4.8 Article

Mitigating Pt Loss in Polymer Electrolyte Membrane Fuel Cell Cathode Catalysts Using Graphene Nanoplatelet Pickering Emulsion Processing

Journal

ADVANCED FUNCTIONAL MATERIALS
Volume 32, Issue 43, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.202205216

Keywords

accelerated stability tests; electrochemical surface area; membrane electrode assemblies; proton exchange membrane fuel cells; rotating disc electrodes

Funding

  1. Robert Bosch LLC
  2. National Research Foundation of Korea (NRF) - Ministry of Education [2020R1A6A3A03038630]
  3. National Science Foundation Scalable Nanomanufacturing Program [NSF CMMI-1727846, NSF CMMI-2039268]
  4. National Science Foundation Future Manufacturing Research Grant Program [NSF CMMI-2037026]
  5. Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF ECCS-1542205]
  6. Materials Research Science and Engineering Center [NSF DMR-1720139]
  7. State of Illinois
  8. Northwestern University
  9. Department of Defense (DoD) through the National Defense Science and Engineering Graduate (NDSEG) Fellowship Program
  10. National Research Foundation of Korea [2020R1A6A3A03038630] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)

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Carbon-supported Pt nanoparticles for cathode oxygen reduction reaction (ORR) in fuel cells suffer from poor durability. This study introduces a pickering emulsion-processing strategy using graphene nanoplatelet dispersions stabilized by ethyl cellulose to mitigate Pt loss. The resulting graphene-Pt/C catalysts demonstrate superior durability and ECSA retention compared to a commercial Pt/C catalyst. The success is attributed to the localization of Pt nanoparticles on graphene defects, which suppresses dissolution and agglomeration without hindering reactant accessibility.
Carbon-supported Pt nanoparticles are the leading catalysts for the cathode oxygen reduction reaction (ORR) in polymer electrolyte membrane fuel cells. However, these ORR catalysts suffer from poor electrochemical durability, particularly the loss of electrochemical surface area (ECSA) due to Pt nanoparticle dissolution and agglomeration. Here, Pt loss is mitigated through a Pickering emulsion-processing strategy that employs graphene nanoplatelet dispersions stabilized by the polymer ethyl cellulose. The resulting graphene-Pt/Vulcan carbon (Pt/C) catalysts exhibit superior durability and ECSA retention throughout an accelerated stress test compared with a commercial Pt/C standard catalyst, both in a diagnostic-rotating disc electrode setup and in a membrane electrode assembly full cell. These graphene-Pt/C catalysts also improve durability at high-voltage conditions, providing further evidence of their exceptional electrochemical stability. Consistent with density functional theory calculations, postelectrochemical characterization reveals that Pt nanoparticles localize at graphene defects both on the basal plane and especially at the edges of the graphene nanoplatelets. Since this Pt nanoparticle localization suppresses Pt nanoparticle dissolution and agglomeration without hindering accessibility of the reactant species to the catalyst surface, the ORR performance under both idealized and practical experimental conditions shows significantly improved durability while maintaining high electrochemical activity.

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