Impact of Polymer Electrolyte Membrane Degradation Products on Oxygen Reduction Reaction Activity for Platinum Electrocatalysts
Abstract
The impact of model membrane degradation compounds on the relevant electrochemical parameters for the oxygen reduction reaction (i.e. electrochemical surface area and catalytic activity), was studied for both polycrystalline Pt and carbon supported Pt electrocatalysts. Model compounds, representing previously published, experimentally determined polymer electrolyte membrane degradation products, were in the form of perfluorinated organic acids that contained combinations of carboxylic and/or sulfonic acid functionality. Perfluorinated carboxylic acids of carbon chain length C1 – C6 were found to have an impact on electrochemical surface area (ECA). The longest chain length acid also hindered the observed oxygen reduction reaction (ORR) performance, resulting in a 17% loss in kinetic current (determined at 0.9 V). Model compounds containing sulfonic acid functional groups alone did not show an effect on Pt ECA or ORR activity. Lastly, greater than a 44% loss in ORR activity at 0.9V was observed for diacid model compounds DA-Naf (perfluoro(2-methyl-3-oxa-5-sulfonic pentanoic) acid) and DA-3M (perfluoro(4-sulfonic butanoic) acid), which contained both sulfonic and carboxylic acid functionalities.
- Authors:
-
- Colorado School of Mines, Golden, CO (United States). Dept. of Chemistry and Geochemistry
- National Renewable Energy Lab. (NREL), Golden, CO (United States). Chemical Materials and Science Center
- Publication Date:
- Research Org.:
- National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office
- OSTI Identifier:
- 1170308
- Report Number(s):
- NREL/JA-5900-62449
Journal ID: ISSN 0013-4651; MainId:21616;UUID:c173831a-c511-e411-8d7c-d89d67132a6d;MainAdminID:10092
- Grant/Contract Number:
- AC36-08GO28308; ZGB-0-4-647-1
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the Electrochemical Society
- Additional Journal Information:
- Journal Volume: 161; Journal Issue: 14; Journal ID: ISSN 0013-4651
- Publisher:
- The Electrochemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 30 DIRECT ENERGY CONVERSION; 36 MATERIALS SCIENCE; electrochemical; electrocatalysts; polymer electrolyte membrane fuel cells
Citation Formats
Christ, J. M., Neyerlin, K. C., Wang, H., Richards, R., and Dinh, H. N. Impact of Polymer Electrolyte Membrane Degradation Products on Oxygen Reduction Reaction Activity for Platinum Electrocatalysts. United States: N. p., 2014.
Web. doi:10.1149/2.0921414jes.
Christ, J. M., Neyerlin, K. C., Wang, H., Richards, R., & Dinh, H. N. Impact of Polymer Electrolyte Membrane Degradation Products on Oxygen Reduction Reaction Activity for Platinum Electrocatalysts. United States. https://doi.org/10.1149/2.0921414jes
Christ, J. M., Neyerlin, K. C., Wang, H., Richards, R., and Dinh, H. N. Thu .
"Impact of Polymer Electrolyte Membrane Degradation Products on Oxygen Reduction Reaction Activity for Platinum Electrocatalysts". United States. https://doi.org/10.1149/2.0921414jes. https://www.osti.gov/servlets/purl/1170308.
