Composition Dependence of the Pore Structure and Water Transport of Composite Catalyst Layers for Polymer Electrolyte Fuel Cells
Open accessAbstract
The material distribution, porous features, and ionomer behavior in the catalyst layer (20wt% platinum on Vulcan carbon impregnated with Nafion) of polymer electrolyte fuel cells were investigated by microscopy, nitrogen adsorption, and water uptake as a function of ionomer loading or relative humidity. As revealed by microscopy, thin ionomer coverage along the carbon surface is observed when ionomer loading is low, while for higher loading, the pore spaces among the carbon agglomerates were mostly flooded. Even at a low ionomer to carbon ratio, the micro-porosity is closed off and the BET surface area decreases by more than 50%. At 100% relative humidity, the water content in the ionomer within the I/C = 0.5 catalyst layer reaches only 4 water molecules per sulfonate, presumably due to the inhibition of swelling by the carbon filler. The resulting structures and properties in the catalyst layer induce a tortuous pathway for water or proton transport in the ionomer phase, particularly at low water content. A distinct feature is observed in the catalyst layers using differential scanning calorimetry (DSC). DSC measurements on the sub-components lead us to conclude that the feature reflects interactions between the ionomer and the carbon or the Pt particles.
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Directly mixing Nafion dispersion solution and Pt/C likely detaches Pt nanoparticles from carbon due to triggered combustion reaction degrading carbon support.
“It has been reported that directly mixing Nafion dispersion solution (the commercial dispersion solution contains the water/1-propanol mixed solvent) and Pt/C likely detaches Pt nanoparticles from carbon due to the triggered combustion reaction that would degrade carbon support [155].”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [155]
The Results and Discussion (page unavailable) report detached Pt particles and say that adding Nafion solution to Pt/C without sufficient water can trigger combustion and damage the carbon support. The claim omits that water condition and presents combustion as the likely cause of detachment, although the paper also names sonication and prolonged stirring as possible causes. The Sample preparation section does not establish that the commercial dispersion itself contains a water/1-propanol solvent mixture. (LLM, conf=0.87)
Experimental — accuracy not yet measuredOrder of ingredients mixing influences size of agglomerates in catalyst ink and material stability through affecting interaction sequence of catalyst, ionomer, and solvent.
“Although only a few studies on the effect of the order of ingredients mixing during the ink preparation process exist, it has an influence on the size of agglomerates in the catalyst ink and the material stability through affecting the interaction sequence of catalyst, ionomer, and solvent [154,155].”
From Effect of Catalyst Ink and Formation Process on the Multiscale Structure of Catalyst Layers in PEM Fuel Cells (2022) · cites this paper as [155]
The Results and Discussion (page unavailable) say that adding Nafion solution to Pt/C without first adding enough water could damage the carbon support, and that detached Pt particles may aggregate in the ink. This supports a possible effect of ingredient-addition sequence on material integrity, but the paper does not show that mixing order changes agglomerate size; its reported cluster-size differences concern Nafion loading in the finished catalyst layer. (LLM, conf=0.86)
Experimental — accuracy not yet measured
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Cites
Sing, K. S. W. (1985) · Pure and Applied Chemistry · doi:10.1351/pac198557040603 · Cited by 24,485 · see citing works
Gasteiger, H. A., Kocha, S. S., Sompalli, B., & Wagner, F. T. (2005) · Applied Catalysis B: Environmental · doi:10.1016/j.apcatb.2004.06.021 · Cited by 4,876 · see citing works
Kreuer, K.-D., Paddison, S. J., Spohr, E., & Schuster, M. (2004) · Chemical Reviews · doi:10.1021/cr020715f · Cited by 2,187 · see citing works
