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Enhancing the Performance of Shape-Controlled Octahedral Rhodium-Doped PtNi Nanoalloys inside Hydrogen–Air Fuel Cell Cathodes Using a Rational Design of Catalysts, Supports, and Layering
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    Enhancing the Performance of Shape-Controlled Octahedral Rhodium-Doped PtNi Nanoalloys inside Hydrogen–Air Fuel Cell Cathodes Using a Rational Design of Catalysts, Supports, and Layering
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    • Lujin Pan
      Lujin Pan
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
      More by Lujin Pan
    • Alice Parnière
      Alice Parnière
      ICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, France
    • Olivia Dunseath
      Olivia Dunseath
      Johnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United Kingdom
    • Dash Fongalland
      Dash Fongalland
      Johnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United Kingdom
    • Guillermo Nicolau
      Guillermo Nicolau
      Johnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United Kingdom
    • C. Cesar Weber
      C. Cesar Weber
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
    • Jiasheng Lu
      Jiasheng Lu
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
      More by Jiasheng Lu
    • Malte Klingenhof
      Malte Klingenhof
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
    • Aleks Arinchtein
      Aleks Arinchtein
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
    • Hyung-Suk Oh
      Hyung-Suk Oh
      Clean Energy Research Center, Korea Institute of Science and Technology, 02792 Seoul, Republic of Korea
      More by Hyung-Suk Oh
    • Pierre-Yves Blanchard
      Pierre-Yves Blanchard
      ICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, France
    • Sara Cavaliere
      Sara Cavaliere
      ICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, France
      Institut Universitaire de France (IUF), 1 rue Descartes, 75231 Paris cedex 05, France
    • Marc Heggen
      Marc Heggen
      Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
      More by Marc Heggen
    • Rafal E. Dunin-Borkowski
      Rafal E. Dunin-Borkowski
      Ernst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, Germany
    • Alex Martinez Bonastre
      Alex Martinez Bonastre
      Johnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United Kingdom
    • Fabio Dionigi*
      Fabio Dionigi
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
      *Email: [email protected]
    • Jonathan Sharman
      Jonathan Sharman
      Johnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United Kingdom
    • Deborah Jones
      Deborah Jones
      ICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, France
    • Peter Strasser*
      Peter Strasser
      Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, Germany
      *Email: [email protected]
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    ACS Catalysis

    Cite this: ACS Catal. 2024, 14, 1, 10–20
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    https://doi.org/10.1021/acscatal.3c02619
    Published December 8, 2023
    Copyright © 2023 American Chemical Society

    Abstract

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    Octahedral PtNi alloy nanoparticles show a very high catalytic activity for the oxygen reduction reaction. However, their integration into membrane electrode assemblies (MEAs) is challenging, resulting in low fuel cell performance. We report the application of three strategies that are promising to improve the MEA-based fuel cell performance of octahedral PtNi alloy nanoparticles: (1) Rh surface doping to stabilize the morphology, (2) high Pt weight percentage loading on carbon to decrease the catalyst layer thickness (at parity of geometric-area-normalized Pt loading), and (3) N-functionalized carbon supports to more homogeneously distribute the ionomer. The surface chemistry of the Rh dopants is analyzed by in situ X-ray absorption spectroscopy (XAS) under applied potentials in a liquid half-cell. The Rh dopants are present at the catalyst surface with a local coordination to oxygen atoms as in Rh oxide and show potential dependent changes in the oxidation states. A rotating disk electrode (RDE) screening showed advantages in using Ketjen Black EC300J instead of carbon Vulcan XC72R to accommodate high Pt weight percentage loading (∼30 Pt wt %). Finally, a Rh-doped PtNi nanoparticle catalyst was grown on 3% nitrogen-doped Ketjen Black and tested in a MEA-based single cell after being annealed and acid washed. The results showed modest mass activity (MA), 0.35 A mgPt–1 at 0.9 V, but significantly high performance at high current density for octahedral PtNi nanoparticles, 1500 mA cm–2 at 0.6 V, to our knowledge the highest to date for this class of catalysts. Despite this achievement, the full potential of N doping could not be utilized, with samples showing negligible differences with respect to undoped carbon in both high- and low-humidity MEA testing. Even though no enhancement of mass transport at high current density by better distribution of the ionomer on the N-doped carbon was seen in MEA, this could be due to the diffusion of Ni cations, affecting ionomer interaction and overwhelming the effect of nitrogen species on the support.

    Copyright © 2023 American Chemical Society

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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/acscatal.3c02619.

    • Experimental details of materials, sample preparation, and structure characterization details; additional TEM and STEM, elemental mapping images; Pt L3-edge and Ni K-edge XAS, K Space of XAS, EXAFS fitting results; compositional details of the N-doped carbons determined by EA, Pt-based catalysts determined by ICP-OES; details of the operando XANES Rh edge and white line; additional electrochemical activity and stability measurement results; additional XRD patterns; BET surface areas of N-doped KB carbons; additional XPS results of N-doped KB carbons and XPS C peak and N peak fitting results; CO-ECSA in MEA; additional MEA measurements under 30 RH% (PDF)

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    This article is cited by 9 publications.

