Standardized Protocols for Evaluating Platinum Group Metal-Free Oxygen Reduction Reaction Electrocatalysts in Polymer Electrolyte Fuel Cells

Zhang, Hanguang; Osmieri, Luigi; Park, Jae Hyung; Chung, Hoon Taek; Cullen, David A.; Neyerlin, Kenneth C.; Myers, Deborah J.; Zelenay, Piotr

doi:10.1038/s41929-022-00778-3

Standardized Protocols for Evaluating Platinum Group Metal-Free Oxygen Reduction Reaction Electrocatalysts in Polymer Electrolyte Fuel Cells

Journal Article · 09 May 2022 · Nature Catalysis

DOI:https://doi.org/10.1038/s41929-022-00778-3· OSTI ID:1871539

Zhang, Hanguang; Osmieri, Luigi; Park, Jae Hyung; Chung, Hoon Taek; Cullen, David A.; Neyerlin, Kenneth C.; Myers, Deborah J.; Zelenay, Piotr

Platinum group metal (PGM)-free electrocatalysts for the oxygen reduction reaction at the polymer electrolyte fuel cell cathode have shown substantial improvements in activity - especially those derived from transition metals, nitrogen and carbon. However, their stability and durability remain insufficient. A key to enabling future improvements and performance comparisons lies in the development of test protocols that are relevant to the operating conditions of the fuel cell cathode, can be completed within a reasonable time and are ubiquitously adopted. Here we propose and validate such protocols, designed with special attention to typical catalyst degradation mechanisms of PGM-free catalysts. The results of the cross-laboratory validation study using two different catalysts attest to the strength and feasibility of the proposed approach. We hope that the information provided here can serve as a broad and effective platform for assessing the performance and durability of PGM-free catalysts for polymer electrolyte fuel cells.

Research Organization:: National Renewable Energy Laboratory (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:: 1871539

Report Number(s):: NREL/JA-5900-80117; MainId:42320; UUID:a2ac4b3a-4271-4706-bcf4-f62fca6074a0; MainAdminID:64627

Journal Information:: Nature Catalysis, Journal Name: Nature Catalysis Vol. 5

Country of Publication:: United States

Language:: English

References (39)

