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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
Na Yang, Gaoqing Yuan
A novel electrochemical route has been developed for the synthesis of 1,5-disubstituted and 1-aryl 1,2,4-triazoles from aryl hydrazines, paraformaldehyde, NH4 OAc, and alcohols. In this multicomponent reaction system, alcohols act as solvents as well as reactants and NH4 OAc is used as the nitrogen source. With the assistance of reactive iodide radical or I2 and NH3 electrogenerated in situ, this process could effectively avoid the use of strong oxidants and transition-metal catalysts and be smoothly carried out at room temperature to give a wide array of 1,2,4-triazole derivatives in good to high yields...
October 5, 2018: Journal of Organic Chemistry
Chen-Yan Cai, Hai-Chao Xu
Dehydrogenative annulation reactions are among the most straightforward and efficient approach for the preparation of cyclic structures. However, the applications of this strategy for the synthesis of saturated heterocycles have been rare. In addition, reported dehydrogenative bond-forming reactions commonly employ stoichiometric chemical oxidants, the use of which reduces the sustainability of the synthesis and brings safety and environmental issues. Herein, we report an organocatalyzed electrochemical dehydrogenative annulation reaction of alkenes with 1,2- and 1,3-diols for the synthesis of 1,4-dioxane and 1,4-dioxepane derivatives...
September 3, 2018: Nature Communications
Yong Jiang, Raymond Jianxiong Zeng
Microbial electrosynthesis (MES) is a novel microbial electrochemical technology proposed for chemicals production with the storage of sustainable energy. However, the practical application of MES is currently restricted by the limited low market value of products in one-step conversion process, mostly acetate. A theme that is pervasive throughout this review is the challenges associated with the expanded product spectrum. Several recent research efforts to improve acetate production, using novel reactor configuration, renewable power supply, and various 3-D cathode are summarized...
December 2018: Bioresource Technology
Saeid Ahmadzadeh, Maryam Dolatabadi
Antibiotics as the severe contaminants of aqueous environments were received growing attention during the last decades. The current work is the first report on investigating the potency and efficiency of electrocoagulation process in the successful removal of metronidazole (MNZ) from pharmaceutical wastewater using response surface methodology based on central composite design. The applied method by optimizing the independent and combined effects of significant variables which affecting the EC process enhanced the removal efficiency of MNZ...
December 2018: Chemosphere
Zhiwei Dong, Haoqi Wang, Shihao Tian, Yang Yang, Hao Yuan, Qiong Huang, Tian-Shun Song, Jingjing Xie
The electricity-driven bioreduction of carbon dioxide to multi-carbon organic compounds, particularly acetate, has been achieved in microbial electrosynthesis (MES). MES performance can be limited by the amount of cathode surface area available for biofilm formation and slow substrate mass transfer. Here, a fluidized three-dimensional electrode, containing granular activated carbon (GAC) particles, was constructed via MES. The volumetric acetate production rate increased by 2.8 times through MES with 16 g L-1 GAC (0...
December 2018: Bioresource Technology
Sebastian Lips, Dieter Schollmeyer, Robert Franke, Siegfried R Waldvogel
A novel strategy for the synthesis of biaryls consisting of a benzothiophene and a phenol moiety is reported. These heterobiaryls are of utmost interest for pharmaceutical, biological, and high-performance optoelectronic applications. The metal- and reagent-free, electrosynthetic, and highly efficient method enables the generation of 2- and 3-(hydroxyphenyl)benzo[b]thiophenes in a regioselective fashion. The described one-step synthesis is easy to conduct, scalable, and inherently safe. The products are afforded in high yields of up to 88 % and with exquisite selectivity...
October 1, 2018: Angewandte Chemie
Niankai Fu, Gregory S Sauer, Song Lin
This protocol describes an electrochemical synthesis of 1,2-diazides from alkenes. Organic azides are highly versatile intermediates for synthetic chemistry, materials, and biological applications. 1,2-Diazides are commonly reduced to form 1,2-diamines, which are prevalent structural motifs in bioactive natural products, therapeutic agents, and molecular catalysts. The electrochemical formation of 1,2-diazides involves the anodic generation of an azidyl radical from sodium azide, followed by two successive additions of this N-centered radical to the alkene, and is assisted by a Mn catalyst...
August 2018: Nature Protocols
Yoo Seok Lee, Seungwoo Baek, Hyeryeong Lee, Stacy Simai Reginald, Yeongeun Kim, Hyunsoo Kang, In-Geol Choi, In Seop Chang
Direct electron transfer (DET) between enzymes and electrodes is a key issue for practical use of bioelectrocatalytic devices as a bioenergy process, such as enzymatic electrosynthesis, biosensors, and enzyme biofuel cells. To date, based on the DET of bioelectrocatalysis, less than 1% of the calculated theoretical current was transferred to final electron acceptor due to energy loss at enzyme-electrode interface. This study describes the design and construction of a synthetic glucose dehydrogenase (GDH; α and γ subunits) combined with a gold-binding peptide at its amino or carboxy terminus for direct contact between enzyme and electrode...
August 29, 2018: ACS Applied Materials & Interfaces
Yansong Zhou, Fanglin Che, Min Liu, Chengqin Zou, Zhiqin Liang, Phil De Luna, Haifeng Yuan, Jun Li, Zhiqiang Wang, Haipeng Xie, Hongmei Li, Peining Chen, Eva Bladt, Rafael Quintero-Bermudez, Tsun-Kong Sham, Sara Bals, Johan Hofkens, David Sinton, Gang Chen, Edward H Sargent
The electrochemical reduction of CO2 to multi-carbon products has attracted much attention because it provides an avenue to the synthesis of value-added carbon-based fuels and feedstocks using renewable electricity. Unfortunately, the efficiency of CO2 conversion to C2 products remains below that necessary for its implementation at scale. Modifying the local electronic structure of copper with positive valence sites has been predicted to boost conversion to C2 products. Here, we use boron to tune the ratio of Cuδ+ to Cu0 active sites and improve both stability and C2 -product generation...
September 2018: Nature Chemistry
Xiang Ren, Guanwei Cui, Liang Chen, Fengyu Xie, Qin Wei, Ziqi Tian, Xuping Sun
A highly attractive, but still a key challenge, is the development of earth-abundant electrocatalysts for efficient NH3 electrosynthesis via the N2 reduction reaction (NRR). In this communication, we report the development of a Mo2N nanorod as a highly efficient and selective NRR electrocatalyst for artificial N2 fixation in acidic electrolytes under ambient conditions. In 0.1 M HCl, this catalyst achieved a high Faradaic efficiency of 4.5% with a NH3 yield of 78.4 μg h-1 mgcat.-1 at -0.3 V vs. a reversible hydrogen electrode, thus outperforming most reported NRR electrocatalysts under ambient conditions and some under harsh conditions...
July 26, 2018: Chemical Communications: Chem Comm
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