Visualization, understanding, and mitigation of process-induced-membrane irregularities in gas diffusion electrode-based polymer electrolyte membrane fuel cells

Wang, Min; Medina, Samantha; Ochoa-Lozano, Josias; Mauger, Scott; Pylypenko, Svitlana; Ulsh, Michael; Bender, Guido

doi:10.1016/j.ijhydene.2021.01.186

Visualization, understanding, and mitigation of process-induced-membrane irregularities in gas diffusion electrode-based polymer electrolyte membrane fuel cells

Journal Article · Fri Feb 19 00:00:00 EST 2021 · International Journal of Hydrogen Energy

DOI:https://doi.org/10.1016/j.ijhydene.2021.01.186· OSTI ID:1769844

^[1]; ^[2]; ^[3]; ^[1]; ^[4]; ^[1]; ^[1]

National Renewable Energy Lab. (NREL), Golden, CO (United States)
Colorado School of Mines, Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of California, Riverside, CA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Colorado School of Mines, Golden, CO (United States)

Polymer electrolyte membrane fuel cells (PEMFC) show substantial promise for their application in electric vehicles. For large-scale manufacturing of PEMFCs, roll-to-roll coated gas-diffusion-electrodes (GDE) offer certain advantages over other production pathways. Procedures including hot pressing and coating an ionomer overlayer may be necessary for this manufacturing pathway to enable a suitable catalyst layer/membrane interface. The same procedures may potentially introduce membrane irregularities, especially when thin membranes are used. Limited understanding exists regarding if and to what extent such irregularities impact PEMFC performance and lifetime, and therefore be considered defects. In this study, NREL's customized fuel cell hardware that enables quasi in-situ infrared (IR) thermography studies was utilized to visualize spatial hydrogen crossover and identify membrane irregularities that originated from the GDE-based MEA fabrication process. The structure of these membrane irregularities was investigated by scanning electron microscopy (SEM) and its impact on initial H2/air performance was determined. Accelerated stress testing (AST) revealed that these irregularities develop into failure point locations. These results were validated across many MEAs with identified process-induced membrane irregularities. By selecting specific gas diffusion media properties and by fine tuning the MEA hot pressing parameters, the formation of such membrane irregularities was mitigated.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Laboratory (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Hydrogen and Fuel Cell Technologies Office (EE-3F)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1769844

Alternate ID(s):: OSTI ID: 1775192

Report Number(s):: NREL/JA-5900-79294; MainId:33520; UUID:08e9549d-33f0-420f-a359-1d35e04fa7a3; MainAdminID:19803

Journal Information:: International Journal of Hydrogen Energy, Journal Name: International Journal of Hydrogen Energy Journal Issue: 27 Vol. 46; ISSN 0360-3199

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (56)

