Chlorine-induced mixed valence of CuO_(x)/C to promote the electroreduction of carbon dioxide to ethylene  

作　　者：Xin Wang Ming Miao Bowen Tang Haotian Duan Fulong Zhu Huigang Zhang Xian Zhang Wen-jin Yin Yongzhu Fu 

机构地区：[1]College of Chemistry,Zhengzhou University,Zhengzhou 450001,China [2]School of Physics and Electronic Science,Hunan University of Science and Technology,Xiangtan 411201,China [3]State Key Laboratory of Multiphase Complex Systems,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China [4]Qian Xuesen Laboratory of Space Technology,China Academy of Space Technology,Beijing 100094,China

出　　处：《Nano Research》2023年第7期8827-8835,共9页纳米研究（英文版）

基　　金：This work was financially supported by the Natural Science Foundation of Henan province(No.212300410281);the National Key Research and Development Program of China(No.2020YFA0406104);the National Natural Science Foundation of China(No.22001263).

摘　　要：Electrochemical conversion of CO_(2)(CO_(2)RR)into high-value fuel is identified as one of the promising approaches to achieve carbon neutrality.The synthesis of high-efficiency CO_(2)reduction electrocatalysts with high C_(2):C_(1) selectivity remains a field of intense interest.Previous studies have shown that the presence of Cu(I)is beneficial for the reduction of CO_(2)into C_(2)products.However,the stable presence of Cu(I)remains controversial,especially in the negative potential window.Here we report a simple and easily scalable catalyst precursor Cu_(2)(OH)_(3)Cl/C,which automatically forms in-situ chlorine-doped Cu/Cu_(2)O heterointerface during electrocatalysis.The catalyst not only exhibits a Faradaic efficiency of 33.03%but also provides a long-term stability of Cu^(+),gaining a stable electrolysis of 11 h,with an ethylene/methane ratio over 50.The experimental results and mechanistic studies confirm that the presence of Cl^(-)inhibits the reduction of Cu^(+),inducing the formation of Cu^(0)/Cu^(+),and reduces the reaction energy of the intermediate ^(*)CO dimerization,thereby facilitating the formation of C_(2)products.This work provides a feasible way to synthesize copper ions with long-term and stable positive charge in CO_(2)RR and expands a new way to synthesize ethylene industrial products in the future.

关 键 词：basic copper chloride chlorine dopant mixed-phase catalysts CO_(2)reduction reaction ETHYLENE 

分 类 号：O64[理学—物理化学]