Electrochemical Characterization of Evolving Ionomer/Electrocatalyst Interactions Throughout Accelerated Stress Tests

Hu, Leiming; Van Cleve, Tim; Yu, Haoran; Park, Jae Hyung; Kariuki, Nancy; Kropf, A. Jeremy; Mukundan, Rangchary; Cullen, David A.; Myers, Deborah J.; Neyerlin, Kenneth C.

doi:10.1016/j.jpowsour.2022.232490

Title: Electrochemical Characterization of Evolving Ionomer/Electrocatalyst Interactions Throughout Accelerated Stress Tests

Journal Article · Sat Dec 17 00:00:00 EST 2022 · Journal of Power Sources

DOI:https://doi.org/10.1016/j.jpowsour.2022.232490· OSTI ID:1908593

;

; Yu, Haoran; Park, Jae Hyung; Kariuki, Nancy; Kropf, A. Jeremy; Mukundan, Rangchary; Cullen, David A.; Myers, Deborah J.; Neyerlin, Kenneth C.

The degradation of polymer electrolyte membrane fuel cells (PEMFCs) catalyst layers used for heavy-duty vehicles was examined using a catalyst-specific accelerated stress test (AST). High surface area carbon supported dispersed Pt (Pt/HSC), annealed Pt (a-Pt/HSC) and PtCo (PtCo/HSC) alloy catalysts were examined over the course of 90,000 cycles by measuring changes in mass activity, O2 transport resistance, electrochemical active surface area (ECSA), catalyst accessibility and ionomer-electrocatalyst interactions. Compared to a-Pt/HSC and Pt/HSC catalyst, the PtCo/HSC showed better initial mass activity, a larger initial mass transport loss, and faster degradation after the first 30k AST cycles, as a large portion of Co leached out during potential cycling. Pt/HSC showed higher initial performance relative to a-Pt/HSC but had faster degradation. STEM characterizations show that the ECSA losses are largely related to Pt dissolution resulting in either catalyst particle growth via the Ostwald ripening mechanism or redeposition in the membrane. Catalyst accessibility measurements showed decreased RH sensitivity for all three samples, while CO impedance measurements revealed a decrease in both Pt-water and carbon-water interactions. This implies that, Pt is either preferentially redepositing on the exterior of the carbon support, or that the ionomer is undergoing morphological changes enabling the enhanced intrusion of mesopores.

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

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

DOE Contract Number:: AC36-08GO28308

OSTI ID:: 1908593

Report Number(s):: NREL/JA-5900-84944; MainId:85717; UUID:192f4ccd-bc2e-47bb-abbb-25a65b8b1188; MainAdminID:68406

Journal Information:: Journal of Power Sources, Vol. 556

Country of Publication:: United States

Language:: English

References (36)

