Impact of Catalyst Ink Dispersing Methodology on Fuel Cell Performance Using in-Situ X-ray Scattering
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This work presents a study of the effects of ultrasonic dispersing methodology and time on catalyst agglomerate size in polymer electrolyte membrane fuel cell (PEMFC) catalyst ink dispersions. Cathode catalyst inks were prepared and characterized to elucidate the influences of ultrasonic dispersing method and time on catalyst ink particle size and CCL electrochemical properties. In-situ ultra-small-, small-, and wide-angle X-ray scattering (USAXS–SAXS–WAXS) analyses were used to study the impact of ultrasonication time and methodology on changes in the agglomerate, aggregate, and particle size and distribution during the dispersing process. Ex-situ transmission electron microscopy was also used to investigate the particle size of these inks. Fuel cell membrane electrode assemblies (MEAs) were prepared and tested to determine the influence of ink properties on CCL electrochemical properties, including the electrochemical active surface area (ECA), mass activity (MA), H 2 /air polarization curves, and oxygen mass-transport resistances. It was found that a combination of brief tip sonication followed by bath sonication was most effective at breaking up agglomerates, leading to maximum catalyst activity and MEA performance. Extended tip sonication was found to be too aggressive and resulted in detachment of the platinum nanoparticles from the carbon black support, which decreased electrochemical surface area and MEA performance. Quantification of oxygen mass transport resistance showed that electrodes with large catalyst agglomerates due to insufficient sonication had a higher non-Fickian (pressure independent) than properly dispersed catalyst. Through correlation of the performance with catalyst particle size, the desired CCL structure was proposed, which will provide insight into dispersion strategies for lab-scale spray coating and other processing techniques as well as for large-scale manufacturing.
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Appropriate dispersion process breaks up large agglomerates, reduces agglomerate size, improves dispersion of catalyst and ionomer, maximizing TPB, avoiding cracks, improving pore volume and mass transport.
“Appropriate dispersion process could effectively break up the large agglomerates, reduce the size of agglomerates, and improve the dispersion of catalyst and ionomer in solvent, which will maximize TPB, avoid the formation of cracks, as well as improve the pore volume of CL and thus the mass transport [24,156] (Figure 9b,e).”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [156]
The Results and Discussion section reports that appropriate sonication breaks large agglomerates into smaller aggregates, distributes ionomer more uniformly, improves catalyst utilization, and lowers gas-transport resistance. It also links insufficient dispersion to fewer three-phase boundaries. Our copy does not establish that the process avoids cracks or improves catalyst-layer pore volume; it instead describes fewer secondary pores with appropriate dispersion. Page numbers were not available in the indexed passages. (LLM, conf=0.87)
Experimental — accuracy not yet measuredPt inside large agglomerates cannot access ionomer, increasing proton transport resistance.
“Therefore, the Pt inside the large agglomerates cannot access ionomer, increasing the proton transport resistance [156].”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [156]
Results and Discussion states that ionomer coats only the exterior of highly agglomerated particles, leaving interior Pt inaccessible to protons. It links this to lower mass activity, but the increased transport resistance it reports is for oxygen, not protons. The Conclusion likewise describes limited ionomer access and poor performance without reporting increased proton transport resistance; page numbers are unavailable in our copy. (LLM, conf=0.88)
Experimental — accuracy not yet measuredLong gas transport distance in interior of large agglomerates adversely affects gas and water transport.
“Further, the long gas transport distance in the interior of the large agglomerates also has an adverse effect on the gas and water transport [156].”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [156]
The Results and Discussion state that larger agglomerates create higher resistance to oxygen diffusing to Pt particles at their centers, supporting the gas-transport part. The same section says liquid-water resistance could be neglected under the study’s slightly dry conditions; it does not establish an adverse effect on water transport. (LLM, conf=0.88)
Experimental — accuracy not yet measuredIonomer molecules mainly adsorb on exterior surface of catalyst agglomerates and barely penetrate, especially large agglomerates.
“Ionomer molecules mainly adsorb on the exterior surface of the catalyst agglomerates and barely penetrate the catalyst agglomerates, especially the large catalyst agglomerates [156].”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [156]
Low exterior-surface-to-volume ratio causes thick ionomer film outside large catalyst agglomerates, increasing gas transport resistance through ionomer film.
“Due to the low exterior-surface-to-volume ratio, a thick ionomer film may be formed outside the large catalyst agglomerates, increasing the gas transport resistance through the ionomer film [156].”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [156]
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- Authors
- Wang, M., Park, J. H., Kabir, S., Neyerlin, K. C., Kariuki, N. N., Lv, H., Stamenkovic, V. R., Myers, D. J., Ulsh, M., & Mauger, S. A.
- Affiliations
- National Laboratory of the Rockies (US)
- Argonne National Laboratory (US)
- Corresponding author
- Mauger, Scott A.
- ORCID
- Venue
- ACS Applied Energy Materials
- Publisher
- American Chemical Society (ACS)
- Published
- 2019-07-26
- Volume
- 2
- Issue
- 9
- Pages
- 6417-6427
- ISSN
- 2574-0962 (ISSN-L)
- OpenAlex
- W2965879713
- Cited by
- 192
- References
- 40
- Citations by year
- 2026: 20 · 2025: 36 · 2024: 33 · 2023: 22 · 2022: 24 · 2021: 34 · 2020: 19 · 2019: 4
- FWCI
- 7.28
- Type
- journal article
- Language
- en
- Open access
- green
- www.osti.gov
- Licence
- Locations
- ACS Applied Energy Materials (publishedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- Argonne National Laboratory (DE-AC02 06CH11357, DE-AC36-08GO28308)
- Topics
- Physical Sciences › Engineering › Electrical and Electronic Engineering › Fuel Cells and Related Materials
- Physical Sciences › Energy › Renewable Energy, Sustainability and the Environment › Electrocatalysts for Energy Conversion
- Physical Sciences › Materials Science › Materials Chemistry › Advancements in Solid Oxide Fuel Cells
- Keywords
- sonication, proton exchange membrane fuel cells, cathode catalyst layer, platinum nanoparticles, carbon black support, electrochemically active surface area, non-Fickian diffusion, in situ X-ray scattering, spray coating
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