@article{osti_1170308,
title = {Impact of Polymer Electrolyte Membrane Degradation Products on Oxygen Reduction Reaction Activity for Platinum Electrocatalysts},
author = {Christ, J. M. and Neyerlin, K. C. and Wang, H. and Richards, R. and Dinh, H. N.},
abstractNote = {The impact of model membrane degradation compounds on the relevant electrochemical parameters for the oxygen reduction reaction (i.e. electrochemical surface area and catalytic activity), was studied for both polycrystalline Pt and carbon supported Pt electrocatalysts. Model compounds, representing previously published, experimentally determined polymer electrolyte membrane degradation products, were in the form of perfluorinated organic acids that contained combinations of carboxylic and/or sulfonic acid functionality. Perfluorinated carboxylic acids of carbon chain length C1 – C6 were found to have an impact on electrochemical surface area (ECA). The longest chain length acid also hindered the observed oxygen reduction reaction (ORR) performance, resulting in a 17% loss in kinetic current (determined at 0.9 V). Model compounds containing sulfonic acid functional groups alone did not show an effect on Pt ECA or ORR activity. Lastly, greater than a 44% loss in ORR activity at 0.9V was observed for diacid model compounds DA-Naf (perfluoro(2-methyl-3-oxa-5-sulfonic pentanoic) acid) and DA-3M (perfluoro(4-sulfonic butanoic) acid), which contained both sulfonic and carboxylic acid functionalities.},
doi = {10.1149/2.0921414jes},
journal = {Journal of the Electrochemical Society},
number = 14,
volume = 161,
place = {United States},
year = {Thu Oct 30 00:00:00 EDT 2014},
month = {Thu Oct 30 00:00:00 EDT 2014}
}
Web of Science
Works referenced in this record:
Scientific Aspects of Polymer Electrolyte Fuel Cell Durability and Degradation
journal, October 2007
- Borup, Rod; Meyers, Jeremy; Pivovar, Bryan
- Chemical Reviews, Vol. 107, Issue 10
Carbon monoxide poisoning of proton exchange membrane fuel cells
journal, January 2001
- Baschuk, J. J.; Li, Xianguo
- International Journal of Energy Research, Vol. 25, Issue 8
Assessing durability of cathodes exposed to common air impurities
journal, November 2004
- Mohtadi, R.; Lee, W. -k.; Van Zee, J. W.
- Journal of Power Sources, Vol. 138, Issue 1-2
Influence of Formic Acid Impurity on Proton Exchange Membrane Fuel Cell Performance
journal, January 2010
- Zhang, Xiaoyu; Galindo, Hugo M.; Garces, Hector F.
- Journal of The Electrochemical Society, Vol. 157, Issue 3
Influence of ammonia on membrane-electrode assemblies in polymer electrolyte fuel cells
journal, November 2009
- Zhang, Xiaoyu; Pasaogullari, Ugur; Molter, Trent
- International Journal of Hydrogen Energy, Vol. 34, Issue 22
Impact of Sulfur Dioxide on the Oxygen Reduction Reaction at Pt/Vulcan Carbon Electrocatalysts
journal, January 2007
- Garsany, Yannick; Baturina, Olga A.; Swider-Lyons, Karen E.
- Journal of The Electrochemical Society, Vol. 154, Issue 7
Effect, mechanism and recovery of nitrogen oxides poisoning on oxygen reduction reaction at Pt/C catalysts
journal, January 2011
- Chen, Meng; Du, Chunyu; Zhang, Jing
- Journal of Power Sources, Vol. 196, Issue 2
A review of PEM hydrogen fuel cell contamination: Impacts, mechanisms, and mitigation
journal, March 2007
- Cheng, Xuan; Shi, Zheng; Glass, Nancy
- Journal of Power Sources, Vol. 165, Issue 2
Assessing the adaptability to varying fuel supply of an autothermal reformer
journal, September 2008
- Nilsson, Marita; Karatzas, Xanthias; Lindström, Bård
- Chemical Engineering Journal, Vol. 142, Issue 3
The effects of mine conditions on the performance of a PEM fuel cell
journal, July 2004
- Bétournay, Marc C.; Bonnell, Gary; Edwardson, Eric
- Journal of Power Sources, Vol. 134, Issue 1
Degradation of polymer electrolyte fuel cells under the existence of anion species
journal, May 2008
- Matsuoka, Koji; Sakamoto, Shigeru; Nakato, Kunihiro
- Journal of Power Sources, Vol. 179, Issue 2
Effects of chlorides on the performance of proton exchange membrane fuel cells
journal, May 2011
- Yan, Wei-Mon; Chu, Hsin-Sen; Liu, You-Lun
- International Journal of Hydrogen Energy, Vol. 36, Issue 9
Influence of toluene contamination at the hydrogen Pt/C anode in a proton exchange membrane fuel cell
journal, November 2010
- Kortsdottir, Katrin; Lindström, Rakel W.; Åkermark, Torbjörn
- Electrochimica Acta, Vol. 55, Issue 26
A comparative study on the adsorption of benzyl alcohol, toluene and benzene on platinum
journal, August 2000
- Rodrı́guez, José Luis; Pastor, Elena
- Electrochimica Acta, Vol. 45, Issue 25-26
Polymer electrolyte membrane fuel cell contamination: Testing and diagnosis of toluene-induced cathode degradation
journal, October 2008
- Li, Hui; Zhang, Jianlu; Fatih, Khalid
- Journal of Power Sources, Vol. 185, Issue 1
PEMFC contamination model: Foreign cation exchange with ionomer protons
journal, August 2011
- St-Pierre, Jean
- Journal of Power Sources, Vol. 196, Issue 15
Contaminant absorption and conductivity in polymer electrolyte membranes
journal, August 2005
- Kelly, Michael J.; Fafilek, Günter; Besenhard, Jürgen O.
