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Electrochemical Dealloying of Ni-Rich Pt–Ni Nanoparticle Network for Robust Oxygen-Reduction Electrocatalysts

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    Research Article

    Electrochemical Dealloying of Ni-Rich Pt–Ni Nanoparticle Network for Robust Oxygen-Reduction Electrocatalysts
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    ACS Sustainable Chemistry & Engineering

    Cite this: ACS Sustainable Chem. Eng. 2023, 11, 42, 15460–15469
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    https://doi.org/10.1021/acssuschemeng.3c04866
    Published October 11, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    Increasing the electrochemically active surface area (ECSA) and alloying Pt with transition metals (TMs) are well-known strategies for enhancing the oxygen reduction reaction (ORR) catalytic activities. Herein, we introduce a strategy to produce highly active ORR electrocatalysts with a large ECSA using an electrochemical dealloying process involving leaching of Ni from a Ni-rich Pt–Ni nanoparticle network. The dealloying process yielded a dealloyed Pt–Ni nanoparticle network with rugged surfaces from the Ni-rich Pt–Ni nanoparticle network, resulting in a large ECSA. We also increased the mass activity and utilization efficiency of Pt by modulating the interactions between Pt and Ni. The dealloyed nanoparticle network exhibited a high ORR mass activity, six times higher than that of commercial Pt/C. Moreover, the dealloyed Pt–Ni nanoparticle network exhibited better catalytic stability than the Pt/C after 10000 potential cycles, even without carbon support. The reduced binding energy of the O intermediate due to the effects of Ni (ligand and strain effects) enhanced the ORR activity of the dealloyed nanoparticle network, according to the results of a mechanistic study performed using density functional theory. This study opens new avenues for designing TM-alloy catalysts with high ORR activity for various applications.

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acssuschemeng.3c04866.

    • Experimental details; computational details; structural characterization of Pt nanoparticle networks; CO stripping experiments; EDS mapping data before and after ADT; Plot for recently reported ORR electrocatalysts mass activity versus Tafel slope; Atomic concentration ratio of the catalysts measured by ICP-MS and XPS; Summarized electrochemical ORR performance for this work; Summarized DFT calculation data of this work (PDF)

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    Cited By

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    This article is cited by 3 publications.

    1. Jiahui Li, Lingyu Li, Weiguo Lin, Xu Chen, Wensheng Yang. Boosting ORR Activity in π-Rich Carbon-Supported Sub-3 nm Pt-Based Intermetallic Electrocatalysts via d–π Interaction. ACS Sustainable Chemistry & Engineering 2024, 12 (13) , 5241-5250. https://doi.org/10.1021/acssuschemeng.3c08557
    2. Yuwei Li, Huiting Huang, Mingkun Jiang, Wanlong Xi, Junyuan Duan, Marina Ratova, Dan Wu. Advancements in transition bimetal catalysts for electrochemical 5-hydroxymethylfurfural (HMF) oxidation. Journal of Energy Chemistry 2024, 98 , 24-46. https://doi.org/10.1016/j.jechem.2024.06.027
    3. Xinyi Wang, Yanyan Zhou, Caiyun Chang, Yelin Qiao, Yang Jiang, Miao Gao, Li Hou. Optimization and regulation of catalytic activity and stability: Pt–Ni diamond-shaped pearl nanochains with core-shell structure as high-efficient oxygen reduction reaction catalysts. Materials Chemistry and Physics 2024, 316 , 129127. https://doi.org/10.1016/j.matchemphys.2024.129127
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    ACS Sustainable Chemistry & Engineering

    Cite this: ACS Sustainable Chem. Eng. 2023, 11, 42, 15460–15469
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acssuschemeng.3c04866
    Published October 11, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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