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Unveiling Electrochemical Urea Synthesis by Co‐Activation of CO 2 and N 2 with Mott–Schottky Heterostructure Catalysts
Author(s) -
Yuan Menglei,
Chen Junwu,
Bai Yiling,
Liu Zhanjun,
Zhang Jingxian,
Zhao Tongkun,
Wang Qin,
Li Shuwei,
He Hongyan,
Zhang Guangjin
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.202101275
Subject(s) - heterojunction , electrochemistry , nucleophile , urea , exothermic reaction , catalysis , adsorption , endothermic process , electrophile , faraday efficiency , molecule , materials science , inorganic chemistry , chemistry , photochemistry , electrode , organic chemistry , optoelectronics
Electrocatalytic C−N bond coupling to convert CO 2 and N 2 molecules into urea under ambient conditions is a promising alternative to harsh industrial processes. However, the adsorption and activation of inert gas molecules and then the driving of the C–N coupling reaction is energetically challenging. Herein, novel Mott–Schottky Bi‐BiVO 4 heterostructures are described that realize a remarkable urea yield rate of 5.91 mmol h −1 g −1 and a Faradaic efficiency of 12.55 % at −0.4 V vs. RHE. Comprehensive analysis confirms the emerging space–charge region in the heterostructure interface not only facilitates the targeted adsorption and activation of CO 2 and N 2 molecules on the generated local nucleophilic and electrophilic regions, but also effectively suppresses CO poisoning and the formation of endothermic *NNH intermediates. This guarantees the desired exothermic coupling of *N=N* intermediates and generated CO to form the urea precursor, *NCON*.