期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 31, 页码 13057-13062出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202004841
关键词
electrocatalysis; hydrogen peroxide; N2O2 coordination; Ni single atoms; three-phase flow cell
资金
- National Key Projects for Fundamental Research and Development of China [2017YFA0206904, 2017YFA0206900, 2018YFB1502002]
- National Natural Science Foundation of China [51825205, 51772305, 21871279, 21802154, 21902168]
- Beijing Natural Science Foundation [2191002, 2182078, 2194089]
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDB17000000]
- Royal Society-Newton Advanced Fellowship [NA170422]
- International Partnership Program of Chinese Academy of Sciences [GJHZ1819, GJHZ201974]
- Beijing Municipal Science and Technology Project [Z181100005118007]
- K.C. Wong Education Foundation
- Youth Innovation Promotion Association of the CAS
- Energy Education Trust of New Zealand
- MacDiarmid Institute for Advanced Materials and Nanotechnology
Carbon-supported Ni-II single-atom catalysts with a tetradentate Ni-N2O2 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 degrees C in Ar. The Ni-N2O2/C catalyst showed excellent performance for the electrocatalytic reduction of O-2 to H2O2 through a two-electron transfer process in alkaline conditions, with a H2O2 selectivity of 96 %. At a current density of 70 mA cm(-2), a H2O2 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-N2O2/C catalyst could electrocatalytically reduce O-2 in air to H2O2 at a high current density, still affording a high H2O2 selectivity (>90 %). A precise Ni-N2O2 coordination was key to the performance.
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