Cu(i)-BTA units.

  12. One-pot enzymatic conversion of carbon dioxide and utilization for improved microbial growth.

    PubMed

    Hong, Sung-Gil; Jeon, Hancheol; Kim, Han Sol; Jun, Seung-Hyun; Jin, EonSeon; Kim, Jungbae

    2015-04-07

    We developed a process for one-pot CO2 conversion and utilization based on simple conversion of CO2 to bicarbonate at ambient temperature with no energy input, by using the cross-linking-based composites of carboxylated polyaniline nanofibers (cPANFs) and carbonic anhydrase. Carbonic anhydrase was immobilized on cPANFs via the approach of magnetically separable enzyme precipitate coatings (Mag-EPC), which consists of covalent enzyme attachment, enzyme precipitation, and cross-linking with amine-functionalized magnetic nanoparticles. Mag-EPC showed a half-life of 236 days under shaking, even resistance to 70% ethanol sterilization, and recyclability via facile magnetic separation. For one-pot CO2 conversion and utilization, Mag-EPC was used to accelerate the growth of microalga by supplying bicarbonate from CO2, representing 1.8-fold increase of cell concentration when compared to the control sample. After two repeated uses via simple magnetic separation, the cell concentration with Mag-EPC was maintained as high as the first cycle. This one-pot CO2 conversion and utilization is an alternative as well as complementary process to adsorption-based CO2 capture and storage as an environmentally friendly approach, demanding no energy input based on the effective action of the stabilized enzyme system.

  13. One-Pot Synthesis of (NiFe2O4)x-(SrFe12O19)1-x Nanocomposites and Their Microwave Absorption Properties.

    PubMed

    Hazra, Subhenjit; Ghosh, Barun Kumar; Patra, Manoj Kumar; Jani, Raj Kumar; Vadera, Sampat Raj; Ghosh, Narendra Nath

    2015-09-01

    In this paper, we report a simple but novel aqueous solution based 'one-pot' method for preparation of (NiFe2O4)x-(SrFe12O19)1-x nanocomposites consist of hard ferrite-soft ferrite phases. A physical mixing method has also been employed to prepare nanocomposites having same compositions. The effects of synthetic methodologies on the microstructures of the nanocomposites as well as their magnetic and microwave absorption properties have been evaluated. Crystal structures and microstructures of these composites have been investigated by using X-ray diffraction, transmission electron microscope and scanning electron microscope. In the nanocomposites, prepared by both methods, presence of nanocrystalline NiFe2O4 and SrFe12O19 phases was detected. However, nanocomposites, prepared by one-pot method, possessed better homogeneous distribution of hard and soft ferrite phases than the nanocomposites, prepared by physical mixing method. Nanocomposites, prepared by one-pot method, demonstrated significant spring exchange coupling interaction between hard and soft ferrite phases and exhibited magnetically single phase behaviour. The spring exchange coupling interaction enhanced the magnetic properties (high saturation magnetization and coercivity) and microwave absorption properties of the nanocomposites, prepared by one-pot method, in comparison with the nanocomposites prepared by physical mixing method as well as pure NiFe2O4 and SrFe12O19 nanoparticles. Minimum reflection loss of the composite was ~ -17 dB (i.e., 98% absorption) at 8.2 GHz for an absorber thickness of 3.2 mm.

  14. Covalent Modification of Organo-Functionalized Graphene Oxide and its Scope as Catalyst for One-Pot Pyrazolo-Pyranopyrimidine Derivatives.

    PubMed

    Rana, Surjyakanta; Maddila, Suresh; Yalagala, Kotaiah; Maddila, Suryanarayana; Jonnalagadda, Sreekantha B

    2015-12-01

    The surface of graphene oxide (GO) was modified using [3-(2-aminoethylamino)propyl]trimethoxysilane (diamine), which exhibited excellent catalytic activity for one-pot multicomponent reactions. The newly synthesized material was fully characterized by various instrumental techniques including Fourier-transfer infrared (FTIR) and Raman spectroscopy, scanning electron microscopy (SEM), and transmission electron microscopy (TEM). The instrumental analysis confirmed the successful grafting of organic amine functional groups onto the graphene oxide surface. The diamine-functionalized GO proved to be an excellent catalyst for the synthesis of pyrazolo-pyranopyrimidine derivatives with 93 % yield and high selectivity. The catalytic activity almost remained unaltered up to three cycles. The newly synthesized pyrazolo-pyranopyrimidine derivatives have potential use as scaffolds in designing new pharmaceutical products.

  15. Synthesis of Diverse Nitrogen-Enriched Heterocyclic Scaffolds Using a Suite of Tunable One-Pot Multicomponent Reactions

    PubMed Central

    2015-01-01

    Five elegant and switchable three-component reactions which enable access to a new series of nitrogen-containing heterocycles are reported. A novel one-step addition of an isocyanide to a hydrazine derived Schiff base affords unique six-membered pyridotriazine scaffolds (A and E). With slight modification of reaction conditions and replacement of the nucleophilic isocyanide moiety with different electrophiles (i.e., isocyanates, isothiocyanates, cyclic anhydrides, and acyl chlorides) five-membered triazolopyridine scaffolds (B, D, F, G) are generated in a single step. Furthermore, the use of phenyl hydrazine enables access to dihydroindazole-carboxamides, devoid of a bridge-head nitrogen (C). All protocols are robust and tolerate a diverse collection of reactants, and as such, it is expected that the new scaffolds and associated chemistry will garner high interest from medicinal chemists involved in either file enhancement or specific target-related drug discovery campaigns. PMID:24788091

  16. Enzymatic Menthol Production: One-Pot Approach Using Engineered Escherichia coli.

    PubMed

    Toogood, Helen S; Ní Cheallaigh, Aisling; Tait, Shirley; Mansell, David J; Jervis, Adrian; Lygidakis, Antonios; Humphreys, Luke; Takano, Eriko; Gardiner, John M; Scrutton, Nigel S

    2015-10-16

    Menthol isomers are high-value monoterpenoid commodity chemicals, produced naturally by mint plants, Mentha spp. Alternative clean biosynthetic routes to these compounds are commercially attractive. Optimization strategies for biocatalytic terpenoid production are mainly focused on metabolic engineering of the biosynthesis pathway within an expression host. We circumvent this bottleneck by combining pathway assembly techniques with classical biocatalysis methods to engineer and optimize cell-free one-pot biotransformation systems and apply this strategy to the mint biosynthesis pathway. Our approach allows optimization of each pathway enzyme and avoidance of monoterpenoid toxicity issues to the host cell. We have developed a one-pot (bio)synthesis of (1R,2S,5R)-(-)-menthol and (1S,2S,5R)-(+)-neomenthol from pulegone, using recombinant Escherichia coli extracts containing the biosynthetic genes for an "ene"-reductase (NtDBR from Nicotiana tabacum) and two menthone dehydrogenases (MMR and MNMR from Mentha piperita). Our modular engineering strategy allowed each step to be optimized to improve the final production level. Moderate to highly pure menthol (79.1%) and neomenthol (89.9%) were obtained when E. coli strains coexpressed NtDBR with only MMR or MNMR, respectively. This one-pot biocatalytic method allows easier optimization of each enzymatic step and easier modular combination of reactions to ultimately generate libraries of pure compounds for use in high-throughput screening. It will be, therefore, a valuable addition to the arsenal of biocatalysis strategies, especially when applied for (semi)-toxic chemical compounds.

  17. One-pot synthesis of 1-iodoalkynes and trisubstituted alkenes from benzylic and allylic bromides.

    PubMed

    Pelletier, Guillaume; Lie, Sharon; Mousseau, James J; Charette, André B

    2012-11-02

    1-Iodoalkynes are formed in moderate to high yields from readily accessible benzylic and allylic alkyl bromides by a one-pot homologation/double elimination procedure with iodoform (CHI(3)). The developed conditions include facile purification and avoid the use of an excess of triphenylphosphine (PPh(3)), as described in classical Corey-Fuchs iodoalkynylation conditions. Replacing CHI(3) with CHI(2)Cl allows the isolation of the corresponding gem-(Z)-chloro-(E)-iodoalkene in good yield and stereoselectivity. Moreover, the use of benzhydryl bromides as nucleophiles enables the synthesis of trisubstituted alkenes under similar reaction conditions.

  18. Diastereoselective one-pot tandem synthesis of 3-substituted isoindolinones: a mechanistic investigation.

    PubMed

    Angelin, Marcus; Rahm, Martin; Fischer, Andreas; Brinck, Tore; Ramström, Olof

    2010-09-03

    The mechanism of a base-catalyzed one-pot reaction of 2-cyanobenzaldehyde and primary nitroalkanes, to produce 3-substituted isoindolinones, has been investigated. A route starting with a nitroaldol (Henry) reaction, followed by a subsequent cyclization and rearrangement, was supported by intermediate analogue synthesis and DFT calculations. Direct diastereoselective crystallization from the reaction mixture was also achieved and studied for a number of substrates. Furthermore, the 3-substituted isoindolinones are an interesting group of compounds, both present important natural products, as well as being precursors to other valuable building blocks.

  19. One-Pot Exfoliation of Graphite and Synthesis of Nanographene/Dimesitylporphyrin Hybrids

    PubMed Central

    Bernal, M. Mar; Pérez, Emilio M.

    2015-01-01

    A simple one-pot process to exfoliate graphite and synthesize nanographene-dimesitylporphyrin hybrids has been developed. Despite the bulky mesityl groups, which are expected to hinder the efficient π–π stacking between the porphyrin core and graphene, the liquid-phase exfoliation of graphite is significantly favored by the presence of the porphyrins. Metallation of the porphyrin further enhances this effect. The resulting graphene/porphyrin hybrids were characterized by spectroscopy (UV-visible, fluorescence, and Raman) and microscopy (STEM, scanning transmission electron microscopy). PMID:25984598

  20. One-pot protection-glycosylation reactions for synthesis of lipid II analogues.

    PubMed

    Mitachi, Katsuhiko; Mohan, Priya; Siricilla, Shajila; Kurosu, Michio

    2014-04-14

    (2,6-Dichloro-4-methoxyphenyl)(2,4-dichlorophenyl)methyl trichloroacetimidate (3) and its polymer-supported reagent 4 can be successfully applied to a one-pot protection-glycosylation reaction to form the disaccharide derivative 7 d for the synthesis of lipid II analogues. The temporary protecting group or linker at the C-6 position and N-Troc protecting group of 7 d can be cleaved simultaneously through a reductive condition. Overall yields of syntheses of lipid II (1) and neryl-lipid II N(ε)-dansylthiourea are significantly improved by using the described methods.

  1. The immobilization of 3-(chloropropyl)triethoxysilane onto silica by a simple one-pot synthesis.

    PubMed

    Adam, Farook; Osman, Hasnah; Hello, Kasim Mohammed

    2009-03-01

    Sodium silicate from rice husk ash (RHA) was transformed to functionalized silica with 3-(chloropropyl)triethoxysilane (CPTES) via a simple sol-gel technique in a one-pot synthesis. The (29)Si MAS NMR of the organo-silica complex (RHACCl) showed the presence of T(2), T(3), Q(3) and Q(4) silicon centers. The (13)C MAS NMR showed that RHACCl had three chemical shifts at 10.37, 26.70 and 47.69 ppm consistent with the three carbon atoms of the CPTES moiety. The presence of carbon, silicon and chlorine was determined by a combination of elemental analysis and EDX study.

  2. Design and one-pot synthesis of new 7-acyl camptothecin derivatives as potent cytotoxic agents.

    PubMed

    Liu, Ying-Qian; Dai, Wei; Wang, Chih-Ya; Morris-Natschke, Susan L; Zhou, Xing-Wen; Yang, Liu; Yang, Xiao-Ming; Li, Wen-Qun; Lee, Kuo-Hsiung

    2012-12-15

    New 7-acyl camptothecin derivatives were designed and synthesized from camptothecin in a one-pot reaction through a Minisci type-reaction and were evaluated for cytotoxicity against four tumor cell lines, A-549, DU-145, KB, and KB-vin. All of the new compounds showed significant inhibition of human tumor cell growth, with IC(50) values ranging from 0.01538 to 13.342 μM. Most of the derivatives were more cytotoxic than irinotecan, and the (7a) and 7-propionyl (7b) analogs exhibited the highest cytotoxic activity against the tumor cell lines tested. This compound class merits further development as anticancer clinical trial candidates.

  3. One-pot Unsymmetrical Ketone Synthesis Employing a Pyrrole-Bearing Formal Carbonyl Dication Linchpin Reagent.

    PubMed

    Heller, Stephen T; Newton, James N; Fu, Tingting; Sarpong, Richmond

    2015-08-17

    A one-pot procedure for the synthesis of unsymmetrical ketones utilizing a pyrrole-bearing carbonyl linchpin reagent (carbonyl linchpin N,O-dimethylhydroxylamine pyrrole; CLAmP) is reported. In contrast to other carbonyl dielectrophile equivalents, CLAmP enables the synthesis of ketones from a variety of organolithium and Grignard reagents. The electrophilic nature of CLAmP enables the addition of less reactive as well as thermally unstable nucleophiles. CLAmP was designed to form kinetically stable tetrahedral intermediates upon the addition of organometallic nucleophiles. Evidence for the existence of persistent tetrahedral intermediates was obtained through in situ IR studies.

  4. Optical interactions of silver nanoparticle decorated cellulose nanocrystals created from a one-pot reduction method

    NASA Astrophysics Data System (ADS)

    Dawson, Nathan J.; Spinella, Stephen; Peters, Kyle C.; Maiorana, Anthony; Qian, Qian; Hepworth, Victoria; Gross, Richard A.; Singer, Kenneth D.

    2017-03-01

    Modified cellulose nanocrystals were decorated with silver nanoparticles using a one-pot reduction method. In contrast to a quasi-uniform distribution of silver nanoparticles, we report on the interactions of non-contact nanoparticle clusters with significant line broadening and red shifts in the extinction spectra. The particle size and cluster distributions were examined using a transmission electron microscope. Monte Carlo random walk (MCRW) simulations of the extinction spectrum show that the interacting silver nanospheres are organized in small, non-contact clusters. We observed that the MCRW optimization using the first-order iterative approximation to the self-consistent dipole field equations quickly approaches the observed localized clusters.

  5. One-pot exfoliation of graphite and synthesis of nanographene/dimesitylporphyrin hybrids.

    PubMed

    Bernal, M Mar; Pérez, Emilio M

    2015-05-12

    A simple one-pot process to exfoliate graphite and synthesize nanographene-dimesitylporphyrin hybrids has been developed. Despite the bulky mesityl groups, which are expected to hinder the efficient π-π stacking between the porphyrin core and graphene, the liquid-phase exfoliation of graphite is significantly favored by the presence of the porphyrins. Metallation of the porphyrin further enhances this effect. The resulting graphene/porphyrin hybrids were characterized by spectroscopy (UV-visible, fluorescence, and Raman) and microscopy (STEM, scanning transmission electron microscopy).

  6. One-pot synthesis of β-acetamido ketones using boric acid at room temperature.

    PubMed

    Karimi-Jaberi, Zahed; Mohammadi, Korosh

    2012-01-01

    β-acetamido ketones were synthesized in excellent yields through one-pot condensation reaction of aldehydes, acetophenones, acetyl chloride, and acetonitrile in the presence of boric acid as a solid heterogeneous catalyst at room temperature. It is the first successful report of boric acid that has been used as solid acid catalyst for the preparation of β-acetamido ketones. The remarkable advantages offered by this method are green catalyst, mild reaction conditions, simple procedure, short reaction times, and good-to-excellent yields of products.

  7. One-pot and two-step synthesis of novel carbonylthioureas and dicarbonyldithioureas derivatives

    NASA Astrophysics Data System (ADS)

    Banaei, Alireza; Shiran, Jafar Abbasi; Saadat, Afshin; Ardabili, Farnaz Fazlalizadeh; McArdle, Patrick

    2015-11-01

    One-pot, two-step synthesis of several 1-cyclopropanecarbonyl-3-(substituted phenyl)-thioureas and 1-(phenylene-1,4-dione)-3,3‧-(substituted phenyl)-dithioureas have been successfully prepared. The structures of the synthesized compounds were confirmed by elemental analysis, FT-IR spectroscopy and NMR. Also the crystal structure one of these compounds was determined by X-ray crystallography. All synthesized compounds were evaluated for antibacterial activity using Salmonella enterica (SE), Micrococcus luteus (ML), Bacillus subtilis (BS) and Pseudomonas aeruginosa (PS).

  8. One-pot palladium-catalyzed borrowing hydrogen synthesis of thioethers.

    PubMed

    Corma, Avelino; Navas, Javier; Ródenas, Tania; Sabater, María J

    2013-12-16

    Palladium on magnesium oxide is able to allow a one-pot reaction to synthesize thioethers from thiols and aldehydes formed in situ from the respective alcohol by means of a borrowing hydrogen method. The reaction is initiated by dehydrogenation of the alcohol to give a palladium hydride intermediate and an aldehyde. The latter reacts with a thiol involving most probably the intermediacy of a thionium ion RCH=S(+)R, which can be reduced in situ by the metal hydride to afford thioethers.

  9. Layered materials with coexisting acidic and basic sites for catalytic one-pot reaction sequences.

    PubMed

    Motokura, Ken; Tada, Mizuki; Iwasawa, Yasuhiro

    2009-06-17

    Acidic montmorillonite-immobilized primary amines (H-mont-NH(2)) were found to be excellent acid-base bifunctional catalysts for one-pot reaction sequences, which are the first materials with coexisting acid and base sites active for acid-base tamdem reactions. For example, tandem deacetalization-Knoevenagel condensation proceeded successfully with the H-mont-NH(2), affording the corresponding condensation product in a quantitative yield. The acidity of the H-mont-NH(2) was strongly influenced by the preparation solvent, and the base-catalyzed reactions were enhanced by interlayer acid sites.

  10. A sharp interface method for coupling multiphase flow, heat transfer and multicomponent mass transfer with interphase diffusion

    NASA Astrophysics Data System (ADS)

    He, Ping; Ghoniem, Ahmed F.

    2017-03-01

    Mixing of partially miscible fluids plays an important role in many physical and chemical processes. The modeling complexities lie in the tight coupling of the multiphase flow, heat transfer and multicomponent mass transfer, as well as diffusions across the phase interface. We present a sharp interface method for modeling such process. The non-ideal equation of state is used to compute the fluid properties such as density, fugacity and enthalpy, and to predict phase equilibrium composition. The phase interface location is tracked using the phase propagation velocity. A third-order one-sided finite difference scheme using a variable grid size according to the interface location is utilized to discretize the partial derivatives immediately next to the interface, while a second-order central scheme is used for the bulk of fluids. An optimization method, the Nelder-Mead method, is applied to search for (1) the phase compositions on both sides of the interface, and (2) the phase propagation velocity based on the coupling of the multicomponent phase equilibrium and the species' balance across the interface. The temperature at the interface is determined by the energy balance. Numerical results are used to demonstrate the convergence of our method and show its capability to simulate the mixing of multicomponent partially miscible fluids.

  11. Precise Tuning of Facile One-Pot Gelatin Methacryloyl (GelMA) Synthesis

    NASA Astrophysics Data System (ADS)

    Shirahama, Hitomi; Lee, Bae Hoon; Tan, Lay Poh; Cho, Nam-Joon

    2016-08-01

    Gelatin-methacryloyl (GelMA) is one of the most commonly used photopolymerizable biomaterials in bio-applications. However, GelMA synthesis remains suboptimal, as its reaction parameters have not been fully investigated. The goal of this study is to establish an optimal route for effective and controllable GelMA synthesis by systematically examining reaction parameters including carbonate-bicarbonate (CB) buffer molarity, initial pH adjustment, MAA concentration, gelatin concentration, reaction temperature, and reaction time. We employed several analytical techniques in order to determine the degree of substitution (DS) and conducted detailed structural analysis of the synthesized polymer. The results enabled us to optimize GelMA synthesis, showing the optimal conditions to balance the deprotonation of amino groups with minimizing MAA hydrolysis, which led to nearly complete substitution. The optimized conditions (low feed ratio of MAA to gelatin (0.1 mL/g), 0.25 M CB buffer at pH 9, and a gelatin concentration of 10–20%) enable a simplified reaction scheme that produces GelMA with high substitution with just one-step addition of MAA in one pot. Looking forward, these optimal conditions not only enable facile one-pot GelMA synthesis but can also guide researchers to explore the efficient, high methacrylation of other biomacromolecules.

  12. One-pot synthesis of hematite@graphene core@shell nanostructures for superior lithium storage.

    PubMed

    Chen, Dezhi; Quan, Hongying; Liang, Junfei; Guo, Lin

    2013-10-21

    Novel hematite@graphene composites have been successfully synthesized by a one-pot surfactant governed approach under mild wet-chemical conditions. A series of characterizations including X-ray diffraction (XRD), Raman spectrum, scanning electron microscopy (SEM) and transmission electron microscopy (TEM) indicated that the hematite nanoparticles with relatively uniform size were encapsulated by graphene layers and were able to form core-shell nanostructures. The electrochemical properties of hematite@graphene core-shell nanostructures as anodes for lithium-ion batteries were evaluated by galvanostatic charge-discharge and AC impedance spectroscopy techniques. The as-prepared hematite@graphene core-shell nanostructures exhibited a high reversible specific capacity of 1040 mA h g(-1) at a current density of 200 mA g(-1) (0.2 C) after 180 cycles and excellent rate capability and long cycle life. Furthermore, a reversible capacity as high as 500 mA h g(-1) was still achieved after 200 cycles even at a high rate of 6 C. The electrochemical test results show that the hematite@graphene composites prepared by the one-pot wet chemical method are promising anode materials for lithium-ion batteries.

  13. One-pot synthesis of class II lanthipeptide bovicin HJ50 via an engineered lanthipeptide synthetase

    PubMed Central

    Wang, Jian; Ge, Xiaoxuan; Zhang, Li; Teng, Kunling; Zhong, Jin

    2016-01-01

    Lanthipeptides are a large class of bacteria-produced, ribosomally-synthesized and post-translationally modified peptides. They are recognized as peptide antibiotics because most of them exhibit potent antimicrobial activities against Gram-positive bacteria especially those that are phylogenetically related to producers. Maturation of class II lanthipeptide like bovicin HJ50 undergoes precursor modification by LanM and a subsequent leader peptide cleavage by LanT. Herein, via co-expression of precursor gene bovA, modification gene bovM and transporter gene bovT in Escherichia coli C43 (DE3), bioactive bovicin HJ50 was successfully produced and secreted. To further achieve in vitro one-pot synthesis of bovicin HJ50, an engineered bovicin HJ50 synthetase BovT150M was obtained by fusing the peptidase domain of BovT (BovT150) to the N-terminus of BovM. BovT150M exhibited dual functions of precursor modification and leader peptide cleavage to release mature bovicin HJ50. Under the guidance of BovA leader peptide, BovT150M exhibited substrate tolerance to modify non-native substrates including suicin and lacticin 481. This work exemplifies the feasibility of enzyme chimera of peptidase domain (LanT150) and modification enzyme (LanM) as a one-pot lanthipeptide synthetase. PMID:27924934

  14. One-pot multienzyme synthesis of Lewis x and sialyl Lewis x antigens.

    PubMed

    Yu, Hai; Lau, Kam; Li, Yanhong; Sugiarto, Go; Chen, Xi

    2012-09-01

    L-Fucose has been found abundantly in human milk oligosaccharides, bacterial lipopolysaccharides, glycolipids, and many N- and O-linked glycans produced by mammalian cells. Fucose-containing carbohydrates have important biological functions. Alterations in the expression of fucosylated oligosaccharides have been observed in several pathological processes such as cancer and atherosclerosis. Chemical formation of fucosidic bonds is challenging due to its acid lability. Enzymatic construction of fucosidic bonds by fucosyltransferases is highly efficient and selective but requires the expensive sugar nucleotide donor guanosine 5'- diphosphate-L-fucose (GDP-Fuc). Here, we describe a protocol for applying a one-pot three-enzyme system in synthesizing structurally defined fucose-containing oligosaccharides from free L-fucose. In this system, GDP-Fuc is generated from L-fucose, adenosine 5'-triphosphate (ATP), and guanosine 5'-triphosphate (GTP) by a bifunctional L-fucokinase/GDP-fucose pyrophosphorylase (FKP). An inorganic pyrophosphatase (PpA) is used to degrade the by-product pyrophosphate (PPi) to drive the reaction towards the formation of GDP-Fuc. In situ generated GDP-Fuc is then used by a suitable fucosyltransferase for the formation of fucosides. The three-enzyme reactions are carried out in one pot without the need for high cost sugar nucleotide or isolation of intermediates. The time for the synthesis is 4-24 hours. Purification and characterization of products can be completed in 2-3 days.

  15. One-pot reaction for the preparation of biofunctionalized self-assembled monolayers on gold surfaces

    NASA Astrophysics Data System (ADS)

    Raigoza, Annette F.; Fies, Whitney; Lim, Amber; Onyirioha, Kristeen; Webb, Lauren J.

    2017-02-01

    The Huisgen cycloaddition reaction ("click" chemistry) has been used extensively to functionalize surfaces with macromolecules in a straightforward manner. We have previously developed a procedure using the copper(I)-catalyzed click reaction to tether synthetic α-helical peptides carrying two alkyne groups to a well-ordered azide-terminated alkanethiol self-assembled monolayer (SAM) on a Au(111) surface. While convenient, click-based strategies potentially pose significant problems from reagents, solvents, and reaction temperatures that may irreversibly damage some molecules or substrates. Tuning click chemistry conditions would allow individual optimization of reaction conditions for a wide variety of biomolecules and substrate materials. Here, we explore the utility of simultaneous SAM formation and peptide-attachment chemistry in a one-pot reaction. We demonstrate that a formerly multistep reaction can be successfully carried out concurrently by mixing azide-terminated alkanethiols, CuCl, and a propargylglycine-containing peptide over a bare gold surface in ethanol and reacting at 70 °C. X-ray photoelectron spectroscopy (XPS), surface infrared spectroscopy, surface circular dichroic (CD) spectroscopy, and scanning tunneling microscopy (STM) were used to determine that this one-pot reaction strategy resulted in a high density of surface-bound α-helices without aggregation. This work demonstrates the simplicity and versatility of a SAM-plus-click chemistry strategy for functionalizing Au surfaces with structured biomolecules.

  16. Seed mediated one-pot growth of versatile heterogeneous upconversion nanocrystals for multimodal bioimaging

    NASA Astrophysics Data System (ADS)

    Wen, Shihui; Li, Du; Liu, Deming; Xu, Xiaoxue; Du, Yi; Mitchell, David R. G.; Shi, Bingyang; Shi, Xiangyang; Jin, Dayong

    2016-12-01

    The rapid development of a variety of molecular contrast agents makes the multimodality bioimaging highly attractive towards higher resolution, more sensitive, informative diagnosis. The key lies in the development of facile material synthesis that allows the integration of multiple contrast agents, ideally in a way that each of the components should be logically assembled to maximize their performances. Here, we report the one-pot programmable growth of multifunctional heterogeneous nanocrystal with tunable size, shape, composition, and properties. We demonstrated a facile one-pot hot-injection method to enable the highly selectively controlled growth of different sodium lanthanide fluoride nanomaterials in either longitudinal or transversal directions with atomic scale precision. This technique allows the upconversion luminescence signal, MRI signal and x-ray signal logically integrated and optimized within one single versatile nanoplatform for multimode bioimaging. These findings suggest that the facile strategy developed here have the promising to get the desired heterogeneous nanocrystals as an all-in-one contrast agent for integrated and self-correlative multimodal bioimaging.

  17. Highly Enantio- and Diastereoselective One-Pot Methods for the Synthesis of Halocyclopropyl Alcohols

    PubMed Central

    Kim, Hun Young; Salvi, Luca; Carroll, Patrick J.; Walsh, Patrick J.

    2009-01-01

    The lack of methods for the stereoselective transfer of functionalized carbenoids is one of the most significant deficiencies of Simmons–Smith cyclopropanation reactions. Outlined herein are one-pot methods for the catalytic asymmetric synthesis of halocyclopropyl alcohols with up to four stereogenic centers from achiral starting materials. The first method involves asymmetric alkyl addition to a conjugated enal to generate an allylic alkoxide followed by tandem diastereoselective iodo-, bromo- or chlorocyclopropanation to furnish halocyclopropyl alcohols. Enantioselectivities in these processes range from 89–99% and dr > 20:1 were achieved with all substrates optimized. The second method consists of an asymmetric vinylation of a saturated or aromatic aldehyde followed by a diastereoselective iodocyclopropanation to produce iodocyclopropyl alcohols with enantioselectivities between 86 and 99% and dr > 20:1. These complementary methods enable the efficient synthesis of a variety of halocyclopropyl alcohols in one-pot procedures. Preliminary efforts to functionalize iodocyclopropanes involve reaction with an excess of LiCu(n-Bu)2 to generate the cyclopropyl cuprate. This intermediate can be quenched with allyl bromides to generate the allylated cyclopropyl alcohols without loss of enantio- or diastereoselectivity. PMID:19154172

  18. Precise Tuning of Facile One-Pot Gelatin Methacryloyl (GelMA) Synthesis

    PubMed Central

    Shirahama, Hitomi; Lee, Bae Hoon; Tan, Lay Poh; Cho, Nam-Joon

    2016-01-01

    Gelatin-methacryloyl (GelMA) is one of the most commonly used photopolymerizable biomaterials in bio-applications. However, GelMA synthesis remains suboptimal, as its reaction parameters have not been fully investigated. The goal of this study is to establish an optimal route for effective and controllable GelMA synthesis by systematically examining reaction parameters including carbonate-bicarbonate (CB) buffer molarity, initial pH adjustment, MAA concentration, gelatin concentration, reaction temperature, and reaction time. We employed several analytical techniques in order to determine the degree of substitution (DS) and conducted detailed structural analysis of the synthesized polymer. The results enabled us to optimize GelMA synthesis, showing the optimal conditions to balance the deprotonation of amino groups with minimizing MAA hydrolysis, which led to nearly complete substitution. The optimized conditions (low feed ratio of MAA to gelatin (0.1 mL/g), 0.25 M CB buffer at pH 9, and a gelatin concentration of 10–20%) enable a simplified reaction scheme that produces GelMA with high substitution with just one-step addition of MAA in one pot. Looking forward, these optimal conditions not only enable facile one-pot GelMA synthesis but can also guide researchers to explore the efficient, high methacrylation of other biomacromolecules. PMID:27503340

  19. D-Fructose-6-phosphate aldolase-catalyzed one-pot synthesis of iminocyclitols.

    PubMed

    Sugiyama, Masakazu; Hong, Zhangyong; Liang, Pi-Hui; Dean, Stephen M; Whalen, Lisa J; Greenberg, William A; Wong, Chi-Huey

    2007-11-28

    A one-pot chemoenzymatic method for the synthesis of a variety of new iminocyclitols from readily available, non-phosphorylated donor substrates has been developed. The method utilizes the recently discovered fructose-6-phosphate aldolase (FSA), which is functionally distinct from known aldolases in its tolerance of different donor substrates as well as acceptor substrates. Kinetic studies were performed with dihydroxyacetone (DHA), the presumed endogenous substrate for FSA, as well as hydroxy acetone (HA) and 1-hydroxy-2-butanone (HB) as donor substrates, in each case using glyceraldehyde-3-phosphate as acceptor substrate. Remarkably, FSA used the three donor substrates with equal efficiency, with kcat/KMvalues of 33, 75, and 20 M-1 s-1, respectively. This level of donor substrate tolerance is unprecedented for an aldolase. Furthermore, DHA, HA, and HB were accepted as donors in FSA-catalyzed aldol reactions with a variety of azido- and Cbz-amino aldehyde acceptors. The broad substrate tolerance of FSA and the ability to circumvent the need for phosphorylated substrates allowed for one-pot synthesis of a number of known and novel iminocyclitols in good yields, and in a very concise fashion. New iminocyclitols were assayed as inhibitors against a panel of glycosidases. Compounds 15 and 16 were specific alpha-mannosidase inhibitors, and 24 and 26 were potent and selective inhibitors of beta-N-acetylglucosaminidases in the submicromolar range. Facile access to these compounds makes them attractive core structures for further inhibitor optimization.

  20. One-pot multienzyme (OPME) systems for chemoenzymatic synthesis of carbohydrates.

    PubMed

    Yu, Hai; Chen, Xi

    2016-03-14

    Glycosyltransferase-catalyzed enzymatic and chemoenzymatic syntheses are powerful approaches for the production of oligosaccharides, polysaccharides, glycoconjugates, and their derivatives. Enzymes involved in the biosynthesis of sugar nucleotide donors can be combined with glycosyltransferases in one pot for efficient production of the target glycans from simple monosaccharides and acceptors. The identification of enzymes involved in the salvage pathway of sugar nucleotide generation has greatly facilitated the development of simplified and efficient one-pot multienzyme (OPME) systems for synthesizing major glycan epitopes in mammalian glycomes. The applications of OPME methods are steadily gaining popularity mainly due to the increasing availability of wild-type and engineered enzymes. Substrate promiscuity of these enzymes and their mutants allows OPME synthesis of carbohydrates with naturally occurring post-glycosylational modifications (PGMs) and their non-natural derivatives using modified monosaccharides as precursors. The OPME systems can be applied in sequence for synthesizing complex carbohydrates. The sequence of the sequential OPME processes, the glycosyltransferase used, and the substrate specificities of the glycosyltransferases define the structures of the products. The OPME and sequential OPME strategies can be extended to diverse glycans in other glycomes when suitable enzymes with substrate promiscuity become available. This Perspective summarizes the work of the authors and collaborators on the development of glycosyltransferase-based OPME systems for carbohydrate synthesis. Future directions are also discussed.

  1. One-pot synthesis and characterization of subnanometre-size benzotriazolate protected copper clusters

    NASA Astrophysics Data System (ADS)

    Salorinne, Kirsi; Chen, Xi; Troff, Ralf W.; Nissinen, Maija; Häkkinen, Hannu

    2012-06-01

    A simple one-pot method for the preparation of subnanometre-size benzotriazolate (BTA) protected copper clusters, CunBTAm, is reported. The clusters were analyzed by optical and infrared spectroscopy, mass spectrometry and transmission electron microscopy together with computational methods. We suggest a structural motif where the copper core of the CunBTAm clusters is protected by BTA-Cu(i)-BTA units.A simple one-pot method for the preparation of subnanometre-size benzotriazolate (BTA) protected copper clusters, CunBTAm, is reported. The clusters were analyzed by optical and infrared spectroscopy, mass spectrometry and transmission electron microscopy together with computational methods. We suggest a structural motif where the copper core of the CunBTAm clusters is protected by BTA-Cu(i)-BTA units. Electronic supplementary information (ESI) available: Additional UV-Vis, ESI-MS, Raman and TEM data; synthesis protocol for the alternative procedure to prepare Cu:BTA clusters; and coordinates of the Cu6BTA4 cluster. See DOI: 10.1039/c2nr30444a

  2. A one-pot synthetic strategy for construction of the dibenzodiazepine skeleton via a transition metal-free process.

    PubMed

    Fang, Shuai; Niu, Xiaoyi; Zhang, Zeyuan; Sun, Yan; Si, Xiaomeng; Shan, Cuicui; Wei, Lei; Xu, Aiqing; Feng, Lei; Ma, Chen

    2014-09-21

    A one-pot transition metal-free methodology for constructing pharmacologically active dibenzodiazepine derivatives was developed. Fluoro-, bromo- and nitro-substituted aryl aldehydes were applied to this reaction efficiently.

  3. Facile production of nanostructured cellulose from Elaeis guineensis empty fruit bunch via one pot oxidative-hydrolysis isolation approach.

    PubMed

    Chen, You Wei; Lee, Hwei Voon; Abd Hamid, Sharifah Bee

    2017-02-10

    Cellulose in nanostructures was successfully isolated from empty fruit bunch biomass via a novel one-pot oxidative-hydrolysis technique. The physicochemical properties of nanocellulose prepared via one-pot process have shown comparable characteristics as products isolated via conventional multistep purification approach (namely dewaxing, chlorite bleaching process, alkalization, and acid hydrolysis). The chemical composition study indicated that the one-pot oxidative-hydrolysis process successfully extracted cellulose (91.0%), with the remaining minority being hemicellulose and lignin (∼6%) in the final product. Crystallinity profile of one-pot treated product (80.3%) was higher than that of multistep isolated nanocellulose (75.4%), which indicated that the disorder region (amorphous) in cellulose fibers was successfully removed. In additional to that, the morphology study demonstrated that nanocellulose prepared by one-pot process rendered spider-web-like network nanostructure, with an average diameter of fibers at a range of 51.6±15.4nm. The nanocellulose product showed high thermal stability (320°C), which was ready for nanocomposite application. One-pot oxidative-hydrolysis technique is a simple and versatile route for the preparation of nanocellulose from complex biomass within 90°C and 6h period, with minimum wastewater as compared to the multistep process.

  4. p-Sulfonic Acid Calix[4]arene as an Efficient Catalyst for One-Pot Synthesis of Pharmaceutically Significant Coumarin Derivatives under Solvent-Free Condition

    PubMed Central

    Tashakkorian, Hamed; Lakouraj, Moslem Mansour; Rouhi, Mona

    2015-01-01

    One-pot and efficient protocol for preparation of some potent pharmaceutically valuable coumarin derivatives under solvent-free condition via direct coupling using biologically nontoxic organocatalyst, calix[4]arene tetrasulfonic acid (CSA), was introduced. Calix[4]arene sulfonic acid has been incorporated lately as a magnificent and recyclable organocatalyst for the synthesis of some organic compounds. Nontoxicity, solvent-free conditions, good-to-excellent yields for pharmaceutically significant structures, and especially ease of catalyst recovery make this procedure valuable and environmentally benign. PMID:26798517

  5. Pseudo five-component synthesis of 2,5-di(hetero)arylthiophenes via a one-pot Sonogashira-Glaser cyclization sequence.

    PubMed

    Urselmann, Dominik; Antovic, Dragutin; Müller, Thomas J J

    2011-01-01

    Based upon a consecutive one-pot Sonogashira-Glaser coupling-cyclization sequence a variety of 2,5-di(hetero)arylthiophenes were synthesized in moderate to good yields. A single Pd/Cu-catalyst system, without further catalyst addition, and easily available, stable starting materials were used, resulting in a concise and highly efficient route for the synthesis of the title compounds. This novel pseudo five-component synthesis starting from iodo(hetero)arenes is particularly suitable as a direct access to well-defined thiophene oligomers, which are of peculiar interest in materials science.

  6. Unified Approach to (Thio)chromenones via One-Pot Friedel-Crafts Acylation/Cyclization: Distinctive Mechanistic Pathways of β-Chlorovinyl Ketones.

    PubMed

    Kim, Hun Young; Song, Eunsun; Oh, Kyungsoo

    2017-01-20

    A facile synthetic method to chromenones and thiochromenones has been developed using a one-pot Friedel-Crafts acylation of alkynes with suitably substituted benzoyl chlorides. This unified approach to (thio)chromenones is readily applicable to aryl- and alkylalkynes where the stereochemically well-defined β-chlorovinyl ketone intermediates undergo distinctively different cyclization pathways. The ready availability of both starting materials, alkynes and benzoyl chlorides, coupled with the experimental simplicity makes the current synthetic method to (thio)chromenones fast, efficient, and practical.

  7. A facile one-pot method to Au–SnO{sub 2}-graphene ternary hybrid

    SciTech Connect

    Xu, Diou; Li, Xiaotian; Zhang, Dawei

    2014-11-15

    In this article, we propose a facile one-pot route for synthesizing Au–SnO{sub 2}-graphene ternary hybrid. In the system, SnCl{sub 2} not only as the precursor of SnO{sub 2}, but also is employed as reducing agent for the effective reduction of both GO and HAuCl{sub 4} to graphene and Au nanoparticles, respectively. The obtained Au–SnO{sub 2}-graphene hybrid materials are characterized by atomic force microscopy, transmission electron microscopy, X-ray diffraction, Raman spectrum, X-ray photo-electron spectroscopy, and thermal gravimetric analysis. It is found that the content of Au nanoparticles decorated on the surface of graphene can be simply adjusted by changing the amount of HAuCl{sub 4} used in the synthesis process.

  8. One-pot construction of multiple contiguous chiral centers using Michael addition of chiral amine.

    PubMed

    Ozeki, Minoru; Ochi, Shunsuke; Hayama, Noboru; Hosoi, Shinzo; Kajimoto, Tetsuya; Node, Manabu

    2010-06-18

    Multiple contiguous chiral centers were constructed in one pot using three types of multistep reactions initiated with the Michael addition of N-benzyl-2(R)-methoxy-(+)-10-bornylamide to alpha,beta-unsaturated esters, i.e., asymmetric Michael-aldol reaction, double Michael addition, and double Michael-aldol reaction. The chiral 2-methoxy-10-bornyl group as well as the benzyl group on the amino group of the products in the Michael-aldol reaction could be easily cleaved by treatment with NIS (4 equiv), and beta-amino esters with multiple contiguous chiral centers were obtained in good yield. As an application, the beta-amino-beta'-hydroxy ester obtained in the asymmetric Michael-aldol reaction was converted to the beta-lactam derivative in good yield.

  9. An efficient one-pot synthesis, characterization and antibacterial activity of novel chromeno-pyrimidine derivatives

    NASA Astrophysics Data System (ADS)

    Suresh, Lingala; Kumar, P. Sagar Vijay; Chandramouli, G. V. P.

    2017-04-01

    A simple and efficient one-pot three component, green protocol was established for the synthesis of chromenopyrano[2,3-d]pyrimidine derivatives starting from 3-amino-pyrano[2,3-c]chromene-2-carbonitrile, N,N-dimethylformamide dimethylacetal and aromatic amines in the presence of 1-butyl-3-methylimidazolium hydrogen sulphate[Bmim]HSO4 ionic liquid. The present procedure offers a domino reaction strategy, cleaner conversion, short reaction times and high yields. Among the screened derivatives, the compounds 4g and 4h were identified as lead molecules which established promising antimicrobial towards Gram-positive bacterial strains such as Staphylococcus aureus MTCC 96, Staphylococcus aureus MLS16 MTCC 2940 and Bacillus subtilis MTCC 121.

  10. A Short, One-Pot Synthesis of Bupropion (Zyban®, Wellbutrin®)

    NASA Astrophysics Data System (ADS)

    Perrine, Daniel M.; Ross, Jason T.; Nervi, Stephen J.; Zimmerman, Richard H.

    2000-11-01

    A one-pot synthesis of (±)-2-(t-butylamino)-3'-chloropropiophenone (bupropion) as its hydrochloride salt (Zyban, Wellbutrin), an important antidepressant drug used in the treatment of nicotine addiction, is described. The procedure, suitable for students in their first year of organic chemistry, can be carried out in less than two hours and provides material of high purity in overall yield of 75-85%. A solution of m-chloropropiophenone in CH2Cl2 is treated with Br2. After removal of the solvent, t-butylamine and N-methylpyrrolidinone are added and the mixture is warmed briefly, quenched with water, and extracted with ether. Concentrated HCl is added to the ether solution to precipitate the product.

  11. Environmentally friendly efficient one-pot esterification of cyclohexane with CuO-promoted sulfated zirconia.

    PubMed

    Wang, Jingjing; Ma, Hongzhu; Wang, Bo

    2008-09-15

    The production of dibutyl phthalate directly from oxidation and esterification of cyclohexane, catalyzed by CuO-modified sulfated zirconia (SZCu) by one-pot under mild condition, was studied. The esterification reaction process was monitored by UV-vis spectra and the distribution of the products was analyzed by gas chromatograph-mass spectrometry (GC-MS). The result revealed that the SZCu catalyst was efficient in the direct oxidation and esterification of cyclohexane to ester. The selectivity for ester (dibutyl phthalate) can reach up to 72.2 wt.%, and the yield of ester was 29.5 wt.%. The esterification reaction, that offers several advantages such as usage of environmental friendly oxidant, simple work-up procedure, no-solvent conditions, short reaction times, easy recovery and reusability of the catalyst, is necessary for chemosynthesis industry from the environment standpoint. The regeneration property of SZCu was also tested in this work.

  12. Improved one-pot multienzyme (OPME) systems for synthesizing UDP-uronic acids and glucuronides†

    PubMed Central

    Muthana, Musleh M.; Qu, Jingyao; Xue, Mengyang; Klyuchnik, Timofey; Siu, Alex; Li, Yanhong; Zhang, Lei; Yu, Hai; Li, Lei; Wang, Peng G.

    2015-01-01

    Arabidopsis thaliana glucuronokinase (AtGlcAK) was cloned and shown to be able to use various uronic acids as substrates to produce the corresponding uronic acid-1-phosphates. AtGlcAK or Bifidobacterium infantis galactokinase (BiGalK) was used with a UDP-sugar pyrophosphorylase, an inorganic pyrophosphatase, with or without a glycosyltransferase for highly efficient synthesis of UDP-uronic acids and glucuronides. These improved cost-effective one-pot multienzyme (OPME) systems avoid the use of nicotinamide adenine dinucleotide (NAD+)-cofactor in dehydrogenase-dependent UDP-glucuronic acid production processes and can be broadly applied for synthesizing various glucuronic acid-containing molecules. PMID:25686901

  13. One-Pot Parallel Synthesis of Alkyl Sulfides, Sulfoxides, and Sulfones.

    PubMed

    Bogolubsky, Andrey V; Moroz, Yurii S; Mykhailiuk, Pavel K; Ostapchuk, Eugeniy N; Rudnichenko, Alexander V; Dmytriv, Yurii V; Bondar, Anna N; Zaporozhets, Olga A; Pipko, Sergey E; Doroschuk, Roman A; Babichenko, Liudmyla N; Konovets, Anzhelika I; Tolmachev, Andrey

    2015-06-08

    A simple and cost-effective one-pot parallel synthesis approach to sulfides, sulfoxides, and sulfones from thiourea was elaborated. The method combines two procedures optimized to the parallel synthesis conditions: alkylation of thiourea with alkyl chlorides and mono or full oxidation of in situ generated sulfides with H2O2 or H2O2-(NH4)2MoO4. The experimental set up required commonly used lab equipment: conventional oven and ultrasonic bath; the work up includes filtration or extraction with chloroform. The method was evaluated on an 81 member library of drug-like sulfides, sulfoxides, and sulfones yielding the compounds on a 30-300 mg scale. A small-scale synthesis of 2-(benzhydrylsulfinyl)acetamide (modafinil) utilizing our approach resulted in similar efficiency to the published procedures.

  14. One-pot synthesis of magnetic nanoclusters enabling atherosclerosis-targeted magnetic resonance imaging.

    PubMed

    Kukreja, Aastha; Lim, Eun-Kyung; Kang, Byunghoon; Choi, Yuna; Lee, Taeksu; Suh, Jin-Suck; Huh, Yong-Min; Haam, Seungjoo

    2014-01-01

    In this study, dextran-encrusted magnetic nanoclusters (DMNCs) were synthesized using a one-pot solution phase method for detection of atherosclerosis by magnetic resonance imaging. Pyrenyl dextran was used as a surfactant because of its electron-stabilizing effect and its amphiphilic nature, rendering the DMNCs stable and water-dispersible. The DMNCs were 65.6±4.3 nm, had a narrow size distribution, and were superparamagnetic with a high magnetization value of 60.1 emu/g. Further, they showed biocompatibility and high cellular uptake efficiency, as indicated by a strong interaction between dextran and macrophages. In vivo magnetic resonance imaging demonstrated the ability of DMNCs to act as an efficient magnetic resonance imaging contrast agent capable of targeted detection of atherosclerosis. In view of these findings, it is concluded that DMNCs can be used as magnetic resonance imaging contrast agents to detect inflammatory disease.

  15. One-pot synthesis of PVA-capped silver nanoparticles their characterization and biomedical application

    NASA Astrophysics Data System (ADS)

    Patil, Rupali S.; Kokate, Mangesh R.; Jambhale, Chitra L.; Pawar, Sambhaji M.; Han, Sung H.; Kolekar, Sanjay S.

    2012-03-01

    The rapid one-pot synthesis of silver nanoparticles (SNPs) at room temperature by using hydrazine hydrate as reducing agent and polyvinyl alcohol as stabilizing agent is reported. The SNPs were characterized with UV-visible (UV-Vis) spectroscopy, x-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), atomic force microscopy (AFM) and transmission electron microscopy (TEM). The synthesized silver nanoparticle shows surface plasmon resonance at 410 nm. The XRD reveals face-centered cubic (FCC) structure of SNPs. FE-SEM, AFM and TEM show that nanoparticles have spherical morphology with diameters in the range of 10-60 nm. The antimicrobial activity of synthesized hybrid material against strains of four different bacteria (Bacillus cereus, Escherichia coli, Staphylococus aureus, Proteus vulgaris), that are commonly found in hospitals has been studied. The results indicate that such particles have potential applications in biotechnology and biomedical science.

  16. Photocatalytic hybrid Au/ZnO nanoparticles assembled through a one-pot method.

    PubMed

    Manna, Joydeb; Vinod, T P; Flomin, Kobi; Jelinek, Raz

    2015-12-15

    Growth of metal domains on semiconductor nanoparticles is known to enhance their photocatalytic properties. We prepared ZnO nanoparticles decorated with metallic Au domains through a new one-pot microwave-based strategy. The synthetic route utilized microwave-heating of a mixture of only three components: Zn(2+) salt, Au(SCN)4(-) which served as a precursor for metallic gold, and Tris base. The Tris molecules had a dual role in the process, both shaping the morphology of the ZnO particles, as well as constituting docking and nucleation sites for the Au(SCN)4(-) ions. The Au complex subsequently underwent spontaneous crystallization/reduction without co-addition of reducing or stabilizing agents, yielding Au nanoparticles attached to the ZnO surface. We show that the hybrid Au/ZnO nanoparticles exhibited enhanced photocatalytic properties compared to the plain ZnO nanoparticles.

  17. Efficient One-Pot Synthesis of Colloidal Zirconium Oxide Nanoparticles for High-Refractive-Index Nanocomposites.

    PubMed

    Liu, Chao; Hajagos, Tibor Jacob; Chen, Dustin; Chen, Yi; Kishpaugh, David; Pei, Qibing

    2016-02-01

    Zirconium oxide nanoparticles are promising candidates for optical engineering, photocatalysis, and high-κ dielectrics. However, reported synthetic methods for the colloidal zirconium oxide nanoparticles use unstable alkoxide precursors and have various other drawbacks, limiting their wide application. Here, we report a facile one-pot method for the synthesis of colloidally stable zirconium oxide nanoparticles. Using a simple solution of zirconium trifluoroacetate in oleylamine, highly stable zirconium oxide nanoparticles have been synthesized with high yield, following a proposed amidization-assisted sol-gel mechanism. The nanoparticles can be readily dispersed in nonpolar solvents, forming a long-term stable transparent solution, which can be further used to fabricate high-refractive-index nanocomposites in both monolith and thin-film forms. In addition, the same method has also been extended to the synthesis of titanium oxide nanoparticles, demonstrating its general applicability to all group IVB metal oxide nanoparticles.

  18. One-pot laser-assisted synthesis of porous carbon with embedded magnetic cobalt nanoparticles

    NASA Astrophysics Data System (ADS)

    Ghimbeu, Camélia Matei; Sopronyi, Mihai; Sima, Felix; Delmotte, Luc; Vaulot, Cyril; Zlotea, Claudia; Paul-Boncour, Valérie; Le Meins, Jean-Marc

    2015-05-01

    A novel one-pot laser-assisted approach is reported herein for the synthesis of ordered carbons with embedded cobalt nanoparticles. The process is based on a UV pulsed laser exposure of an ethanolic solution consisting of green carbon precursors, a structure directing agent and a cobalt salt. Very short irradiation times (5 to 30 min) are only required to polymerize and cross-link carbon precursors (i.e. phloroglucinol and glyoxylic acid) independent of a catalyst presence. The influence of three metallic salts (acetate, nitrate and chloride) on the phenolic resin and carbon characteristics (structure, texture and particle size/distribution) was systematically studied. When exposed to UV laser, the metallic salt exhibited a strong influence on the particle size and distribution in the carbon matrix rather than on the textural carbon properties. Using cobalt acetate, very small (3.5 nm) and uniformly dispersed particles were obtained by this simple, fast and green one-pot synthesis approach. An original combined 13C CP-MAS and DP-DEC solid state NMR spectroscopy analysis allowed to determine the structure of phenolic resins as well as the location of the cobalt salt in the resin. Complementarily, the 1H solid-state and relaxation NMR provided unique insights into the rigidity (cross-linking) of the phenolic resin and dispersion of the cobalt salt. The magnetic properties of cobalt nanoparticles were found to be size-dependent: large Co nanoparticles (~50 nm) behave as bulk Co whereas small Co nanoparticles are superparamagnetic.A novel one-pot laser-assisted approach is reported herein for the synthesis of ordered carbons with embedded cobalt nanoparticles. The process is based on a UV pulsed laser exposure of an ethanolic solution consisting of green carbon precursors, a structure directing agent and a cobalt salt. Very short irradiation times (5 to 30 min) are only required to polymerize and cross-link carbon precursors (i.e. phloroglucinol and glyoxylic acid

  19. UV-VIS spectroscopic study of one pot synthesized strontium oxide quantum dots

    NASA Astrophysics Data System (ADS)

    Nemade, K. R.; Waghuley, S. A.

    The properties of drastically change when matter makes transition from 1D, 2D, 3D, to 0D. The quantum dots (QDs) of strontium oxide (SrO) were synthesized by one pot chemical precipitation method using hexamethylenetetramine (HMT). The radius of SrO QDs was calculated from hyperbolic band model (HBM). The direct and indirect band gaps of SrO QDs were estimated from UV-VIS analysis. The particle size was found to be 2.48 nm. The quantum confinement effect in SrO QDs is discussed through exciton Bohr radius. The particle size from UV-VIS analysis is in excellent agreement with fluorescence and TEM.

  20. Surface modification of magnesium aluminum hydroxide nanoparticles with poly(methyl methacrylate) via one-pot in situ polymerization

    NASA Astrophysics Data System (ADS)

    Guo, Xiaojun; Zhao, Leihua; Zhang, Li; Li, Jing

    2012-01-01

    Hydrophobic magnesium aluminum hydroxide composite particles (PMMA-MAH) were obtained by means of grafting poly(methyl methacrylate) (PMMA) onto the surface of magnesium aluminum hydroxide(MAH) nanoparticles after a novel type of phosphate coupling agent (DN-27) modification. The introduction of functional double bonds was firstly conducted on the surface of nanoparticles by DN-27 modification, followed by one-pot in situ polymerization on the particles surface using methyl methacrylate (MMA) as monomer, azoisobutyronitrile (AIBN) as initiator and sodium dodecyl sulfate (SDS) as stabilizer to graft PMMA on the surface of DN-27-modified MAH particles. The obtained composite particles were characterized by field-emission scanning electron microscope (FESEM), Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), X-ray powder diffraction (XRD). The results show that the organic macromolecule PMMA could be successfully grafted on the surface of DN-27-modified MAH nanoparticles and the thermal stability of the PMMA-MAH composite particles had been improved. Compared with unmodified blank MAH sample, the product obtained with this method possesses better hydrophobic properties such as a higher water contact angle of 108° and a well dispersion.

  1. Synthesis of α-methylene-δ-oxo-γ-amino esters via Rh(ii)-catalyzed coupling of 1-sulfonyl-1,2,3-triazoles with Morita-Baylis-Hillman adducts.

    PubMed

    Jeon, Hyun Ji; Kwak, Mi Soo; Jung, Da Jung; Bouffard, Jean; Lee, Sang-Gi

    2016-11-29

    A rhodium(ii)-catalyzed coupling of 1-sulfonyl-1,2,3-triazoles, prepared from 1-alkynes and sulfonyl azides, with Morita-Baylis-Hillman (MBH) adducts afforded highly functionalized α-methylene-δ-oxo-γ-amino esters in excellent yields with broad functional group tolerance. This transformation can also be successfully accomplished as a multicomponent all-in-one-pot reaction of 1-alkynes, sulfonyl azides and MBH adducts in the presence of Cu(i) and Rh(ii) catalysts.

  2. Symmetry breaking polymerization: one-pot synthesis of plasmonic hybrid Janus nanoparticles

    NASA Astrophysics Data System (ADS)

    Wang, Yanming; Ding, Tao; Baumberg, Jeremy J.; Smoukov, Stoyan K.

