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Efficient Alkaline Water Oxidation with a Regenerable Nickel Pseudo-Complex

  • Peikun Zhang
    Peikun Zhang
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Peikun Zhang
  • Pai Wang
    Pai Wang
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    More by Pai Wang
  • Wei Wang
    Wei Wang
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    Yangtza Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, China
    More by Wei Wang
  • Qianbao Wu
    Qianbao Wu
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
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  • Mengjun Xiao
    Mengjun Xiao
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
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  • Roger Alberto
    Roger Alberto
    Department of Chemistry, University of Zürich, Winterthurerstrasse 190, Zürich CH-8057, Switzerland
  • Yanning Zhang*
    Yanning Zhang
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    *Email: [email protected]
  • , and 
  • Chunhua Cui*
    Chunhua Cui
    Molecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
    Yangtza Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, China
    *Email: [email protected]
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Cite this: ACS Appl. Mater. Interfaces 2021, 13, 41, 48661–48668
Publication Date (Web):October 7, 2021
https://doi.org/10.1021/acsami.1c13609
Copyright © 2021 American Chemical Society
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Abstract

Efficient and robust electrocatalysts are required for the oxygen evolution reaction (OER). Photosystem II-inspired synthetic transition metal complexes have shown promising OER activity in water-poor or mild conditions, yet challenges remain in the improvement of current density and performance stability for practical applications in alkaline electrolytes in contrast to solid-state oxide catalysts. Here, we report that a nickel pseudo-complex (bpy)zNiOxHy (bpy = 2,2′-bipyridine) catalyst, which bridges solid oxide and molecular catalysts, exhibits the highest OER activity among nickel-based catalysts with a turnover frequency of 1.1 s–1 at an overpotential of 0.30 volts, even outperforming iron-incorporated nickel (oxy)hydroxide under an identical nickel mass load. Benefiting from the strong coordination between bpy and nickel, this (bpy)zNiOxHy catalyst exhibits long-term stability in highly alkaline media at 1.0 mA cm–2 for over 200 h and at 20 mA cm–2 for over 60 h. Our findings indicate that dynamically coordinating a small amount of bpy in the catalyst layer efficiently sustains highly active nickel sites for water oxidation, demonstrating a general strategy for improving the activity of transition metal sites with active ligands beyond the incorporation of metal cations to form double-layered hydroxides.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.1c13609.

  • Details of catalysts preparation; DFT calculation methods; coordination stability of M–bpy complexes; 1H NMR spectra of Ni–bpy; jV curve of bare FTO; in situ deposition of (bpy)zNiOxHy; coordination of bpy toward NiOxHy; mass loading of active Ni sites; charge transfer, Faradaic efficiency, FTIR spectra, and stability of (bpy)zNiOxHy; additional DFT calculation; comparison of OER performance of nickel-based electrocatalysts (PDF)

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