Author:
Jin Zhaoyong,Yang Meiqi,Dong Yilong,Ma Xingcheng,Wang Ying,Wu Jiandong,Fan Jinchang,Wang Dewen,Xi Rongshen,Zhao Xiao,Xu Tianyi,Zhao Jingxiang,Zhang Lei,Singh David J.,Zheng Weitao,Cui Xiaoqiang
Abstract
AbstractElectrochemical carbon dioxide reduction reaction (CO2RR) involves a variety of intermediates with highly correlated reaction and ad-desorption energies, hindering optimization of the catalytic activity. For example, increasing the binding of the *COOH to the active site will generally increase the *CO desorption energy. Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO2RR, but remains an unsolved challenge. Herein, we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier. This system shows an unprecedented CO2RR intrinsic activity with TOF of 3336 h−1, high selectivity toward CO production, Faradaic efficiency of 95.96% at − 0.60 V and excellent stability. Theoretical calculations show that the Mo-Fe diatomic sites increased the *COOH intermediate adsorption energy by bridging adsorption of *COOH intermediates. At the same time, d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of *CO intermediates. Thus, the undesirable correlation between these steps is broken. This work provides a promising approach, specifically the use of di-atoms, for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.
Funder
Shanghai Jiao Tong University
Publisher
Springer Science and Business Media LLC
Subject
Electrical and Electronic Engineering,Surfaces, Coatings and Films,Electronic, Optical and Magnetic Materials
Cited by
10 articles.
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