    2015-06-01

    Asymmetric hybrid nanoparticles have many important applications in catalysis, nanomotion, sensing, and diagnosis, however ways to generate the asymmetric hybrid nanoparticles are quite limited and inefficient. Most current methods rely on interfacial adhesion and modification of already formed particles. In this article we report a one-pot, facile and scalable synthesis of anisotropic Au-polymer hybrid nanoparticles via interfacial oxidative dispersion polymerization. The interfacial nucleation and polymerization lead to spontaneous symmetry breaking and formation of the Janus particles. The reaction is initiated by monomer radicals generated by the strong oxidant HAuCl4, which is itself later reduced by the electron-rich monomers to self-nucleate and form Au nanoparticles (NPs). The competition between divinylbenzene adsorption and the PVP capping agent results in effective partial surface wetting, forming asymmetric Au-PDVB hybrid nanoparticles, by confining growth of each material to its own phase. Such spontaneous symmetry breaking, important in morphogenesis, with control over the subsequent growth processes should lead to significant advances in the synthesis of asymmetric nanostructures.Asymmetric hybrid nanoparticles have many important applications in catalysis, nanomotion, sensing, and diagnosis, however ways to generate the asymmetric hybrid nanoparticles are quite limited and inefficient. Most current methods rely on interfacial adhesion and modification of already formed particles. In this article we report a one-pot, facile and scalable synthesis of anisotropic Au-polymer hybrid nanoparticles via interfacial oxidative dispersion polymerization. The interfacial nucleation and polymerization lead to spontaneous symmetry breaking and formation of the Janus particles. The reaction is initiated by monomer radicals generated by the strong oxidant HAuCl4, which is itself later reduced by the electron-rich monomers to self-nucleate and form Au nanoparticles

  3. Isothermal DNA origami folding: avoiding denaturing conditions for one-pot, hybrid-component annealing

    NASA Astrophysics Data System (ADS)

    Kopielski, Andreas; Schneider, Anne; Csáki, Andrea; Fritzsche, Wolfgang

    2015-01-01

    The DNA origami technique offers great potential for nanotechnology. Using biomolecular self-assembly, defined 2D and 3D nanoscale DNA structures can be realized. DNA origami allows the positioning of proteins, fluorophores or nanoparticles with an accuracy of a few nanometers and enables thereby novel nanoscale devices. Origami assembly usually includes a thermal denaturation step at 90 °C. Additional components used for nanoscale assembly (such as proteins) are often thermosensitive, and possibly damaged by such harsh conditions. They have therefore to be attached in an extra second step to avoid defects. To enable a streamlined one-step nanoscale synthesis - a so called one-pot folding - an adaptation of the folding procedures is required. Here we present a thermal optimization of this process for a 2D DNA rectangle-shaped origami resulting in an isothermal assembly protocol below 60 °C without thermal denaturation. Moreover, a room temperature protocol is presented using the chemical additive betaine, which is biocompatible in contrast to chemical denaturing approaches reported previously.The DNA origami technique offers great potential for nanotechnology. Using biomolecular self-assembly, defined 2D and 3D nanoscale DNA structures can be realized. DNA origami allows the positioning of proteins, fluorophores or nanoparticles with an accuracy of a few nanometers and enables thereby novel nanoscale devices. Origami assembly usually includes a thermal denaturation step at 90 °C. Additional components used for nanoscale assembly (such as proteins) are often thermosensitive, and possibly damaged by such harsh conditions. They have therefore to be attached in an extra second step to avoid defects. To enable a streamlined one-step nanoscale synthesis - a so called one-pot folding - an adaptation of the folding procedures is required. Here we present a thermal optimization of this process for a 2D DNA rectangle-shaped origami resulting in an isothermal assembly

  4. One-pot, bioinspired coatings to reduce the flammability of flexible polyurethane foams.

    PubMed

    Davis, Rick; Li, Yu-Chin; Gervasio, Michelle; Luu, Jason; Kim, Yeon Seok

    2015-03-25

    In this manuscript, natural materials were combined into a single "pot" to produce flexible, highly fire resistant, and bioinspired coatings on flexible polyurethane foam (PUF). In one step, PUF was coated with a fire protective layer constructed of a polysaccharide binder (starch or agar), a boron fire retardant (boric acid or derivative), and a dirt char former (montmorillonite clay). Nearly all coatings produced a 63% reduction in a critical flammability value, the peak heat release rate (PHRR). One formulation produced a 75% reduction in PHRR. This technology was validated in full-scale furniture fire tests, where a 75% reduction in PHRR was measured. At these PHRR values, this technology could reduce the fire threat of furniture from significant fire damage in and beyond the room of fire origin to being contained to the burning furniture. This flammability reduction was caused by three mechanisms-the gas-phase and condensed-phase processes of the boron fire retardant and the condensed-phase process of the clay. We describe the one-pot coating process and the impact of the coating composition on flammability.

  5. One-pot facile synthesis of PEGylated superparamagnetic iron oxide nanoparticles for MRI contrast enhancement.

    PubMed

    Dai, Lingling; Liu, Yongkang; Wang, Zhongqiu; Guo, Fangfang; Shi, Donglu; Zhang, Bingbo

    2014-08-01

    Polyethylene glycol (PEG)-coated superparamagnetic iron oxide nanoparticles (PEG·SPIONs) were prepared by a facile one-pot approach. The synthesized PEG·SPIONs were found to be uniform in size with an average hydrodynamic diameter of 11.7 nm. PEG·SPIONs exhibited excellent dispersibility in water, colloidal stability, and biocompatibility. The magnetic resonance imaging (MRI) properties of PEG·SPIONs were characterized both in vitro and in vivo. The dual contrast both in T1 and T2-weighted imaging was well enhanced with longitudinal and transverse relaxivity (r1, r2) of 35.92 s(-1) per mM of Fe(3+) and 206.91 s(-1) per mM of Fe(3+) respectively. In vivo T2-weighted MRI shows pronounced enhancement in the liver and spleen but not in T1-weighted MRI. Accumulations of nanoparticles were found primarily in the liver, spleen, and intestine, while much lower uptake in the kidney, heart, and lungs. A gradual excretion of PEG·SPIONs was observed via hepatobiliary (HB) processing over a period of 14 days. The toxicity of PEG·SPIONs was also evaluated in vitro and in vivo. PEG·SPIONs were found to be biocompatible by investigating organ tissues after hematoxylin-eosin staining. The conclusion of the study indicates a high potential of PEG·SPIONs in medical MRI.

  6. One-Pot synthesis of phosphorylated mesoporous carbon heterogeneous catalysts with tailored surface acidity

    SciTech Connect

    Fulvio, Pasquale F; Mahurin, Shannon Mark; Mayes, Richard T; Bauer, Christopher; Wang, Xiqing; Veith, Gabriel M; Dai, Sheng

    2012-01-01

    Soft-templated phosphorylated mesoporous carbons with homogeneous distributions of phosphate groups were prepared by a 'one-pot' synthesis method using mixtures of phosphoric acid with hydrochloric, or nitric acids in the presence of Pluronic F127 triblock copolymer. Adjusting the various ratios of phosphoric acid used in these mixtures resulted in carbons with distinct adsorption, structural and surface acidity properties. The pore size distributions (PSDs) from nitrogen adsorption at -196 C showed that mesoporous carbons exhibit specific surface areas as high as 551 m{sup 2}/g and mesopores as large as 13 nm. Both structural ordering of the mesopores and the final phosphate contents were strongly dependent on the ratios of H{sub 3}PO{sub 4} in the synthesis gels, as shown by transmission electron microscopy (TEM), X-ray photoelectron (XPS) and energy dispersive X-ray spectroscopy (EDS). The number of surface acid sites determined from temperature programmed desorption of ammonia (NH{sub 3}-TPD) were in the range of 0.3-1.5 mmol/g while the active surface areas are estimated to comprise 5-54% of the total surface areas. Finally, the conversion temperatures for the isopropanol dehydration were lowered by as much as 100 C by transitioning from the least acidic to the most acidic catalysts surface.

  7. Rapid approach to biobased telechelics through two one-pot thiol-ene click reactions.

    PubMed

    Lluch, Cristina; Ronda, Joan C; Galià, Marina; Lligadas, Gerard; Cádiz, Virginia

    2010-06-14

    The application of environmentally friendly thiol-ene chemistry to the preparation of biobased telechelics is presented in this work. This methodology is based on two one-pot photoinitiated thiol-ene click processes: step-growth polymerization using a 3,6-dioxa-1,8-octanedithiol and end-group postpolymerization modification with three functional thiols: 2-mercaptoethanol, 3-mercaptopropionic acid, and 3-mercaptopropyltrimethoxysilane. We applied this approach to a potentially 100% biomass-derived monomer, allyl ester of 10-undecenoic acid (UDA). To show the generality and scope of this methodology, a series of well-defined telechelics with molecular weight ranging from 1000-3000 g/mol and hydroxyl, carboxyl, or trimethoxysilyl groups at the polymer terminus were prepared. An exhaustive (1)H NMR and MALDI-TOF MS analyses demonstrates the highly end-group fidelity of this methodology being an interesting procedure for the accelerated preparation of telechelics derived from divinyl monomers. UDA-based thelechelic diol prepared using this methodology was reacted with 4,4'-methylenebis(phenylisocyanate) and 1,4-butanediol as the chain extender to obtain multiblock poly(ester urethane).

  8. 'One-pot' synthesis of multifunctional GSH-CdTe quantum dots for targeted drug delivery.

    PubMed

    Chen, Xiaoqin; Tang, Yajun; Cai, Bing; Fan, Hongsong

    2014-06-13

    A novel quantum dots-based multifunctional nanovehicle (DOX-QD-PEG-FA) was designed for targeted drug delivery, fluorescent imaging, tracking, and cancer therapy, in which the GSH-CdTe quantum dots play a key role in imaging and drug delivery. To exert curative effects, the antineoplastic drug doxorubicin hydrochloride (DOX) was loaded on the GSH-CdTe quantum dots through a condensation reaction. Meanwhile, a polyethylene glycol (PEG) shell was introduced to wrap the DOX-QD, thus stabilizing the structure and preventing clearance and drug release during systemic circulation. To actively target cancer cells and prevent the nanovehicles from being absorbed by normal cells, the nanoparticles were further decorated with folic acid (FA), allowing them to target HeLa cells that express the FA receptor. The multifunctional DOX-QD-PEG-FA conjugates were simply prepared using the 'one pot' method. In vitro study demonstrated that this simple, multifunctional nanovehicle can deliver DOX to the targeted cancer cells and localize the nanoparticles. After reaching the tumor cells, the FA on the DOX-QD-PEG surface allowed folate receptor recognition and increased the drug concentration to realize a higher curative effect. This novel, multifunctional DOX-QD-PEG-FA system shows great potential for tumor imaging, targeting, and therapy.

  9. TiO2 Hollow Spheres: One-Pot Synthesis and Enhanced Photocatalysis

    NASA Astrophysics Data System (ADS)

    Jia, Changchao; Cao, Yongqiang; Yang, Ping

    2013-04-01

    Hollow TiO2 microspheres were successfully fabricated by metal salts with low solubility in ethanol acting as intelligent templates using a simple one-pot solvothermal method. Hollow spheres with large diameter were obtained using CuSO4ṡ5H2O as templates while small ones were obtained using Sr(NO3)2 as templates. It is found that titanium precursor plays an important role for the morphology of samples. Solid TiO2 microspheres were prepared by using titanium tetrabutoxide (TBT). In contrast, bowl-like hollow microspheres were obtained by using titanium tetrachloride (TiCl4). Furthermore, the amount of H2O can stimulate the hydrolysis rate of TiCl4 to form solid spheres. Compared with solid microspheres, hollow TiO2 microspheres depending on their interior cavity structure exhibited enhanced photocatalysis efficiency for the UV-light photodegradation of methyl orange. Quantificationally, the apparent photocatalytic degradation pseudo-first-rate constant of the hollow microspheres is 1.25 times of that of the solid ones.

  10. Preparing hydrophobic nanocellulose-silica film by a facile one-pot method.

    PubMed

    Le, Duy; Kongparakul, Suwadee; Samart, Chanatip; Phanthong, Patchiya; Karnjanakom, Surachai; Abudula, Abuliti; Guan, Guoqing

    2016-11-20

    Hydrophobic nanocellulose-silica film was successfully prepared by a facile one-pot method using tetraethoxysilane (TEOS) and dodecyl triethoxylsilane (DTES). Morphological characterization of the hydrophobic nanocellulose-silica (NC-SiO2-DTES) film showed well self-assembled DTES modified silica spherical nanoparticles with the particle sizes in the range of 88-126nm over the nanocellulose film. The hydrophobicity of the NC-SiO2-DTES film was achieved owing to the improvement of roughness of the nanocellulose film by coating dodecyl- terminated silica nanoparticles. An increase in DTES loading amount and reaction time increased the hydrophobicity of the film, and the optimum condition for NC-SiO2-DTES film preparation was achieved at DTES/TEOS molar ratio of 2.0 for 8h reaction time. Besides, the NC-SiO2-DTES film performed superoleophilic property with octane and hexadecane contact angles of 0°. It also showed an excellent hydrophobic property over all pH values ranged from 1 to 14.

  11. Photothermal cancer therapy using graphitic carbon–coated magnetic particles prepared by one-pot synthesis

    PubMed Central

    Lee, Hyo-Jeong; Sanetuntikul, Jakkid; Choi, Eun-Sook; Lee, Bo Ram; Kim, Jung-Hee; Kim, Eunjoo; Shanmugam, Sangaraju

    2015-01-01

    We describe here a simple synthetic strategy for the fabrication of carbon-coated Fe3O4 (Fe3O4@C) particles using a single-component precursor, iron (III) diethylenetriaminepentaacetic acid complex. Physicochemical analyses revealed that the core of the synthesized particles consists of ferromagnetic Fe3O4 material ranging several hundred nanometers, embedded in nitrogen-doped graphitic carbon with a thickness of ~120 nm. Because of their photothermal activity (absorption of near-infrared [NIR] light), the Fe3O4@C particles have been investigated for photothermal therapeutic applications. An example of one such application would be the use of Fe3O4@C particles in human adenocarcinoma A549 cells by means of NIR-triggered cell death. In this system, the Fe3O4@C can rapidly generate heat, causing >98% cell death within 10 minutes under 808 nm NIR laser irradiation (2.3 W cm−2). These Fe3O4@C particles provided a superior photothermal therapeutic effect by intratumoral delivery and NIR irradiation of tumor xenografts. These results demonstrate that one-pot synthesis of carbon-coated magnetic particles could provide promising materials for future clinical applications and encourage further investigation of this simple method. PMID:25565819

  12. One-pot synthesis and antimicrobial evaluation of novel 3-cyanopyridine derivatives of (-)-β-pinene.

    PubMed

    Liao, Shengliang; Shang, Shibin; Shen, Minggui; Rao, Xiaoping; Si, Hongyan; Song, Jie; Song, Zhanqian

    2016-03-15

    A series of novel 3-cyanopyridine derivatives of (-)-β-pinene were designed and synthesized by one-pot four-component domino reactions. The targeted compounds were evaluated for their antimicrobial activity against four bacteria (Klebsiella pneumoniae, Enterobacter aerogenes, Staphylococcus aureus, Staphylococcus epidermidis) and a fungus (Candida albicans). The results showed that most of the minimal inhibitory concentrations (MICs) of these 3-cyanopyridine derivatives against the tested strains was in the range of 15.6-125 mg/L. Among these 3-cyanopyridine derivatives, the MICs of compound 5h against S. epidermidis and C. albicans were 15.6 mg/L, which revealed that compound 5h featured double fluoro substituents at meta- and para-position was the most active compound. In addition, the preliminary structure-activity relationship analysis indicated that the change of substituents on the pyridine ring and benzene ring of 3-cyanopyridine derivatives was an important factor for inducing antimicrobial activity. This research would promote the development of heterocyclic derivatives of β-pinene with antimicrobial activity.

  13. One-pot pseudomorphic crystallization of mesoporous porous silica to hierarchical porous zeolites

    SciTech Connect

    Xing, Jun-Ling; Jiang, Shu-Hua; Pang, Jun-Ling; Yuan, En-Hui; Ma, Xiao-Jing; Lam, Koon-Fung; Xue, Qing-Song; Zhang, Kun

    2015-09-15

    Hierarchically porous silica with mesopore and zeolitic micropore was synthesized via pseudomorphic crystallization under high-temperature hydrothermal treatment in the presence of cetyltrimethylammonium tosylate and tetrapropylammonium ions. A combined characterization using small-angle X-ray diffraction (XRD), nitrogen adsorption, high-resolution transmission electron microscopy (TEM), thermogravimetric analysis (TG), and elemental analysis showed that dual templates, CTA{sup +} and TPA{sup +} molecules, can work in a cooperative manner to synthesize mesoporous zeolite in a one-pot system by precisely tuning the reaction conditions, such as reaction time and temperature, and type and amount of heterometal atoms. It is found that the presence of Ti precursor is critical to the successful synthesis of such nanostructure. It not only retards the nucleation and growth of crystalline MFI domains, but also acts as nano-binder or nano-glue to favor the assembly of zeolite nanoblocks. - Graphical abstract: Display Omitted - Highlights: • A facile method to synthesize mesoporous zeolites with hierarchical porosity was presented. • It gives a new insight into keeping the balance between mesoscopic and molecular ordering in hierarchical porous materials. • A new understanding on the solid–solid transformation mechanism for the synthesis of titanosilicate zeolites was proposed.

  14. Supercapacitive performance of hierarchical porous carbon microspheres prepared by simple one-pot method

    NASA Astrophysics Data System (ADS)

    Zhao, Qinglan; Wang, Xianyou; Wu, Chun; Liu, Jing; Wang, Hao; Gao, Jiao; Zhang, Youwei; Shu, Hongbo

    2014-05-01

    The hierarchical porous carbon microspheres (HPCMSs) using furfuryl alcohol as carbon resource have been prepared by a simple one-pot method. The HPCMSs are characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM) and nitrogen adsorption/desorption isotherm at 77 K, cyclic voltammetry (CV), galvanostatic charge/discharge tests, electrochemical impedance spectroscopy (EIS) and cycle life measurements in 6 M KOH. The results show that all the HPCMSs samples, which can be fabricated by adjusting the ratio of furfuryl alcohol/tetraethyl orthosilicate, possess three-dimensionally tailored pore structures with unique micro-, meso- and macroporous systems. Particularly, the HPCMS-2 prepared at the mole ratio of 2/1 (furfuryl alcohol/tetraethyl orthosilicate) shows the largest specific surface area of 709 m2 g-1, and the HPCMS-2 electrode owns specific capacitance as high as 221 F g-1 at the current density of 1 A g-1. The supercapacitor using HPCMS-2 as the active material shows high specific capacitance and excellent cycle stability, which exhibits a specific capacitance of 56 F g-1 at the charge/discharge current density of 0.5 A g-1. Furthermore, the HPCMS-2 supercapacitor delivers high energy densities of 6.1 Wh kg-1 at the power density of 5000 W kg-1, revealing a promising application in supercapacitors.

  15. One-pot synthesis of hollow superparamagnetic CoPt nanospheres.

    PubMed

    Vasquez, Yolanda; Sra, Amandeep K; Schaak, Raymond E

    2005-09-14

    Hollow metal nanospheres are of interest for a variety of academic and technological applications, including drug delivery, catalysis, plasmonics, and lightweight structural composites. Despite recent advances in synthesizing metal nanostructures with controlled morphologies, there are very few reports of hollow bimetallic nanospheres, although such systems promise to offer advantages over single-metal systems. Here, were report a one-pot synthetic strategy for accessing hollow CoPt nanospheres with a Co-Pt alloy structure. The approach utilizes an in situ Co template and exploits galvanic displacement reactions to selectively dissolve the Co core while depositing a Pt shell. The combination of reducing conditions and a polymer stabilizer appears to allow the Co and Pt to co-reduce and form a Co-Pt fcc alloy phase with a morphology that is templated by the sacrificial Co core. The hollow CoPt nanospheres, which show magnetic hysteresis at low temperatures, are thermally stable up to 300 degrees C. The approach, which adds to a growing toolbox of reactions that yield morphologically controlled magnetic CoPt and FePt nanomaterials, is likely to be general for a variety of alloy systems.

  16. Polyacrylamide-metal nanocomposites: one-pot synthesis, antibacterial properties, and thermal stability

    NASA Astrophysics Data System (ADS)

    Li, Cuiyan; Cai, Yanling; Zhu, Yihua; Ma, Mingguo; Zheng, Wei; Zhu, Jiefang

    2013-09-01

    The incorporation of inorganic nanoparticles into polymers is a hot research spot, since it endows the nanocomposites with new or improved properties by exploiting synergistic effects. Here we report a facile one-pot synthesis of polyacrylamide (PAM)-metal (M = Au, Ag, or Pd) nanocomposites in ethylene glycol (EG). The simultaneous polymerization of the acylamide (AM) monomer and formation of metal nanoparticles lead to a homogeneous distribution of metal nanoparticles in the PAM matrix. The sizes of Au, Ag, and Pd nanoparticles are 55.50 ± 10.6, 14.15 ± 2.57, and 7.74 ± 1.82 nm, respectively. The reaction system only includes EG, AM monomer, and corresponding metal salt. EG acts as both the solvent and the reducing reagent. Also, no initiator for AM polymerization and no surfactant for stabilization of metal nanoparticles are used. Furthermore, this simple synthetic route does not rely on any special or expensive equipment, thus can be exploited to the synthesis of similar polymer-inorganic nanocomposites. Compared to PAM, the PAM-metal nanocomposites showed enhanced thermal stability and antibacterial properties.

  17. One-Pot Synthesis, Spectroscopic and Physicochemical Studies of Quinoline Based Blue Emitting Donor-Acceptor Chromophores with Their Biological Application.

    PubMed

    Asiri, Abdullah M; Khan, Salman A; Al-Thaqafya, Saad H

    2015-09-01

    Blue emitting cyano substituted isoquinoline dyes were synthesized by one-pot multicomponent reactions (MCRs) of aldehydes, malononitrile, 6-methoxy-1,2,3,4-tetrahydro-naphthalin-1-one and ammonium acetate. Results obtained from spectroscopic (FT-IR, (1)H-NMR, (13)C-NMR, EI-MS) and elemental analysis of synthesized compounds was in good agreement with their chemical structures. UV-vis and fluorescence spectroscopy measurements proved that all compounds are good absorbent and fluorescent. Fluorescence polarity study demonstrated that these compounds were sensitive to the polarity of the microenvironment provided by different solvents. In addition, spectroscopic and physicochemical parameters, including electronic absorption, excitation coefficient, stokes shift, oscillator strength, transition dipole moment and fluorescence quantum yield were investigated in order to explore the analytical potential of synthesized compounds. The anti-bacterial activity of these compounds were first studied in vitro by the disk diffusion assay against two Gram-positive and two Gram-negative bacteria then the minimum inhibitory concentration (MIC) was determined with the reference of standard drug chloramphenicol. The results displayed that compound 3 was better inhibitors of both types of the bacteria (Gram-positive and Gram-negative) than chloramphenicol. Graphical Abstract ᅟ.

  18. One-pot conversion of cellulose to ethylene glycol with multifunctional tungsten-based catalysts.

    PubMed

    Wang, Aiqin; Zhang, Tao

    2013-07-16

    With diminishing fossil resources and increasing concerns about environmental issues, searching for alternative fuels has gained interest in recent years. Cellulose, as the most abundant nonfood biomass on earth, is a promising renewable feedstock for production of fuels and chemicals. In principle, the ample hydroxyl groups in the structure of cellulose make it an ideal feedstock for the production of industrially important polyols such as ethylene glycol (EG), according to the atom economy rule. However, effectively depolymerizing cellulose under mild conditions presents a challenge, due to the intra- and intermolecular hydrogen bonding network. In addition, control of product selectivity is complicated by the thermal instabilities of cellulose-derived sugars. A one-pot catalytic process that combines hydrolysis of cellulose and hydrogenation/hydrogenolysis of cellulose-derived sugars proves to be an efficient way toward the selective production of polyols from cellulose. In this Account, we describe our efforts toward the one-pot catalytic conversion of cellulose to EG, a typical petroleum-dependent bulk chemical widely applied in the polyester industry whose annual consumption reaches about 20 million metric tons. This reaction opens a novel route for the sustainable production of bulk chemicals from biomass and will greatly decrease the dependence on petroleum resources and the associated CO₂ emission. It has attracted much attention from both industrial and academic societies since we first described the reaction in 2008. The mechanism involves a cascade reaction. First, acid catalyzes the hydrolysis of cellulose to water-soluble oligosaccharides and glucose (R1). Then, oligosaccharides and glucose undergo C-C bond cleavage to form glycolaldehyde with catalysis of tungsten species (R2). Finally, hydrogenation of glycolaldehyde by a transition metal catalyst produces the end product EG (R3). Due to the instabilities of glycolaldehyde and cellulose

  19. One-pot formation of multifunctional Pt-conducting polymer intercalated nanostructures

    NASA Astrophysics Data System (ADS)

    Liu, Yang; Lu, Ning; Poyraz, Selcuk; Wang, Xiaolong; Yu, Yajiao; Scott, Julie; Smith, James; Kim, Moon J.; Zhang, Xinyu

    2013-04-01

    A novel multifunctional Pt nanoparticle@PPy nanofiber intercalated structure (Pt NP@PPy NF) has been synthesized facilely in one-pot. Pt NPs, with size and facet control, were nicely assembled and embedded into the polymer nanofiber network. Polyvinylpyrrolidone (PVP) was used during the synthesis process which would assist the self-assembly of the metal nanoparticles and polymer backbones into the intercalated structure. Space-confined distribution of the Pt NPs was achieved within the large dimension PPy nanofiber network, which could enhance the interfacial electron transfer process as well as diminish the catalyst deformation. The as-formed Pt NPs have a cluster-like structure and are mainly composed of 3.5 nm primary Pt particles with (100) surface atoms. Enhanced electrocatalytic properties were shown by the Pt NP@PPy NF intercalated structure, with sufficiently high enzyme-less glucose biosensitivity and a long linear range from 1-30 mM (R = 0.9995). High electrochemical cycling stability, chloride (Cl-) tolerance and good selectivity are also obtained for the Pt NP@PPy NF structure, as the electrode showed no obvious response to the common interfering agents, such as ascorbic acid (AA), uric acid (UA), and 4-acetamidophenol (AP). Furthermore, the Pt NP@PPy NF showed excellent catalytic activity for the methanol oxidation reaction (MOR) and oxygen reduction reaction (ORR), which displayed sufficient CO tolerance, and higher activity compared to the commercial Pt/C catalyst. This intrinsically multifunctional Pt NP@PPy NF with well-controlled Pt facets thus could serve as an advanced electrocatalyst for biosensing and fuel cell applications, surpassing the performance of many existing materials.A novel multifunctional Pt nanoparticle@PPy nanofiber intercalated structure (Pt NP@PPy NF) has been synthesized facilely in one-pot. Pt NPs, with size and facet control, were nicely assembled and embedded into the polymer nanofiber network. Polyvinylpyrrolidone (PVP

  20. One-pot synthesis of ZnO nanowires and belts through orientation attachment mechanism

    NASA Astrophysics Data System (ADS)

    Hossain, Mohammad Kamal

    2017-01-01

    Zinc oxide (ZnO) is one of the promising materials for optoelectronics and advanced electronics-based device fabrication. Nanostructured features include further flavor to the applications as well due to inherent and unprecedented properties. With this view, a sol-gel route for the synthesis of nanostructured ZnO, such as nanoparticles, nanowires and nanobelts subsequently obtained in one-pot has been reported. The process includes synthesis of monodispersed nanoparticles that can find potential applications as gas sensing layers and transparent conducting layers. Hexagonal wurtzite crystal structure with cell constants, a = 3.2427 Ǻ and c = 5.1948 Ǻ was confirmed by X-ray diffraction. Strong preferential growth along {101} plane indicated the growth of ZnO crystallites along c-axis. Vibrational band for Zn-O stretching and deformation modes was confirmed by Fourier transform infrared absorption spectroscopy. A reasonably well-coverage of ZnO nanoparticles, ca. 1 × 107 nanoparticles/cm2 along with size distribution of (13.5 ± 9.0) nm diameter, was obtained by topographic observation of scanning electron microscopy. A series of scanning electron micrographs revealed that as-synthesized nanoparticles were further processed to obtain nanometric wires and belts under controlled conditions. The nanowires were formed from anisotropic agglomeration of nanometric particles, and the belts were formed by agglomeration of these nanometric wires into bundles. A close observation indicated that ZnO nanowires of diameter 40-50 nm were consisted of one to three constituent colloids. Control of these selective agglomeration processes is a key challenge for application of nanowires and belts into useful devices.

  1. Cell compatible arginine containing cationic polymer: one-pot synthesis and preliminary biological assessment.

    PubMed

    Zavradashvili, Nino; Memanishvili, Tamar; Kupatadze, Nino; Baldi, Lucia; Shen, Xiao; Tugushi, David; Wandrey, Christine; Katsarava, Ramaz

    2014-01-01

    Synthetic cationic polymers are of interest as both nonviral vectors for intracellular gene delivery and antimicrobial agents. For both applications synthetic polymers containing guanidine groups are of special interest since such kind of organic compounds/polymers show a high transfection potential along with antibacterial activity. It is important that the delocalization of the positive charge of the cationic group in guanidine significantly decreases the toxicity compared to the ammonium functionality. One of the most convenient ways for incorporating guanidine groups is the synthesis of polymers composed of the amino acid arginine (Arg) via either application of Arg-based monomers or chemical modification of polymers with derivatives of Arg. It is also important to have biodegradable cationic polymers that will be cleared from the body after their function as transfection or antimicrobial agent is fulfilled. This chapter deals with a two-step/one-pot synthesis of a new biodegradable cationic polymer-poly(ethylene malamide) containing L-arginine methyl ester covalently attached to the macrochains in β-position of the malamide residue via the α-amino group. The goal cationic polymer was synthesized by in situ interaction of arginine methyl ester dihydrochloride with intermediary poly(ethylene epoxy succinimide) formed by polycondensation of di-p-nitrophenyl-trans-epoxy succinate with ethylenediamine. The cell compatibility study with Chinese hamster ovary (CHO) and insect Schneider 2 cells (S2) within the concentration range of 0.02-500 mg/mL revealed that the new polymer is not cytotoxic. It formed nanocomplexes with pDNA (120-180 nm in size) at low polymer/DNA weight ratios (WR = 5-10). A preliminarily transfection efficiency of the Arg-containing new cationic polymer was assessed using CHO, S2, H5, and Sf9 cells.

  2. Extraction with SPME and synthesis of 2-methyl-6-vinylpyrazine by a 'one pot' reaction using microwaves.

    PubMed

    Robledo, Norma; Escalante, Jaime; Arzuffi, René

    2009-06-15

    A synthesis of 2-methyl-6-vinylpyrazine was carried out by way of a 'one pot' reaction. In order to establish the efficiency of this synthesis the extraction of the volatiles released by male papaya fruit flies was performed by SPME (solid phase micro-extraction). The compound was separated and identified using GC/MSD (gas chromatography/mass spectrometry detector).

  3. Praseodymium methanesulfonate catalyzed one-pot synthesis of 3,4-dihydropyrimidin-2-(1H)-ones.

    PubMed

    Wang, Min; Song, Zhiguo; Gong, Hong; Jiang, Heng

    2008-01-01

    A series of 3,4-dihydropyrimidin-2-(1H)-ones compounds was synthesized efficiently by a one-pot cyclocondensation of an aldehyde, 1,3-dicarbonyl compound, and urea in absolute ethanol under refluxing temperature using praseodymium methanesulfonate as catalyst. After the reaction, the catalyst can be easily recovered and reused several times without distinct decrease in reaction yields.

  4. One-pot preparation of unsaturated polyester nanocomposites containing functionalized graphene sheets via a novel solvent-exchange method

    Technology Transfer Automated Retrieval System (TEKTRAN)

    This paper reports a convenient one-pot method integrating a novel solvent-exchange method into in situ melt polycondensation to fabricate unsaturated polyester nanocomposites containing functionalized graphene sheets (FGS). A novel solvent-exchange method was first developed to prepare graphene oxi...

  5. Highly efficient one-pot three-component synthesis of naphthopyran derivatives in water catalyzed by hydroxyapatite

    EPA Science Inventory

    An expeditious and efficient protocol for the synthesis of naphthopyrans has been developed that proceeds via one-pot three-component sequential reaction in water catalyzed by hydroxyapatite or sodium-modified-hydroxyapatite. The title compounds have been obtained in high yield a...

  6. Preparation of glycosyl thiourea derivatives from glycosyl azides using sulfamic acid and sodium iodide in one-pot.

    PubMed

    Gucchait, Arin; Jana, Manas; Jana, Kuladip; Misra, Anup Kumar

    2016-11-03

    Novel one-pot reaction conditions have been developed for the preparation of glycosyl thiourea derivatives directly from glycosyl azides mediated by a combination of sulfamic acid and sodium iodide. The reaction conditions were clean, non-toxic and the products were isolated in good to excellent yield.

  7. Aqueous hydrotrope: an efficient and reusable medium for a green one-pot, diversity-oriented synthesis of quinazolinone derivatives.

    PubMed

    Patil, Amol; Barge, Madhuri; Rashinkar, Gajanan; Salunkhe, Rajashri

    2015-08-01

    A library of quinazolinones was prepared by the one-pot three-component reaction of isatoic anhydride, ammonium salts/amines, and various electrophiles using aqueous hydrotropic solution as an efficient, economical, reusable, and green medium giving good to excellent yields of products in very short time. The method offers a versatile way for the development of diversity-oriented synthesis of quinazolinones.

  8. A facile one-pot synthesis of ruthenium hydroxide nanoparticles on magnetic silica: Aqueous hydration of nitriles to amides

    EPA Science Inventory

    One-pot synthesis of ruthenium hydroxide nanoparticles on magnetic silica is described which involve the in situ generation of magnetic silica (Fe3O4@ SiO2) and ruthenium hydroxide immobilization; the hydration of nitriles occurs in high yield and excellent selectivity using this...

  9. One-Pot Catalyst-Free Synthesis of β- and γ-Hydroxy Sulfides using Diaryliodonium Salts and Microwave Irradiation

    EPA Science Inventory

    A facile one-pot high-yield protocol is described for the preparation of β- and γ-hydroxy sulfides directly from diaryliodonium salts, potassium thiocyanate, and ethane-1,2-diol (ethylene glycol)/propane-1,3-diol (β-propylene glycol) without the need for any additional catalyst o...

  10. One-pot Catalyst-free Synthesis of β- and γ-Hydroxy Sulfides Using Diaryliodonium Salts and Microwaves

    EPA Science Inventory

    A facile one-pot high-yield protocol is described for the preparation of β- and γ-hydroxy sulfides directly from diaryliodonium salts, potassium thiocyanate, and ethane-1,2-diol (ethylene glycol)/propane-1,3-diol (β-propylene glycol) without the need for any addit...

  11. One-pot synthesis of antiviral acyclovir and other nucleosides derivatives using doped natural phosphate as lewis acid catalyst.

    PubMed

    Lazrek, Hassan B; Baddi, Laila; Smietana, Michael; Vasseur, Jean-Jacques; Sebti, Said; Zahouily, Mohamed

    2008-10-01

    Natural phosphate doped with iodine or potassium iodide is an active catalyst for the one-pot synthesis of acyclonucleosides. To demonstrate the utility of the new catalyst system, the highly important antiviral drug acyclovir was directly and regioselectively obtained from NAcG with no byproducts.

  12. Synthesis of Quaternary Ammonium Salts of Tricyclic Cationic Drugs: A One-Pot Synthesis for the Bioorganic Chemistry Laboratory

    ERIC Educational Resources Information Center

    Brunauer, Linda S.; Mogannam, Abid C.; Hwee, Won B.; Chen, James Y.

    2007-01-01

    A one-pot conversion of tricyclic cationic drugs to their quaternary ammonium forms is described for a widely used bioactive drug: chlorpromazine, a phenothiazine-based antipsychotic. After conversion to its free base, the parent drug was methylated using substoichiometric amounts of methyl iodide dissolved in ether; the charged quaternary…

  13. Indium-mediated one-pot three-component reaction of aromatic amines, enol ethers, and allylic bromides.

    PubMed

    Jang, Taeg-Su; Ku, Il Whea; Jang, Min Seok; Keum, Gyochang; Kang, Soon Bang; Chung, Bong Young; Kim, Youseung

    2006-01-19

    [reaction: see text] A new and efficient indium-mediated one-pot three-component reaction for the synthesis of N-aryl-substituted homoallylamines from aromatic amines, enol ethers, and allylic bromides in THF at room temperature is described.

  14. One-pot synthesis of 1-alkyl-1H-indazoles from 1,1-dialkylhydrazones via aryne annulation.

    PubMed

    Markina, Nataliya A; Dubrovskiy, Anton V; Larock, Richard C

    2012-03-28

    The reaction of readily accessible 1,1-dialkylhydrazones with commercially available o-(trimethylsilyl)aryl triflates provides a direct one-step route to pharmaceutically important 1-alkylindazoles. The products are obtained in high yields by one-pot NCS-chlorination/aryne annulation or Ac(2)O-acylation/deprotection/aromatization protocols.

  15. One-pot bioethanol production from cellulose by co-culture of Acremonium cellulolyticus and Saccharomyces cerevisiae

    PubMed Central

    2012-01-01

    Background While the ethanol production from biomass by consolidated bioprocess (CBP) is considered to be the most ideal process, simultaneous saccharification and fermentation (SSF) is the most appropriate strategy in practice. In this study, one-pot bioethanol production, including cellulase production, saccharification of cellulose, and ethanol production, was investigated for the conversion of biomass to biofuel by co-culture of two different microorganisms such as a hyper cellulase producer, Acremonium cellulolyticus C-1 and an ethanol producer Saccharomyces cerevisiae. Furthermore, the operational conditions of the one-pot process were evaluated for maximizing ethanol concentration from cellulose in a single reactor. Results Ethanol production from cellulose was carried out in one-pot bioethanol production process. A. cellulolyticus C-1 and S. cerevisiae were co-cultured in a single reactor. Cellulase producing-medium supplemented with 2.5 g/l of yeast extract was used for productions of both cellulase and ethanol. Cellulase production was achieved by A. cellulolyticus C-1 using Solka-Floc (SF) as a cellulase-inducing substrate. Subsequently, ethanol was produced with addition of both 10%(v/v) of S. cerevisiae inoculum and SF at the culture time of 60 h. Dissolved oxygen levels were adjusted at higher than 20% during cellulase producing phase and at lower than 10% during ethanol producing phase. Cellulase activity remained 8–12 FPU/ml throughout the one-pot process. When 50–300 g SF/l was used in 500 ml Erlenmeyer flask scale, the ethanol concentration and yield based on initial SF were as 8.7–46.3 g/l and 0.15–0.18 (g ethanol/g SF), respectively. In 3-l fermentor with 50–300 g SF/l, the ethanol concentration and yield were 9.5–35.1 g/l with their yields of 0.12–0.19 (g/g) respectively, demonstrating that the one-pot bioethanol production is a reproducible process in a scale-up bioconversion of cellulose to ethanol. Conclusion A. cellulolyticus

  16. Coupling between geochemical reactions and multicomponent gas and solute transport in unsaturated media: A reactive transport modeling study

    NASA Astrophysics Data System (ADS)

    Molins, S.; Mayer, K. U.

    2007-05-01

    The two-way coupling that exists between biogeochemical reactions and vadose zone transport processes, in particular gas phase transport, determines the composition of soil gas. To explore these feedback processes quantitatively, multicomponent gas diffusion and advection are implemented into an existing reactive transport model that includes a full suite of geochemical reactions. Multicomponent gas diffusion is described on the basis of the dusty gas model, which accounts for all relevant gas diffusion mechanisms. The simulation of gas attenuation in partially saturated landfill soil covers, methane production, and oxidation in aquifers contaminated by organic compounds (e.g., an oil spill site) and pyrite oxidation in mine tailings demonstrate that both diffusive and advective gas transport can be affected by geochemical reactions. Methane oxidation in landfill covers reduces the existing upward pressure gradient, thereby decreasing the contribution of advective methane emissions to the atmosphere and enhancing the net flux of atmospheric oxygen into the soil column. At an oil spill site, methane oxidation causes a reversal in the direction of gas advection, which results in advective transport toward the zone of oxidation both from the ground surface and the deeper zone of methane production. Both diffusion and advection contribute to supply atmospheric oxygen into the subsurface, and methane emissions to the atmosphere are averted. During pyrite oxidation in mine tailings, pressure reduction in the reaction zone drives advective gas flow into the sediment column, enhancing the oxidation process. In carbonate-rich mine tailings, calcite dissolution releases carbon dioxide, which partly offsets the pressure reduction caused by O2 consumption.

  17. Coupling between geochemical reactions and multicomponent gas and solute transport in unsaturated media: A reactive transport modeling study

    USGS Publications Warehouse

    Molins, S.; Mayer, K.U.

    2007-01-01

    The two-way coupling that exists between biogeochemical reactions and vadose zone transport processes, in particular gas phase transport, determines the composition of soil gas. To explore these feedback processes quantitatively, multicomponent gas diffusion and advection are implemented into an existing reactive transport model that includes a full suite of geochemical reactions. Multicomponent gas diffusion is described on the basis of the dusty gas model, which accounts for all relevant gas diffusion mechanisms. The simulation of gas attenuation in partially saturated landfill soil covers, methane production, and oxidation in aquifers contaminated by organic compounds (e.g., an oil spill site) and pyrite oxidation in mine tailings demonstrate that both diffusive and advective gas transport can be affected by geochemical reactions. Methane oxidation in landfill covers reduces the existing upward pressure gradient, thereby decreasing the contribution of advective methane emissions to the atmosphere and enhancing the net flux of atmospheric oxygen into the soil column. At an oil spill site, methane oxidation causes a reversal in the direction of gas advection, which results in advective transport toward the zone of oxidation both from the ground surface and the deeper zone of methane production. Both diffusion and advection contribute to supply atmospheric oxygen into the subsurface, and methane emissions to the atmosphere are averted. During pyrite oxidation in mine tailings, pressure reduction in the reaction zone drives advective gas flow into the sediment column, enhancing the oxidation process. In carbonate-rich mine tailings, calcite dissolution releases carbon dioxide, which partly offsets the pressure reduction caused by O2 consumption.

  18. Simple one-pot synthesis of solid-core@porous-shell alloyed PtAg nanocrystals for the superior catalytic activity toward hydrogen evolution and glycerol oxidation.

    PubMed

    Weng, Xuexiang; Liu, Qing; Wang, Ai-Jun; Yuan, Junhua; Feng, Jiu-Ju

    2017-05-15

    In this work, solid-core@porous-shell alloyed PtAg nanocrystals (PtAg NCs) were fabricated via a simple one-pot co-reduction wet-chemical method on a large scale. Diprophylline (DPP) was employed as the stabilizing agent and shape-directing agent, without any surfactant, polymer, seed or template. The products were mainly analyzed by a series of characterization technique. The hierarchical architectures had enhanced stability and improved electrocatalytic activity for hydrogen evolution reaction (HER) and glycerol oxidation reaction (GOR) in contrast with commercial available Pt/C and Pt black catalysts. For the prepared PtAg NCs catalyst, the Tafel slope is 40mVdec(-1) toward HER in 0.5M H2SO4, coupled with the specific activity and mass activity of 77.91mAcm(-2) and 1303mAmg(-1)Pt toward GOR, respectively.

  19. One-pot glyco-affinity precipitation purification for enhanced proteomics: the flexible alignment of solution-phase capture/release and solid-phase separation.

    PubMed

    Sun, Xue-Long; Haller, Carolyn A; Wu, XiaoYi; Conticello, Vincent P; Chaikof, Elliot L

    2005-01-01

    A one-pot affinity precipitation purification of carbohydrate-binding protein was demonstrated by designing thermally responsive glyco-polypeptide polymers, which were synthesized by selective coupling of pendant carbohydrate groups to a recombinant elastin-like triblock protein copolymer (ELP). The thermally driven inverse transition temperature of the ELP-based triblock polymer is maintained upon incorporation of carbohydrate ligands, which was confirmed by differential scanning calorimetry and (1)H NMR spectroscopy experiments. As a test system, lactose derivatized ELP was used to selectively purify a galactose-specific binding lectin through simple temperature-triggered precipitation in a high level of efficiency. Potential opportunities might be provided for enhanced proteomic, cell isolation as well as pathogen detection applications.

  20. One-pot phase transfer and surface modification of CdSe-ZnS quantum dots using a synthetic functional copolymer.

    PubMed

    Finetti, Chiara; Colombo, Miriam; Prosperi, Davide; Alessio, Giulia; Morasso, Carlo; Sola, Laura; Chiari, Marcella

    2014-01-07

    We present a facile, one-pot procedure for the organic-to-water phase transfer and biofunctionalization of semiconductor nanocrystals (quantum dots, or QDs) which employs a synthetic functional copolymer, namely poly(DMA-NAS-MAPS), consisting of three components: a surface interacting monomer, N,N-dimethylacrylamide (DMA), a chemically reactive monomer, N-acryloyloxysuccinimide (NAS), and a silane monomer, [3-(methacryloyloxy)-propyl]-trimethoxysilane (MAPS). The nanocrystals were transferred to water by exploiting the amphiphilic character of the copolymer backbone. Hydrolyzed MAPS units contributed to improve the solubility of QDs in water, whereas NAS exhibited reactivity toward biomolecules. A solution of streptavidin in phosphate buffer exhibited good dispersion ability leading to a clear and transparent colloidal suspension, indicative of good QD dispersion during phase transfer and purification. Unlike most of the published methods, the proposed functionalization approach does not require coupling agents and multistep reactions.

  1. HYDROGEOCHEM: A coupled model of HYDROlogic transport and GEOCHEMical equilibria in reactive multicomponent systems

    SciTech Connect

    Yeh, G.T.; Tripathi, V.S.

    1990-11-01

    This report presents the development of a hydrogeochemical transport model for multicomponent systems. The model is designed for applications to proper hydrological setting, accommodation of complete suite of geochemical equilibrium processes, easy extension to deal with chemical kinetics, and least constraints of computer resources. The hydrological environment to which the model can be applied is the heterogeneous, anisotropic, saturated-unsaturated subsurface media under either transient or steady state flow conditions. The geochemical equilibrium processes included in the model are aqueous complexation, adsorption-desorption, ion exchange, precipitation-dissolution, redox, and acid-base reactions. To achieve the inclusion of the full complement of these geochemical processes, total analytical concentrations of all chemical components are chosen as the primary dependent variables in the hydrological transport equations. Attendant benefits of this choice are to make the extension of the model to deal with kinetics of adsorption-desorption, ion exchange, precipitation-dissolution, and redox relatively easy. To make the negative concentrations during the iteration between the hydrological transport and geochemical equilibrium least likely, an implicit form of transport equations are proposed. To alleviate severe constraints of computer resources in terms of central processing unit (CPU) time and CPU memory, various optional numerical schemes are incorporated in the model. The model consists of a hydrological transport module and geochemical equilibrium module. Both modules were thoroughly tested in code consistency and were found to yield plausible results. The model is verified with ten examples. 79 refs., 21 figs., 17 tabs.

  2. One-pot electrodeposition, characterization and photoactivity of stoichiometric copper indium gallium diselenide (CIGS) thin films for solar cells.

    PubMed

    Harati, Mohammad; Jia, Jia; Giffard, Kévin; Pellarin, Kyle; Hewson, Carly; Love, David A; Lau, Woon Ming; Ding, Zhifeng

    2010-12-14

    Herein we report the one-pot electrodeposition of copper indium gallium diselenide, CuIn(1-x)Ga(x)Se(2) (CIGS), thin films as the p-type semiconductor in an ionic liquid medium consisting of choline chloride/urea eutectic mixture known as Reline. The thin films were characterized by scanning electron microscopy with energy dispersive X-ray analysis, transmission electron microscopy, X-ray photoelectron spectroscopy, Raman microspectroscopy, and UV-visible spectroscopy. Based on the results of the characterizations, the electrochemical bath recipe was optimized to obtain stoichiometric CIGS films with x between 0.2 and 0.4. The chemical activity and photoreactivity of the optimized CIGS films were found to be uniform using scanning electrochemical microscopy and scanning photoelectrochemical microscopy. Low-cost stoichiometric CIGS thin films in one-pot were successfully fabricated.

  3. One-pot synthesis of enantiomerically pure N-protected allylic amines from N-protected α-amino esters

    PubMed Central

    Silveira-Dorta, Gastón; Álvarez-Méndez, Sergio J; Martín, Víctor S

    2016-01-01

    Summary An improved protocol for the synthesis of enantiomerically pure allylic amines is reported. N-Protected α-amino esters derived from natural amino acids were submitted to a one-pot tandem reduction–olefination process. The sequential reduction with DIBAL-H at −78 °C and subsequent in situ addition of organophosphorus reagents yielded the corresponding allylic amines without the need to isolate the intermediate aldehyde. This circumvents the problem of instability of the aldehydes. The method tolerates well both Wittig and Horner–Wadsworth–Emmons organophosphorus reagents. A better Z-(dia)stereoselectivity was observed when compared to the previous one-pot method. The (dia)stereoselectivity of the process was affected neither by the reaction solvent nor by the amount of DIBAL-H employed. The method is compatible with the presence of free hydroxy groups as shown with serine and threonine derivatives. PMID:27340486

  4. Organic-soluble antimicrobial silver nanoparticle-polymer composites in gram scale by one-pot synthesis.

    PubMed

    Nair, A Sreekumaran; Binoy, Nadappuram P; Ramakrishna, Seeram; Kurup, T R R; Chan, Lai Wah; Goh, Cheong Hian; Islam, Md Rafiqul; Utschig, Thomas; Pradeep, T

    2009-11-01

    We report a one-pot synthesis of silver nanoparticle-polymer composites (Ag-PNCs) in water by a novel finding involving the polycondensation of methoxybenzyl chlorides (MeO-BzCl) directly on Ag nanoparticle surfaces at room temperature, leading to highly soluble antimicrobial nanocomposites. The composites, which are soluble in a range of organic solvents, precipitate in the reaction vessel, making their separation simple. Solutions of the composites can be casted directly on substrates or made into freestanding films. The material was found to be stable for nearly 2 years. A range of substrates have been shown to become antibacterial by direct application of this material. The experiments were conducted with Ag-PNC-loaded filter paper strips and glass substrates. The samples were found to be antimicrobial (against Escerichia coli and Aspergillus niger). The simple one-pot approach of this kind to make organic-soluble antibacterial coatings could have wide implications.

  5. Gold Nanoparticles Supported on a Layered Double Hydroxide as Efficient Catalysts for the One-Pot Synthesis of Flavones.

    PubMed

    Yatabe, Takafumi; Jin, Xiongjie; Yamaguchi, Kazuya; Mizuno, Noritaka

    2015-11-02

    Flavones are a class of natural products with diverse biological activities and have frequently been synthesized by step-by-step procedures using stoichiometric amounts of reagents. Herein, a catalytic one-pot procedure for the synthesis of flavone and its derivatives is developed. In the presence of gold nanoparticles supported on a Mg-Al layered double hydroxide (Au/LDH), various kinds of flavones can be synthesized starting from 2'-hydroxyacetophenones and benzaldehydes (or benzyl alcohols). The present one-pot procedure consists of a sequence of several reactions, and Au/LDH can catalyze all these different types of reactions. The catalysis is shown to be truly heterogeneous, and Au/LDH can be readily recovered and reused.

  6. Synergistic Degradation of a Hyperuricemia-Causing Metabolite Using One-Pot Enzyme-Nanozyme Cascade Reactions

    PubMed Central

    Jung, Secheon; Kwon, Inchan

    2017-01-01

    Multi-enzyme cascade reactions are frequently found in living organisms, in particular when an intermediate should be eliminated. Recently, enzyme-mimic nanomaterials (nanozymes) received much attention for various applications, because they are usually more stable and cost-effective than enzymes. However, enzyme-nanozyme cascade reations have not been yet extensively exploited. Therefore, in this study, we investigated one-pot enzyme-nanozyme cascade reactions using urate oxidase (UOX) and catalase-mimic gold nanoparticle nanozyme (AuNP) with the ultimate goal of treatment of hyperuricemia. UOX degrades hyperuricemia-causing uric acid, but also generates hydrogen peroxide raising several health concerns. We successfully demonstrated that one-pot UOX-AuNP cascade systems degrade uric acid more than five times faster than UOX alone, by eliminating potentially cytotoxic hydrogen peroxide, similar to enzyme-enzyme reactions. PMID:28287162

  7. Combining silver catalysis and organocatalysis: a sequential Michael addition/hydroalkoxylation one-pot approach to annulated coumarins.

    PubMed

    Hack, Daniel; Chauhan, Pankaj; Deckers, Kristina; Hermann, Gary N; Mertens, Lucas; Raabe, Gerhard; Enders, Dieter

    2014-10-03

    A highly stereoselective one-pot procedure for the synthesis of five-membered annulated hydroxycoumarins has been developed. By merging primary amine catalysis with silver catalysis, a series of functionalized coumarin derivatives were obtained in good yields (up to 91%) and good to excellent enantioselectivities (up to 99% ee) via a Michael addition/hydroalkoxylation reaction. Depending on the substituents on the enynone, the synthesis of annulated six-membered rings is also feasible.

  8. Electrochemistry for the generation of renewable chemicals: One-pot electrochemical deoxygenation of xylose to δ-valerolactone.

    PubMed

    James, Olusola Oladele; Sauter, Waldemer; Schröder, Uwe

    2017-03-22

    In this study, we demonstrate the electrochemical conversion of xylose to δ-valerolactone via carbonyl intermediates. The conversion was achieved in aqueous media and at ambient conditions. This study also demonstrates that feedstocks for the use of electrochemistry for production of renewable chemicals and biofuels can be extended to primary carbohydrate molecules. This is the first report on a one-pot electrochemical deoxygenation of xylose to δ-valerolactone.

  9. Self-Assembly of Disorazole C1 through a One-Pot Alkyne Metathesis Homodimerization Strategy**

    PubMed Central

    Ralston, Kevin J; Ramstadius, H Clinton; Brewster, Richard C; Niblock, Helen S; Hulme, Alison N

    2015-01-01

    Alkyne metathesis is increasingly explored as a reliable method to close macrocyclic rings, but there are no prior examples of an alkyne-metathesis-based homodimerization approach to natural products. In this approach to the cytotoxic C2-symmetric marine-derived bis(lactone) disorazole C1, a highly convergent, modular strategy is employed featuring cyclization through an ambitious one-pot alkyne cross-metathesis/ring-closing metathesis self-assembly process. PMID:25926364

  10. One-pot synthesis of acyclic nucleosides from carbohydrate derivatives, by combination of tandem and sequential reactions.

    PubMed

    Boto, Alicia; Hernández, Dácil; Hernández, Rosendo; Alvarez, Eleuterio

    2007-12-07

    The design of processes which combine tandem and sequential reactions allows the transformation of readily available precursors into high-profit products. This strategy is illustrated by the one-pot synthesis of acyclic nucleosides, which are potential antiviral compounds, from readily available carbohydrates. The reaction conditions are mild, compatible with most functional groups. Depending on the starting sugar, both common and uncommon acyclic chains can be prepared. These polyhydroxylated chains can be combined with different bases to generate diversity.

  11. NBS/DBU mediated one-pot synthesis of α-acyloxyketones from benzylic secondary alcohols and carboxylic acids.

    PubMed

    Zhu, Minghui; Wei, Wei; Yang, Daoshan; Cui, Hong; Cui, Huanhuan; Sun, Xuejun; Wang, Hua

    2016-11-22

    A simple and efficient one-pot NBS/DBU-mediated method has been developed for the synthesis of α-acyloxyketones from various benzylic secondary alcohols and carboxylic acids. Through this methodology, a series of α-acyloxyketones could be obtained in good to excellent yields under mild conditions. Importantly, this new reaction avoids the direct usage of toxic metal catalysts or potentially dangerous peroxide oxidants.

  12. Novel and efficient one-pot tandem synthesis of 2-styryl-substituted 4(3H)-quinazolinones.

    PubMed

    Dabiri, Minoo; Baghbanzadeh, Mostafa; Delbari, Akram Sadat

    2008-01-01

    A novel one-pot tandem synthesis of 2-styryl-4(3 H)-quinazolinones in an acidic ionic liquid is reported. In this procedure isatoic anhydride, a primary aniline or ammonium acetate, and triethylorthoacetate are reacted in the presence of imidazolium trifluoroacetate [Hmim]TFA. Subsequently an aromatic aldehyde is added to the mixture to afford the title compounds in high to excellent yields.

