NiSn Atomic Pair on an Integrated Electrode for Synergistic Electrocatalytic CO2 Reduction

• Published in: Angewandte Chemie International Edition Vol. 60; no. 13; pp. 7382 - 7388
• Main Authors: Xie, Wenfu, Li, Hao, Cui, Guoqing, Li, Jianbo, Song, Yuke, Li, Shijin, Zhang, Xin, Lee, Jin Yong, Shao, Mingfei, Wei, Min
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 22.03.2021
• Edition: International ed. in English
• Subjects: Carbon dioxide; carbon dioxide fixation; Catalysis; Catalysts; Chemical reduction; Electrocatalysts; electrochemistry; Electrodes; heterogeneous catalysis; Nitrogen atoms; reduction; Selectivity; structure elucidation; Synergistic effect
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202014655

The development of efficient electrocatalysts for the CO2 reduction reaction (CO2RR) remains a challenge. Demonstrated here is a NiSn atomic‐pair electrocatalyst (NiSn‐APC) on a hierarchical integrated electrode, which exhibits a synergistic effect in simultaneously promoting the activity and selectivity of the CO2RR to formate. The NiSn atomic pair consists of adjacent Ni and Sn, each coordinated with four nitrogen atoms (N4‐Ni‐Sn‐N4). The as‐prepared NiSn‐APC displays exceptional activity for the CO2RR to formate with a turnover frequency of 4752 h−1, a formate productivity of 36.7 mol h−1 gSn−1 and an utilization degree of active sites (57.9 %), which are superior to previously reported single‐atomic catalysts. Both experimental data and density‐functional theory calculations verify the electron redistribution of Sn imposed by adjacent Ni, which reduces the energy barrier of the *OCHO intermediate and makes this potential‐determining step thermodynamically spontaneous. This synergistic catalysis provides a successful paradigm for rational design and preparation of atomic‐pair electrocatalysts with enhanced performance. A NiSn atomic‐pair electrocatalyst (NiSn‐APC) that consists of adjacent Ni and Sn, each coordinated with four nitrogen atoms (N4‐Ni‐Sn‐N4), has been synthesized. By virtue of the synergistic effect and the enhanced utilization degree of the active site, NiSn‐APC exhibits outstanding electrocatalytic activity and selectivity for the CO2 reduction reaction (CO2RR) to formate.