Revealing in-plane movement of platinum in polymer electrolyte fuel cells after heavy-duty vehicle lifetime

Khedekar, Kaustubh; Zaffora, Andrea; Santamaria, Monica; Coats, Matthew; Pylypenko, Svitlana; Braaten, Jonathan; Atanassov, Plamen; Tamura, Nobumichi; Cheng, Lei; Johnston, Christina; Zenyuk, Iryna V.

doi:10.1038/s41929-023-00993-6

Revealing in-plane movement of platinum in polymer electrolyte fuel cells after heavy-duty vehicle lifetime

Journal Article · Thu Jul 27 04:00:00 EDT 2023 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-023-00993-6· OSTI ID:2375464

Khedekar, Kaustubh ^[1]; Zaffora, Andrea ^[2]; Santamaria, Monica ^[3]; Coats, Matthew ^[4]; Pylypenko, Svitlana ^[4]; Braaten, Jonathan ^[5]; ^[1]; ^[6]; ^[5]; ^[5]; ^[1]

Univ. of California, Irvine, CA (United States)
Univ. of California, Irvine, CA (United States); University of Palermo (Italy)
University of Palermo (Italy)
Colorado School of Mines, Golden, CO (United States)
Bosch Research and Technology Center North America, Sunnyvale, CA (United States)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Fuel cell heavy-duty vehicles (HDVs) require increased durability of oxygen-reduction-reaction electrocatalysts, making knowledge of realistic degradation mechanisms critical. Here identical-location micro-X-ray fluorescence spectroscopy was performed on membrane electrode assemblies. The results exposed heavy in-plane movement of electrocatalyst after HDV lifetime, suggesting that electrochemical Ostwald ripening may not be a local effect. Development of local loading hotspots and preferential movement of electrocatalyst away from cathode catalyst layer cracks was observed. The heterogeneous degradation exhibited by a modified cathode gas diffusion layer membrane electrode assembly after HDV lifetime was successfully quantified by the identical-location approach. Further synchrotron micro-X-ray diffraction and micro-X-ray fluorescence experiments were performed to obtain the currently unknown correlation between electrocatalyst nanoparticle size increase and loading change. A direct correlation was discovered which developed only after HDV lifetime. Finally, the work provides a route to engineer immediate system-level mitigation strategies and to develop structured cathode catalyst layers with durable electrocatalysts.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 2375464

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 8 Vol. 6; ISSN 2520-1158

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

References (34)