  13. Combining Silver Catalysis and Organocatalysis: A Sequential Michael Addition/Hydroalkoxylation One-Pot Approach to Annulated Coumarins

    PubMed Central

    2014-01-01

    A highly stereoselective one-pot procedure for the synthesis of five-membered annulated hydroxycoumarins has been developed. By merging primary amine catalysis with silver catalysis, a series of functionalized coumarin derivatives were obtained in good yields (up to 91%) and good to excellent enantioselectivities (up to 99% ee) via a Michael addition/hydroalkoxylation reaction. Depending on the substituents on the enynone, the synthesis of annulated six-membered rings is also feasible. PMID:25250728

  14. Synthesis and biological evaluation of the Forssman antigen pentasaccharide and derivatives by a one-pot glycosylation procedure.

    PubMed

    Tanaka, Hiroshi; Takeuchi, Ryota; Jimbo, Mitsuru; Kuniya, Nami; Takahashi, Takashi

    2013-02-25

    The synthesis and biological evaluation of the Forssman antigen pentasaccharide and derivatives thereof by using a one-pot glycosylation and polymer-assisted deprotection is described. The Forssman antigen pentasaccharide, composed of GalNAcα(1,3)GalNAcβ(1,3)Galα(1,4)Galβ(1,4)Glc, was recently identified as a ligand of the lectin SLL-2 isolated from an octocoral Sinularia lochmodes. The chemo- and α-selective glycosylation of a thiogalactoside with a hemiacetal donor by using a mixture of Tf(2)O, TTBP and Ph(2)SO, followed by activation of the remaining thioglycoside, provided the trisaccharide at the reducing end in a one-pot procedure. The pentasaccharide was prepared by the α-selective glycosylation of the N-Troc-protected (Troc=2,2,2-trichloroethoxycarbonyl) thioglycoside with a 2-azide-1-hydroxyl glycosyl donor, followed by glycosidation of the resulting disaccharide at the C3 hydroxyl group of the trisaccharide acceptor in a one-pot process. We next applied the one-pot glycosylation method to the synthesis of pentasaccharides in which the galactosamine units were partially and fully replaced by galactose units. Among the three possible pentasaccharides, Galα(1,3)GalNAc and Galα(1,3)Gal derivatives were successfully prepared by the established method. An assay of the binding of the synthetic oligosaccharides to a fluorescent-labeled SLL-2 revealed that the NHAc substituents and the length of the oligosaccharide chain were both important for the binding of the oligosaccharide to SLL-2. The inhibition effect of the oligosaccharide relative to the morphological changes of Symbiodinium by SLL-2, was comparable to their binding affinity to SLL-2. In addition, we fortuitously found that the synthetic Forssman antigen pentasaccharide directly promotes a morphological change in Symbiodinium. These results strongly indicate that the Forssman antigen also functions as a chemical mediator of Symbiodinium.

  15. General and efficient one-pot synthesis of novel sugar/heterocyclic(aryl) 1,2-diketones from sugar terminal alkynes by Sonogashira/tetra-n- butylammonium permanganate oxidation.

    PubMed

    Zhang, Fuyi; Wu, Xiaopei; Wang, Liming; Liu, Hong; Zhao, Yufen

    2015-11-19

    A new approach for one-pot synthesis of novel sugar/heterocyclic(aryl) 1,2-diketones has been achieved by the reaction of various sugar terminal alkynes with heterocyclic(aryl) iodides at room temperature. This one-pot protocol includes Sonogashira coupling and mild n-Bu4NMnO4 oxidation reaction. This method is mild, general and efficient. Fifty-six examples have been given and the sugar/heterocyclic(aryl) 1,2-diketones were obtained in 71-94% yields. The sugar terminal alkynes include 9 structurally different sugars in pyranose, furanose, and acyclic form which have various protecting groups, sensitive groups, and sterically bulky substituents. The heterocyclic(aryl) iodides include sterically bulky heterocyclic compounds and iodobenzenes with electron-donating, electron-neutral, and electron-withdrawing substituents.

  16. One-pot hydrothermal synthesis of zeolite/sodium tantalate composite and its photodegradation of methyl orange

    SciTech Connect

    Gu, Xiaoli; Lu, Haiqiang; Kan, Chun; Yao, Jianfeng

    2015-08-15

    Highlights: • Sodalite/NaTaO{sub 3} composite is prepared by a one-pot hydrothermal synthesis. • Enhanced photodegradation is achieved due to the heterogeneous doping effect. • Structure distortion is found for NaTaO{sub 3} after removing sodalite by acid washing. - Abstract: Sodalite/NaTaO{sub 3} composite was prepared by a one-pot hydrothermal synthesis method. Sodalite and NaTaO{sub 3} grow interpenetrated, and the resulting composites have similar morphology as the pure sodalite. The sodalite/NaTaO{sub 3} composite has a lower band gap of 3.35 eV due to the heterogeneous doping effect, and exhibits an enhanced photodegradation of methyl orange under UV irradiation as compared to the pure NaTaO{sub 3}. A slight structure distortion is found for NaTaO{sub 3} after removing sodalite by acid washing the sodalite/NaTaO{sub 3} composite, and such result further confirms the co-growth of the two crystals. This one-pot hydrothermal method opens up new avenues for the preparation of photocatalytic composites.

  17. Environmentally friendly, one-pot synthesis of folic acid-decorated graphene oxide-based drug delivery system

    NASA Astrophysics Data System (ADS)

    Lin, Quankui; Huang, Xiaojie; Tang, Junmei; Han, Yuemei; Chen, Hao

    2013-12-01

    A targeted drug delivery system based on graphene oxide (GO) was produced via one-pot synthesis method, taking advantages of the self-polymerization of the dopamine (DA). The polymerization of dopamine resulted in polydopamine capped GO nanocomposite. Meanwhile, the anti-tumor drug doxorubicin (DOX) can be loaded in the nanocomposite and the tumor cell targeting molecule folic acid (FA) can also been immobilized on the nanocomposite surface simultaneously. The size of the obtained FA-decorated GO-based drug delivery system (DA/GO(DOX)-FA) is about 600 nm. It renders a sustained drug release manner. The cell culture results reveal that the FA-decorated GO-based drug delivery system (DA/GO(DOX)-FA) via one-pot method shows property of targeted killing of cancer cells in vitro. This one-pot method just needs the pH adjusting to induce the self-polymerization of DA, but excludes the fussy chemical grafting process and the organic solvents, which make it an environmentally friendly method to synthesize FA-decorated GO-based drug delivery system.

  18. One-pot preparation of a sulfamethoxazole functionalized affinity monolithic column for selective isolation and purification of trypsin.

    PubMed

    Xiao, Yuan; Guo, Jialiang; Ran, Danni; Duan, Qianqian; Crommen, Jacques; Jiang, Zhengjin

    2015-06-26

    A facile and efficient "one-pot" copolymerization strategy was used for the preparation of sulfonamide drug (SA) functionalized monolithic columns. Two novel SA-immobilized methacrylate monolithic columns, i.e. poly(GMA-SMX-co-EDMA) and poly(GMA-SAA-co-EDMA) were prepared by one-pot in situ copolymerization of the drug ligand (sulfamethoxazole (SMX) or sulfanilamide (SAA)), the monomer (glycidyl methacrylate, GMA) and the cross-linker (ethylene dimethacrylate, EDMA) within 100 μm i.d. capillaries under optimized polymerization conditions. The physicochemical properties and column performance of the fabricated monolithic columns were characterized by elemental analysis, scanning electron microscopy and micro-HPLC. Satisfactory column permeability, efficiency and separation performance were obtained on the optimized poly(GMA-SMX-co-EDMA) monolithic column for small molecules, such as a standard test mixture and eight aromatic ketones. Notably, it was found that the poly(GMA-SMX-co-EDMA) monolith showed a selective affinity to trypsin, while the poly(GMA-SAA-co-EDMA) monolith containing sulfanilamide did not exhibit such affinity at all. This research not only provides a novel monolith for the selective isolation and purification of trypsin, but it also offers the possibility to easily prepare novel drug functionalized methacrylate monoliths through a one-pot copolymerization strategy.

  19. One-pot synthesis of oxamidato-bridged hexarhenium trigonal prisms adorned with ester functionality.

    PubMed

    Nagarajaprakash, R; Govindarajan, R; Manimaran, Bala

    2015-07-14

    Oxamidato-bridged Re(I)-based hexanuclear trigonal prisms with ester functionality have been synthesised via a multicomponent self-assembly process under solvothermal conditions. The self-assembly of Re2(CO)10, oxamide ligands (H2L1 = N,N′-dibutyloxamide, H2L2 = N,N′-dioctyloxamide, H2L3 = N,N′-didodecyloxamide and H2L4 = N,N′-dibenzyloxamide) and phenyl-1,3,5-tris(isonicotinate) (ptin) resulted in the formation of metallaprisms with the general formula [{(CO)3Re(μ–η(4)-L)Re(CO)3}3(μ3-ptin)2] (1–4). The metallaprisms 1–4 have been characterised using spectroscopic techniques, and the molecular structure of 4 has been elucidated by single-crystal X-ray diffraction methods. Investigations on the guest binding ability of 2 with a few aromatic alcohols and L-tryptophan using UV–vis and fluorescence spectroscopic titration experiments revealed strong host–guest interactions. The luminescence enhancement studies of 2 and 3 have been carried out using organic-aqueous solvent mixtures.

  20. Efficient syntheses of [¹¹C]zidovudine and its analogs by convenient one-pot palladium(0)-copper(I) co-mediated rapid C-[¹¹C]methylation.

    PubMed

    Zhang, Zhouen; Doi, Hisashi; Koyama, Hiroko; Watanabe, Yasuyoshi; Suzuki, Masaaki

    2014-06-30

    The nucleosides zidovudine (AZT), stavudine (d4T), and telbivudine (LdT) are approved for use in the treatment of human immunodeficiency virus (HIV) and hepatitis B virus (HBV) infections. To promote positron emission tomography (PET) imaging studies on their pharmacokinetics, pharmacodynamics, and applications in cancer diagnosis, a convenient one-pot method for Pd(0)-Cu(I) co-mediated rapid C-C coupling of [(11)C]methyl iodide with stannyl precursor was successfully established and applied to synthesize the PET tracers [(11)C]zidovudine, [(11)C]stavudine, and [(11)C]telbivudine. After HPLC purification and radiopharmaceutical formulation, the desired PET tracers were obtained with high radioactivity (6.4-7.0 GBq) and specific radioactivity (74-147 GBq/µmol) and with high chemical (>99%) and radiochemical (>99.5%) purities. This one-pot Pd(0)-Cu(I) co-mediated rapid C-[(11)C]methylation also worked well for syntheses of [methyl-(11)C]thymidine and [methyl-(11)C]4'-thiothymidine, resulting twice the radioactivity of those prepared by a previous two-pot method. The mechanism of one-pot Pd(0)-Cu(I) co-mediated rapid C-[(11)C]methylation was also discussed.

  1. One-Pot Catalytic Enantio- and Diastereoselective Syntheses of anti-, syn-cis-Disubstituted, and syn-Vinyl Cyclopropyl Alcohols

    PubMed Central

    Kim, Hun Young; Salvi, Luca; Carroll, Patrick J.; Walsh, Patrick J.

    2009-01-01

    Highly enantio- and diastereoselective methods for the synthesis of a variety of cyclopropyl alcohols are reported. These methods represent the first one-pot approaches to syn-vinyl cyclopropyl alcohols, syn-cis-disubstituted cyclopropyl alcohols, and anti-cyclopropyl alcohols from achiral precursors. The methods begin with enantioselective C–C bond formations promoted by a MIB-based zinc catalyst to generate allylic alkoxide intermediates. The intermediates are then subjected to in situ alkoxide-directed cyclopropanation to provide cyclopropyl alcohols. In the synthesis of vinyl cyclopropyl alcohols, hydroboration of enynes is followed by transmetalation of the resulting dienylborane to zinc to provide dienylzinc reagents. Enantioselective addition to aldehydes generates the requisite dienyl zinc alkoxides, which are then subjected to in situ cyclopropanation to furnish vinyl cyclopropyl alcohols. Cyclopropanation occurs at the double bond allylic to the alkoxide. Using this method, syn-vinylcyclopropyl alcohols are obtained in 65–85% yield, 76–93% ee, and >19:1 dr. To prepare anti-cyclopropanols, enantioselective addition of alkylzinc reagents to conjugated enals provides allylic zinc alkoxides. Because direct cyclopropanation provides syn-cyclopropyl alcohols, the intermediate allylic alkoxides were treated with TMSCl/Et3N to generate intermediate silyl ethers. In situ cyclopropanation of the allylic silyl ether resulted in cyclopropanation to form the anti-cyclopropyl silyl ether. Workup with TBAF affords the anti-cyclopropyl alcohols in one-pot in 60–82% yield, 89–99% ee, and ≥10:1 dr. For the synthesis of cis-disubstituted cyclopropyl alcohols, in situ generated (Z)-vinyl zinc reagents were employed in asymmetric addition to aldehydes to generate (Z)-allylic zinc alkoxides. In situ cyclopropanation provides syn-cis-disubstituted cyclopropyl alcohols in 42–70% yield, 88–97% ee, and >19:1 dr. These one-pot procedures enable the synthesis of a

  2. One-Pot Reverse Transcriptional Loop-Mediated Isothermal Amplification (RT-LAMP) for Detecting MERS-CoV

    PubMed Central

    Lee, Se Hee; Baek, Yun Hee; Kim, Yang-Hoon; Choi, Young-Ki; Song, Min-Suk; Ahn, Ji-Young

    2017-01-01

    Due to the limitation of rapid development of specific antiviral drug or vaccine for novel emerging viruses, an accurate and rapid diagnosis is a key to manage the virus spread. We developed an efficient and rapid method with high specificity for the Middle East Respiratory Syndrome coronavirus (MERS-CoV), based on one-pot reverse transcription loop-mediated isothermal amplification (one-pot RT-LAMP). A set of six LAMP primers [F3, B3, FIP, BIP, LF (Loop-F), and LB (Loop-B)] were designed using the sequence of nucleocapsid (N) gene with optimized RT-LAMP enzyme conditions: 100 U M-MLV RTase and 4 U Bst polymerase, implying that the reaction was able to detect four infectious viral genome copies of MERS-CoV within a 60 min reaction time period. Significantly, EvaGreen dye has better signal read-out properties in one-pot RT-LAMP reaction and is more compatible with DNA polymerase than SYBR green I. Isothermally amplified specific N genes were further evaluated using field-deployable microchamber devices, leading to the specific identification of as few as 0.4 infectious viral genome copies, with no cross-reaction to the other acute respiratory disease viruses, including influenza type A (H1N1 and H3N2), type B, human coronavirus 229E, and human metapneumovirus. This sensitive, specific and feasible method provides a large-scale technical support in emergencies, and is also applied as a sample-to-detection module in Point of Care Testing devices. PMID:28119682

  3. One-Pot Reverse Transcriptional Loop-Mediated Isothermal Amplification (RT-LAMP) for Detecting MERS-CoV.

    PubMed

    Lee, Se Hee; Baek, Yun Hee; Kim, Yang-Hoon; Choi, Young-Ki; Song, Min-Suk; Ahn, Ji-Young

    2016-01-01

    Due to the limitation of rapid development of specific antiviral drug or vaccine for novel emerging viruses, an accurate and rapid diagnosis is a key to manage the virus spread. We developed an efficient and rapid method with high specificity for the Middle East Respiratory Syndrome coronavirus (MERS-CoV), based on one-pot reverse transcription loop-mediated isothermal amplification (one-pot RT-LAMP). A set of six LAMP primers [F3, B3, FIP, BIP, LF (Loop-F), and LB (Loop-B)] were designed using the sequence of nucleocapsid (N) gene with optimized RT-LAMP enzyme conditions: 100 U M-MLV RTase and 4 U Bst polymerase, implying that the reaction was able to detect four infectious viral genome copies of MERS-CoV within a 60 min reaction time period. Significantly, EvaGreen dye has better signal read-out properties in one-pot RT-LAMP reaction and is more compatible with DNA polymerase than SYBR green I. Isothermally amplified specific N genes were further evaluated using field-deployable microchamber devices, leading to the specific identification of as few as 0.4 infectious viral genome copies, with no cross-reaction to the other acute respiratory disease viruses, including influenza type A (H1N1 and H3N2), type B, human coronavirus 229E, and human metapneumovirus. This sensitive, specific and feasible method provides a large-scale technical support in emergencies, and is also applied as a sample-to-detection module in Point of Care Testing devices.

  4. Cascade intermolecular Michael addition-intramolecular azide/internal alkyne 1,3-dipolar cycloaddition reaction in one pot.

    PubMed

    Arigela, Rajesh K; Mandadapu, Anil K; Sharma, Sudhir K; Kumar, Brijesh; Kundu, Bijoy

    2012-04-06

    A rapid one-pot protocol for the synthesis of indole-based polyheterocycles via a sequential Lewis acid catalyzed intermolecular Michael addition and an intramolecular azide/internal alkyne 1,3-dipolar cycloaddition reaction has been described. The generality of the method has been demonstrated by treating a series of aromatic/aliphatic 2-alkynyl indoles with substituted (E)-1-azido-2-(2-nitrovinyl)benzenes to furnish annulated tetracyclic indolo[2,3-c][1,2,3]triazolo[1,5-a][1]benzazepines in good yields.

  5. Controlled silver delivery by silver-cellulose nanocomposites prepared by a one-pot green synthesis assisted by microwaves.

    PubMed

    Silva, Ana Rosa; Unali, Gianfranco

    2011-08-05

    Controlled silver release from cellulosic nanocomposites was achieved by synthesizing silver nanoparticles, under microwave heating for 1-15 min, in a one-pot, versatile and sustainable process in which microcrystalline cellulose simultaneously functions as reducing, stabilizing and supporting agent in water; chitin, starch and other cellulose derivatives could also be used as reducing, stabilizing and supporting agents for silver nanoparticles and the method was also found to be extensible to the preparation of noble metal (Au, Pt) and metal oxide nanoparticle (ZnO, Cu, CuO and Cu(2)O) nanocomposites.

  6. Brönsted Acid-Catalyzed One-Pot Synthesis of Indoles from o-Aminobenzyl Alcohols and Furans

    PubMed Central

    Kuznetsov, Alexey; Makarov, Anton; Rubtsov, Alexandr E.; Butin, Alexander V.; Gevorgyan, Vladimir

    2013-01-01

    Brönsted acid-catalyzed one-pot synthesis of indoles from o-aminobenzyl alcohols and furans has been developed. This method operates via the in situ formation of aminobenzylfuran, followed by its recyclization into the indole core. The method proved to be efficient for substrates possessing different functional groups, including -OMe, -CO2Cy, and -Br. The resulting indoles can easily be transformed into diverse scaffolds, including 2,3- and 1,2-fused indoles, and indole possessing an α,β-unsaturated ketone moiety at the C-2 position. PMID:24255969

  7. Synthesis of Alkylidene(gem-Difluorocyclopropanes) from Propargyl Glycolates by a One-Pot Difluorocyclopropenation/Ireland-Claisen Rearrangement Sequence.

    PubMed

    Ernouf, Guillaume; Brayer, Jean-Louis; Folléas, Benoît; Demoute, Jean-Pierre; Meyer, Christophe; Cossy, Janine

    2017-03-24

    A one-pot difluorocyclopropenation/Ireland-Claisen rearrangement sequence applied to readily available propargyl glycolates was developed as a route toward functionalized alkylidene(gem-difluorocyclopropanes). This strategy conveniently avoids the isolation of the unstable 3,3-difluorocyclopropenylcarbinyl glycolates arising from the difluorocyclopropenation. The Ireland-Claisen rearrangement proceeds with high diastereoselectivity and chirality transfer to afford alkylidene(gem-difluorocyclopropanes) incorporating a quaternary stereocenter and a protected glycolic acid moiety, which are useful building blocks for the preparation of functionalized gem-difluorocyclopropanes.

  8. Sequential one-pot ruthenium-catalyzed azide-alkyne cycloaddition from primary alkyl halides and sodium azide.

    PubMed

    Johansson, Johan R; Lincoln, Per; Nordén, Bengt; Kann, Nina

    2011-04-01

    An experimentally simple sequential one-pot RuAAC reaction, affording 1,5-disubstituted 1H-1,2,3-triazoles in good to excellent yields starting from an alkyl halide, sodium azide, and an alkyne, is reported. The organic azide is formed in situ by treating the primary alkyl halide with sodium azide in DMA under microwave heating. Subsequent addition of [RuClCp*(PPh(3))(2)] and the alkyne yielded the desired cycloaddition product after further microwave irradiation.

  9. Facile rhenium-peptide conjugate synthesis using a one-pot derived Re(CO)3 reagent.

    PubMed

    Chanawanno, Kullapa; Kondeti, Vinay; Caporoso, Joel; Paruchuri, Sailaja; Leeper, Thomas C; Herrick, Richard S; Ziegler, Christopher J

    2016-03-21

    We have synthesized two Re(CO)3-modified lysine complexes (1 and 2), where the metal is attached to the amino acid at the Nε position, via a one-pot Schiff base formation reaction. These compounds can be used in the solid phase synthesis of peptides, and to date we have produced four conjugate systems incorporating neurotensin, bombesin, leutenizing hormone releasing hormone, and a nuclear localization sequence. We observed uptake into human umbilical vascular endothelial cells as well as differential uptake depending on peptide sequence identity, as characterized by fluorescence and rhenium elemental analysis.

  10. Red florescent Ag2S-CdS hybrid nanoparticles prepared by a one pot and rapid microwave method

    NASA Astrophysics Data System (ADS)

    Karimipour, Masoud; Molaei, Mehdi

    2016-03-01

    In this work, Ag2S-CdS hybrid composite with novel luminescence property was synthesized using a one pot and rapid microwave method. Structural analysis by means of XRD and TEM obtained the formation of the composite. Optical spectroscopy by means of UV-Vis and Photoluminescence measurements revealed that the functional composite has an intensive red light emission at 657 nm with a large stocks shift of about 150 nm. The quantum efficiency of the prepared hybrid material in red region is 10% which is comparable with the efficiency of pure CdS (11%) with green emission. [Figure not available: see fulltext.

  11. Synchronous One-Pot (SOP) synthesis of hybrid structures: metal nanoparticles in self-assemblies of amphiphilic calix[6]biscrowns.

    PubMed

    Liang, Qing; Li, Changxi; Chen, Guosong; Jiang, Ming

    2012-10-01

    In this paper, we present a novel strategy, named Synchronous One-Pot (SOP) synthesis, to prepare gold nanoparticles (AuNPs) with a diameter of 2nm incorporated in self-assembled organic spheres with a diameter around 60nm (denoted as NPAs). Merits of this method include: (1) self-assembly of the organic component (calix[6]biscrown TAC) into spheres and the reduction of chloroauric acid (HAuCl(4)) take place simultaneously; (2) preparation combining UV irradiation and formaldehyde addition reduces the size and homogenizes the distribution of the resultant AuNPs within the TAC spheres. (3) Obtained material NPA gives attractive catalytic property to hydrogenation reaction.

  12. Shape-controlled synthesis of Cu2O nanocrystals by one pot solution-phase reduction process

    NASA Astrophysics Data System (ADS)

    Zhang, Meili; Yu, Jinpeng; Zhang, Jianmin; Lan, Qi; Dai, Jia; Huang, Yaohan; Li, Guangli; Fan, Qingfei; Fan, Ximei; Zhou, Zuowan

    2017-03-01

    An interesting evolution to prepare shape-controlled Cu2O nanocrystals was realized by a convenient one pot synthesis. The Cu2O nanocrystals with different shapes can be obtained simply by adjusting the composition of reaction system. And, a plausible mechanism was also proposed to explain the nanostructures formation. The surface of Cu2O spheres with thorn exhibited high photocatalytic activity on the degradation of methyl orange (MO) solution under visible light irradiation. The photodegradation efficiency of MO solution reach up to 99.67% at the first 10 min. It is still as high as 98% even at the end of the fourth cycle.

  13. One-pot synthesis and antifungal activity against plant pathogens of quinazolinone derivatives containing an amide moiety.

    PubMed

    Zhang, Jin; Liu, Jia; Ma, Yangmin; Ren, Decheng; Cheng, Pei; Zhao, Jiawen; Zhang, Fan; Yao, Yuan

    2016-05-01

    An efficient one-pot, three-component synthesis of quinazolinone derivatives containing 3-acrylamino motif was carried out using CeO2 nanoparticles as catalyst. Thirty-nine synthesized compounds were obtained with satisfied yield and elucidated by spectroscopic analysis. Four phytopathogenic fungi were chosen to test the antifungal activities by minimum inhibitory concentration (MIC) method. Compounds 4ag, 4bb, 4bc showed broad antifungal activities against at least three fungi, and dramatic effects of substituents on the activities were observed. Docking studies were established to explore the potential antifungal mechanism of quinazolinone derivatives as the chitinase inhibitors, and also verified the importance of the amide moiety.

  14. Controlled silver delivery by silver-cellulose nanocomposites prepared by a one-pot green synthesis assisted by microwaves

    NASA Astrophysics Data System (ADS)

    Rosa Silva, Ana; Unali, Gianfranco

    2011-08-01

    Controlled silver release from cellulosic nanocomposites was achieved by synthesizing silver nanoparticles, under microwave heating for 1-15 min, in a one-pot, versatile and sustainable process in which microcrystalline cellulose simultaneously functions as reducing, stabilizing and supporting agent in water; chitin, starch and other cellulose derivatives could also be used as reducing, stabilizing and supporting agents for silver nanoparticles and the method was also found to be extensible to the preparation of noble metal (Au, Pt) and metal oxide nanoparticle (ZnO, Cu, CuO and Cu2O) nanocomposites.

  15. A general and expeditious one-pot synthesis of sulfoxides in high optical purity from norephedrine-derived sulfamidites.

    PubMed

    García Ruano, José L; Alemparte, Carlos; Aranda, M Teresa; Zarzuelo, María M

    2003-01-09

    A general and simple procedure for preparing any kind of enantiomerically enriched sulfoxide starting from norephedrine-derived N-benzyloxycarbonylsulfamidite 3a is reported. After one-pot reaction of 3a with RMgX, HBF(4), and R'MgX, a variety of sulfoxides 6 are obtained in ee usually higher than 93% and isolated yields ranging between 50 and 78%. The obtained configuration is tunable by simply electing the order of the addition of the reagents. [reaction--see text

  16. Regioselective synthesis of 2H-indazoles using a mild, one-pot condensation-Cadogan reductive cyclization.

    PubMed

    Genung, Nathan E; Wei, Liuqing; Aspnes, Gary E

    2014-06-06

    An operationally simple and efficient one-pot synthesis of 2H-indazoles from commercially available reagents is reported. Ortho-imino-nitrobenzene substrates, generated via condensation, undergo reductive cyclization promoted by tri-n-butylphosophine to afford substituted 2H-indazoles under mild reaction conditions. A variety of electronically diverse ortho-nitrobenzaldehydes and anilines were examined. To further extend the scope of the transformation, aliphatic amines were also employed to form N2-alkyl indazoles selectively under the optimized reaction conditions.

  17. A convenient four-component one-pot strategy toward the synthesis of pyrazolo[3,4-d]pyrimidines

    PubMed Central

    Liu, Mingxing; Li, Jiarong; Chai, Hongxin; Zhang, Kai; Yang, Deli; Zhang, Qi

    2015-01-01

    Summary An efficient one-pot synthesis of pyrazolo[3,4-d]pyrimidine derivatives by the four-component condensation of hydrazines, methylenemalononitriles, aldehydes and alcohols has been developed via two different reaction pathways. The structures of target products were characterized by IR spectroscopy, NMR (1H and 13C) spectroscopy and HRMS (ESI) spectrometry. The crystal structure of 4-ethoxy-6-(2-nitrophenyl)-1-phenyl-1H-pyrazolo[3,4-d]pyrimidine was determined by single crystal X-ray diffraction. PMID:26664633

  18. Multicomponent linchpin couplings. Reaction of dithiane anions with terminal epoxides, epichlorohydrin, and vinyl epoxides: efficient, rapid, and stereocontrolled assembly of advanced fragments for complex molecule synthesis.

    PubMed

    Smith, Amos B; Pitram, Suresh M; Boldi, Armen M; Gaunt, Matthew J; Sfouggatakis, Chris; Moser, William H

    2003-11-26

    The development, application, and advantages of a one-flask multicomponent dithiane linchpin coupling protocol, over the more conventional stepwise addition of dithiane anions to electrophiles leading to the rapid, efficient, and stereocontrolled assembly of highly functionalized intermediates for complex molecule synthesis, are described. Competent electrophiles include terminal epoxides, epichlorohydrin, and vinyl epoxides. High chemoselectivity can be achieved with epichlorohydrin and vinyl epoxides. For vinyl epoxides, the steric nature of the dithiane anion is critical; sterically unencumbered dithiane anions afford S(N)2 adducts, whereas encumbered anions lead primarily to SN2' adducts. Mechanistic studies demonstrate that the SN2' process occurs via syn addition to the vinyl epoxide. Integration of the multicomponent tactic with epichlorohydrin and vinyl epoxides permits the higher-order union of four and five components.

  19. Employing Arynes in Diels-Alder Reactions and Transition-Metal-Free Multicomponent Coupling and Arylation Reactions.

    PubMed

    Bhojgude, Sachin Suresh; Bhunia, Anup; Biju, Akkattu T

    2016-09-20

    Arynes are highly reactive intermediates having several applications in organic synthesis for the construction of various ortho-disubstituted arenes. Traditionally, arynes are generated in solution from haloarenes under strongly basic conditions. However, the scopes of many of the aryne reactions are limited because of the harsh conditions used for their generation. The renaissance of interest in aryne chemistry is mainly due to the mild conditions for their generation by the fluoride-induced 1,2-elimination of 2-(trimethylsilyl)aryl triflates. This Account is focused on the Diels-Alder reaction of arynes and their transition-metal-free application in multicomponent couplings as well as arylation reactions. The Diels-Alder reaction of arynes is a powerful tool for constructing benzo-fused carbocycles and heterocycles. In 2012, we developed an efficient, broad-scope, and scalable Diels-Alder reaction of pentafulvenes with arynes affording benzonorbornadiene derivatives. Subsequently, we accomplished the Diels-Alder reaction of arynes with dienes such as 1,2-benzoquinones and tropones. Moreover, we uncovered a transition-metal-free protocol for the synthesis of 9,10-dihydrophenanthrenes by the reaction of arynes with styrenes that proceeds via a Diels-Alder/ene-reaction cascade. In addition, we demonstrated the reaction of arynes with indene/benzofurans, which proceeds via a tandem [4 + 2]/[2 + 2] sequence. Multicomponent coupling (MCC) involving arynes mainly comprises the initial addition of a nucleophile to the aryne followed by interception of the aryl anion intermediate with an electrophile (provided the nucleophilic and electrophilic moieties do not belong to the same molecule). We have disclosed aryne MCCs initiated by N-heterocycles such as (iso)quinoline, pyridine, and aziridines. When (iso)quinoline is used as the nucleophilic trigger and N-substituted isatin as the third component, the reaction affords spirooxazino(iso)quinolines via 1,4-dipolar

  20. Evaluation of the metal uptake of several algae strains in a multicomponent matrix utilizing inductively coupled plasma emission spectrometry.

    PubMed

    Mahan, C A; Majidi, V; Holcombe, J A

    1989-03-15

    Three freshwater heat-killed, lyophilized blue-green algae strains have been characterized as to their ability to accumulate heavy metals with a focus on the utilization of these algae as an analytical preconcentration technique. This study examines the metal uptake in several multicomponent mixtures by using inductively coupled plasma optical emission spectrometry (ICP-OES). Six milligrams of a pure strain of algae was added to 20-mL aliquots of buffered (pH 5.5-6.5) multielement solutions containing 0.1, 0.5, 1.0, 2.0, and 4.0 mg/L of K, Mg, Ca, Fe, Sr, Co, Cu, Mn, Ni, V, Zn, As, Cd, Mo, Pb, and Se. All three algae strains exhibit relatively high adsorption affinities for Fe, Pb, and Cu, with uptake between 70 and 98% at the 4 ppm concentration level. Biosorption occurs for essentially every element with the relative affinities decreasing in the order Pb greater than Fe greater than Cu greater than Cd greater than Zn greater than Mn greater than Mo greater than Sr greater than Ni greater than V greater than Se greater than As greater than Co for Chlorella pyrenoidosa at the 4 mg/L concentration level. Although some minor differences were seen, the other algae strains (Stichococcus bacillaris and Chlamydomonas reinharti) displayed similar adsorption behavior over the concentration range studied, indicating similar cell wall binding sites. Langmuirian isotherms exhibited a minimum of two slopes over the concentration range of 0.1-4.0 mg/L, indicating the probable existence of at least two adsorption mechanisms.

  1. Selection of DNA Aptamers for Ovarian Cancer Biomarker CA125 Using One-Pot SELEX and High-Throughput Sequencing

    PubMed Central

    Scoville, Delia J.; Uhm, Tae Kyu Brian; Shallcross, Jamie A.

    2017-01-01

    CA125 is a mucin glycoprotein whose concentration in serum correlates with a woman's risk of developing ovarian cancer and also indicates response to therapy in diagnosed patients. Accurate detection of this large, complex protein in patient samples is of great clinical relevance. We suggest that powerful new diagnostic tools may be enabled by the development of nucleic acid aptamers with affinity for CA125. Here, we report on our use of One-Pot SELEX to isolate single-stranded DNA aptamers with affinity for CA125, followed by high-throughput sequencing of the selected oligonucleotides. This data-rich approach, combined with bioinformatics tools, enabled the entire selection process to be characterized. Using fluorescence anisotropy and affinity probe capillary electrophoresis, the binding affinities of four aptamer candidates were evaluated. Two aptamers, CA125_1 and CA125_12, both without primers, were found to bind to clinically relevant concentrations of the protein target. Binding was differently influenced by the presence of Mg2+ ions, being required for binding of CA125_1 and abrogating binding of CA125_12. In conclusion, One-Pot SELEX was found to be a promising selection method that yielded DNA aptamers to a clinically important protein target. PMID:28280637

  2. One-pot preparation of a molecularly imprinted hybrid monolithic capillary column for selective recognition and capture of lysozyme.

    PubMed

    Lin, Zian; Lin, Yao; Sun, Xiaobo; Yang, Huanghao; Zhang, Lan; Chen, Guonan

    2013-04-05

    A molecularly imprinted inorganic-organic hybrid monolithic capillary column (MIP hybrid monolith) was synthesized by one-pot process and its application in selective recognition and capture of lysozyme (Lyz) from complex biological samples was described for the first time. Due to a combination of rigid silica matrices and flexible organic hydrogels in one-pot process, stable and accessible recognition sites in the as-prepared MIP hybrid monolith could be obtained after the removal of template protein, which facilitated the rebinding of template and provided good reproducibility and lifetime of use. The morphology, permeability, and pore properties of the as-prepared MIP hybrid monolith were characterized and a uniform monolithic matrix with high surface area and large through-pores was observed. The recognition behavior of MIP and non-imprinted (NIP) hybrid monolith was evaluated by separating template protein from unfractionated protein mixture and the result indicated that the MIP hybrid monolith has much higher affinity toward the template protein than NIP hybrid monolith. High imprinted factor (IF) and separation efficiency could be obtained. In addition, the practicality of the Lyz-MIP hybrid monolith was further evaluated by selective separation of Lyz from egg white and capture of Lyz from human serum by adopting it as an in-tube solid phase microextraction (in-tube SPME), and the good results demonstrated its potential in proteome analysis.

  3. Highly Photoluminescent Molybdenum Oxide Quantum Dots: One-Pot Synthesis and Application in 2,4,6-Trinitrotoluene Determination.

    PubMed

    Xiao, Sai Jin; Zhao, Xiao Jing; Hu, Ping Ping; Chu, Zhao Jun; Huang, Cheng Zhi; Zhang, Li

    2016-03-01

    As a well-studied transition-metal semiconductor material, MoOx has a wider band gap than molybdenum disulfide (MoS2), and its property varies dramatically for the existence of several different allotropes and suboxide phases of molybdenum oxides (MoOx, x < 3). In this manuscript, a one-pot method possessing the advantages of one pot, easily prepared, rapid, and environmentally friendly, has been developed for facile synthesis of highly photoluminescent MoOx quantum dots (MoOx QDs), in which commercial molybdenum disulfide (MoS2) powder and hydrogen peroxide (H2O2) are employed as the precursor and oxidant, respectively. The obtained MoOx QDs can be further utilized as an efficient photoluminescent probe, and a new turn-off sensor is developed for 2,4,6-trinitrotoluene (TNT) determination based on the fact that the photoluminescence of MoOx QDs can be quenched by the Meisenheimer complexes formed in the strong alkali solution through the inner filter effect (IFE). Under the optimal conditions, the decreased photoluminescence of MoOx QDs shows a good linear relationship to the concentration of TNT ranging from 0.5 to 240.0 μM, and the limit of detection was 0.12 μM (3σ/k). With the present turn-off sensor, TNT in river water samples can be rapidly and selectively detected without tedious sample pretreatment processes.

  4. A mild one-pot process for synthesising hydroxyapatite/biomolecule bone scaffolds for sustained and controlled antibiotic release.

    PubMed

    Hess, Ulrike; Hill, Sebastian; Treccani, Laura; Streckbein, Philipp; Heiss, Christian; Rezwan, Kurosch

    2015-01-16

    The release of active molecules or the control of nosocomial infections for improved osteoinduction is ideally addressed by a bone substitute material. For this purpose, the feasibility of a mild one-pot process is probed for incorporating directly active proteins and antibiotics in a hydroxyapatite (HAp) based scaffold. The effect of two serum model proteins, bovine serum albumin (BSA) and fibrinogen (FIB), on the microstructure, on selected mechanical properties as well as on degradation behaviour and on protein release are investigated. By protein incorporation, the porosity can be adjusted between 54 and 70% especially due to the foaming ability of BSA. The addition of 5 wt% FIB doubles the biaxial flexural strength up to 6 MPa in comparison to samples without proteins (3 MPa). Protein release experiments show that a rapid release takes place within the first days (between around 3% for FIB and 38% for BSA). As a possible application for osteomyelitis treatment, vancomycin and gentamicin were subsequently added instead of proteins to study their release behaviour and their antibacterial activity, respectively. A controlled antibiotic release was observed for a period of 18 d. By varying the protein type, mixture and quantity, the mechanical strength porosity as well as the protein release and calcium solubility can be controlled. Our studies underpin the suitability of this mild one-pot process as a promising simple-to-use platform for controlled local drug release and bone treatment.

  5. Iodine catalyzed one-pot diamination of glycals with chloramine-T: a new approach to 2-amino-beta-glycosylamines for applications in N-glycopeptide synthesis.

    PubMed

    Kumar, Vipin; Ramesh, Namakkal G

    2006-12-21

    Iodine catalyzes a facile one-pot direct diamination of glycals with chloramine-T to afford stereoselectively 2-amino-beta-glycosylamine derivatives that serve as convenient precursors for the synthesis of N-linked glycopeptides.

  6. Application of Silica-Supported Alkylating Reagents in a One-Pot, Sequential Protocol to Diverse Benzoxathiazepine 1,1-Dioxides.

    PubMed

    Faisal, Saqib; Maity, Pradip K; Zang, Qin; Samarakoon, Thiwanka B; Sourk, Robert L; Hanson, Paul R

    2016-07-11

    Applications of silica-ROMP reagents in a one-pot, sequential protocol have been developed for the synthesis of a variety of diverse benzoxathiazepine 1,1-dioxides. This protocol includes sulfonylation, intramolecular SNAr, alkylation with silica-supported oligomeric benzyl (Si-OBPn) and triazole (Si-OTPn) phosphates, and intermolecular SNAr addition with a number of secondary amines in one-pot to afford a variety of unique benzoxathiazepine 1,1-dioxides sultams in good to excellent yields.

  7. Compressible and monolithic microporous polymer sponges prepared via one-pot synthesis

    PubMed Central

    Lim, Yoonbin; Cha, Min Chul; Chang, Ji Young

    2015-01-01

    Compressible and monolithic microporous polymers (MPs) are reported. MPs were prepared as monoliths via a Sonogashira–Hagihara coupling reaction of 1,3,5-triethynylbenzene (TEB) with the bis(bromothiophene) monomer (PBT-Br). The polymers were reversibly compressible, and were easily cut into any form using a knife. Microscopy studies on the MPs revealed that the polymers had tubular microstructures, resembling those often found in marine sponges. Under compression, elastic buckling of the tube bundles was observed using an optical microscope. MP-0.8, which was synthesized using a 0.8:1 molar ratio of PBT-Br to TEB, showed microporosity with a BET surface area as high as 463 m2g–1. The polymer was very hydrophobic, with a water contact angle of 145° and absorbed 7–17 times its own weight of organic liquids. The absorbates were released by simple compression, allowing recyclable use of the polymer. MPs are potential precursors of structured carbon materials; for example, a partially graphitic material was obtained by pyrolysis of MP-0.8, which showed a similar tubular structure to that of MP-0.8. PMID:26534834

  8. Compressible and monolithic microporous polymer sponges prepared via one-pot synthesis

    NASA Astrophysics Data System (ADS)

    Lim, Yoonbin; Cha, Min Chul; Chang, Ji Young

    2015-11-01

    Compressible and monolithic microporous polymers (MPs) are reported. MPs were prepared as monoliths via a Sonogashira-Hagihara coupling reaction of 1,3,5-triethynylbenzene (TEB) with the bis(bromothiophene) monomer (PBT-Br). The polymers were reversibly compressible, and were easily cut into any form using a knife. Microscopy studies on the MPs revealed that the polymers had tubular microstructures, resembling those often found in marine sponges. Under compression, elastic buckling of the tube bundles was observed using an optical microscope. MP-0.8, which was synthesized using a 0.8:1 molar ratio of PBT-Br to TEB, showed microporosity with a BET surface area as high as 463 m2g-1. The polymer was very hydrophobic, with a water contact angle of 145° and absorbed 7-17 times its own weight of organic liquids. The absorbates were released by simple compression, allowing recyclable use of the polymer. MPs are potential precursors of structured carbon materials; for example, a partially graphitic material was obtained by pyrolysis of MP-0.8, which showed a similar tubular structure to that of MP-0.8.

  9. One-Pot dry chemo-mechanical deconstruction for bioethanol production from sugarcane bagasse.

    PubMed

    Sambusiti, C; Licari, A; Solhy, A; Aboulkas, A; Cacciaguerra, T; Barakat, A

    2015-04-01

    The aim of this study was the application of an innovative dry chemo-mechanical pretreatment using different mechanical stresses to produce bioethanol from sugarcane bagasse (SB). The effect of different milling methods on physicochemical composition, enzymatic hydrolysis, bioethanol production and energy efficiency was also evaluated. SB was pretreated with NaOH and H3PO4 at high materials concentration (5 kg/L). Results indicate that vibratory milling (VBM) was more effective in the reduction of particles size and cellulose crystallinity compared to centrifugal (CM) and ball (BM) milling. NaOH pretreatment coupling to BM and VBM was preferred to enhance glucose yields and bioethanol production, while CM consumed less energy compared to BM and VBM. Moreover, the highest energy efficiency (η=0.116 kg glucose/kWh) was obtained with NaOH-CM. Therefore, the combination of dry NaOH and CM appears the most suitable and interesting pretreatment for the production of bioethanol from SB.

  10. Study of a dual frequency capacitively coupled rf discharge in the background of multi-component plasma and its validation by a simple analytical sheath model

    NASA Astrophysics Data System (ADS)

    Bhuyan, Heman; Saikia, Partha; Favre, Mario; Wyndham, Edmundo; Veloso, Felipe

    2016-10-01

    The behavior of a phase-locked dual frequency capacitively coupled rf discharges (2f-CCRF) in the background of multi-component plasma is experimentally studied by rf current-voltage measurements and optical emission spectroscopy (OES). The multi-component plasma is produced by adding hydrogen to the argon CCRF discharge. Variation of experimental parameters, like working pressure, low frequency (LF) and high frequency (HF) rf power indicate significant changes in the electron density and temperature as well as the DC self-bias developed on the power electrode. It is observed that the electron density decreases as the percentage of hydrogen increases in the argon plasma while the electron temperature follows opposite trend. An analytical sheath model for the 2f-CCRF discharge in the background of multi-component plasma is developed and its prediction on the observed variation of DC self-bias is well agreed with the experimental observations. Authors acknowledge Proyecto Puente No P1611 and FONDECYT 3160179.

  11. Carboxylic acid-grafted mesoporous material and its high catalytic activity in one-pot three-component coupling reaction

    NASA Astrophysics Data System (ADS)

    Gomes, Ruth; Dutta, Saikat; Bhaumik, Asim

    2014-11-01

    A new carboxylic acid functionalized mesoporous organic polymer has been synthesized via in situ radical polymerization of divinylbenzene and acrylic acid using a mesoporous silica as a seed during the polymerization process under solvothermal conditions. The mesoporous material MPDVAA-1 has been thoroughly characterized employing powder XRD, solid state 13C cross polarization magic angle spinning-nuclear magnetic resonance, FT-IR spectroscopy, N2 sorption, HR-TEM, and NH3 temperature programmed desorption-thermal conductivity detector (TPD-TCD) analysis to understand its porosity, chemical environment, bonding, and surface properties. The mesoporous polymer was used as a catalyst for a three comp onent Biginelli condensation between various aldehydes, β-keto esters, and urea/thioureas to give 3,4-dihydropyrimidine-2(1H)-ones. The reactions were carried out under conventional heating as well as solvent-free microwave irradiation of solid components, and in both the cases, the mesoporous polymer MPDVAA-1 proved to be a powerful, robust, and reusable catalyst with high catalytic efficiency.

  12. Carboxylic acid-grafted mesoporous material and its high catalytic activity in one-pot three-component coupling reaction

    SciTech Connect

    Gomes, Ruth; Bhaumik, Asim; Dutta, Saikat

    2014-11-01

    A new carboxylic acid functionalized mesoporous organic polymer has been synthesized via in situ radical polymerization of divinylbenzene and acrylic acid using a mesoporous silica as a seed during the polymerization process under solvothermal conditions. The mesoporous material MPDVAA-1 has been thoroughly characterized employing powder XRD, solid state {sup 13}C cross polarization magic angle spinning-nuclear magnetic resonance, FT-IR spectroscopy, N{sub 2} sorption, HR-TEM, and NH{sub 3} temperature programmed desorption-thermal conductivity detector (TPD-TCD) analysis to understand its porosity, chemical environment, bonding, and surface properties. The mesoporous polymer was used as a catalyst for a three comp onent Biginelli condensation between various aldehydes, β-keto esters, and urea/thioureas to give 3,4-dihydropyrimidine-2(1H)-ones. The reactions were carried out under conventional heating as well as solvent-free microwave irradiation of solid components, and in both the cases, the mesoporous polymer MPDVAA-1 proved to be a powerful, robust, and reusable catalyst with high catalytic efficiency.

  13. Synthesis of annulated 2H-indazoles and 1,2,3- and 1,2,4-triazoles via a one-pot palladium-catalyzed alkylation/direct arylation reaction.

    PubMed

    Laleu, Benoît; Lautens, Mark

    2008-11-21

    A variety of six-membered-ring annulated 2H-indazoles and 1,2,3- and 1,2,4-triazoles were synthesized in good to excellent yields from the corresponding bromoethyl azoles and aryl iodides. The annulation process involves a one-pot norbornene-mediated palladium-catalyzed sequence whereby an alkyl-aryl bond and an aryl-heteroaryl bond are successively formed through two C-H bond activations. Subsequent functionalizations of the resulting polycyclic through cross-coupling reactions are also presented.

  14. One-pot preparation of superparamagnetic attapulgite/Fe3O4/polydopamine nanocomposites for adsorption of methylene blue

    NASA Astrophysics Data System (ADS)

    Mu, Bin; Kang, Yuru; Zheng, Maosong; Wang, Aiqin

    2016-05-01

    Superparamagnetic attapulgite/Fe3O4/polydopamine nanocomposites have been facilely prepared by a one-pot process without the nitrogen protection, in which Fe(III) was served as both of the oxidant for dopamine and the precursor of Fe3O4 in the presence of attapulgite. The introduction of attapulgite can effectively induce the uniform encapsulation of polydopamine and Fe3O4 nanoparticles on the surface of attapulgite, preventing from the formation of the free aggregates of Fe3O4 nanoparticles. The as-prepared APT/Fe3O4/PANI nanocomposites can be used as an adsorbent for the removal of methylene blue, and the adsorption ratio toward 100 ppm of methylene blue could reach 95.8%.

  15. Facile, one-pot synthesis, and antibacterial activity of mesoporous silica nanoparticles decorated with well-dispersed silver nanoparticles.

    PubMed

    Tian, Yue; Qi, Juanjuan; Zhang, Wei; Cai, Qiang; Jiang, Xingyu

    2014-08-13

    In this study, we exploit a facile, one-pot method to prepare MCM-41 type mesoporous silica nanoparticles decorated with silver nanoparticles (Ag-MSNs). Silver nanoparticles with diameter of 2-10 nm are highly dispersed in the framework of mesoporous silica nanoparticles. These Ag-MSNs possess an enhanced antibacterial effect against both Gram-positive and Gram-negative bacteria by preventing the aggregation of silver nanoparticles and continuously releasing silver ions for one month. The cytotoxicity assay indicates that the effective antibacterial concentration of Ag-MSNs shows little effect on human cells. This report describes an efficient and economical route to synthesize mesoporous silica nanoparticles with uniform silver nanoparticles, and these nanoparticles show promising applications as antibiotics.

  16. Eco-friendly one-pot synthesis of highly dispersible functionalized graphene nanosheets with free amino groups

    NASA Astrophysics Data System (ADS)

    Liu, Zhiting; Duan, Xuezhi; Qian, Gang; Zhou, Xinggui; Yuan, Weikang

    2013-02-01

    An eco-friendly, facile and scalable hydrothermal approach, in which the reduction and functionalization of graphite oxide (GO) are completed in one pot, is proposed for the synthesis of monolayer 3-aminopropyltriethoxysilane (APTES)-functionalized graphenes (A-FGs). Atomic force microscopy, transmission electron microscopy and x-ray diffraction analyses indicate that the as-synthesized A-FGs consist of only one or a few layered graphenes, while x-ray photoelectron spectroscopy, Fourier transform infrared spectroscopy and thermogravimetric analysis reveal that APTES is bonded to graphene by the dehydration reaction between the Si-OH (produced by APTES hydration) and the -OH on the GO surface. As a result, free amino groups are left on the A-FGs. Moreover, A-FGs are highly dispersible in dimethylsulfoxide, APTES and ethylene glycol, and their solubilities are up to 0.89, 4.03 and 0.90 mg ml-1, respectively.

  17. One-pot non-enzymatic formation of firefly luciferin in a neutral buffer from p-benzoquinone and cysteine.

    PubMed

    Kanie, Shusei; Nishikawa, Toshio; Ojika, Makoto; Oba, Yuichi

    2016-04-21

    Firefly luciferin, the substrate for the bioluminescence reaction of luminous beetles, possesses a benzothiazole ring, which is rare in nature. Here, we demonstrate a novel one-pot reaction to give firefly luciferin in a neutral buffer from p-benzoquinone and cysteine without any synthetic reagents or enzymes. The formation of firefly luciferin was low in yield in various neutral buffers, whereas it was inhibited or completely prevented in acidic or basic buffers, in organic solvents, or under a nitrogen atmosphere. Labelling analysis of the firefly luciferin using stable isotopic cysteines showed that the benzothiazole ring was formed via the decarboxylation and carbon-sulfur bond rearrangement of cysteine. These findings imply that the biosynthesis of firefly luciferin can be developed/evolved from the non-enzymatic production of firefly luciferin using common primary biosynthetic units, p-benzoquinone and cysteine.

  18. One-Pot Evolution of Ageladine A through a Bio-Inspired Cascade towards Selective Modulators of Neuronal Differentiation.

    PubMed

    Iwata, Takayuki; Otsuka, Satoshi; Tsubokura, Kazuki; Kurbangalieva, Almira; Arai, Daisuke; Fukase, Koichi; Nakao, Yoichi; Tanaka, Katsunori

    2016-10-04

    A bio-inspired cascade reaction has been developed for the construction of the marine natural product ageladine A and a de novo array of its N1-substituted derivatives. This cascade features a 2-aminoimidazole formation that is modeled after an arginine post-translational modification and an aza-electrocyclization. It can be effectively carried out in a one-pot procedure from simple anilines or guanidines, leading to structural analogues of ageladine A that had been otherwise synthetically inaccessible. We found that some compounds out of this structurally novel library show a significant activity in modulating the neural differentiation. Namely, these compounds selectively activate or inhibit the differentiation of neural stem cells to neurons, while being negligible in the differentiation to astrocytes. This study represents a successful case in which the native biofunction of a natural product could be altered by structural modifications.

  19. One-Pot Solvothermal Synthesis of Bi4V2O11 as A New Solar Water Oxidation Photocatalyst.

    PubMed

    Jiang, Zaiyong; Liu, Yuanyuan; Li, Mengmeng; Jing, Tao; Huang, Baibiao; Zhang, Xiaoyang; Qin, Xiaoyan; Dai, Ying

    2016-03-07

    Bi4V2O11 was prepared via a one-pot solvothermal method and characterized via XRD, Raman, XPS, Electrochemical impedance spectroscopy. The as-prepared Bi4V2O11 sample displays excellent photocatalytic activity towards oxygen evolution under light irradiation. The hierarchical structure is in favour of the spatial separation of photogenerated electrons and holes. Furthermore, the internal polar field also plays a role in improving the charge separation. Both of the two results are responsible for excellent activity of O2 evolution. The resulting hierarchical Bi4V2O11 sample should be very promising photocatalyst for the application of photocatalytic O2 evolution in the future.

  20. One-pot synthesis of amino acid precursors with insoluble organic matter in planetesimals with aqueous activity.

    PubMed

    Kebukawa, Yoko; Chan, Queenie H S; Tachibana, Shogo; Kobayashi, Kensei; Zolensky, Michael E

    2017-03-01

    The exogenous delivery of organic molecules could have played an important role in the emergence of life on the early Earth. Carbonaceous chondrites are known to contain indigenous amino acids as well as various organic compounds and complex macromolecular materials, such as the so-called insoluble organic matter (IOM), but the origins of the organic matter are still subject to debate. We report that the water-soluble amino acid precursors are synthesized from formaldehyde, glycolaldehyde, and ammonia with the presence of liquid water, simultaneously with macromolecular organic solids similar to the chondritic IOM. Amino acid products from hydrothermal experiments after acid hydrolysis include α-, β-, and γ-amino acids up to five carbons, for which relative abundances are similar to those extracted from carbonaceous chondrites. One-pot aqueous processing from simple ubiquitous molecules can thus produce a wide variety of meteoritic organic matter from amino acid precursors to macromolecular IOM in chondrite parent bodies.

  1. One-pot facile synthesis of CuS/graphene composite as anode materials for lithium ion batteries

    NASA Astrophysics Data System (ADS)

    Tao, Hua-Chao; Yang, Xue-Lin; Zhang, Lu-Lu; Ni, Shi-Bing

    2014-11-01

    CuS/graphene composite has been synthesized by the one-pot hydrothermal method using thiourea as the sulfur source and reducing agent. The formation of CuS nanoparticles and the reduction of graphene oxide occur simultaneously during the hydrothermal process, which enables a uniform dispersion of CuS nanoparticles on the graphene nanosheets. The electrochemical performance of CuS/graphene composite was studied as anode materials for lithium ion batteries. The obtained CuS/graphene composite exhibits a relative high reversible capacity and good cycling stability. The good electrochemical performance of CuS/graphene composite can be attributed to graphene, which improves the electronic conductivity of composite and enhances the interfacial stability of electrode and electrolyte.

