Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells
Abstract
Improvements in polymer electrolyte fuel cell (PEFC) electrode performance have primarily focused on catalyst and ionomer developments, marginalizing the importance of catalyst ink formulation. In this study, the effect of ink formulation is examined across a series of cathodes comprised of PtCo supported on high surface area carbon (PtCo/HSC) and Nafion ionomer using an array of in situ electrochemical and ex situ characterization techniques. In contrast to prior work on Pt/Vu systems, ink water content had little effect on the electrochemically determined ionomer coverage for the PtCo/HSC electrocatalyst examined here. Characterization using nano-scale resolution X-ray computed tomography (nano-CT) demonstrated that water-rich ink formulations lead to a reduction in aggregate size (ionomer + PtCo/HSC), improving local O2 transport. This understanding, combined with the use of a commercially-available electrocatalyst was used to produced state-of-the-art membrane electrode assemblies with Pt loadings of 0.03/0.08 mgPt/cm2 on the anode and cathode respectively, having; i) > 1 A/mgPt (0.9 ViR-free, 150 kPa, 80 °C, 100% RH, H2/O2), ii) 320 mA/cm2 at 0.8 V, 150 kPa, 80 °C, 100% RH, H2/Air), and iii) > 1 W/cm2elec at rated power (0.67 V, 250 kPa, 94 °C, 65% RH, H2/Air) or < 0.11 gPt/kWrated.
- Authors:
-
[1];
[2];
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- National Renewable Energy Lab. (NREL), Golden, CO (United States); The Ohio State Univ., Columbus, OH (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States); Assiut University (Egypt)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); USDOE Office of Science (SC), Workforce Development for Teachers and Scientists (WDTS); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1777138
- Alternate Identifier(s):
- OSTI ID: 1811042
- Grant/Contract Number:
- AC02-06CH11357; AC36-08GO28308
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Power Sources
- Additional Journal Information:
- Journal Volume: 482; Journal ID: ISSN 0378-7753
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; ink solvent effects; nano-CT; O-2 transport; polymer electrolyte fuel cells; USAXS Ionomer-catalyst interface
Citation Formats
Van Cleve, Tim, Wang, Guanxiong, Mooney, Mason, Cetinbas, C. Firat, Kariuki, Nancy, Park, Jaehyung, Farghaly, Ahmed, Myers, Deborah, and Neyerlin, K. C. Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells. United States: N. p., 2020.
Web. doi:10.1016/j.jpowsour.2020.228889.
Van Cleve, Tim, Wang, Guanxiong, Mooney, Mason, Cetinbas, C. Firat, Kariuki, Nancy, Park, Jaehyung, Farghaly, Ahmed, Myers, Deborah, & Neyerlin, K. C. Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells. United States. https://doi.org/10.1016/j.jpowsour.2020.228889
Van Cleve, Tim, Wang, Guanxiong, Mooney, Mason, Cetinbas, C. Firat, Kariuki, Nancy, Park, Jaehyung, Farghaly, Ahmed, Myers, Deborah, and Neyerlin, K. C. Mon .
"Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells". United States. https://doi.org/10.1016/j.jpowsour.2020.228889. https://www.osti.gov/servlets/purl/1777138.
@article{osti_1777138,
title = {Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells},
author = {Van Cleve, Tim and Wang, Guanxiong and Mooney, Mason and Cetinbas, C. Firat and Kariuki, Nancy and Park, Jaehyung and Farghaly, Ahmed and Myers, Deborah and Neyerlin, K. C.},
abstractNote = {Improvements in polymer electrolyte fuel cell (PEFC) electrode performance have primarily focused on catalyst and ionomer developments, marginalizing the importance of catalyst ink formulation. In this study, the effect of ink formulation is examined across a series of cathodes comprised of PtCo supported on high surface area carbon (PtCo/HSC) and Nafion ionomer using an array of in situ electrochemical and ex situ characterization techniques. In contrast to prior work on Pt/Vu systems, ink water content had little effect on the electrochemically determined ionomer coverage for the PtCo/HSC electrocatalyst examined here. Characterization using nano-scale resolution X-ray computed tomography (nano-CT) demonstrated that water-rich ink formulations lead to a reduction in aggregate size (ionomer + PtCo/HSC), improving local O2 transport. This understanding, combined with the use of a commercially-available electrocatalyst was used to produced state-of-the-art membrane electrode assemblies with Pt loadings of 0.03/0.08 mgPt/cm2 on the anode and cathode respectively, having; i) > 1 A/mgPt (0.9 ViR-free, 150 kPa, 80 °C, 100% RH, H2/O2), ii) 320 mA/cm2 at 0.8 V, 150 kPa, 80 °C, 100% RH, H2/Air), and iii) > 1 W/cm2elec at rated power (0.67 V, 250 kPa, 94 °C, 65% RH, H2/Air) or < 0.11 gPt/kWrated.},
doi = {10.1016/j.jpowsour.2020.228889},
journal = {Journal of Power Sources},
number = ,
volume = 482,
place = {United States},
year = {Mon Sep 21 00:00:00 EDT 2020},
month = {Mon Sep 21 00:00:00 EDT 2020}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Study of the charge displacement at constant potential during CO adsorption on Pt(110) and Pt(111) electrodes in contact with a perchloric acid solution
journal, July 1992
- Clavilier, J.; Albalat, R.; Gomez, R.