The effects of pinholes on proton exchange membrane fuel cell performance Lü, Weizhong; Liu, Zhixiang; Wang, Cheng International Journal of Energy Research, Vol. 35, Issue 1 https://doi.org/10.1002/er.1728	journal	December 2010
Understanding Membrane Failure in PEMFC: Comparison of Diagnostic Tools at Different Observation Scales De Moor, G.; Bas, C.; Charvin, N. Fuel Cells, Vol. 12, Issue 3 https://doi.org/10.1002/fuce.201100161	journal	March 2012
Defect Detection in Fuel Cell Gas Diffusion Electrodes Using Infrared Thermography Ulsh, M.; Porter, J. M.; Bittinat, D. C. Fuel Cells, Vol. 16, Issue 2 https://doi.org/10.1002/fuce.201500137	journal	March 2016
Utilizing a Segmented Fuel Cell to Study the Effects of Electrode Coating Irregularities on PEM Fuel Cell Initial Performance Phillips, A.; Ulsh, M.; Porter, J. Fuel Cells, Vol. 17, Issue 3 https://doi.org/10.1002/fuce.201600214	journal	April 2017
The Effect of Membrane Casting Irregularities on Initial Fuel Cell Performance Phillips, A.; Ulsh, M.; Mackay, J. Fuel Cells, Vol. 20, Issue 1 https://doi.org/10.1002/fuce.201900149	journal	January 2020
Improvement of the proton exchange membrane fuel cell performances by optimization of the hot pressing process for membrane electrode assembly Martemianov, S.; Raileanu Ilie, V. A.; Coutanceau, C. Journal of Solid State Electrochemistry, Vol. 18, Issue 5 https://doi.org/10.1007/s10008-013-2273-2	journal	October 2013
Influence of hot-pressing temperature on the performance of PEMFC and catalytic activity Lin, Jing-Chie; Lai, Chien-Ming; Ting, Fu-Ping Journal of Applied Electrochemistry, Vol. 39, Issue 7 https://doi.org/10.1007/s10800-008-9758-1	journal	January 2009
Review and analysis of PEM fuel cell design and manufacturing Mehta, Viral; Cooper, Joyce Smith Journal of Power Sources, Vol. 114, Issue 1 https://doi.org/10.1016/S0378-7753(02)00542-6	journal	February 2003
Importance of electrode hot-pressing conditions for the catalyst performance of proton exchange membrane fuel cells Andersen, Shuang Ma; Dhiman, Rajnish; Larsen, Mikkel Juul Applied Catalysis B: Environmental, Vol. 172-173 https://doi.org/10.1016/j.apcatb.2015.02.023	journal	August 2015
Impact of manufacturing processes on proton exchange membrane fuel cell performance Shahgaldi, Samaneh; Alaefour, Ibrahim; Li, Xianguo Applied Energy, Vol. 225 https://doi.org/10.1016/j.apenergy.2018.05.086	journal	September 2018
Application of a segmented cell setup to detect pinhole and catalyst loading defects in proton exchange membrane fuel cells Reshetenko, Tatyana V.; Bender, Guido; Bethune, Keith Electrochimica Acta, Vol. 76 https://doi.org/10.1016/j.electacta.2012.04.138	journal	August 2012
Investigation of membrane electrode assembly (MEA) hot-pressing parameters for proton exchange membrane fuel cell Therdthianwong, Apichai; Manomayidthikarn, Phochan; Therdthianwong, Supaporn Energy, Vol. 32, Issue 12 https://doi.org/10.1016/j.energy.2007.07.005	journal	December 2007
Optimization of parameters for hot-pressing manufacture of membrane electrode assembly for PEM (polymer electrolyte membrane fuel cells) fuel cell Okur, Osman; İyigün Karadağ, Çiğdem; Boyacı San, Fatma Gül Energy, Vol. 57 https://doi.org/10.1016/j.energy.2013.05.001	journal	August 2013
A review of accelerated stress tests of MEA durability in PEM fuel cells Zhang, S.; Yuan, X.; Wang, H. International Journal of Hydrogen Energy, Vol. 34, Issue 1 https://doi.org/10.1016/j.ijhydene.2008.10.012	journal	January 2009
Fuel cell vehicles: State of the art with economic and environmental concerns Veziroglu, Ayfer; Macario, Rosario International Journal of Hydrogen Energy, Vol. 36, Issue 1 https://doi.org/10.1016/j.ijhydene.2010.08.145	journal	January 2011
Non precious metal catalysts for the PEM fuel cell cathode Othman, Rapidah; Dicks, Andrew L.; Zhu, Zhonghua International Journal of Hydrogen Energy, Vol. 37, Issue 1 https://doi.org/10.1016/j.ijhydene.2011.08.095	journal	January 2012