  2. One-pot non-enzymatic formation of firefly luciferin in a neutral buffer from p-benzoquinone and cysteine

    PubMed Central

    Kanie, Shusei; Nishikawa, Toshio; Ojika, Makoto; Oba, Yuichi

    2016-01-01

    Firefly luciferin, the substrate for the bioluminescence reaction of luminous beetles, possesses a benzothiazole ring, which is rare in nature. Here, we demonstrate a novel one-pot reaction to give firefly luciferin in a neutral buffer from p-benzoquinone and cysteine without any synthetic reagents or enzymes. The formation of firefly luciferin was low in yield in various neutral buffers, whereas it was inhibited or completely prevented in acidic or basic buffers, in organic solvents, or under a nitrogen atmosphere. Labelling analysis of the firefly luciferin using stable isotopic cysteines showed that the benzothiazole ring was formed via the decarboxylation and carbon-sulfur bond rearrangement of cysteine. These findings imply that the biosynthesis of firefly luciferin can be developed/evolved from the non-enzymatic production of firefly luciferin using common primary biosynthetic units, p-benzoquinone and cysteine. PMID:27098929

  3. One-Pot Solvothermal Synthesis of Bi4V2O11 as A New Solar Water Oxidation Photocatalyst

    PubMed Central

    Jiang, Zaiyong; Liu, Yuanyuan; Li, Mengmeng; Jing, Tao; Huang, Baibiao; Zhang, Xiaoyang; Qin, Xiaoyan; Dai, Ying

    2016-01-01

    Bi4V2O11 was prepared via a one-pot solvothermal method and characterized via XRD, Raman, XPS, Electrochemical impedance spectroscopy. The as-prepared Bi4V2O11 sample displays excellent photocatalytic activity towards oxygen evolution under light irradiation. The hierarchical structure is in favour of the spatial separation of photogenerated electrons and holes. Furthermore, the internal polar field also plays a role in improving the charge separation. Both of the two results are responsible for excellent activity of O2 evolution. The resulting hierarchical Bi4V2O11 sample should be very promising photocatalyst for the application of photocatalytic O2 evolution in the future. PMID:26947126

  4. One-pot electrochemical synthesis of functionalized fluorescent carbon dots and their selective sensing for mercury ion.

    PubMed

    Hou, Yuxin; Lu, Qiujun; Deng, Jianhui; Li, Haitao; Zhang, Youyu

    2015-03-25

    We propose a simple, economical, and one-pot method to synthesize water-soluble functionalized fluorescent carbon dots (C-Dots) through electrochemical carbonization of sodium citrate and urea. The as-prepared C-Dots have good photostability and exhibit a high quantum yield of 11.9%. The sizes of the C-Dots are mainly distributed in the range of 1.0-3.5 nm with an average size of 2.4 nm. It has been further used as a novel label-free sensing probe for selective detection of Hg(2+) ions with detection limit as low as 3.3 nM. The detection linear range is 0.01-10 μM. The as-prepared C-Dots are also successfully applied for the determination of Hg(2+) in real water samples.

  5. One-pot synthesis of MWW zeolite nanosheets using a rationally designed organic structure-directing agent

    PubMed Central

    Luo, Helen Y.; Michaelis, Vladimir K.; Hodges, Sydney; Griffin, Robert G.

    2015-01-01

    A new material MIT-1 comprised of delaminated MWW zeolite nanosheets is synthesized in one-pot using a rationally designed organic structure-directing agent (OSDA). The OSDA is comprised of a hydrophilic head segment that resembles the OSDA used to synthesize the zeolite precursor MCM22(P), a hydrophobic tail segment that resembles the swelling agent used to swell MCM22(P), and a di-quaternary ammonium linker that connects both segments. MIT-1 features high crystallinity and surface areas exceeding 500 m2g−1, and can be synthesized over a wide synthesis window that includes Si/Al ratios ranging from 13 to 67. Characterization data reveal high mesoporosity and acid strength with no detectable amorphous silica phases. Compared to MCM-22 and MCM-56, MIT-1 shows a three-fold increase in catalytic activity for the Friedel-Crafts alkylation of benzene with benzyl alcohol. PMID:26478803

  6. One-pot synthesis of Fe, Co and Ni-doped carbon xerogels and their magnetic properties

    NASA Astrophysics Data System (ADS)

    Liu, Zhi; Lv, Cong; Tan, Xiuli

    2013-09-01

    Transition metal (Fe, Co and Ni)-doped carbon xerogels were synthesized by a facile one-pot pyrolysis of the sol-gel polymer of resorcinol and formaldehyde in the presence of the corresponding metal nitrates. N2 adsorption-desorption, scanning and transmission electron microscopy proved that addition of different metals could exert a remarkable influence on the textural properties. From X-ray diffraction the phases of the metallic species were identified. Scanning electron microscopy images revealed that the surface morphologies of resultant metal-carbon xerogels were composed of carbon microspheres with diameters from 5 to 15 µm. Transmission electron microscopy observations illustrated that Ni-carbon xerogel was made of uniform carbon nanotubes which differed from the approximative core/shell structures of Fe- and Co-carbon xerogels. Measurements on magnetic properties indicated that the Fe-, Co-, and Ni-carbon xerogels exhibited typical ferromagnetic characteristics at room temperature.

  7. One-pot aqueous synthesis of gadolinium doped CdTe quantum dots with dual imaging modalities.

    PubMed

    Jiang, Chunli; Shen, Zhitao; Luo, Chunhua; Lin, Hechun; Huang, Rong; Wang, Yiting; Peng, Hui

    2016-08-01

    A facile one-pot strategy has been developed for the aqueous synthesis of Gd doped CdTe (Gd:CdTe) QDs as fluorescence and magnetic resonance imaging dual-modal agent. The prepared Gd:CdTe QDs showed narrow size distribution and the average size was less than 5nm. The amount of Gd(3+) dopant in Gd:CdTe QDs significantly affected the optical properties of obtained QDs. The highest PL QY for the prepared Gd:CdTe QDs was up to 42.5%. The QDs showed the weak toxicity and significant enhancement in MRI signal. The specific relaxivity value (r1) was determined to be 4.22mM(-1)s(-1). These properties make the prepared Gd:CdTe QDs be an effective dual-modal imaging agent and have great potential applications in biomedical field.

  8. Bifunctional Mesoporous Carbon Nitride: Highly Efficient Enzyme-like Catalyst for One-pot Deacetalization-Knoevenagel Reaction

    NASA Astrophysics Data System (ADS)

    Zhong, Lin; Anand, Chokkalingam; Lakhi, Kripal Singh; Lawrence, Geoffrey; Vinu, Ajayan

    2015-08-01

    Recently, mesoporous carbon nitride (MCN) has aroused extensive interest for its potential applications in organocatalysis, photo- and electrochemistry and CO2 capture. However, further surface functionalization of MCN for advanced nanomaterials and catalysis still remains very challenging. Here we show that acidic carboxyl groups can be smoothly introduced onto the surface of well-ordered MCN without annihilation between the introduced acid groups and MCN’s inherent basic groups through a facile UV light oxidation method. The functionalization generates a novel bifunctional nanocatalyst which offers an enzyme-like catalytic performance in the one-pot deacetalization-Knoevenagel reaction of benzaldehyde dimethylacetal and malononitrile with 100% conversion and more than 99% selectivity due to the cooperative catalysis between the acid and base groups separated on the surface of the catalyst. The results provide a general method to create multifunctional nanomaterials and open new opportunities for the development of high efficient catalyst for green organic synthesis.

  9. Thiophene-forming one-pot synthesis of three thienyl-bridged oligophenothiazines and their electronic properties.

    PubMed

    Urselmann, Dominik; Deilhof, Konstantin; Mayer, Bernhard; Müller, Thomas J J

    2016-01-01

    The pseudo five-component Sonogashira-Glaser cyclization synthesis of symmetrically 2,5-diaryl-substituted thiophenes is excellently suited to access thienyl-bridged oligophenothiazines in a one-pot fashion. Three thienyl-bridged systems were intensively studied by UV-vis and fluorescence spectroscopy as well as by cyclic voltammetry. The oxidation proceeds with lower oxidation potentials and consistently reversible oxidations can be identified. The Stokes shifts are large and substantial fluorescence quantum yields can be measured. Computational chemistry indicates lowest energy conformers with sigmoidal and helical structure, similar to oligophenothiazines. TD-DFT and even semiempirical ZINDO calculations reproduce the trends of longest wavelengths absorption bands and allow the assignment of these transitions to possess largely charge-transfer character from the adjacent phenothiazinyl moieties to the central thienyl unit.

  10. Thiophene-forming one-pot synthesis of three thienyl-bridged oligophenothiazines and their electronic properties

    PubMed Central

    Urselmann, Dominik; Deilhof, Konstantin; Mayer, Bernhard

    2016-01-01

    Summary The pseudo five-component Sonogashira–Glaser cyclization synthesis of symmetrically 2,5-diaryl-substituted thiophenes is excellently suited to access thienyl-bridged oligophenothiazines in a one-pot fashion. Three thienyl-bridged systems were intensively studied by UV–vis and fluorescence spectroscopy as well as by cyclic voltammetry. The oxidation proceeds with lower oxidation potentials and consistently reversible oxidations can be identified. The Stokes shifts are large and substantial fluorescence quantum yields can be measured. Computational chemistry indicates lowest energy conformers with sigmoidal and helical structure, similar to oligophenothiazines. TD-DFT and even semiempirical ZINDO calculations reproduce the trends of longest wavelengths absorption bands and allow the assignment of these transitions to possess largely charge-transfer character from the adjacent phenothiazinyl moieties to the central thienyl unit. PMID:27829911

  11. One-pot synthesis of FePt/CNTs nanocomposites for efficient cellular imaging and cancer therapy

    NASA Astrophysics Data System (ADS)

    Chen, Weihong; Zheng, Xiuwen; Li, Shulian; Zhang, Wei; Wen, Xin; Yue, Ludan; Wang, Jinlong

    2015-11-01

    Here, we developed a facile route to synthesize carbon nanotube-based FePt nanocomposites (FePt/CNTs) as a potential theranostic platform in the cancer treatment. FePt/CNTs were firstly synthesized via one-pot polyol route, and then functionalized with 6-arm-polyethylene glycol-amine polymer. The average size of FePt nanoparticles (NPs) is 3-4 nm, which is dispersed on the CNT surface (ca.50-150 nm). The as-prepared FePt NPs display high cytotoxicity by highly reactive oxygen species in cancer cells. Folic acid and fluorescein isothiocyanate are assembled onto the surface of FePt/CNTs for effective targeting of folate receptor-positive cancer cells and simultaneously for the visualization of cellular uptake. Therefore, the FePt/CNTs NPs capability of simultaneously performing diagnosis, therapy, and targeting is, therefore, promising for future potential widespread application in biomedicine.

  12. Bio-inspired one-pot route to prepare robust and repairable micro-nanoscale superhydrophobic coatings.

    PubMed

    Si, Yifan; Yang, Fuchao; Guo, Zhiguang

    2017-03-16

    Superhydrophobic (SHP) coatings inspired by lotus have great application prospect for our daily life. Regrettably, three formidable challenges, namely, complex fabrication, weak mechanical stability and large-scale fabrication, have already existed for a long time in this research field. Here, a robust micro-nanoscale P25 (Nano TiO2)/MgO/epoxy resin (ER) SHP coating has been fabricated via facile one-pot route, which can be applied to arbitrary substrates through multiples methods. P25/MgO/ER SHP coating not only displays excellent mechanical stability but also shows unique repairable ability to recover its superhydrophobicity under various damages by extreme environment such as low temperature, strong acid or alkali and this repairable process can be repeated for many times. P25/MgO/ER SHP coating also is easy to large-scale fabrication with very low cost.

  13. One-pot process combining transesterification and selective hydrogenation for biodiesel production from starting material of high degree of unsaturation.

    PubMed

    Yang, Ru; Su, Mengxing; Li, Min; Zhang, Jianchun; Hao, Xinmin; Zhang, Hua

    2010-08-01

    A one-pot process combining transesterification and selective hydrogenation was established to produce biodiesel from hemp (Cannabis sativa L.) seed oil which is eliminated as a potential feedstock by a specification of iodine value (IV; 120 g I(2)/100g maximum) contained in EN 14214. A series of alkaline earth metal oxides and alkaline earth metal supported copper oxide were prepared and tested as catalysts. SrO supported 10 wt.% CuO showed the superior catalytic activity for transesterification with a biodiesel yield of 96% and hydrogenation with a reduced iodine value of 113 and also exhibited a promising selectivity for eliminating methyl linolenate and increasing methyl oleate without rising methyl stearate in the selective hydrogenation. The fuel properties of the selective hydrogenated methyl esters are within biodiesel specifications. Furthermore, cetane numbers and iodine values were well correlated with the compositions of the hydrogenated methyl esters according to degrees of unsaturation.

  14. One-pot synthesis of MWW zeolite nanosheets using a rationally designed organic structure-directing agent

    SciTech Connect

    Luo, Helen Y.; Michaelis, Vladimir K.; Hodges, Sydney; Griffin, Robert G.; Roman-Leshkov, Yuriy

    2015-07-22

    A new material MIT-1 comprised of delaminated MWW zeolite nanosheets is synthesized in one-pot using a rationally designed organic structure-directing agent (OSDA). The OSDA is comprised of a hydrophilic head segment that resembles the OSDA used to synthesize the zeolite precursor MCM22(P), a hydrophobic tail segment that resembles the swelling agent used to swell MCM22(P), and a di-quaternary ammonium linker that connects both segments. MIT-1 features high crystallinity and surface areas exceeding 500 m2g-1, and can be synthesized over a wide synthesis window that includes Si/Al ratios ranging from 13 to 67. Characterization data reveal high mesoporosity and acid strength with no detectable amorphous silica phases. In conclusion, compared to MCM-22 and MCM-56, MIT-1 shows a three-fold increase in catalytic activity for the Friedel-Crafts alkylation of benzene with benzyl alcohol.

  15. One-pot synthesis of MWW zeolite nanosheets using a rationally designed organic structure-directing agent

    DOE PAGES

    Luo, Helen Y.; Michaelis, Vladimir K.; Hodges, Sydney; ...

    2015-07-22

    A new material MIT-1 comprised of delaminated MWW zeolite nanosheets is synthesized in one-pot using a rationally designed organic structure-directing agent (OSDA). The OSDA is comprised of a hydrophilic head segment that resembles the OSDA used to synthesize the zeolite precursor MCM22(P), a hydrophobic tail segment that resembles the swelling agent used to swell MCM22(P), and a di-quaternary ammonium linker that connects both segments. MIT-1 features high crystallinity and surface areas exceeding 500 m2g-1, and can be synthesized over a wide synthesis window that includes Si/Al ratios ranging from 13 to 67. Characterization data reveal high mesoporosity and acid strengthmore » with no detectable amorphous silica phases. In conclusion, compared to MCM-22 and MCM-56, MIT-1 shows a three-fold increase in catalytic activity for the Friedel-Crafts alkylation of benzene with benzyl alcohol.« less

  16. One-pot synthesis of amino acid precursors with insoluble organic matter in planetesimals with aqueous activity

    PubMed Central

    Kebukawa, Yoko; Chan, Queenie H. S.; Tachibana, Shogo; Kobayashi, Kensei; Zolensky, Michael E.

    2017-01-01

    The exogenous delivery of organic molecules could have played an important role in the emergence of life on the early Earth. Carbonaceous chondrites are known to contain indigenous amino acids as well as various organic compounds and complex macromolecular materials, such as the so-called insoluble organic matter (IOM), but the origins of the organic matter are still subject to debate. We report that the water-soluble amino acid precursors are synthesized from formaldehyde, glycolaldehyde, and ammonia with the presence of liquid water, simultaneously with macromolecular organic solids similar to the chondritic IOM. Amino acid products from hydrothermal experiments after acid hydrolysis include α-, β-, and γ-amino acids up to five carbons, for which relative abundances are similar to those extracted from carbonaceous chondrites. One-pot aqueous processing from simple ubiquitous molecules can thus produce a wide variety of meteoritic organic matter from amino acid precursors to macromolecular IOM in chondrite parent bodies. PMID:28345041

  17. The first one-pot synthesis of metal-organic frameworks functionalised with two transition-metal complexes.

    PubMed

    Platero-Prats, Ana E; Bermejo Gómez, Antonio; Samain, Louise; Zou, Xiaodong; Martín-Matute, Belén

    2015-01-07

    The synthesis of a metal-organic framework (UiO-67) functionalised simultaneously with two different transition metal complexes (Ir and Pd or Rh) through a one-pot procedure is reported for the first time. This has been achieved by an iterative modification of the synthesis parameters combined with characterisation of the resulting materials using different techniques, including X-ray absorption spectroscopy (XAS). The method also allows the first synthesis of UiO-67 with a very wide range of loadings (from 4 to 43 mol %) of an iridium complex ([IrCp*(bpydc)(Cl)Cl](2-) ; bpydc=2,2'-bipyridine-5,5'-dicarboxylate, Cp*=pentamethylcyclopentadienyl) through a pre-functionalisation methodology.

  18. Highly regioselective synthesis of amino-functionalized dendritic polyglycerols by a one-pot hydroformylation/reductive amination sequence.

    PubMed

    Koç, Fikret; Wyszogrodzka, Monika; Eilbracht, Peter; Haag, Rainer

    2005-03-18

    [reaction: see text] Dendritic architectures with neutral core structures and amines groups in the shell are a synthetic challenge, and there is a need for an efficient access. In this paper, highly selective Rh-catalysts are used for sequential hydroformylation/reductive amination of dendritic perallylated polyglycerols 1 with various amines in a one-pot procedure to give dendritic polyamines 3a-e in high yields (73-99%). In all cases, complete conversion of the allyl ether and aldehyde intermediate has been observed. Furthermore, the use of protected amines provides reactive core-shell-type architectures after deprotection. These soluble but membrane filterable multifunctional dendritic polyamines are of high interest as reagents in synthesis or as supports in homogeneous catalysis as well as nonviral vectors for DNA-transfection.

  19. One-pot synthesis of MnO2-chitin hybrids for effective removal of methylene blue.

    PubMed

    Dassanayake, Rohan S; Rajakaruna, Erandathi; Moussa, Hanna; Abidi, Noureddine

    2016-12-01

    Manganese dioxide (MnO2)-chitin-hybrid material was prepared by a facile "one-pot" synthesis method. MnO2-chitin hybrid was used for the effective removal of methylene blue (MB) from liquid solution as model for wastewater treatment. The hybrid obtained was characterized by field emission scanning electron microscopy and energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy, X-ray diffraction and thermogravimetric analysis. The effect of pH and temperature were studied. MnO2-chitin hybrid showed high performance for oxidative decolorization and removal of MB. Typically, 25mL of MB (20mg/L) can be completely decolorized in 2.5min with 8.5mg of the MnO2-chitin hybrid. The hybrid material exhibited excellent recyclability and durability with the degradation value of 99% for MB after ten consecutive cycles.

  20. One-pot preparation of a mixed-mode organic-silica hybrid monolithic capillary column and its application in determination of endogenous gibberellins in plant tissues.

    PubMed

    Zhang, Zheng; Hao, Yan-Hong; Ding, Jun; Xu, Sheng-Nan; Yuan, Bi-Feng; Feng, Yu-Qi

    2015-10-16

    A newly improved one-pot method, based on "thiol-ene" click chemistry and sol-gel approach in microemulsion system, was developed for the preparation of C8/PO(OH)2-silica hybrid monolithic capillary column. The prepared monolith possesses large specific surface area, narrow mesopore size distribution and high column efficiency. The monolithic column was demonstrated to have cation exchange/reversed-phase (CX/RP) mixed-mode retention for analytes on nano-liquid chromatography (nano-LC). On the basis of the developed nano-LC system with MS detector coupled to pipette tip solid phase extraction (PT-SPE) and derivatization process, we then realized simultaneous determination of 10 gibberellins (GAs) with low limits of detection (LODs, 0.003-0.025 ng/mL). Furthermore, 6 endogenous GAs in only 5mg rice leaves (fresh weight) were successfully detected and quantified. The developed PT-SPE-nano-LC-MS strategy may offer promising applications in the determination of low abundant bioactive molecules from complex matrix.

  1. Differentiation of Sialyl Linkage Isomers by One-Pot Sialic Acid Derivatization for Mass Spectrometry-Based Glycan Profiling.

    PubMed

    Nishikaze, Takashi; Tsumoto, Hiroki; Sekiya, Sadanori; Iwamoto, Shinichi; Miura, Yuri; Tanaka, Koichi

    2017-02-21

    Matrix-assisted laser desorption/ionization mass spectrometry (MALDI-MS) has been used for high-throughput glycan profiling analysis. In spite of the biological importance of sialic acids on nonreducing ends of glycans, it is still difficult to analyze glycans containing sialic acid residues due to their instability and the presence of linkage isomers. In this Article, we describe a one-pot glycan purification/derivatization method employing a newly developed linkage-specific sialic acid derivatization for MS-based glycan profiling with differentiation of sialyl linkage isomer. The derivatization, termed sialic acid linkage specific alkylamidation (SALSA), consists of sequential two-step alkylamidations. As a result of the reactions, α2,6- and α2,3-linked sialic acids are selectively amidated with different length of alkyl chains, allowing distinction of α2,3-/α2,6-linkage isomers from given mass spectra. Our studies using N-glycan standards with known sialyl linkages proved high suitability of SALSA for reliable relative quantification of α2,3-/α2,6-linked sialic acids compared with existing sialic acid derivatization approaches. SALSA fully stabilizes both α2,3- and α2,6-linked sialic acids by alkylamidation; thereby, it became possible to combine SALSA with existing glycan analysis/preparation methods as follows. The combination of SALSA and chemoselective glycan purification using hydrazide beads allows easy one-pot purification of glycans from complex biological samples, together with linkage-specific sialic acid stabilization. Moreover, SALSA-derivatized glycans can be labeled via reductive amination without causing byproducts such as amide decomposition. This solid-phase SALSA followed by glycan labeling has been successfully applied to human plasma N-glycome profiling.

  2. A simple one pot purification of bacterial amylase from fermented broth based on affinity toward starch-functionalized magnetic nanoparticle.

    PubMed

    Paul, Tanima; Chatterjee, Saptarshi; Bandyopadhyay, Arghya; Chattopadhyay, Dwiptirtha; Basu, Semanti; Sarkar, Keka

    2015-08-18

    Surface-functionalized adsorbant particles in combination with magnetic separation techniques have received considerable attention in recent years. Selective manipulation on such magnetic nanoparticles permits separation with high affinity in the presence of other suspended solids. Amylase is used extensively in food and allied industries. Purification of amylase from bacterial sources is a matter of concern because most of the industrial need for amylase is met by microbial sources. Here we report a simple, cost-effective, one-pot purification technique for bacterial amylase directly from fermented broth of Bacillus megaterium utilizing starch-coated superparamagnetic iron oxide nanoparticles (SPION). SPION was prepared by co-precipitation method and then functionalized by starch coating. The synthesized nanoparticles were characterized by transmission electron microscopy (TEM), a superconducting quantum interference device (SQUID, zeta potential, and ultraviolet-visible (UV-vis) and Fourier-transform infrared (FTIR) spectroscopy. The starch-coated nanoparticles efficiently purified amylase from bacterial fermented broth with 93.22% recovery and 12.57-fold purification. Sodium dodecyl sulfate polyacrylamide gel electrophoresis (SDS-PAGE) revealed that the molecular mass of the purified amylase was 67 kD, and native gel showed the retention of amylase activity even after purification. Optimum pH and temperature of the purified amylase were 7 and 50°C, respectively, and it was stable over a range of 20°C to 50°C. Hence, an improved one-pot bacterial amylase purification method was developed using starch-coated SPION.

  3. Microwave-assisted copper(II)-catalyzed one-pot four-component synthesis of multifunctionalized dihydropyridines.

    PubMed

    Pasunooti, Kalyan Kumar; Nixon Jensen, Chantel; Chai, Hua; Leow, Min Li; Zhang, Da-Wei; Liu, Xue-Wei

    2010-07-12

    A fast and highly efficient copper-catalyzed multicomponent synthesis of 1,4-dihydropyridines under microwave irradiation is described. The protocol utilizes mild reaction conditions with low catalytic loading, leading to high yields. This methodology provides us with biologically active 1,4-dihydropyridine library for medicinal chemistry applications.

  4. Magnetic properties of hard-soft SrFe10Al2O19/Co0.8Ni0.2Fe2O4 ferrite synthesized by one-pot sol-gel auto-combustion

    NASA Astrophysics Data System (ADS)

    Torkian, Shahab; Ghasemi, Ali; Razavi, Reza Shoja

    2016-10-01

    SrFe10Al2O19/Co0.8Ni0.2Fe2O4 hard/soft nanocomposite ferrites with different content of soft phase have been prepared by simple one-pot sol-gel auto-combustion route. X-ray diffraction (XRD), field emission scanning electron microscopy and vibrating ample magnetometer were employed to analysis of structural and magnetic features of synthesized samples. XRD patterns reflect the formation of hard/soft composites of ferrites without the existence of any kind of secondary phases. Narrow size distributions of particles were formed by sol-gel method. Single smooth hysteresis loops of nanocomposites show the presence of exchange coupling between hard and soft phases. Nanocomposite with 15 wt% of soft phase reaches the highest Mr/Ms ratio of 0.63. Compared to the physical mixing of hard/ soft nanocomposites, the one-pot sol-gel auto-combustion method could be considered as a suitable method for synthesizing exchange coupled magnet.

  5. Exfoliated Pd/HNb3O8 nanosheet as highly efficient bifunctional catalyst for one-pot cascade reaction

    NASA Astrophysics Data System (ADS)

    Lee, Nahaeng; Chung, Young-Min

    2016-05-01

    Ultrathin two-dimensional metal oxide nanosheets have drawn attention as potential solid acid catalysts owing to their strong acidity, attributed to the bridged OH groups formed on the nanosheets. In this study, a new class of bifunctional acid-metal catalyst was realized by the deposition of Pd on layered niobium oxide (KNb3O8 and HNb3O8) or its exfoliated nanosheet (Pd/HNb3O8-NS) and applied to one-pot cascade deacetalization and hydrogenation. It was found that the acid strength of the support exerted a large influence not only on the promotion of the first deacetalization step, but also on the acceleration of the subsequent hydrogenation step. Comparative experiments using a series of Pd/HZSM-5 catalysts with different acidities reconfirmed the crucial role of acid strength on hydrogenation. However, the superior catalytic activity of Pd/HNb3O8-NS for hydrogenation compared to that of Pd/HZSM-5 of similar acidity suggests a more efficient ensemble effect of the strong acid sites with the nearby metal sites on the nanosheet surface. Among the catalysts used, Pd/HNb3O8-NS showed the best catalytic performance for one-pot cascade reaction affording the desired product (benzyl alcohol) in approximately 92% yield, which was 7.1 and 1.2 times higher than that of layered Pd/KNb3O8 or Pd/HNb3O8, respectively. The excellent catalytic performance of Pd/HNb3O8-NS may result from the characteristic features of nanosheets: (i) the synergistic cooperation between the bifunctional active sites and (ii) the two-dimensional open surface offering easier access of the reactants to the active sites. Although the use of NaBH4 as hydrogen source was effective in improving the initial reaction performance, the basic nature of NaBH4 adversely resulted in weakening the acid strength of the catalyst, and consequently led to a reduction in catalytic activity.

  6. One-pot synthesis of iniferter-bound polystyrene core nanoparticles for the controlled grafting of multilayer shells

    NASA Astrophysics Data System (ADS)

    Marchyk, Nataliya; Maximilien, Jacqueline; Beyazit, Selim; Haupt, Karsten; Sum Bui, Bernadette Tse

    2014-02-01

    A novel approach using one-pot synthesis for the production of uniform, iniferter-bound polystyrene core nanoparticles of size 30-40 nm is described. Conventional oil-in-water emulsion polymerisation of styrene and divinylbenzene, combining a hybrid initiation system (thermal and UV), triggered sequentially, was employed to form the surface-bound thiocarbamate iniferters in situ. The iniferter cores were then used as seeds for re-initiating further polymerisation by UV irradiation to produce water-compatible core-shell nanoparticles. Grafting of various shell-types is demonstrated: linear polymers of poly(N-isopropylacrylamide) brushes, crosslinked polymers bearing different surface charges and molecularly imprinted polymers. The shell thickness was readily tuned by varying the monomers' concentration and polymerisation time. Our method is straightforward and in addition, gives access to the preparation of fluorescent seeds and the possibility of grafting nanosized multiple shells. The core-shell nanoparticles were fully characterised by dynamic light scattering, transmission electron microscopy, Fourier transform infrared spectroscopy and microelemental analysis.A novel approach using one-pot synthesis for the production of uniform, iniferter-bound polystyrene core nanoparticles of size 30-40 nm is described. Conventional oil-in-water emulsion polymerisation of styrene and divinylbenzene, combining a hybrid initiation system (thermal and UV), triggered sequentially, was employed to form the surface-bound thiocarbamate iniferters in situ. The iniferter cores were then used as seeds for re-initiating further polymerisation by UV irradiation to produce water-compatible core-shell nanoparticles. Grafting of various shell-types is demonstrated: linear polymers of poly(N-isopropylacrylamide) brushes, crosslinked polymers bearing different surface charges and molecularly imprinted polymers. The shell thickness was readily tuned by varying the monomers' concentration and

  7. Cooperative catalysis of noncompatible catalysts through compartmentalization: wacker oxidation and enzymatic reduction in a one-pot process in aqueous media.

    PubMed

    Sato, Hirofumi; Hummel, Werner; Gröger, Harald

    2015-04-07

    A Wacker oxidation using CuCl/PdCl2 as a catalyst system was successfully combined with an enzymatic ketone reduction to convert styrene enantioselectively into 1-phenylethanol in a one-pot process, although the two reactions conducted in aqueous media are not compatible due to enzyme deactivation by Cu ions. The one-pot feasibility was achieved via compartmentalization of the reactions. Conducting the Wacker oxidation in the interior of a polydimethylsiloxane thimble enables diffusion of only the organic substrate and product into the exterior where the biotransformation takes place. Thus, the Cu ions detrimental to the enzyme are withheld from the reaction media of the biotransformation. In this one-pot process, which formally corresponds to an asymmetric hydration of alkenes, a range of 1-arylethanols were formed with high conversions and 98-99 % ee. In addition, the catalyst system of the Wacker oxidation was recycled 15 times without significant decrease in conversion.

  8. Asymmetric Synthesis of Highly Functionalized Tetrahydropyrans via a One-Pot Organocatalytic Michael/Henry/Ketalization Sequence

    PubMed Central

    Hahn, Robert; Raabe, Gerhard; Enders, Dieter

    2015-01-01

    A diastereo- and enantioselective Michael/Henry/ketalization sequence to functionalized tetrahydropyrans is described. The multicomponent cascade reaction uses acetylacetone or β-keto esters, β-nitrostyrenes, and alkynyl aldehydes as substrates affording tetrahydropyrans with five contiguous stereocenters. Employing a bifunctional quinine-based squaramide organocatalyst, the title compounds are obtained in moderate to good yields (27–80%), excellent enantiomeric excesses (93–99% ee), and high diastereomeric ratios (dr > 20:1) after one crystallization. PMID:24971998

  9. Single-step One-pot Synthesis of Graphene Foam/TiO2 Nanosheet Hybrids for Effective Water Treatment

    NASA Astrophysics Data System (ADS)

    Wang, Weilin; Wang, Zhaofeng; Liu, Jingjing; Zhang, Zhengguo; Sun, Luyi

    2017-03-01

    Millions of tons of wastewater containing both inorganic and organic pollutants are generated every day, leading to significant social, environmental, and economic issues. Herein, we designed a graphene foam/TiO2 nanosheet hybrid, which is able to effectively remove both chromium (VI) cations and organic pollutants simultaneously. This graphene foam/TiO2 nanosheet hybrid was synthesized via a facile single-step one-pot hydrothermal method. The structure of the hybrid was characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The hybrid was evaluated for both chromium (VI) and organic pollutants (using methyl blue (MB) as an example) removal, and the removal mechanism was also investigated. During water treatment, graphene and TiO2 nanosheets function complimentarily, leading to a significant synergy. The hybrid exhibited outstanding chromium (VI) and MB removal capacity, much superior to the performance of the individual pure TiO2 sheets or pure graphene foam. The hybrid could also be easily separated after water treatment, and exhibited excellent recycle stability. Considering the very facile synthesis of this graphene foam/TiO2 nanosheet hybrid, and its excellent water treatment performance and recycle stability, such a hybrid is promising for large scale production for practical applications where both chromium (VI) cations and organic dyes are the main pollutants.

  10. Novel hierarchical tantalum oxide-PDMS hybrid coating for medical implants: One pot synthesis, characterization and modulation of fibroblast proliferation.

    PubMed

    Tran, Phong A; Fox, Kate; Tran, Nhiem

    2017-01-01

    Surface properties such as morphology, roughness and charge density have a strong influence on the interaction of biomaterials and cells. Hierarchical materials with a combination of micron/submicron and nanoscale features for coating of medical implants could therefore have significant potential to modulate cellular responses and eventually improve the performance of the implants. In this study, we report a simple, one pot wet chemistry preparation of a hybrid coating system with hierarchical surface structures consisting of polydimethylsiloxane (PDMS) and tantalum oxide. Medical grade, amine functional PDMS was mixed with tantalum ethoxide which subsequently formed Ta2O5in situ through hydrolysis and condensation during coating process. The coatings were characterized by SEM, EDS, XPS, confocal scanning microscopy, contact angle measurement and in vitro cell culture. Varying PDMS and tantalum ethoxide ratios resulted in coatings of different surface textures ranging from smooth to submicro- and nano-structured. Strikingly, hierarchical surfaces containing both microscale (1-1.5μm) and nanoscale (86-163nm) particles were found on coatings synthesized with 20% and 40% (v/v) tantalum ethoxide. The coatings were similar in term of hydrophobicity but showed different surface roughness and chemical composition. Importantly, higher cell proliferation was observed on hybrid surface with hierarchical structures compared to pure PDMS or pure tantalum oxide. The coating process is simple, versatile, carried out under ambient condition and requires no special equipment.

  11. One-Pot Synthesis of Biocompatible CdSe/CdS Quantum Dots and Their Applications as Fluorescent Biological Labels.

    PubMed

    Zhai, Chuanxin; Zhang, Hui; Du, Ning; Chen, Bingdi; Huang, Hai; Wu, Yulian; Yang, Deren

    2011-12-01

    We developed a novel one-pot polyol approach for the synthesis of biocompatible CdSe quantum dots (QDs) using poly(acrylic acid) (PAA) as a capping ligand at 240°C. The morphological and structural characterization confirmed the formation of biocompatible and monodisperse CdSe QDs with several nanometers in size. The encapsulation of CdS thin layers on the surface of CdSe QDs (CdSe/CdS core-shell QDs) was used for passivating the defect emission (650 nm) and enhancing the fluorescent quantum yields up to 30% of band-to-band emission (530-600 nm). Moreover, the PL emission peak of CdSe/CdS core-shell QDs could be tuned from 530 to 600 nm by the size of CdSe core. The as-prepared CdSe/CdS core-shell QDs with small size, well water solubility, good monodispersity, and bright PL emission showed high performance as fluorescent cell labels in vitro. The viability of QDs-labeled 293T cells was evaluated using a 3-(4,5-dimethylthiazol)-2-diphenyltertrazolium bromide (MTT) assay. The results showed the satisfactory (>80%) biocompatibility of as-synthesized PAA-capped QDs at the Cd concentration of 15 μg/ml.

  12. One-pot synthesis of holey MoS2 nanostructures as efficient electrocatalysts for hydrogen evolution

    NASA Astrophysics Data System (ADS)

    Wang, Lanlan; Li, Xuan; Zhang, Jian; Liu, Hongzhong; Jiang, Weitao; Zhao, Hong

    2017-02-01

    In this work, highly porous MoS2 nanostructures have been synthesized via a one-pot and versatile calcination of cyanamide and (NH4)2MoS4 precursors. At first, the thermal polymerization of cyanamide into carbon nitride suppresses the aggregation of MoS2. Then, the thermal decomposition of the formed carbon nitride brings about plentiful pores with a size of 4-70 nm in MoS2 nanostructures, generating an extremely large specific surface area up to 311 m2 g-1. Due to the high specific surface area and abundant exposed edge sites, the resultant porous MoS2 (p-MoS2) nanostructures exhibited outstanding electrochemical hydrogen evolution (HER) activity in a 0.5 M H2SO4 aqueous solution. The onset overpotential and the overpotential at a current density of 10 mA/cm2 were as low as ∼30 mV and ∼130 mV, respectively, which is superior to the previously-reported MoS2-based HER electrocatalysts.

  13. Single-step One-pot Synthesis of Graphene Foam/TiO2 Nanosheet Hybrids for Effective Water Treatment

    PubMed Central

    Wang, Weilin; Wang, Zhaofeng; Liu, Jingjing; Zhang, Zhengguo; Sun, Luyi

    2017-01-01

    Millions of tons of wastewater containing both inorganic and organic pollutants are generated every day, leading to significant social, environmental, and economic issues. Herein, we designed a graphene foam/TiO2 nanosheet hybrid, which is able to effectively remove both chromium (VI) cations and organic pollutants simultaneously. This graphene foam/TiO2 nanosheet hybrid was synthesized via a facile single-step one-pot hydrothermal method. The structure of the hybrid was characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The hybrid was evaluated for both chromium (VI) and organic pollutants (using methyl blue (MB) as an example) removal, and the removal mechanism was also investigated. During water treatment, graphene and TiO2 nanosheets function complimentarily, leading to a significant synergy. The hybrid exhibited outstanding chromium (VI) and MB removal capacity, much superior to the performance of the individual pure TiO2 sheets or pure graphene foam. The hybrid could also be easily separated after water treatment, and exhibited excellent recycle stability. Considering the very facile synthesis of this graphene foam/TiO2 nanosheet hybrid, and its excellent water treatment performance and recycle stability, such a hybrid is promising for large scale production for practical applications where both chromium (VI) cations and organic dyes are the main pollutants. PMID:28251998

  14. Novel Strategy for One-Pot Synthesis of Gold Nanoplates on Carbon Nanotube Sheet As an Effective Flexible SERS Substrate.

    PubMed

    Xin, Wenbo; Yang, Jenn-Ming; Li, Chao; Goorsky, Mark S; Carlson, Larry; De Rosa, Igor M

    2017-02-22

    In this work, we demonstrate a novel route for one-pot synthesis of two-dimensional gold nanoplates (2-D AuNPLs) on carbon nanotube (CNT) sheet. Well-defined AuNPLs are grafted onto CNT sheet via a facile hydrothermal reduction process, during which bromine ions are employed as the surfactant for gold anisotropic growth. Scanning electron microscopy (SEM) shows large-scale AuNPLs with micrometer-scaled length and sub-100 nm thickness are deposited uniformly on the CNT sheet. Transmission electron microscopy (TEM) and X-ray diffraction (XRD) results confirm the synthesized AuNPLs are single-crystalline with preferential {111} orientation. Based on the CNT sheet/AuNPLs hybrid, we have fabricated a flexible surface-enhanced Raman scattering (SERS) substrate, which can effectively detect the analyte Rhodamine 6G (Rh6G) at the concentration as low as 1 × 10(-7) M. The excellent SERS performance of this novel flexible substrate is mainly attributed to nanoscaled gaps between the neighbors, large surface area with roughness, and their sharp edges and corners.

  15. One-pot facile synthesis of branched Ag-ZnO heterojunction nanostructure as highly efficient photocatalytic catalyst

    NASA Astrophysics Data System (ADS)

    Huang, Qingli; Zhang, Qitao; Yuan, Saisai; Zhang, Yongcai; Zhang, Ming

    2015-10-01

    In this paper, the branched Ag-ZnO heterojunction nanostructure and the branched ZnO were synthesized successfully by a facile, green and one-pot hydrothermal method. Such branched heterojunction and the comparing branched pure ZnO were characterized by X-ray diffraction, field emission scanning electron microscopy (FESEM), high resolution transmission electron microscopy (HRTEM), energy-dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), photoluminescence spectroscopy (PL) and UV-vis diffuse reflectance spectra (DRS). The photocatalytic degradation of RhB aqueous solution and acetaldehyde (CH3CHO) gas results both showed that the branched Ag-ZnO heterojunction possessed the enhanced photocatalytic properties in comparison to the branched ZnO and Ag-ZnO counterparts due to its special interface structures and fast separation of its photogenerated charge carriers. This method is simple, feasible and can provide an important clue for synthesis and application of other branched metal/semiconductor heterojunction nanostructures.

  16. Single-step One-pot Synthesis of Graphene Foam/TiO2 Nanosheet Hybrids for Effective Water Treatment.

    PubMed

    Wang, Weilin; Wang, Zhaofeng; Liu, Jingjing; Zhang, Zhengguo; Sun, Luyi

    2017-03-02

    Millions of tons of wastewater containing both inorganic and organic pollutants are generated every day, leading to significant social, environmental, and economic issues. Herein, we designed a graphene foam/TiO2 nanosheet hybrid, which is able to effectively remove both chromium (VI) cations and organic pollutants simultaneously. This graphene foam/TiO2 nanosheet hybrid was synthesized via a facile single-step one-pot hydrothermal method. The structure of the hybrid was characterized by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The hybrid was evaluated for both chromium (VI) and organic pollutants (using methyl blue (MB) as an example) removal, and the removal mechanism was also investigated. During water treatment, graphene and TiO2 nanosheets function complimentarily, leading to a significant synergy. The hybrid exhibited outstanding chromium (VI) and MB removal capacity, much superior to the performance of the individual pure TiO2 sheets or pure graphene foam. The hybrid could also be easily separated after water treatment, and exhibited excellent recycle stability. Considering the very facile synthesis of this graphene foam/TiO2 nanosheet hybrid, and its excellent water treatment performance and recycle stability, such a hybrid is promising for large scale production for practical applications where both chromium (VI) cations and organic dyes are the main pollutants.

  17. One-Pot Green Synthesis of Graphene Nanosheets Encapsulated Gold Nanoparticles for Sensitive and Selective Detection of Dopamine

    NASA Astrophysics Data System (ADS)

    Thirumalraj, Balamurugan; Rajkumar, Chellakannu; Chen, Shen-Ming; Palanisamy, Selvakumar

    2017-01-01

    We report a simple new approach for green preparation of gallic acid supported reduced graphene oxide encapsulated gold nanoparticles (GA-RGO/AuNPs) via one-pot hydrothermal method. The as-prepared composites were successfully characterized by using Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray powder diffraction techniques (XRD), scanning electron microscope (SEM), high resolution transmission electron microscopy (HRTEM) and elemental analysis. The GA-RGO/AuNPs modified electrode behaves as a hybrid electrode material for sensitive and selective detection of dopamine (DA) in presence of ascorbic acid (AA) and uric acid (UA). The GA-RGO/AuNPs modified electrode displays an excellent electrocatalytic activity towards the oxidation of DA and exhibits a wide linear response range over the DA concentrations from 0.01–100.3 μM with a detection limit (LOD) of 2.6 nM based on S/N = 3. In addition, the proposed sensor could be applied for the determination of DA in human serum and urine samples for practical analysis.

  18. One-pot synthesis of linear-hyperbranched amphiphilic block copolymers based on polyglycerol derivatives and their micelles.

    PubMed

    Oikawa, Yurie; Lee, Sueun; Kim, Do Hyung; Kang, Dae Hwan; Kim, Byeong-Su; Saito, Kyohei; Sasaki, Shigeko; Oishi, Yoshiyuki; Shibasaki, Yuji

    2013-07-08

    This paper describes the one-pot synthesis of a polyglycidol (PG)-based polymer, poly(ethoxyethyl glycidyl ether) (PEEGE)-b-[hyperbranched polyglycerol (hbPG)-co-PEEGE]x/y, its micelle formulation, and the ability to encapsulate a model therapeutic molecule. Amphiphilic block copolymers were prepared by the sequential addition of ethoxyethyl glycidyl ether (EEGE) to glycidol. The composition of the block copolymers varied from 62:38 to 92:8. Block copolymers with composition x:y≥66:34 were soluble only in organic solvents. Micelles were formulated by injection of deionized water into a tetrahydrofuran block copolymer solution with or without pyrene as a model hydrophobic molecule. The critical micelle concentration was 18.2-30.9 mg/L, and the micelle size was 100-250 nm. The pyrene-containing micelle rapidly collapsed on acidic exposure, allowing conversion of hydrophobic PEEGE to hydrophilic PG, thus, facilitating the release of the encapsulated pyrene. Cytotoxicity data showed high biocompatibility of PG-based block copolymers, suggesting their potential as a drug delivery carrier.

  19. Continuous, One-pot Synthesis and Post-Synthetic Modification of NanoMOFs Using Droplet Nanoreactors

    NASA Astrophysics Data System (ADS)

    Jambovane, Sachin R.; Nune, Satish K.; Kelly, Ryan T.; McGrail, B. Peter; Wang, Zheming; Nandasiri, Manjula I.; Katipamula, Shanta; Trader, Cameron; Schaef, Herbert T.

    2016-11-01

    Metal-organic frameworks (MOFs); also known as porous coordination polymers (PCP) are a class of porous crystalline materials constructed by connecting metal clusters via organic linkers. The possibility of functionalization leads to virtually infinite MOF designs using generic modular methods. Functionalized MOFs can exhibit interesting physical and chemical properties including accelerated adsorption kinetics and catalysis. Although there are discrete methods to synthesize well-defined nanoscale MOFs, rapid and flexible methods are not available for continuous, one-pot synthesis and post-synthetic modification (functionalization) of MOFs. Here, we show a continuous, scalable nanodroplet-based microfluidic route that not only facilitates the synthesis of MOFs at a nanoscale, but also offers flexibility for direct functionalization with desired functional groups (e.g., -COCH3, fluorescein isothiocyanate; FITC). In addition, the presented route of continuous manufacturing of functionalized nanosized MOFs takes significantly less time compared to state-of-the-art batch methods currently available (1 hr vs. several days). We envisage our approach to be a breakthrough method for synthesizing complex functionalized nanomaterials (metal, metal oxides, quantum dots and MOFs) that are not accessible by direct batch processing and expand the range of a new class of functionalized MOF-based functional nanomaterials.

  20. One-pot synthesis of hollow NiSe-CoSe nanoparticles with improved performance for hybrid supercapacitors

    NASA Astrophysics Data System (ADS)

    Chen, Haichao; Fan, Meiqiang; Li, Chao; Tian, Guanglei; Lv, Chunju; Chen, Da; Shu, Kangying; Jiang, Jianjun

    2016-10-01

    Hollow NiSe-CoSe samples have been synthesized for the first time via a one-pot solvothermal approach. The strategy is robust enough to synthesize NiSe-CoSe nanoparticles with different NiSe to CoSe ratios but with a similar hollow structure. Co ions in the NiSe-CoSe nanoparticles play decisive role for formation of the hollow structure; otherwise, the nanoparticles become solid for the NiSe sample. When used as the positive electroactive materials for energy storage, the NiSe-CoSe samples show excellent electrochemical activity in alkaline electrolyte. Using the synergistic effect between NiSe and CoSe, the electrochemical performance of NiSe-CoSe can be tuned by varying the NiSe to CoSe ratios. The NiSe-CoSe sample with a NiSe to CoSe ratio of 4:2 shows the best electrochemical performance in terms of superior specific capacity, improved rate capability and excellent cycling stability. In addition, the electrochemical performance of NiSe-CoSe sample with a NiSe to CoSe ratio of 4:2 is also evaluated via assembling hybrid supercapacitors with RGO, and the hybrid supercapacitor delivers both high power and energy densities (41.8 Wh kg-1 at 750 W kg-1 and 20.3 Wh kg-1 at 30 kW kg-1).

  1. Sliding over the Blocks in Enzyme-Free RNA Copying – One-Pot Primer Extension in Ice

    PubMed Central

    Löffler, Philipp M. G.; Groen, Joost; Dörr, Mark; Monnard, Pierre-Alain

    2013-01-01

    Template-directed polymerization of RNA in the absence of enzymes is the basis for an information transfer in the ‘RNA-world’ hypothesis and in novel nucleic acid based technology. Previous investigations established that only cytidine rich strands are efficient templates in bulk aqueous solutions while a few specific sequences completely block the extension of hybridized primers. We show that a eutectic water/ice system can support Pb2+/Mg2+-ion catalyzed extension of a primer across such sequences, i.e. AA, AU and AG, in a one-pot synthesis. Using mixtures of imidazole activated nucleotide 5′-monophosphates, the two first “blocking” residues could be passed during template-directed polymerization, i.e., formation of triply extended products containing a high fraction of faithful copies was demonstrated. Across the AG sequence, a mismatch sequence was formed in similar amounts to the correct product due to U·G wobble pairing. Thus, the template-directed extension occurs both across pyrimidine and purine rich sequences and insertions of pyrimidines did not inhibit the subsequent insertions. Products were mainly formed with 2′-5′-phosphodiester linkages, however, the abundance of 3′–5′-linkages was higher than previously reported for pyrimidine insertions. When enzyme-free, template-directed RNA polymerization is performed in a eutectic water ice environment, various intrinsic reaction limitations observed in bulk solution can then be overcome. PMID:24058695

  2. One-pot solventless preparation of PEGylated black phosphorus nanoparticles for photoacoustic imaging and photothermal therapy of cancer.

    PubMed

    Sun, Caixia; Wen, Ling; Zeng, Jianfeng; Wang, Yong; Sun, Qiao; Deng, Lijuan; Zhao, Chongjun; Li, Zhen

    2016-06-01

    Black phosphorus (BP) nanostructures such as nanosheets and nanoparticles have attracted considerable attention in recent years due to their unique properties and great potential in various physical, chemical, and biological fields. In this article, water-soluble and biocompatible PEGylated BP nanoparticles with a high yield were prepared by one-pot solventless high energy mechanical milling technique. The resultant BP nanoparticles can efficiently convert near infrared (NIR) light into heat, and exhibit excellent photostability, which makes them suitable as a novel nanotheranostic agent for photoacoustic (PA) imaging and photothermal therapy of cancer. The in-vitro results demonstrate the excellent biocompatibility of PEGylated BP nanoparticles, which can be used for photothermal ablation of cancer cells under irradiation with NIR light. The in-vivo PA images demonstrate that these BP nanoparticles can be efficiently accumulated in tumors through the enhanced permeability retention effect. The resultant BP nanoparticles can be further utilized for photothermal ablation of tumors by irradiation with NIR light. The tumor-bearing mice were completely recovered after photothermal treatment with BP nanoparticles, in comparison with mice from control groups. Our research highlights the great potential of PEGylated BP nanoparticles in detection and treatment of cancer.

  3. Rapid "one-pot" preparation of polymeric monolith via photo-initiated thiol-acrylate polymerization for capillary liquid chromatography.

    PubMed

    Bai, Jingyao; Wang, Hongwei; Ou, Junjie; Liu, Zhongshan; Shen, Yehua; Zou, Hanfa

    2016-06-21

    A facile approach was exploited for fast preparation of polymer-based monoliths in UV-transparent fused-silica capillaries via "one-pot" photo-initiated thiol-acrylate polymerization reaction of dipentaerythritolpenta-/hexaacrylate (DPEPA) and 1-octadecanethiol (ODT) in the presence of porogenic solvents (1-butanol and ethylene glycol). Due to relative insensitivity of oxygen inhibition in thiol-ene free-radical polymerization, the polymerization could be performed within 5 min. The effects of composition of prepolymerization solution on the morphology and permeability of poly(ODT-co-DPEPA) monoliths were investigated in detail by adjusting the content of monomer and binary porogen ratio. The physical properties of poly(ODT-co-DPEPA) monoliths were characterized by Fourier transform infrared spectroscopy (FT-IR), mercury intrusion porosimetry (MIP) and nitrogen adsorption/desorption measurement. The evaluation of chromatographic performance was carried out by capillary liquid chromatography (cLC). The results indicated that the poly(ODT-co-DPEPA) monolith was homogeneous and permeable, and also possessed a typical reversed-phase retention mechanism in cLC with high efficiency (∼75,000 N m(-1)) for separation of alkylbenzenes. Eventually, the further separation of tryptic digest of proteins by cLC tandem mass spectrometry (cLC-MS/MS) demonstrated its potential in the analysis of biological samples.

  4. Efficient one-pot synthesis of peapod-like hollow carbon nanomaterials for utrahigh drug loading capacity.

    PubMed

    Guo, Jingxin; Zhang, Haijiao; Geng, Hongya; Mi, Xianqiang; Ding, Guoji; Jiao, Zheng

    2015-01-01

    In this paper, peapod-like hollow carbon nanomaterial was fabricated via an efficient one-pot hydrothermal route. The carbon-silica composite was employed as the precursor and cetyltrimethylammonium bromide (CTAB) as the morphology-controlled agent. SEM and TEM results indicated that the carbon shell and the silica core in the precursor were not closely linked but rattle-type structure. After removing the silica template, the obtained carbon product had uniform peapod-like morphology, interconnected pores and high specific surface areas (above 800.0 m(2)/g). We found that CTAB played an important role in the formation of the products with peapod-like morphology. The particle sizes of the hollow carbon nanospheres were readily adjusted by varying the dosage of tetraethoxysilane (TEOS) and the volume ratio of ethanol and water. Based on the experimental results, the formation mechanism of the hollow carbon nanomaterial was also discussed. By virtue of their unique nanostructure and porous properties, the peapod-like hollow carbon nanomaterial exhibited ultrahigh drug loading capacity above 98.4% for doxorubicin hydrochloride (DOX).

  5. One-pot synthesis of magnetite nanorods/graphene composites and its catalytic activity toward electrochemical detection of dopamine.

    PubMed

    Salamon, J; Sathishkumar, Y; Ramachandran, K; Lee, Yang Soo; Yoo, Dong Jin; Kim, Ae Rhan; Gnana Kumar, G

    2015-02-15

    Magnetite (Fe3O4) nanorods anchored over reduced graphene oxide (rGO) were synthesized through a one-pot synthesis method, where the reduction of GO and in-situ generation of Fe3O4 nanorods occurred concurrently. The average head and tail diameter of Fe3O4 nanorods anchored over the rGO matrix are found to be 32 and 11 nm, respectively, and morphology, structure and diameter of bare Fe3O4 nanorods were not altered even after the composite formation with rGO. The increased structural disorders and decrement in the sp(2) domains stimulated the high electrical conductivity and extended catalytic active sites for the prepared rGO/Fe3O4 nanocomposite. The constructed rGO/Fe3O4/GCE sensor exhibited excellent electrocatalytic activity toward the electrooxidation of dopamine (DA) with a quick response time of 6s, a wide linear range between 0.01 and 100.55 µM, high sensitivity of 3.15 µA µM(-1) cm(-2) and a lower detection limit of 7 nM. Furthermore, the fabricated sensor exhibited a practical applicability in the quantification of DA in urine samples with an excellent recovery rate. The excellent electroanalytical performances and straight-forward, surfactant and template free preparation method construct the rGO/Fe3O4 composite as an extremely promising material for the diagnosis of DA related diseases in biomedical applications.

  6. Three-component, one-pot synthesis of anthranilamide Schiff bases bearing 4-aminoquinoline moiety as Mycobacterium tuberculosis gyrase inhibitors.

    PubMed

    Salve, Preeti S; Alegaon, Shankar G; Sriram, Dharmarajan

    2017-02-17

    An efficient three-component, one-pot protocol is described for the synthesis of biologically interesting 2-(benzylideneamino)-N-(7-chloroquinolin-4-yl)benzohydrazide derivatives from isatoic anhydride, 7-chloro-4-hydrazinylquinoline and aromatic and/or hetero aromatic aldehydes under catalyst free condensation by using water as reaction media. All synthesized compounds were evaluated for their antimycobacterial activity against Mycobacterium tuberculosis (MTB) and cytotoxicity activity against normal VERO cell lines. The synthesized compounds exhibited minimum inhibitory concentration (MIC) ranging from 0.78 to 25μM. Among the tested compounds 4c, 4o, 4r, and 4u exhibited promising inhibitory activity (MIC=3.12μM). Compounds 4h and 4i stand out, showing MIC values of 0.78 and 1.56μM respectively. Both compounds were further screened for their Mycobacterium tuberculosis DNA gyrase inhibitory assay which suggested that these compounds have a great potential for further optimization and development as antitubercular agents.

  7. Inspired by efficient cellulose-dissolving system: Facile one-pot synthesis of biomass-based hydrothermal magnetic carbonaceous materials.

    PubMed

    Ma, Jian-Feng; Xing, Jian-Xiong; Wang, Kun; Yang, Hai-Yan; Fei, Ben-Hua; Liu, Xing-E

    2017-05-15

    The core-shell structure of carbon encapsulated magnetic nanoparticles (CEMNs) displays unique properties. Enhancing the magnetization of iron core, in parallel, improving the encapsulation of carbon shell are the two major challenges in the synthesis of CEMNs. Inspired by efficient cellulose-dissolving system, carbon encapsulated magnetic nano-Fe3O4 particles (Fe3O4@C) with ∼10.0nm Fe3O4 cores and 1.9-3.3nm carbon shell, were successfully one-pot synthesized via a novel hydrothermal carbonization (HTC) process. The dissolving process in ionic liquids ([Emim]Ac and [Amim]Cl) completely cleaved the intra- and intermolecular H-bonds in cellulose, and favored the incorporation of Fe3O4 nanoparticles into the cellulose H-bonds systems during the regeneration process. Some stable linkages were formed in Fe3O4@C, taking Fe3O4 nanoparticles as a structure guiding agent. The morphology and properties of Fe3O4@C depended strongly on the type of carbon precursors and pyrolysis temperature. Well encapsulated nanostructure was obtained at HTC temperature 280°C, when [Emim]Ac-treated holocellulose was used as the carbon source. Meanwhile, the thickness of the amorphous shell and magnetization increased with HTC temperature. More importantly, a novel elements for understanding the growth mechanism for the Fe3O4@C composite under HTC conditions was proposed.