Characterization of porous solids and powders: surface area, pore size, and density
Lowell, S. (2005) · Choice Reviews Online · doi:10.5860/choice.42-5288 · Cited by 1,640 · see citing works
Water Uptake by and Transport Through Nafion® 117 Membranes
Zawodzinski, T. A., Derouin, C., Radzinski, S., Sherman, R. J., Smith, V. T., Springer, T. E., & Gottesfeld, S. (1993) · Journal of The Electrochemical Society · doi:10.1149/1.2056194 · Cited by 1,530 · see citing works
Self-citationAn improved method for the calculation of pore size distribution from adsorption data
Dollimore, D., & Heal, G. R. (1964) · Journal of Applied Chemistry · doi:10.1002/jctb.5010140302 · Cited by 891 · see citing works
Thin-film catalyst layers for polymer electrolyte fuel cell electrodes
Wilson, M. S., & Gottesfeld, S. (1992) · Journal of Applied Electrochemistry · doi:10.1007/bf01093004 · Cited by 870 · see citing works
Parthasarathy, A., Srinivasan, S., Appleby, A. J., & Martin, C. R. (1992) · Journal of The Electrochemical Society · doi:10.1149/1.2221258 · Cited by 689 · see citing works
High Performance Catalyzed Membranes of Ultra‐low Pt Loadings for Polymer Electrolyte Fuel Cells
Wilson, M. S., & Gottesfeld, S. (1992) · Journal of The Electrochemical Society · doi:10.1149/1.2069277 · Cited by 510 · see citing works
Study of the Exchange Current Density for the Hydrogen Oxidation and Evolution Reactions
Neyerlin, K. C., Gu, W., Jorné, J., & Gasteiger, H. A. (2007) · Journal of The Electrochemical Society · doi:10.1149/1.2733987 · Cited by 445 · see citing works
Soboleva, T., Zhao, X., Malek, K., Xie, Z., Navessin, T., & Holdcroft, S. (2010) · ACS Applied Materials & Interfaces · doi:10.1021/am900600y · Cited by 424 · see citing works
Uchida, M., Aoyama, Y., Eda, N., & Ohta, A. (1995) · Journal of The Electrochemical Society · doi:10.1149/1.2048477 · Cited by 408 · see citing works
Core/Shell Pd/FePt Nanoparticles as an Active and Durable Catalyst for the Oxygen Reduction Reaction
Mazumder, V., Chi, M., More, K. L., & Sun, S. (2010) · Journal of the American Chemical Society · doi:10.1021/ja1024436 · Cited by 373 · see citing works
Self-citationBROKA, K., & Ekdunge, P. (1997) · Journal of Applied Electrochemistry · doi:10.1023/a:1018469520562 · Cited by 361 · see citing works
Uchida, M., Fukuoka, Y., Sugawara, Y., Eda, N., & Ohta, A. (1996) · Journal of The Electrochemical Society · doi:10.1149/1.1836988 · Cited by 309 · see citing works
Liu, Y., Murphy, M. W., Baker, D. R., Gu, W., Ji, C., Jorné, J., & Gasteiger, H. A. (2009) · Journal of The Electrochemical Society · doi:10.1149/1.3143965 · Cited by 290 · see citing works
Lefebvre, M. C. (1999) · Electrochemical and Solid-State Letters · doi:10.1149/1.1390804 · Cited by 279 · see citing works
Self-Assembly and Transport Limitations in Confined Nafion Films
Modestino, M. A., Paul, D. K., Dishari, S. K., Petrina, S. A., Allen, F. I., Hickner, M. A., Karan, K., Segalman, R. A., & Weber, A. Z. (2013) · Macromolecules · doi:10.1021/ma301999a · Cited by 233 · see citing works
Cheng, X., Yi, B., Han, M., Zhang, J., Qiao, Y., & Yu, J. (1999) · Journal of Power Sources · doi:10.1016/s0378-7753(99)00046-4 · Cited by 210 · see citing works
Experimental analysis of the reaction layer structure in a gas diffusion electrode
Watanabe, M., Tomikawa, M., & Motoo, S. (1985) · Journal of Electroanalytical Chemistry · doi:10.1016/0022-0728(85)80007-3 · Cited by 182 · see citing works
Depression of proton conductivity in recast Nafion® film measured on flat substrate
Siroma, Z., Kakitsubo, R., Fujiwara, N., Ioroi, T., Yamazaki, S., & Yasuda, K. (2009) · Journal of Power Sources · doi:10.1016/j.jpowsour.2008.12.141 · Cited by 143 · see citing works
Weber, A. Z., & Hickner, M. A. (2008) · Electrochimica Acta · doi:10.1016/j.electacta.2008.05.018 · Cited by 134 · see citing works
Porosimetry of MEAs Made by “Thin Film Decal” Method and Its Effect on Performance of PEFCs
Xie, J., More, K. L., Zawodzinski, T. A., & Smith, W. H. (2004) · Journal of The Electrochemical Society · doi:10.1149/1.1796991 · Cited by 126 · see citing works
Self-citationLiu, Z. Y., Zhang, J. L., Yu, P., et al. (2010) · Journal of The Electrochemical Society · doi:10.1149/1.3391737 · Cited by 112 · see citing works