- Journal of Electroanalytical Chemistry, Vol. 330, Issue 1-2
The Priority and Challenge of High-Power Performance of Low-Platinum Proton-Exchange Membrane Fuel Cells
journal, March 2016
- Kongkanand, Anusorn; Mathias, Mark F.
- The Journal of Physical Chemistry Letters, Vol. 7, Issue 7
Effects of carbon supports on Pt distribution, ionomer coverage and cathode performance for polymer electrolyte fuel cells
journal, May 2016
- Park, Young-Chul; Tokiwa, Haruki; Kakinuma, Katsuyoshi
- Journal of Power Sources, Vol. 315
Analysis of Oxygen-Transport Diffusion Resistance in Proton-Exchange-Membrane Fuel Cells
journal, January 2011
- Nonoyama, Nobuaki; Okazaki, Shinobu; Weber, Adam Z.
- Journal of The Electrochemical Society, Vol. 158, Issue 4
Effect of the Side-Chain Structure of Perfluoro-Sulfonic Acid Ionomers on the Oxygen Reduction Reaction on the Surface of Pt
journal, December 2017
- Kodama, Kensaku; Motobayashi, Kenta; Shinohara, Akihiro
- ACS Catalysis, Vol. 8, Issue 1
Support materials for PEMFC and DMFC electrocatalysts—A review
journal, June 2012
- Sharma, Surbhi; Pollet, Bruno G.
- Journal of Power Sources, Vol. 208
Utilizing ink composition to tune bulk-electrode gas transport, performance, and operational robustness for a Fe–N–C catalyst in polymer electrolyte fuel cell
journal, September 2020
- Osmieri, Luigi; Wang, Guanxiong; Cetinbas, Firat C.
- Nano Energy, Vol. 75
Impact of Substrate and Processing on Confinement of Nafion Thin Films
journal, April 2014
- Kusoglu, Ahmet; Kushner, Douglas; Paul, Devproshad K.
- Advanced Functional Materials, Vol. 24, Issue 30
Understanding inks for porous-electrode formation
journal, January 2017
- Hatzell, Kelsey B.; Dixit, Marm B.; Berlinger, Sarah A.
- J. Mater. Chem. A, Vol. 5, Issue 39
Recent advances in activity and durability enhancement of Pt/C catalytic cathode in PEMFC
journal, October 2007
- Yu, Xingwen; Ye, Siyu
- Journal of Power Sources, Vol. 172, Issue 1
Determination of O 2 Mass Transport at the Pt | PFSA Ionomer Interface under Reduced Relative Humidity
journal, December 2015
- Novitski, David; Holdcroft, Steven
- ACS Applied Materials & Interfaces, Vol. 7, Issue 49
Electrical resistance and microstructure of typical gas diffusion layers for proton exchange membrane fuel cell under compression
journal, December 2018
- Qiu, Diankai; Janßen, Holger; Peng, Linfa
- Applied Energy, Vol. 231
Microstructural Analysis and Transport Resistances of Low-Platinum-Loaded PEFC Electrodes
journal, January 2017
- Cetinbas, Firat C.; Wang, Xiaohua; Ahluwalia, Rajesh K.