Mapping of Heterogeneous Catalyst Degradation in Polymer Electrolyte Fuel Cells Cheng, Lei; Khedekar, Kaustubh; Rezaei Talarposhti, Morteza Advanced Energy Materials, Vol. 10, Issue 28 https://doi.org/10.1002/aenm.202000623	journal	June 2020
Probing Heterogeneous Degradation of Catalyst in PEM Fuel Cells under Realistic Automotive Conditions with Multi‐Modal Techniques Khedekar, Kaustubh; Rezaei Talarposhti, Morteza; Besli, Münir M. Advanced Energy Materials, Vol. 11, Issue 35 https://doi.org/10.1002/aenm.202101794	journal	July 2021
Operando 3D Visualization of Migration and Degradation of a Platinum Cathode Catalyst in a Polymer Electrolyte Fuel Cell Matsui, Hirosuke; Ishiguro, Nozomu; Uruga, Tomoya Angewandte Chemie International Edition, Vol. 56, Issue 32 https://doi.org/10.1002/anie.201703940	journal	July 2017
Effect of Commercial Gas Diffusion Layers on Catalyst Durability of Polymer Electrolyte Fuel Cells in Varied Cathode Gas Environment Khedekar, Kaustubh; Satjaritanun, Pongsarun; Stewart, Sarah Small, Vol. 18, Issue 33 https://doi.org/10.1002/smll.202201750	journal	July 2022
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
Pt Catalyst Degradation in Aqueous and Fuel Cell Environments studied via In-Operando Anomalous Small-Angle X-ray Scattering Gilbert, James A.; Kariuki, Nancy N.; Wang, Xiaoping Electrochimica Acta, Vol. 173 https://doi.org/10.1016/j.electacta.2015.05.032	journal	August 2015
Effect of porosity and pressure on the PEM fuel cell performance Larbi, Badreddine; Alimi, Wael; Chouikh, Ridha International Journal of Hydrogen Energy, Vol. 38, Issue 20 https://doi.org/10.1016/j.ijhydene.2012.11.022	journal	July 2013
Dependence of PEM fuel cell performance on catalyst loading Gasteiger, H. A.; Panels, J. E.; Yan, S. G. Journal of Power Sources, Vol. 127, Issue 1-2 https://doi.org/10.1016/j.jpowsour.2003.09.013	journal	March 2004
Identical locations transmission electron microscopy study of Pt/C electrocatalyst degradation during oxygen reduction reaction Perez-Alonso, Francisco J.; Elkjær, Christian F.; Shim, Signe S. Journal of Power Sources, Vol. 196, Issue 15 https://doi.org/10.1016/j.jpowsour.2011.03.064	journal	August 2011
Durability of platinum-based fuel cell electrocatalysts: Dissolution of bulk and nanoscale platinum Cherevko, Serhiy; Kulyk, Nadiia; Mayrhofer, Karl J. J. Nano Energy, Vol. 29 https://doi.org/10.1016/j.nanoen.2016.03.005	journal	November 2016
Pt–Co/C Cathode Catalyst Degradation in a Polymer Electrolyte Fuel Cell Investigated by an Infographic Approach Combining Three-Dimensional Spectroimaging and Unsupervised Learning Tan, Yuanyuan; Matsui, Hirosuke; Ishiguro, Nozomu The Journal of Physical Chemistry C, Vol. 123, Issue 31 https://doi.org/10.1021/acs.jpcc.9b05005	journal	July 2019
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
Importance of Chemical Activation and the Effect of Low Operation Voltage on the Performance of Pt-Alloy Fuel Cell Electrocatalysts Gatalo, Matija; Bonastre, Alejandro Martinez; Moriau, Léonard Jean ACS Applied Energy Materials, Vol. 5, Issue 7 https://doi.org/10.1021/acsaem.2c01359	journal	June 2022
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
Recreating Fuel Cell Catalyst Degradation in Aqueous Environments for Identical-Location Scanning Transmission Electron Microscopy Studies Yu, Haoran; Zachman, Michael J.; Li, Chenzhao ACS Applied Materials & Interfaces, Vol. 14, Issue 18 https://doi.org/10.1021/acsami.1c23281	journal	March 2022
Toward a Comprehensive Understanding of Cation Effects in Proton Exchange Membrane Fuel Cells Lee, ChungHyuk; Wang, Xiaohua; Peng, Jui-Kun ACS Applied Materials & Interfaces, Vol. 14, Issue 31 https://doi.org/10.1021/acsami.2c07085	journal	July 2022
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
The Oxygen Reduction Reaction on Pt: Why Particle Size and Interparticle Distance Matter Inaba, Masanori; Zana, Alessandro; Quinson, Jonathan ACS Catalysis, Vol. 11, Issue 12 https://doi.org/10.1021/acscatal.1c00652	journal	June 2021
Tracking the Catalyst Layer Depth-Dependent Electrochemical Degradation of a Bimodal Pt/C Fuel Cell Catalyst: A Combined Operando Small- and Wide-Angle X-ray Scattering Study Schröder, Johanna; Pittkowski, Rebecca K.; Martens, Isaac ACS Catalysis, Vol. 12, Issue 3 https://doi.org/10.1021/acscatal.1c04365	journal	January 2022
