Recreating Fuel Cell Catalyst Degradation in Aqueous Environments for Identical-Location Scanning Transmission Electron Microscopy Studies

Yu, Haoran; Zachman, Michael J.; Li, Chenzhao; Hu, Leiming; Kariuki, Nancy N.; Mukundan, Rangachary; Xie, Jian; Neyerlin, Kenneth C.; Myers, Deborah J.; Cullen, David A.

doi:10.1021/acsami.1c23281

Title: Recreating Fuel Cell Catalyst Degradation in Aqueous Environments for Identical-Location Scanning Transmission Electron Microscopy Studies

Journal Article · 28 February 2022 · ACS Applied Materials and Interfaces

DOI: https://doi.org/10.1021/acsami.1c23281 · OSTI ID:1855585

Yu, Haoran ^[1];

^[1]; Li, Chenzhao ^[2];

^[3]; Kariuki, Nancy N. ^[4]; Mukundan, Rangachary ^[5];

^[2];

^[3];

^[4];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Indiana Univ.-Purdue Univ. Indianapolis (IUPUI), Indianapolis, IN (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemistry and Nanoscience Center
Argonne National Lab. (ANL), Argonne, IL (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

The recent surge in interest of proton exchange membrane fuel cells (PEMFCs) for heavy-duty vehicles increases the demand on the durability of oxygen reduction reaction electrocatalysts used in the fuel cell cathode. This prioritizes efforts aimed at understanding and subsequently controlling catalyst degradation. Identical-location scanning transmission electron microscopy (IL-STEM) is a powerful method that enables precise characterization of degradation processes in individual catalyst nanoparticles across various stages of cycling. Recreating the degradation processes that occur in PEMFC membrane electrode assemblies (MEAs) within the aqueous cell used for IL-STEM experiments is vital for generating an accurate understanding of these processes. In this work, we investigate the type and degree of catalyst degradation achieved by cycling in an aqueous cell compared to a PEMFC MEA. While significant degradation is observed in IL-STEM experiments performed on a traditional Pt catalyst using the standard accelerated stress test potential window (0.6-0.95 VRHE), degradation of a PtCo catalyst designed for heavy-duty vehicle use is very limited compared to that observed in MEAs. We therefore explore various experimental parameters such as temperature, acid type, acid concentration, ionomer content, and potential window to identify conditions that reproduce the degradation observed in MEAs. We find that by extending the cycling potential window to 0.4-1.0 V_RHE in an electrolyte containing Pt ions, the degraded particle size distribution and alloy composition better match that observed in MEAs. In particular, these conditions increase the relative contribution of Ostwald ripening, which appears to play a more significant role in the degradation of larger alloy particles supported on high-surface-area carbons than coalescence. Results from this work highlight the potential for discrepancies between ex situ aqueous experiments and MEA tests. While different catalysts may require a unique modification to the AST protocol, strategies provided in this work enable future in situ and identical-location experiments that will play an important role in the development of robust catalysts for heavy-duty vehicle applications.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); National Renewable Energy Laboratory (NREL), Golden, CO (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Hydrogen and Fuel Cell Technologies Office; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office

Grant/Contract Number:: 89233218CNA000001; AC02-06CH11357; AC05-00OR22725; AC36-08GO28308

OSTI ID:: 1855585

Report Number(s):: LA-UR-22-22491; NREL/JA-5900-81610; MainId:82383; UUID:ff2e650e-bc8f-483f-a228-a22dca8be993; MainAdminID:64059

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 18 Vol. 14; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Recreating Fuel Cell Catalyst Degradation in Aqueous Environments for Identical-Location Scanning Transmission Electron Microscopy Studies

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