Microstructural Analysis and Transport Resistances of Low-Platinum-Loaded PEFC Electrodes Cetinbas, Firat C.; Wang, Xiaohua; Ahluwalia, Rajesh K. Journal of The Electrochemical Society, Vol. 164, Issue 14 https://doi.org/10.1149/2.1111714jes	journal	January 2017
Controlling electric double-layer capacitance and pseudocapacitance in heteroatom-doped carbons derived from hypercrosslinked microporous polymers Lee, Jet-Sing M.; Briggs, Michael E.; Hu, Chi-Chang Nano Energy, Vol. 46 https://doi.org/10.1016/j.nanoen.2018.01.042	journal	April 2018
Asymmetric Volcano Trend in Oxygen Reduction Activity of Pt and Non-Pt Catalysts: In Situ Identification of the Site-Blocking Effect Li, Jingkun; Alsudairi, Amell; Ma, Zi-Feng Journal of the American Chemical Society, Vol. 139, Issue 4 https://doi.org/10.1021/jacs.6b11072	journal	January 2017
High-Performance Electrocatalysts for Oxygen Reduction Derived from Polyaniline, Iron, and Cobalt Wu, G.; More, K. L.; Johnston, C. M. Science, Vol. 332, Issue 6028, p. 443-447 https://doi.org/10.1126/science.1200832	journal	April 2011
Titanium dioxide-supported non-precious metal oxygen reduction electrocatalyst Wu, Gang; Nelson, Mark A.; Mack, Nathan H. Chemical Communications, Vol. 46, Issue 40, p. 7489-7491 https://doi.org/10.1039/c0cc03088k	journal	January 2010
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
A Reverse-Current Decay Mechanism for Fuel Cells Reiser, Carl A.; Bregoli, Lawrence; Patterson, Timothy W. Electrochemical and Solid-State Letters, Vol. 8, Issue 6 https://doi.org/10.1149/1.1896466	journal	January 2005
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
Highly stable precious metal-free cathode catalyst for fuel cell application Serov, Alexey; Workman, Michael J.; Artyushkova, Kateryna Journal of Power Sources, Vol. 327 https://doi.org/10.1016/j.jpowsour.2016.07.087	journal	September 2016
Development of Novel Non-Pt Group Metal Electrocatalysts for PEM Fuel Cell Applications Mukerjee, Sanjeev; Atanassov, Plamen; Barton, Scott https://doi.org/10.2172/1332697	report	January 2016
Degradation by Hydrogen Peroxide of Metal-Nitrogen-Carbon Catalysts for Oxygen Reduction Goellner, Vincent; Armel, Vanessa; Zitolo, Andrea Journal of The Electrochemical Society, Vol. 162, Issue 6 https://doi.org/10.1149/2.1091506jes	journal	January 2015
Progress in the Development of Fe‐Based PGM‐Free Electrocatalysts for the Oxygen Reduction Reaction Martinez, Ulises; Komini Babu, Siddharth; Holby, Edward F. Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201806545	journal	December 2018
Iron-based cathode catalyst with enhanced power density in polymer electrolyte membrane fuel cells Proietti, Eric; Jaouen, Frédéric; Lefèvre, Michel Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1427	journal	August 2011
Stability of Fe-N-C Catalysts in Acidic Medium Studied by Operando Spectroscopy Choi, Chang Hyuck; Baldizzone, Claudio; Grote, Jan-Philipp Angewandte Chemie, Vol. 127, Issue 43 https://doi.org/10.1002/ange.201504903	journal	August 2015
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
ElectroCat: DOE's approach to PGM-free catalyst and electrode R&D Thompson, Simon T.; Wilson, Adria R.; Zelenay, Piotr Solid State Ionics, Vol. 319 https://doi.org/10.1016/j.ssi.2018.01.030	journal	June 2018
On the Influence of Oxygen on the Degradation of Fe‐N‐C Catalysts Kumar, Kavita; Dubau, Laetitia; Mermoux, Michel Angewandte Chemie, Vol. 132, Issue 8 https://doi.org/10.1002/ange.201912451	journal	January 2020
Experimental Observation of Redox-Induced Fe–N Switching Behavior as a Determinant Role for Oxygen Reduction Activity Jia, Qingying; Ramaswamy, Nagappan; Hafiz, Hasnain ACS Nano, Vol. 9, Issue 12 https://doi.org/10.1021/acsnano.5b05984	journal	October 2015
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
Direct atomic-level insight into the active sites of a high-performance PGM-free ORR catalyst Chung, Hoon T.; Cullen, David A.; Higgins, Drew Science, Vol. 357, Issue 6350 https://doi.org/10.1126/science.aan2255	journal	August 2017
Measurement of Catalyst Layer Electrolyte Resistance in PEFCs Using Electrochemical Impedance Spectroscopy Makharia, Rohit; Mathias, Mark F.; Baker, Daniel R. Journal of The Electrochemical Society, Vol. 152, Issue 5 https://doi.org/10.1149/1.1888367	journal	January 2005
