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High‐Efficiency Oxygen Reduction to Hydrogen Peroxide Catalyzed by Nickel Single‐Atom Catalysts with Tetradentate N 2 O 2 Coordination in a Three‐Phase Flow Cell
Author(s) -
Wang Yulin,
Shi Run,
Shang Lu,
Waterhouse Geoffrey I. N.,
Zhao Jiaqi,
Zhang Qinghua,
Gu Lin,
Zhang Tierui
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.202004841
Subject(s) - catalysis , nickel , selectivity , ligand (biochemistry) , schiff base , chemistry , hydrogen peroxide , carbon fibers , pyrolysis , adsorption , inorganic chemistry , materials science , crystallography , organic chemistry , biochemistry , receptor , composite number , composite material
Carbon‐supported Ni II single‐atom catalysts with a tetradentate Ni‐N 2 O 2 coordination formed by a Schiff base ligand‐mediated pyrolysis strategy are presented. A Ni II complex of the Schiff base ligand ( R , R )‐(−)‐N,N′‐bis(3,5‐di‐tert‐butylsalicylidene)‐1,2‐cyclohexanediamine was adsorbed onto a carbon black support, followed by pyrolysis of the modified carbon material at 300 °C in Ar. The Ni‐N 2 O 2 /C catalyst showed excellent performance for the electrocatalytic reduction of O 2 to H 2 O 2 through a two‐electron transfer process in alkaline conditions, with a H 2 O 2 selectivity of 96 %. At a current density of 70 mA cm −2 , a H 2 O 2 production rate of 5.9 mol g cat. −1 h −1 was achieved using a three‐phase flow cell, with good catalyst stability maintained over 8 h of testing. The Ni‐N 2 O 2 /C catalyst could electrocatalytically reduce O 2 in air to H 2 O 2 at a high current density, still affording a high H 2 O 2 selectivity (>90 %). A precise Ni‐N 2 O 2 coordination was key to the performance.