High-selectivity electroreduction of low-concentration CO_(2)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 

机构地区：[1]MOE International Joint Laboratory of Materials Microstructure,Analysis and Testing Center,Institute for New Energy Materials and Low Carbon Technologies,School of Materials Science and Engineering,School of Chemistry and Chemical Engineering,Tianjin University of Technology,Tianjin300384,China [2]Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),NankaiUniversity,Tianjin 30007,China

出　　处：《Science China Chemistry》2025年第4期1620-1626,共7页中国科学(化学英文版)

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 CO_(2)reduction reaction(CO_(2)RR)has been regarded as one of the most promising solutions to achieving“zero carbon emission”.In most of the CO_(2)RR-related studies;high-purity CO_(2)has been employed as the feed gas;however;in practice;CO_(2)is generally emitted in low concentrations;so it is of great significance to realize high-selectivity electroreduction of low-concentration CO_(2)with large concentration fluctuation.In this work;we constructed a dual-active-site catalyst and successfully achieved CO_(2)local enrichment and conversion for low-concentration CO_(2).Operando experiments reveal that the catalyst has one type of site for activating CO_(2)and 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 vs.RHE).Even when fed with a low-concentration CO_(2)stream(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 CO_(2)volume ratio is as low as 5%.This work offers a feasible route for converting low-concentration CO_(2)via a synergistic effect for dual-active-site catalysts.

关 键 词：electrochemical CO_(2)reduction low-concentration CO_(2) high-selectivity dual-active-site catalyst operando infrared spectroscopy 

分 类 号：O643.3[理学—物理化学]