Accelerating CO2 Electroreduction to Multicarbon Products via Synergistic Electric–Thermal Field on Copper Nanoneedles

Yang, Baopeng, Liu, Kang, Li, HuangJingWei, Liu, Changxu, Fu, Junwei, Li, Hongmei, Huang, Jianan Erick, Ou, Pengfei, Alkayyali, Tartela, Cai, Chao, Duan, Yuxia, Liu, Hui, An, Pengda, Zhang, Ning, Li, Wenzhang, Qiu, Xiaoqing, Jia, Chuankun, Hu, Junhua, Chai, Liyuan, Lin, Zhang, Gao, Yongli, Miyauchi, Masahiro, Cortés, Emiliano, Maier, Stefan A. and Liu, Min (2022) Accelerating CO2 Electroreduction to Multicarbon Products via Synergistic Electric–Thermal Field on Copper Nanoneedles. Journal of the American Chemical Society, 144 (7). pp. 3039-3049. ISSN 0002-7863

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Official URL: https://doi.org/10.1021/jacs.1c11253

Abstract

Electrochemical CO2 reduction is a promising way to mitigate CO2 emissions and close the anthropogenic carbon cycle. Among products from CO2RR, multicarbon chemicals, such as ethylene and ethanol with high energy density, are more valuable. However, the selectivity and reaction rate of C2 production are unsatisfactory due to the sluggish thermodynamics and kinetics of C–C coupling. The electric field and thermal field have been studied and utilized to promote catalytic reactions, as they can regulate the thermodynamic and kinetic barriers of reactions. Either raising the potential or heating the electrolyte can enhance C–C coupling, but these come at the cost of increasing side reactions, such as the hydrogen evolution reaction. Here, we present a generic strategy to enhance the local electric field and temperature simultaneously and dramatically improve the electric–thermal synergy desired in electrocatalysis. A conformal coating of ∼5 nm of polytetrafluoroethylene significantly improves the catalytic ability of copper nanoneedles (∼7-fold electric field and ∼40 K temperature enhancement at the tips compared with bare copper nanoneedles experimentally), resulting in an improved C2 Faradaic efficiency of over 86% at a partial current density of more than 250 mA cm–2 and a record-high C2 turnover frequency of 11.5 ± 0.3 s–1 Cu site–1. Combined with its low cost and scalability, the electric–thermal strategy for a state-of-the-art catalyst not only offers new insight into improving activity and selectivity of value-added C2 products as we demonstrated but also inspires advances in efficiency and/or selectivity of other valuable electro-/photocatalysis such as hydrogen evolution, nitrogen reduction, and hydrogen peroxide electrosynthesis.

Item Type: Article
Additional Information: Funding information: This work was supported by the Natural Science Foundation of China (Grant Nos. 21872174, 22002189, 22011530423, and U1932148), Technology Cooperation Program (Grant Nos. 2017YFE0127800 and 2018YFE0203400), Hunan Provincial Key Research and Development Program (2020WK2002), Hunan Provincial Natural Science Foundation of China (2020JJ2041 and 2020JJ5691), Hunan Provincial Science and Technology Program (2017XK2026), Shenzhen Science and Technology Innovation Project (Grant No. JCYJ20180307151313532), National Postdoctoral Program for Innovative Talents of China, Postdoctoral Science Foundation of China (Grant No. 2018M640759), Thousand Youth Talents Plan of China and Hundred Youth Talents Program of Hunan, the Hunan Provincial Science and Technology Plan Project (Grant No. 2017TP1001), the Outstanding Youth Exchange Program of China Association for Science and Technology (Grant No. 2018CASTQNJL56), and Fundamental Research Funds for the Central Universities of Central South University (2021zzts0060). We thank Prof. Edward Sargent and Dr. Joshua Wicks for helpful discussions. We acknowledge financial support from the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) under grant numbers EXC 2089/1 − 390776260 (Germany ś Excellence Strategy), the Bavarian State Ministry of Science, Research, and Arts through the program “Solar Technologies Go Hybrid (SolTech)” and the European Commission through the ERC Starting Grant CATALIGHT (802989). S.M. additionally acknowledges the Lee-Lucas Chair in Physics as well as the Engineering and Physical Sciences Research Council (EPSRC UK).
Subjects: F200 Materials Science
H700 Production and Manufacturing Engineering
H800 Chemical, Process and Energy Engineering
Department: Faculties > Engineering and Environment > Mathematics, Physics and Electrical Engineering
Depositing User: John Coen
Date Deposited: 17 Feb 2022 14:49
Last Modified: 16 Mar 2022 14:45
URI: http://nrl.northumbria.ac.uk/id/eprint/48490

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