PFSA-Ionomer Adsorption to C and Pt/C Particles in Fuel-Cell Inks

Rajupet, Siddharth; Weber, Adam Z.; Radke, Clayton J.

doi:10.1021/acsami.5c00211

PFSA-Ionomer Adsorption to C and Pt/C Particles in Fuel-Cell Inks

Journal Article · Mon Apr 28 00:00:00 EDT 2025 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.5c00211· OSTI ID:2573786

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University of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
University of California, Berkeley, CA (United States)

Catalyst inks used to make fuel-cell electrodes consist of Pt/C catalyst particles and a perfluorosulfonic acid (PFSA) ionomer dispersed in water/alcohol solvent mixtures. PFSA ionomer in the ink adsorbs to the surface of the catalyst particles, dictating the dispersion colloid properties. Following adsorption, the subsequent distribution of excess nonadsorbed ionomer in the ink then governs the final structure of the electrode. Here, we characterize the adsorption of the PFSA ionomer onto Pt/C catalyst particles. PFSA adsorption is largely irreversible. Adsorbed sulfonic-acid moieties impart a negative charge on the catalyst surface, causing electrostatic repulsion between the free ionomer in solution and the ionomer-covered Pt/C particle surface. The amount of adsorption is limited by the resulting electrostatic charge that grows as more ionomer adsorbs, and the catalyst surface becomes more negatively charged. Attenuating electrostatic repulsion by increasing the ink ionic strength promotes ionomer adsorption. Electrostatically limited adsorption is observed, irrespective of the solvent water/n-propanol ratio or the catalyst particle porosity and Pt loading. Experimentally measured ionomer adsorption isotherms are well predicted by a Smoluchowski-based kinetic adsorption model, in which the electrostatic energy barrier for adsorption is predicted from DLVO theory. Furthermore, these findings help to unravel the complex phenomena within these colloidal dispersions, allowing for subsequent tailoring of inks to optimize fuel-cell electrode structure and performance.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2573786

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 18 Vol. 17; ISSN 1944-8244; ISSN 1944-8252

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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