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Rational Fabrication of Low‐Coordinate Single‐Atom Ni Electrocatalysts by MOFs for Highly Selective CO 2 Reduction
Author(s) -
Zhang Yan,
Jiao Long,
Yang Weijie,
Xie Chenfan,
Jiang HaiLong
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202016219
Subject(s) - catalysis , rational design , selectivity , faraday efficiency , atom (system on chip) , transition metal , battery (electricity) , metal , chemistry , materials science , nanotechnology , coordination number , combinatorial chemistry , crystallography , electrode , ion , electrochemistry , metallurgy , organic chemistry , physics , computer science , embedded system , power (physics) , quantum mechanics
Single‐atom catalysts (SACs) have attracted tremendous interests due to their ultrahigh activity and selectivity. However, the rational control over coordination microenvironment of SACs remains a grand challenge. Herein, a post‐synthetic metal substitution (PSMS) strategy has been developed to fabricate single‐atom Ni catalysts with different N coordination numbers (denoted Ni‐N x ‐C) on pre‐designed N‐doped carbon derived from metal‐organic frameworks. When served for CO 2 electroreduction, the obtained Ni‐N 3 ‐C catalyst achieves CO Faradaic efficiency (FE) up to 95.6 %, much superior to that of Ni‐N 4 ‐C. Theoretical calculations reveal that the lower Ni coordination number in Ni‐N 3 ‐C can significantly enhance COOH* formation, thereby accelerating CO 2 reduction. In addition, Ni‐N 3 ‐C shows excellent performance in Zn–CO 2 battery with ultrahigh CO FE and excellent stability. This work opens up a new and general avenue to coordination microenvironment modulation (MEM) of SACs for CO 2 utilization.