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Outstanding Oxygen Reduction Reaction Catalytic Performance of In–PtNi Octahedral Nanoparticles Designed via Computational Dopant Screening

  • Jeonghoon Lim
    Jeonghoon Lim
    Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
  • Kihyun Shin
    Kihyun Shin
    Department of Chemistry and the Oden Institute for Computational Engineering and Science, The University of Texas at Austin, Austin, Texas 78712-1224, United States
    More by Kihyun Shin
  • Junu Bak
    Junu Bak
    Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    More by Junu Bak
  • JeongHan Roh
    JeongHan Roh
    Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    More by JeongHan Roh
  • SangJae Lee
    SangJae Lee
    Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    More by SangJae Lee
  • Graeme Henkelman*
    Graeme Henkelman
    Department of Chemistry and the Oden Institute for Computational Engineering and Science, The University of Texas at Austin, Austin, Texas 78712-1224, United States
    *Email: [email protected]
  • , and 
  • EunAe Cho*
    EunAe Cho
    Department of Materials Science and Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea
    *Email: [email protected]
    More by EunAe Cho
Cite this: Chem. Mater. 2021, 33, 22, 8895–8903
Publication Date (Web):November 1, 2021
https://doi.org/10.1021/acs.chemmater.1c03196
Copyright © 2021 American Chemical Society

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    Abstract

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    PtNi octahedral nanoparticles are considered as one of the best-performing catalysts for the oxygen reduction reaction (ORR). However, Ni dissolution deteriorates their catalytic activity and stability during the ORR. Here, we report a strategy that improves the ORR activity and stability of the PtNi octahedral nanoparticle catalyst through the incorporation of a novel dopant. Computational screening with seven different elements (Bi, In, Ru, Sn, Te, Zn, and Zr) suggests In as the most promising candidate based on the metal doping energy and the OH* adsorption energy. Consideration of the OH* coverage and Ni diffusion energy demonstrates the superior ORR activity and stability of the In-doped PtNi(111) structure. The calculation results were validated by synthesizing In-doped PtNi octahedral nanoparticles on a carbon support (In–PtNi/C). In–PtNi/C demonstrated excellent ORR performance outcomes (1.36 A mgPt–1 and 2.64 mA cm–2@0.9 VRHE), which were 2.1 and 7.9 times higher in terms of the mass activity and 2.4 and 13.4 times higher in terms of the specific activity compared to PtNi/C and Pt/C, respectively. After 12k potential cycles, In–PtNi/C showed excellent stability with high Ni retention; 2.4 and 43% of Ni were lost from In–PtNi/C and PtNi/C, respectively. Computational and experimental investigation demonstrates that surface-doped In creates a new active site toward the ORR and blocks Ni diffusion to the surface by making Pt less oxophilic.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.chemmater.1c03196.

    • Detailed experimental and computational procedures, more characterization and electrochemical details including DFT calculations, XRD, ICP–OES, TEM, EDS mapping, and additional ORR performance outcomes (PDF)

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    Cited By

    This article is cited by 8 publications.

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    4. Jinmei Li, Yumao Kang, Ziqiang Lei, Peng Liu. Well-controlled 3D flower-like CoP3/CeO2/C heterostructures as bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries. Applied Catalysis B: Environmental 2023, 321 , 122029. https://doi.org/10.1016/j.apcatb.2022.122029
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    6. L. Payattikul, L. Intakhuen, T. Kiatsiriroat, K. Punyawudho. The effect of supporting carbons on the gas phase synthesis of octahedral Pt3Ni electrocatalysts with various H2:CO ratios. Scientific Reports 2022, 12 (1) https://doi.org/10.1038/s41598-022-16742-x
    7. Chia‐Jui Hsieh, Yi‐Hong Liu, Chi‐Yen Tsao, Jui‐Tai Lin, Chong‐Chi Chi, Chun‐Wei Chang, Yueh‐Chun Hsiao, Cheng‐Yu Wu, Tung‐Han Yang. Bromide‐Mediated Reduction Kinetics and Oxidative Etching for Manipulating the Twin Structure and Facet of Pd Nanocrystals for Catalysis. Advanced Materials Interfaces 2022, 9 (26) , 2201036. https://doi.org/10.1002/admi.202201036
    8. Jeonghoon Lim, Chanwon Jung, Doosun Hong, Junu Bak, Jaewook Shin, MinJoong Kim, DongHoon Song, Changsoo Lee, Jinkyu Lim, Hyunjoo Lee, Hyuck Mo Lee, EunAe Cho. Atomically ordered Pt 3 Mn intermetallic electrocatalysts for the oxygen reduction reaction in fuel cells. Journal of Materials Chemistry A 2022, 10 (13) , 7399-7408. https://doi.org/10.1039/D2TA00127F

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