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    Rational Molecular Design of Electrocatalysts Based on Single-Atom Modified Covalent Organic Frameworks for Efficient Oxygen Reduction Reaction
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    • Kazuyuki Iwase
      Kazuyuki Iwase
      Department of Applied Chemistry, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
      Research Center for Solar Energy Chemistry, Osaka University, 1-3 Machikane-yama, Toyonaka, Osaka 560-8531, Japan
      More by Kazuyuki Iwase
      Orcidhttp://orcid.org/0000-0002-5196-741X
    • Shuji Nakanishi
      Shuji Nakanishi
      Research Center for Solar Energy Chemistry, Osaka University, 1-3 Machikane-yama, Toyonaka, Osaka 560-8531, Japan
      Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
      More by Shuji Nakanishi
      Orcidhttp://orcid.org/0000-0002-3313-2689
    • Masaru Miyayama
      Masaru Miyayama
      Department of Applied Chemistry, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
      More by Masaru Miyayama
    • Kazuhide Kamiya*
      Kazuhide Kamiya
      Research Center for Solar Energy Chemistry, Osaka University, 1-3 Machikane-yama, Toyonaka, Osaka 560-8531, Japan
      Graduate School of Engineering Science, Osaka University, 1-3 Machikaneyama, Toyonaka, Osaka 560-8531, Japan
      Japan Science and Technology Agency (JST) PRESTO, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan
      *(K.K.) E-mail [email protected]
      More by Kazuhide Kamiya
      Orcidhttp://orcid.org/0000-0002-6018-9277
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    ACS Applied Energy Materials

    Cite this: ACS Appl. Energy Mater. 2020, 3, 2, 1644–1652
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    https://doi.org/10.1021/acsaem.9b02141
    Published January 13, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    The development of oxygen reduction reaction (ORR) electrocatalysts comprising abundant elements is highly desirable for achieving widespread use of fuel cells. Optimal ORR catalysts should have moderate binding strength (ΔEads) with O2-derived intermediates, where the metal species and its coordination numbers are the essential determining factors for ΔEads. However, in conventional non-noble-metal-based ORR catalysts, such as metal–nitrogen-doped carbons, the metal species and its coordination structure cannot freely be chosen. In contrast, covalent organic frameworks (COFs), which are cross-linked microporous polymers, have high design flexibility; as such, they can be purposefully designed by using a wide range of monomers. The present work investigated the adsorption strength of ORR intermediates on single 3d metal atoms (Mn, Fe, Co, Ni, and Cu) doped in COFs with different coordination structures using first-principles calculations toward the development of efficient non-noble-metal ORR catalysts. The adsorption strength of the intermediates was found to monotonically increase as either the number of d-electrons or coordination number of metal centers decreased, and a volcano-type relationship was observed between the adsorption energies of the intermediates and the theoretical ORR activities. Therefore, to develop efficient non-noble-metal-based ORR electrocatalysts, the adsorption strength should be tuned close to the volcano peak by an appropriate choice of metal species and/or coordination number as the control parameters. Considering the high designability of metal species and of its coordination numbers in COFs, COFs are expected to become the next-generation platform of supports of single-atom catalysts using the design direction provided by the present work.

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    • Model structures of graphitic materials with metal centers coordinated by four nitrogen atoms constructed by following previous reports, adsorption energies of their ORR intermediates, and their volcano plots; calculated values and experimental parameters in this study; stabilization energies of metal atoms in M–COFs; ΔEO using the GGA + U method; PDOS of M–COFs; free energy diagrams of all of the metal-modified COFs in this study; free energy diagrams with O2 molecule adsorption and H2O2 formation steps for the analyses of the ORR reaction path of M–COFs; potential plots for the limiting steps of ORR against ΔEO; collected data of solvation energies of ORR intermediates for molecular catalysts used in previous studies; replot of potential plots for the limiting steps of the ORR against the ΔEads values with error bars for Cu–N3, Co–N4, and Fe–N4 (PDF)

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    Cite this: ACS Appl. Energy Mater. 2020, 3, 2, 1644–1652
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsaem.9b02141
    Published January 13, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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