The electrochemical reactions for the storage of Zn while embracing more electron transfer is a foundation of the future high-energy aqueous zinc batteries. Herein, we report a six-electron transfer electrochemistry of nano-sized TeO /C (n-TeO /C) cathode by facilitating the reversible conversion of TeO ↔Te and Te↔ZnTe. Benefitting from the integrated conductive nanostructure and the proton-rich environment in providing optimized electrochemical kinetics (facilitated Zn uptake and high electronic conductivity) and feasible thermodynamic process (low Gibbs free energy change), the as-prepared n-TeO /C with stable cycling performance exhibits a superior reversible capacity of over 800 mAh g at 0.1 A g . A precise understanding of the reaction mechanism via ex situ and in situ characterizations presents that the reversible six-electron transfer reaction is proton-dependent, and a proton generating and consuming mechanism of three-phase conversion n-TeO /C in the weakly acidic electrolyte is thoroughly revealed.
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http://dx.doi.org/10.1002/anie.202312000 | DOI Listing |
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January 2025
Department of Physics, Vidyasagar University, Midnapore, West Bengal, 721102, India.
Recently electrochemical urea oxidation reaction (UOR) has emerged as the technology of demand for commercialization of urea-based energy conversion. However, the nascent idea is limited by the energy burden of threshold voltage and the sluggish reaction kinetics involving a six-electron transfer mechanism. Herein, for the first time, the engineering of electrocatalysts are proposed with simultaneous inclusion of UOR activator and UOR accelerator.
View Article and Find Full Text PDFLangmuir
November 2024
School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing 210094, China.
Urea oxidation reaction (UOR) is an attractive alternative anodic reaction to oxygen evolution reaction (OER) for its low thermodynamic potential (0.37 V vs RHE). A major challenge that prohibits its practical application is the six-electron transfer process during UOR, demanding enhancements in the catalytic activity.
View Article and Find Full Text PDFJ Am Chem Soc
July 2024
Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States.
Immobilized cobalt phthalocyanine (CoPc) is a highly promising architecture for the six-proton, six-electron reduction of CO to methanol. This electroreduction process relies on proton-coupled electron transfer (PCET) reactions that can occur by sequential or concerted mechanisms. Immobilization on a conductive support such as carbon nanotubes or graphitic flakes can fundamentally alter the PCET mechanisms.
View Article and Find Full Text PDFAdv Mater
July 2024
Department of Materials Science and Engineering, City University of Hong Kong, 83 Tat Chee Avenue, Kowloon, Hong Kong, 999077, China.
Sulfur is a promising conversion-type cathode for zinc batteries (ZBs) due to its high discharge capacity and cost-effectiveness. However, the redox conversion of multivalent S in ZBs is still limited, only having achieved S/S redox conversion with low discharge voltage and poor reversibility. This study presents significant progress by demonstrating, for the first time, the reversible S/S redox behavior in ZBs with up to six-electron transfer (with an achieved discharge capacity of ≈1284 mAh g) using a highly concentrated ClO -containing electrolyte.
View Article and Find Full Text PDFJ Inorg Biochem
July 2024
Department of Biochemistry & Molecular Biology, Michigan State University, East Lansing, MI, USA. Electronic address:
Cytochrome c nitrite reductase, NrfA, is a soluble, periplasmic pentaheme cytochrome responsible for the reduction of nitrite to ammonium in the Dissimilatory Nitrate Reduction to Ammonium (DNRA) pathway, a vital reaction in the global nitrogen cycle. NrfA catalyzes this six-electron and eight-proton reduction of nitrite at a single active site with the help of its quinol oxidase partners. In this review, we summarize the latest progress in elucidating the reaction mechanism of ammonia production, including new findings about the active site architecture of NrfA, as well as recent results that elucidate electron transfer and storage in the pentaheme scaffold of this enzyme.
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