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The Controllable Reconstruction of Bi‐MOFs for Electrochemical CO 2 Reduction through Electrolyte and Potential Mediation
Author(s) -
Yao Dazhi,
Tang Cheng,
Vasileff Anthony,
Zhi Xing,
Jiao Yan,
Qiao ShiZhang
Publication year - 2021
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.202104747
Subject(s) - formate , electrochemistry , catalysis , electrolyte , materials science , raman spectroscopy , rational design , dissociation (chemistry) , chemical engineering , surface reconstruction , selectivity , nanotechnology , inorganic chemistry , chemistry , electrode , organic chemistry , physics , geometry , mathematics , engineering , surface (topology) , optics
Monitoring and controlling the reconstruction of materials under working conditions is crucial for the precise identification of active sites, elucidation of reaction mechanisms, and rational design of advanced catalysts. Herein, a Bi‐based metal–organic framework (Bi‐MOF) for electrochemical CO 2 reduction is selected as a case study. In situ Raman spectra combined with ex situ electron microscopy reveal that the intricate reconstruction of the Bi‐MOF can be controlled using two steps: 1) electrolyte‐mediated dissociation and conversion of Bi‐MOF to Bi 2 O 2 CO 3 , and 2) potential‐mediated reduction of Bi 2 O 2 CO 3 to Bi. The intentionally reconstructed Bi catalyst exhibits excellent activity, selectivity, and durability for formate production, and the unsaturated surface Bi atoms formed during reconstruction become the active sites. This work emphasizes the significant impact of pre‐catalyst reconstruction under working conditions and provides insight into the design of highly active and stable electrocatalysts through the regulation of these processes.