- Journal of Power Sources, Vol. 145, Issue 2
In situ metal ion contamination and the effects on proton exchange membrane fuel cell performance
journal, November 2011
- Sulek, Mark; Adams, Jim; Kaberline, Steve
- Journal of Power Sources, Vol. 196, Issue 21
PEM fuel cell cathode contamination in the presence of cobalt ion (Co2+)
journal, August 2010
- Li, Hui; Gazzarri, Javier; Tsay, Ken
- Electrochimica Acta, Vol. 55, Issue 20
Durability of PEM fuel cell cathode in the presence of Fe3+ and Al3+
journal, December 2010
- Li, Hui; Tsay, Ken; Wang, Haijiang
- Journal of Power Sources, Vol. 195, Issue 24
Effect of cation contamination and hydrated pressure loading on the mechanical properties of proton exchange membranes
journal, April 2011
- Jia, Ruiliang; Han, Binghong; Levi, Kemal
- Journal of Power Sources, Vol. 196, Issue 8
Impact of Structural Plastics as Balance of Plant Components on Proton Exchange Membrane Fuel Cell Performance
journal, August 2013
- Yu, P. T.; Bonn, E. A.; Lakshmanan, B.
- ECS Transactions, Vol. 58, Issue 1
Understanding the effects of Contaminants from Balance of Plant Assembly Aids Materials on PEMFCs -In Situ Studies
journal, March 2013
- Opu, M. S.; Ohashi, M.; Cho, H. -S.
- ECS Transactions, Vol. 50, Issue 2
Characterizing Polymeric Leachants for Potential System Contaminants of Fuel Cells
journal, October 2010
- Macomber, Clay; Wang, Heli; O'Neill, Kevin
- ECS Transactions, Vol. 33, Issue 1
Evaluating Polymeric Materials as Potential Sources of PEMFC System Contaminants
conference, January 2010
- Wang, Heli; Coombs, Sidney; Macomber, Clay
- 218th ECS Meeting, ECS Transactions
The Effect on PEMFC Contamination of Functional Groups of Some Organic Contaminants
journal, October 2011
- Cho, Hyun-Seok; Ohashi, Masato; Van Zee, J. W.
- ECS Transactions, Vol. 41, Issue 1
Characterizing Leachant Contaminants from Fuel Cell Assembly Aids, a Prelude to Effects on Performance
journal, March 2013
- Macomber, C. S.; Christ, J.; Wang, H.
- ECS Transactions, Vol. 50, Issue 2
Evaluation of PEMFC System Contaminants on the Performance of Pt Catalyst Via Cyclic Voltammetry
journal, March 2013
- Wang, H.; Macomber, C. S.; Dinh, H. N.