Effects of MEA fabrication method on durability of polymer electrolyte membrane fuel cells
Prasanna, M. D., Cho, E. A., Lim, T.-H., & Oh, I.-H. (2008) · Electrochimica Acta · doi:10.1016/j.electacta.2008.02.068 · Cited by 107 · see citing works
Liu, Y., Ji, C., Gu, W., Baker, D. R., Jorné, J., & Gasteiger, H. A. (2010) · Journal of The Electrochemical Society · doi:10.1149/1.3435323 · Cited by 86 · see citing works
Ionomer Segregation in Composite MEAs and Its Effect on Polymer Electrolyte Fuel Cell Performance
Xie, J., Garzón, F. H., Zawodzinski, T. A., & Smith, W. H. (2004) · Journal of The Electrochemical Society · doi:10.1149/1.1756887 · Cited by 85 · see citing works
Self-citationSaab, A. P., Garzón, F. H., & Zawodzinski, T. A. (2002) · Journal of The Electrochemical Society · doi:10.1149/1.1516771 · Cited by 85 · see citing works
Self-citationBlom, D. A., Dunlap, J. R., Nolan, T. A., & Allard, L. F. (2003) · Journal of The Electrochemical Society · doi:10.1149/1.1556593 · Cited by 59 · see citing works
Scheiba, F., Benker, N., Kunz, U., Roth, C., & Fueß, H. (2007) · Journal of Power Sources · doi:10.1016/j.jpowsour.2007.11.085 · Cited by 47 · see citing works
Gas diffusion electrodes containing sulfonated poly (arylene ether) ionomer for PEFCs
Yoda, T., Shimura, T., Bae, B., et al. (2009) · Electrochimica Acta · doi:10.1016/j.electacta.2009.02.099 · Cited by 46 · see citing works
Impact of Solvent on Ionomer Structure and Fuel Cell Durability
Johnston, C., Lee, K., Rockward, T., Labouriau, A., Mack, N. H., & Kim, Y. S. (2009) · ECS Transactions · doi:10.1149/1.3210717 · Cited by 27 · see citing works
Hillman, A. R., Dong, Q., Mohamoud, M. A., et al. (2010) · Electrochimica Acta · doi:10.1016/j.electacta.2010.05.024 · Cited by 15 · see citing works
Pt-Co Bimetallic Catalysts for PEM Fuel Cell Cathodes
More, K. L., Reeves, K., & Borup, R. L. (2009) · Microscopy and Microanalysis · doi:10.1017/s1431927609098961 · Cited by 2 · see citing works
Self-citationExploring Water Transport in PEFC Catalyst Layers
Sun, C., & Zawodzinski, T. A. (2012) · ECS Electrochemistry Letters · doi:10.1149/2.010205eel · Cited by 1 · see citing works
Self-citation
Flagged first, then by citations
Research works printed but not linked: 34
- [1]1. T. Yoda, T. Shimura, B. Bae, K. Miyatake, M. Uchida, H. Uchida, and M. Watanabe, Electrochimica Acta, 54, 4328 (2009). Journal of The Electrochemical Society, 160 (9) F1000-F1005 (2013) F1005
- [2]2. K. C. Neyerlin, W. Gu, J. Jorne, and H. A. Gasteiger, Journal of The Electrochemical Society, 154, B631 (2007).
- [3]3. H. Gasteiger, S. Kocha, B. Sompalli, and F. Wagner, Applied Catalysis B: Environ- mental, 56, 9 (2005).
- [4]4. A. Parthasarathy, Journal of The Electrochemical Society, 139, 2530 (1992).
- [5]5. A. P. Saab, F. H. Garzon, and T. A. Zawodzinski, Journal of The Electrochemical Society, 149, A1541 (2002).
- [6]6. M. C. Lefebvre, Electrochemical and Solid-State Letters, 2, 259 (1999).
- [7]7. Y. Liu, M. W. Murphy, D. R. Baker, W. Gu, C. Ji, J. Jorne, and H. A. Gasteiger, Journal of The Electrochemical Society, 156, B970 (2009).
- [8]8. A. Z. Weber and M. A. Hickner, Electrochimica Acta, 53, 7668 (2008).
- [9]9. C.-N. Sun and T. A. Zawodzinski, ECS Electrochemistry Letters, 1, F36 (2012).
- [10]10. M. Watanabe, M. Tomikawa, and S. Motoo, Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, 195, 81 (1985).
- [11]11. M. Uchida, Y. Aoyama, N. Eda, and A. Ohta, Journal of The Electrochemical Society, 142, 4143 (1995).
- [12]12. M. Uchida, Y. Fukuoka, Y. Sugawara, N. Eda, and A. Ohta, Journal of The Electro- chemical Society, 143, 2245 (1996).
- [13]13. J. Xie, F. Garzon, T. A. Zawodzinski, and W. H. Smith, Journal of The Electrochem- ical Society, 151, A1084 (2004).
- [14]14. M. S. Wilson and S. Gottesfeld, Journal of The Electrochemical Society, 139, L28 (1992).
- [15]15. K. More, K. Reeves, and R. Borup, Microscopy and Microanalysis, 15, 146 (2009).
- [16]16. Z. Y. Liu, J. L. Zhang, P. T. Yu, J. X. Zhang, R. Makharia, K. L. More, and E. A. Stach, Journal of The Electrochemical Society, 157, B906 (2010).
- [17]17. V. Mazumder, M. Chi, K. L. More, and S. Sun, Journal of the American Chemical Society, 132, 7848 (2010).
