3D Analysis of Fuel Cell Electrocatalyst Degradation on Alternate Carbon Supports

Sneed, Brian T.; Cullen, David A.; Reeves, Kimberly S.; Dyck, Ondrej E.; Langlois, David Alan; Mukundan, Rangachary; Borup, Rodney L.; More, Karren L.

doi:10.1021/acsami.7b09716

Title: 3D Analysis of Fuel Cell Electrocatalyst Degradation on Alternate Carbon Supports

Journal Article · Tue Aug 15 00:00:00 EDT 2017 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.7b09716· OSTI ID:1414157

^[1];

^[1]; Reeves, Kimberly S. ^[1]; Dyck, Ondrej E. ^[1]; Langlois, David Alan ^[2];

^[2];

^[2]; More, Karren L. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Understanding the mechanisms associated with Pt/C electrocatalyst degradation in proton exchange membrane fuel cell (PEMFC) cathodes is critical for the future development of higher-performing materials; however, there is a lack of information regarding Pt coarsening under PEMFC operating conditions within the cathode catalyst layer. We report a direct and quantitative 3D study of Pt dispersions on carbon supports (high surface area carbon (HSAC), Vulcan XC-72, and graphitized carbon) with varied surface areas, graphitic character, and Pt loadings ranging from 5 to 40 wt %. This is accomplished both before and after catalyst-cycling accelerated stress tests (ASTs) through observations of the cathode catalyst layer of membrane electrode assemblies. Electron tomography results show Pt nanoparticle agglomeration occurs predominantly at junctions and edges of aggregated graphitized carbon particles, leading to poor Pt dispersion in the as-prepared catalysts and increased coalescence during ASTs. Tomographic reconstructions of Pt/HSAC show much better initial Pt dispersions, less agglomeration, and less coarsening during ASTs in the cathode. However, a large loss of the electrochemically active surface area (ECSA) is still observed and is attributed to accelerated Pt dissolution and nanoparticle coalescence. Moreover, a strong correlation between Pt particle/agglomerate size and measured ECSA is established and is proposed as a more useful metric than average crystallite size in predicting degradation behavior across different catalyst systems.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

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

Grant/Contract Number:: AC52-06NA25396; AC05-00OR22725

OSTI ID:: 1414157

Alternate ID(s):: OSTI ID: 1414700

Report Number(s):: LA-UR-17-27245; TRN: US1800678

Journal Information:: ACS Applied Materials and Interfaces, Vol. 9, Issue 35; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 58 works

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