Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination

Banas, Charles J.; Uddin, Md. Aman; Park, Jaehyung; Bonville, Leonard J.; Pasaogullari, Ugur

doi:10.1149/2.0021806jes

Title: Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination

Abstract

Four hundred hour fuel cell tests were performed on commercial, as-received and Ca²⁺ contaminated catalyst coated membranes (CCMs) to evaluate the effects of long term exposure of foreign cations on fuel cell performance and degradation. Following testing, significant thinning of the cathode catalyst layer was observed across the entire active area in the contaminated cell, while only localized thinning was observed in the as-received baseline CCM. Analysis of the elemental maps and line intensity profiles of platinum (Pt) obtained from energy dispersive X-ray spectrum (EDX) shows minimal change in total platinum content across the thickness of the catalyst layer, and hence loss of carbon is suspected to be the cause of the thinning. A numerical model is employed to show the foreign cation redistribution during testing, which shows proton depletion in the cathode catalyst layer when the CCM is contaminated with foreign cations. We hypothesize that this lack of protons leads to accelerated carbon corrosion in the cathode to supply protons to oxygen reduction where foreign cations block transport of protons. Here, a carbon corrosion scheme is presented which shows that under the operating potentials of the cell, carbon oxidation can occur, leading to the observed thinning.

Authors:

; Uddin, Md. Aman; Park, Jaehyung; Bonville, Leonard J.; Pasaogullari, Ugur

Publication Date:: Fri Feb 09 00:00:00 EST 2018

Research Org.:: Univ. of Hawaii, Honolulu, HI (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

OSTI Identifier:: 1420205

Alternate Identifier(s):: OSTI ID: 1509896

Grant/Contract Number:: EE0000467

Resource Type:: Published Article

Journal Name:: Journal of the Electrochemical Society

Additional Journal Information:: Journal Name: Journal of the Electrochemical Society Journal Volume: 165 Journal Issue: 6; Journal ID: ISSN 0013-4651

Publisher:: The Electrochemical Society

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE; Carbon Corrosion; Catalyst Layer Thinning; Cation Contamination

Citation Formats


                    Banas, Charles J., Uddin, Md. Aman, Park, Jaehyung, Bonville, Leonard J., and Pasaogullari, Ugur. Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination.  United States: N. p., 2018. 
Web.  doi:10.1149/2.0021806jes.

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                    Banas, Charles J., Uddin, Md. Aman, Park, Jaehyung, Bonville, Leonard J., & Pasaogullari, Ugur. Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination.  United States.  https://doi.org/10.1149/2.0021806jes

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                    Banas, Charles J., Uddin, Md. Aman, Park, Jaehyung, Bonville, Leonard J., and Pasaogullari, Ugur. Fri .  
"Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination".  United States.  https://doi.org/10.1149/2.0021806jes.

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@article{osti_1420205,

  title        = {Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination},

  author       = {Banas, Charles J. and Uddin, Md. Aman and Park, Jaehyung and Bonville, Leonard J. and Pasaogullari, Ugur},

  abstractNote = {Four hundred hour fuel cell tests were performed on commercial, as-received and Ca2+ contaminated catalyst coated membranes (CCMs) to evaluate the effects of long term exposure of foreign cations on fuel cell performance and degradation. Following testing, significant thinning of the cathode catalyst layer was observed across the entire active area in the contaminated cell, while only localized thinning was observed in the as-received baseline CCM. Analysis of the elemental maps and line intensity profiles of platinum (Pt) obtained from energy dispersive X-ray spectrum (EDX) shows minimal change in total platinum content across the thickness of the catalyst layer, and hence loss of carbon is suspected to be the cause of the thinning. A numerical model is employed to show the foreign cation redistribution during testing, which shows proton depletion in the cathode catalyst layer when the CCM is contaminated with foreign cations. We hypothesize that this lack of protons leads to accelerated carbon corrosion in the cathode to supply protons to oxygen reduction where foreign cations block transport of protons. Here, a carbon corrosion scheme is presented which shows that under the operating potentials of the cell, carbon oxidation can occur, leading to the observed thinning.},

