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Haimin Zhang, Guoqiang Liu, Zhiqing Cui, Miaomiao Han, Shengbo Zhang, Cuijiao Zhao, Chun Chen, Guozhong Wang
Electrosynthesis of NH3 from N2 reduction reaction (NRR) at ambient conditions has been regarded as a promising technology to replace the industrial energy and capital intensive Haber-Bosch process. Here we report a room-temperature spontaneous redox approach to fabricate core-shell structure Au@CeO2 composite with Au nanoparticle sizes below ~10 nm and loading amount of 3.6 wt.% for the NRR. The results demonstrate that the as-synthesized Au@CeO2 possesses a surface area of 40.7 m2 g-1 and porous structure, as electrocatalyst exhibiting high NRR activity with a NH3 yield rate of 28...
February 14, 2019: Chemistry: a European Journal
Jeannine Mayr, Jan-Hendrick Grosch, Lena Hartmann, Luis F M Rosa, Antje C Spiess, Falk Harnisch
Chiral alcohols constitute important building blocks that can be produced enantioselectively using NAD(P)H-dependent oxidoreductases. For NAD(P)H regeneration, electricity delivers the cheapest reduction equivalents. Enzymatic electrosynthesis suffers from cofactor and enzyme instability, whereas microbial electrosynthesis (MES) exploits whole cells. Here, we demonstrate MES using resting Escherichia coli as biocatalytic chassis for a production platform towards fine chemicals using electric power. This chassis was exemplified for the synthesis of chiral alcohols by using a NADPH-dependent alcohol dehydrogenase from Lactobacillus brevis for synthesis of (R)-1-phenylethanol from acetophenone...
February 14, 2019: ChemSusChem
Adolf Krige, Magnus Sjöblom, Kerstin Ramser, Paul Christakopoulos, Ulrika Rova
Bio-electrochemical systems such as microbial fuel cells and microbial electrosynthesis cells depend on efficient electron transfer between the microorganisms and the electrodes. Understanding the mechanisms and dynamics of the electron transfer is important in order to design more efficient reactors, as well as modifying microorganisms for enhanced electricity production. Geobacter are well known for their ability to form thick biofilms and transfer electrons to the surfaces of electrodes. Currently, there are not many "on-line" systems for monitoring the activity of the biofilm and the electron transfer process without harming the biofilm...
February 12, 2019: Molecules: a Journal of Synthetic Chemistry and Natural Product Chemistry
Garrett W Roell, Jian Zha, Rhiannon R Carr, Mattheos A Koffas, Stephen S Fong, Yinjie J Tang
During microbial applications, metabolic burdens can lead to a significant drop in cell performance. Novel synthetic biology tools or multi-step bioprocessing (e.g., fermentation followed by chemical conversions) are therefore needed to avoid compromised biochemical productivity from over-burdened cells. A possible solution to address metabolic burden is Division of Labor (DoL) via natural and synthetic microbial consortia. In particular, consolidated bioprocesses and metabolic cooperation for detoxification or cross feeding (e...
February 8, 2019: Microbial Cell Factories
Zaiqiang Wu, Junsong Wang, Jun Liu, Yan Wang, Changhao Bi, Xueli Zhang
BACKGROUND: Electrochemical energy is a key factor of biosynthesis, and is necessary for the reduction or assimilation of substrates such as CO2 . Previous microbial electrosynthesis (MES) research mainly utilized naturally electroactive microbes to generate non-specific products. RESULTS: In this research, an electroactive succinate-producing cell factory was engineered in E. coli T110(pMtrABC, pFccA-CymA) by expressing mtrABC, fccA and cymA from Shewanella oneidensis MR-1, which can utilize electricity to reduce fumarate...
January 28, 2019: Microbial Cell Factories
Hlamulo Makelane, Tesfaye Waryo, Usisipho Feleni, Emmanuel Iwuoha
A sensitive dendritic star copolymer-based sensor for pyrene (PY), was developed by in situ electrosynthesis of generation 3 poly(propylene thiophenoimine)-co-poly(3-hexylthiophene) (G3PPT-co-P3HT) on a gold disk electrode (Au). The electrochemical reactivity and the signal transduction properties of the Au|G3PPT-co-P3HT co-polymer electrode were studied by second harmonic alternating current voltammetry (SHACV) and alternating current voltammetry (ACV), respectively. SHACV analysis confirmed the occurrence of Faradaic electrode process (with a standard rate constant, k0 value of 3...
