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Synergistic interactions between PtRu catalyst and nitrogen-doped carbon support boost hydrogen oxidation

Nature Catalysis volume 6, pages 773–783 (2023)Cite this article

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Abstract

Hydroxide exchange membrane fuel cell (HEMFC) is a potentially cost-effective energy conversion technology. However, current state-of-the-art HEMFCs require a high loading of platinum-group-metal (PGM) catalysts, especially for the hydrogen oxidation reaction. Here we develop a porous nitrogen-doped carbon-suppported PtRu hydrogen oxidation reaction catalyst (PtRu/pN-C) that has a high intrinsic and mass activity in alkaline condition. Spectroscopic and microscopic data indicate the presence of Pt single atoms in addition to PtRu nanoparticles on pN-C. Mechanistic study suggests Ru modulates the electronic structure of Pt for an optimized hydrogen binding energy, while Pt single atoms on pN-C optimize the interfacial water structure. These synergetic interactions are responsible for the high catalytic activity of this catalyst. An HEMFC with a low loading of this catalyst and a commercial Fe–N–C oxygen reduction reaction catalyst achieves a high PGM utilization rate. The current density at 0.65 V of this HEMFC reaches 1.5 A cm−2, exceeding the US Department of Energy 2022 target (1 A cm−2) by 50%.

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Fig. 1: Catalyst synthesis and characterization.
Fig. 2: X-ray spectroscopic characterization.
Fig. 3: Mechanistic study.
Fig. 4: Electrochemical test for optimized PtRu/pN-C catalyst.

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Data availability

All data are available in the article and its Supplementary Information. The source data were deposited in the Zenodo repository (https://zenodo.org/record/8114588)53. Source data are provided with this paper.

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Acknowledgements

W.N., J.L.M., M.C., L.B., S.L., W.C.M. and X.H. acknowledge the financial support of EPFL. W.E.M. and N.U.H. gratefully acknowledge the financial support of the US DOE Office of Energy Efficiency and Renewable Energy under the Hydrogen and Fuel Cells Technologies Office (HFTO) (award number DE-EE0008433) to perform the AEMFC experiments. Y.-C.C. and H.M.C. acknowledge the Ministry of Science and Technology, Taiwan (contract no. MOST 110-2628-M-002-001-RSP); S.S., S.J. and J.S.L. were supported by the Swiss National Science Foundation Grant 200021_182605 as well as the European Union’s Horizon 2020 Research and innovation programme (starting grant CATACOAT, no. 758653). We acknowledge the help of B. Victor from CIME, EPFL, for conducting aberration-corrected HAADF-STEM and corresponding analysis.

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Authors and Affiliations

  1. Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland

    Weiyan Ni, Josephine Lederballe Meibom, Miyeon Chang, Yiwei Zheng, Lichen Bai, Wenchao Ma, Seunghwa Lee & Xile Hu

  2. Department of Chemical Engineering, University of South Carolina, Columbia, SC, USA

    Noor Ul Hassan & William E. Mustain

  3. Department of Chemistry, National Taiwan University, Taipei, Taiwan

    You-Chiuan Chu & Hao Ming Chen

  4. Solar Energy and Building Physics Laboratory, Institute of Civil Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland

    Anna Krammer & Andreas Schüler

  5. Laboratory of Sustainable and Catalytic Processing, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), Lausanne, Switzerland

    Songlan Sun, Seongmin Jin & Jeremy S. Luterbacher

  6. Department of Chemical Engineering, Changwon National University, Changwon, South Korea

    Seunghwa Lee

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Contributions

W.N. designed and synthesized the catalysts and performed the majority of electrochemical tests, characterization and analysis; J.L.M. contributed to the synthesis of catalysts and electrochemical measurements; N.U.H. and Y.Z. assembled the MEA and performed the fuel cell performance; W.N., M.C. and S.L. conducted the in situ SEIRAS experiments; Y.-C.C. conducted XAS measurement under the supervision of H.M.C.; S.S. and S.J. performed the chemisorption experiments under the supervision of J.S.L.; A.K. performed the XPS measurements under the supervision of A.S.; L.B. performed the aberration-corrected HAADF-STEM; W.M. contributed to TEM and SEM measurements. W.N. and X.H. wrote the paper, with input from all the other co-authors. W.E.M. and X.H. directed the research.

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Correspondence to William E. Mustain or Xile Hu.

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Ni, W., Meibom, J.L., Hassan, N.U. et al. Synergistic interactions between PtRu catalyst and nitrogen-doped carbon support boost hydrogen oxidation. Nat Catal 6, 773–783 (2023). https://doi.org/10.1038/s41929-023-01007-1

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