Electrochemical characterization of evolving ionomer/electrocatalyst interactions throughout accelerated stress tests

Hu, Leiming; Van Cleve, Tim; Yu, Haoran; Park, Jae Hyung; Kariuki, Nancy; Kropf, A. Jeremy; Mukundan, Rangachary; Cullen, David A.; Myers, Deborah J.; Neyerlin, K. C.

doi:10.1016/j.jpowsour.2022.232490

Electrochemical characterization of evolving ionomer/electrocatalyst interactions throughout accelerated stress tests

Journal Article · Fri Dec 16 23:00:00 EST 2022 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2022.232490· OSTI ID:1908593

; Van Cleve, Tim; Yu, Haoran; Park, Jae Hyung; Kariuki, Nancy; Kropf, A. Jeremy; Mukundan, Rangachary; Cullen, David A.; Myers, Deborah J.;

Here, the degradation of polymer electrolyte membrane fuel cells (PEMFCs) catalyst layers used for heavy-duty vehicles was examined using a catalyst-specific accelerated stress test (AST). High surface area carbon supported dispersed Pt (Pt/HSC), annealed Pt (a-Pt/HSC) and PtCo (PtCo/HSC) alloy catalysts were examined over the course of 90,000 cycles by measuring changes in mass activity, O₂ transport resistance, electrochemical active surface area (ECSA), catalyst accessibility and ionomer-electrocatalyst interactions. Compared to a-Pt/HSC and Pt/HSC catalyst, the PtCo/HSC showed better initial mass activity, a larger initial mass transport loss, and faster degradation after the first 30k AST cycles, as a large portion of Co leached out during potential cycling. Pt/HSC showed higher initial performance relative to a-Pt/HSC but had faster degradation. STEM characterizations show that the ECSA losses are largely related to Pt dissolution resulting in either catalyst particle growth via the Ostwald ripening mechanism or redeposition in the membrane. Catalyst accessibility measurements showed decreased RH sensitivity for all three samples, while CO impedance measurements revealed a decrease in both Pt-water and carbon-water interactions. This implies that, Pt is either preferentially redepositing on the exterior of the carbon support, or that the ionomer is undergoing morphological changes enabling the enhanced intrusion of mesopores.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office; USDOE Office of Nuclear Energy (NE), Nuclear Fuel Cycle and Supply Chain. Fuel Cycle Research and Development Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

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

OSTI ID:: 1908593

Alternate ID(s):: OSTI ID: 2310266
OSTI ID: 1909088

Report Number(s):: NREL/JA--5900-84944; MainId:85717; UUID:192f4ccd-bc2e-47bb-abbb-25a65b8b1188; MainAdminId:68406

Journal Information:: Journal of Power Sources, Journal Name: Journal of Power Sources Vol. 556; ISSN 0378-7753

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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25 ENERGY STORAGE
30 DIRECT ENERGY CONVERSION
accelerated stress test
catalyst layers
heavy-duty vehicles
polymer electrolyte membrane fuel cells

Electrochemical characterization of evolving ionomer/electrocatalyst interactions throughout accelerated stress tests

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