Super-Coordinated Nickel N4 Ni1 O2 Site Single-Atom Catalyst for Selective H2 O2 Electrosynthesis at High Current Densities

Chuqian Xiao; Ling Cheng; Yihua Zhu; Gengchao Wang; Luyang Chen; Yating Wang; Rongzhen Chen; Yuhang Li; Chunzhong Li

doi:10.1002/anie.202206544

Super-Coordinated Nickel N₄ Ni₁ O₂ Site Single-Atom Catalyst for Selective H₂ O₂ Electrosynthesis at High Current Densities

Angew Chem Int Ed Engl. 2022 Sep 19;61(38):e202206544. doi: 10.1002/anie.202206544. Epub 2022 Aug 16.

Authors

Chuqian Xiao¹, Ling Cheng², Yihua Zhu¹, Gengchao Wang¹, Luyang Chen¹, Yating Wang¹, Rongzhen Chen¹, Yuhang Li¹, Chunzhong Li^{1

2}

Affiliations

¹ Key Laboratory for Ultrafine Materials of Ministry of Education, Shanghai Engineering Research Center of Hierarchical Nanomaterials, Frontiers Science Center for Materiobiology and Dynamic Chemistry, School of Materials Science and Engineering, East China University of Science & Technology, Shanghai, 200237, China.
² School of Chemical Engineering, East China University of Science & Technology, Shanghai, 200237, China.

PMID: 35916327
DOI: 10.1002/anie.202206544

Abstract

Electrochemical production of hydrogen peroxide (H₂ O₂ ) from O₂ on single-atom catalysts has attracted great attention, yet the quest for robust catalysts is driven by achieving >90 % Faradaic efficiency (FE) under industrial-relevant current densities (>100 mA cm^-2 ). Herein we synthesize a catalyst that contains single nickel site coordinated by four nitrogen and two oxygen atoms (i.e., N₄ Ni₁ O₂ ) via involving carboxyl functionalized multiwall carbon nanotubes as a substrate to provide extra O coordination to the regular NiN₄ site. It has a cathodic energy efficiency of approximately 82 % and a H₂ O₂ FE of around 96 % at 200 mA cm^-2 current density, outperforming the reported single-atom catalysts for H₂ O₂ electrosynthesis.

Keywords: Electrocatalysis; Hydrogen Peroxide; Nickel; Single-Atom Catalyst; Super Coordination Number.

Abstract

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