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Highly Efficient CO 2 Electroreduction on ZnN 4 ‐based Single‐Atom Catalyst
Author(s) -
Yang Fa,
Song Ping,
Liu Xiaozhi,
Mei Bingbao,
Xing Wei,
Jiang Zheng,
Gu Lin,
Xu Weilin
Publication year - 2018
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.201805871
Subject(s) - overpotential , catalysis , faraday efficiency , carbon monoxide , electrochemistry , atom (system on chip) , carbon fibers , selectivity , chemistry , redox , inorganic chemistry , electrochemical reduction of carbon dioxide , materials science , electrode , organic chemistry , composite material , composite number , computer science , embedded system
The electrochemical reduction reaction of carbon dioxide (CO2RR) to carbon monoxide (CO) is the basis for the further synthesis of more complex carbon‐based fuels or attractive feedstock. Single‐atom catalysts have unique electronic and geometric structures with respect to their bulk counterparts, thus exhibiting unexpected catalytic activities. A nitrogen‐anchored Zn single‐atom catalyst is presented for CO formation from CO2RR with high catalytic activity (onset overpotential down to 24 mV), high selectivity (Faradaic efficiency for CO (FE CO ) up to 95 % at −0.43 V), remarkable durability (>75 h without decay of FE CO ), and large turnover frequency (TOF, up to 9969 h −1 ). Further experimental and DFT results indicate that the four‐nitrogen‐anchored Zn single atom (Zn‐N 4 ) is the main active site for CO2RR with low free energy barrier for the formation of *COOH as the rate‐limiting step.