May 1, 2019: Talanta
Wojciech Grochala, Piotr Polczynski, Rafal Jurczakowski, Adam Grzelak, Evgeny Goreshnik, Zoran Mazej
We report the use of the boron doped diamond electrode as a sufficiently stable electrode for electrochemical measurements/synthesis in liquid anhydrous hydrogen fluoride medium. Electrooxidation of silver(I) has been studied in this solvent by using classical transient electrochemical methods and impedance spectroscopy. It has been found that faradaic currents related to silver(I) oxidation and the fluorine evolution reaction are reasonably separated at the potential scale which allows for efficient electrosynthesis of Ag(II)F2, a powerful oxidizer...
January 25, 2019: Chemistry: a European Journal
Peng Qian, Zicong Yan, Zhenghong Zhou, Kangfei Hu, Jiawei Wang, Zhibin Li, Zhenggen Zha, Zhiyong Wang
An NH4I-mediated tandem electrosynthesis of 1,3-disubstituted imidazo[1,5-a]quinolines was developed from readily available starting materials in aqueous medium, affording a variety of 1,3-disubstituted imidazo[1,5-a]quinolines with good to excellent yields.
January 16, 2019: Journal of Organic Chemistry
Hathaichanok Seelajaroen, Marianne Haberbauer, Christine Hemmelmair, Abdalaziz Aljabour, Liviu Mihai Dumitru, Achim Walter Hassel, Niyazi Serdar Sariciftci
Microbial electrosynthesis cells containing Methylobacterium extorquens were studied for reduction of CO2 to formate via direct electron injection and redox mediator-assisted approaches with CO2 as the sole carbon source. The study revealed the formation of the biofilm on a carbon felt electrode while applying a constant potential of -0.75 V vs. Ag/AgCl under CO2-saturated condition. During the biofilm growth period, continuous H2 evolution was observed. The long-term performance for CO2 reduction of the biofilm with and without neutral red as redox mediator was studied by an applied potential of -0...
January 4, 2019: Chembiochem: a European Journal of Chemical Biology
Long Zou, Yun-Hong Huang, Zhong-Er Long, Yan Qiao
Microbial electrochemical system (MES) has attracted ever-growing interest as a promising platform for renewable energy conversion and bioelectrochemical remediation. Shewanella species, the dissimilatory metal reduction model bacteria with versatile extracellular electron transfer (EET) strategies, are the well-received microorganisms in diverse MES devices for various practical applications as well as microbial EET mechanism investigation. Meanwhile, the available genomic information and the unceasing established gene-editing toolbox offer an unprecedented opportunity to boost the applications of Shewanella species in MES...
December 19, 2018: World Journal of Microbiology & Biotechnology
Nianjun Yang, Siyu Yu, Julie V Macpherson, Yasuaki Einaga, Hongying Zhao, Guohua Zhao, Greg M Swain, Xin Jiang
Conductive diamond possesses unique features as compared to other solid electrodes, such as a wide electrochemical potential window, a low and stable background current, relatively rapid rates of electron-transfer for soluble redox systems without conventional pretreatment, long-term responses, stability, biocompatibility, and a rich surface chemistry. Conductive diamond microcrystalline and nanocrystalline films, structures and particles have been prepared using a variety of approaches. Given these highly desirable attributes, conductive diamond has found extensive use as an enabling electrode across a variety of fields encompassing chemical and biochemical sensing, environmental degradation, electrosynthesis, electrocatalysis, and energy storage and conversion...
November 16, 2018: Chemical Society Reviews
Yong Jiang, Harold D May, Lu Lu, Peng Liang, Xia Huang, Zhiyong Jason Ren
Carbon-rich waste materials (solid, liquid, or gaseous) are largely considered to be a burden on society due to the large capital and energy costs for their treatment and disposal. However, solid and liquid organic wastes have inherent energy and value, and similar as waste CO2 gas they can be reused to produce value-added chemicals and materials. There has been a paradigm shift towards developing a closed loop, biorefinery approach for the valorization of these wastes into value-added products, and such an approach enables a more carbon-efficient and circular economy...
November 2, 2018: Water Research
Jun Li, Fanglin Che, Yuanjie Pang, Chengqin Zou, Jane Y Howe, Thomas Burdyny, Jonathan P Edwards, Yuhang Wang, Fengwang Li, Ziyun Wang, Phil De Luna, Cao-Thang Dinh, Tao-Tao Zhuang, Makhsud I Saidaminov, Shaobo Cheng, Tianpin Wu, Y Zou Finfrock, Lu Ma, Shang-Hsien Hsieh, Yi-Sheng Liu, Gianluigi A Botton, Way-Faung Pong, Xiwen Du, Jinghua Guo, Tsun-Kong Sham, Edward H Sargent, David Sinton
The electrochemical reduction of carbon monoxide is a promising approach for the renewable production of carbon-based fuels and chemicals. Copper shows activity toward multi-carbon products from CO reduction, with reaction selectivity favoring two-carbon products; however, efficient conversion of CO to higher carbon products such as n-propanol, a liquid fuel, has yet to be achieved. We hypothesize that copper adparticles, possessing a high density of under-coordinated atoms, could serve as preferential sites for n-propanol formation...