- [18]18. F. Scheiba, N. Benker, U. Kunz, C. Roth, and H. Fuess, Journal of Power Sources, 177, 273 (2008).
- [19]19. T. Soboleva, X. Zhao, K. Malek, Z Xie, T. Navessin, and S. Holdcroft, ACS applied materials & interfaces, 2, 375 (2010).
- [20]20. M. S. Wilson and S. Gottesfeld, Journal of Applied Electrochemistry, 22, 1 (1992).
- [21]21. C. M. Johnston, K. Lee, T. Rockward, A. Labouriau, N. Mack, and Y. Kim, ECS Transactions, 25, 1617 (1992).
- [22]22. M. Prasanna, E. Cho, T. Lim, and I. Oh, Electrochimica Acta, 53, 5434 (2008).
- [23]23. D. A. Blom, J. R. Dunlap, T. A. Nolan, and L. F. Allard, Journal of The Electrochem- ical Society, 150, A414 (2003).
- [24]24. X. Cheng, B. Yi, M. Han, J. Zhang, Y. Qiao, and J. Yu, Journal of Power Sources, 79, 75 (1999).
- [25]25. K. S. W. Sing, D. H. Everett, R. A. W. Haul, L. Moscou, R. A. Pierotti, J. Rouquerol, and T. Siemieniewska, International Unionof Pureand Applied Chemistry, 57, 603 (1985).
- [27]27. D. Dollimore and G. R. Heal, Journal of Applied Chemistry, 14, 109 (1964).
- [28]28. T. A. Zawodzinski, C. Derouin, S. Radzinski, R. J. Sherman, V. T. Smith, T. E. Springer, and S. Gottesfeld, Journal of The Electrochemical Society, 140, 1041 (1993).
- [29]29. K. Broka and P. Ekdunge, Journal of Applied Electrochemistry, 27, 117 (1997).
- [30]30. K.-D. Kreuer, S. J. Paddison, E. Spohr, and M. Schuster, Chemical reviews, 104, 4637 (2004).
- [31]31. M. A. Modestino, D. K. Paul, S. Dishari, S. A. Petrina, F. I. Allen, M. A. Hickner, K. Karan, R. A. Segalman, and A. Z. Weber, Macromolecules, 46, 867 (2013).
- [32]32. A. R. Hillman, Q. Dong, M. A. Mohamoud, and I. Efimov, Electrochmica Acta, 55, 8142 (2010).
- [33]33. Z. Siroma, R. Kakitsubo, N. Fujiwara, T. Ioroi, S.-i. Yamazaki, and K. Yasuda, Journal of Power Sources, 189, 994 (2009).
- [34]34. Y. Liu, C. Ji, W. Gu, D. R. Baker, J. Jorne, and H. A. Gasteiger, Journal of The Electrochemical Society, 157, B1154 (2010).
- [35]35. J. Xie, K. L. More, T. A. Zawodzinski, and W. H. Smith, Journal of The Electro- chemical Society, 151, A1841 (2004).
Cited by
Sorted by citations
Liu, H., Ney, L., Zamel, N., & Li, X. (2022) · Applied Sciences · doi:10.3390/app12083776 · Cited by 85 · see citing works
Andersen, S. M., & Grahl-Madsen, L. (2016) · International Journal of Hydrogen Energy · doi:10.1016/j.ijhydene.2015.11.101 · Cited by 61 · see citing works
- Authors
- Sun, C.-N., More, K. L., Veith, G. M., & Zawodzinski, T. A.
- Affiliations
- Oak Ridge National Laboratory (US)
- Venue
- Journal of The Electrochemical Society
- Publisher
- The Electrochemical Society
- Published
- 2013
- Volume
- 160
- Issue
- 9
- Pages
- F1000-F1005
- ISSN
- 0013-4651 (ISSN-L)
- 1945-7111
- OpenAlex
- W2059607905
- Cited by
- 28
- References
- 35
- Citations by year
- 2025: 1 · 2024: 2 · 2023: 1 · 2022: 2 · 2021: 4 · 2019: 1 · 2018: 4 · 2017: 4 · 2016: 3 · 2015: 5 · 2014: 1
- FWCI
- 1.80
- Type
- journal article
- Language
- en
- Open access
- bronze
- doi.org
- Locations
- Journal of The Electrochemical Society (publishedVersion)
- Funders
- U.S. Department of Energy
- Battelle
- UT-Battelle
- Basic Energy Sciences
- Oak Ridge National Laboratory
- Los Alamos National Laboratory
- Division of Materials Sciences and Engineering
- 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
- proton exchange membrane fuel cells, catalyst layer, ionomer loading, Nafion, platinum catalysts, Vulcan carbon, pore structure, water transport, relative humidity, ionomer swelling, carbon fillers, microporosity, water absorption, proton transport
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