- Journal of The Electrochemical Society, Vol. 164, Issue 14
The impact of short side chain ionomer on polymer electrolyte membrane fuel cell performance and durability
journal, May 2018
- Shahgaldi, Samaneh; Alaefour, Ibrahim; Li, Xianguo
- Applied Energy, Vol. 217
Effect of gas diffusion layer compression on PEM fuel cell performance
journal, September 2006
- Ge, Jiabin; Higier, Andrew; Liu, Hongtan
- Journal of Power Sources, Vol. 159, Issue 2
Impact of Compressive Stress on MEA Pore Structure and Its Consequence on PEMFC Performance
journal, January 2016
- Sassin, M. B.; Garsany, Y.; Gould, B. D.
- Journal of The Electrochemical Society, Vol. 163, Issue 8
Fe Stabilization by Intermetallic L1 0 -FePt and Pt Catalysis Enhancement in L1 0 -FePt/Pt Nanoparticles for Efficient Oxygen Reduction Reaction in Fuel Cells
journal, February 2018
- Li, Junrui; Xi, Zheng; Pan, Yung-Tin
- Journal of the American Chemical Society, Vol. 140, Issue 8
Agglomerates in Polymer Electrolyte Fuel Cell Electrodes: Part II. Transport Characterization
journal, January 2018
- Cetinbas, Firat C.; Ahluwalia, Rajesh K.
- Journal of The Electrochemical Society, Vol. 165, Issue 13
Ultra-small-angle X-ray scattering at the Advanced Photon Source
journal, April 2009
- Ilavsky, Jan; Jemian, Pete R.; Allen, Andrew J.
- Journal of Applied Crystallography, Vol. 42, Issue 3
Irena : tool suite for modeling and analysis of small-angle scattering
journal, February 2009
- Ilavsky, Jan; Jemian, Peter R.
- Journal of Applied Crystallography, Vol. 42, Issue 2
A Review of the Terms Agglomerate and Aggregate with a Recommendation for Nomenclature Used in Powder and Particle Characterization
journal, October 2002
- Nichols, Gary; Byard, Stephen; Bloxham, Mark J.
- Journal of Pharmaceutical Sciences, Vol. 91, Issue 10
Dictating Pt-Based Electrocatalyst Performance in Polymer Electrolyte Fuel Cells, from Formulation to Application
journal, November 2019
- Van Cleve, Tim; Khandavalli, Sunilkumar; Chowdhury, Anamika
- ACS Applied Materials & Interfaces, Vol. 11, Issue 50
Cathode Loading Impact on Voltage Cycling Induced PEMFC Degradation: A Voltage Loss Analysis
journal, January 2018
- Harzer, Gregor S.; Schwämmlein, Jan N.; Damjanović, Ana Marija
- Journal of The Electrochemical Society, Vol. 165, Issue 6
Characterizing Electrolyte and Platinum Interface in PEM Fuel Cells Using CO Displacement
journal, December 2016
- Garrick, Taylor R.; Moylan, Thomas E.; Yarlagadda, Venkata
- Journal of The Electrochemical Society, Vol. 164, Issue 2
Proton Conduction and Oxygen Reduction Kinetics in PEM Fuel Cell Cathodes: Effects of Ionomer-to-Carbon Ratio and Relative Humidity
journal, January 2009
- Liu, Yuxiu; Murphy, Michael W.; Baker, Daniel R.
- Journal of The Electrochemical Society, Vol. 156, Issue 8
Nanoscale 3D imaging at the Advanced Photon Source
journal, May 2016
- De Andrade, Vincent; Deriy, Alex; Wojcik, Michael J.
- SPIE Newsroom
Nanofiber Electrodes with Low Platinum Loading for High Power Hydrogen/Air PEM Fuel Cells
journal, January 2013
- Brodt, Matthew; Wycisk, Ryszard; Pintauro, Peter N.
- Journal of The Electrochemical Society, Vol. 160, Issue 8
Effect of the catalytic ink preparation method on the performance of polymer electrolyte membrane fuel cells
journal, April 2002
- Shin, S. -J.; Lee, J. -K.; Ha, H. -Y.
- Journal of Power Sources, Vol. 106, Issue 1-2
Controlling Nafion Structure and Properties via Wetting Interactions
journal, May 2012
- Modestino, Miguel A.; Kusoglu, Ahmet; Hexemer, Alexander
- Macromolecules, Vol. 45, Issue 11, p. 4681-4688
Multimetallic Core/Interlayer/Shell Nanostructures as Advanced Electrocatalysts
journal, October 2014
- Kang, Yijin; Snyder, Joshua; Chi, Miaofang
- Nano Letters, Vol. 14, Issue 11
Integration of TomoPy and the ASTRA toolbox for advanced processing and reconstruction of tomographic synchrotron data
journal, April 2016
- Pelt, Daniël M.; Gürsoy, Dogˇa; Palenstijn, Willem Jan
- Journal of Synchrotron Radiation, Vol. 23, Issue 3
High power, Low-Pt membrane electrode assemblies for proton exchange membrane fuel cells
journal, December 2018
- Garsany, Yannick; Atkinson, Robert W.; Gould, Benjamin D.