November 5, 2018: Nature Communications
Laura Rago, Sarah Zecchin, Federica Villa, Andrea Goglio, Anna Corsini, Lucia Cavalca, Andrea Schievano
A new approach to microbial electrosynthesis is proposed, aimed at producing whole biomass from N2 and inorganic carbon, by electrostimulation of complex microbial communities. On a carbon-based conductor under constant polarization (-0.7 V vs SHE), an electroactive biofilm was enriched with autotrophic nitrogen fixing microorganims and led to biomass synthesis at higher amounts (up to 18 fold), as compared to controls kept at open circuit (OC). After 110 days, the electron transfer had increased by 30-fold, as compared to abiotic conditions...
February 2019: Bioelectrochemistry
Clifford Morrison, Elizabeth Heitmann, William Armiger, David Dodds, Mattheos Koffas
Two seemingly distinct fields, industrial biocatalysis and microbial electrosynthesis, can be viewed together through the lens of electrochemical bioreactor technology in order to highlight the challenges that exist in creating a versatile platform technology for use in chemical and biological applications. Industrial biocatalysis applications requiring NAD(P)H to perform redox transformations often necessitate convoluted coupled-enzyme regeneration systems to regenerate reduced cofactor, NAD(P)H from oxidized cofactor, NAD(P)...
2018: Advances in Applied Microbiology
Zhipeng Chen, Xiaohan Wang, Licheng Liu
The electrochemical reduction of carbon dioxide (CO2 ) to value-added products obtains great attention and investigation worldwide in recent years. The commercialization of this green process relies on the progress of relating high-performance electrocatalysts and their feasibility with proper reactor design. The microbial electrosynthesis (MES) is an alternative route to reduce CO2 with electroactive bio-film electrode as catalyst. This review presents the research status and development of cathode catalysts, particularly focusing on the active sites and development tendency, for highly efficient electrochemical reduction CO2 from personal viewpoint...
October 9, 2018: Chemical Record: An Official Publication of the Chemical Society of Japan ... [et Al.]
Jianbin Chen, Shide Lv, Siyu Tian
Transition-metal-catalyzed C-H activation attracts tremendous attentions in organic synthetic community because it obviates pre-functionalization of substrates.[1] Significant advances have been dedicated in the past several decades. However, it should be notated that super stoichiometric chemical oxidants, such as copper- or silver-based metal oxidants, benzoquinones (BQ), organic peroxides, potassium persulfate (K2S2O8), hypervalent iodine molecular oxygen (O2) and so on that are required for most of the reactions...
October 2, 2018: ChemSusChem
Zhi-Qin Liang, Tao-Tao Zhuang, Ali Seifitokaldani, Jun Li, Chun-Wei Huang, Chih-Shan Tan, Yi Li, Phil De Luna, Cao Thang Dinh, Yongfeng Hu, Qunfeng Xiao, Pei-Lun Hsieh, Yuhang Wang, Fengwang Li, Rafael Quintero-Bermudez, Yansong Zhou, Peining Chen, Yuanjie Pang, Shen-Chuan Lo, Lih-Juann Chen, Hairen Tan, Zheng Xu, Suling Zhao, David Sinton, Edward H Sargent
Copper-based materials are promising electrocatalysts for CO2 reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO2 reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO2 reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C2+ products...
September 20, 2018: Nature Communications
Zhenhua Li, Junya Cui, Yunke Liu, Jianbo Li, Ke Liu, Mingfei Shao
An efficient and controllable method to synthesize continuous metal-organic framework (MOF) films is highly desired. Herein, we demonstrate a facile and universal electrochemical method to synthesize homogeneous and uniform zeolitic imidazolate framework (ZIF, a typical class of MOF family) films on various macroconductive substrates (e.g., conductive glass, Ni foam and carbon cloth) as well as nanostructured substrates (one-dimensional nanorod array, two-dimensional nanowall array, and three-dimensional nanoframework)...
October 10, 2018: ACS Applied Materials & Interfaces
Huai-Bo Zhao, Pin Xu, Jinshuai Song, Hai-Chao Xu
The synthesis of polycyclic N-heteroaromatic compounds and their corresponding N-oxides has been developed through electrochemical C-H functionalization of biaryl ketoximes. The oxime substrates undergo dehydrogenative cyclization when a Pt cathode is used, resulting in unprecedented access to a wide range of N-heteroaromatic N-oxides. The products of the electrosynthesis are switched to the deoxygenated N-heteroaromatics by employing a Pb cathode through sequential anode-promoted dehydrogenative cyclization and cathodic cleavage of the N-O bond in the initially formed N-oxide...
September 17, 2018: Angewandte Chemie
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