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Title: Boosting electrocatalytic hydrogen evolution with anodic oxidative upgrading of formaldehyde over trimetallic carbides
Authors: Du, Xiangbowen
Wei, Tong
Tan, Mingwu
Kobayashi, Hisayoshi
Peng, Zhengxin
Zhu, Hongliang
Jin, Zhikang
Song, Junjie
Liu, Wen
Li, Renhong
Keywords: Engineering::Chemical engineering
Issue Date: 2022
Source: Du, X., Wei, T., Tan, M., Kobayashi, H., Peng, Z., Zhu, H., Jin, Z., Song, J., Liu, W. & Li, R. (2022). Boosting electrocatalytic hydrogen evolution with anodic oxidative upgrading of formaldehyde over trimetallic carbides. ACS Sustainable Chemistry & Engineering, 10(21), 7108-7116.
Journal: ACS Sustainable Chemistry & Engineering
Abstract: Coupling the electrochemical oxidative upgrading of organic molecules with hydrogen evolution reaction could enable the energy-efficient production of H2 from renewable electricity with simultaneous chemical production. This work shows that a trimetallic carbide (Co3Fe3W6C), derived from one-pot synthesis, could act as a robust electrocatalyst for formaldehyde upgrading reaction (FUR) to produce formate at a high faradaic efficiency (>98%), without any production of CO2 or O2. Compared to OER, the input voltages of Co3Fe3W6C-catalyzed FUR are 150 and 120 mV lower to achieve current densities of 10 and 50 mA cm-2, respectively, thereby facilitating a significant boost in the energy efficiency of electrochemical H2 production from water. Density functional theory calculations reveal that the trimetallic carbide system modulates the d band of the transition-metal active sites to achieve optimal adsorption toward the selective oxidation of formaldehyde, while suppressing the further formation of CO2. Co3Fe3W6C was also found to be highly stable under considerably high-throughput electrochemical conditions in an alkaline electrolyte. This work offers a new strategy of synergizing water electrolysis with the oxidative upgrading of organic molecules to simultaneously boost the cost competitiveness of green hydrogen production and the electrochemical upgrading of organic feedstocks.
ISSN: 2168-0485
DOI: 10.1021/acssuschemeng.2c01229
Schools: School of Chemical and Biomedical Engineering 
Rights: This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Sustainable Chemistry & Engineering, copyright © 2022 American Chemical Society, after peer review and technical editing by the publisher. To access the final edited and published work see
Fulltext Permission: open
Fulltext Availability: With Fulltext
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