  8. One pot electrochemical synthesis of poly(melamine) entrapped gold nanoparticles composite for sensitive and low level detection of catechol.

    PubMed

    Palanisamy, Selvakumar; Ramaraj, Sayee Kannan; Chen, Shen-Ming; Chiu, Te-Wei; Velusamy, Vijayalakshmi; Yang, Thomas C K; Chen, Tse-Wei; Selvam, Sonadevi

    2016-12-29

    A simple and cost effective synthesis of nanomaterials with advanced physical and chemical properties have received much attention to the researchers, and is of interest to the researchers from different disciplines. In the present work, we report a simple and one pot electrochemical synthesis of poly(melamine) entrapped gold nanoparticles (PM-AuNPs) composite. The PM-AuNPs composite was prepared by a single step electrochemical method, wherein the AuNPs and PM were simultaneously fabricated on the electrode surface. The as-prepared materials were characterized by various physicochemical methods. The PM-AuNPs composite modified electrode was used as an electrocatalyst for oxidation of catechol (CC) due to its well-defined redox behavior and enhanced electro-oxidation ability towards CC than other modified electrodes. Under optimized conditions, the differential pulse voltammetry (DPV) was used for the determination of CC. The DPV response of CC was linear over the concentration ranging from 0.5 to 175.5μM with a detection limit of 0.011μM. The PM-AuNPs composite modified electrode exhibits the high selectivity in the presence of range of potentially interfering compounds including dihydroxybenzene isomers. The sensor shows excellent practicality in CC containing water samples, which reveals the potential ability of PM-AuNPs composite modified electrode towards the determination of CC in real samples.

  9. One-pot synthesis of gold nanostars using plant polyphenols for cancer photoacoustic imaging and photothermal therapy

    NASA Astrophysics Data System (ADS)

    Zhang, Xiao-Long; Zheng, Cheng; Zhang, Yun; Yang, Huang-Hao; Liu, Xiaolong; Liu, Jingfeng

    2016-07-01

    Branched plasmonic nanostructures have been found to exhibit strong enhancement of the electromagnetic field surrounding their multi-branched petals. This feature endows them with improved performance in catalysis, surface-enhanced Raman scattering, photoacoustic imaging, and photothermal therapy. Albeit several synthesis techniques have been developed, the precisely controlled growth of highly branched nanostructures with a one-pot surfactant-free procedure is still challenging. Herein, we present a simple seedless route to synthesize gold nanostars (AuNSs) using a natural plant polyphenol, gallic acid (GA), as a reducing and stabilizing agent. The size and shape of AuNSs can be tuned by simply adjusting the amount of added GA. Under the optimum condition, the as-prepared AuNSs with diameters about 100 nm exhibit strong near-infrared absorption, good photothermal efficiency, and high biocompatibility. We demonstrate that AuNSs can be utilized for simultaneous photoacoustic imaging and photothermal therapy in living cancer cells. This study highlights facile synthesized AuNSs could serve as a promising platform for cancer diagnosis and therapy.

  10. In situ one-pot preparation of reduced graphene oxide/polyaniline composite for high-performance electrochemical capacitors

    NASA Astrophysics Data System (ADS)

    Chen, Nali; Ren, Yapeng; Kong, Peipei; Tan, Lin; Feng, Huixia; Luo, Yongchun

    2017-01-01

    Reduced graphene oxide/polyaniline (rGO/PANI) composites are prepared through an effective in situ one-pot synthesis route that includes the reduction of graphene oxide (GO) by aniline under weak alkali condition via hydrothermal method and then followed by in situ polymerization of aniline. X-ray diffraction, Fourier transform infrared spectroscopy, Raman spectroscopy, ultraviolet-visible spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscope and transmission electron microscope are employed to reveal that GO is successfully reduced by aniline under weak alkali condition and PANI can be deposited on the surfaces of reduced graphene oxide (rGO) sheets. The effect of rGO is optimized by tuning the mass ratios of aniline to GO to improve the electrochemical performance of rGO/PANI composites. The maximum specific capacitance of rGO/PANI composites achieves 524.4 F/g with a mass ratio of aniline to GO 10:1 at a current density of 0.5 A/g, in comparison to the specific capacitance of 397 F/g at the same current density of pure PANI. Particularly, the specific capacity retention rate is 81.1% after 2000 cycles at 100 mv/s scan rate, which is an improvement over that of pure PANI (55.5%).

  11. Low cost, surfactant-less, one pot synthesis of Cu{sub 2}O nano-octahedra at room temperature

    SciTech Connect

    Ahmed, Asar; Gajbhiye, Namdeo S.; Joshi, Amish G.

    2011-08-15

    Cu{sub 2}O octahedra were successfully synthesized via a novel wet-chemical method using D-glucose and hydrazine as reducing agent at room temperature without the presence of any other surfactant. Presence of D-glucose was important for the stabilization of the evolved copper octahedra and also for facilitating the reduction of the Cu(II) ions. The existence of glucose moieties on the surface as capping agent was confirmed by the FT-IR spectra while there was presence of excess oxygen atoms on the surface leading to the formation of a thin CuO layer at the octahedra surface, as confirmed by the XPS study, probably promoted by the capping glucose. Effect of NaOH concentration on the reaction and the formation of octahedra was also studied. The formation mechanism of obtained Cu{sub 2}O octahedra has been discussed. These octahedra were then studied for their photocatalytic properties in degradation of organic dyes, rhodamine B and methyl orange. - Graphical abstract: Cu{sub 2}O octahedra were found to have thin layer of CuO, due to oxidation of surface Cu{sup +} atoms by the surfactant O atoms. Highlights: > Simple and inexpensive one pot synthesis of various Cu{sub 2}O nanostructures. > Surface properties studied by XPS. > Used as photocatalysis for degradation of rhodamine B.

  12. One-pot, green synthesis of gold nanoparticles by gelatin and investigation of their biological effects on Osteoblast cells.

    PubMed

    Suarasan, Sorina; Focsan, Monica; Soritau, Olga; Maniu, Dana; Astilean, Simion

    2015-08-01

    It is useful to find new methods to synthesize and, more importantly, to control the size and shape of gold nanoparticles (AuNPs) without using relatively toxic-reducing agents and surfactants. In this work, we present a one-pot, green synthesis of AuNPs taking the advantage of gelatin biopolymer to operate as unique reducing, growth controlling and stabilizing agent in aqueous solution of tetrachloroauric acid (HAuCl4) at temperatures above its melting point (∼35°C). The shape and size of AuNPs were found to be strongly influenced by the gelatin concentration (0.5-5%), while the growth rate of AuNPs is controlled by temperature of synthesis (40-80°C) and viscosity of the biopolymer. A specific class of gelatin-coated AuNPs was selected to investigate its stability in simulated physiological conditions and cellular media and subsequently to evaluate the in vitro biocompatibility and capacity to sustain proliferation and differentiation of Osteoblast cells. Dark-field microscopy and Rayleigh scattering spectra prove a more efficient internalization of gelatin-coated AuNPs as compared with citrate-coated AuNPs, while methylthiazoltetrazolium bromide (MTT) assay demonstrates enhanced cell proliferation. Interestingly, in the presence of gelatin-coated AuNPs, we find out a first sign of Osteoblast cells differentiation with bone nodules formation, as confirmed by alkaline phosphatase (ALP) activity assay.

  13. One-Pot Hydrothermal Synthesis of Magnetite Prussian Blue Nano-Composites and Their Application to Fabricate Glucose Biosensor

    PubMed Central

    Jomma, Ezzaldeen Younes; Ding, Shou-Nian

    2016-01-01

    In this work, we presented a simple method to synthesize magnetite Prussian blue nano-composites (Fe3O4-PB) through one-pot hydrothermal process. Subsequently, the obtained nano-composites were used to fabricate a facile and effective glucose biosensor. The obtained nanoparticles were characterized using transmission electron microscopy, scanning electron microscopy, Fourier-transform infrared spectroscopy, UV-vis absorbance spectroscopy, cyclic voltammetry and chronoamperometry. The resultant Fe3O4-PB nanocomposites have magnetic properties which could easily controlled by an external magnetic field and the electro-catalysis of hydrogen peroxide. Thus, a glucose biosensor based on Fe3O4-PB was successfully fabricated. The biosensor showed super-electrochemical properties toward glucose detection exhibiting fast response time within 3 to 4 s, low detection limit of 0.5 µM and wide linear range from 5 µM to 1.2 mM with sensitivity of 32 µA∙mM−1∙cm−2 and good long-term stability. PMID:26901204

  14. One-pot synthesis of carbon dots-embedded molecularly imprinted polymer for specific recognition of sterigmatocystin in grains.

    PubMed

    Xu, Longhua; Fang, Guozhen; Pan, Mingfei; Wang, Xuefeng; Wang, Shuo

    2016-03-15

    A novel sensitive fluorescent sensor for determination of sterigmatocystin (ST), which was based on carbon dots-embedded molecularly imprinted polymer (CDs@MIP), was prepared by an efficient one-pot reaction. First, highly blue luminescent CDs were synthesized via a one-step reaction. Then, through a non-hydrolytic sol-gel process, MIP was formed on the CDs surface in the presence of 1,8-dihydroxyanthraquinone as an alternative template molecule to obtain CDs@MIP. The CDs acted as antennas for signal amplification and optical readout, and the MIP coated on the CDs surface provided specific binding sites for ST. The performance of CDs@MIP was compared with that of CDs embedded in non-imprinted polymer (CDs@NIP). CDs@MIP exhibited high selectivity and sensitivity toward ST. Under optimized conditions, the relative fluorescence intensity of CDs@MIP decreased linearly with the concentration of ST from 0.05 to 2.0 mgL(-1) with a detection limit of 0.019 mgL(-1) (S/N=3) and the precision for five replicate detections of 0.10 mgL(-1) ST was 2.31%. The sensor was also used to determine the content of ST in grains with satisfactory results.

  15. One-Pot Green Synthesis of Graphene Nanosheets Encapsulated Gold Nanoparticles for Sensitive and Selective Detection of Dopamine

    PubMed Central

    Thirumalraj, Balamurugan; Rajkumar, Chellakannu; Chen, Shen-Ming; Palanisamy, Selvakumar

    2017-01-01

    We report a simple new approach for green preparation of gallic acid supported reduced graphene oxide encapsulated gold nanoparticles (GA-RGO/AuNPs) via one-pot hydrothermal method. The as-prepared composites were successfully characterized by using Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy, X-ray powder diffraction techniques (XRD), scanning electron microscope (SEM), high resolution transmission electron microscopy (HRTEM) and elemental analysis. The GA-RGO/AuNPs modified electrode behaves as a hybrid electrode material for sensitive and selective detection of dopamine (DA) in presence of ascorbic acid (AA) and uric acid (UA). The GA-RGO/AuNPs modified electrode displays an excellent electrocatalytic activity towards the oxidation of DA and exhibits a wide linear response range over the DA concentrations from 0.01–100.3 μM with a detection limit (LOD) of 2.6 nM based on S/N = 3. In addition, the proposed sensor could be applied for the determination of DA in human serum and urine samples for practical analysis. PMID:28128225

  16. One-pot DNA construction for synthetic biology: the Modular Overlap-Directed Assembly with Linkers (MODAL) strategy

    PubMed Central

    Casini, Arturo; MacDonald, James T.; Jonghe, Joachim De; Christodoulou, Georgia; Freemont, Paul S.; Baldwin, Geoff S.; Ellis, Tom

    2014-01-01

    Overlap-directed DNA assembly methods allow multiple DNA parts to be assembled together in one reaction. These methods, which rely on sequence homology between the ends of DNA parts, have become widely adopted in synthetic biology, despite being incompatible with a key principle of engineering: modularity. To answer this, we present MODAL: a Modular Overlap-Directed Assembly with Linkers strategy that brings modularity to overlap-directed methods, allowing assembly of an initial set of DNA parts into a variety of arrangements in one-pot reactions. MODAL is accompanied by a custom software tool that designs overlap linkers to guide assembly, allowing parts to be assembled in any specified order and orientation. The in silico design of synthetic orthogonal overlapping junctions allows for much greater efficiency in DNA assembly for a variety of different methods compared with using non-designed sequence. In tests with three different assembly technologies, the MODAL strategy gives assembly of both yeast and bacterial plasmids, composed of up to five DNA parts in the kilobase range with efficiencies of between 75 and 100%. It also seamlessly allows mutagenesis to be performed on any specified DNA parts during the process, allowing the one-step creation of construct libraries valuable for synthetic biology applications. PMID:24153110

  17. Facile one-pot synthesis of uniform TiO2-Ag hybrid hollow spheres with enhanced photocatalytic activity.

    PubMed

    Wang, Sunli; Qian, Huanhuan; Hu, Yong; Dai, Wei; Zhong, Yijun; Chen, Jiafu; Hu, Xiao

    2013-01-28

    TiO(2)-Ag hybrid hollow spheres (about 700 nm in diameter) with a highly uniform morphology and good structural stability were facilely prepared via a one-pot hydrothermal method, using carbon spheres as templates followed by an annealing treatment. Through this route, the as-prepared hybrid hollow spheres preserved the uniformity of the initial carbon sphere templates and the loading amount of the Ag nanocrystals can be conveniently varied or controlled by the concentration of the Ag precursor. The investigation of the photocatalytic ability demonstrated that the as-prepared TiO(2)-Ag hybrid hollow spheres possess excellent photocatalytic activity, superior to commercial TiO(2) nanoparticles (Degussa P25), for the degradation of rhodamine B (RhB) and methyl orange (MO) dyes under visible-light illumination. Furthermore, the ˙OH radicals formed during photocatalysis with different Ag content hybrids were revealed by means of a terephthalic acid fluorescence probe method, which uncovers that the Ag content in the TiO(2)-Ag hybrids was crucial to obtain an optimal synergistic effect between the Ag and TiO(2) for the degradation of organic pollutants. Accordingly, the optimum matching for the best photocatalytic activity was investigated thoroughly and a reasonable mechanism was also proposed.

  18. One-pot deposition of palladium on hybrid TiO2 nanoparticles and catalytic applications in hydrogenation.

    PubMed

    Mehri, Afef; Kochkar, Hafedh; Daniele, Stéphane; Mendez, Violaine; Ghorbel, Abdelhamid; Berhault, Gilles

    2012-03-01

    One-pot deposition of Pd onto TiO(2) has been achieved through directly contacting palladium(II) salt with nanosized functionalized TiO(2) support initially obtained by sol-gel process using titanium isopropoxide and citric acid. Citrate groups act as functional moieties able to directly reduce the Pd salt avoiding any further reducing treatment. Various palladium salts (Na(2)PdCl(4) and Pd(NH(3))(4)Cl(2)·H(2)O) and titanium to citrate (Ti/CA) ratios (20, 50, and 100) were used in order to study the effect of the nature of the precursor and of the citrate content on the final Pd particle size and catalytic properties of the as-obtained Pd/TiO(2) systems. Characterization was performed using N(2) adsorption-desorption isotherms, ICP-AES, FTIR, XRD, XPS, and TEM. The as-obtained hybrid Pd/TiO(2) catalysts were tested in the selective hydrogenation (HYD) of an α,β-unsaturated aldehyde, i.e. cinnamaldehyde. Citrate-free Pd/TiO(2)-based catalysts present lower selectivity into saturated alcohol. However, citrate-functionalized Pd/TiO(2) catalyst seems to control the selectivity, the particle size and dispersion of Pd NPs leading to high intrinsic activity.

  19. One-Pot Reductive 1,3-Dipolar Cycloaddition of Secondary Amides: A Two-Step Transformation of Primary Amides.

    PubMed

    Huang, Pei-Qiang; Lang, Qi-Wei; Hu, Xiu-Ning

    2016-11-04

    The one-pot reductive 1,3-dipolar cycloaddition of secondary aromatic N-(trimethylsilylmethyl)amides with reactive dipolarophiles is reported. The method relies on the in situ generation of nonstabilized NH azomethine ylide dipoles via amide activation with triflic anhydride, partial reduction with 1,1,3,3-tetramethyldisiloxane (TMDS), and desilylation with cesium fluoride (CsF). Running under mild conditions, the reaction tolerated several sensitive functional groups and provided cycloadducts in 71-93% yields. The use of less reactive dipolarophile methyl acrylate led to the cycloadduct in only 40% yield. A (Z) geometric intermediate of NH-azomethine 1,3-dipole was postulated to account for the observed higher yields and higher cis diastereoselectivity for the substrates bearing an electron-withdrawing group. This model features an unconventional cyclic transition state via carbanion-aryl ring interaction. Because the starting secondary amides can be prepared from common primary amides, the current method also constitutes a two-step transformation of primary amides.

  20. One-pot synthesis of hierarchical Cu2O/Cu hollow microspheres with enhanced visible-light photocatalytic activity

    NASA Astrophysics Data System (ADS)

    Hong, Tianjie; Tao, Feifei; Lin, Jiudong; Ding, Wei; Lan, Mingxuan

    2015-08-01

    The hierarchical Cu2O/Cu hollow microspheres have been fabricated by the one-pot solvothermal redox method, which is one-step approach without any surfactant and template. By using the HRTEM, XRD, XPS and UV-vis spectroscopy, the as-prepared product is composed of Cu2O and Cu with energy band gap of 1.72 eV. Based on the time-dependent experiments, the content of Cu2O and Cu compositions can be effectively controlled by adjusting the reaction time and a possible mechanism is proposed. In addition, using various dye molecules to stimulate pollutants, the hierarchical Cu2O/Cu hollow microspheres reacted for 8 h exhibit excellent visible-light photocatalytic activities, which is much higher than those of the Cu2O/Cu catalysts formed at the shorter reaction time, commercial Cu2O powder and the mixture of alone Cu2O and Cu. This enhanced photocatalytic performance makes these hierarchical Cu2O/Cu hollow microspheres a kind of efficient visible-light photocatalyst in removing some organic compounds in wastewater.

  1. One-Pot Synthesis of Fe3O4@PS@P(AEMH-FITC) Magnetic Fluorescent Nanocomposites for Bimodal Imaging.

    PubMed

    Wang, Xuandong; Liu, Huiyu; Jun, Ren; Fu, Changhui; Li, Linlin; Li, Tianlong; Tang, Fangqiong; Meng, Xianwei

    2016-03-01

    Magnetic fluorescent nanocomposites have attracted much attention because of their merging magnetic and fluorescent properties for biomedical application. However, the procedure of synthesis of magnetic fluorescent nanocomposites is always complicated. In addition, the properties of fluorescent component could be easily influenced by magnetic component, retaining both of the magnetic and fluorescent properties into one single nanoparticle considered to be a significant challenge. Herein, we report one-pot method to synthesize multifunctional magnetic fluorescent Fe3O4@PS@P(AEMH-FITC) nanocomposites for bimodal imaging. The asprepared Fe3O4@PS@P(AEMH-FITC) nanocomposites with well-define spherical core/shell structure were stable properties. Moreover, the Fe3O4@PS@P(AEMH-FITC) nanocomposites displayed efficient fluorescent and magnetic properties, respectively. Meanwhile, the magnetic resonance imaging (MRI) and HePG2 cancer cell fluorescent images experiment results suggested that Fe3O4@PS@P(AEMH-FITC) nanocomposites could be used as MRI contrast agents and Fluorescence Imaging (FLI) agents for bioimaging application. Our investigation paves a facile avenue for synthesized magnetic fluorescent nanostructures with well biocompatibility for potential bioimaging application in MRI and FLI.

  2. One-pot green synthesis of graphene oxide/gold nanocomposites as SERS substrates for malachite green detection.

    PubMed

    Fu, Wen Liang; Zhen, Shu Jun; Huang, Cheng Zhi

    2013-05-21

    In this contribution, graphene oxide/gold nanoparticle (GO/AuNPs) hybrids were in situ fabricated through a green one-pot procedure by using tyrosine as an environment friendly and biocompatible reducing agent, which can be used as highly efficient surface enhanced Raman scattering (SERS) substrates with the enhancement factor at 3.8 × 10(3). The as-prepared GO/AuNPs hybrids have good biocompatibility, providing the prospect of applications for biomedicine determinations. In addition, taking the advantages of the electromagnetic and chemical enhancement mechanism and the high affinity of GO and AuNPs towards positive dyes, a sensitive, selective and label-free malachite green (MG) detection method was demonstrated. The SERS measurement showed that the minimum detection concentration of MG in water was as low as 2.5 μmol L(-1) with a linear response range from 2.5 to 100 μmol L(-1) (R(2) = 0.996). Moreover, this method can be applied to detect MG in a fishery water sample with satisfactory results.

  3. Continuous, One-pot Synthesis and Post-Synthetic Modification of NanoMOFs Using Droplet Nanoreactors

    PubMed Central

    Jambovane, Sachin R.; Nune, Satish K.; Kelly, Ryan T.; McGrail, B. Peter; Wang, Zheming; Nandasiri, Manjula I.; Katipamula, Shanta; Trader, Cameron; Schaef, Herbert T.

    2016-01-01

    Metal-organic frameworks (MOFs); also known as porous coordination polymers (PCP) are a class of porous crystalline materials constructed by connecting metal clusters via organic linkers. The possibility of functionalization leads to virtually infinite MOF designs using generic modular methods. Functionalized MOFs can exhibit interesting physical and chemical properties including accelerated adsorption kinetics and catalysis. Although there are discrete methods to synthesize well-defined nanoscale MOFs, rapid and flexible methods are not available for continuous, one-pot synthesis and post-synthetic modification (functionalization) of MOFs. Here, we show a continuous, scalable nanodroplet-based microfluidic route that not only facilitates the synthesis of MOFs at a nanoscale, but also offers flexibility for direct functionalization with desired functional groups (e.g., -COCH3, fluorescein isothiocyanate; FITC). In addition, the presented route of continuous manufacturing of functionalized nanosized MOFs takes significantly less time compared to state-of-the-art batch methods currently available (1 hr vs. several days). We envisage our approach to be a breakthrough method for synthesizing complex functionalized nanomaterials (metal, metal oxides, quantum dots and MOFs) that are not accessible by direct batch processing and expand the range of a new class of functionalized MOF-based functional nanomaterials. PMID:27821866

  4. One-pot template-free synthesis of porous CdMoO4 microspheres and their enhanced photocatalytic activity

    NASA Astrophysics Data System (ADS)

    Madhusudan, Puttaswamy; Zhang, Jinfeng; Yu, Jiaguo; Cheng, Bei; Xu, Difa; Zhang, Jun

    2016-11-01

    The optical and catalytic performances of materials strongly depend on their size, morphology, dimensionality and structure. Herein, we demonstrate a facile one-pot template free synthesis of hierarchical CdMoO4 porous microspheres via a simple low temperature oil bath method. The photoactivity of the as-prepared samples was evaluated by photocatalytic decolorization of Methyl Orange (MO) and Methylene Blue (MB) mixed dye aqueous solutions at ambient temperature under full solar spectrum. The results indicated that the concentration of ammonium molybdate and reaction time greatly influence the diameter, average crystallite size, specific surface area, pore structure and photocatalytic activity of the prepared samples. Especially, under the suitable conditions the prepared hierarchical CdMoO porous microspheres exhibited enhanced photocatalytic activity and high stability. Furthermore, it is found that the photocatalytic activity and formation rate of hydroxyl radicals greatly depend on the particle sizes and morphology of as-prepared samples. This work not only demonstrates a simple way to fabricate the hierarchical CdMoO4 porous microspheres but also shows a possibility for utilization of CdMoO4 porous microspheres for the photocatalytic treatment of waste water pollutants.

  5. One-pot synthesis of γ-MnS/reduced graphene oxide with enhanced performance for aqueous asymmetric supercapacitors

    NASA Astrophysics Data System (ADS)

    Zhang, Guanggao; Kong, Menglai; Yao, Yadong; Long, Lu; Yan, Minglei; Liao, Xiaoming; Yin, Guangfu; Huang, Zhongbing; Asiri, Abdullah M.; Sun, Xuping

    2017-02-01

    In this work, γ-MnS/reduced graphene oxide composites (γ-MnS/rGO) were prepared using a facile one-pot hydrothermal method. As an electrode material for supercapacitors, the γ-MnS/rGO-60 composite obtained under dosages of graphene oxide was 60 mg and exhibited an enhanced specific capacitance of 547.6 F g-1 at a current density of 1 A g-1, and outstanding rate capability (65% capacitance retention at 20 A g-1), with superior cycling stability and electrochemical reversibility. An asymmetric supercapacitor assembled from γ-MnS/rGO-60 composite and rGO (γ-MnS/rGO-60//rGO) showed a voltage window of 0-1.6 V and delivered a high energy density of 23.1 W h kg-1 at a power density of 798.8 W kg-1, and 15.9 W h kg-1 at 4.5 kW kg-1. Moreover, two such 1.0 × 1.0 cm2 devices connected together in series easily light up a group of LED lights, showing its potential practical application as an attractive energy storage device.

  6. One-pot template-free preparation of mesoporous TiO{sub 2} hollow spheres and their photocatalytic activity

    SciTech Connect

    Kang, Shizhao; Yin, Dieer; Li, Xiangqing; Li, Liang; Mu, Jin

    2012-11-15

    Highlights: ► Mesoporous TiO{sub 2} hollow spheres were prepared in a one-pot process. ► The process does not involve any templates and surfactants. ► The TiO{sub 2} hollow spheres display high photocatalytic activity. -- Abstract: Mesoporous TiO{sub 2} hollow spheres were prepared in a solvothermal process, which did not involve any templates and surfactants. Meanwhile, the photocatalytic activity of TiO{sub 2} hollow spheres was studied using methyl orange as a probe. The results indicate that the anatase TiO{sub 2} hollow spheres with mesoporous walls and high specific surface area (141 m{sup 2} g{sup −1}) can be obtained using this simple method. The mean diameter and wall thickness of spheres are about 700 nm and 90 nm, respectively. Moreover, the as-prepared TiO{sub 2} hollow spheres display high photocatalytic activity with 98% of degradation ratio of methyl orange after 30 min irradiation.

  7. One-pot green fabrication and antibacterial activity of thermally stable corn-like CNC/Ag nanocomposites

    NASA Astrophysics Data System (ADS)

    Yu, Hou-Yong; Qin, Zong-Yi; Sun, Bin; Yan, Chen Feng; Yao, Ju-Ming

    2014-01-01

    Corn-like cellulose nanocrystals/silver (CNC/Ag) nanocomposites were prepared by formic acid/hydrochloric acid hydrolysis of commercial microcrystalline cellulose (MCC), and redox reaction with silver ammonia aqueous solution (Ag(NH3)2(OH)) in one-pot green synthesis, in which the preparation and modification of CNCs were performed simultaneously and the resultant modified CNCs could be as reducing, stabilizing and supporting agents for silver nanoparticles. The influences of the Ag+ ion concentrations on the morphology, microstructure, and properties of the CNC/Ag nanocomposites were investigated. It is found that corn-like CNC/Ag nanocomposites containing Ag nanoparticles with diameter of about 20-40 nm were obtained. Compared to the MCCs, high crystallinity of 88.5 % and the maximum degradation temperature ( T max) of 364.5 °C can be achieved. Moreover, the CNC/Ag nanocomposites showed strong antibacterial activity against both Gram-negative Escherichia coli and Gram-positive Staphylococcus aureus. Furthermore, such nanocomposites can act as bifunctional nanofillers to improve thermal stability, mechanical property, and antibacterial activity of commercial poly(3-hydroxybutyrate-co-3-hydroxyvalerate) and poly(lactic acid).

  8. Electrolyte-added one-pot synthesis for producing monodisperse, micrometer-sized silica particles up to 7 microm.

    PubMed

    Nakabayashi, Hiroyuki; Yamada, Akira; Noba, Masahiro; Kobayashi, Yoshio; Konno, Mikio; Nagao, Daisuke

    2010-05-18

    A facile one-pot synthesis to produce micrometer-sized silica particles with low polydispersity was examined in a semibatch process where an ethanol solution of tetraethyl orthosilicate (TEOS) was continuously supplied to another ethanol solution of water and ammonia containing an electrolyte of LiCl, NaCl, or KCl. Supply rates of the TEOS solution was ranged with the water and electrolyte concentrations, which indicated that the addition of KCl at a low water concentration was effective to increase size of silica particles in a micrometer range. Highly monodisperse silica particles with an average size of 6.6 microm were successfully produced at 3 mol/m(3) KCl and 5 kmol/m(3) water. The efficiency of KCl addition for producing the large particles is interpreted by the previously proposed nucleation and growth mechanism that expects rapid particle coagulation in early reaction stage for particles which have reduced surface potential by the adsorption of cations with a large ionic radius. It is confirmed from competitive growth reactions that the silica particle growth follows the reaction-limited mechanism even in the semibatch process.

  9. One-pot inimer promoted ROCP synthesis of branched copolyesters using α-hydroxy-γ-butyrolactone as the branching reagent.

    PubMed

    Hua, Geng; Franzén, Johan; Odelius, Karin

    2016-07-01

    An array of branched poly(ɛ-caprolactone)s was successfully synthesized using an one-pot inimer promoted ring-opening multibranching copolymerization (ROCP) reaction. The biorenewable, commercially available yet unexploited comonomer and initiator 2-hydroxy-γ-butyrolactone was chosen as the inimer to extend the use of 5-membered lactones to branched structures and simultaneously avoiding the typical tedious work involved in the inimer preparation. Reactions were carried out both in bulk and in solution using stannous octoate (Sn(Oct)2) as the catalyst. Polymerizations with inimer equivalents varying from 0.01 to 0.2 were conducted which resulted in polymers with a degree of branching ranging from 0.049 to 0.124. Detailed ROCP kinetics of different inimer systems were compared to illustrate the branch formation mechanism. The resulting polymer structures were confirmed by (1)H, (13)C, and 1H-13C HSQC NMR and SEC (RI detector and triple detectors). The thermal properties of polymers with different degree of branching were investigated by DSC, confirming the branch formation. Through this work, we have extended the current use of the non-homopolymerizable γ-butyrolactone to the branched polymers and thoroughly examined its behaviors in ROCP. © 2016 The Authors. Journal of Polymer Science Part A: Polymer Chemistry Published by Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2016, 54, 1908-1918.

  10. Continuous, One-pot Synthesis and Post-Synthetic Modification of NanoMOFs Using Droplet Nanoreactors

    SciTech Connect

    Jambovane, Sachin R.; Nune, Satish K.; Kelly, Ryan T.; McGrail, B. Peter; Wang, Zheming; Nandasiri, Manjula I.; Katipamula, Shanta; Trader, Cameron; Schaef, Herbert T.

    2016-11-08

    Metal-organic frameworks (MOFs); also known as porous coordination polymers (PCP) are a class of porous crystalline materials constructed by connecting metal clusters via organic linkers. The possibility of functionalization leads to virtually infinite MOF designs using generic modular methods. Functionalized MOFs can exhibit interesting physical and chemical properties including accelerated adsorption kinetics and catalysis. Although there are discrete methods to synthesize well-defined nanoscale MOFs, rapid and flexible methods are not available for continuous, one-pot synthesis and post synthesis modification (functionalization) of MOFs. Here, we show a continuous, scalable nanodroplet-based microfluidic route that not only facilitates the synthesis of MOFs at nanoscale, but also offers flexibility for direct functionalization with desired functional groups (e.g., -NH2, -COCH3, fluorescein isothiocyanate; FITC). In addition, the presented route of continuous manufacturing of functionalized MOFs takes significantly less time compared to state-of-the-art batch methods currently available (1 hr vs. several days). We envisage our approach to be a breakthrough method for synthesizing complex functionalized nanomaterials (metal, metal oxides, quantum dots and MOFs) that are not accessible by direct batch processing, and expand the range of a new class of functionalized MOF-based functional nanomaterials.

  11. Sequential and one-pot reactions of phenols with bromoalkynes for the synthesis of (Z)-2-bromovinyl phenyl ethers and benzo[b]furans.

    PubMed

    Wang, Shihua; Li, Pinhua; Yu, Lin; Wang, Lei

    2011-11-18

    Benzo[b]furans were prepared in one pot based on the addition/palladium-catalyzed C-H bond functionalization of phenols with bromoalkynes. The addition reactions of phenols to bromoalkynes generated (Z)-2-bromovinyl phenyl ethers in high yields with excellent regio- and stereoselectivity. The obtained (Z)-2-bromovinyl phenyl ethers subsequently proceeded by intramolecular cyclization to afford 2-substituted benzo[b]furans in good yields through palladium-catalyzed direct C-H bond functionalizations. It is important to note that the transformation of phenols with bromoalkynes into benzo[b]furans could be carried out in one pot with a simple and efficient tandem procedure.

  12. Facile synthesis of brush poly(phosphoamidate)s via one-pot tandem ring-opening metathesis polymerization and atom transfer radical polymerization.

    PubMed

    Ding, Liang; Qiu, Jun; Wei, Jun; Zhu, Zhenshu

    2014-09-01

    Poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA)-based brush poly(phosphoamidate)s are successfully synthesized by a combination of ring-opening metathesis polymerization (ROMP) and atom transfer radical polymerization (ATRP) following either a commutative two-step procedure or a straightforward one-pot process using Grubbs ruthenium-based catalysts for tandem catalysis. Compared with the traditional polymerization method, combining ROMP and ATRP in a one-pot process allows the preparation of brush copolymers characterized by a relatively moderate molecular weight distribution and quantitative conversion of monomer. Moreover, the surface morphologies and aggregation behaviors of these polymers are studied by AFM and TEM measurements.

  13. Catalyst-free synthesis of skipped dienes from phosphorus ylides, allylic carbonates, and aldehydes via a one-pot SN2' allylation-Wittig strategy.

    PubMed

    Xu, Silong; Zhu, Shaoying; Shang, Jian; Zhang, Junjie; Tang, Yuhai; Dou, Jianwei

    2014-04-18

    A catalyst-free allylic alkylation of stabilized phosphorus ylides with allylic carbonates via a regioselective SN2' process is presented. Subsequent one-pot Wittig reaction with both aliphatic and aromatic aldehydes as well as ketenes provides structurally diverse skipped dienes (1,4-dienes) in generally high yields and moderate to excellent stereoselectivity with flexible substituent patterns. This one-pot SN2' allylation-Wittig strategy constitutes a convenient and efficient synthetic method for highly functionalized skipped dienes from readily available starting materials.

  14. Protein-directed one-pot synthesis of Ag microspheres with good biocompatibility and enhancement of radiation effects on gastric cancer cells

    NASA Astrophysics Data System (ADS)

    Huang, Peng; Yang, Da-Peng; Zhang, Chunlei; Lin, Jing; He, Meng; Bao, Le; Cui, Daxiang

    2011-09-01

    Biocompatible Ag@BSA microspheres were successfully synthesized via one-pot reaction in aqueous phase at room temperature by using BSA as soft templates. The individual Ag microsphere is composed of nanoscale Ag assemblies and shows enhanced radiation effects on gastric cancer cells.Biocompatible Ag@BSA microspheres were successfully synthesized via one-pot reaction in aqueous phase at room temperature by using BSA as soft templates. The individual Ag microsphere is composed of nanoscale Ag assemblies and shows enhanced radiation effects on gastric cancer cells. Electronic supplementary information (ESI) available. See DOI: 10.1039/c1nr10586h

  15. One-Pot Trimetallic Relay Catalysis: A Unified Approach for the Synthesis of β-Carbolines and Other [c]-Fused Pyridines.

    PubMed

    Dhiman, Seema; Mishra, Uttam K; Ramasastry, S S V

    2016-06-27

    A divergent strategy is presented for the synthesis of 1,3-di- and 1,3,4-trisubstituted β-carbolines through an unprecedented one-pot triple-orthogonal-metal relay catalysis, and 1,3-disubstituted 4-hydroxy-β-carbolines through a one-pot bimetallic relay catalysis from readily accessible 3-(2-aminophenyl)-5-hexenyn-3-ols. These strategies were elaborated to enable the synthesis of benzofuro[2,3-c]pyridines, benzothieno[2,3-c]pyridines, and isoquinolines, which otherwise require multistep synthesis.

  16. A one-pot method for the selective conversion of hemicellulose from crop waste into C5 sugars and furfural by using solid acid catalysts.

    PubMed

    Sahu, Ramakanta; Dhepe, Paresh Laxmikant

    2012-04-01

    We present a solid-acid catalyzed one-pot method for the selective conversion of solid hemicellulose without its separation from other lignocellulosic components, such as cellulose and lignin. The reactions were carried out in aqueous and biphasic media to yield xylose, arabinose, and furfural. To overcome the drawbacks posed by mineral acid methods in converting hemicelllulose, we used heterogeneous catalysts that work at neutral pH. In a batch reactor, these heterogeneous catalysts, such as solid acids (zeolites, clays, metal oxides etc.), resulted in >90 % conversion of hemicellulose. It has been shown that the selectivity for the products can be tuned by changing the reaction conditions, for example, a reaction carried out in water at 170 °C for 1 h with HBeta (Si/Al=19) and HUSY (Si/Al=15) catalysts gave yields of 62 and 56 % for xylose and arabinose, respectively. With increased reaction time (6 h) and in presence of only water, HUSY resulted in yields of 30 % xylose + arabinose and 18 % furfural. However, in a biphasic reaction system (water + p-xylene, 170 °C, 6 h) yields of 56 % furfural with 17 % xylose+arabinose could be achieved. It was shown that with the addition of organic solvent the furfural yield could be increased from 18 to 56 %. Under optimized reaction conditions, >90 % carbon balance was observed. The study revealed that catalysts were recyclable with a 20 % drop in activity for each subsequent run. It was observed that temperature, pressure, reaction time, substrate to catalyst ratio, solvent, and so forth had an effect on product formation. The catalysts were characterized by means of X-ray diffraction, temperature-programmed desorption of NH(3), inductively coupled plasma spectroscopy, elemental analysis, and solid-state NMR ((29)Si, (27)Al) spectroscopy techniques.

  17. One-pot system for synthesis, assembly, and display of functional single-span membrane proteins on oil-water interfaces.

    PubMed

    Yunker, Peter J; Asahara, Haruichi; Hung, Kuo-Chan; Landry, Corey; Arriaga, Laura R; Akartuna, Ilke; Heyman, John; Chong, Shaorong; Weitz, David A

    2016-01-19

    Single-span membrane proteins (ssMPs) represent approximately one-half of all membrane proteins and play important roles in cellular communications. However, like all membrane proteins, ssMPs are prone to misfolding and aggregation because of the hydrophobicity of transmembrane helices, making them difficult to study using common aqueous solution-based approaches. Detergents and membrane mimetics can solubilize membrane proteins but do not always result in proper folding and functionality. Here, we use cell-free protein synthesis in the presence of oil drops to create a one-pot system for the synthesis, assembly, and display of functional ssMPs. Our studies suggest that oil drops prevent aggregation of some in vitro-synthesized ssMPs by allowing these ssMPs to localize on oil surfaces. We speculate that oil drops may provide a hydrophobic interior for cotranslational insertion of the transmembrane helices and a fluidic surface for proper assembly and display of the ectodomains. These functionalized oil drop surfaces could mimic cell surfaces and allow ssMPs to interact with cell surface receptors under an environment closest to cell-cell communication. Using this approach, we showed that apoptosis-inducing human transmembrane proteins, FasL and TRAIL, synthesized and displayed on oil drops induce apoptosis of cultured tumor cells. In addition, we take advantage of hydrophobic interactions of transmembrane helices to manipulate the assembly of ssMPs and create artificial clusters on oil drop surfaces. Thus, by coupling protein synthesis with self-assembly at the water-oil interface, we create a platform that can use recombinant ssMPs to communicate with cells.

  18. One pot synthesis of CdS/TiO{sub 2} hetero-nanostructures for enhanced H{sub 2} production from water and removal of pollutants from aqueous streams

    SciTech Connect

    Mani, A. Daya; Subrahmanyam, Ch.

    2016-01-15

    Highlights: • Novel one pot synthesis of CdS/TiO{sub 2} hetero nanostructures by combustion synthesis. • Excellent visible light photocatalytic activity for H{sub 2} production from water. • Enhanced activity for the removal of Cr(VI) from aqueous streams. - Abstract: To achieve more effective coupling of cadmium sulfide (CdS) to the TiO{sub 2}, single step synthesis of CdS/TiO{sub 2} composites is advantageous. In the present study a novel one pot synthesis of several CdS/TiO{sub 2} hetero-nanostructures was explored through combustion technique. As the process involves the simultaneous nucleation of CdS and TiO{sub 2} it leads to the proper connectivity between the constituent materials. All the catalysts were characterized by using several techniques and the excellent visible light activity of the composites has been asserted by the H{sub 2} production from water containing sacrificial reagents, removal of methylene blue and Cr(VI) from aqueous streams. Therefore the present synthetic strategy which is devoid of using molecular linker at interface is more suitable for solar applications, which require faster rates of electron transfer at the hetero junctions.

  19. Multi-Component Protein - Protein Docking Based Protocol with External Scoring for Modeling Dimers of G Protein-Coupled Receptors.

    PubMed

    Kaczor, Agnieszka A; Guixà-González, Ramon; Carrió, Pau; Poso, Antti; Dove, Stefan; Pastor, Manuel; Selent, Jana

    2015-04-01

    In order to apply structure-based drug design techniques to GPCR complexes, it is essential to model their 3D structure. For this purpose, a multi-component protocol was derived based on protein-protein docking which generates populations of dimers compatible with membrane integration, considering all reasonable interfaces. At the next stage, we applied a scoring procedure based on up to eleven different parameters including shape or electrostatics complementarity. Two methods of consensus scoring were performed: (i) average scores of 100 best scored dimers with respect to each interface, and (ii) frequencies of interfaces among 100 best scored dimers. In general, our multi-component protocol gives correct indications for dimer interfaces that have been observed in X-ray crystal structures of GPCR dimers (opsin dimer, chemokine CXCR4 and CCR5 dimers, κ opioid receptor dimer, β1 adrenergic receptor dimer and smoothened receptor dimer) but also suggests alternative dimerization interfaces. Interestingly, at times these alternative interfaces are scored higher than the experimentally observed ones suggesting them to be also relevant in the life cycle of studied GPCR dimers. Further results indicate that GPCR dimer and higher-order oligomer formation may involve transmembrane helices (TMs) TM1-TM2-TM7, TM3-TM4-TM5 or TM4-TM5-TM6 but not TM1-TM2-TM3 or TM2-TM3-TM4 which is in general agreement with available experimental and computational data.

  20. Au-ZnO hybrid nanoflowers, nanomultipods and nanopyramids: one-pot reaction synthesis and photocatalytic properties

    NASA Astrophysics Data System (ADS)

    Chen, Yuanzhi; Zeng, Deqian; Zhang, Kun; Lu, Aolin; Wang, Laisen; Peng, Dong-Liang

    2013-12-01

    The preparation of noble metal-semiconductor hybrid nanocrystals with controlled morphologies has received intensive interest in recent years. In this study, facile one-pot reactions have been developed for the synthesis of Au-ZnO hybrid nanocrystals with different interesting morphologies, including petal-like and urchin-like nanoflowers, nanomultipods and nanopyramids. In the synthesis strategy, oleylamine-containing solution serves as the reaction medium, and the in situ generated Au seeds play an important role in the subsequently induced growth of ZnO nanocrystals. With the aid of several surfactants, hybrid nanocrystals with different morphologies that have considerable influences on their optical and photocatalytic activities are readily achieved. Through high-resolution transmission electron microscopy measurements, an observed common orientation relationship between ZnO and Au is that ZnO nanocrystals prefer to grow with their polar {001} facets on the {111} facets of Au nanocrystals, and well-defined interfaces are evident. Surface plasmon resonance bands of Au with different positions are observed in the UV-vis spectra, and the UV and visible emissions of ZnO are found to be dramatically reduced. Finally, the as-prepared Au-ZnO nanocrystals exhibit excellent photocatalytic activity for the photodegradation of rhodamine B compared with pure ZnO nanocrystals. The Au-ZnO hybrid nanopyramids show the highest catalytic efficiency, which is correlated with the exposed crystal facets, crystallinity and the formation of hybrid nanostructures. The as-prepared Au-ZnO hybrid nanocrystals are expected to find diverse potential applications in the fields such as photocatalysis, solar energy conversion, sensing and biological detection.The preparation of noble metal-semiconductor hybrid nanocrystals with controlled morphologies has received intensive interest in recent years. In this study, facile one-pot reactions have been developed for the synthesis of Au

  1. One-pot one-cluster synthesis of fluorescent and bio-compatible Ag14 nanoclusters for cancer cell imaging

    NASA Astrophysics Data System (ADS)

    Yang, Jie; Xia, Nan; Wang, Xinan; Liu, Xianhu; Xu, An; Wu, Zhikun; Luo, Zhixun

    2015-11-01

    Small-molecule-protected silver nanoclusters have smaller hydrodynamic diameter, and thus may hold greater potential in biomedicine application compared with the same core-sized, macromolecule (i.e. DNA)-protected silver nanoclusters. However, the live cell imaging labeled by small-molecule-protected silver nanoclusters has not been reported until now, and the synthesis and atom-precise characterization of silver nanoclusters have been challenging for a long time. We develop a one-pot one-cluster synthesis method to prepare silver nanoclusters capped with GSH which is bio-compatible. The as-prepared silver nanoclusters are identified to be Ag14(SG)11 (abbreviated as Ag14, SG: glutathione) by isotope-resolvable ESI-MS. The structure is probed by 1D NMR spectroscopy together with 2D COSY and HSQC. This cluster species is fluorescent and the fluorescence quantum yield is solvent-dependent. Very importantly, Ag14 was successfully applied to label lung cancer cells (A549) for imaging, and this work represents the first attempt to image live cells with small-molecule-protected silver nanoclusters. Furthermore, it is revealed that the Ag14 nanoclusters exhibit lower cytotoxicity compared with some other silver species (including silver salt, silver complex and large silver nanoparticles), and the explanation is also provided. The comparison of silver nanoclusters to state-of-the-art labeling materials in terms of cytotoxicity and photobleaching lifetime is also conducted.Small-molecule-protected silver nanoclusters have smaller hydrodynamic diameter, and thus may hold greater potential in biomedicine application compared with the same core-sized, macromolecule (i.e. DNA)-protected silver nanoclusters. However, the live cell imaging labeled by small-molecule-protected silver nanoclusters has not been reported until now, and the synthesis and atom-precise characterization of silver nanoclusters have been challenging for a long time. We develop a one-pot one

  2. One-pot preparation of new copolymer electrolytes with tunable network structure for all-solid-state lithium battery

    NASA Astrophysics Data System (ADS)

    Chen, Bo; Xu, Qiang; Huang, Zhen; Zhao, Yanran; Chen, Shaojie; Xu, Xiaoxiong

    2016-11-01

    A new class of copolymer electrolytes with tunable network structure is successfully designed and prepared via a facile one-pot reaction. The trimethylolpropane triglycidyl ether (TMPEG) is cross-linked with poly (ethylene glycol) diamine (NPEG) to create well-defined solid network polymer electrolyte (SNPE). The network structure could be tuned by changing the molar ratio of TMPEG and NPEG or the molecular weight of NPEG. The effects of molecular weight of NPEG and molar ratio of EO/Li+ on the ionic conductivity are systematically investigated. The optimal electrolyte TMPEG-NPEG4K[2:1]-16:1 presents a maximum conductivity of 1.10 × 10-4 S cm-1 under 30 °C, and an 18-fold ionic conductivity enhancement in that of PEO-based electrolyte. Furthermore, it also exhibits wide electrochemical window (0-5.4 V), excellent compatibility with metallic Li, and superior mechanical properties. The all-solid-state lithium batteries LiFePO4/Li are assembled with TMPEG-NPEG4K[2:1]-16:1 electrolyte, and present good cycling and rate performance under 60 °C. The initial discharge specific capacities of the batteries are 161.7 mAh g-1 at 0.2 C and 132.7 mAh g-1 at 1 C, and the capacity retention ratio can be retained at 90.6% and 90.5% after 100 cycles. This new copolymer electrolyte may become a promising candidate for applications in all-solid-state lithium battery.

  3. One-pot solvothermal synthesis of dual-phase titanate/titania Nanoparticles and their adsorption and photocatalytic Performances

    SciTech Connect

    Cheng, Yu Hua; Gong, Dangguo; Tang, Yuxin; Ho, Jeffery Weng Chye; Tay, Yee Yan; Lau, Wei Siew; Wijaya, Olivia; Lim, Jiexiang; Chen, Zhong

    2014-06-01

    Dual phase titanate/titania nanoparticles undergo phase transformation gradually with the increase of solvothermal synthesis temperature from 100 °C to 200 °C, and eventually are fully transformed into anatase TiO{sub 2}. The crystal structure change results in the changes of optical absorption, sensitizer/dopant formation and surface area of the materials which finally affect the overall dye removal ability. Reactions under dark and light have been conducted to distinguish the contributions of surface adsorption from photocatalytic degradation. The sample synthesized at 160 °C (S160) shows the best performances for both adsorption under dark and photocatalytic degradation of methylene blue (MB) under visible light irradiation. The adsorption mechanism for S160 is determined as monolayer adsorption based on the adsorption isotherm test under dark condition, and an impressive adsorption capacity of 162.19 mg/g is achieved. For the photocatalytic application, this sample at 0.1 g/L loading is also able to degrade 20 ppm MB within 6 hours under the visible light (>420 nm) condition. - Graphical abstract: The effect of solvothermal synthesis temperature on the formation and dye removal performance of dual phase titanate/titania nanoparticles was unveiled and optimized. - Highlights: • Low temperature one-pot solvothermal synthesis of dual-phase photocatalysts. • Correlation of the synthesis temperature is made with the phase composition. • Adsorption isotherm, kinetics, photocatalytic degradation were studied. • Synthesis at 160 °C yields the best material for adsorption of MB in dark. • The same sample also shows the best visible light degradation of MB.

  4. An efficient route for annulation of pyrimidines to steroids and non-steroids via a base catalyzed one-pot three component reaction.

    PubMed

    Saikia, Pallabi; Gogoi, Shyamalee; Gogoi, Sanjib; Boruah, Romesh C

    2014-10-01

    A facile strategy for the synthesis of steroidal A- and D-ring fused pyrimidines has been accomplished in high yields via a one-pot reaction of steroidal ketones, aromatic aldehydes and amidine derivatives in presence of potassium tert-butoxide in refluxing ethanol. The generality of the reaction was also extended to non-steroidal ketones.

  5. A Robust, "One-Pot" Method for Acquiring Kinetic Data for Hammett Plots Used to Demonstrate Transmission of Substituent Effects in Reactions of Aromatic Ethyl Esters

    ERIC Educational Resources Information Center

    Yau, Hon Man; Haines, Ronald S.; Harper, Jason B.

    2015-01-01

    A "one-pot" method for acquiring kinetic data for the reactions of a series of substituted aromatic esters with potassium hydroxide using [supserscript 13]C NMR spectroscopy is described, which provides an efficient way to obtain sufficient data to demonstrate the Hammett equation in undergraduate laboratories. The method is…

  6. Greener and rapid access to bio-active heterocycles: one-pot solvent-free synthesis of 1,3,4-oxadiazoles and 1,3,4-thiadiazoles

    EPA Science Inventory

    A novel one-pot solvent free synthesis of 1,3,4-oxadiazoles and 1,3,4-thiadiazoles by condensation of acid hydrazide and triethyl orthoalkanates under microwave irradiations is reported. This green protocol was catalyzed efficiently by solid supported Nafion®NR50 and phosphorus p...

  7. One-pot synthesis of 1,4-disubstituted pyrazoles from arylglycines via copper-catalyzed sydnone-alkyne cycloaddition reaction.

    PubMed

    Specklin, Simon; Decuypere, Elodie; Plougastel, Lucie; Aliani, Soifia; Taran, Frédéric

    2014-08-15

    A robust method for constructing 1,4-pyrazoles from arylglycines was developed using the copper-catalyzed sydnone-alkyne cycloaddition reaction. The procedure offers a straightforward and general route to the pyrazole heterocycle through a three-step one-pot procedure.

  8. Initiator and Photocatalyst-Free Visible Light Induced One-Pot Reaction: Concurrent RAFT Polymerization and CuAAC Click Reaction.

    PubMed

    Wang, Jie; Wang, Xinbo; Xue, Wentao; Chen, Gaojian; Zhang, Weidong; Zhu, Xiulin

    2016-05-01

    A new, visible light-catalyzed, one-pot and one-step reaction is successfully employed to design well-controlled side-chain functionalized polymers, by the combination of ambient temperature revisible addtion-fragmentation chain transfer (RAFT) polymerization and click chemistry. Polymerizations are well controlled in a living way under the irradiation of visible light-emitting diode (LED) light without photocatalyst and initiator, using the trithiocarbonate agent as iniferter (initiator-transfer agent-terminator) agent at ambient temperature. Fourier transfer infrared spectroscopy (FT-IR), NMR, and matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF-MS) data confirm the successful one-pot reaction. Compared to the reported zero-valent metal-catalyzed one-pot reaction, the polymerization rate is much faster than that of the click reaction, and the visible light-catalyzed one-pot reaction can be freely and easily regulated by turning on and off the light.

  9. TANDEM BIS-ALDOL REACTION OF KETONES: A FACILE ONE-POT SYNTHESIS OF 1,3-DIOXANES IN AQUEOUS MEDIUM

    EPA Science Inventory

    A novel tandem bis-aldol reaction of ketone with paraformaldehyde catalyzed by polystyrenesulfonic acid in aqueous medium delivers 1,3-dioxanes in high yield. This one pot, operationally simple microwave-assisted synthetic protocol proceeds efficiently in water in the absence of ...

  10. Successively recycle waste as catalyst: a one-pot Wittig/1,4-reduction/Paal-Knorr sequence for modular synthesis of substituted furans.

    PubMed

    Chen, Long; Du, Yi; Zeng, Xing-Ping; Shi, Tao-Da; Zhou, Feng; Zhou, Jian

    2015-03-20

    A one-pot tandem Wittig/conjugate reduction/Paal-Knorr reaction is reported for the synthesis of di- or trisubstituted furans. This novel sequence first demonstrates the possibility of successively recycling waste from upstream steps to catalyze downstream reactions.

  11. A new one-pot three-component synthesis of 2,4-diamino-5H-chromeno[2,3-b]pyridine-3-carbonitrile derivatives.

    PubMed

    Shaabani, Ahmad; Hajishaabanha, Fatemeh; Mofakham, Hamid; Maleki, Ali

    2010-02-01

    In this study, a three-component one-pot synthesis of new 2,4-diamino-5H-chromeno[2,3-b]pyridine-3-carbonitriles derived from 2-amino-1,1,3-tricyanopropene, salicylic aldehydes and secondary cyclic amines is reported. The reaction is conducted in ethanol at ambient temperature in good-to-excellent yields.

  12. A one-pot synthesis of 1,6,9,13-tetraoxadispiro(4.2.4.2)tetradecane by hydrodeoxygenation of xylose using a palladium catalyst

    Technology Transfer Automated Retrieval System (TEKTRAN)

    In an effort to expand the number of biobased chemicals available from sugars, xylose has been converted to 1,6,9,13-tetraoxadispiro(4.2.4.2)tetradecane in a one-pot reaction using palladium supported on silica-alumina as the catalyst. The title compound is produced in 35-40% yield under 7 MPa H2 pr...

  13. One-Pot Synthesis of Polysubstituted Spirofluorene-Indene via Ru(II)-Catalyzed [3 + 2] Annulation and Intramolecular Friedel-Crafts Cyclization.

    PubMed

    Zhu, Yu-Qin; Dong, Lin

    2015-10-16

    Ru(II)-catalyzed one-pot synthesis of polysubstituted spirofluorene-indenes via [3 + 2] annulation and then intramolecular Friedel-Crafts alkylation has been achieved. The simple method provides a broad scope of aryl ketones and internal alkynes, achieving PAHs skeletons in moderate to good yields.

  14. Synthesis of fluorous and nonfluorous polycyclic systems by one-pot, double intramolecular 1,3-dipolar cycloaddition of azomethine ylides.