Role of the glass transition temperature of Nafion 117 membrane in the preparation of the membrane electrode assembly in a direct methanol fuel cell (DMFC) Jung, Ho-Young; Kim, Jung Won International Journal of Hydrogen Energy, Vol. 37, Issue 17 https://doi.org/10.1016/j.ijhydene.2012.05.121	journal	September 2012
Experimental investigation of pinhole effect on MEA/cell aging in PEMFC Huang, B. T.; Chatillon, Y.; Bonnet, C. International Journal of Hydrogen Energy, Vol. 38, Issue 1 https://doi.org/10.1016/j.ijhydene.2012.09.058	journal	January 2013
Understanding the formation of pinholes in PFSA membranes with the essential work of fracture (EWF) Moukheiber, E.; Bas, C.; Flandin, L. International Journal of Hydrogen Energy, Vol. 39, Issue 6 https://doi.org/10.1016/j.ijhydene.2013.03.031	journal	February 2014
A review of fuel cell based hybrid power supply architectures and algorithms for household appliances Boscaino, V.; Miceli, R.; Capponi, G. International Journal of Hydrogen Energy, Vol. 39, Issue 3 https://doi.org/10.1016/j.ijhydene.2013.10.165	journal	January 2014
Hydrogen and fuel cell technologies for heating: A review Dodds, Paul E.; Staffell, Iain; Hawkes, Adam D. International Journal of Hydrogen Energy, Vol. 40, Issue 5 https://doi.org/10.1016/j.ijhydene.2014.11.059	journal	February 2015
Perfluorosulfonic acid membrane degradation in the hydrogen inlet region: A macroscopic approach De Moor, G.; Bas, C.; Charvin, N. International Journal of Hydrogen Energy, Vol. 41, Issue 1 https://doi.org/10.1016/j.ijhydene.2015.10.066	journal	January 2016
Investigation of porous structure formation of catalyst layers for proton exchange membrane fuel cells and their effect on cell performance Suzuki, Takahiro; Tanaka, Hiroki; Hayase, Masanori International Journal of Hydrogen Energy, Vol. 41, Issue 44 https://doi.org/10.1016/j.ijhydene.2016.09.078	journal	November 2016
A comprehensive review on unitized regenerative fuel cells: Crucial challenges and developments Sadhasivam, T.; Dhanabalan, K.; Roh, Sung-Hee International Journal of Hydrogen Energy, Vol. 42, Issue 7 https://doi.org/10.1016/j.ijhydene.2016.10.140	journal	February 2017
Gas diffusion layer modifications and treatments for improving the performance of proton exchange membrane fuel cells and electrolysers: A review Omrani, Reza; Shabani, Bahman International Journal of Hydrogen Energy, Vol. 42, Issue 47 https://doi.org/10.1016/j.ijhydene.2017.09.132	journal	November 2017
Impacts of electrode coating irregularities on polymer electrolyte membrane fuel cell lifetime using quasi in-situ infrared thermography and accelerated stress testing Phillips, Adam; Ulsh, Michael; Neyerlin, K. C. International Journal of Hydrogen Energy, Vol. 43, Issue 12 https://doi.org/10.1016/j.ijhydene.2018.02.050	journal	March 2018
“The development of a through-plane reactive excitation technique for detection of pinholes in membrane-containing MEA sub-assemblies” Ulsh, Michael; DeBari, Annalisa; Berliner, Jacob M. International Journal of Hydrogen Energy, Vol. 44, Issue 16 https://doi.org/10.1016/j.ijhydene.2018.12.181	journal	March 2019
Wetting phenomena during processing of high-viscosity shear-thinning fluid Bhamidipati, Kanthi Latha; Didari, Sima; Bedell, Prince Journal of Non-Newtonian Fluid Mechanics, Vol. 166, Issue 12-13 https://doi.org/10.1016/j.jnnfm.2011.03.009	journal	July 2011
Fatigue and creep to leak tests of proton exchange membranes using pressure-loaded blisters Li, Yongqiang; Dillard, David A.; Case, Scott W. Journal of Power Sources, Vol. 194, Issue 2 https://doi.org/10.1016/j.jpowsour.2009.06.083	journal	December 2009