Boosting Fuel Cell Performance with Accessible Carbon Mesopores Yarlagadda, Venkata; Carpenter, Michael K.; Moylan, Thomas E. ACS Energy Letters, Vol. 3, Issue 3 https://doi.org/10.1021/acsenergylett.8b00186	journal	February 2018
Recent developments in catalyst-related PEM fuel cell durability Borup, Rodney L.; Kusoglu, Ahmet; Neyerlin, Kenneth C. Current Opinion in Electrochemistry, Vol. 21 https://doi.org/10.1016/j.coelec.2020.02.007	journal	June 2020
Effect of Pt and Ionomer Distribution on Polymer Electrolyte Fuel Cell Performance and Durability Kobayashi, Aki; Fujii, Takahiro; Harada, Chie ACS Applied Energy Materials, Vol. 4, Issue 3 https://doi.org/10.1021/acsaem.0c02841	journal	February 2021
Mitigation of PEM Fuel Cell Catalyst Degradation with Porous Carbon Supports Padgett, Elliot; Yarlagadda, Venkata; Holtz, Megan E. Journal of The Electrochemical Society, Vol. 166, Issue 4 https://doi.org/10.1149/2.0371904jes	journal	January 2019
Instability of Pt∕C Electrocatalysts in Proton Exchange Membrane Fuel Cells Ferreira, P. J.; la O’, G. J.; Shao-Horn, Y. Journal of The Electrochemical Society, Vol. 152, Issue 11 https://doi.org/10.1149/1.2050347	journal	January 2005
Effect of Voltage on Platinum Dissolution Wang, Xiaoping; Kumar, Romesh; Myers, Deborah J. Electrochemical and Solid-State Letters, Vol. 9, Issue 5 https://doi.org/10.1149/1.2180536	journal	January 2006
Studying Pt-based fuel cell electrode degradation with nanoscale X-ray computed tomography Braaten, Jonathan P.; Ogawa, Shohei; Yarlagadda, Venkata Journal of Power Sources, Vol. 478 https://doi.org/10.1016/j.jpowsour.2020.229049	journal	December 2020
Pt Band Formation Enhances the Stability of Fuel Cell Membranes Macauley, N.; Ghassemzadeh, L.; Lim, C. ECS Electrochemistry Letters, Vol. 2, Issue 4 https://doi.org/10.1149/2.007304eel	journal	January 2013
Platinum-Alloy Cathode Catalyst Degradation in Proton Exchange Membrane Fuel Cells: Nanometer-Scale Compositional and Morphological Changes Chen, Shuo; Gasteiger, Hubert A.; Hayakawa, Katsuichiro Journal of The Electrochemical Society, Vol. 157, Issue 1 https://doi.org/10.1149/1.3258275	journal	January 2010
Potential Dependence of Pt and Co Dissolution from Platinum-Cobalt Alloy PEFC Catalysts Using Time-Resolved Measurements Ahluwalia, Rajesh K.; Papadias, Dionissios D.; Kariuki, Nancy N. Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0031806jes	journal	January 2018
Real-time imaging of activation and degradation of carbon supported octahedral Pt–Ni alloy fuel cell catalysts at the nanoscale using in situ electrochemical liquid cell STEM Beermann, Vera; Holtz, Megan E.; Padgett, Elliot Energy & Environmental Science, Vol. 12, Issue 8 https://doi.org/10.1039/C9EE01185D	journal	January 2019
Enthalpies of formation of liquid and solid binary alloys based on 3d metals Niessen, A. K.; Miedema, A. R.; de Boer, F. R. Physica B+C, Vol. 151, Issue 3 https://doi.org/10.1016/0378-4363(88)90296-3	journal	August 1988
High-Current Density Durability of Pt/C and PtCo/C Catalysts at Similar Particle Sizes in PEMFCs Ramaswamy, Nagappan; Kumaraguru, Swami; Gu, Wenbin Journal of The Electrochemical Society, Vol. 168, Issue 2 https://doi.org/10.1149/1945-7111/abe5ea	journal	February 2021
Contaminant Cation Effect on Oxygen Transport through the Ionomers of Polymer Electrolyte Membrane Fuel Cells Braaten, Jonathan P.; Xu, Xiaomin; Cai, Yun Journal of The Electrochemical Society, Vol. 166, Issue 16 https://doi.org/10.1149/2.0671916jes	journal	January 2019
Durability of Pt-Co Alloy Polymer Electrolyte Fuel Cell Cathode Catalysts under Accelerated Stress Tests Papadias, D. D.; Ahluwalia, R. K.; Kariuki, N. Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0171806jes	journal	January 2018
Suppression of oxygen reduction reaction activity on Pt-based electrocatalysts from ionomer incorporation Shinozaki, Kazuma; Morimoto, Yu; Pivovar, Bryan S. Journal of Power Sources, Vol. 325 https://doi.org/10.1016/j.jpowsour.2016.06.062	journal	September 2016
Catalyst Poisoning Property of Sulfonimide Acid Ionomer on Pt (111) Surface Kodama, Kensaku; Shinohara, Akihiro; Hasegawa, Naoki Journal of The Electrochemical Society, Vol. 161, Issue 5 https://doi.org/10.1149/2.051405jes	journal	January 2014
