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Coordination Tunes Selectivity: Two‐Electron Oxygen Reduction on High‐Loading Molybdenum Single‐Atom Catalysts
Author(s) -
Tang Cheng,
Jiao Yan,
Shi Bingyang,
Liu JiaNing,
Xie Zhenhua,
Chen Xiao,
Zhang Qiang,
Qiao ShiZhang
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202003842
Subject(s) - catalysis , electrocatalyst , molybdenum , selectivity , chemistry , electrochemistry , atom (system on chip) , metal , scanning transmission electron microscopy , x ray absorption fine structure , dopant , transmission electron microscopy , inorganic chemistry , crystallography , photochemistry , nanotechnology , materials science , electrode , organic chemistry , spectroscopy , physics , quantum mechanics , computer science , embedded system , optoelectronics , doping
Single‐atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and metal loading. However, doing so is still a great challenge because of the limited synthesis approach and insufficient understanding of the structure–property relationships. Herein, we report a new kind of Mo SAC with a unique O,S coordination and a high metal loading over 10 wt %. The isolation and local environment was identified by high‐angle annular dark‐field scanning transmission electron microscopy and extended X‐ray absorption fine structure. The SACs catalyze the oxygen reduction reaction (ORR) via a 2 e − pathway with a high H 2 O 2 selectivity of over 95 % in 0.10 m KOH. The critical role of the Mo single atoms and the coordination structure was revealed by both electrochemical tests and theoretical calculations.