- ECS Transactions, Vol. 50, Issue 2
Evaluating the Influence of PEMFC System Contaminants on the Performance of Pt Catalyst via Cyclic Voltammetry
journal, October 2013
- Wang, Heli; Macomber, Clay; Christ, Jason
- Electrocatalysis, Vol. 5, Issue 1
Chemical Durability Studies of Perfluorinated Sulfonic Acid Polymers and Model Compounds under Mimic Fuel Cell Conditions
journal, November 2007
- Zhou, Chun; Guerra, Miguel A.; Qiu, Zai-Ming
- Macromolecules, Vol. 40, Issue 24
Chemical Degradation of Nafion Membranes under Mimic Fuel Cell Conditions as Investigated by Solid-State NMR Spectroscopy
journal, August 2010
- Ghassemzadeh, Lida; Kreuer, Klaus-Dieter; Maier, Joachim
- The Journal of Physical Chemistry C, Vol. 114, Issue 34
Aspects of the Chemical Degradation of PFSA Ionomers used in PEM Fuel Cells
journal, April 2005
- Healy, J.; Hayden, C.; Xie, T.
- Fuel Cells, Vol. 5, Issue 2
The Development of New Membranes for Proton Exchange Membrane Fuel Cells
conference, January 2007
- Emery, Mike; Frey, Matthew; Guerra, Mike
- 212th ECS Meeting, ECS Transactions
The effects of anions on hydrogen electrosorption on platinum single-crystal electrodes
journal, December 1986
- Markovic, N.; Hanson, M.; McDougall, G.
- Journal of Electroanalytical Chemistry and Interfacial Electrochemistry, Vol. 214, Issue 1-2
Oxygen reduction reaction on Pt(111): effects of bromide
journal, June 1999
- Marković, N. M.; Gasteiger, H. A.; Grgur, B. N.
- Journal of Electroanalytical Chemistry, Vol. 467, Issue 1-2
Structure-relationships in electrocatalysis: oxygen reduction and hydrogen oxidation reactions on Pt(111) and Pt(100) in solutions containing chloride ions
journal, March 2001
- Stamenkovic, V.; M. Markovic, N.; Ross, P. N.
- Journal of Electroanalytical Chemistry, Vol. 500, Issue 1-2
The oxygen reduction reaction on a Pt/carbon fuel cell catalyst in the presence of chloride anions
journal, July 2001
- Schmidt, T. J.; Paulus, U. A.; Gasteiger, H. A.
- Journal of Electroanalytical Chemistry, Vol. 508, Issue 1-2
Degradation Study of PFSA Polymer Electrolytes: Approach from Decomposition Product Analysis
journal, May 2009
- Takasaki, Mari; Nakagawa, Yoshitsugu; Sakiyama, Yoko
- ECS Transactions, Vol. 17, Issue 1
Site-Specific vs Specific Adsorption of Anions on Pt and Pt-Based Alloys
journal, July 2007
- Teliska, Maggie; Murthi, Vivek S.; Mukerjee, Sanjeev
- The Journal of Physical Chemistry C, Vol. 111, Issue 26
Voltammetric characterization of Pt single crystal electrodes with basal orientations in trifluoromethanesulphonic acid
journal, November 2008
- Berná, A.; Feliu, J. M.; Gancs, L.
- Electrochemistry Communications, Vol. 10, Issue 11
Potential-Dependent Adsorption and Desorption of Perfluorosulfonated Ionomer on a Platinum Electrode Surface Probed by Electrochemical Quartz Crystal Microbalance and Atomic Force Microscopy
journal, July 2013
- Masuda, Takuya; Sonsudin, Faridah; Singh, Pankaj R.
- The Journal of Physical Chemistry C, Vol. 117, Issue 30
Three Phase Interfaces at Electrified Metal−Solid Electrolyte Systems 1. Study of the Pt( hkl )−Nafion Interface
journal, April 2010
- Subbaraman, Ram; Strmcnik, Dusan; Stamenkovic, Vojislav
- The Journal of Physical Chemistry C, Vol. 114, Issue 18
Oxygen Reduction Reaction at Three-Phase Interfaces
journal, July 2010
- Subbaraman, Ram; Strmcnik, Dusan; Paulikas, Arvydas P.