3D Analysis of Fuel Cell Electrocatalyst Degradation on Alternate Carbon Supports Sneed, Brian T.; Cullen, David A.; Reeves, Kimberly S. ACS Applied Materials & Interfaces, Vol. 9, Issue 35 https://doi.org/10.1021/acsami.7b09716	journal	August 2017
Measurement of Oxygen Transport Resistance in PEM Fuel Cells by Limiting Current Methods Baker, Daniel R.; Caulk, David A.; Neyerlin, Kenneth C. Journal of The Electrochemical Society, Vol. 156, Issue 9 https://doi.org/10.1149/1.3152226	journal	January 2009
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
Characterizing Electrolyte and Platinum Interface in PEM Fuel Cells Using CO Displacement Garrick, Taylor R.; Moylan, Thomas E.; Yarlagadda, Venkata Journal of The Electrochemical Society, Vol. 164, Issue 2 https://doi.org/10.1149/2.0551702jes	journal	December 2016
Tailoring electrode microstructure via ink content to enable improved rated power performance for platinum cobalt/high surface area carbon based polymer electrolyte fuel cells Van Cleve, Tim; Wang, Guanxiong; Mooney, Mason Journal of Power Sources, Vol. 482 https://doi.org/10.1016/j.jpowsour.2020.228889	journal	January 2021
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
Tracking Nanoparticle Degradation across Fuel Cell Electrodes by Automated Analytical Electron Microscopy Yu, Haoran; Zachman, Michael J.; Reeves, Kimberly S. ACS Nano, Vol. 16, Issue 8 https://doi.org/10.1021/acsnano.2c02307	journal	July 2022
Ultra-small-angle X-ray scattering at the Advanced Photon Source Ilavsky, Jan; Jemian, Pete R.; Allen, Andrew J. Journal of Applied Crystallography, Vol. 42, Issue 3 https://doi.org/10.1107/S0021889809008802	journal	April 2009
Ultra-Small-Angle X-ray Scattering Instrument at the Advanced Photon Source: History, Recent Development, and Current Status Ilavsky, J.; Zhang, F.; Allen, A. J. Metallurgical and Materials Transactions A, Vol. 44, Issue 1 https://doi.org/10.1007/s11661-012-1431-y	journal	October 2012
Nika : software for two-dimensional data reduction Ilavsky, Jan Journal of Applied Crystallography, Vol. 45, Issue 2 https://doi.org/10.1107/S0021889812004037	journal	March 2012
Degradation of Platinum-Cobalt Alloy PEMFC Cathode Catalysts in Catalyst-Ionomer Inks Myers, Deborah J.; Kropf, A. Jeremy; Wegener, Evan C. Journal of The Electrochemical Society, Vol. 168, Issue 4 https://doi.org/10.1149/1945-7111/abf4ab	journal	April 2021
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Atomic Structure and Composition of “Pt ₃ Co” Nanocatalysts in Fuel Cells: An Aberration-Corrected STEM HAADF Study Patrick, Brian; Ham, Hyung Chul; Shao-Horn, Yang Chemistry of Materials, Vol. 25, Issue 4 https://doi.org/10.1021/cm3029164	journal	February 2013
Relative Humidity Dependence of Pt Utilization in Polymer Electrolyte Fuel Cell Electrodes: Effects of Electrode Thickness, Ionomer-to-Carbon Ratio, Ionomer Equivalent Weight, and Carbon Support Shinozaki, Kazuma; Yamada, Haruhiko; Morimoto, Yu Journal of The Electrochemical Society, Vol. 158, Issue 5 https://doi.org/10.1149/1.3556906	journal	January 2011
The Priority and Challenge of High-Power Performance of Low-Platinum Proton-Exchange Membrane Fuel Cells Kongkanand, Anusorn; Mathias, Mark F. The Journal of Physical Chemistry Letters, Vol. 7, Issue 7 https://doi.org/10.1021/acs.jpclett.6b00216	journal	March 2016
Carbon Corrosion in PEM Fuel Cells and the Development of Accelerated Stress Tests Macauley, Natalia; Papadias, Dennis D.; Fairweather, Joseph Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0061806jes	journal	January 2018
Does an Ionomer Penetrate a Carbon Mesopore? Free-Energy Analysis Using Molecular Dynamics Simulations Kikkawa, Nobuaki; Jinnouchi, Ryosuke The Journal of Physical Chemistry C, Vol. 126, Issue 28 https://doi.org/10.1021/acs.jpcc.2c03845	journal	July 2022
Conductivity and Wettability Changes of Ultrathin Nafion Films Subjected to Thermal Annealing and Liquid Water Exposure Paul, Devproshad K.; Karan, Kunal The Journal of Physical Chemistry C, Vol. 118, Issue 4 https://doi.org/10.1021/jp410510x	journal	January 2014
Investigation of cathode catalyst layer interfaces evolution during accelerated stress tests for polymer electrolyte fuel cells Perego, Andrea; Avid, Arezoo; Mamania, Divija N. Applied Catalysis B: Environmental, Vol. 301 https://doi.org/10.1016/j.apcatb.2021.120810	journal	February 2022

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