卤素
电化学
分子内力
化学
拉曼光谱
立体化学
电极
物理化学
光学
有机化学
物理
烷基
作者
Fengya Ma,Pengfang Zhang,Xiaoyan Zheng,Liang Chen,Yunrui Li,Zechao Zhuang,Yameng Fan,Peng Jiang,Hui Zhao,Jiawei Zhang,Yuming Dong,Yongfa Zhu,Dingsheng Wang,Xiaojing Yao
标识
DOI:10.1002/anie.202412785
摘要
Electrocatalytic reduction of CO2 into C2 products of high economic value provides a promising strategy to realize resourceful CO2 utilization. Rational design and construct dual sites to realize the CO protonation and C-C coupling to unravel their structure-performance correlation is of great significance in catalysing electrochemical CO2 reduction reactions. Herein, Cu-Cu dual sites with different site distance coordinated by halogen at the first-shell are constructed and shows a higher intramolecular electron redispersion and coordination symmetry configurations. The long-range Cu-Cu (Cu-I-Cu) dual sites show an enhanced Faraday efficiency of C2 products, up to 74.1%, and excellent stability. In addition, the linear relationships that the long-range Cu-Cu dual site is accelerated to C2H4 generation and short-range Cu-Cu (Cu-Cl-Cu) dual site is beneficial for C2H5OH formation are disclosed. In situ electrochemical attenuated total reflection surface enhanced infrared absorption spectroscopy, in situ Raman and theoretical calculations manifest that long-range Cu-Cu dual sites can weaken reaction energy barriers of CO hydrogenation and C-C coupling, as well as accelerating deoxygenation of *CH2CHO. This study uncovers the exploitation of site-distance-dependent electrochemical property to steer the CO2 reduction pathway, as well as a potential generic tactic to target C2 synthesis by constructing the desired Cu-Cu dual sites.
科研通智能强力驱动
Strongly Powered by AbleSci AI