- Journal of Power Sources, Vol. 408
Measurement of Catalyst Layer Electrolyte Resistance in PEFCs Using Electrochemical Impedance Spectroscopy
journal, January 2005
- Makharia, Rohit; Mathias, Mark F.; Baker, Daniel R.
- Journal of The Electrochemical Society, Vol. 152, Issue 5
Impact of Platinum Loading and Catalyst Layer Structure on PEMFC Performance
journal, January 2013
- Owejan, Jon P.; Owejan, Jeanette E.; Gu, Wenbin
- Journal of The Electrochemical Society, Vol. 160, Issue 8
Boosting Fuel Cell Performance with Accessible Carbon Mesopores
journal, February 2018
- Yarlagadda, Venkata; Carpenter, Michael K.; Moylan, Thomas E.
- ACS Energy Letters, Vol. 3, Issue 3
Modifying the Electrocatalyst–Ionomer Interface via Sulfonated Poly(ionic liquid) Block Copolymers to Enable High-Performance Polymer Electrolyte Fuel Cells
journal, April 2020
- Li, Yawei; Van Cleve, Tim; Sun, Rui
- ACS Energy Letters, Vol. 5, Issue 6
Measurement of Oxygen Transport Resistance in PEM Fuel Cells by Limiting Current Methods
journal, January 2009
- Baker, Daniel R.; Caulk, David A.; Neyerlin, Kenneth C.
- Journal of The Electrochemical Society, Vol. 156, Issue 9
Rheological Investigation on the Microstructure of Fuel Cell Catalyst Inks
journal, December 2018
- Khandavalli, Sunilkumar; Park, Jae Hyung; Kariuki, Nancy N.
- ACS Applied Materials & Interfaces, Vol. 10, Issue 50
The Impact of Platinum Loading on Oxygen Transport Resistance
journal, January 2012
- Greszler, Thomas A.; Caulk, David; Sinha, Puneet
- Journal of The Electrochemical Society, Vol. 159, Issue 12
Control of Architecture in Rhombic Dodecahedral Pt–Ni Nanoframe Electrocatalysts
journal, August 2017
- Becknell, Nigel; Son, Yoonkook; Kim, Dohyung
- Journal of the American Chemical Society, Vol. 139, Issue 34
An in situ technique for analyzing ionomer coverage in catalyst layers
journal, March 2013
- Iden, Hiroshi; Ohma, Atsushi
- Journal of Electroanalytical Chemistry, Vol. 693
Tailoring the Membrane-Electrode Interface in PEM Fuel Cells: A Review and Perspective on Novel Engineering Approaches
journal, September 2017
- Breitwieser, Matthias; Klingele, Matthias; Vierrath, Severin
- Advanced Energy Materials, Vol. 8, Issue 4
Characterization of 9Cr-1MoVNb steel by anomalous small-angle X-ray scattering
journal, November 1991
- Jemian, P. R.; Weertman, J. R.; Long, G. G.
- Acta Metallurgica et Materialia, Vol. 39, Issue 11
Modeling Air Electrodes with Low Platinum Loading
journal, January 2019
- Darling, Robert
- Journal of The Electrochemical Society, Vol. 166, Issue 7
Analysis of the Microstructure Formation Process and Its Influence on the Performance of Polymer Electrolyte Fuel-Cell Catalyst Layers
journal, July 2015
- Takahashi, Shinichi; Mashio, Tetsuya; Horibe, Norifumi
- ChemElectroChem, Vol. 2, Issue 10
Resolving Electrode Morphology’s Impact on Platinum Group Metal-Free Cathode Performance Using Nano-CT of 3D Hierarchical Pore and Ionomer Distribution
journal, November 2016
- Komini Babu, Siddharth; Chung, Hoon T.; Zelenay, Piotr
- ACS Applied Materials & Interfaces, Vol. 8, Issue 48
Fuel-Cell Catalyst-Layer Resistance via Hydrogen Limiting-Current Measurements
journal, January 2019
- Schuler, Tobias; Chowdhury, Anamika; Freiberg, Anna T.