    PubMed

    Zhang, Wei; Lu, Yimin; Geib, Steven

    2005-05-26

    [reaction: see text]. Under microwave irradiation, a one-pot, double intramolecular [3 + 2]-cycloaddition reaction of azomethine ylides leads to formation of a novel hexacyclic ring system. The major diastereomer is isolated, and its stereochemistry is determined by X-ray crystal structure analysis.

  15. Consecutive condensation, C-N and N-N bond formations: a copper- catalyzed one-pot three-component synthesis of 2H-indazole.

    PubMed

    Kumar, Manian Rajesh; Park, Ahbyeol; Park, Namjin; Lee, Sunwoo

    2011-07-01

    2H-Indazoles are synthesized using copper-catalyzed, one-pot, three-component reactions of 2-bromobenzaldehydes, primary amines, and sodium azide. A copper catalyst plays the key role in the formation of C-N and N-N bonds. This method has a broad substrate scope with a high tolerance for a variety of functional groups.

  16. Heterogeneous asymmetric Henry-Michael one-pot reaction synergically catalyzed by grafted chiral bases and inherent achiral hydroxyls on mesoporous silica surface.

    PubMed

    Yang, Shanshan; He, Jing

    2012-10-25

    Highly efficient and enantioselective asymmetric Henry-Michael one-pot reaction has been achieved on bifunctional heterogeneous catalysts with inherent achiral hydroxyls as acidic sites and immobilized chiral amines as basic sites. Final products were afforded in yields of up to 85% and ee of 99%.

  17. One-pot preparation of trifluoromethylated homoallylic N-acylhydrazines or α-methylene-γ-lactams from acylhydrazines, trifluoroacetaldehyde methyl hemiacetal, allyl bromide and tin.

    PubMed

    Du, Ganggang; Huang, Danfeng; Wang, Ke-Hu; Chen, Xiaowei; Xu, Yanli; Ma, Junyan; Su, Yingpeng; Fu, Ying; Hu, Yulai

    2016-01-28

    An efficient and convenient one-pot method for the preparation of trifluoromethylated homoallylic N-acylhydrazines or α-methylene-γ-lactams has been described. In this process, allyl bromide and metal tin are used instead of toxic stannanes, and commercially available aqueous trifluoroacetaldehyde methyl hemiacetal was used as a trifluoromethyl source.

  18. Multicomponent membranes

    DOEpatents

    Kulprathipanja, Santi; Kulkarni, Sudhir S.; Funk, Edward W.

    1988-01-01

    A multicomponent membrane which may be used for separating various components which are present in a fluid feed mixture comprises a mixture of a plasticizer such as a glycol and an organic polymer cast upon a porous organic polymer support. The membrane may be prepared by casting an emulsion or a solution of the plasticizer and polymer on the porous support, evaporating the solvent and recovering the membrane after curing.

  19. Facile one-pot formulation of TRAIL-embedded paclitaxel-bound albumin nanoparticles for the treatment of pancreatic cancer.

    PubMed

    Min, Sun Young; Byeon, Hyeong Jun; Lee, Changkyu; Seo, Jisoo; Lee, Eun Seong; Shin, Beom Soo; Choi, Han-Gon; Lee, Kang Choon; Youn, Yu Seok

    2015-10-15

    Nanoparticle albumin-bound (nab™) technology is an effective way of delivering hydrophobic chemotherapeutics. We developed a one-pot/one-step formulation of paclitaxel (PTX)-bound albumin nanoparticles with embedded tumor necrosis factor-related apoptosis-inducing ligand (TRAIL/PTX HSA-NP) for the treatment of pancreatic cancer. TRAIL/PTX HSA-NPs were fabricated using a high-pressure homogenizer at a TRAIL feeding ratio of 0.2%, 1.0%, and 2.0%. TRAIL/PTX HSA-NPs were spherical and became larger in size (170-230 nm) with increasing TRAIL amount (0.2-2.0%). The loading efficiencies of PTX were in the range of ∼86.4% and significantly low at 2.0% TRAIL (60.4%). Specifically, the inhibitory concentrations (IC50) of TRAIL (1.0 or 2.0%)/PTX HSA-NPs were >20-fold lower than that of plain PTX-HSA NP (0.032±0.06, 0.022±0.005, and 0.96±0.15 ng/ml, respectively) in pancreatic Mia Paca-2 cells. Considering TRAIL loading, bioactivity, and particle size, TRAIL(1.0%)/PTX HSA-NPs were determined as the optimal candidate for further studies. TRAIL(1.0%)/PTX HSA-NPs displayed substantially greater apoptotic activity than plain PTX HSA-NP in both FACS and TUNEL analysis. The loaded PTX and TRAIL were gradually released from the TRAIL(1.0%)/PTX HSA-NPs until ∼24 h, which is considered to be a sufficient time for delivery to the tumor tissue. TRAIL(1.0%)/PTX HSA-NP displayed markedly more antitumor efficacy than plain PTX HSA-NP in Mia Paca-2 cell-xenografted mice in terms of tumor volume (size) and weight (213.9 mm(3) and 0.18 g vs. 1126.8 mm(3) and 0.80 g, respectively). These improved in vitro and in vivo performances were due to the combined synergistic effects of PTX and TRAIL. We believe that this TRAIL/PTX HSA-NP would have potential as a novel apoptosis-based anticancer agent.

  20. In situ one-pot preparation of superparamagnetic hydrophilic porous microspheres for covalently immobilizing penicillin G acylase to synthesize amoxicillin

    NASA Astrophysics Data System (ADS)

    Xue, Ping; Gu, Yaohua; Su, Weiguang; Shuai, Huihui; Wang, Julan

    2016-01-01

    Magnetic hydrophilic porous microspheres were successfully one-pot synthesized for the first time via in situ inverse suspension polymerization of glycidyl methacrylate, N,N‧-methylene bisacrylamide and 2-hydroxyethyl methacrylate in the presence of Fe3+ and Fe2+ dispersed in formamide, which were denoted as magnetic Fe3O4-GMH microspheres. The morphology and properties of magnetic Fe3O4-GMH microspheres were characterized by SEM, VSM, XRD, FTIR, and so on. The formamide content had an important influence on the morphology of Fe3O4-GMH, and nearly perfectly spherical Fe3O4-GMH particles were formed when the amount of formamide was 15 ml. The diameters of the microspheres were in the range of 100-200 μm and Fe3O4-GMH exhibited superparamagnetic behavior with the saturation magnetization of 5.44 emu/g. The specific surface area of microspheres was 138.7 m2/g, the average pore diameter and pore volume were 15.1 nm and 0.60 cm3/g, respectively. The content of oxirane groups on Fe3O4-GMH was 0.40 mmol/g. After penicillin G acylase (PGA) was covalently immobilized on Fe3O4-GMH microspheres, the catalytic performance for amoxicillin synthesis by 6-aminopenicillanic acid and D-hydroxyphenylglycine methyl ester was largely improved. As a result, 90.1% amoxicillin yield and 1.18 of the synthesis/hydrolysis (S/H) ratio were achieved on PGA/Fe3O4-GMH with ethylene glycol as solvent, but only 62.6% amoxicillin yield and 0.37 of the S/H ratio were obtained on free PGA under the same reaction conditions. Furthermore, the amoxicillin yield and S/H ratio were still kept at 88.2% and 1.06, respectively after the immobilized PGA was magnetically separated and recycled for 10 times, indicating that PGA/Fe3O4-GMH had a very good reusability.

  1. Selective One-Pot Production of High-Grade Diesel-Range Alkanes from Furfural and 2-Methylfuran over Pd/NbOPO4.

    PubMed

    Xia, Qineng; Xia, Yinjiang; Xi, Jinxu; Liu, Xiaohui; Zhang, Yongguang; Guo, Yong; Wang, Yanqin

    2017-02-22

    A one-pot method for the selective production of high-grade diesel-range alkanes from biomass-derived furfural and 2-methylfuran (2-MF) was developed by combining the hydroxyalkylation/alkylation (HAA) condensation of furfural with 2-MF and the subsequent hydrodeoxygenation (HDO) over a multifunctional Pd/NbOPO4 catalyst. The effects of various reaction conditions as well as a variety of solid-acid catalysts and metal-loaded NbOPO4 catalysts were systematically investigated to optimize the reaction conditions for both reactions. Under the optimal reaction conditions up to 89.1 % total yield of diesel-range alkanes was obtained from furfural and 2-MF by this one-pot method.

  2. One-Pot Synthesis of Organic-Sulfur-Zinc Hybrid Materials via Polycondensation of a Zinc Salt and Thiols Generated in Situ from Cyclic Dithiocarbonates.

    PubMed

    Ochiai, Bungo; Konta, Hirohisa

    2015-08-17

    Soluble organic-sulfur-zinc hybrid polymers were prepared via a one-pot reaction consisting of ring-opening addition and subsequent polycondensation. The first reaction is the nucleophilic ring-opening addition of 2-ethylhexylamine to multifunctional cyclic dithiocarbonates giving multiple thiols in situ. The sequential polycondensation of the in situ generated thiols with Zn(OAc)2 gave the target hybrid polymers. This one-pot method enabled the use of a shorter amine than the previous polycondensation of Zn(OAc)2 and purified thiols, which required octadecylamine to obtain a soluble product. The obtained hybrid polymers may be cast as composite films with polystyrene and poly(methyl methacrylate). Owing to the shorter alkyl chain, the calculated nD values of the products (1.60 or 1.61) are higher than that of the previous product bearing octadecyl chains (1.53).

  3. Excellent performance of one-pot synthesized Cu-SSZ-13 catalyst for the selective catalytic reduction of NOx with NH3.

    PubMed

    Xie, Lijuan; Liu, Fudong; Ren, Limin; Shi, Xiaoyan; Xiao, Feng-Shou; He, Hong

    2014-01-01

    Cu-SSZ-13 samples prepared by a novel one-pot synthesis method achieved excellent NH3-SCR performance and high N2 selectivity from 150 to 550 °C after ion exchange treatments. The selected Cu3.8-SSZ-13 catalyst was highly resistant to large space velocity (800 000 h(-1)) and also maintained high NOx conversion in the presence of CO2, H2O, and C3H6 in the simulated diesel exhaust. Isolated Cu(2+) ions located in three different sites were responsible for its excellent NH3-SCR activity. Primary results suggest that the one-pot synthesized Cu-SSZ-13 catalyst is a promising candidate as an NH3-SCR catalyst for the NOx abatement from diesel vehicles.

  4. One-pot synthesis of reverse type-I In2O3@In2S3 core-shell nanoparticles.

    PubMed

    Sun, Zhaoyong; Kumbhar, Amar; Sun, Kai; Liu, Qingsheng; Fang, Jiye

    2008-04-28

    A novel method to one-pot-synthesize high-quality In(2)O(3)@In(2)S(3) core-shell nanoparticles, consisting of a step of reducing In(2)O(3) core surface into a layer of active indium metal in high-temperature organic solution and a step of converting this layer to In(2)S(3) using CS(2), has been developed.

  5. Direct, one-pot reductive alkylation of anilines with functionalized acetals mediated by triethylsilane and TFA. Straightforward route for unsymmetrically substituted ethylenediamine.

    PubMed

    Righi, Marika; Bedini, Annalida; Piersanti, Giovanni; Romagnoli, Federica; Spadoni, Gilberto

    2011-01-21

    A new, robust, and reliable method has been developed for the selective reductive N-alkylation of primary and secondary aromatic amines with some functionalized acetals using TFA/Et(3)SiH as a reagent combination. A variety of unsymmetrically substituted ethylenediamines can be synthesized in a one-pot procedure in excellent yields at room temperature. This new procedure offers significant advantages over previous synthetic approaches, including brevity, mild reaction conditions, excellent yields, and high functional group tolerance.

  6. Asymmetric synthesis of functionalized cyclohexanes bearing five stereocenters via a one-pot organocatalytic Michael-Michael-1,2-addition sequence.

    PubMed

    Chauhan, Pankaj; Urbanietz, Gregor; Raabe, Gerhard; Enders, Dieter

    2014-07-04

    A highly stereoselective one-pot procedure involving an enantioselective Michael addition promoted by low loading of an amino-squaramide catalyst followed by an achiral base catalyzed domino Michael-Knoevenagel-type 1,2-addition sequence provides efficient access to fully substituted cyclohexanes bearing five contiguous stereogenic centers in good yields (68-86%) and excellent stereoselectivities (>30 : 1 dr and 96-99% ee).

  7. Asymmetric organocatalyzed Michael addition of nitromethane to a 2-oxoindoline-3-ylidene acetaldehyde and the three one-pot sequential synthesis of (-)-horsfiline and (-)-coerulescine.

    PubMed

    Mukaiyama, Takasuke; Ogata, Kento; Sato, Itaru; Hayashi, Yujiro

    2014-10-13

    (-)-Horsfiline and (-)-coerulescine were synthesized through three one-pot operations in 33 and 46% overall yield, respectively. Key to the success was the efficient use of a diarylprolinol silyl ether to catalyze the asymmetric Michael addition of nitromethane to a 2-oxoindoline-3-ylidene acetaldehyde. This allowed the all-carbon quaternary, spirocyclic carbon stereocenter to be constructed in good yield with excellent enantioselectivity.

  8. One-pot stereoselective synthesis of α,β-differentiated diamino esters via the sequence of aminochlorination, aziridination and intermolecular SN2 reaction.

    PubMed

    Xiong, Yiwen; Qian, Ping; Cao, Chenhui; Mei, Haibo; Han, Jianlin; Li, Guigen; Pan, Yi

    2014-01-01

    We report here an efficient one-pot method for the synthesis of α,β-differentiated diamino esters directly from cinnamate esters using N,N-dichloro-p-toluenesulfonamide and benzylamine as nitrogen sources. The key transformations include a Cu-catalyzed aminohalogenation and aziridination, followed by an intermolecular SN2 nucleophilic ring opening by benzylamine. The reactions feature a wide scope of substrates and proceed with excellent stereo- and regioselectivity (anti:syn >99:1) .

  9. Zeolitic imidazolate framework-8 (ZIF-8) as a sacrificial template: one-pot synthesis of hollow poly(dopamine) nanocapsules and yolk-structured poly(dopamine) nanocomposites

    NASA Astrophysics Data System (ADS)

    Ran, Jingyu; Xiao, Lihua; Wu, Weidang; Liu, Yike; Qiu, Wei; Wu, Jianming

    2017-02-01

    Hollow poly(dopamine) (PDA) nanocapsules and yolk-structured PDA nanocomposites were prepared by an aqueous one-pot synthesis method utilizing zeolitic imidazolate framework-8 (ZIF-8) nanocrystals as a sacrificial template without any special etchant. The resulting PDA nanocapsules show negligible cytotoxicity in HeLa cells after incubation for 48 h at various doses, which implies their potential as candidates for practical applications in drug transport and targeting.

  10. One-pot synthesis of 2-amino-4(3H)-quinazolinones via ring-opening of isatoic anhydride and palladium-catalyzed oxidative isocyanide-insertion.

    PubMed

    Ji, Fei; Lv, Mei-Fang; Yi, Wen-Bin; Cai, Chun

    2014-08-14

    An efficient and practical two-step process has been developed for the synthesis of 2-amino-4(3H)-quinazolinones via ring-opening of isatoic anhydride and palladium-catalyzed oxidative isocyanide-insertion in one pot. This regioselective procedure could construct a wide range of 2-amino-4(3H)-quinazolinones in moderate to excellent yields. Furthermore, the methodology also had distinct advantages of easily accessible starting materials and operational simplicity.

  11. New pyridinium-based ionic liquid as an excellent solvent-catalyst system for the one-pot three-component synthesis of 2,3-disubstituted quinolines.

    PubMed

    Anvar, Salma; Mohammadpoor-Baltork, Iraj; Tangestaninejad, Shahram; Moghadam, Majid; Mirkhani, Valiollah; Khosropour, Ahmad Reza; Landarani Isfahani, Amir; Kia, Reza

    2014-03-10

    The synthesis of a variety of 2,3-disubstituted quinolines has been achieved successfully via a one-pot three-component reaction of arylamines, arylaldehydes and aliphatic aldehydes in the presence of butylpyridinium tetrachloroindate(III), [bpy][InCl4], ionic liquid as a green catalyst and solvent. Mild conditions with excellent conversions, and simple product isolation procedure are noteworthy advantages of this method. The recyclability of the ionic liquid makes this protocol environmentally benign.

  12. Synthesis of polyhydroxylated decalins via two consecutive one-pot reactions: 1,4-addition/aldol reaction followed by RCM/syn-dihydroxylation.

    PubMed

    Malik, Michał; Jarosz, Sławomir

    2016-01-01

    Synthesis of novel polyhydroxylated derivatives of decalin is described. The presented methodology consists in a one-pot copper-catalyzed 1,4-addition of vinylmagnesium bromide to sugar-derived cyclohexenone, followed by an aldol reaction with a derivative of but-3-enal. The obtained diene is then subjected to an assisted tandem catalytic sequence: ring-closing metathesis with the subsequent reuse of the Ru-catalyst in the syn-dihydroxylation. The stereochemical outcome of these reactions is discussed.

  13. Recycle waste salt as reagent: a one-pot substitution/Krapcho reaction sequence to α-fluorinated esters and sulfones.

    PubMed

    Zhu, Feng; Xu, Peng-Wei; Zhou, Feng; Wang, Cui-Hong; Zhou, Jian

    2015-02-20

    A "one-pot" tandem substitution/Krapcho reaction is reported for the facile synthesis of α-fluorinated esters and sulfones, which utilizes the byproduct salt formed in the substitution step as an indispensible reagent to facilitate the Krapcho reaction step. This represents the first sustainable tandem reaction that internally recycles the waste salt formed in the upstream step as the reagent for the downstream step.

  14. A novel one-pot pseudo-five-component synthesis of 4,5,6,7-tetrahydro-1H-1,4-diazepine-5-carboxamide derivatives.

    PubMed

    Shaabani, Ahmad; Maleki, Ali; Mofakham, Hamid; Moghimi-Rad, Jafar

    2008-05-16

    A novel one-pot pseudo-five-component synthesis of 4,5,6,7-tetrahydro-1 H-1,4-diazepine-5-carboxamide derivatives starting from simple and readily available inputs including 2,3-diaminomaleonitrile, a cyclic or acyclic ketone, an isocyanide, and water in the presence of a catalytic amount of p-toluenesulfonic acid in aqueous medium at ambient temperature in high yields is described.

  15. Zeolitic imidazolate framework-8 (ZIF-8) as a sacrificial template: one-pot synthesis of hollow poly(dopamine) nanocapsules and yolk-structured poly(dopamine) nanocomposites.

    PubMed

    Ran, Jingyu; Xiao, Lihua; Wu, Weidang; Liu, Yike; Qiu, Wei; Wu, Jianming

    2017-02-03

    Hollow poly(dopamine) (PDA) nanocapsules and yolk-structured PDA nanocomposites were prepared by an aqueous one-pot synthesis method utilizing zeolitic imidazolate framework-8 (ZIF-8) nanocrystals as a sacrificial template without any special etchant. The resulting PDA nanocapsules show negligible cytotoxicity in HeLa cells after incubation for 48 h at various doses, which implies their potential as candidates for practical applications in drug transport and targeting.

  16. One-Pot Synthesis of Indoles by a Sequential Ugi-3CR/Wittig Reaction Starting from Odorless Isocyanide-Substituted Phosphonium Salts.

    PubMed

    Yan, Yan-Mei; Rao, Yong; Ding, Ming-Wu

    2017-03-03

    A new one-pot preparation of indoles by a Ugi-3CR/Wittig sequence has been developed. The reaction of odorless isocyanide-substituted phosphonium salt 5, aldehyde 6, and amine 7 produced the indoles 9 in 45-82% yields via a sequential Ugi-3CR/Wittig reaction in the presence of H3PO4 and solid K2CO3, respectively.

  17. One-pot hydrogen peroxide and hydrohalic acid induced ring closure and selective aromatic halogenation to give new ring-fused benzimidazoles.

    PubMed

    Gurry, Michael; Sweeney, Martin; McArdle, Patrick; Aldabbagh, Fawaz

    2015-06-05

    A new series of selectively dichlorinated and dibrominated five- to eight-membered-ring [1,2-a]-fused benzimidazoles and [1,4]oxazino[4,3-a]benzimidazoles are synthesized in mostly high yields of >80% using the reaction of hydrogen peroxide and hydrohalic acid with commercially available o-cyclic amine substituted anilines. Domestic bleach with HCl can also be used for a one-pot ring closure and chlorination.

  18. Ultrasound-assisted one-pot, three-component synthesis of 1H-pyrazolo[1,2-b]phthalazine-5,10-diones.

    PubMed

    Nabid, Mohammad Reza; Rezaei, Seyed Jamal Tabatabaei; Ghahremanzadeh, Ramin; Bazgir, Ayoob

    2010-01-01

    Triethylamine was found to be an efficient catalyst for the synthesis of 1H-pyrazolo[1,2-b]phthalazine-5,10-diones by one-pot reaction of phthalhydrazide, aromatic aldehydes, and malononitrile or ethyl cyanoacetate in ethanol under ultrasonic irradiation. The advantages of this method are the use of an inexpensive and readily available catalyst, easy workup, improved yields, and the use of ethanol as a solvent that is considered to be relatively environmentally benign.

  19. Ultrasound-promoted one-pot, three-component synthesis of spiro[indoline-3,1'-pyrazolo[1,2-b]phthalazine] derivatives.

    PubMed

    Wang, Juxian; Bai, Xiaoguang; Xu, Changliang; Wang, Yucheng; Lin, Wei; Zou, Yi; Shi, Daqing

    2012-07-23

    A series of 3'-aminospiro[indoline-3,1'-pyrazolo[1,2-b]phthalazine]-2,5',10'-trione derivatives have been synthesized by a one-pot three-component reaction of isatin, malononitrile or ethyl cyanoacetate and phthalhydrazide catalyzed by piperidine under ultrasound irradiation. For comparison the reactions were carried out under both conventional and ultrasonic conditions. In general, improvement in rates and yields were observed when the reactions were carried out under sonication compared with classical conditions.

  20. Asymmetric one-pot sequential Friedel-Crafts-type alkylation and α-oxyamination catalyzed by a peptide and an enzyme.

    PubMed

    Akagawa, Kengo; Umezawa, Ryota; Kudo, Kazuaki

    2012-01-01

    In the presence of a peptide catalyst and the oxidative enzyme laccase, a one-pot sequential reaction including a Friedel-Crafts-type alkylation of α,β-unsaturated aldehydes followed by an α-oxyamination was realized. The reaction in aqueous solvent to promote the enzymatic oxidation, and the use of a peptide catalyst compatible with such conditions, were essential. The present sequential reaction afforded oxygen-functionalized indole or pyrrole derivatives in a highly enantioselective manner.

  1. Synthesis of polyhydroxylated quinolizidine and indolizidine scaffolds from sugar-derived lactams via a one-pot reduction/Mannich/Michael sequence.

    PubMed

    Szcześniak, Piotr; Stecko, Sebastian; Maziarz, Elżbieta; Staszewska-Krajewska, Olga; Furman, Bartłomiej

    2014-11-07

    A direct approach to the synthesis of indolizidine and quinolizidine scaffolds of iminosugars is described. The presented strategy is based on a one-pot sugar lactam reduction with Schwartz's reagent followed by a diastereoselective Mannich/Michael tandem reaction of the resulting sugar imine with Danishefsky's diene. The stereochemical course of the investigated reaction has been explained in detail. The obtained bicyclic products are attractive building blocks for the synthesis of various naturally occurring polyhydroxylated alkaloids and their derivatives.

  2. One pot iridium-catalyzed asymmetrical double allylations of sodium sulfide: a fast and economic way to construct chiral C2-symmetric bis(1-substituted-allyl)sulfane.

    PubMed

    Zheng, Shengcai; Huang, Weiqing; Gao, Ning; Cui, Ruimin; Zhang, Min; Zhao, Xiaoming

    2011-06-28

    One pot asymmetrical double allylations of sodium sulfide catalyzed by an iridium complex along with a combination of caesium fluoride and water in dichloromethane have been realized and the double allylation products with two C-S bond chiral centers were obtained in 67-99% yields with b/l 81/19-99/1, dr 85/15-99/1, and 96-99% ee.

  3. Palladium-catalyzed sequential one-pot reaction of aryl bromides with O-homoallylhydroxylamines: synthesis of N-aryl-beta-amino alcohols.

    PubMed

    Peng, Jinsong; Jiang, Dahong; Lin, Wenqing; Chen, Yuanwei

    2007-05-07

    The palladium-catalyzed sequential one-pot N-arylation-carbo-amination-C-arylation of O-homoallylhydroxylamines with two different aryl bromides provides rapid entry to differentially arylated N-aryl-3-arylmethylisoxazolidines in good yields with excellent diastereoselectivity. The obtained isoxazolidines can be reductively cleaved to cis-N-aryl-beta-amino alcohols in short times and in high yields at room temperature.

  4. Recent advances in the chemistry of Rh carbenoids: multicomponent reactions of diazocarbonyl compounds

    NASA Astrophysics Data System (ADS)

    Medvedev, J. J.; Nikolaev, V. A.

    2015-07-01

    Multicomponent reactions of diazo compounds catalyzed by RhII complexes become a powerful tool for organic synthesis. They enable three- or four-step processes to be carried out as one-pot procedures (actually as one step) with high stereoselectivity to give complex organic molecules, including biologically active compounds. This review addresses recent results in the chemistry of Rh-catalyzed multicomponent reactions of diazocarbonyl compounds with the intermediate formation of N-, O- and C=O-ylides. The diastereo- and enantioselectivity of these reactions and the possibility of using various co-catalysts to increase the efficiency of the processes under consideration are discussed. The bibliography includes 120 references.

  5. Simple preparation of new [(18) F]F-labeled synthetic amino acid derivatives with two click reactions in one-pot and SPE purification.

    PubMed

    Yook, Cheol-Min; Lee, Sang Ju; Oh, Seung Jun; Ha, Hyun-Joon; Lee, Jong Jin

    2015-06-30

    New [(18) F]fluorinated 1,2,3-triazolyl amino acid derivatives were efficiently prepared from Huisgen 1,3-dipolar cycloaddition reactions, well known as click reaction. We developed two simultaneous click reactions in one-pot with a simple solid-phase extraction (SPE) purification method. [(18) F]fluoro-1-propyne was obtained at a 45% non-decay corrected radiochemical yield based on the [(18) F]fluoride ion. The one-pot and simultaneous two click reactions were performed with unprotected azido-alkyl amino acid, [(18) F]fluoro-1-propyne, and lipophilic additive alkyne to produce three synthetic amino acid derivatives, AMC-101 ([(18) F]-6a), AMC-102 ([(18) F]-6b), and AMC-103 ([(18) F]-6c) with 29%, 28%, and 24% of non-decay corrected radiochemical yields, respectively. All radiotracers indicated that radiochemical purities were >95% without any residual organic solvent. Our new method involving two click reactions in one-pot showed high radiochemical and chemical purity by easy removal of the residual precursor from the simultaneous two click reactions.

  6. A new approach to determine vapor pressures of compounds in multicomponent systems by comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry.

    PubMed

    Parshintsev, Jevgeni; Lai, Ching Kwan; Hartonen, Kari; Kulmala, Markku; Riekkola, Marja-Liisa

    2014-06-01

    A method is described to determine vapor pressures of compounds in multicomponent systems simultaneously. The method is based on temperature-gradient analysis by comprehensive two-dimensional gas chromatography coupled to time-of-flight mass spectrometry (GCxGC-TOFMS). Vapor pressures are determined with the aid of known vapor pressure values of reference compounds eluting before and after the analytes. Reference compounds with the same functionalities as the analytes are preferred, but when these are not available, the alkane series can be utilized. The number of compounds whose vapor pressures can be determined is limited only by the peak capacity of the chromatographic system. Although the lowest subcooled vapor pressure determined was 0.006 Pa, for tetrahydroaraucarolone in an atmospheric aerosol sample, vapor pressures as low as 10(-6) Pa can be measured with the described set-up. Even lower values can be measured with higher GC temperatures and longer analysis times. Since only a few picograms of compound is required, in a mixture of any complexity, the GCxGC-TOFMS method offers unique sensitivity, rapidity, and comprehensiveness.

  7. High Glass Transition Temperature Renewable Polymers via Biginelli Multicomponent Polymerization.

    PubMed

    Boukis, Andreas C; Llevot, Audrey; Meier, Michael A R

    2016-04-01

    A novel and straightforward one-pot multicomponent polycondensation method was established in this work. The Biginelli reaction is a versatile multicomponent reaction of an aldehyde, a β-ketoester (acetoacetate) and urea, which can all be obtained from renewable resources, yielding diversely substituted 3,4-dihydropyrimidin-2(1H)-ones (DHMPs). In this study, renewable diacetoacetate monomers with different spacer chain lengths (C3, C6, C10, C20) were prepared via simple transesterification of renewable diols and commercial acetoacetates. The diacetoacetate monomers were then reacted with renewable dialdehydes, i.e., terephthalaldehyde and divanillin in a Biginelli type step-growth polymerization. The obtained DHMP polymers (polyDHMPs) displayed high molar masses, high glass transition temperatures (Tg) up to 203 °C and good thermal stability (Td5%) of 280 °C. The Tg of the polyDHMPs could be tuned by variation of the structure of the dialdehyde or the diacetoacetate component.

  8. Coupling shell-isolated nanoparticle enhanced Raman spectroscopy with paper chromatography for multi-components on-site analysis.

    PubMed

    Zhang, Kun; Qing, Jiang; Gao, Han; Ji, Ji; Liu, Baohong

    2017-01-01

    By coupling shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) with paper chromatography, two birds with one stone method were developed for simultaneous on-site separation and optical detection of multiple components. The established method features high sensitivity of plasmon-enhanced sensing strategies and sufficient temporal and spatial resolution of planar chromatographic techniques.

  9. One-pot mechanosynthesis with three levels of molecular self-assembly: coordination bonds, hydrogen bonds and host-guest inclusion.

    PubMed

    Friscić, Tomislav; Mestrović, Ernest; Skalec Samec, Dijana; Kaitner, Branko; Fábián, László

    2009-11-23

    Liquid-assisted grinding (LAG) was used to combine three levels of molecular self-assembly into a one-pot mechanochemical approach for the construction of metal-organic materials. The approach was applied for the construction of three adducts of cobalt(II) dibenzoylmethanate with isonicotinamide, nicotinamide and imidazole, to screen for their inclusion compounds. The one-pot process consists of: i) The coordination-driven binding of addends to the equatorially-protected metal ion, resulting in "wheel-and-axle"-shaped complexes; ii) self-assembly of resulting complexes by way of hydrogen-bonded synthons to form metal-organic inclusion hosts; iii) in situ inclusion of the grinding liquid in the resulting host. This approach provided quantitatively and within 20 min the known inclusion compounds of the bis(isonicotinamide) adduct in a single synthetic step. Changing the liquid phase in LAG was used to explore the inclusion behaviour of new wheel-and-axle adducts with nicotinamide and imidazole, revealing several inclusion compounds, as well as two polymorphs, of the bis(nicotinamide) host. Preliminary results suggest that one-pot LAG is superior to solution synthesis in screening for metal-organic inclusion compounds. The difference between the methods is rationalised in terms of reactant solubility and solvent competition. In contrast to the nicotinamide adduct, the bis(imidazole) adduct did not form inclusion compounds. The difference in the inclusion properties of the two adducts is rationalised by structural information gathered by single crystal and powder X-ray diffraction.

  10. A facile one-pot hydrothermal synthesis of β-MnO{sub 2} nanopincers and their catalytic degradation of methylene blue

    SciTech Connect

    Cheng, Gao; Yu, Lin Lin, Ting; Yang, Runnong; Sun, Ming; Lan, Bang; Yang, Lili; Deng, Fangze

    2014-09-15

    Branched β-MnO{sub 2} bipods with novel nanopincer morphology were prepared by a facile one-pot hydrothermal method via a redox reaction between NaClO{sub 3} and MnSO{sub 4} in sulfuric acid solution without using any surfactants or templates. The products were characterized in detail by various techniques including X-ray powder diffraction, Raman spectroscopy, X-ray photoelectron spectroscopy, surface area analyzer, field emission scanning electron microscopy and transmission electron microscopy. Results show that the obtained β-MnO{sub 2} nanopincers consist of two sharp nanorods with a diameter of 100–200 nm and a length of 1–2 μm. The concentration of H{sub 2}SO{sub 4} solution plays an important role in controlling the crystal phase and morphology of the final product. A possible formation mechanism for the β-MnO{sub 2} nanopincers was proposed. Moreover, these β-MnO{sub 2} nanostructures exhibited better catalytic performance than the commercial MnO{sub 2} particles to decompose methyl blue (MB) in the presence of H{sub 2}O{sub 2}. - Graphical abstract: Branched β-MnO{sub 2} bipods with novel nanopincer morphology were prepared by a facile one-pot hydrothermal method through oxidizing MnSO{sub 4} with NaClO{sub 3} in H2SO{sub 4} condition without using any surfactants or templates. - Highlights: {sup •} Branched β-MnO{sub 2} nanopincers were prepared by a facile one-pot hydrothermal method. {sup •} Morphology and crystal phase of MnO{sub 2} were controlled by the H{sub 2}SO{sub 4} concentration. {sup •} A possible formation mechanism for the obtained β-MnO{sub 2} nanopincers was proposed. {sup •} The products showed great catalytic performance in degradation of methylene blue.

  11. A novel water-soluble fluorescent polymer based on perylene bisimides dyes: one-pot preparation and its bio-imaging.

    PubMed

    Tan, Haijian; Liu, Hongmei; Liu, Yaojun; Duan, Wenfeng; Yi, Xuegang; Wu, Yonggang; Zhao, Hongchi; Bai, Libin

    2016-01-01

    Perylene bisimides dye-based water-soluble fluorescent polymer P3, N,N'-bis(3-amyl)-1-bromo-7-{4'-[3''-(S-poly(N-acryloyl ethylene diamine hydrochloride)-2'''-methyl propionic acid)propionyloxy hexyloxy]phenyl} perylene-3,4:9,10-tetracarboxylic bisimides, was synthesized with polyelectrolyte modification via one-pot reaction (the reduction reaction of trithioester and click reaction between the thiol group and carbon-carbon double bond were simultaneously conducted in one pot with high conversion). One-pot method can overcome the limitation that usual click reaction between thiol and other groups has low conversion because thiol group is subject to rapid oxidation during purification and storage. Chemical, structural, and optical properties of P3 and intermediate products were fully characterized by nuclear magnetic resonance spectroscopy, Fourier transform infrared, gel permeation chromatograph, UV-vis spectra, and fluorescence spectra, respectively. The results revealed that P3 displayed excellent water solubility and not only exhibited red strong fluorescence emission band in water but also had the similar photoluminescent spectra to those of intermediate products (M4 and P2) in chloroform. Allowing for the potential application in biological detection field, cell viability and live cell imaging with the presence of P3 were further investigated with Hela cells. The results showed that P3 had low cytotoxicity with strong intracellular fluorescence entry. Meanwhile, with the augment of concentration of P3 (0-0.500 mg mL(-1)), the cell uptake and accumulation of P3 increased and thereby result in enhancement of the intracellular fluorescence. These experiment results suggested that P3 had enormous potential as a fluorescence probe to be an important component in biological detection field.

  12. One-pot, two-step, microwave-assisted palladium-catalyzed conversion of aryl alcohols to aryl fluorides via aryl nonaflates.

    PubMed

    Wannberg, Johan; Wallinder, Charlotta; Ünlüsoy, Meltem; Sköld, Christian; Larhed, Mats

    2013-04-19

    A convenient procedure for converting aryl alcohols to aryl fluorides via aryl nonafluorobutylsulfonates (ArONf) is presented. Moderate to good one-pot, two-step yields were achieved by this nonaflation and microwave-assisted, palladium-catalyzed fluorination sequence. The reductive elimination step was investigated by DFT calculations to compare fluorination with chlorination, proving a larger thermodynamic driving force for the aryl fluoride product. Finally, a key aryl fluoride intermediate for the synthesis of a potent HCV NS3 protease inhibitor was smoothly prepared with the novel protocol.

  13. Mechanochemical solid-state synthesis of 2-aminothiazoles, quinoxalines and benzoylbenzofurans from ketones by one-pot sequential acid- and base-mediated reactions.

    PubMed

    Nagarajaiah, Honnappa; Mishra, Abhaya Kumar; Moorthy, Jarugu Narasimha

    2016-04-26

    α-Chloroketones - obtained by the atom-economical chlorination of ketones with trichloroisocyanuric acid (TCCA) in the presence of p-TSA under ball-milling conditions - were set up for a sequential base-mediated condensation reaction with thiourea/thiosemicarbazides, o-phenylenediamine and salicylaldehyde to afford 2-aminothiazoles, 2-hydrazinylthiazoles, quinoxalines and benzoylbenzofurans, respectively, in respectable yields. The viability of one-pot sequential acid- and base-mediated reactions in the solid state under ball-milling conditions is thus demonstrated.

  14. One-Pot Click Access to a Cyclodextrin Dimer-Based Novel Aggregation Induced Emission Sensor and Monomer-Based Chiral Stationary Phase

    PubMed Central

    Li, Xiaoli; Zhao, Rui; Tang, Xiaoying; Shi, Yanyan; Li, Chunyi; Wang, Yong

    2016-01-01

    A ‘two birds, one stone’ strategy was developed via a one-pot click reaction to simultaneously prepare a novel cyclodextrin (CD) dimer based aggregation induced emission (AIE) sensor (AIE-DCD) and a monomer based chiral stationary phase (CSP-MCD) for chiral high performance liquid chromatography (CHPLC). AIE-DCD was found to afford satisfactory AIE response for specific detection of Zn2+ with a detection limit of 50 nM. CSP-MCD exhibits excellent enantioseparation ability toward dansyl amino acids, where the resolution of dansyl amino leucine reaches 5.43. PMID:27886123

  15. Improved and optimized one-pot method for N-succinimidyl-4-[(18)F]fluorobenzoate ([(18)F]SFB) synthesis using microwaves.

    PubMed

    Li, Kang-Po; Hu, Ming-Kuan; Kwang-Fu Shen, Clifton; Lin, Wei-Yu; Hou, Shuang; Zhao, Li-Bo; Cheng, Cheng-Yi; Shen, Daniel H

    2014-12-01

    N-Succinimidyl-4-[(18)F]fluorobenzoate ([(18)F]SFB) is a potential prosthetic agent for novel tracer development in positron emission tomography (PET). Previously, we reported a microwave-assisted one-pot synthesis of [(18)F]SFB with high efficacy. Herein, we reveal an improved and optimized approach based on this former model for producing [(18)F]SFB. With optimized approaches, the entire protocol can be completed within 25min, and [(18)F]SFB is generated in satisfactory quality for direct use without further purification via high-performance liquid chromatography.

  16. Synthesis of polyhydroxylated decalins via two consecutive one-pot reactions: 1,4-addition/aldol reaction followed by RCM/syn-dihydroxylation

    PubMed Central

    2016-01-01

    Synthesis of novel polyhydroxylated derivatives of decalin is described. The presented methodology consists in a one-pot copper-catalyzed 1,4-addition of vinylmagnesium bromide to sugar-derived cyclohexenone, followed by an aldol reaction with a derivative of but-3-enal. The obtained diene is then subjected to an assisted tandem catalytic sequence: ring-closing metathesis with the subsequent reuse of the Ru-catalyst in the syn-dihydroxylation. The stereochemical outcome of these reactions is discussed. PMID:28144329

  17. Chiroptical Probing of Lanthanide-Directed Self-Assembly Formation Using btp Ligands Formed in One-Pot Diazo-Transfer/Deprotection Click Reaction from Chiral Amines.

    PubMed

    Byrne, Joseph P; Martínez-Calvo, Miguel; Peacock, Robert D; Gunnlaugsson, Thorfinnur

    2016-01-11

    A series of enantiomeric 2,6-bis(1,2,3-triazol-4-yl)pyridines (btp)-containing ligands was synthesized by a one-pot two-step copper-catalyzed amine/alkyne click reaction. The Eu(III) - and Tb(III) -directed self-assembly formation of these ligands was studied in CH3 CN by monitoring their various photophysical properties, including their emerging circular dichroism and circularly polarized luminescence. The global analysis of the former enabled the determination of both the stoichiometry and the stability constants of the various chiral supramolecular species in solution.

  18. Modular, One-Pot, Sequential Aziridine Ring Opening-S(N)Ar Strategy to 7-, 10-, and 11-Membered Benzo-Fused Sultams.

    PubMed

    Loh, Joanna K; Asad, Naeem; Samarakoon, Thiwanka B; Hanson, Paul R

    2015-10-16

    The generation of common and stereochemically rich medium-sized benzo-fused sultams via complementary pairing of heretofore-unknown (o-fluoroaryl)sulfonyl aziridine building blocks with an array of amino alcohols/amines in a modular one-pot, sequential protocol using an aziridine ring opening and intramolecular nucleophilic aromatic substitution is reported. The strategy employs a variety of amino alcohols/amines and proceeds with 6 + 4/6 + 5 and 6 + 1 cycloetherification pathways in a highly chemo- and regioselective fashion to obtain skeletally and structurally diverse, polycyclic, 10- to 11- and 7-membered benzo-fused sultams for broad-scale screening.

  19. Tetraethylene glycol promoted two-step, one-pot rapid synthesis of indole-3-[1-11C]acetic acid

    DOE PAGES

    Lee, Sojeong; Qu, Wenchao; Alexoff, David L.; ...

    2014-12-12

    An operationally friendly, two-step, one-pot process has been developed for the rapid synthesis of carbon-11 labeled indole-3-acetic acid ([11]IAA or [11]auxin). By replacing an aprotic polar solvent with tetraethylene glycol, nucleophilic [11]cyanation and alkaline hydrolysis reactions were performed consecutively in a single pot without a time-consuming intermediate purification step. The entire production time for this updated procedure is 55 min, which dramatically simplifies the entire synthesis and reduces the starting radioactivity required for a whole plant imaging study.

  20. Pseudo five-component synthesis of 2,5-di(hetero)arylthiophenes via a one-pot Sonogashira–Glaser cyclization sequence

    PubMed Central

    Urselmann, Dominik; Antovic, Dragutin

    2011-01-01

    Summary Based upon a consecutive one-pot Sonogashira–Glaser coupling–cyclization sequence a variety of 2,5-di(hetero)arylthiophenes were synthesized in moderate to good yields. A single Pd/Cu-catalyst system, without further catalyst addition, and easily available, stable starting materials were used, resulting in a concise and highly efficient route for the synthesis of the title compounds. This novel pseudo five-component synthesis starting from iodo(hetero)arenes is particularly suitable as a direct access to well-defined thiophene oligomers, which are of peculiar interest in materials science. PMID:22238523

  1. One-pot wet-chemical co-reduction synthesis of bimetallic gold-platinum nanochains supported on reduced graphene oxide with enhanced electrocatalytic activity

    NASA Astrophysics Data System (ADS)

    Chen, De-Jun; Zhang, Qian-Li; Feng, Jin-Xia; Ju, Ke-Jian; Wang, Ai-Jun; Wei, Jie; Feng, Jiu-Ju

    2015-08-01

    In this work, a simple, rapid and facile one-pot wet-chemical co-reduction method is developed for synthesis of bimetallic Au-Pt alloyed nanochains supported on reduced graphene oxide (Au-Pt NCs/RGO), in which caffeine is acted as a capping agent and a structure-directing agent, while no any seed, template, surfactant or polymer involved. The as-prepared nanocomposites display enlarged electrochemical active surface area, significantly enhanced catalytic activity and better stability for methanol and ethylene glycol oxidation, compared with commercial Pt-C (Pt 50 wt%), PtRu-C (Pt 30 wt% and Ru 15 wt%) and Pt black.

  2. Tetraethylene glycol promoted two-step, one-pot rapid synthesis of indole-3-[1-11C]acetic acid

    SciTech Connect

    Lee, Sojeong; Qu, Wenchao; Alexoff, David L.; Shea, Colleen; Kim, Dohyun; Schueller, Michael; Fowler, Joanna S.

    2014-12-12

    An operationally friendly, two-step, one-pot process has been developed for the rapid synthesis of carbon-11 labeled indole-3-acetic acid ([11]IAA or [11]auxin). By replacing an aprotic polar solvent with tetraethylene glycol, nucleophilic [11]cyanation and alkaline hydrolysis reactions were performed consecutively in a single pot without a time-consuming intermediate purification step. The entire production time for this updated procedure is 55 min, which dramatically simplifies the entire synthesis and reduces the starting radioactivity required for a whole plant imaging study.

  3. Synthesis and Evaluation of Cu/SAPO-34 Catalysts for NH3-SCR 2: Solid-state Ion Exchange and One-pot Synthesis

    SciTech Connect

    Gao, Feng; Walter, Eric D.; Washton, Nancy M.; Szanyi, Janos; Peden, Charles HF

    2015-01-01

    Cu-SAPO-34 catalysts are synthesized using two methods: solid-state ion exchange (SSIE) and one-pot synthesis. SSIE is conducted by calcining SAPO-34/CuO mixtures at elevated temperatures. For the one-pot synthesis method, Cu-containing chemicals (CuO and CuSO4) are added during gel preparation. A high-temperature calcination step is also needed for this method. Catalysts are characterized with surface area/pore volume measurements, temperature programmed reduction (TPR), electron paramagnetic resonance (EPR) and nuclear magnetic resonance (NMR) spectroscopies, and scanning electron microscopy (SEM). Catalytic properties are examined using standard ammonia selective catalytic reduction (NH3-SCR) and ammonia oxidation reactions. In Cu-SAPO-34 samples formed using SSIE, Cu presents both as isolated Cu2+ ions and unreacted CuO. The former is highly active and selective in NH3-SCR, while the latter catalyzes a side reaction; notably, the non-selective oxidation of NH3 above 350 ºC. Using the one-pot method followed by a high-temperature aging treatment, it is possible to form Cu SAPO-34 samples with predominately isolated Cu2+ ions at low Cu loadings. However at much higher Cu loadings, isolated Cu2+ ions that bind weakly with the CHA framework and CuO clusters also form. These Cu moieties are very active in catalyzing non-selective NH3 oxidation above 350 ºC. Low-temperature reaction kinetics indicate that Cu-SAPO-34 samples formed using SSIE have core-shell structures where Cu is enriched in the shell layers; while Cu is more evenly distributed within the one-pot samples. Reaction kinetics also suggest that at low temperatures, the local environment next to Cu2+ ion centers plays little role on the overall catalytic properties. The authors gratefully acknowledge the US Department of Energy (DOE), Energy Efficiency and Renewable Energy, Vehicle Technologies Office for the support of this work. The research described in this paper was performed at the Environmental

  4. A facile one-pot preparation of alkyl aminoaryl sulfides for the synthesis of GW7647 as an agonist of peroxisome proliferator-activated receptor alpha.

    PubMed

    Ham, Jungyeob; Cho, Sung Jin; Ko, Jaeyoung; Chin, Jungwook; Kang, Heonjoong

    2006-07-21

    We have developed two simple and high yielding one-pot syntheses of alkyl aminoaryl sulfides containing a series of four-steps: in situ protection of the free amine by reaction with a Grignard reagent, halogen-lithium exchange, sulfur insertion, and a substitution reaction with various electrophiles. Through this protocol, we have successfully synthesized tert-butyl-2-[4-(2-aminoethyl)phenylsulfanyl]-2-methylpropanoate, a key intermediate for the synthesis of GW7647 and GW9578 (ureido-TiBAs), in 92% yield. Furthermore, we were able to improve the overall yield of GW7647 to 66%, 3 times the yield previously reported.

  5. Copper ferrite nanoparticles: an efficient and reusable nanocatalyst for a green one-pot, three-component synthesis of spirooxindoles in water.

    PubMed

    Bazgir, Ayoob; Hosseini, Ghaffar; Ghahremanzadeh, Ramin

    2013-10-14

    A green reaction of isatins, active cyanomethanes, and cyclic 1,3-dicarbonyl derivatives for the efficient and simple one-pot three-component synthesis of spirooxindole fused heterocycles in refluxing water by use of magnetically recoverable and reusable catalyst is reported. The features of this procedure are, the use of magnetically recoverable and reusable catalyst, mild reaction conditions, high to excellent product yields, operational simplicity, and easy workup procedures. Most importantly of all, easy magnetic separation of the catalyst eliminates the requirement of catalyst filtration after completion of the reaction. Furthermore, the catalyst remained highly active even after 5 repeated uses.

  6. Catalytic regioselective introduction of allyl alcohol into the nonpolar polyolefins: development of one-pot synthesis of hydroxyl-capped polyolefins mediated by a new metallocene IF catalyst.

    PubMed

    Imuta, Jun-ichi; Kashiwa, Norio; Toda, Yoshihisa

    2002-02-20

    A new catalytic regioselective one-pot synthesis of hydroxyl-capped polyolefins is reported. This synthesis employs a new stereorigid bridged metallocene having an indenyl and a fluorenyl ligand named IF catalyst 1, exhibiting high catalytic performances. Here, we report on (1) the first example of allyl alcohol incorporation into the nonpolar polymer backbone using IF catalyst 1 and methylaluminoxane with high activity, high molecular weight, and high polar monomer uptake at high temperature, and (2) the first example of predominant end-site-selective introduction of an alcohol group into the polyolefins. Moreover, we observed the mixed regioselectivity by the type of alkylaluminum.

  7. A one step/one pot synthesis of N,N-bis(phosphonomethyl)amino acids and their effects on adipogenic and osteogenic differentiation of human mesenchymal stem cells.

    PubMed

    Kasser, Johanna; Nazarov, Alexey A; Hartinger, Christian G; Wdziekonski, Brigitte; Dani, Christian; Kuznetsov, Maxim L; Arion, Vladimir B; Keppler, Bernhard K

    2009-05-01

    The one pot reaction of amino acids with diethylphosphite and formaldehyde yielded N,N-bis(phosphonomethyl)amino acids. This synthetic route does not require harsh reagents to cleave the ester group. The molecular structures of the new compounds were determined by X-ray diffraction methods. By employing DFT calculations the hydrolysis of the intermediate phosphonic esters to the respective acids could be explained by the decreasing P-OEt bond strength for C(alpha)-bisalkylated amino acids. Biological evaluation on the adipogenic and osteogenic differentiation of mesenchymal stem cells revealed no modification of the adipocyte differentiation, but inhibition of osteoblast formation at concentrations without detectable cytotoxicity.

  8. Macrocyclic bis(phenanthroline-pyrrole): a convenient one-pot synthesis, structure(s), spectroscopic, and redox properties, and the binding of amine guests, protons, and lanthanide ions.

    PubMed

    McSkimming, Alex; Shrestha, Sumi; Bhadbhade, Mohan M; Thordarson, Pall; Colbran, Stephen B

    2014-01-01

    This paper reports a convenient, one-pot, easily scalable and readily modifiable synthesis of a novel large-ring bis(1,10-phenanthrolinyl-2,5-pyrrole) macrocycle, H2LMC, and describes its spectroscopic and electrochemical properties, protonation, cooperative amine binding, electrocatalysis of the oxidation of primary amines, photosensitization of the decomposition of dichloromethane, and the first lanthanide complexes of the hexaaza-dianion LMC(2-) including the novel dimer, [(NO3)(LMC)Eu(μ-OH)Eu(LMC )(H2 O)2]·2py.

  9. Multicomponent synthesis of spiropyrrolidine analogues derived from vinylindole/indazole by a 1,3-dipolar cycloaddition reaction

    PubMed Central

    Narayanarao, Manjunatha; Koodlur, Lokesh; Revanasiddappa, Vijayakumar G; Gopal, Subramanya

    2016-01-01

    A new series of spiropyrrolidine compounds containing indole/indazole moieties as side chains have been accomplished via a one-pot multicomponent synthesis. The method uses the 1,3-dipolar cycloaddition reaction between N-alkylvinylindole/indazole and azomethine ylides, prepared in situ from cyclic/acyclic amino acids. The 1,3-dipolar cycloaddition proceeds efficiently under thermal conditions to afford the regio- and stereospecific cyclic adducts. PMID:28144362

  10. Multicomponent synthesis of spiropyrrolidine analogues derived from vinylindole/indazole by a 1,3-dipolar cycloaddition reaction.

    PubMed

    Narayanarao, Manjunatha; Koodlur, Lokesh; Revanasiddappa, Vijayakumar G; Gopal, Subramanya; Kamila, Susmita

    2016-01-01

    A new series of spiropyrrolidine compounds containing indole/indazole moieties as side chains have been accomplished via a one-pot multicomponent synthesis. The method uses the 1,3-dipolar cycloaddition reaction between N-alkylvinylindole/indazole and azomethine ylides, prepared in situ from cyclic/acyclic amino acids. The 1,3-dipolar cycloaddition proceeds efficiently under thermal conditions to afford the regio- and stereospecific cyclic adducts.

  11. WO3/g-C3N4 composites: one-pot preparation and enhanced photocatalytic H2 production under visible-light irradiation.

    PubMed

    Cheng, Cheng; Shi, Jinwen; Hu, Yuchao; Guo, Liejin

    2017-04-21

    A series of WO3/g-C3N4 composites with different WO3 contents were prepared via a facile one-pot pyrolysis method, and showed notably enhanced visible-light-driven photocatalytic H2-evolution activities, with the highest rate of 400 μmol h(-1) gcat(-1) that was 15.0 times of that for pristine g-C3N4. Contents and sizes of WO3 crystallites in the composites were easily adjusted by changing the molar ratios of (NH4)2WS4 to C3H6N6 in the feed reagents, thereby successfully optimizing the Z-scheme system constructed by WO3 and g-C3N4 and thus effectively reducing the recombination of photogenerated charge carriers in g-C3N4. Moreover, pore volumes and surface areas of the composites were gradually enlarged by introducing WO3 into g-C3N4 via the one-pot preparation strategy, therefore promoting the redox reactions to evolve H2. This work presented an effective route to simultaneously optimize the phase compositions and textural structures of photocatalysts for enhanced H2 evolution.

  12. One-pot synthesis of silicon based nanoparticles with incorporated phthalocyanine for long-term bioimaging and photo-dynamic therapy of tumors

    NASA Astrophysics Data System (ADS)

    Liu, Jiaojiao; Wang, Rui; Wu, Sicong; Yuan, Bing; Bao, Meimei; Li, Jingliang; Dou, Yujiang; He, Yao; Yang, Kai

    2017-03-01

    Combining the merits of delivery vectors with drug molecules is one of the key directions for development of efficient cancer monitoring and treatment techniques. In this work, a novel type of silicon based composite nanoparticles (NPs) with incorporated hydrophobic phthalocyanine molecules (Pc) was synthesized via a facile one-pot method. The as-synthesized Pc@Si NPs, with a small size of 4.2 ± 0.8 nm, have excellent dispersibility in water and good biocompatibility with cells, in addition to favorable photoluminescence and robust photostability even in cells. Moreover, the Pc@Si NPs show significant in vitro cancer cell killing and in vivo tumor inhibiting abilities upon near-infrared light exposure, due to the photodynamic therapy (PDT) effect of Pc. This work develops an efficient fluorescent PDT drug carrier; moreover, the facile one-pot synthesis strategy may be used generally to prepare silicon-based composite NPs incorporated with diverse hydrophobic drugs/diagnostic molecules for a wide range of biomedical applications.

  13. Ultrasonic-assisted one-pot preparation of ZnO/Ag3VO4 nanocomposites for efficiently degradation of organic pollutants under visible-light irradiation

    NASA Astrophysics Data System (ADS)

    Kiantazh, Fariba; Habibi-Yangjeh, Aziz

    2015-11-01

    We report a facile ultrasonic-assisted one-pot method for preparation of ZnO/Ag3VO4 nanocomposites with different mole fractions of silver vanadate. The preparation method has considerable merits such as short preparation time, large-scale, and one-pot strategy. The resultant samples were fairly characterized by means of XRD, EDX, SEM, TEM, UV-vis DRS, FT-IR, and PL techniques. Visible-light activity of the resultant samples was investigated by degradation of rhodamine B (RhB), methylene blue (MB), and methyl orange (MO). Among the prepared nanocomposites, the ZnO/Ag3VO4 nanocomposite with 0.073 mole fraction of Ag3VO4 exhibited the best activity and excessive amount of Ag3VO4 resulted in decrease of the activity. Photocatalytic activity of this nanocomposite under visible-light irradiation is about 21, 56, and 2.8-fold higher than that of the ZnO sample in degradation of RhB, MB, and MO, respectively. The highly enhanced activity of the nanocomposite was attributed to greater generation of electron-hole pairs, due to photosensitizing role of Ag3VO4 under visible-light irradiation, and efficiently separation of the photogenerated electron-hole pairs, due to formation of n-n heterojunction between the counterparts. Furthermore, it was revealed that the photocatalytic activity largely depends on ultrasonic irradiation time, calcination temperature, and scavengers of the reactive species.