The effect of hydrogen crossover on open-circuit voltage in polymer electrolyte membrane fuel cells Vilekar, Saurabh A.; Datta, Ravindra Journal of Power Sources, Vol. 195, Issue 8 https://doi.org/10.1016/j.jpowsour.2009.10.023	journal	April 2010
Applying infrared thermography as a quality-control tool for the rapid detection of polymer-electrolyte-membrane-fuel-cell catalyst-layer-thickness variations Aieta, Niccolo V.; Das, Prodip K.; Perdue, Andrew Journal of Power Sources, Vol. 211, p. 4-11 https://doi.org/10.1016/j.jpowsour.2012.02.030	journal	August 2012
Investigation of membrane degradation in polymer electrolyte fuel cells using local gas permeation analysis Kreitmeier, Stefan; Schuler, Gabriel A.; Wokaun, Alexander Journal of Power Sources, Vol. 212 https://doi.org/10.1016/j.jpowsour.2012.03.071	journal	August 2012
Rapid detection of defects in fuel-cell electrodes using infrared reactive-flow-through technique Das, Prodip K.; Weber, Adam Z.; Bender, Guido Journal of Power Sources, Vol. 261 https://doi.org/10.1016/j.jpowsour.2013.11.124	journal	September 2014
Detecting and localizing failure points in proton exchange membrane fuel cells using IR thermography Bender, Guido; Felt, Wyatt; Ulsh, Michael Journal of Power Sources, Vol. 253 https://doi.org/10.1016/j.jpowsour.2013.12.045	journal	May 2014
Membrane degradation during combined chemical and mechanical accelerated stress testing of polymer electrolyte fuel cells Lim, C.; Ghassemzadeh, L.; Van Hove, F. Journal of Power Sources, Vol. 257 https://doi.org/10.1016/j.jpowsour.2014.01.106	journal	July 2014
Effect of pinhole location on degradation in polymer electrolyte fuel cells Bodner, Merit; Hochenauer, Christoph; Hacker, Viktor Journal of Power Sources, Vol. 295 https://doi.org/10.1016/j.jpowsour.2015.07.021	journal	November 2015
Reactive impinging-flow technique for polymer-electrolyte-fuel-cell electrode-defect detection Zenyuk, Iryna V.; Englund, Nicholas; Bender, Guido Journal of Power Sources, Vol. 332 https://doi.org/10.1016/j.jpowsour.2016.09.109	journal	November 2016
Life-cycle implications of hydrogen fuel cell electric vehicle technology for medium- and heavy-duty trucks Lee, Dong-Yeon; Elgowainy, Amgad; Kotz, Andrew Journal of Power Sources, Vol. 393 https://doi.org/10.1016/j.jpowsour.2018.05.012	journal	July 2018
Direct hydrogen fuel cell electric vehicle cost analysis: System and high-volume manufacturing description, validation, and outlook Thompson, Simon T.; James, Brian D.; Huya-Kouadio, Jennie M. Journal of Power Sources, Vol. 399 https://doi.org/10.1016/j.jpowsour.2018.07.100	journal	September 2018
Fabrication of high-performance gas-diffusion-electrode based membrane-electrode assemblies Mauger, Scott A.; Pfeilsticker, Jason R.; Wang, Min Journal of Power Sources, Vol. 450 https://doi.org/10.1016/j.jpowsour.2019.227581	journal	February 2020
Thermal management strategy for a proton exchange membrane fuel cell system with a large active cell area Yu, Sangseok; Jung, Dohoy Renewable Energy, Vol. 33, Issue 12 https://doi.org/10.1016/j.renene.2008.02.015	journal	December 2008
Analysis of mechanism of Nafion ® conductivity change due to hot pressing treatment DeBonis, D.; Mayer, M.; Omosebi, A. Renewable Energy, Vol. 89 https://doi.org/10.1016/j.renene.2015.11.081	journal	April 2016
Fabrication Method for Laboratory-Scale High-Performance Membrane Electrode Assemblies for Fuel Cells Sassin, Megan B.; Garsany, Yannick; Gould, Benjamin D. Analytical Chemistry, Vol. 89, Issue 1 https://doi.org/10.1021/acs.analchem.6b03005	journal	December 2016
Impact of Catalyst Ink Dispersing Methodology on Fuel Cell Performance Using in-Situ X-ray Scattering Wang, Min; Park, Jae Hyung; Kabir, Sadia ACS Applied Energy Materials, Vol. 2, Issue 9 https://doi.org/10.1021/acsaem.9b01037	journal	July 2019
