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Key Single‐Atom Electrocatalysis in Metal—Organic Framework (MOF)‐Derived Bifunctional Catalysts
Author(s) -
Zhao Wanpeng,
Wan Gang,
Peng Chunlei,
Sheng Huaping,
Wen Jianguo,
Chen Hangrong
Publication year - 2018
Publication title -
chemsuschem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 2.412
H-Index - 157
eISSN - 1864-564X
pISSN - 1864-5631
DOI - 10.1002/cssc.201801473
Subject(s) - electrocatalyst , catalysis , bifunctional , electrochemistry , metal organic framework , chemistry , metal , selectivity , cobalt , nanotechnology , combinatorial chemistry , materials science , inorganic chemistry , organic chemistry , adsorption , electrode
Metal–organic framework (MOF)‐derived materials have attracted increasing interest and show promising catalytic performances in many fields. Intensive efforts have been focused on the structure design and metal‐site integration in MOF‐derived catalysts. However, the key catalytic processes related with the metal sites in MOF‐derived catalysts that dominate the electrocatalytic performance still remain obscure. Herein, we show a neglected but critical issue in the pyrolytic synthesis of MOF‐derived catalysts: the coupled evolution of dual sites, that is, metallic sites and single‐atom metal sites. The identification of active sites of single‐atom sites from the visible particles has been elucidated through the combined X‐ray spectroscopic, electron microscopic, and electrochemical studies. Interestingly, after a total removal of metallic cobalt sites, catalysts with purified single‐atom metal sites show no faltering activity for either the oxygen reduction reaction (ORR) or hydrogen evolution reaction (HER), while significantly enhanced ORR selectivity is achieved; this reveals the dominant activity and selectivity contribution from single‐atom electrocatalysis. The insight of the coupled evolution of dual sites and the as‐demonstrated dual‐site decoupling strategies open up a new routine for the design and synthesis of MOF‐derived catalysts with the optimized single‐atom electrocatalysis towards various electrochemical reactions.