  14. One-pot chemical route for morphology-controllable fabrication of Sn-Sb micro/nano-structures: Advanced anode materials for lithium and sodium storage

    NASA Astrophysics Data System (ADS)

    Yi, Zheng; Han, Qigang; Geng, Di; Wu, Yaoming; Cheng, Yong; Wang, Limin

    2017-02-01

    A series of morphology/component-controllable Sn-Sb micro/nano-structures are fabricated by a one-pot replacement reaction technique employing metallic Sn as both template and reducing agent. Typically, nanoscaled Sn as template and ethyl alcohol as solvent give the hollow structure, while micron-sized Sn as precursor and ethylene glycol as solvent produce the dendritic product. Other mixed structures are also obtained by this one-pot route. As anode materials for lithium-ion batteries, the hollow or dendritic Sn-Sb materials exhibit higher discharge capacities compared with the corresponding Sb samples as well as the Sn templates. Especially, for the Sn-Sb hollow spheres, a high discharge capacity of 820.7 mAh g-1 after first cycle and a reversible capacity of 751 mAh g-1 are achieved after 100 cycles at a current density of 100 mA g-1. Meanwhile, the hollow Sn-Sb structure delivers a specific capacity of 451.3 mA h g-1 at 500 mA g-1 after 150 cycles when used for sodium ion batteries. The superior electrochemical performance that are higher than many reported results can be attributed to the special morphology and structure, which can shorten the transportation distance of lithium/sodium ion and provide extra free space to buffer the volume expansion during the lithium/sodium insertion/extraction.

  15. A novel one-pot process for near-net-shape fabrication of open-porous resorbable hydroxyapatite/protein composites and in vivo assessment.

    PubMed

    Mueller, Berit; Koch, Dietmar; Lutz, Rainer; Schlegel, Karl A; Treccani, Laura; Rezwan, Kurosch

    2014-09-01

    We present a mild one-pot freeze gelation process for fabricating near-net, complex-shaped hydroxyapatite scaffolds and to directly incorporate active proteins during scaffold processing. In particular, the direct protein incorporation enables a simultaneous adjustment and control of scaffold microstructure, porosity, resorbability and enhancement of initial mechanical and handling stability. Two proteins, serum albumin and lysozyme, are selected and their effect on scaffold stability and microstructure investigated by biaxial strength tests, electron microscopy, and mercury intrusion porosimetry. The resulting hydroxyapatite/protein composites feature adjustable porosities from 50% to 70% and a mechanical strength ranging from 2 to 6 MPa comparable to that of human spongiosa without any sintering step. Scaffold degradation behaviour and protein release are assessed by in vitro studies. A preliminary in vivo assessment of scaffold biocompatibility and resorption behaviour in adult domestic pigs is discussed. After implantation, composites were resorbed up to 50% after only 4 weeks and up to 65% after 8 weeks. In addition, 14% new bone formation after 4 weeks and 37% after 8 weeks were detected. All these investigations demonstrate the outstanding suitability of the one-pot-process to create, in a customisable and reliable way, biocompatible scaffolds with sufficient mechanical strength for handling and surgical insertion, and for potential use as biodegradable bone substitutes and versatile platform for local drug delivery.

  16. Cyanogel-derived N-doped C nanosheets immobilizing Pd-P nanoparticles: One-pot synthesis and enhanced hydrogenation catalytic performance

    NASA Astrophysics Data System (ADS)

    Zhang, Hao; Yan, Xiaohong; Huang, Yundi; Zhang, Mengru; Tang, Yawen; Sun, Dongmei; Xu, Lin; Wei, Shaohua

    2017-02-01

    For Pd-based nanocatalysts, stabilization of Pd nanoparticles on carbon support could not only effectively avoid particle aggregation and maintain catalytic stability during catalytic processes, but also facilitate enhancing the catalytic activity due to the synergy between Pd nanoparticles and carbon support. Furthermore, the incorporation of non-metal of phosphorus (P) into Pd could effectively modulate the electronic structure of Pd and thus help to boost the catalytic properties. However, one-pot synthesis of such nanohybrids remains a great challenge due to the distinct physiochemical properties of Pd, P and C components. Herein, we demonstrate a one-pot and scalable synthesis of highly dispersed PdP alloy nanoparticle-immobilized on N-doped graphitic carbon nanosheets (abbreviated as Pd-P@N-C nanosheets) by using inorganic-organic hybrid cyanogel as a reaction precursor. In virtue of both compositional and structural advantages, the as-synthesized Pd-P@N-C nanosheets manifest a superior catalytic activity and stability toward the hydrogenation of 4-nitrophenol (4-NP). We believe that the present work will provide a feasible and versatile strategy for the development of efficient catalysts for environmental remediation and can also be extendable to other carbon-based nanohybrids with desirable functionalities.

  17. One-pot synthesis and visible light photocatalytic activity of monodispersed AgIn{sub 5}S{sub 8} microspheres

    SciTech Connect

    Li, Xiangqing; Wang, Lei; Wei, Dailong; Kang, Shizhao; Mu, Jin

    2013-02-15

    Graphical abstract: Display Omitted Highlights: ► Monodispersed AgIn{sub 5}S{sub 8} microspheres were prepared in a one-pot process. ► The process is environmental friendly. ► The AgIn{sub 5}S{sub 8} microspheres display high photocatalytic activity. -- Abstract: Monodispersed AgIn{sub 5}S{sub 8} microspheres were synthesized using a one-pot solution method and characterized with X-ray diffraction, UV–vis diffuse reflectance spectroscopy, scanning electron microscope, energy dispersive X-ray spectroscopy and N{sub 2} adsorption–desorption isotherm. The results indicated that the AgIn{sub 5}S{sub 8} microspheres were of cubic spinel structure and the mean diameter of about 0.5 μm. In addition, the visible light photocatalytic activity of AgIn{sub 5}S{sub 8} microspheres was also investigated at room temperature. The AgIn{sub 5}S{sub 8} microspheres showed very high photocatalytic activity for the degradation of methyl orange with a degradation efficiency of about 98% under visible light irradiation for 20 min.

  18. WO3/g-C3N4 composites: one-pot preparation and enhanced photocatalytic H2 production under visible-light irradiation

    NASA Astrophysics Data System (ADS)

    Cheng, Cheng; Shi, Jinwen; Hu, Yuchao; Guo, Liejin

    2017-04-01

    A series of WO3/g-C3N4 composites with different WO3 contents were prepared via a facile one-pot pyrolysis method, and showed notably enhanced visible-light-driven photocatalytic H2-evolution activities, with the highest rate of 400 μmol h‑1 gcat ‑1 that was 15.0 times of that for pristine g-C3N4. Contents and sizes of WO3 crystallites in the composites were easily adjusted by changing the molar ratios of (NH4)2WS4 to C3H6N6 in the feed reagents, thereby successfully optimizing the Z-scheme system constructed by WO3 and g-C3N4 and thus effectively reducing the recombination of photogenerated charge carriers in g-C3N4. Moreover, pore volumes and surface areas of the composites were gradually enlarged by introducing WO3 into g-C3N4 via the one-pot preparation strategy, therefore promoting the redox reactions to evolve H2. This work presented an effective route to simultaneously optimize the phase compositions and textural structures of photocatalysts for enhanced H2 evolution.

  19. One-pot synthesis of silicon based nanoparticles with incorporated phthalocyanine for long-term bioimaging and photo-dynamic therapy of tumors.

    PubMed

    Liu, Jiaojiao; Wang, Rui; Wu, Sicong; Yuan, Bing; Bao, Meimei; Li, Jingliang; Dou, Yujiang; He, Yao; Yang, Kai

    2017-03-01

    Combining the merits of delivery vectors with drug molecules is one of the key directions for development of efficient cancer monitoring and treatment techniques. In this work, a novel type of silicon based composite nanoparticles (NPs) with incorporated hydrophobic phthalocyanine molecules (Pc) was synthesized via a facile one-pot method. The as-synthesized Pc@Si NPs, with a small size of 4.2 ± 0.8 nm, have excellent dispersibility in water and good biocompatibility with cells, in addition to favorable photoluminescence and robust photostability even in cells. Moreover, the Pc@Si NPs show significant in vitro cancer cell killing and in vivo tumor inhibiting abilities upon near-infrared light exposure, due to the photodynamic therapy (PDT) effect of Pc. This work develops an efficient fluorescent PDT drug carrier; moreover, the facile one-pot synthesis strategy may be used generally to prepare silicon-based composite NPs incorporated with diverse hydrophobic drugs/diagnostic molecules for a wide range of biomedical applications.

  20. Facile, one-pot solvothermal method to synthesize ultrathin Sb2S3 nanosheets anchored on graphene.

    PubMed

    Lu, Baoping; Tang, Jilin

    2014-10-07

    Ultrathin, two-dimensional (2D) nanosheets of layered transition-metal chalcogenides are theoretically and technologically intriguing. However, it still remains a great challenge to synthesize ultrathin nanosheets because of the lack of an intrinsic driving force for the anisotropic growth of 2D superposed microstructures. Here we demonstrate, for the first time to our knowledge, the in situ synthesis of large-scale ultrathin Sb2S3 nanosheets on graphene sheets (G) by solvothermal method in a water-ethylene glycol mixed solvent. Owing to the synergetic chemical coupling effects between G and Sb2S3, Sb2S3-G hybrid nanosheets exhibit high catalytic performance for the degradation of methylene blue in the presence of H2O2. Moreover, it was found that the resulting Sb2S3-G shows good electrocatalytic activity towards hydrazine oxidation. This work not only offers a low-cost and high performance alternative technology for synthesizing sheet-like Sb2S3, but also opens the door toward the fabrication of varying types of metal sulfide-graphene nanomaterials that will have wide applications in catalysis, environmental, and new energy fields.

  1. One-pot synthesis of crosslinked amphiphilic polycarbonates as stable but reduction-sensitive carriers for doxorubicin delivery

    NASA Astrophysics Data System (ADS)

    Yi, Xiaoqing; Zhang, Quan; Dong, Hui; Zhao, Dan; Xu, Jia-qi; Zhuo, Renxi; Li, Feng

    2015-10-01

    In this paper, we first synthesized a novel disulfide-coupled bis-(cyclic carbonate) (TDCSS) monomer. After ring-opening co-polymerization (ROP) of TDCSS and trimethylene carbonate (TMC) initiated by mono-methoxyl poly(ethylene glycol), the crosslinked reduction-sensitive copolymer PEG-P(TMC-co-TDCSS) was obtained via a facile one-step procedure for efficient delivery of doxorubicin (DOX) into cancer cells. To serve as controls, PEG-P(TMC-co-TDCCC), which has an analogous structure without disulfide bond, and a linear polymer PEG-PTMC were also prepared. The copolymers could self-assemble to form nano-sized micelles in an aqueous solution. As compared to PEG-PTMC, crosslinked PEG-P(TMC-co-TDCSS) and PEG-P(TMC-co-TDCCC) showed lower CMC values and thus induced a much better micelle-forming ability. In vitro release studies revealed that the drug release behavior of DOX-loaded PEG-P(TMC-co-TDCSS) micelles, which could be accelerated in the presence of 10 mM dithiothreitol (DTT), showed a similar trend in the absence of DTT compared to DOX-loaded PEG-P(TMC-co-TDCCC) micelles. Furthermore, confocal laser scanning microscopy (CLSM) indicated that DOX-loaded PEG-P(TMC-co-TDCSS) micelles were efficiently internalized into HeLa cells, releasing DOX into the cytoplasm after which the drug finally entered the nuclei, while MTT assays also demonstrated potent cytotoxic activity against HeLa cells. DOX was mainly located in the cytoplasm for reduction-insensitive PEG-P(TMC-co-TDCCC) and PEG-PTMC controls.

  2. Ultrasonic irradiation-promoted one-pot synthesis of CH3NH3PbBr3 quantum dots without using flammable CH3NH2 precursor

    NASA Astrophysics Data System (ADS)

    Jiang, Han; Wang, Chunlei; Lv, Changgui; Xu, Shuhong; Zhu, Li; Zhang, Ruohu; Cui, Yiping

    2017-02-01

    At present, the CH3NH3PbBr3 quantum dots (QDs) reported in the literature usually contain two synthesis steps: the initial preparation of CH3NH3Br via the reaction of flammable CH3NH2 and HBr, together with the subsequent formation of CH3NH3PbBr3 QDs. To avoid the use of dangerous CH3NH2, this work develops a novel one-pot method for synthesizing CH3NH3PbBr3 QDs using safe and commercially available reactants (CH3NH3Cl, KBr and PbCl2). It is found that ultrasonic treatment plays a key role during the synthesis of CH3NH3PbBr3 QDs. Without ultrasonic irradiation, it is not possible to synthesize CH3NH3PbBr3 QDs under heating or vigorous stirring. Aliquots of samples taken at different ultrasonic irradiation time intervals show a time-dependent redshift in the emission wavelength. This suggests the formation of CH3NH3PbCl3 QDs first, followed by the formation of CH3NH3PbBr3 QDs through ultrasonically promoted halide exchange. Moreover, mixed CH3NH3PbCl x Br3‑x QDs with a tunable emission wavelength can also be prepared through this one-pot method by controlling the ultrasonic irradiation time. In comparison to the previous two-step method, the current one-pot method is simpler, less time-consuming and does not use flammable CH3NH2. The as-prepared CH3NH3PbBr3 QDs show a comparable photoluminescence (PL) quantum yield (QY) to that of the literature. What is more, the ultrasonic time-controlled emission wavelength of CH3NH3PbCl x Br3‑x QDs also provides an alternative way of tuning QD emission to the traditional way of controlling the halide ratios.

  3. One-pot synthesis of silicon nanoparticles trapped in ordered mesoporous carbon for use as an anode material in lithium-ion batteries.

    PubMed

    Park, Junsu; Kim, Gil-Pyo; Nam, Inho; Park, Soomin; Yi, Jongheop

    2013-01-18

    Silicon nanoparticles trapped in an ordered mesoporous carbon composite were prepared by a one-step self-assembly with solvent evaporation using the triblock copolymer Pluronic F127 and a resorcinol-formaldehyde polymer as the templating agent and carbon precursor respectively. Such a one-pot synthesis of Si/ordered mesoporous carbon nanocomposite is suitable for large-scale synthesis. Characterization confirmed that the Si nanoparticles were trapped in the ordered mesoporous carbon, as evidenced by transmission electron microscopy, x-ray diffraction analysis and nitrogen sorption isotherms. The composite showed a high reversible capacity above 700 mA h g(-1) during 50 cycles at 2 A g(-1). The improved electrochemical performance of the composite can be ascribed to the buffering effect of spaces formed in the ordered pore channels during the volume expansion of silicon and the rapid movement of lithium ions through the uniform cylindrical pore structure of the mesopores.

  4. One-pot chemical synthesis of small ubiquitin-like modifier protein-peptide conjugates using bis(2-sulfanylethyl)amido peptide latent thioester surrogates.

    PubMed

    Boll, Emmanuelle; Drobecq, Hervé; Ollivier, Nathalie; Blanpain, Annick; Raibaut, Laurent; Desmet, Rémi; Vicogne, Jérôme; Melnyk, Oleg

    2015-02-01

    Small ubiquitin-like modifier (SUMO) post-translational modification (PTM) of proteins has a crucial role in the regulation of important cellular processes. This protocol describes the chemical synthesis of functional SUMO-peptide conjugates. The two crucial stages of this protocol are the solid-phase synthesis of peptide segments derivatized by thioester or bis(2-sulfanylethyl)amido (SEA) latent thioester functionalities and the one-pot assembly of the SUMO-peptide conjugate by a sequential native chemical ligation (NCL)/SEA native peptide ligation reaction sequence. This protocol also enables the isolation of a SUMO SEA latent thioester, which can be attached to a target peptide or protein in a subsequent step. It is compatible with 9-fluorenylmethoxycarbonyl (Fmoc) chemistry, and it gives access to homogeneous, reversible and functional SUMO conjugates that are not easily produced using living systems. The synthesis of SUMO-peptide conjugates on a milligram scale takes 20 working days.

  5. Unsaturated C3,5,7,9-Monocarboxylic Acids by Aqueous, One-Pot Carbon Fixation: Possible Relevance for the Origin of Life

    NASA Astrophysics Data System (ADS)

    Scheidler, Christopher; Sobotta, Jessica; Eisenreich, Wolfgang; Wächtershäuser, Günter; Huber, Claudia

    2016-06-01

    All scientific approaches to the origin of life share a common problem: a chemical path to lipids as main constituents of extant cellular enclosures. Here we show by isotope-controlled experiments that unsaturated C3,5,7,9-monocarboxylic acids form by one-pot reaction of acetylene (C2H2) and carbon monoxide (CO) in contact with nickel sulfide (NiS) in hot aqueous medium. The primary products are toto-olefinic monocarboxylic acids with CO-derived COOH groups undergoing subsequent stepwise hydrogenation with CO as reductant. In the resulting unsaturated monocarboxylic acids the double bonds are mainly centrally located with mainly trans-configuration. The reaction conditions are compatible with an origin of life in volcanic-hydrothermal sub-seafloor flow ducts.

  6. One-pot, template- and surfactant-free solvothermal synthesis of high-crystalline Fe3O4 nanostructures with adjustable morphologies and high magnetization

    NASA Astrophysics Data System (ADS)

    Zong, Yan; Xin, Hongna; Zhang, Jiarui; Li, Xinghua; Feng, Juan; Deng, Xia; Sun, Yong; Zheng, Xinliang

    2017-02-01

    In the present study, high-crystalline and well-defined Fe3O4 nanostructures with tunable morphologies were fabricated through a facile one-pot solvothermal approach. The morphology, crystal structure and chemical compositions of the products were characterized at the nanoscale. X-ray diffraction and selected area electron diffraction patterns indicate that the products have a pure spinel phase without the presence of any other impurity. Based on the transmission electron microscope technology, shape evolution of the products were investigated. Several morphologies including irregular particles, clusters, hollow sphere and octahedrons can be obtained by only adjusting the amount of NaOH without using any surfactant. Magnetism investigations show that all the products perform ferromagnetic behavior with high saturation magnetization at room temperature, which mainly originates from their high crystalline nature and template-free fabrication process.

  7. One-Pot Fabrication of Mesoporous Core-Shell Au@PtNi Ternary Metallic Nanoparticles and Their Enhanced Efficiency for Oxygen Reduction Reaction.

    PubMed

    Shi, Qiurong; Zhu, Chengzhou; Fu, Shaofang; Du, Dan; Lin, Yuehe

    2016-02-01

    Currently, Pt-based nanomaterials with tailorable shapes, structures, and morphologies are the most popular electrocatalysts for oxygen reduction reaction, which is a significant cathode reaction in fuel cells for renewable energy applications. We have successfully synthesized mesoporous core-shell Au@PtNi ternary metallic nanoparticles through a one-pot reduction method for cathodic materials used as oxygen reduction reaction catalysts. The as-synthesized nanoparticles exhibited superior catalytic activities and long-term stabilities compared with mesoporous core-shell Au@Pt nanoparticles and commercial Pt/C. The unique mesoporous core-shell structures as well as the alloy shells enable the enhanced electrochemical oxygen reduction reaction performances of the Pt-based materials via the electronic effect and geometric effect, holding great promise in fuel cell application.

  8. One pot three components microwave assisted and conventional synthesis of new 3-(4-chloro-2-hydroxyphenyl)-2-(substituted) thiazolidin-4-one as antimicrobial agents.

    PubMed

    Pansare, Dattatraya N; Mulla, Nayeem A; Pawar, Chandrakant D; Shende, Vikas R; Shinde, Devanand B

    2014-08-01

    A one-pot, three-component, microwave assisted and conventional synthesis of new 3-(4-chloro-2-hydroxyphenyl)-2-(substituted) thiazolidin-4-one (4a-n) was carried out by using N,N-dimethylformamide as a solvent with high product yield. Among these synthesized compounds (4f, 4g, 4l and 4m) were found to be a broad spectrum molecule active against all bacterial and fungus strains tested, except fungus Aspergillus niger. Amongst the compounds (4g, 4l and 4m) were found to be more potent than respective standard drugs used in the experiment against Candida albicans, Staphylococcus aureus and Aspergillus flavus, respectively. All synthesized compounds were also tested for their cytotoxic activity against HeLa and MCF-7 cell lines by the sulforhodamine B (SRB) assay. This study shows that all compounds were non-cytotoxic in nature, and confirmed their antimicrobial specificity apart from any general cytotoxicity.

  9. One-pot enzymatic synthesis of docosahexaenoic acid-rich triacylglycerols at the sn-1(3) position using by-product from selective hydrolysis of tuna oil.

    PubMed

    Nagao, Toshihiro; Watanabe, Yomi; Maruyama, Kazuaki; Momokawa, Yuusuke; Kishimoto, Noriaki; Shimada, Yuji

    2011-01-31

    Docosahexaenoic acid (DHA)-rich oil has been industrially produced by selective hydrolysis of tuna oil with a lipase that acts weakly on DHA. The free fatty acids (FFAs) generated in this process as by-products contain a high DHA concentration (46wt%) but are treated as industrial waste. This study attempted to reuse these by-product FFAs using a one-pot process, and succeeded in producing triacylglycerols (TAGs) through the esterification of the by-product FFAs with glycerol using immobilized Rhizomucor miehei lipase. Regiospecific analysis of the resulting TAGs showed that the content of DHA at the sn-1(3) position (51.7mol%) was higher than the content of DHA at the sn-2 position (17.3mol%). The DHA distribution in TAGs synthesized in this study was similar to the DHA distribution in TAGs from seal oil.

  10. One-pot green synthesis of Prussian blue nanocubes decorated reduced graphene oxide using mushroom extract for efficient 4-nitrophenol reduction.

    PubMed

    Chen, Ruixue; Zhang, Qiuping; Gu, Yue; Tang, Liu; Li, Cong; Zhang, Zhiquan

    2015-01-01

    One-pot green approach to the synthesis of Prussian blue nanocubes/reduced graphene oxide (PBNCs/RGO) nanocomposite had been attempted. It was based on the extract of mushroom with K3[Fe(CN)6] and graphene oxide (GO) as precursors, where the reduction of GO and the deposition of PBNCs occurred simultaneously. The obtained nanocomposite was characterized by transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray diffraction (XRD), Raman spectroscopy and electrochemical techniques. With the introduction of β-cyclodextrin (β-CD), the β-CD/PBNCs/RGO system showed linear behavior in the range from 0.01 to 700 μM for 4-nitrophenol with a low detection limit of 2.34 nM (S/N=3).

  11. Click chemistry inspired one-pot synthesis of 1,4-disubstituted 1,2,3-triazoles and their Src kinase inhibitory activity.

    PubMed

    Kumar, Dalip; Reddy, V Buchi; Kumar, Anil; Mandal, Deendayal; Tiwari, Rakesh; Parang, Keykavous

    2011-01-01

    Two classes of 1,4-disubstituted 1,2,3-triazoles were synthesized using one-pot reaction of α-tosyloxy ketones/α-halo ketones, sodium azide, and terminal alkynes in the presence of aq PEG (1:1, v/v) using the click chemistry approach and evaluated for Src kinase inhibitory activity. Structure-activity relationship analysis demonstrated that insertion of C(6)H(5)- and 4-CH(3)C(6)H(4)- at position 4 for both classes and less bulkier aromatic group at position 1 in class 1 contribute critically to the modest Src inhibition activity (IC(50) = 32-43 μM) of 1,4-disubstituted 1,2,3-triazoles.

  12. Unsaturated C3,5,7,9-Monocarboxylic Acids by Aqueous, One-Pot Carbon Fixation: Possible Relevance for the Origin of Life

    PubMed Central

    Scheidler, Christopher; Sobotta, Jessica; Eisenreich, Wolfgang; Wächtershäuser, Günter; Huber, Claudia

    2016-01-01

    All scientific approaches to the origin of life share a common problem: a chemical path to lipids as main constituents of extant cellular enclosures. Here we show by isotope-controlled experiments that unsaturated C3,5,7,9-monocarboxylic acids form by one-pot reaction of acetylene (C2H2) and carbon monoxide (CO) in contact with nickel sulfide (NiS) in hot aqueous medium. The primary products are toto-olefinic monocarboxylic acids with CO-derived COOH groups undergoing subsequent stepwise hydrogenation with CO as reductant. In the resulting unsaturated monocarboxylic acids the double bonds are mainly centrally located with mainly trans-configuration. The reaction conditions are compatible with an origin of life in volcanic-hydrothermal sub-seafloor flow ducts. PMID:27283227

  13. Supramolecular capping-ligand effect of lamellar silica mesostructures for the one-pot synthesis of highly dispersed ZnO nanoparticles

    NASA Astrophysics Data System (ADS)

    Fernández, Lorenzo; Garro, Núria; Morales, José Manuel; Burguete, Pedro; Latorre, Julio; Guillem, Carmen; Beltrán, Aurelio; Beltrán, Daniel; Amorós, Pedro

    2006-09-01

    ZnO-SiO2 lamellar nanocomposites with high zinc content (5<=Si/Zn<=50) have been synthesized through a one-pot surfactant-assisted procedure from aqueous solution and starting from molecular atrane complexes of Zn and Si as inorganic hydrolytic precursors. This approach allows optimization of the dispersion of the ZnO nanodomains in the silica sheets. The nature of the layered silica materials has been confirmed by x-ray diffraction. Spectroscopic (ultraviolet-visible and photoluminescence) study of these layered silica materials shows that, regardless of the Si/Zn ratio, Zn atoms are organized in well-dispersed, uniform ZnO nanodomains (about 1.2 nm) partially embedded within the silica sheets. Quantum confinement effects have been observed in the optical response of the ZnO nanoparticles included in these nanocomposites.

  14. Type II Anion Relay Chemistry: Exploiting Bifunctional Weinreb Amide Linchpins for the One-Pot Synthesis of Differentiated 1,3-Diketones, Pyrans, and Spiroketals

    PubMed Central

    Farrell, Mark; Melillo, Bruno

    2016-01-01

    The design, synthesis, and validation of new highly effective bifunctional linchpins for type II anion relay chemistry (ARC) has been achieved. The mechanistically novel negative-charge migration that comprises the Brook rearrangement is now initiated by a stabilized tetrahedral intermediate, which is generated by nucleophilic addition to a Weinreb amide, rather than by a simple oxyanion that is generated from an epoxide. As a result, the linchpin preserves the carbonyl functionality in the ARC adducts, thus permitting access to functionally complex systems in a single flask without the need for further chemical manipulations. This tactic was validated with the one-pot preparation of monoprotected 1,3-diketones as well as pyran and spiroketal scaffolds, depending on the choice of nucleophile, electrophile, and work-up conditions. PMID:26586577

  15. Inorganic-organic hybrid silica based tin complex as a novel, highly efficient and recyclable heterogeneous catalyst for the one-pot preparation of spirooxindoles in water.

    PubMed

    Ghahremanzadeh, Ramin; Rashid, Zahra; Zarnani, Amir-Hassan; Naeimi, Hossein

    2014-11-14

    In the present study, a tin complex immobilized on silica gel as a novel, green, highly efficient and heterogeneous reusable catalyst was synthesized by grafting 2-amino benzamide onto the silica gel surface as a result of the reaction between isatoic anhydride and 3-aminopropyl-functionalized silica gel, followed by complexing with tin chloride. The resulting organic-inorganic hybrid material was evaluated in the one-pot three-component synthesis of spiro[indoline-pyrazolo[4',3':5,6]pyrido[2,3-d]pyrimidine]trione derivatives in water via the condensation reaction of isatins, barbituric acids, and 1H-pyrazol-5-amines. All the reactions were completed in short reaction times and all the products were obtained in high to excellent yields with high purity. In addition, the synthesized novel catalyst could be separated from the reaction mixture by simple filtration and can be reused up to seven runs without significant loss in activity.

  16. One-pot synthesis, structural characterization, UV-Vis and electrochemical analyses of new Schiff base complexes of Fe(III), Ni(II) and Cu(II)

    NASA Astrophysics Data System (ADS)

    Back, Davi Fernando; de Oliveira, Gelson Manzoni; Fontana, Liniquer Andre; Ramão, Brenda Fiorin; Roman, Daiane; Iglesias, Bernardo Almeida

    2015-11-01

    The complexes [Ni(Pyr2tetam-2H)]·2H2O (1) (Pyr2tetam = (pyridoxyl)2-N1,N4-triethylenetetramine), [Fe(Pyr2tetam-2H)](ClO4)·H2O (2) and [Cu(Pyrtetam-H)](ClO4) (3) (Pyrtetam = pyridoxyl-N1-triethylenetetramine) were obtained through one pot reactions of triethylenetetramine, pyridoxal chloridrate, triethylamine and the metal salts Ni(ClO4)2·6H2O, Fe(ClO4)2·6H2O and Cu(ClO4)2·6H2O. In complexes 1 and 2 the metal centers present a distorted octahedral coordination, while complex 3 shows a square pyramidal configuration. The structures were characterized through X-ray diffractometry, IR and UV-Vis spectra. Cyclic voltammograms of the title compounds are also presented and discussed.

  17. Novel ultrasound-promoted parallel synthesis of trifluoroatrolactamide library via a one-pot Passerini/hydrolysis reaction sequence and their fungicidal activities.

    PubMed

    Yu, Shu-Jing; Zhu, Cong; Bian, Qiang; Cui, Can; Du, Xiu-Jiang; Li, Zheng-Ming; Zhao, Wei-Guang

    2014-01-13

    An ultrasound-promoted one-pot Passerini/hydrolysis reaction sequence has been developed for the synthesis of trifluoroatrolactamide derivatives using a diverse range of trifluoroacetophenones and isonitriles in acetic acid. Parallel synthesis in a centrifuge tube using a noncontact ultrasonic cell crusher was used in this study as an efficient method for the rapid generation of combinatorial trifluoroatrolactamide libraries, and subsequent biochemical evaluation of the resulting compounds indicated that they possessed excellent broad-spectrum fungicidal activities. N-(4-chlorophenyl)-2-(4-ethylphenyl)-3,3,3-trifluoro-2-hydroxypropanamide and N-(4-chlorophenyl)-3,3,3-trifluoro-2-hydroxy-2-(4-methoxyphenyl)propanamide, in particular, showed significant fungicidal activities against all of the fungal species tested in the current study.

  18. Design and one-pot synthesis of alpha-aminophosphonates and bis(alpha-aminophosphonates) by iron(III) chloride and cytotoxic activity.

    PubMed

    Rezaei, Zahra; Firouzabadi, Habib; Iranpoor, Nasser; Ghaderi, Abbas; Jafari, Mohammad Reza; Jafari, Abbas Ali; Zare, Hamid Reza

    2009-11-01

    In this study, we used a solution of FeCl(3) in THF to facilitate the Mannich-type reaction of aldehyde, amine and phosphite compounds to form corresponding alpha-aminophosphonates in a one-pot, three-component reaction. Selected alpha-aminophosphonates were entered into a biological assay test and were studied by docking methods, using Autodock 3.0. The results showed that the reactions were carried out mildly and eco-friendly to form alpha-aminophosphonates in high yields. Some were found to have cytotoxic activity on the cell lines RAJI, JURKAT and MCF-7. An indole derived bis(alpha-aminophosphonates) showed maximum cytotoxic effect comparable to doxorubicin. Although the FDE (Final Docking Energy) for the most cytotoxic compound was of the most negative value, there is no correlation between FDE and cytotoxicity.

  19. Versatile acetylation of carbohydrate substrates with bench-top sulfonic acids and application to one-pot syntheses of peracetylated thioglycosides.

    PubMed

    Chao, Chin-Sheng; Chen, Min-Chun; Lin, Shih-Che; Mong, Kwok-Kong T

    2008-04-07

    Inexpensive and readily available sulfonic acids, p-toluenesulfonic acid, and sulfuric acid are versatile and efficient catalysts for the peracetylation of a broad spectrum of carbohydrate substrates in good yield and in a practical time frame. Three appealing features in sulfonic acid-catalyzed acetylation of free sugars were explored including (1) suppression of furanosyl acetate formation for D-galactose and L-fucose; (2) high yielding chemoselective acetylation of sialic acid under appropriate conditions; and (3) peracetylation of amino sugars with different amino protecting functions. Simple one-pot two step acetylation-thioglycosidation methods for the expeditious synthesis of p-tolyl per-O-acetyl thioglycosides were also delineated.

  20. β-Cyclodextrin-Propyl Sulfonic Acid Catalysed One-Pot Synthesis of 1,2,4,5-Tetrasubstituted Imidazoles as Local Anesthetic Agents.

    PubMed

    Ran, Yan; Li, Ming; Zhang, Zong-Ze

    2015-11-12

    Some functionalized 1,2,4,5-tetrasubstituted imidazole derivatives were synthesized using a one-pot, four component reaction involving 1,2-diketones, aryl aldehydes, ammonium acetate and substituted aromatic amines. The synthesis has been efficiently carried out in a solvent free medium using β-cyclodextrin-propyl sulfonic acid as a catalyst to afford the target compounds in excellent yields. The local anesthetic effect of these derivatives was assessed in comparison to lidocaine as a standard using a rabbit corneal and mouse tail anesthesia model. The three most potent promising compounds were subjected to a rat sciatic nerve block assay where they showed considerable local anesthetic activity, along with minimal toxicity. Among the tested analogues, 4-(1-benzyl-4,5-diphenyl-1H-imidazol-2-yl)-N,N-dimethylaniline (5g) was identified as most potent analogue with minimal toxicity. It was further characterized by a more favourable therapeutic index than the standard.

  1. ZnO Nanoparticles as an Efficient, Heterogeneous, Reusable, and Ecofriendly Catalyst for Four-Component One-Pot Green Synthesis of Pyranopyrazole Derivatives in Water

    PubMed Central

    Sachdeva, Harshita; Saroj, Rekha

    2013-01-01

    An extremely efficient catalytic protocol for the synthesis of a series of pyranopyrazole derivatives developed in a one-pot four-component approach in the presence of ZnO nanoparticles as heterogeneous catalyst using water as a green solvent is reported. Greenness of the process is well instituted as water is exploited both as reaction media and medium for synthesis of catalyst. The ZnO nanoparticles exhibited excellent catalytic activity, and the proposed methodology is capable of providing the desired products in good yield (85–90%) and short reaction time. After reaction course, ZnO nanoparticles can be recycled and reused without any apparent loss of activity which makes this process cost effective and hence ecofriendly. All the synthesized compounds have been characterized on the basis of elemental analysis, IR, 1H NMR, and 13C NMR spectral studies. PMID:24282386

  2. An effective one-pot access to polynuclear dispiroheterocyclic structures comprising pyrrolidinyloxindole and imidazothiazolotriazine moieties via a 1,3-dipolar cycloaddition strategy

    PubMed Central

    Izmest’ev, Alexei N; Sigay, Natalya V; Serkov, Sergei A; Kachala, Vadim V; Shashkov, Alexander S; Zanin, Igor E; Kravchenko, Angelina N; Makhova, Nina N

    2016-01-01

    An effective and highly regio- and diastereoselective one-pot method for the synthesis of new polynuclear dispiroheterocyclic systems with five stereogenic centers (dispiro[imidazo[4,5-e]thiazolo[3,2-b]-1,2,4-triazine-6,3′-pyrrolidine-2′,3′′-indoles]) comprising pyrrolidinyloxindole and imidazo[4,5-e]thiazolo[3,2-b]-1,2,4-triazine moieties has been developed. The method relies on a 1,3-dipolar cycloaddition of azomethine ylides generated in situ from isatin derivatives and sarcosine to 6-benzylideneimidazo[4,5-e]thiazolo[3,2-b]-1,2,4-triazine-2,7-diones. PMID:28144290

  3. One-pot synthesis of porous Fe3O4 shell/silver core nanocomposites used as recyclable magnetic antibacterial agents

    NASA Astrophysics Data System (ADS)

    Fang, Weijun; Zheng, Jun; Chen, Cheng; Zhang, Huabing; Lu, Yunxia; Ma, Ling; Chen, Guangjun

    2014-05-01

    Porous Fe3O4 shell/silver core nanocomposites featuring sustainable and recyclable antibacterial activity have been successfully prepared via a facile one-pot hydrothermal method. The unique structural feature of the Ag@Fe3O4 nanocomposites with Ag embedded in porous Fe3O4 shell endows them with the ability of sustained-release of silver ions. Their antimicrobial activity studies were investigated on both Gram negative Escherichia coli and Gram positive Bacillus subtilis, which demonstrate that the nanocomposites are highly toxic to microorganisms and exhibit sustainable antibacterial activity. Besides, the Ag@Fe3O4 nanocomposites can be separated easily from the medium by a small magnet, which provided an effective way to eliminate the residual nanosilver from the surroundings. We finally demonstrate that the recovered nanocomposites exhibit recyclable antibacterial activity, acting as an ideal long-acting antibacterial agent.

  4. An alkaline one-pot reaction to synthesize luminescent Eu-BTC MOF nanorods, highly pure and water-insoluble, under room conditions

    NASA Astrophysics Data System (ADS)

    Medina-Velazquez, D. Y.; Alejandre-Zuniga, B. Y.; Loera-Serna, S.; Ortiz, E. M.; Morales-Ramirez, A. de J.; Garfias-Garcia, E.; Garcia-Murillo, A.; Falcony, C.

    2016-12-01

    The increasing demand for optoelectronic devices requires the development of luminescent materials with high luminescence efficiency and low energy demands, and the metalorganic frameworks (MOFs) with lanthanides ions offer great potential in this area. The metalorganic materials provide properties of flexibility, low density, low-cost methods of synthesis, and insolubility in water, which gives them an advantage over traditional phosphors. In this study, a benzenetricarboxylate ligand (BTC) with a Eu3+ MOF was synthesized, and its structural and luminescent properties were measured. The metalorganic compound was generated in a one-pot reaction from europium nitrate and trimesic acid precursors. Through characterization by X-ray diffraction powder, infrared spectroscopy, SEM structural characterization, and luminescent spectroscopy, the formation of Europium benzenetricarboxylate (Eu-BTC) MOF nanorods was tested and the calculated value was in the range of 30-60 nm. A red luminescent emission with high intensity was observed for all the procedures.

  5. A novel one-pot and one-step microwave-assisted cyclization-methylation reaction of amino alcohols and acetylated derivatives with dimethyl carbonate and TBAC.

    PubMed

    Ochoa-Terán, Adrián; Guerrero, Leticia; Rivero, Ignacio A

    2014-01-01

    A simple and efficient microwave-assisted methodology for the synthesis of 4-substituted-3-methyl-1,3-oxazolidin-2-ones from amino alcohols catalyzed by a ionic liquid was developed. This novel one-pot and one-step cyclization-methylation reaction represents an easier and faster method than any other reported protocols that can be used to obtain the desired products in good yields and high purity. Applying microwave irradiation at 130°C in the presence of TBAC, dimethyl carbonate acts simultaneously as carbonylating and methylating agent and surprisingly promotes an in situ basic trans esterification when a N-acetylated amino alcohol is used as starting material. Furthermore, dimethyl carbonate worked better than diethyl carbonate in performing this reaction.

  6. A Novel One-Pot and One-Step Microwave-Assisted Cyclization-Methylation Reaction of Amino Alcohols and Acetylated Derivatives with Dimethyl Carbonate and TBAC

    PubMed Central

    Ochoa-Terán, Adrián; Guerrero, Leticia; Rivero, Ignacio A.

    2014-01-01

    A simple and efficient microwave-assisted methodology for the synthesis of 4-substituted-3-methyl-1,3-oxazolidin-2-ones from amino alcohols catalyzed by a ionic liquid was developed. This novel one-pot and one-step cyclization-methylation reaction represents an easier and faster method than any other reported protocols that can be used to obtain the desired products in good yields and high purity. Applying microwave irradiation at 130°C in the presence of TBAC, dimethyl carbonate acts simultaneously as carbonylating and methylating agent and surprisingly promotes an in situ basic trans esterification when a N-acetylated amino alcohol is used as starting material. Furthermore, dimethyl carbonate worked better than diethyl carbonate in performing this reaction. PMID:25692177

  7. Mechanostereoselective One-Pot Synthesis of Functionalized Head-to-Head Cyclodextrin [3]Rotaxanes and Their Application as Magnetic Resonance Imaging Contrast Agents.

    PubMed

    Fredy, Jean Wilfried; Scelle, Jérémy; Ramniceanu, Gregory; Doan, Bich-Thuy; Bonnet, Célia S; Tóth, Éva; Ménand, Mickaël; Sollogoub, Matthieu; Vives, Guillaume; Hasenknopf, Bernold

    2017-02-21

    A versatile, five-component, one-pot synthesis of cyclodextrin (CD) [3]rotaxanes using copper-catalyzed azide-alkyne cycloaddition has been developed. Head-to-head [3]rotaxanes of α-CD selectively functionalized by one or two gadolinium 1,4,7,10-tetraazacyclododecane-1,4,7-triacetic acid monoamide complexes were obtained mechanostereoselectively. The magnetic resonance imaging efficiency, expressed by the longitudinal proton relaxivity of the rotaxanes, was significantly improved as compared to the functionalized CD. In vitro and in vivo preclinical studies showed a higher contrast and retention in the kidney than gadolinium 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid complex, demonstrating the potential of these rotaxanes as MRI contrast agent.

  8. Unsaturated C3,5,7,9-Monocarboxylic Acids by Aqueous, One-Pot Carbon Fixation: Possible Relevance for the Origin of Life.

    PubMed

    Scheidler, Christopher; Sobotta, Jessica; Eisenreich, Wolfgang; Wächtershäuser, Günter; Huber, Claudia

    2016-06-10

    All scientific approaches to the origin of life share a common problem: a chemical path to lipids as main constituents of extant cellular enclosures. Here we show by isotope-controlled experiments that unsaturated C3,5,7,9-monocarboxylic acids form by one-pot reaction of acetylene (C2H2) and carbon monoxide (CO) in contact with nickel sulfide (NiS) in hot aqueous medium. The primary products are toto-olefinic monocarboxylic acids with CO-derived COOH groups undergoing subsequent stepwise hydrogenation with CO as reductant. In the resulting unsaturated monocarboxylic acids the double bonds are mainly centrally located with mainly trans-configuration. The reaction conditions are compatible with an origin of life in volcanic-hydrothermal sub-seafloor flow ducts.

  9. Acid-induced crystallinity enhancement of graphite-like C3N3+xHy synthesized through a facile one-pot approach

    NASA Astrophysics Data System (ADS)

    Yin, Hao; Guo, Qixun; He, Dingzeng; Li, Juntao; Sun, Shigang

    2017-02-01

    Graphite-like C3N3+xHy with s-triazine rings as building blocks were synthesized through a facile one-pot approach. It is surprising that the degree of crystallinity of the synthesized sample at 330 °C (sample CNH-330) was remarkably enhanced by the dilute hydrochloric acid treatment. The mechanism of the acid-induced crystallinity enhancement was preliminarily studied. XRD, FTIR, SEM, photoluminescence spectra, elemental analysis, and XPS were performed to investigate the composition and structure of the obtained samples. The remarkable enhancement of the degree of crystallinity may be attributed to the ordered formation of ammonium-salt-like structure by the reaction of HCl with dbnd NH or sbnd NH2 in CNH-330.

  10. Direct hydrogenation and one-pot reductive amidation of nitro compounds over Pd/ZnO nanoparticles as a recyclable and heterogeneous catalyst

    NASA Astrophysics Data System (ADS)

    Hosseini-Sarvari, Mona; Razmi, Zahra

    2015-01-01

    A novel Pd supported on ZnO nanoparticles was readily synthesized and characterized. The amount of palladium on ZnO is 9.84 wt% which was determined by ICP analysis and atomic absorption spectroscopy (AAS). Percentage of accessible Pd as active catalyst is also estimated to 2.72% based on the thermogravimetric (TG) analysis. This nano-sized Pd/ZnO with an average particle size of 20-25 nm and specific surface area 40.61 m2 g-1 was used as a new reusable heterogeneous catalyst for direct hydrogenation and one-pot reductive amidation of nitro compounds without the use of any ligands under atmospheric pressure. The catalyst can be recovered and recycled several times without marked loss of activity.

  11. One-pot synthesis of gold nanorods via autocatalytic growth of sonochemically formed gold seeds: the effect of irradiation time on the formation of seeds and nanorods.

    PubMed

    Okitsu, Kenji; Nunota, Yuho

    2014-11-01

    A one-pot synthesis for gold nanorods was developed using sonochemical reduction of gold ions in an aqueous solution in the presence of cetyltrimethylammonium bromide, silver nitrate, and ascorbic acid, where we focused on the autocatalytic growth of gold seeds formed by ultrasonic irradiation for short times. In growth experiments with these sonochemically formed gold seeds, sigmoidal shape growth curves were observed, and the induction period before growth began was longer for shorter irradiation times. This result indicated that the number of sonochemically formed gold seeds increased with increasing irradiation time. The average aspect ratio of the gold nanorods produced changed from 2.0 at an irradiation time of 0.5min to 3.6 at 15min. The gold nanorods produced were longer and wider when the irradiation time was shorter.

  12. Type II Anion Relay Chemistry: Exploiting Bifunctional Weinreb Amide Linchpins for the One-Pot Synthesis of Differentiated 1,3-Diketones, Pyrans, and Spiroketals.

    PubMed

    Farrell, Mark; Melillo, Bruno; Smith, Amos B

    2016-01-04

    The design, synthesis, and validation of new highly effective bifunctional linchpins for type II anion relay chemistry (ARC) has been achieved. The mechanistically novel negative-charge migration that comprises the Brook rearrangement is now initiated by a stabilized tetrahedral intermediate, which is generated by nucleophilic addition to a Weinreb amide, rather than by a simple oxyanion that is generated from an epoxide. As a result, the linchpin preserves the carbonyl functionality in the ARC adducts, thus permitting access to functionally complex systems in a single flask without the need for further chemical manipulations. This tactic was validated with the one-pot preparation of monoprotected 1,3-diketones as well as pyran and spiroketal scaffolds, depending on the choice of nucleophile, electrophile, and work-up conditions.

  13. Chitosan supported Zn(II) mixed ligand complexes as heterogeneous catalysts for one-pot synthesis of amides from ketones via Beckmann rearrangement

    NASA Astrophysics Data System (ADS)

    Anuradha; Kumari, Shweta; Layek, Samaresh; Pathak, Devendra D.

    2017-02-01

    Chitosan supported Zn(II) mixed ligand complexes have been synthesized and characterized by FT-IR, UV-Vis, TGA, XRD, FESEM, EDX, AAS and Elemental Analysis. These complexes have been found to be efficient and recyclable heterogeneous catalysts for the one-pot synthesis of amides via Beckmann rearrangement. All three complexes can be easily filtered out from the reaction medium and reused up to five times without significant loss of catalytic activity. The reported protocol is economical and novel in the sense that amides can be easily synthesized in only one-step. All products were obtained as white to off-white crystalline solids and fully characterized by 1H NMR, FT-IR and Mass Spectra.

  14. Experimental and theoretical study on one-pot, three-component route to 2H-indazolo[2,1-b]phthalazine-triones catalyzed by nano-alumina sulforic acid

    NASA Astrophysics Data System (ADS)

    Kiasat, Ali Reza; Noorizadeh, Siamak; Ghahremani, Mahboubeh; Saghanejad, Seyed Jafar

    2013-03-01

    A simple, efficient, and high yielding one-pot protocol for the synthesis of 2H-indazolo[2,1-b]phthalazine-trione derivatives has been developed by three-component coupling of phthalhydrazide, dimedone and some aromatic aldehydes in ecofriendly neat conditions promoted by nano-γ-alumina sulforic acid. This protocol avoids the use of expensive catalysts, toxic solvents and chromatographic separation. Also the proposed protocol was extended to the linear β-diketone (acetylaceton) instead of cyclic diketone (dimedone). The generality and functional tolerance of this convergent and environmentally benign method is demonstrated. The nature of each step of the suggested mechanism for this condensation reaction is also identified through Density Functional Theory (DFT) calculations using B3LYP/6-31G** level of theory. It is shown that the first step is charge controlled; whereas the second one is controlled by frontier molecular orbitals. The 1H and 13C chemical shift values together with the structural parameters of the title compound have been also computed and the scaled values have been compared with the corresponding experimental NMR and X-ray spectra. As a result, the calculated spectroscopic data and optimized geometry show a good agreement with the experimental results.

  15. A green one-pot three-component synthesis of spirooxindoles under conventional heating conditions or microwave irradiation by using Fe3O4@SiO2-imid-PMAn magnetic porous nanospheres as a recyclable catalyst

    NASA Astrophysics Data System (ADS)

    Esmaeilpour, Mohsen; Javidi, Jaber; Divar, Masoumeh

    2017-02-01

    An efficient, green and environmentally procedure for the synthesis of spirooxindole derivatives has been developed by a one-pot three-component reaction of isatin derivatives, activated methylene, and 1,3-dicarbonyl compounds in the presence of Fe3O4@SiO2-imid-PMAn magnetic nanocatalyst under conventional heating conditions in water or microwave irradiation under solvent-free conditions. The reactions under conventional heating conditions were compared with the microwave-assisted reactions. The suggested method offers several advantages such as excellent yields, short reaction times, operational simplicity, a cleaner reaction, absence of any tedious workup or purification and ease of recovery and reusability of the catalyst by a magnetic field. In addition, the excellent catalytic performance in a water medium and the easy preparation, thermal stability and separation of the catalyst make it a good heterogeneous system and a useful alternative to other heterogeneous catalysts. The catalyst can be easily recovered by a magnetic field and reused for six consecutive reaction cycles without significant loss of activity. Also, the morphology of Fe3O4@SiO2-imid-PMAn, particle size distribution and leaching of nano H3PMo12O40 (PMAn) after reaction cycles were investigated by scanning electron microscopy (SEM), dynamic light scattering (DLS), and inductively coupled plasma (ICP) analyzer.

  16. Amplification and modulation of fluorescent signals by using hybridization chain reactions for multiplexed sensing of biomolecules in a one-pot

    NASA Astrophysics Data System (ADS)

    Nishimura, Takahiro; Ogura, Yusuke; Yamada, Kenji; Ohno, Yuko; Tanida, Jun

    2014-02-01

    Fluorescence readout of molecular information is a promising approach for biomolecular sensing. For detection of enormous biomolecules via uorescence, biomolecular information should be converted to codes that can be readout easily and simultaneously. For the purpose, we study a biomolecule uorescence color (B/F) encoders that modulate uorescence signals by control of uorescence resonance energy transfer (FRET). The B/F encoder converts biomolecular signals into uorescent color codes represented with uorescent wavelengths and intensity levels. The combination offers a great number of codes for representing the biomolecular information. In this study, we discuss multiplexed detection of target biomolecules using B/F encoders. Use of the B/F encoders would offer a multiplexed biomolecular sensing in a one-pot without micro-fabrication like DNA microarray. In the experiments, we prepared B/F encoders based on two kinds of hybridization chain reactions (HCR) that make long double-stranded DNA polymers to control positions of uorescence and quencher molecules. In the B/F encoders, target molecules trigger to start assembling the polymer structures. The uorescent molecules in the absence of the targets are near the quenchers and the output uorescence is suppressed by FRET. The polymerization process separates the uorescent and quencher dyes and the uorescent signal increase. The experimental results show that the B/F encoders based on HCRs have linear and independent response to each target, and temporal signals during the encoding reactions are usable for multiplexed readout. This result leads to the multiplexed sensing in a one-pot by uorescent ampli cation and multiple uorescent color-coding.

  17. Accessing a Biologically Relevant Benzofuran Skeleton by a One-Pot Tandem Heck Alkynylation/Cyclization Reaction Using Well-Defined Palladium N-Heterocyclic Carbene Complexes.

    PubMed

    Kumar, Anuj; Gangwar, Manoj Kumar; Prakasham, A P; Mhatre, Darshan; Kalita, Alok Ch; Ghosh, Prasenjit

    2016-03-21

    Well-defined palladium N-heterocyclic carbene (NHC) complexes were employed in the one-pot tandem Heck alkynylation/cyclization sequence for preparing biologically relevant benzofuran compounds under copper-free conditions in a time-efficient step-reduced fashion. In particular, a series of binuclear palladium complexes, 1b-1e and 2b-2e, of the alkyl-bridged NHC ligands, namely, {1,1'-di-R1-4,4'-R2-di-1,2,4-triazoline-5,5'-diylid-2-ene] (R1 = i-Pr; R2 = -(CH2)2-, -(CH2)3-), and their mononuclear analogues, trans-(NHC)PdBr2(pyridine) (3b) and cis-(NHC)PdBr2(PPh3) (3c), successfully catalyzed the one-pot tandem Heck alkynylation/cyclization reaction of 2-iodophenol with a variety of terminal alkyne substrates, yielding 2-substituted benzofuran derivatives. The mononuclear complexes 3b and 3c were nearly half as active as the representative dinuclear analogue 1c under analogous reaction conditions, thereby implying that, at the same mole percent of the palladium loading, the monometallic 3b and 3c and the bimetallic 1c complexes were equally effective as catalysts. The two sites of the bimetallic complex 1c performed as two separate independent catalytic sites, displaying no cooperativity effect in the catalysis. Finally, the practical utility of the aforementioned catalysts was demonstrated for a representative catalyst 1c through the convenient synthesis of a key intermediate, 3-[2-(benzo[d][1,3]dioxol-5-yl)-7-methoxybenzofuran-5-yl]propan-1-ol, in a total-synthesis protocol of the natural product Egonol.

  18. A Fully-automated One-pot Synthesis of [18F]Fluoromethylcholine with Reduced Dimethylaminoethanol Contamination via [18F]Fluoromethyl Tosylate

    PubMed Central

    Rodnick, Melissa E.; Brooks, Allen F.; Hockley, Brian G.; Henderson, Bradford D.; Scott, Peter J. H.

    2013-01-01

    Introduction A novel one-pot method for preparing [18F]fluoromethylcholine ([18F]FCH) via in situ generation of [18F]fluoromethyl tosylate ([18F]FCH2OTs), and subsequent [18F]fluoromethylation of dimethylaminoethanol (DMAE), has been developed. Methods [18F]FCH was prepared using a GE TRACERlab FXFN, although the method should be readily adaptable to any other fluorine-18 synthesis module. Initially ditosylmethane was fluorinated to generate [18F]FCH2OTs. DMAE was then added and the reaction was heated at 120°C for 10 min to generate [18F]FCH. After this time, reaction solvent was evaporated, and the crude reaction mixture was purified by solid-phase extraction using C18-Plus and CM-Light Sep-Pak cartridges to provide [18F]FCH formulated in USP saline. The formulated product was passed through a 0.22 μm filter into a sterile dose vial, and submitted for quality control testing. Total synthesis time was 1.25 hours from end-of-bombardment. Results Typical non-decay-corrected yields of [18F]FCH prepared using this method were 91 mCi (7% non-decay corrected based upon ~1.3 Ci [18F]fluoride), and doses passed all other quality control (QC) tests. Conclusion A one-pot liquid-phase synthesis of [18F]FCH has been developed. Doses contain extremely low levels of residual DMAE (31.6 μg / 10 mL dose or ~3 ppm) and passed all other requisite QC testing, confirming their suitability for use in clinical imaging studies. PMID:23665261

  19. Multi-Component Dark Matter

    SciTech Connect

    Zurek, Kathryn M.

    2008-11-01

    We explore multi-component dark matter models where the dark sector consists of multiple stable states with different mass scales, and dark forces coupling these states further enrich the dynamics. The multi-component nature of the dark matter naturally arises in supersymmetric models, where both R parity and an additional symmetry, such as a Z{sub 2}, is preserved. We focus on a particular model where the heavier component of dark matter carries lepton number and annihilates mostly to leptons. The heavier component, which is essentially a sterile neutrino, naturally explains the PAMELA, ATIC and synchrotron signals, without an excess in antiprotons which typically mars other models of weak scale dark matter. The lighter component, which may have a mass from a GeV to a TeV, may explain the DAMA signal, and may be visible in low threshold runs of CDMS and XENON, which search for light dark matter.

  20. A one-pot, three-step process for the diastereoselective synthesis of aminobicyclo[4.3.0]nonanes using consecutive palladium(II)- and ruthenium(II)-catalysis.

