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One-Step Facile Synthesis of High-Activity Nitrogen-Doped PtNiN Oxygen Reduction Catalyst

  • Liang Song
    Liang Song
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11790, United States
    More by Liang Song
  • Yun Cai
    Yun Cai
    Global Fuel Cell Business, General Motors, Pontiac, Michigan 48340, United States
    More by Yun Cai
  • Yang Liu
    Yang Liu
    Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11790, United States
    More by Yang Liu
  • Xueru Zhao
    Xueru Zhao
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    More by Xueru Zhao
  • Kurian A. Kuttiyiel
    Kurian A. Kuttiyiel
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
  • Nebojsa Marinkovic
    Nebojsa Marinkovic
    Synchrotron Catalysis Consortium and Department of Chemical Engineering, Columbia University, New York, New York 10027, United States
  • Anatoly I. Frenkel
    Anatoly I. Frenkel
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, New York 11790, United States
  • Anusorn Kongkanand
    Anusorn Kongkanand
    Global Fuel Cell Business, General Motors, Pontiac, Michigan 48340, United States
  • YongMan Choi
    YongMan Choi
    College of Photonics, National Yang Ming Chiao Tung University, Tainan 71150, Taiwan
    More by YongMan Choi
  • Radoslav R. Adzic
    Radoslav R. Adzic
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
  • , and 
  • Kotaro Sasaki*
    Kotaro Sasaki
    Chemistry Division, Brookhaven National Laboratory, Upton, New York 11973, United States
    *Email: [email protected]
Cite this: ACS Appl. Energy Mater. 2022, 5, 4, 5245–5255
Publication Date (Web):April 14, 2022
https://doi.org/10.1021/acsaem.2c00631
Copyright © 2022 American Chemical Society

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    Abstract

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    PtM alloy electrocatalysts (M = Fe, Co, Ni) have been the subject of many investigations aimed at increasing their attractive properties, in particular their oxygen reduction reaction (ORR) activity, while reducing total platinum-group-metal content and improving durability. Despite some success, these catalysts still have relatively high Pt content and lack the necessary durability, as M metals leach out from the alloys during potential cycling. Previously, we synthesized nitrogen (N)-doped PtMN/C catalysts consisting of thin Pt shells on M nitride cores by a two-step method, which showed higher ORR activity and stability than their PtM counterparts. In the present study, we developed a facile one-step synthesis method, which comprises a single thermal annealing process of the N-doped PtNiN/C alloy. The ORR performance of the one-step-synthesized PtNiN/C catalyst is much higher than that of the two-step-synthesized PtNiN/C, as revealed by rotating disk electrode measurements. Membrane electrode assembly fuel cell testing demonstrated superb durability and high activity. Formation of Pt monolayer shells on the nitrided (PtxNi1–x)4N cores was confirmed by in situ X-ray absorption spectroscopy. The origins of the enhanced activity and stability of the one-step-synthesized PtNiN/C catalyst are elucidated based on density functional theory calculations together with the experimental results.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsaem.2c00631.

    • TEM-EDS analysis, fcc structure models, CV curves and ECSA in MEA testing, voltage losses in MEA testing, procedures of DFT calculations, table of MEA performance in literature, table of experimental and theoretical bond distances, and table of the number of atoms used for the DFT models (PDF)

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    Cited By

    This article is cited by 3 publications.

    1. Chenzhao Li, Liang Song, Xueru Zhao, Kotaro Sasaki, Jian Xie. Nitrogen-Doped PtNi Catalysts on Polybenzimidazole-Functionalized Carbon Support for the Oxygen Reduction Reaction in Polymer Electrolyte Membrane Fuel Cells. ACS Applied Materials & Interfaces 2022, 14 (23) , 26814-26823. https://doi.org/10.1021/acsami.2c05717
    2. Chenzhao Li, Limin Zhu, Liang Song, Guangqi Zhu, Qi Zhang, Yuyue Zhao, Qing Gong, Chengjun Sun, Yuzi Liu, Kotaro Sasaki, Jian Xie. Synergistic effect of polyaniline on stabilizing Pt nanoparticles in PEMFCs. Journal of Materials Chemistry A 2023, 6 https://doi.org/10.1039/D2TA08135K
    3. Tina Đukić, Luka Pavko, Primož Jovanovič, Nik Maselj, Matija Gatalo, Nejc Hodnik. Stability challenges of carbon-supported Pt-nanoalloys as fuel cell oxygen reduction reaction electrocatalysts. Chemical Communications 2022, 58 (100) , 13832-13854. https://doi.org/10.1039/D2CC05377B

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