Imaging Heterogeneous Electrocatalyst Stability and Decoupling Degradation Mechanisms in Operating Hydrogen Fuel Cells Martens, Isaac; Vamvakeros, Antonis; Martinez, Nicolas ACS Energy Letters, Vol. 6, Issue 8 https://doi.org/10.1021/acsenergylett.1c00718	journal	July 2021
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
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
New roads and challenges for fuel cells in heavy-duty transportation Cullen, David A.; Neyerlin, K. C.; Ahluwalia, Rajesh K. Nature Energy, Vol. 6, Issue 5 https://doi.org/10.1038/s41560-021-00775-z	journal	March 2021
Capabilities and limitations of rotating disk electrodes versus membrane electrode assemblies in the investigation of electrocatalysts Lazaridis, Timon; Stühmeier, Björn M.; Gasteiger, Hubert A. Nature Catalysis, Vol. 5, Issue 5 https://doi.org/10.1038/s41929-022-00776-5	journal	May 2022
Effect of Hydrogen and Oxygen Partial Pressure on Pt Precipitation within the Membrane of PEMFCs Zhang, Jingxin; Litteer, Brian A.; Gu, Wenbin Journal of The Electrochemical Society, Vol. 154, Issue 10 https://doi.org/10.1149/1.2764240	journal	January 2007
Investigating the Particle Growth in Bimodal Pt/C Catalysts by In-Situ Small-Angle X-ray Scattering: Challenges in the Evaluation of Stress Test Protocol-Dependent Degradation Mechanisms Schröder, Johanna; Pittkowski, Rebecca K.; Du, Jia Journal of The Electrochemical Society, Vol. 169, Issue 10 https://doi.org/10.1149/1945-7111/ac99a5	journal	October 2022
Direct Simulations of Pore-Scale Water Transport through Diffusion Media Cetinbas, Firat C.; Ahluwalia, Rajesh K.; Shum, Andrew D. Journal of The Electrochemical Society, Vol. 166, Issue 7 https://doi.org/10.1149/2.0011907jes	journal	January 2019
Cathode Loading Impact on Voltage Cycling Induced PEMFC Degradation: A Voltage Loss Analysis Harzer, Gregor S.; Schwämmlein, Jan N.; Damjanović, Ana Marija Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0161806jes	journal	January 2018
Potentiostatic and Potential Cycling Dissolution of Polycrystalline Platinum and Platinum Nano-Particle Fuel Cell Catalysts Myers, Deborah J.; Wang, Xiaoping; Smith, Matt C. Journal of The Electrochemical Society, Vol. 165, Issue 6 https://doi.org/10.1149/2.0211806jes	journal	January 2018
Effect of Dwell Time and Scan Rate during Voltage Cycling on Catalyst Degradation in PEM Fuel Cells Kneer, Alexander; Wagner, Nadja; Sadeler, Christian Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.0651810jes	journal	January 2018
Influence of the Gas Diffusion Layer Compression on the Oxygen Transport in PEM Fuel Cells at High Water Saturation Levels Simon, Christoph; Hasché, Frédéric; Gasteiger, Hubert A. Journal of The Electrochemical Society, Vol. 164, Issue 6 https://doi.org/10.1149/2.0691706jes	journal	January 2017
The Impact of Potential Cycling on PEMFC Durability Zhang, Hao; Haas, Herwig; Hu, Jingwei Journal of The Electrochemical Society, Vol. 160, Issue 8 https://doi.org/10.1149/2.083308jes	journal	January 2013
Recent Advances in Catalyst Accelerated Stress Tests for Polymer Electrolyte Membrane Fuel Cells Stariha, Sarah; Macauley, Natalia; Sneed, Brian T. Journal of The Electrochemical Society, Vol. 165, Issue 7 https://doi.org/10.1149/2.0881807jes	journal	January 2018
Design criteria for stable Pt/C fuel cell catalysts Meier, Josef C.; Galeano, Carolina; Katsounaros, Ioannis Beilstein Journal of Nanotechnology, Vol. 5 https://doi.org/10.3762/bjnano.5.5	journal	January 2014

Similar Records

Durability of PGM catalyst MEAs of polymer electrolyte membrane fuel cells for heavy-duty vehicles

Journal Article · Thu Mar 06 23:00:00 EST 2025 · Chem Catalysis · OSTI ID:2573268

Pt Nanoparticles on Atomic-Metal-Rich Carbon for Heavy-Duty Fuel Cell Catalysts: Durability Enhancement and Degradation Behavior in Membrane Electrode Assemblies

Journal Article · Thu Aug 24 00:00:00 EDT 2023 · ACS Catalysis · OSTI ID:2224159

Model electrode structures for studies of electrocatalyst degradation.

Conference · Fri Oct 01 00:00:00 EDT 2010 · OSTI ID:1026959

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
chemical engineering
electrocatalysis
fuel cells

Revealing in-plane movement of platinum in polymer electrolyte fuel cells after heavy-duty vehicle lifetime

Citation Formats

References (34)

Similar Records

Related Subjects