    PubMed

    Mostafa, Mohamed A B; Grafton, Mark W; Wilson, Claire; Sutherland, Andrew

    2016-03-28

    A diastereoselective synthesis of highly substituted aminobicyclo[4.3.0]nonanes has been attained using a one-pot multi-bond forming process. A four-step synthetic route was developed for the efficient synthesis of a series of C-7 substituted hept-2-en-6-yn-1-ols. These compounds were then investigated as substrates for a one-pot, three-step tandem process involving a palladium(ii)-catalysed Overman rearrangement, a ruthenium(ii)-catalysed ring closing enyne metathesis reaction followed by a hydrogen bond directed Diels-Alder reaction. The optimisation of the one-pot process has allowed the rapid preparation of a library of aminobicyclo[4.3.0]nonanes with significant molecular complexity and up to four stereogenic centres.

  1. Photoinduced Multicomponent Reactions.

    PubMed

    Garbarino, Silvia; Ravelli, Davide; Protti, Stefano; Basso, Andrea

    2016-12-12

    The combination of multicomponent approaches with light-driven processes opens up new scenarios in the area of synthetic organic chemistry, where the need for sustainable, atom- and energy-efficient reactions is increasingly urgent. Photoinduced multicomponent reactions are still in their infancy, but significant developments in this area are expected in the near future.

  2. Multicomponent Syntheses of Macrocycles

    NASA Astrophysics Data System (ADS)

    Masson, Géraldine; Neuville, Luc; Bughin, Carine; Fayol, Aude; Zhu, Jieping

    How to access efficiently the macrocyclic structure remained to be a challenging synthetic topic. Although many elegant approaches/reactions have been developed, construction of diverse collection of macrocycles is still elusive. This chapter summarized the recently emerged research area dealing with multicomponent synthesis of macrocycles, with particular emphasis on the approach named "multiple multicomponent reaction using two bifunctional building blocks".

  3. Ultrasound mediation for one-pot sonosynthesis and deposition of magnetite nanoparticles on cotton/polyester fabric as a novel magnetic, photocatalytic, sonocatalytic, antibacterial and antifungal textile.

    PubMed

    Rastgoo, Madine; Montazer, Majid; Malek, Reza M A; Harifi, Tina; Mahmoudi Rad, Mahnaz

    2016-07-01

    A magnetic cotton/polyester fabric with photocatalytic, sonocatalytic, antibacterial and antifungal activities was successfully prepared through in-situ sonosynthesis method under ultrasound irradiation. The process involved the oxidation of Fe(2+) to Fe(3+) via hydroxyl radicals generated through bubbles collapse in ultrasonic bath. The treated samples were analyzed by X-ray diffraction, field emission scanning electron microscopy, energy dispersive X-ray spectroscopy and vibrating sample magnetometry. Photocatalytic and sonocatalytic activities of magnetite treated fabrics were also evaluated toward Reactive Blue 2 decoloration under sunlight and ultrasound irradiation. Central composite design based on response surface methodology was applied to study the influence of iron precursor, pH and surfactant concentration to obtain appropriate amount for the best magnetism. Findings suggested the potential of one-pot sonochemical method to synthesize and fabricate Fe3O4 nanoparticles on cotton/polyester fabric possessing appropriate saturation magnetization, 95% antibacterial efficiency against Staphylococcus aureus and 99% antifungal effect against Candida albicans, 87% and 70% dye photocatalytic and sonocatalytic decoloration along with enhanced mechanical properties using only one iron rich precursor at low temperature.

  4. Iridium ultrasmall nanoparticles, worm-like chain nanowires, and porous nanodendrites: One-pot solvothermal synthesis and catalytic CO oxidation activity

    NASA Astrophysics Data System (ADS)

    Zhang, Tao; Li, Shuai-Chen; Zhu, Wei; Ke, Jun; Yu, Jing-Wen; Zhang, Zhi-Ping; Dai, Lin-Xiu; Gu, Jun; Zhang, Ya-Wen

    2016-06-01

    We report a facile one-pot solvothermal synthesis of monodisperse iridium (Ir) ultrasmall (1.5-2.5 nm in diameter) nanoparticles (NPs), worm-like chain nanowires (NWs), and porous nanodendrites (NDs), for which CO oxidation reaction has been employed as a probe reaction to investigate the effects of nanoparticle size and surface-capping organics on the catalytic activities. Time-dependent experiments revealed that an oriented attachment mechanism induced by the strong adsorption of halide anions (Br- and I-) on specific facet of Ir nanoclusters or by decreasing the reduction rate of Ir precursors with changing their concentrations during the synthesis was responsible for the formation of Ir NWs and NDs. Annealing tests indicated that an O2-H2 atmosphere treatment turned out to be an effective measure to clean up the surface-capping organics of Ir NPs supported on commercial SiO2. Catalytic CO oxidation reaction illustrated that a significant improvement in the catalytic activity of CO oxidation reaction was achieved together with the changing of activation energies after such atmosphere treatment for the supported catalysts of the ultrasmall Ir NPs. It is noteworthy that this enhancement in catalytic activity could be ascribed to the changes in the surface status (including populations of Ir species in metallic and oxidized states, removal of surface capping organics, the variety of active sites, and total effective active site number) for the supported nanocatalysts during the atmosphere treatment.

  5. One-pot synthesis of carbon supported calcined-Mg/Al layered double hydroxides for antibiotic removal by slow pyrolysis of biomass waste

    NASA Astrophysics Data System (ADS)

    Tan, Xiaofei; Liu, Shaobo; Liu, Yunguo; Gu, Yanling; Zeng, Guangming; Cai, Xiaoxi; Yan, Zhili; Yang, Chunping; Hu, Xinjiang; Chen, Bo

    2016-12-01

    A biochar supported calcined-Mg/Al layered double hydroxides composite (CLDHs/BC) was synthesized by a one-pot slow pyrolysis of LDHs preloaded bagasse biomass. Multiple characterizations of the product illustrated that the calcined-Mg/Al layered double hydroxides (CLDHs) were successfully coated onto the biochar in slow pyrolysis of pre-treated biomass. The as-synthesized CLDHs/BC could efficiently remove antibiotic tetracycline from aqueous solutions. The coating of CLDHs significantly increased the adsorption ability of biochar, and CLDHs/BC exhibited more than 2 times higher adsorption capacity than that of the pristine biochar (BC) in the tested pH range. The maximum adsorption capacity of CLDHs/BC for tetracycline was 1118.12 mg/g at 318 K. The experimental results suggested that the interaction with LDHs on biochar played a dominant role in tetracycline adsorption, accompanied with π–π interaction and hydrogen bond. This study provides a feasible and simple approach for the preparation of high-performance material for antibiotics contaminated wastewater treatment in a cost-effective way.

  6. One-pot synthesis of carbon supported calcined-Mg/Al layered double hydroxides for antibiotic removal by slow pyrolysis of biomass waste

    PubMed Central

    Tan, Xiaofei; Liu, Shaobo; Liu, Yunguo; Gu, Yanling; Zeng, Guangming; Cai, Xiaoxi; Yan, ZhiLi; Yang, Chunping; Hu, Xinjiang; Chen, Bo

    2016-01-01

    A biochar supported calcined-Mg/Al layered double hydroxides composite (CLDHs/BC) was synthesized by a one-pot slow pyrolysis of LDHs preloaded bagasse biomass. Multiple characterizations of the product illustrated that the calcined-Mg/Al layered double hydroxides (CLDHs) were successfully coated onto the biochar in slow pyrolysis of pre-treated biomass. The as-synthesized CLDHs/BC could efficiently remove antibiotic tetracycline from aqueous solutions. The coating of CLDHs significantly increased the adsorption ability of biochar, and CLDHs/BC exhibited more than 2 times higher adsorption capacity than that of the pristine biochar (BC) in the tested pH range. The maximum adsorption capacity of CLDHs/BC for tetracycline was 1118.12 mg/g at 318 K. The experimental results suggested that the interaction with LDHs on biochar played a dominant role in tetracycline adsorption, accompanied with π–π interaction and hydrogen bond. This study provides a feasible and simple approach for the preparation of high-performance material for antibiotics contaminated wastewater treatment in a cost-effective way. PMID:28000759

  7. One-pot synthesis of ternary Ag₂CO₃/Ag/AgCl photocatalyst in natural geothermal water with enhanced photocatalytic activity under visible light irradiation.

    PubMed

    Yao, Xiaxi; Liu, Xiaoheng

    2014-09-15

    Geothermal water is a clean, cheap and renewable resource and it is widely distributed all over the world. In this work, ternary Ag2CO3/Ag/AgCl photocatalyst has been successfully synthesized via a one-pot precipitation method in natural geothermal water at room temperature, wherein the geothermal water serves as the source of chlorine and carbonate. The results suggest that the Ag/AgCl nanoparticles are anchored on the surface of Ag2CO3 and Ag2CO3/Ag/AgCl composite shows strong absorption ability in the visible light region. The evaluation of the photocatalytic activity indicates that the as-synthesized Ag2CO3/Ag/AgCl photocatalyst exhibits higher photocatalytic performance for the degradation of methylene blue (MB) aqueous solution under visible light irradiation than one-component (Ag2CO3), two-component (Ag/AgCl, Ag2CO3/AgCl) and the mechanical mixture of Ag2CO3 and Ag/AgCl. The trapping experiments confirmed that holes (h(+)) and (•)O2(-) were the two main active species in the photocatalytic process. Finally, a possible Z-scheme photocatalytic mechanism of the charge transfer was proposed for the enhanced photocatalytic performance. This work may open up new insights into the application of cheap geothermal water resources in the word and provide new opportunities for facile fabrication of Ag/AgCl-based photocatalysts.

  8. One-pot hydrothermal synthesis of CuBi co-doped mesoporous zeolite Beta for the removal of NOx by selective catalytic reduction with ammonia

    NASA Astrophysics Data System (ADS)

    Xie, Zhiguo; Zhou, Xiaoxia; Wu, Huixia; Chen, Lisong; Zhao, Han; Liu, Yan; Pan, Linyu; Chen, Hangrong

    2016-07-01

    A series of CuBi co-doped mesoporous zeolite Beta (CuxBiy-mBeta) were prepared by a facile one-pot hydrothermal treatment approach and were characterized by XRD, N2 adsorption-desorption, TEM/SEM, XPS, H2-TPR, NH3-TPD and in situ DRIFTS. The catalysts CuxBiy-mBeta were applied to the removal of NOx by selective catalytic reduction with ammonia (NH3-SCR), especially the optimized Cu1Bi1-mBeta achieved the high efficiency for the removal of NOx and N2 selectivity, superior water and sulfur resistance as well as good durability. The excellent catalytic performance could be attributed to the acid sites of the support and the synergistic effect between copper and bismuth species. Moreover, in situ DRIFTS results showed that amides NH2 and NH4+ generated from NH3 adsorption could be responsible for the high selective catalytic reduction of NOx to N2. In addition, a possible catalytic reaction mechanism on Cu1Bi1-mBeta for the removal of NOx by NH3-SCR was proposed for explaining this catalytic process.

  9. Synthesis and characterization of Fe3O4@SiO2 magnetic composite nanoparticles by a one-pot process

    NASA Astrophysics Data System (ADS)

    Zhang, Le; Shao, Hui-ping; Zheng, Hang; Lin, Tao; Guo, Zhi-meng

    2016-09-01

    Fe3O4@SiO2 core-shell composite nanoparticles were successfully prepared by a one-pot process. Tetraethyl-orthosilicate was used as a surfactant to synthesize Fe3O4@SiO2 core-shell structures from prepared Fe3O4 nanoparticles. The properties of the Fe3O4 and Fe3O4@SiO2 composite nanoparticles were studied by X-ray diffraction, transmission electron microscopy, energy dispersive spectroscopy, and Fourier transform infrared spectroscopy. The prepared Fe3O4 particles were approximately 12 nm in size, and the thickness of the SiO2 coating was approximately 4 nm. The magnetic properties were studied by vibrating sample magnetometry. The results show that the maximum saturation magnetization of the Fe3O4@SiO2 powder (34.85 A·m2·kg-1) was markedly lower than that of the Fe3O4 powder (79.55 A·m2·kg-1), which demonstrates that Fe3O4 was successfully wrapped by SiO2. The Fe3O4@SiO2 composite nanoparticles have broad prospects in biomedical applications; thus, our next study will apply them in magnetic resonance imaging.

  10. One-pot synthesis of platinum-based nanoparticles incorporated into mesoporous niobium oxide-carbon composites for fuel cell electrodes.

    PubMed

    Orilall, M Christopher; Matsumoto, Futoshi; Zhou, Qin; Sai, Hiroaki; Abruña, Héctor D; DiSalvo, Francis J; Wiesner, Ulrich

    2009-07-08

    Catalyst-electrode design is crucial for the commercialization and widespread use of polymer electrolyte membrane fuel cells. There are considerable challenges in making less expensive, more durable, and more active catalysts. Herein, we report the one-pot synthesis of Pt and Pt-Pb nanoparticles incorporated into the pores of mesoporous niobium oxide-carbon composites. The self-assembly of block copolymers with niobium oxide and metal precursors results in an ordered mesostructured hybrid. Appropriate heat treatment of this hybrid produces highly crystalline, well-ordered mesoporous niobium oxide-carbon composites with Pt (or Pt-Pb) nanoparticles incorporated into the mesopores. The in situ-generated graphitic-like carbon material prevents the collapse of the mesostructure, while the metal oxide crystallizes at high temperatures and enhances the electrical conductivity of the final material. Formic acid electrooxidation with this novel material shows 4 times higher mass activities (3.3 mA/microg) and somewhat lower onset potentials (-0.24 V vs Ag/AgCl) than the best previously reported values employing Pt-Pb intermetallic nanoparticles supported on conducting carbon (0.85 mA/microg and -0.18 V, respectively).

  11. A facile one-pot self-assembly approach to incorporate SnOx nanoparticles in ordered mesoporous carbon with soft templating for fuel cells.

    PubMed

    Huang, Yingqiang; Zhai, Zhicheng; Luo, Zhigang; Liu, Yingju; Liang, Zhurong; Fang, Yueping

    2014-04-04

    Unique SnO(x) (x = 1,2)/ordered mesoporous carbon nanocomposites (denoted as SnO(x)/OMC) are firstly synthesized through a 'one-pot' synthesis together with the soft template self-assembly approach. The obtained SnO(x)/OMC nanocomposites with various SnO(x) contents exhibit uniform pore sizes between 3.9 and 4.2 nm, high specific surface areas between 497 and 595 m(2) g(-1), and high pore volumes between 0.39 and 0.48 cm(3) g(-1). With loading of Pt, Pt-SnO(x)/OMC with relatively low SnO(x) content exhibits superior electrocatalytic performance, long-term durability, and resistance to CO poisoning for methanol oxidation, as compared to Pt/OMC, PtRu/C and Pt-SnO(x)/C, which may be attributed not only to the synergetic effect of embedded SnO(x), but also to the highly ordered mesostructure with high specific surface areas and large pore volumes affording plenty of surface area for support of Pt nanoparticles. This work supplies an efficient way to synthesize novel ordered mesoporous carbon self-supported metallic oxide as catalyst support and its further potential application to reduce the cost of catalysts in direct methanol fuel cells.

  12. Facile One-pot Transformation of Iron Oxides from Fe2O3 Nanoparticles to Nanostructured Fe3O4@C Core-Shell Composites via Combustion Waves.

    PubMed

    Shin, Jungho; Lee, Kang Yeol; Yeo, Taehan; Choi, Wonjoon

    2016-02-23

    The development of a low-cost, fast, and large-scale process for the synthesis and manipulation of nanostructured metal oxides is essential for incorporating materials with diverse practical applications. Herein, we present a facile one-pot synthesis method using combustion waves that simultaneously achieves fast reduction and direct formation of carbon coating layers on metal oxide nanostructures. Hybrid composites of Fe2O3 nanoparticles and nitrocellulose on the cm scale were fabricated by a wet impregnation process. We demonstrated that self-propagating combustion waves along interfacial boundaries between the surface of the metal oxide and the chemical fuels enabled the release of oxygen from Fe2O3. This accelerated reaction directly transformed Fe2O3 into Fe3O4 nanostructures. The distinctive color change from reddish-brown Fe2O3 to dark-gray Fe3O4 confirmed the transition of oxidation states and the change in the fundamental properties of the material. Furthermore, it simultaneously formed carbon layers of 5-20 nm thickness coating the surfaces of the resulting Fe3O4 nanoparticles, which may aid in maintaining the nanostructures and improving the conductivity of the composites. This newly developed use of combustion waves in hybridized nanostructures may permit the precise manipulation of the chemical compositions of other metal oxide nanostructures, as well as the formation of organic/inorganic hybrid nanostructures.

  13. One-pot Solvothermal Synthesis of Well-ordered Layered Sodium Aluminoalcoholate Complex: A Useful Precursor for the Preparation of Porous Al2O3 Particles.

    PubMed

    Li, Xiansen; Michaelis, Vladimir K; Ong, Ta-Chung; Smith, Stacey J; McKay, Ian; Müller, Peter; Griffin, Robert G; Wang, Evelyn N

    2014-04-14

    One-pot solvothermal synthesis of a robust tetranuclear sodium hexakis(glycolato)tris(methanolato)aluminate complex Na3[Al4(OCH3)3(OCH2CH2O)6] via a modified yet rigorous base-catalyzed transesterification mechanism is presented here. Single crystal X-ray diffraction (SCXRD) studies indicate that this unique Al complex contains three penta-coordinate Al(3+) ions, each bound to two bidentate ethylene glycolate chelators and one monodentate methanolate ligand. The remaining fourth Al(3+) ion is octahedrally coordinated to one oxygen atom from each of the six surrounding glycolate chelators, effectively stitching the three penta-coordinate Al moieties together into a novel tetranuclear Al complex. This aluminate complex is periodically self-assembled into well-ordered layers normal to the [110] axis with the intra-/inter-layer bindings involving extensive ionic bonds from the three charge-counterbalancing Na(+) cations rather than the more typical hydrogen bonding interactions as a result of the fewer free hydroxyl groups present in its structure. It can also serve as a valuable precursor toward the facile synthesis of high-surface-area alumina powders using a very efficient rapid pyrolysis technique.

  14. One-pot synthesis of a metal–organic framework as an anode for Li-ion batteries with improved capacity and cycling stability

    SciTech Connect

    Gou, Lei Hao, Li-Min; Shi, Yong-Xin; Ma, Shou-Long; Fan, Xiao-Yong; Xu, Lei; Li, Dong-Lin Wang, Kang

    2014-02-15

    Metal–organic framework is a kind of novel electrode materials for lithium ion batteries. Here, a 3D metal–organic framework Co{sub 2}(OH){sub 2}BDC (BDC=1,4-benzenedicarboxylate) was synthesized for the first time by the reaction of Co{sup 2+} with a bio-inspired renewable organic ligand 1,4-benzenedicarboxylic acid through a solvothermal method. As an anode material for lithium ion batteries, this material exhibited an excellent cyclic stability as well as a large reversible capacity of ca. 650 mA h g{sup −1} at a current density of 50 mA g{sup −1} after 100 cycles within the voltage range of 0.02–3.0 V, higher than that of other BDC based anode. - Graphical abstract: The PXRD pattern and the cycleability curves (inset) of Co{sub 2}(OH){sub 2}BDC. Display Omitted - Highlights: • Co{sub 2}(OH){sub 2}BDC was synthesized through a one pot solvothermal process. • The solvent had a great effect on the purity of this material. • This material was used as anode material for lithium ion batteries for the first time. • Co{sub 2}(OH){sub 2}BDC showed improved capacity and cycling stability.

  15. A facile one-pot solvothermal method to produce superparamagnetic graphene-Fe3O4 nanocomposite and its application in the removal of dye from aqueous solution.

    PubMed

    Wu, Qiuhua; Feng, Cheng; Wang, Chun; Wang, Zhi

    2013-01-01

    A superparamagnetic graphene-Fe(3)O(4) nanocomposite (G/Fe(3)O(4)) was synthesized by a facile one-pot solvothermal method. The nanocomposite G/Fe(3)O(4) prepared by the new method was firstly used as an adsorbent to remove dye for water pollution remediation. In comparison with G/Fe(3)O(4) prepared by the in situ chemical coprecipitation, the newly prepared G/Fe(3)O(4) had a higher adsorption efficiency for the dye. The adsorption characteristics of the nanocomposite adsorbent were examined using the organic dye pararosaniline as the adsorbate. The adsorption kinetics, adsorption capacity of the adsorbent, and the effect of the adsorbent dosage and solution pH on the removal efficiency of pararosaniline were investigated. The adsorption capacity of G/Fe(3)O(4) for pararosaniline was evaluated using the Freundlich and Langmuir adsorption isotherm models. The G/Fe(3)O(4) hybrid composite can be easily manipulated in magnetic field for desired separation, leading to an easy removal of the dye from polluted water. The G/Fe(3)O(4) hybrid composite would have a great potential in removing organic dyes from polluted water.

  16. Synthesis of pH and temperature sensitive, core-shell nano/microgels, by one pot, soap-free emulsion polymerization.

    PubMed

    Serrano-Medina, A; Cornejo-Bravo, J M; Licea-Claveríe, A

    2012-03-01

    The synthesis and properties of thermal/pH-sensitive core-shell copolymer nano/microgels were investigated. The crosslinked core consisted of N-isopropylacrylamide (NIPAAm) while the shell was stabilized by poly(ethylene glycol) methyl ether methacrylate (PEGMA) and 2-methacryloyloxybenzoic acid (2MBA) using a "one pot" soapless emulsion polymerization method. Monodisperse particles were produced with average hydrodynamic diameters ranging from 40 to 880 nm, as determined by dynamic light scattering (DLS) in water at 25°C, depending on the synthetic recipe used. The influence of PEGMA and 2MBA content on size and temperature transition at different pH values was studied. Zeta potential measurements and acid-base titration studies demonstrated almost complete incorporation of acid comonomer (2MBA) into the nano/microgels. Two different crosslinkers, a stable and an acid labile, were compared. The crosslinker used has a major influence on the size and charge density of the nano/microgels produced. Microscopic studies confirmed the core-shell morphology of the nano/microgels.

  17. Facile "one-pot" synthesis of poly(methacrylic acid)-based hybrid monolith via thiol-ene click reaction for hydrophilic interaction chromatography.

    PubMed

    Lv, Xumei; Tan, Wangming; Chen, Ye; Chen, Yingzhuang; Ma, Ming; Chen, Bo; Yao, Shouzhuo

    2016-07-08

    A novel sol-gel "one-pot" approach in tandem with a radical-mediated thiol-ene reaction for the synthesis of a methacrylic acid-based hybrid monolith was developed. The polymerization monomers, tetramethoxysilane (TMOS) and 3-mercaptopropyl trimethoxysilane (MPTS), were hydrolyzed in high-concentration methacrylic acid solution that also served as a hydrophilic functional monomer. The resulting solution was then mixed with initiator (2, 2'-azobis (2-methylpropionamide) dihydrochloride) and porogen (urea, polyethylene glycol 20,000) in a capillary column and polymerized in water bath. The column had a uniform porous structure and a good permeability. The evaluation of the monolith was performed by separation of small molecules including nucleosides, phenols, amides, bases and Triton X-100. The calibration curves for uridine, inosine, adenosine and cytidine were determined. All the calibration curves exhibited good linear regressions (R(2)≥0.995) within the test ranges of 0.5-40μg/mL for four nucleosides. Additionaliy, atypical hydrophilic mechanism was proved by elution order from low to high according to polarity retention time increased with increases in the content of the organic solvent in the mobile phase. Further studies indicated that hydrogen bond and electrostatic interactions existed between the polar analytes and the stationary phase. This was the mechanism of retention. The excellent separation of the BSA digest showed good hydrophility of the column and indicated the potential in separation of complex biological samples.

  18. One-pot solvothermal synthesis of ordered intermetallic Pt2In3 as stable and efficient electrocatalyst towards direct alcohol fuel cell application

    NASA Astrophysics Data System (ADS)

    Jana, Rajkumar; Peter, Sebastian C.

    2016-10-01

    Ordered intermetallic Pt2In3 nanoparticles have been synthesized by superhydride reduction of K2PtCl4 and InCl3.xH2O precursors using facile, one-pot solvothermal method. We report surfactant free solvothermal synthesis of a novel ordered Pt2In3 intermetallic nanoparticles for the first time. The structure and morphology of the catalyst has been confirmed by powder X-ray diffraction, transmission electron microscopy, field emission scanning electron microscopy, energy-dispersive spectrometry and X-ray photoelectron spectroscopy. The electrocatalytic properties of the catalysts have been investigated by cyclic voltammetry and chronoamperometry. The as prepared Pt2In3 catalyst exhibit far superior electrocatalytic activity and stability towards alcohol oxidation over commercial Pt/C. The specific activity of as synthesized catalyst was found to be ~3.2 and ~2.3 times higher than commercial Pt/C for methanol and ethanol oxidation, respectively. This improved activity and durability of the Pt2In3 nanoparticles can make the catalyst an ideal catalyst candidate for direct alcohol fuel cell.

  19. Facile One-pot Transformation of Iron Oxides from Fe2O3 Nanoparticles to Nanostructured Fe3O4@C Core-Shell Composites via Combustion Waves

    NASA Astrophysics Data System (ADS)

    Shin, Jungho; Lee, Kang Yeol; Yeo, Taehan; Choi, Wonjoon

    2016-02-01

    The development of a low-cost, fast, and large-scale process for the synthesis and manipulation of nanostructured metal oxides is essential for incorporating materials with diverse practical applications. Herein, we present a facile one-pot synthesis method using combustion waves that simultaneously achieves fast reduction and direct formation of carbon coating layers on metal oxide nanostructures. Hybrid composites of Fe2O3 nanoparticles and nitrocellulose on the cm scale were fabricated by a wet impregnation process. We demonstrated that self-propagating combustion waves along interfacial boundaries between the surface of the metal oxide and the chemical fuels enabled the release of oxygen from Fe2O3. This accelerated reaction directly transformed Fe2O3 into Fe3O4 nanostructures. The distinctive color change from reddish-brown Fe2O3 to dark-gray Fe3O4 confirmed the transition of oxidation states and the change in the fundamental properties of the material. Furthermore, it simultaneously formed carbon layers of 5–20 nm thickness coating the surfaces of the resulting Fe3O4 nanoparticles, which may aid in maintaining the nanostructures and improving the conductivity of the composites. This newly developed use of combustion waves in hybridized nanostructures may permit the precise manipulation of the chemical compositions of other metal oxide nanostructures, as well as the formation of organic/inorganic hybrid nanostructures.

  20. One-pot pyrolysis of lithium sulfate and graphene nanoplatelet aggregates: in situ formed Li₂S/graphene composite for lithium-sulfur batteries.

    PubMed

    Li, Zhe; Zhang, Shiguo; Zhang, Ce; Ueno, Kazuhide; Yasuda, Tomohiro; Tatara, Ryoichi; Dokko, Kaoru; Watanabe, Masayoshi

    2015-09-14

    Lithium sulfide (Li2S) as a cathodic material in Li-S batteries can not only deliver a high theoretical specific capacity of 1166 mA h g(-1), but also is essential for batteries using Li-free anode materials such as silicon and graphite. Various efforts have been made to synthesize a highly efficient Li2S-carbon composite; however, the electronically and ionically insulating nature and high melting point of Li2S strongly complicate the synthetic procedures, making it difficult to realize the expected capacity. Herein, a very simple method is proposed to prepare Li2S/graphene composites by one-pot pyrolysis of a mixture of graphene nanoplatelet aggregates (GNAs) and low-cost lithium sulfate (Li2SO4). For the first time, the entire pyrolysis process is clarified by thermogravimetry-mass spectrometry, wherein GNAs were found to partly serve as a carbon source to reduce Li2SO4 to Li2S, while the remaining GNAs formed thin graphene sheets as a result of this in situ etching, as a highly conductive host can immobilize the generated Li2S by intimate contact. Consequently, the obtained Li2S/graphene composite, combined with a Li2Sx-insoluble (x = 4-8) electrolyte developed by our group, exhibits excellent electrochemical behavior for Li-S batteries.

  1. One-pot self-assembly of graphene/carbon nanotube/sulfur hybrid with three dimensionally interconnected structure for lithium-sulfur batteries

    NASA Astrophysics Data System (ADS)

    Niu, Shuzhang; Lv, Wei; Zhang, Chen; Shi, Yanting; Zhao, Jianfeng; Li, Baohua; Yang, Quan-Hong; Kang, Feiyu

    2015-11-01

    A graphene/carbon nanotube (CNT)/sulfur (denoted GCS) hybrid with interconnected structure is prepared through a one-pot self-assembly approach initiated by L-ascorbic acid reduction under a mild condition. In such a solution-based assembly process, the formation of an interconnected graphene/CNT conductive network is accompanied by the uniform loading of sulfur, whose fraction is as high as of 70 wt%. The as-prepared GCS hybrid delivers an initial capacity of 1008 mAh g-1 at 0.3C and maintains 704 mAh g-1 after 100 cycles. Remarkably, at a high rate of 1.0C, the cathode shows an excellent cyclic performance with a capacity of 657 mAh g-1 after 450 ycles and the capacity decay is only 0.04% per cycle. Moreover, the superior rate performance of GCS hybrid is attributed to the conductive network formed by interconnected graphene sheets and CNT, which supply an unimpeded and continuous path for electron and Li ion transfer and accommodate the volume variation of sulfur during charge/discharge cycling. In addition, the residual functional groups on GCS can retain intimate contact of the conducting matrix with sulfur and effectively confine the diffusion of polysulfides. This study gives an eco-friendly and highly effective solution-based approach for carbon-sulfur electrode for lithium-sulfur battery.

  2. One-pot green synthesis of reduced graphene oxide (RGO)/Fe3O4 nanocomposites and its catalytic activity toward methylene blue dye degradation.

    PubMed

    Vinothkannan, M; Karthikeyan, C; Gnana kumar, G; Kim, Ae Rhan; Yoo, Dong Jin

    2015-02-05

    The reduced graphene oxide (RGO)/Fe3O4 nanocomposites were synthesized through a facile one-pot green synthesis by using solanum trilobatum extract as a reducing agent. Spherical shaped Fe3O4 nanoparticles with the diameter of 18 nm were uniformly anchored over the RGO matrix and the existence of fcc structured Fe3O4 nanoparticles over the RGO matrix was ensured from X-ray diffraction patterns. The amide functional groups exist in the solanum trilobatum extract is directly responsible for the reduction of Fe(3+) ions and GO. The thermal stability of GO was increased by the removal of hydrophilic functional groups via solanum trilobatum extract and was further promoted by the ceramic Fe3O4 nanoparticles. The ID/IG ratio of RGO/Fe3O4 was increased over GO, indicating the extended number of structural defects and disorders in the RGO/Fe3O4 composite. The catalytic efficiency of prepared nanostructures toward methylene blue (MB) dye degradation mediated through the electron transfer process of BH4(-) ions was studied in detail. The π-π stacking, hydrogen bonding and electrostatic interaction exerted between the RGO/Fe3O4 composite and methylene blue, increased the adsorption efficiency of dye molecules and the large surface area and extended number of active sites completely degraded the MB dye within 12 min.

  3. One-Pot Synthesis of Fe3O4 Nanoparticle Loaded 3D Porous Graphene Nanocomposites with Enhanced Nanozyme Activity for Glucose Detection.

    PubMed

    Wang, Qingqing; Zhang, Xueping; Huang, Liang; Zhang, Zhiquan; Dong, Shaojun

    2017-03-01

    A novel one-pot strategy is proposed to fabricate 3D porous graphene (3D GN) decorated with Fe3O4 nanoparticles (Fe3O4 NPs) by using hemin as iron source. During the process, graphene oxide was simultaneously reduced and self-assembled to form 3D graphene hydrogel while Fe3O4 NPs synthesized from hemin distributed uniformly on 3D GN. The preparation process is simple, facile, economical, and green. The obtained freeze-dried product (3D GH-5) exhibits outstanding peroxidase-like activity. Compared to the traditional 2D graphene-based nanocomposites, the introduced 3D porous structure dramatically improved the catalytic activity, as well as the catalysis velocity and its affinity for substrate. The high catalytic activity could be ascribed to the formation of Fe3O4 NPs and 3D porous graphene structures. Based on its peroxidase-like activity, 3D GH-5 was used for colorimetric determination of glucose with a low detection limit of 0.8 μM.

  4. Facile one-pot synthesis and application of nitrogen and sulfur-doped activated graphene in simultaneous electrochemical determination of hydroquinone and catechol.

    PubMed

    Xiao, Lili; Yin, Jiao; Li, Yingchun; Yuan, Qunhui; Shen, Hangjia; Hu, Guangzhi; Gan, Wei

    2016-10-07

    Nitrogen (N) and sulfur (S) co-doped activated graphene (N,S-AGR) was prepared by the one-pot pyrolysis of a mixture of graphene oxide (GO), thiourea, and potassium hydroxide (KOH), where thiourea acts as the source of N and S dopants and KOH is the activator for porosity. N,S-AGR with a dopant abundance of 2.8 at% N and 2.3 at% S was then used as a high-activity electrocatalyst in the fabrication of an electrochemical sensor for simultaneous determination of dihydroxybenzene isomers, hydroquinone (HQ) and catechol (CC), in aqueous solution. Compared with the bare glassy carbon electrode (GCE), the electrodes modified with N,S-AGR showed enhanced electrochemical performance toward HQ and CC in both cyclic voltammetric (CV) and differential pulse voltammetric (DPV) measurements because of their enlarged surface area, enhanced electron-transfer rate and increased active sites. Compared with some recently reported electrochemical sensors based on graphene composites, the N,S-AGR modified electrode exhibits higher sensitivity, a much lower detection limit and a comparable linear range for the simultaneous determination of HQ and CC. Moreover, the proposed sensor is promising in practical application for the satisfactory recoveries obtained in real water sample analyses.

  5. One-pot hydrothermal synthesis of CuBi co-doped mesoporous zeolite Beta for the removal of NOx by selective catalytic reduction with ammonia

    PubMed Central

    Xie, Zhiguo; Zhou, Xiaoxia; Wu, Huixia; Chen, Lisong; Zhao, Han; Liu, Yan; Pan, Linyu; Chen, Hangrong

    2016-01-01

    A series of CuBi co-doped mesoporous zeolite Beta (CuxBiy-mBeta) were prepared by a facile one-pot hydrothermal treatment approach and were characterized by XRD, N2 adsorption-desorption, TEM/SEM, XPS, H2-TPR, NH3-TPD and in situ DRIFTS. The catalysts CuxBiy-mBeta were applied to the removal of NOx by selective catalytic reduction with ammonia (NH3-SCR), especially the optimized Cu1Bi1-mBeta achieved the high efficiency for the removal of NOx and N2 selectivity, superior water and sulfur resistance as well as good durability. The excellent catalytic performance could be attributed to the acid sites of the support and the synergistic effect between copper and bismuth species. Moreover, in situ DRIFTS results showed that amides NH2 and NH4+ generated from NH3 adsorption could be responsible for the high selective catalytic reduction of NOx to N2. In addition, a possible catalytic reaction mechanism on Cu1Bi1-mBeta for the removal of NOx by NH3-SCR was proposed for explaining this catalytic process. PMID:27445009

  6. One-pot fabrication of FRET-based fluorescent probe for detecting copper ion and sulfide anion in 100% aqueous media

    NASA Astrophysics Data System (ADS)

    Lv, Kun; Chen, Jian; Wang, Hong; Zhang, Peisheng; Yu, Maolin; Long, Yunfei; Yi, Pinggui

    2017-04-01

    The design of effective tools for detecting copper ion (Cu2 +) and sulfide anion (S2 -) is of great importance due to the abnormal level of Cu2 + and S2 - has been associated with an increase in risk of many diseases. Herein, we report on the fabrication of fluorescence resonance energy transfer (FRET) based fluorescent probe PF (PEI-FITC) for detecting Cu2 + and S2 - in 100% aqueous media via a facile one-pot method by covalent linking fluorescein isothiocyanate (FITC) with branched-polyethylenimine (b-PEI). PF could selectively coordinate with Cu2 + among 10 metal ions to form PF-Cu2 + complex, resulting in fluorescence quenching through FRET mechanism. Furthermore, the in situ generated PF-Cu2 + complex can be used to selectively detect S2 - based on the displacement approach, resulting in an off-on type sensing. There is no obvious interference from other anions, such as Cl-, NO3-, ClO4-, SO42 -, HCO3-, CO32 -, Br-, HPO42 -, F- and S2O32 -. In addition, PF was successfully used to determine Cu2 + and S2 - in human serum and tap water samples. Therefore, the FRET-based probe PF may provide a new method for selective detection of multifarious analysts in biological and environmental applications, and even hold promise for application in more complicated systems.

  7. Synthesis of boronate-silica hybrid affinity monolith via a one-pot process for specific capture of glycoproteins at neutral conditions.

    PubMed

    Yang, F; Mao, J; He, X W; Chen, L X; Zhang, Y K

    2013-08-01

    In this study, a boronate-silica hybrid affinity monolith was prepared for specific capture of glycoproteins at neutral pH condition. The monolith was synthesized via a facile one-pot procedure in a stainless steel column by concurrently mixing hydrolyzed alkoxysilanes tetramethoxysilane and vinyltrimethoxysilane, organic monomer 3-acrylamidophenylboronic acid and initiator 2,2'-azobisisobutyronitrile together. The polycondensation of alkoxysilanes and copolymerization of organic monomer and vinyl-silica monolith were carried out successively by reacting at different temperatures. After optimizing the preparation conditions, the resulting hybrid affinity monolith was systematically characterized and exhibited excellent affinity to both cis-diol-containing small molecules and glycoproteins at neutral and physiological pH, including adenosine, horseradish peroxidase, transferrin and ovalbumin. The binding capacity of ovalbumin on monolith was measured to be 2.5 mg g(-1) at pH 7.0. Furthermore, the hybrid affinity monolith was applied to the separation of transferrin from bovine serum sample at a physiological condition. Good repeatability was obtained and the relative standard deviations of retention time were 1.15 and 4.77 % (n = 5) for run-to-run and column-to-column, respectively.

  8. Facile one-pot preparation of a novel imidazolium-based monolith by thiol-ene click chemistry for capillary liquid chromatography.

    PubMed

    Zhang, Peng; Yang, Haiguan; Chen, Tao; Qin, Yuemei; Ye, Fanggui

    2016-11-09

    In this work, a novel imidazolium-based monolith was fabricated through a simple route. With 1-vinyl-3-octadecylimidazolium bromide and ethylene dimethacrylate as monomers, pentaerythritol tetra-(3-mercaptopropionate) as crosslinker, AIBN as thermal initiator, the monolith was facilely fabricated by one-pot thiol-ene click chemistry. The influences of both the content of monomer/crosslinker and porogenic systems on the morphology, and permeability of the monolith were studied. The optimal reaction conditions were used to prepare a homogeneous and permeable monolith. The optimal preparation of monolithic column was characterized by scanning electron microscopy, Fourier transform infrared spectrometry, X-ray photoelectron spectroscopy, and thermogravimetric analysis. High efficiency and quick separation of alkylbenzenes, styrene and ethylbenzene, polycyclic aromatic hydrocarbon, phenols, anilines, and aromatic acids were achieved. The minimum plate height of this monolith were determined as 11.42 μm for thiourea and 13.26 μm for benzene. All results indicated that thiol-ene click chemistry provides a quick way for the fabrication of imidazolium-based monolith.

  9. One-pot synthesis of visible-light-driven Ag/Ag3PO4 photocatalyst immobilized on exfoliated montmorillonite by clay-mediated in situ reduction

    NASA Astrophysics Data System (ADS)

    Liu, Chang; Zhang, Xiaoyuan; Wu, Jianning; Meng, Guihua; Guo, Xuhong; Liu, Zhiyong

    2016-11-01

    In order to find efficient photocatalytic materials and convenient preparation method, a well-designed Ag/Ag3PO4-OMMT (organically modified montmorillonite) plasmonic photocatalyst was synthesized via the "one-pot" process without any reducing species. Ag+ could be reduced by Si-OH moiety on the surface of OMMT. The resulting samples were thoroughly studied by using X-ray diffraction, X-ray photoelectron spectra, transmission electron microscopy, scanning electron microscope, energy-dispersive X-ray spectroscopy, UV-Vis diffuse reflectance spectra, and so on. The as-prepared Ag/Ag3PO4-OMMT photocatalyst exhibited efficient, stable photocatalytic activity and recyclability for the degradation of Rhodamine B (RhB) under visible light radiation ( λ > 420 nm). The optimum synergetic effect of Ag3PO4/OMMT was found at a weight ratio of 50 %. The degradation efficiency of RhB over Ag/Ag3PO4-OMMT (1:1) was about 92.9 %, and photocatalytic activity remained stable after three cycles. The results show that the designed photocatalyst is feasible and effective. The proposed photocatalysis mechanism is probably attributed to surface plasmon resonance of metallic Ag nanoparticles (NPs) and also attributed to negatively charged exfoliated montmorillonite. The Ag/Ag3PO4-OMMT composites showed highly visible light photocatalytic activity, which makes them promising nanomaterials for further applications in water treatment.

  10. One-pot solvothermal synthesis of novel cobalt salicylaldimine-urea complexes: A new approach to Co3O4 nanoparticles

    NASA Astrophysics Data System (ADS)

    Nassar, M. Y.; Mohamed, T. Y.; Ahmed, I. S.

    2013-10-01

    Three novel Cobalt salicylaldimine-urea complexes {[CoxLy(H2O)n]Clz; where, L = 1,3-bis(salicylaldehydimine)urea Schiff base; x, y = 1 or 2; n = 2 or 8; z = 0 or 2} were synthesized by one-pot solvothermal treatment of methanolic solutions of urea, salicylaldehyde, and cobalt chloride at 120 °C for 3 h. Subsequently, normal spinel-type Co3O4 nanoparticles, with an average crystallite size in the range 22-38 nm, were easily produced via thermal decomposition of the synthesized complexes at 400 °C for 2 h. The synthesized compounds were characterized by elemental analysis, thermal analysis (TG-DTA/DTG), X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), UV-Vis spectroscopy, transmission electron microscopy (TEM) and EI mass spectroscopy. Investigation of the optical properties of the produced cobalt oxide, using UV-Vis spectroscopy, confirmed its semiconducting properties by revealing two optical band gabs in the range of 1.42-1.50 and 1.83-1.95 eV.

  11. Synthetic and theoretical investigation on the one-pot halogenation of β-amino alcohols and nucleophilic ring opening of aziridinium ions.

    PubMed

    Chen, Yunwei; Sun, Xiang; Wu, Ningjie; Li, Jingbai; Jin, Shengnan; Zhong, Yongliang; Liu, Zirui; Rogachev, Andrey; Chong, Hyun-Soon

    2016-01-21

    Aziridinium ions are useful reactive intermediates for the synthesis of enantiomerically enriched building blocks. However, N,N-dialkyl aziridinium ions are relatively underutilized in the synthesis of optically active molecules as compared to other three-membered ring cogeners, aziridines and epoxides. The characterization of both optically active aziridinium ions and secondary β-halo amines as the precursor molecules of aziridinium ions has been scarcely reported and is often unclear. In this paper, we report for the first time the preparation and experimental and theoretical characterization of optically active aziridinium ions and secondary β-halo amines. Optically active secondary N,N-substituted β-halo amines were efficiently synthesized from N,N-substituted alaninol via formation and ring opening at the more hindered carbon of aziridinium ions by halides. Optically active β-halo amines and aziridinium ions were characterized by NMR and computational analyses. The structure of an optically active β-chloro amine was confirmed via X-ray crystallographic analysis. The aziridinium ions derived from N,N-dibenzyl alaniol remained stable only for several hours, which was long enough for analyses of NMR and optical activity. The stereospecific ring opening of aziridinium ions by halides was computationally studied using DFT and highly-accurate DLPNO-CCSD(T) methods. The highly regioselective and stereoselective ring opening of aziridinium ions was applied for efficient one-pot conversion of β-alaninols to enantiomerically enriched β-amino alcohols, β-amino nitriles, and vicinal diamine derivatives.

  12. Accelerated Combinatorial High Throughput Star Polymer Synthesis via a Rapid One-Pot Sequential Aqueous RAFT (rosa-RAFT) Polymerization Scheme.

    PubMed

    Cosson, Steffen; Danial, Maarten; Saint-Amans, Julien Rosselgong; Cooper-White, Justin J

    2017-02-21

    Advanced polymerization methodologies, such as reversible addition-fragmentation transfer (RAFT), allow unprecedented control over star polymer composition, topology, and functionality. However, using RAFT to produce high throughput (HTP) combinatorial star polymer libraries remains, to date, impracticable due to several technical limitations. Herein, the methodology "rapid one-pot sequential aqueous RAFT" or "rosa-RAFT," in which well-defined homo-, copolymer, and mikto-arm star polymers can be prepared in very low to medium reaction volumes (50 µL to 2 mL) via an "arm-first" approach in air within minutes, is reported. Due to the high conversion of a variety of acrylamide/acrylate monomers achieved during each successive short reaction step (each taking 3 min), the requirement for intermediary purification is avoided, drastically facilitating and accelerating the star synthesis process. The presented methodology enables RAFT to be applied to HTP polymeric bio/nanomaterials discovery pipelines, in which hundreds of complex polymeric formulations can be rapidly produced, screened, and scaled up for assessment in a wide range of applications.

  13. One-Pot Synthesis of CoSex -rGO Composite Powders by Spray Pyrolysis and Their Application as Anode Material for Sodium-Ion Batteries.

    PubMed

    Park, Gi Dae; Kang, Yun Chan

    2016-03-14

    A simple one-pot synthesis of metal selenide/reduced graphene oxide (rGO) composite powders for application as anode materials in sodium-ion batteries was developed. The detailed mechanism of formation of the CoSe(x)-rGO composite powders that were selected as the first target material in the spray pyrolysis process was studied. The crumple-structured CoSe(x)-rGO composite powders prepared by spray pyrolysis at 800 °C had a crystal structure consisting mainly of Co0.85 Se with a minor phase of CoSe2. The bare CoSe(x) powders prepared for comparison had a spherical shape and hollow structure. The discharge capacities of the CoSe(x)-rGO composite and bare CoSe(x) powders in the 50th cycle at a constant current density of 0.3 A g(-1) were 420 and 215 mA h g(-1), respectively, and their capacity retentions measured from the second cycle were 80 and 46%, respectively. The high structural stability of the CoSe(x)-rGO composite powders for repeated sodium-ion charge and discharge processes resulted in superior sodium-ion storage properties compared to those of the bare CoSe(x) powders.

  14. Reduced graphene oxide-Hemin-Au nanohybrids: Facile one-pot synthesis and enhanced electrocatalytic activity towards the reduction of hydrogen peroxide.

    PubMed

    Gu, Chang-Jie; Kong, Fen-Ying; Chen, Zhi-Dong; Fan, Da-He; Fang, Hai-Lin; Wang, Wei

    2016-04-15

    A facile and effective strategy is demonstrated for the synthesis of ternary reduced graphene oxide-Hemin-Au (rGO-H-Au) nanohybrids. The nanohybrids were synthesized through a one-pot in situ reduction of GO and HAuCl4 under alkaline conditions using GO, Hemin and HAuCl4 as the starting materials. The synthesis process can be finished within 1h in a solution phase, without adding any additional surfactant, stabilizing agent and toxic or harsh chemical reducing agents. The resulting nanohybrids were characterized by UV-vis spectroscopy, Raman spectroscopy, transmission electron microscopy (TEM), and so on. Electrochemical measurements showed that the rGO-H-Au nanohybrids exhibited good electrocatalytic activity for the reduction of hydrogen peroxide (H2O2). Based on this property, a simple and highly sensitive amperometric biosensor for H2O2 had been developed. The linear relationships were obtained from 0.1 µM to 40 µM and the detection limit was estimated to be 30 nM. The simple and sensitive sensing platform showed great promising applications in the pharmaceutical, clinical and industrial detection of H2O2.

  15. Sustainable one-pot integration of ZnO nanoparticles into carbon spheres: manipulation of the morphological, optical and electrochemical properties.

    PubMed

    Patrinoiu, Greta; Calderon-Moreno, Jose M; Birjega, Ruxandra; Culita, Daniela C; Somacescu, Simona; Musuc, Adina M; Spataru, Tanta; Carp, Oana

    2016-11-09

    ZnO-carbon composite spheres were synthesized via starch hydrothermal carbonization (HTC) in the presence of a soluble zinc salt (acetate), followed by thermal processing under an argon atmosphere. Besides sustainability, the one-pot procedure represents a scalable synthesis of tailored carbon-metal oxide spheres with a structurally-ordered carbon matrix obtained at a relatively low temperature (700 °C). The ability of zinc cations to develop different linkages with starch's hydrophilic functional groups and to act as external nucleators determines an increase in HTC yield; the effect is obvious even in the presence of small concentrations of zinc in the reaction medium (0.005 M), thus providing a way to improve the carbonization process efficiency. It is also shown that zinc content is the control vector of the spherical composite's properties: a variation from 0.3 to 4.8 at% not only induces a variation in their size (200 nm-10 μm), interconnectivity (from disperse spheres to necklace-like aggregations), surface area and connected porosity (from micro- to mesoporosity), but also of their electrochemical and white light adsorption and emission features. Since the variation in zinc content is made by a simple adjustment of the raw material concentrations, the functionality of these carbon-based materials can be modulated in a straightforward manner.

  16. AlOOH-reduced graphene oxide nanocomposites: one-pot hydrothermal synthesis and their enhanced electrochemical activity for heavy metal ions.

    PubMed

    Gao, Chao; Yu, Xin-Yao; Xu, Ren-Xia; Liu, Jin-Huai; Huang, Xing-Jiu

    2012-09-26

    This work described the preparation, characterization, and electrochemical behavior toward heavy metal ions of the AlOOH-reduced graphene oxide nanocomposites. This new material was synthesized through a green one-pot hydrothermal method. The morphologic and structure of the nanocomposites were characterized using atomic force microscopy, X-ray diffraction, Raman spectroscopy, X-ray photoemission spectroscopy, Fourier transform-infrared spectroscopy, and transmission electron microscopy. Electrochemical properties were characterized by cyclic voltammetry and electrochemical impedance spectroscopy. The chemical and electrochemical parameters that have influence on deposition and stripping of metal ions, such as pH value, deposition potential, and deposition time, were also studied. Due to the strong affinity of AlOOH to heavy metal ions and the fast electron-transfer kinetics of graphene, the combination of solid-phase extraction and stripping voltammetric analysis allowed fast and sensitive determination of Cd(II) and Pb(II) in drinking water, making these new nanocomposites promising candidates for practical applications in the fields of detecting heavy metal ions. Most importantly, these new nanocomposites may possess many unknown properties waiting to be explored.

  17. One-pot heterogeneous synthesis of Δ(3)-tetrahydrocannabinol analogues and xanthenes showing differential binding to CB(1) and CB(2) receptors.

    PubMed

    Rosati, Ornelio; Messina, Federica; Pelosi, Azzurra; Curini, Massimo; Petrucci, Vanessa; Gertsch, Jürg; Chicca, Andrea

    2014-10-06

    Δ(9)-tetrahydrocannabinol (Δ(9)-THC) is the major psychoactive cannabinoid in hemp (Cannabis sativa L.) and responsible for many of the pharmacological effects mediated via cannabinoid receptors. Despite being the major cannabinoid scaffold in nature, Δ(9)-THC double bond isomers remain poorly studied. The chemical scaffold of tetrahydrocannabinol can be assembled from the condensation of distinctly substituted phenols and monoterpenes. Here we explored a microwave-assisted one pot heterogeneous synthesis of Δ(3)-THC from orcinol (1a) and pulegone (2). Four Δ(3)-THC analogues and corresponding Δ(4a)-tetrahydroxanthenes (Δ(4a)-THXs) were synthesized regioselectively and showed differential binding affinities for CB1 and CB2 cannabinoid receptors. Here we report for the first time the CB1 receptor binding of Δ(3)-THC, revealing a more potent receptor binding affinity for the (S)-(-) isomer (hCB1Ki = 5 nM) compared to the (R)-(+) isomer (hCB1Ki = 29 nM). Like Δ(9)-THC, also Δ(3)-THC analogues are partial agonists at CB receptors as indicated by [(35)S]GTPγS binding assays. Interestingly, the THC structural isomers Δ(4a)-THXs showed selective binding and partial agonism at CB2 receptors, revealing a simple non-natural natural product-derived scaffold for novel CB2 ligands.

  18. One-pot synthesis of new triazole--Imidazo[2,1-b][1,3,4]thiadiazole hybrids via click chemistry and evaluation of their antitubercular activity.

    PubMed

    Ramprasad, Jurupula; Nayak, Nagabhushana; Dalimba, Udayakumar; Yogeeswari, Perumal; Sriram, Dharmarajan

    2015-10-01

    A new series of triazole-imidazo[2,1-b][1,3,4]thiadiazole hybrids (6a-s, 7a) were designed by a molecular hybridisation approach and the target molecules were synthesized via one pot click chemistry protocol. All the intermediates and final molecules were characterised using spectral methods and one of the target compounds (6c) was analysed by the single crystal XRD study. The derivatives were screened for their antimycobacterial activity against Mycobacterium tuberculosis H37Rv strain. Two compounds, 6f and 6n, demonstrated significant growth inhibitory activity against the bacterial strain with a MIC of 3.125 μg/mL. The presence of chloro substituent on the imidazo[2,1-b][1,3,4]thiadiazole ring and ethyl, benzyl or cyanomethylene groups on the 1,2,3-triazole ring enhance the inhibition activity of the molecules. The active compounds are not toxic to a normal cell line which signifies the lack of general cellular toxicity of these compounds.

  19. A green one-pot synthesis of Pt/TiO2/Graphene composites and its electro-photo-synergistic catalytic properties for methanol oxidation.

    PubMed

    Ye, Lingting; Li, Zhongshui; Zhang, Lian; Lei, Fengling; Lin, Shen

    2014-11-01

    A facile and green one-pot method was used to synthesize Pt/TiO2/Graphene composites with ethanol as a reducing agent under microwave irradiation. The as-prepared composites were characterized by SEM, TEM, EDX, XPS, XRD and Raman. Electrocatalytic performance of the Pt/TiO2/GNs composites was investigated by cyclic voltammetry (CV), chronoamperometric (CA), COad stripping voltammetry and electrochemical impedance spectrum (EIS). All experimental data have revealed that TiO2 (P25) not only enhanced the reduction ability of ethanol under microwave irradiation but also promoted Pt heterogeneous nucleation to form Pt nanoclusters which are around P25 and loaded on graphene nanosheets (GNs) surface. Electrochemical experiments showed that Pt/TiO2/GNs had much higher catalytic activity and stability toward methanol oxidation reaction (MOR) and better resistance to CO poisoning compared with Pt/GNs and the commercially available Johnson Matthey 20% Pt/C catalyst (Pt/C-JM). Especially under UV irradiation with 20min, Pt/TiO2/GNs composites showed an ultrahigh forward peak current density of 1354mAmg(-1), nearly 2.5 times higher than that of Pt/C-JM, which indicated that the electrocatalytic and photocatalytic properties of Pt/TiO2/GNs had been integrated to boost the catalytic performance for MOR.

  20. In-vitro evaluation of copper nanoparticles cytotoxicity on prostate cancer cell lines and their antioxidant, sensing and catalytic activity: One-pot green approach.

    PubMed

    Prasad, P Reddy; Kanchi, S; Naidoo, E B

    2016-08-01

    In this study, Broccoli green extract was reported as a green and environmental friendly precursor for the one-pot biosynthesis of copper nanoparticles. The synthesized nanoparticles were characterized by UV-vis, FTIR, TEM, DLS, XRD and cyclic voltammetry. The TEM and DLS results showed that the NPs are in spherical and monodispersed with an average particle size of ~4.8nm. The FTIR results confirmed the occurrence of bioactive functional groups that are responsible for reducing cupric sulphate to copper ions. The UV-vis spectrophotometry was used for catalytic reduction of 4-nitrophenol and its dynamic reaction in Britton-Robinson buffer solution. This catalytic activity was further supported with methylene blue and methyl red dyes degradation. The nanocatalyst can be recovered from the reaction mixture and reused many times with none vital loss of catalytic activity. The Broccoli green extract modified copper nanoparticles coated on screen printing electrode laid a new sensing platform and has an excellent electrocatalytic activity. Furthermore, surface modified CuNPs with Broccoli green extract exhibited no cytotoxicity at the concentration ranging from 0.5 to 1.5μM on the prostate cancer (PC-3) cell lines. The maximum scavenging % of Broccoli green extract modified CuNPs was found to be >70.50% at the concentration of 0.25mM against 1,1-diphenyl-2-picrylhydrazyl.