- ChemPhysChem, Vol. 11, Issue 13
Ethanol, Acetaldehyde and Acetic Acid Adsorption/Electrooxidation on a Pt Thin Film Electrode under Continuous Electrolyte Flow: An in Situ ATR-FTIRS Flow Cell Study
journal, May 2010
- Heinen, M.; Jusys, Z.; Behm, R. J.
- The Journal of Physical Chemistry C, Vol. 114, Issue 21
An FTIR study on the adsorption of acetate at the basal planes of platinum single-crystal electrodes
journal, October 1994
- Rodes, A.; Pastor, E.; Iwasita, T.
- Journal of Electroanalytical Chemistry, Vol. 376, Issue 1-2
Spectroscopic investigations on the adsorption of trifluoracetate at Pt(100), Pt(110) and Pt(111)
journal, March 1996
- Pastor, E.; Rodes, A.; Iwasita, T.
- Journal of Electroanalytical Chemistry, Vol. 404, Issue 1
Study of acetate adsorption at the platinum electrode/acid electrolyte interface using “blocking effects”: Influences of acetate adsorption on ethanol fuel cell electrodes
journal, March 2012
- Gilman, S.
- Electrochimica Acta, Vol. 65
Influence of Adsorbate Ordering on Rates of UV Photooxidation of Self-Assembled Monolayers
journal, January 1996
- Hutt, David A.; Leggett, Graham J.
- The Journal of Physical Chemistry, Vol. 100, Issue 16
Static Secondary Ion Mass Spectrometry Studies of Self-Assembled Monolayers: Influence of Adsorbate Chain Length and Terminal Functional Group on Rates of Photooxidation of Alkanethiols on Gold
journal, August 1998
- Cooper, Elaine; Leggett, Graham J.
- Langmuir, Vol. 14, Issue 17
Effect of Chain Length on the Protection of Copper by n -Alkanethiols
journal, October 1998
- Jennings, G. Kane; Munro, Jeffrey C.; Yong, Tseh-Hwan
- Langmuir, Vol. 14, Issue 21
Functionalized Self-Assembled Alkanethiol Monolayers on Au(111) Electrodes: 1. Surface Structure and Electrochemistry
journal, February 2001
- Esplandiú, M. J.; Hagenström, H.; Kolb, D. M.
- Langmuir, Vol. 17, Issue 3
The role of non-covalent interactions in electrocatalytic fuel-cell reactions on platinum
journal, August 2009
- Strmcnik, D.; Kodama, K.; van der Vliet, D.
- Nature Chemistry, Vol. 1, Issue 6
Influence of Tail-Group Hydrogen Bonding on the Stabilities of Self-Assembled Monolayers of Alkylthiols on Gold
journal, February 1999
- Cooper, Elaine; Leggett, Graham J.
- Langmuir, Vol. 15, Issue 4
Influence of Nafion® film on oxygen reduction reaction and hydrogen peroxide formation on Pt electrode for proton exchange membrane fuel cell
journal, December 2010
- Ohma, Atsushi; Fushinobu, Kazuyoshi; Okazaki, Ken
- Electrochimica Acta, Vol. 55, Issue 28
Works referencing / citing this record:
Chemical Stability of Perfluorobis(sulfonyl)imide-Acid (PFIA) Ionomers in Open Circuit Voltage (OCV) Accelerated Test Conditions
journal, January 2018
- Yandrasits, Michael; Lindell, Matthew; Peppin, Daniel
- Journal of The Electrochemical Society, Vol. 165, Issue 6
Adsorption Characteristics of Perfluorosulfonic Acid Membrane Decomposition Products on a Platinum Electrode: An EQCM Study
journal, January 2018
- Christ, Jason M.; Staub, Charles B.; Richards, Ryan
- Journal of The Electrochemical Society, Vol. 165, Issue 13