Critical advancements in achieving high power and stable nonprecious metal catalyst–based MEAs for real-world proton exchange membrane fuel cell applications Banham, Dustin; Kishimoto, Takeaki; Zhou, Yingjie Science Advances, Vol. 4, Issue 3 https://doi.org/10.1126/sciadv.aar7180	journal	March 2018
Platinum group metal-free catalysts boost cost competitiveness of fuel cell vehicles Thompson, Simon T.; Papageorgopoulos, Dimitrios Nature Catalysis, Vol. 2, Issue 7 https://doi.org/10.1038/s41929-019-0291-x	journal	July 2019
Carbon materials for the electrochemical storage of energy in capacitors Frackowiak, Elzbieta; Béguin, François Carbon, Vol. 39, Issue 6, p. 937-950 https://doi.org/10.1016/S0008-6223(00)00183-4	journal	May 2001
Utilizing ink composition to tune bulk-electrode gas transport, performance, and operational robustness for a Fe–N–C catalyst in polymer electrolyte fuel cell Osmieri, Luigi; Wang, Guanxiong; Cetinbas, Firat C. Nano Energy, Vol. 75 https://doi.org/10.1016/j.nanoen.2020.104943	journal	September 2020
Performance of advanced automotive fuel cell systems with heat rejection constraint Ahluwalia, R. K.; Wang, X.; Steinbach, A. J. Journal of Power Sources, Vol. 309 https://doi.org/10.1016/j.jpowsour.2016.01.060	journal	March 2016
Acid Stability and Demetalation of PGM-Free ORR Electrocatalyst Structures from Density Functional Theory: A Model for “Single-Atom Catalyst” Dissolution Holby, Edward F.; Wang, Guofeng; Zelenay, Piotr ACS Catalysis, Vol. 10, Issue 24 https://doi.org/10.1021/acscatal.0c02856	journal	November 2020
Low-PGM and PGM-Free Catalysts for Proton Exchange Membrane Fuel Cells: Stability Challenges and Material Solutions Du, Lei; Prabhakaran, Venkateshkumar; Xie, Xiaohong Advanced Materials https://doi.org/10.1002/adma.201908232	journal	April 2020
A specific demetalation of Fe–N ₄ catalytic sites in the micropores of NC_Ar + NH ₃ is at the origin of the initial activity loss of the highly active Fe/N/C catalyst used for the reduction of oxygen in PEM fuel cells Chenitz, Régis; Kramm, Ulrike I.; Lefèvre, Michel Energy & Environmental Science, Vol. 11, Issue 2 https://doi.org/10.1039/C7EE02302B	journal	January 2018
Ionic Conductivity of PEMFC Electrodes Li, Guangchun; Pickup, Peter G. Journal of The Electrochemical Society, Vol. 150, Issue 11 https://doi.org/10.1149/1.1611493	journal	January 2003
Stability of Atomically Dispersed Fe–N–C ORR Catalyst in Polymer Electrolyte Fuel Cell Environment Ahluwalia, R. K.; Wang, X.; Osmieri, L. Journal of The Electrochemical Society, Vol. 168, Issue 2 https://doi.org/10.1149/1945-7111/abe34c	journal	February 2021
PGM‐Free Cathode Catalysts for PEM Fuel Cells: A Mini‐Review on Stability Challenges Shao, Yuyan; Dodelet, Jean‐Pol; Wu, Gang Advanced Materials, Vol. 31, Issue 31 https://doi.org/10.1002/adma.201807615	journal	December 2018
Durability evaluation of a Fe–N–C catalyst in polymer electrolyte fuel cell environment via accelerated stress tests Osmieri, Luigi; Cullen, David A.; Chung, Hoon T. Nano Energy, Vol. 78 https://doi.org/10.1016/j.nanoen.2020.105209	journal	December 2020
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
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
Reactivity Descriptors for the Activity of Molecular MN4 Catalysts for the Oxygen Reduction Reaction Zagal, José H.; Koper, Marc T. M. Angewandte Chemie International Edition, Vol. 55, Issue 47 https://doi.org/10.1002/anie.201604311	journal	September 2016
Systems Strategies to Mitigate Carbon Corrosion in Fuel Cells Perry, Mike L.; Patterson, Timothy; Reiser, Carl 210th ECS Meeting, ECS Transactions https://doi.org/10.1149/1.2356198	conference	January 2006
The Achilles' heel of iron-based catalysts during oxygen reduction in an acidic medium Choi, Chang Hyuck; Lim, Hyung-Kyu; Chung, Min Wook Energy & Environmental Science, Vol. 11, Issue 11 https://doi.org/10.1039/C8EE01855C	journal	January 2018
Status and challenges for the application of platinum group metal-free catalysts in proton-exchange membrane fuel cells Osmieri, Luigi; Park, Jaehyung; Cullen, David A. Current Opinion in Electrochemistry, Vol. 25 https://doi.org/10.1016/j.coelec.2020.08.009	journal	February 2021

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DIRECT ENERGY CONVERSION
catalysts
oxygen reduction reaction
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Standardized Protocols for Evaluating Platinum Group Metal-Free Oxygen Reduction Reaction Electrocatalysts in Polymer Electrolyte Fuel Cells

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