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Controlled Synthesis of a Vacancy‐Defect Single‐Atom Catalyst for Boosting CO 2 Electroreduction
Author(s) -
Rong Xin,
Wang HongJuan,
Lu XiuLi,
Si Rui,
Lu TongBu
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.201912458
Subject(s) - vacancy defect , catalysis , nitrogen , atom (system on chip) , oxygen atom , oxygen , materials science , nitrogen atom , crystallography , faraday efficiency , chemistry , electrode , electrochemistry , ring (chemistry) , molecule , organic chemistry , computer science , embedded system
The reaction of precursors containing both nitrogen and oxygen atoms with Ni II under 500 °C can generate a N/O mixing coordinated Ni‐N 3 O single‐atom catalyst (SAC) in which the oxygen atom can be gradually removed under high temperature due to the weaker Ni−O interaction, resulting in a vacancy‐defect Ni‐N 3 ‐V SAC at Ni site under 800 °C. For the reaction of Ni II with the precursor simply containing nitrogen atoms, only a no‐vacancy‐defect Ni‐N 4 SAC was obtained. Experimental and DFT calculations reveal that the presence of a vacancy‐defect in Ni‐N 3 ‐V SAC can dramatically boost the electrocatalytic activity for CO 2 reduction, with extremely high CO 2 reduction current density of 65 mA cm −2 and high Faradaic efficiency over 90 % at −0.9 V vs. RHE, as well as a record high turnover frequency of 1.35×10 5 h −1 , much higher than those of Ni‐N 4 SAC, and being one of the best reported electrocatalysts for CO 2 ‐to‐CO conversion to date.