High-selectivity electroreduction of low-concentration CO2 with large concentration fluctuation

作     者：Mengyu Qi Yanbin Ma Chao Zhang Bingwei Li Xueqing Yang Zhaolin Shi Simeng Liu Changhua An Jiqing Jiao Tongbu Lu 

作者机构：MOE International Joint Laboratory of Materials MicrostructureAnalysis and Testing CenterInstitute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringSchool of Chemistry and Chemical EngineeringTianjin University of Technology Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Nankai University 

出 版 物：《Science China Chemistry》 (中国科学:化学(英文版))

年 卷 期：2025年

核心收录：

学科分类：083002[工学-环境工程] 0830[工学-环境科学与工程（可授工学、理学、农学学位）] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 080502[工学-材料学] 0805[工学-材料科学与工程（可授工学、理学学位）] 

基　　金：supported by the National Key R&D Program of China (2022YFA1502902) the National Natural Science Foundation of China (52072260, 52472236, 21931007, 21790052, U21A20317) the Tianjin Natural Science Foundation (21JCZXJC00130, B2021201074) the Science and Technology Support Program for Youth Innovation in Universities of Shandong Province (2020KJA012) the Key Project of Natural Science Foundation of Tianjin City (22JCZDJC00510) 

摘      要：Electrochemical CO2reduction reaction（CO2RR） has been regarded as one of the most promising solutions to achieving “zero carbon emission. In most of the CO2RR-related studies, high-purity CO2has been employed as the feed gas; however, in practice, CO2is generally emitted in low concentrations, so it is of great significance to realize high-selectivity electroreduction of low-concentration CO2with large concentration fluctuation. In this work, we constructed a dual-active-site catalyst and successfully achieved CO2local enrichment and conversion for low-concentration CO2. Operando experiments reveal that the catalyst has one type of site for activating CO2and one type of site for binding the reaction intermediates. The dual-active-site catalyst displays a selectivity for formic acid consistently above 97% over a broad potential window（from-0.9 to-1.6 V ***）. Even when fed with a low-concentration CO2stream（volume ratio from 50% down to 10%）, the dual-active-site catalyst could display high activity and selectivity（91%）. In particular, the selectivity is still above 85% when the CO2volume ratio is as low as 5%. This work offers a feasible route for converting low-concentration CO2via a synergistic effect for dual-active-site catalysts.