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Temperature-dependent pathways in carbon dioxide electroreduction


Abstract Temperature affects both the thermodynamics of intermediate adsorption and the kinetics of elementary reactions. Despite its extensive study in thermocatalysis, temperature effect is typically overlooked in electrocatalysis. This study investigates how electrolyte temperature influences CO2 electroreduction over Cu catalysts. Theoretical calculations reveal the significant impact of temperature on *CO and *H intermediate adsorption thermodynamics, water microenvironment at the electrode surface, and the electron density and covalent property of the C–O bond in the *CH–COH intermediate, crucial for the reaction pathways. The theoretical calculations are strongly verified by experimental results over different Cu catalysts. Faradaic efficiency (FE) toward multicarbon (C2+) products is favored at low temperatures. Cu nanorod electrode could achieve a FEC2+ value of 90.1% with a current density of ∼400 mA cm−2 at −3 °C. FEC2H4 and FEC2H5OH show opposite trends with decreasing temperature. The FEC2H4/FEC2H5OH ratio can decrease from 1.86 at 40 °C to 0.98 at −3 °C.
Authors Shiqiang Liu ORCID , Yaoyu Yin ORCID , Jiahao Yang ORCID , Wenling Zhao ORCID , Meng Zhou ORCID , Huisheng Qin , Jiapeng Jiao , Yiyong Wang , Hengan Wang , Xing Tong , Yi Xu ORCID , Xiaofu Sun ORCID , Qinggong Zhu ORCID , Maohong Fan University of WyomingORCID , Xinchen Kang ORCID , Buxing Han ORCID
Journal Info Elsevier BV | Science Bulletin
Publication Date 1/1/2025
ISSN 2095-9273
TypeKeyword Image article
Open Access green Green Access
DOI https://doi.org/10.1016/j.scib.2024.12.052
KeywordsKeyword Image