- Journal of The Electrochemical Society, Vol. 166, Issue 7
Comparative investigation into the performance and durability of long and short side chain ionomers in Polymer Electrolyte Membrane Fuel Cells
journal, November 2019
- Talukdar, Krishan; Gazdzicki, Pawel; Friedrich, K. Andreas
- Journal of Power Sources, Vol. 439
Catalyst-Layer Ionomer Imaging of Fuel Cells
journal, September 2015
- Guetaz, L.; Lopez-Haro, M.; Escribano, S.
- ECS Transactions, Vol. 69, Issue 17
PEFC catalyst layers: Effect of support microstructure on both distributions of Pt and ionomer and cell performance and durability
journal, June 2020
- Uchida, Makoto
- Current Opinion in Electrochemistry, Vol. 21
Inherent Acidity of Perfluorosulfonic Acid Ionomer Dispersions and Implications for Ink Aggregation
journal, July 2018
- Berlinger, Sarah A.; McCloskey, Bryan D.; Weber, Adam Z.
- The Journal of Physical Chemistry B, Vol. 122, Issue 31
Oxidation of Platinum Nickel Nanowires to Improve Durability of Oxygen-Reducing Electrocatalysts
journal, January 2016
- Alia, Shaun M.; Pylypenko, Svitlana; Dameron, Arrelaine
- Journal of The Electrochemical Society, Vol. 163, Issue 3
Fabrication Method for Laboratory-Scale High-Performance Membrane Electrode Assemblies for Fuel Cells
journal, December 2016
- Sassin, Megan B.; Garsany, Yannick; Gould, Benjamin D.
- Analytical Chemistry, Vol. 89, Issue 1
Pt alloy oxygen-reduction electrocatalysts: Synthesis, structure, and property
journal, May 2020
- Wang, Xiao Xia; Sokolowski, Joshua; Liu, Hui
- Chinese Journal of Catalysis, Vol. 41, Issue 5
Ink Solvent Dependence of the Ionomer Distribution in the Catalyst Layer of a PEMFC
journal, January 2018
- Orfanidi, Alin; Rheinländer, Philipp J.; Schulte, Nicole
- Journal of The Electrochemical Society, Vol. 165, Issue 14
Exceptional Oxygen Reduction Reaction Activity and Durability of Platinum–Nickel Nanowires through Synthesis and Post-Treatment Optimization
journal, April 2017
- Alia, Shaun M.; Ngo, Chilan; Shulda, Sarah
- ACS Omega, Vol. 2, Issue 4
Humidity and Temperature Dependences of Oxygen Transport Resistance of Nafion Thin Film on Platinum Electrode
journal, August 2016
- Kudo, Kenji; Jinnouchi, Ryosuke; Morimoto, Yu
- Electrochimica Acta, Vol. 209
Water Management in Cathode Catalyst Layers of PEM Fuel Cells
journal, January 2006
- Eikerling, M.
- Journal of The Electrochemical Society, Vol. 153, Issue 3
On the Micro-, Meso-, and Macroporous Structures of Polymer Electrolyte Membrane Fuel Cell Catalyst Layers
journal, January 2010
- Soboleva, Tatyana; Zhao, Xinsheng; Malek, Kourosh
- ACS Applied Materials & Interfaces, Vol. 2, Issue 2
Performance of advanced automotive fuel cell systems with heat rejection constraint
journal, March 2016
- Ahluwalia, R. K.; Wang, X.; Steinbach, A. J.
- Journal of Power Sources, Vol. 309
Influence of the Gas Diffusion Layer Compression on the Oxygen Transport in PEM Fuel Cells at High Water Saturation Levels
journal, January 2017
- Simon, Christoph; Hasché, Frédéric; Gasteiger, Hubert A.
- Journal of The Electrochemical Society, Vol. 164, Issue 6
New results of PEFC electrodes produced by the DLR dry preparation technique
journal, April 2002
- Gülzow, Erich; Kaz, Till
- Journal of Power Sources, Vol. 106, Issue 1-2
Agglomerates in Polymer Electrolyte Fuel Cell Electrodes: Part I. Structural Characterization
journal, January 2018
- Cetinbas, Firat C.; Ahluwalia, Rajesh K.; Kariuki, Nancy N.
- Journal of The Electrochemical Society, Vol. 165, Issue 13