    1. Shlomi Polani, Raffaele Amitrano, Adrian Felix Baumunk, Lujin Pan, Jiasheng Lu, Nicolai Schmitt, Ulrich Gernert, Malte Klingenhof, Sören Selve, Christian M. Günther, Bastian J. M. Etzold, Peter Strasser. Oxygen Reduction Reaction Activity and Stability of Shaped Metal-Doped PtNi Electrocatalysts Evaluated in Gas Diffusion Electrode Half-Cells. ACS Applied Materials & Interfaces 2024, 16 (39) , 52406-52413. https://doi.org/10.1021/acsami.4c11068
    2. Chao Zhang, Qian Liu, Shujun Ming, Chao Wang, Zhiguo Lv, Tao Zhuang. Integrating Pt single atoms and Mo into PtNi/C through Mo doping-displacement synchronisation strategy for enhanced HER at all pH values. Fuel 2025, 381 , 133356. https://doi.org/10.1016/j.fuel.2024.133356
    3. Lujin Pan, Jiasheng Lu, Olivia Dunseath, Michal Ronovský, An Guo, Malte Klingenhof, Xingli Wang, Elisabeth Hornberger, Alex Martinez Bonastre, Harriet Burdett, Jonathan Sharman, Fabio Dionigi, Peter Strasser. Unveiling the origins of the activity gap between rotating disk electrodes and membrane electrode assemblies: Pt seed-mediated iridium-doped octahedral platinum nickel catalysts for proton exchange membrane fuel cells. EES Catalysis 2025, 3 (1) , 128-139. https://doi.org/10.1039/D4EY00172A
    4. Lulu Jiang, Chao Zhang, Haipeng Wang, Delu Zhang, Yongsheng Gao, Shujun Ming, Tao Zhuang, Zhiguo Lv. Integrated self-assembly core–shell PtNi alloy@Ni(OH)2 film with enhanced alkaline HER. Fuel 2025, 380 , 133088. https://doi.org/10.1016/j.fuel.2024.133088
    5. Xin Zeng, Sushanta K. Mitra, Xianguo Li. One-pot synthesis of supported PtCox bifunctional catalysts for oxygen reduction and hydrogen evolution reactions. International Journal of Hydrogen Energy 2024, 86 , 577-585. https://doi.org/10.1016/j.ijhydene.2024.08.472
    6. Siphelo Ngqoloda, Nyiko Chauke, Thelma Ngwenya, Mpfunzeni Raphulu. Shaped and structured Pt-3d-transition metal alloy nanocrystals as electrocatalysts for the oxygen reduction reaction. Results in Chemistry 2024, 11 , 101831. https://doi.org/10.1016/j.rechem.2024.101831
    7. Chandran Balamurugan, Young Yong Kim, Yong-Ryun Jo, Kyusang Cho, Byoungwook Park, Woochul Kim, Namsoo Lim, Yusin Pak, Hyeonghun Kim, Hyeonryul Lee, Keun Hwa Chae, Ji Hoon Shim, Changhoon Lee, Sooncheol Kwon. In-situ probing polarization-induced stability of single-atom alloy electrocatalysts in metal-air battery via synchrotron-based X-ray diffraction. Applied Catalysis B: Environment and Energy 2024, 353 , 124072. https://doi.org/10.1016/j.apcatb.2024.124072
    8. Yu‐Cheng Hou, Tao Shen, Kan Hu, Xue Wang, Qing‐Na Zheng, Jia‐Bo Le, Jin‐Chao Dong, Jian‐Feng Li. Synergistic Modulation of Multiple Sites Boosts Anti‐Poisoning Hydrogen Electrooxidation Reaction with Ultrasmall (Pt 0.9 Rh 0.1 ) 3 V Ternary Intermetallic Nanoparticles. Angewandte Chemie 2024, 136 (35) https://doi.org/10.1002/ange.202402496
    9. Yu‐Cheng Hou, Tao Shen, Kan Hu, Xue Wang, Qing‐Na Zheng, Jia‐Bo Le, Jin‐Chao Dong, Jian‐Feng Li. Synergistic Modulation of Multiple Sites Boosts Anti‐Poisoning Hydrogen Electrooxidation Reaction with Ultrasmall (Pt 0.9 Rh 0.1 ) 3 V Ternary Intermetallic Nanoparticles. Angewandte Chemie International Edition 2024, 63 (35) https://doi.org/10.1002/anie.202402496

    ACS Catalysis

    Cite this: ACS Catal. 2024, 14, 1, 10–20
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acscatal.3c02619
    Published December 8, 2023
    Copyright © 2023 American Chemical Society

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