Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability
Abstract
We investigate the effect of the poly(acrylic acid) (PAA) carrier polymer concentration on the microstructure and rheological properties of catalyst inks for electrospun polymer–electrolyte membrane fuel-cell catalyst layers. Characterization of an ink microstructure using oscillatory shear rheology showed that the catalyst particles (platinum on carbon) are significantly agglomerated in the absence of PAA or an ionomer. Both the ionomer and PAA promoted the stability of the particles against agglomeration via electrosteric stabilization by adsorbing onto the particle surface. Increasing the PAA concentration increased the stability of the particles (or reduced the agglomerated structure) due to increasing PAA coverage onto the free surface area of the particles. However, beyond a certain increase in concentration, PAA was found to predominantly remain as an excess free polymer in the ink due to an insufficient free/available surface area on the particles for further PAA coverage. Extensional rheology measurements demonstrated that PAA enhances the extensional viscosities of the inks. Consequently, increasing the PAA concentration in the ink promoted the evolution of uniform nanofibers. However, beyond a certain concentration, a significant increase in the shear viscosities of the inks led to defective fiber morphologies because of the onset of flow instabilities. Electrochemical performance comparisons between catalystmore »
- Authors:
-
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Univ. of Massachusetts, Amherst, MA (United States)
- Publication Date:
- Research Org.:
- National Renewable Energy Laboratory (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1779800
- Report Number(s):
- NREL/JA-5900-79228
Journal ID: ISSN 2637-6105; MainId:33454;UUID:c2fe02fe-38af-48f2-a59c-ab3e2c5afdb1;MainAdminID:21274
- Grant/Contract Number:
- AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Applied Polymer Materials
- Additional Journal Information:
- Journal Volume: 3; Journal Issue: 5; Journal ID: ISSN 2637-6105
- Publisher:
- ACS Publications
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; electrospinning; poly(acrylic acid); extensional rheology; fuel cells; catalyst inks; nanofibers
Citation Formats
Khandavalli, Sunilkumar, Sharma-Nene, Nisha, Kabir, Sadia, Sur, Samrat, Rothstein, Jonathan P., Neyerlin, Kenneth C., Mauger, Scott A., and Ulsh, Michael. Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability. United States: N. p., 2021.
Web. doi:10.1021/acsapm.0c01354.
Khandavalli, Sunilkumar, Sharma-Nene, Nisha, Kabir, Sadia, Sur, Samrat, Rothstein, Jonathan P., Neyerlin, Kenneth C., Mauger, Scott A., & Ulsh, Michael. Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability. United States. https://doi.org/10.1021/acsapm.0c01354
Khandavalli, Sunilkumar, Sharma-Nene, Nisha, Kabir, Sadia, Sur, Samrat, Rothstein, Jonathan P., Neyerlin, Kenneth C., Mauger, Scott A., and Ulsh, Michael. Fri .
"Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability". United States. https://doi.org/10.1021/acsapm.0c01354. https://www.osti.gov/servlets/purl/1779800.
@article{osti_1779800,
title = {Toward Optimizing Electrospun Nanofiber Fuel Cell Catalyst Layers: Polymer–Particle Interactions and Spinnability},
author = {Khandavalli, Sunilkumar and Sharma-Nene, Nisha and Kabir, Sadia and Sur, Samrat and Rothstein, Jonathan P. and Neyerlin, Kenneth C. and Mauger, Scott A. and Ulsh, Michael},
abstractNote = {We investigate the effect of the poly(acrylic acid) (PAA) carrier polymer concentration on the microstructure and rheological properties of catalyst inks for electrospun polymer–electrolyte membrane fuel-cell catalyst layers. Characterization of an ink microstructure using oscillatory shear rheology showed that the catalyst particles (platinum on carbon) are significantly agglomerated in the absence of PAA or an ionomer. Both the ionomer and PAA promoted the stability of the particles against agglomeration via electrosteric stabilization by adsorbing onto the particle surface. Increasing the PAA concentration increased the stability of the particles (or reduced the agglomerated structure) due to increasing PAA coverage onto the free surface area of the particles. However, beyond a certain increase in concentration, PAA was found to predominantly remain as an excess free polymer in the ink due to an insufficient free/available surface area on the particles for further PAA coverage. Extensional rheology measurements demonstrated that PAA enhances the extensional viscosities of the inks. Consequently, increasing the PAA concentration in the ink promoted the evolution of uniform nanofibers. However, beyond a certain concentration, a significant increase in the shear viscosities of the inks led to defective fiber morphologies because of the onset of flow instabilities. Electrochemical performance comparisons between catalyst layers with different PAA concentrations showed maximum performance at the PAA concentration that led to the least agglomerated structure of the catalyst, most uniform fiber morphologies, and low concentrations of free (non-adsorbing) PAA in the electrode. These results provide a rationale for optimization of electrospun catalyst nanofibers for both spinnability and electrochemical performance.},
doi = {10.1021/acsapm.0c01354},
journal = {ACS Applied Polymer Materials},
number = 5,
volume = 3,
place = {United States},
year = {Fri Apr 09 00:00:00 EDT 2021},
month = {Fri Apr 09 00:00:00 EDT 2021}
}
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