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Title: Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks

Abstract

We present a rheological investigation of fuel cell catalyst inks. The effects of ink parameters, which include carbon black-support structure, Pt presence on carbon support (Pt-carbon), and ionomer (Nafion) concentration, on the ink microstructure of catalyst inks were studied using rheometry in combination with ultrasmall-angle X-ray scattering (USAXS) and dynamic light scattering (DLS). Dispersions of a high-surface-area carbon (HSC), or Ketjen black type, demonstrated a higher viscosity than Vulcan XC-72 carbon due to both a higher internal porosity and a more agglomerated structure that increased the effective particle volume fraction of the inks. The presence of Pt catalyst on both the carbon supports reduced the viscosity through electrostatic stabilization. For carbon-only dispersions (without Pt), the addition of ionomer up to a critical concentration decreased the viscosity due to electrosteric stabilization of carbon agglomerates. However, with Pt-carbon dispersions, the addition of ionomer showed contrasting behavior between Vulcan and HSC supports. In the Pt-Vulcan dispersions, the effect of ionomer addition on the rheology was qualitatively similar to Vulcan dispersions without Pt. The Pt-HSC dispersions showed an increased viscosity with ionomer addition and a strong shear-thinning nature, indicating that Nafion likely flocculated the Pt-HSC aggregates. These results were verified using DLS and USAXS.more » Further, the observations of the effect of ionomer:carbon ratio and a comparison between carbons of different surface areas provided insights on the microstructure of the catalyst ink corresponding to the optimized I/C ratio for fuel cell performance reported in the literature.« less

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [1];  [1];  [1];  [1]; ORCiD logo [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
National Renewable Energy Lab. (NREL), Golden, CO (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office
OSTI Identifier:
1487191
Alternate Identifier(s):
OSTI ID: 1491398
Report Number(s):
NREL/JA-5900-72333
Journal ID: ISSN 1944-8244
Grant/Contract Number:  
AC36-08GO28308; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 50; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; carbon; catalyst inks; catalyst layer; ionomer; platinum; proton-exchange membrane fuel cells; rheology

Citation Formats

Khandavalli, Sunilkumar, Park, Jae Hyung, Kariuki, Nancy N., Myers, Deborah J., Stickel, Jonathan J., Hurst, Katherine, Neyerlin, K. C., Ulsh, Michael, and Mauger, Scott A. Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks. United States: N. p., 2018. Web. doi:10.1021/acsami.8b15039.
Khandavalli, Sunilkumar, Park, Jae Hyung, Kariuki, Nancy N., Myers, Deborah J., Stickel, Jonathan J., Hurst, Katherine, Neyerlin, K. C., Ulsh, Michael, & Mauger, Scott A. Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks. United States. https://doi.org/10.1021/acsami.8b15039
Khandavalli, Sunilkumar, Park, Jae Hyung, Kariuki, Nancy N., Myers, Deborah J., Stickel, Jonathan J., Hurst, Katherine, Neyerlin, K. C., Ulsh, Michael, and Mauger, Scott A. Mon . "Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks". United States. https://doi.org/10.1021/acsami.8b15039. https://www.osti.gov/servlets/purl/1487191.
@article{osti_1487191,
title = {Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks},
author = {Khandavalli, Sunilkumar and Park, Jae Hyung and Kariuki, Nancy N. and Myers, Deborah J. and Stickel, Jonathan J. and Hurst, Katherine and Neyerlin, K. C. and Ulsh, Michael and Mauger, Scott A.},
abstractNote = {We present a rheological investigation of fuel cell catalyst inks. The effects of ink parameters, which include carbon black-support structure, Pt presence on carbon support (Pt-carbon), and ionomer (Nafion) concentration, on the ink microstructure of catalyst inks were studied using rheometry in combination with ultrasmall-angle X-ray scattering (USAXS) and dynamic light scattering (DLS). Dispersions of a high-surface-area carbon (HSC), or Ketjen black type, demonstrated a higher viscosity than Vulcan XC-72 carbon due to both a higher internal porosity and a more agglomerated structure that increased the effective particle volume fraction of the inks. The presence of Pt catalyst on both the carbon supports reduced the viscosity through electrostatic stabilization. For carbon-only dispersions (without Pt), the addition of ionomer up to a critical concentration decreased the viscosity due to electrosteric stabilization of carbon agglomerates. However, with Pt-carbon dispersions, the addition of ionomer showed contrasting behavior between Vulcan and HSC supports. In the Pt-Vulcan dispersions, the effect of ionomer addition on the rheology was qualitatively similar to Vulcan dispersions without Pt. The Pt-HSC dispersions showed an increased viscosity with ionomer addition and a strong shear-thinning nature, indicating that Nafion likely flocculated the Pt-HSC aggregates. These results were verified using DLS and USAXS. Further, the observations of the effect of ionomer:carbon ratio and a comparison between carbons of different surface areas provided insights on the microstructure of the catalyst ink corresponding to the optimized I/C ratio for fuel cell performance reported in the literature.},
doi = {10.1021/acsami.8b15039},
journal = {ACS Applied Materials and Interfaces},
number = 50,
volume = 10,
place = {United States},
year = {Mon Dec 10 00:00:00 EST 2018},
month = {Mon Dec 10 00:00:00 EST 2018}
}

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