Impact of Microporous Layer Roughness on Gas-Diffusion-Electrode-Based Polymer Electrolyte Membrane Fuel Cell Performance Wang, Min; Medina, Samantha; Pfeilsticker, Jason R. ACS Applied Energy Materials, Vol. 2, Issue 11 https://doi.org/10.1021/acsaem.9b01871	journal	October 2019
Elucidating the Dynamic Nature of Fuel Cell Electrodes as a Function of Conditioning: An ex Situ Material Characterization and in Situ Electrochemical Diagnostic Study Kabir, Sadia; Myers, Deborah J.; Kariuki, Nancy ACS Applied Materials & Interfaces, Vol. 11, Issue 48 https://doi.org/10.1021/acsami.9b11365	journal	November 2019
Dictating Pt-Based Electrocatalyst Performance in Polymer Electrolyte Fuel Cells, from Formulation to Application Van Cleve, Tim; Khandavalli, Sunilkumar; Chowdhury, Anamika ACS Applied Materials & Interfaces, Vol. 11, Issue 50 https://doi.org/10.1021/acsami.9b17614	journal	November 2019
Scientific Aspects of Polymer Electrolyte Fuel Cell Durability and Degradation Borup, Rod; Meyers, Jeremy; Pivovar, Bryan Chemical Reviews, Vol. 107, Issue 10 https://doi.org/10.1021/cr050182l	journal	October 2007
Glass Transition Temperature of Perfluorosulfonic Acid Ionomers Osborn, Shawn J.; Hassan, Mohammad K.; Divoux, Gilles M. Macromolecules, Vol. 40, Issue 10 https://doi.org/10.1021/ma062029e	journal	May 2007
Challenges to High-Volume Production of Fuel Cell Materials: Quality Control Ulsh, M.; Sopori, B.; Aieta, N. V. ECS Transactions, Vol. 50, Issue 2 https://doi.org/10.1149/05002.0919ecst	journal	March 2013
Defect Detection in Fuel Cell Gas Diffusion Electrodes Using Infrared Thermography Bittinat, D. C.; Bender, G.; Porter, J. M. ECS Transactions, Vol. 58, Issue 1 https://doi.org/10.1149/05801.0495ecst	journal	August 2013
Effective Electrode Edge Protection for Proton Exchange Membrane Fuel Cell Drive Cycle Operation Wang, Min; Rome, Grace; Phillips, Adam ECS Transactions, Vol. 92, Issue 8 https://doi.org/10.1149/09208.0351ecst	journal	July 2019
Determination of Catalyst Unique Parameters for the Oxygen Reduction Reaction in a PEMFC Neyerlin, K. C.; Gu, Wenbin; Jorne, Jacob Journal of The Electrochemical Society, Vol. 153, Issue 10 https://doi.org/10.1149/1.2266294	journal	January 2006
Gravure Coating for Roll-to-Roll Manufacturing of Proton-Exchange-Membrane Fuel Cell Catalyst Layers Mauger, Scott A.; Neyerlin, K. C.; Yang-Neyerlin, Ami C. Journal of The Electrochemical Society, Vol. 165, Issue 11 https://doi.org/10.1149/2.0091813jes	journal	January 2018
Accelerated Stress Testing of Fuel Cell Membranes Subjected to Combined Mechanical/Chemical Stressors and Cerium Migration Lai, Yeh-Hung; Rahmoeller, Kenneth M.; Hurst, James H. Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0241806jes	journal	January 2018
A Mechanistic Model for Pinhole Growth in Fuel-Cell Membranes during Cyclic Loads Kusoglu, Ahmet; Weber, Adam Z. Journal of The Electrochemical Society, Vol. 161, Issue 8 https://doi.org/10.1149/2.036408jes	journal	January 2014

Similar Records

Impacts of electrode coating irregularities on polymer electrolyte membrane fuel cell lifetime using quasi in-situ infrared thermography and accelerated stress testing

Journal Article · Thu Mar 01 19:00:00 EST 2018 · International Journal of Hydrogen Energy · OSTI ID:1426642

Fabrication of high-performance gas-diffusion-electrode based membrane-electrode assemblies

Journal Article · Tue Jan 28 19:00:00 EST 2020 · Journal of Power Sources · OSTI ID:1603262

Development of high-performance roll-to-roll-coated gas-diffusion-electrode-based fuel cells

Journal Article · Sun Jun 06 20:00:00 EDT 2021 · Journal of Power Sources · OSTI ID:1788428

Related Subjects

08 HYDROGEN
AST
IR
MEA
PEMFC
hot pressing
membrane irregularity

Visualization, understanding, and mitigation of process-induced-membrane irregularities in gas diffusion electrode-based polymer electrolyte membrane fuel cells

Citation Formats

References (56)

Similar Records

Related Subjects