  doi          = {10.1149/2.0021806jes},

  journal      = {Journal of the Electrochemical Society},

  number       = 6,

  volume       = 165,

  place        = {United States},

  year         = {Fri Feb 09 00:00:00 EST 2018},

  month        = {Fri Feb 09 00:00:00 EST 2018}

}

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Title: Thinning of Cathode Catalyst Layer in Polymer Electrolyte Fuel Cells Due to Foreign Cation Contamination

Abstract

Citation Formats

Kinetic model of the electrochemical oxidation of graphitic carbon in acidic environments journal, January 2009

Carbon Corrosion in PEM Fuel Cell Dead-Ended Anode Operations journal, January 2011

Effect of Chloride on PEFCs in Presence of Various Cations journal, January 2015

Conductivity of polymer electrolyte membranes by impedance spectroscopy with microelectrodes journal, August 2005

Theory for water management in membranes for polymer electrolyte fuel cells journal, April 1999

Modeling the steady-state effects of cationic contamination on polymer electrolyte membranes journal, February 2009

A Carbon Corrosion Model to Evaluate the Effect of Steady State and Transient Operation of a Polymer Electrolyte Membrane Fuel Cell journal, January 2013

Degradation of polymer electrolyte membranes journal, October 2006

Fuel Cell Perfluorinated Sulfonic Acid Membrane Degradation Correlating Accelerated Stress Testing and Lifetime journal, September 2012

Modeling the cation transport in an operating polymer electrolyte fuel cell (PEFC) journal, June 2010

Effect of cationic contaminants on polymer electrolyte fuel cell performance journal, July 2015

Scientific Aspects of Polymer Electrolyte Fuel Cell Durability and Degradation journal, October 2007

Cation and Water Diffusion in Nafion Ion Exchange Membranes: Influence of Polymer Structure journal, January 1981

Theory for water management in membranes for polymer electrolyte fuel cells journal, April 1999

Effect of Al 3+ Contaminant on Polymer Electrolyte Fuel Cell Performance journal, January 2013

Ion and Water Transport Characteristics in Membranes for Polymer Electrolyte Fuel Cells Containing H[sup +] and Ca[sup 2+] Cations journal, January 1997

Investigation of Pt catalytic effects on carbon support corrosion of the cathode catalyst in PEM fuel cells using DEMS spectra journal, June 2009

Ca 2+ as an Air Impurity in Polymer Electrolyte Membrane Fuel Cells journal, January 2014

A Comprehensive Model for Carbon Corrosion during Fuel Cell Start-Up journal, January 2015

Mechanisms of Ion and Water Transport in Perfluorosulfonated Ionomer Membranes for Fuel Cells journal, October 2004

Understanding the mechanism of membrane electrode assembly degradation by carbon corrosion by analyzing the microstructural changes in the cathode catalyst layers and polarization losses in proton exchange membrane fuel cell journal, November 2012

Study of Self-Diffusion of Monovalent and Divalent Cations in Nafion-117 Ion-Exchange Membrane journal, September 2001

Computational Modeling of Foreign Cation Contamination in PEFCs journal, January 2014

Cationic Contamination Effects on Polymer Electrolyte Membrane Fuel Cell Performance journal, January 2011

Distributed cation contamination from cathode to anode direction in polymer electrolyte fuel cells journal, October 2015

Carbon Corrosion in PEM Fuel Cells during Drive Cycle Operation journal, September 2015

Carbon corrosion induced by membrane failure: The weak link of PEMFC long-term performance journal, December 2014

Polymer Electrolyte Fuel Cell Model journal, January 1991

The influence of metal ions on the conductivity of Nafion 112 in polymer electrolyte membrane fuel cell journal, September 2008

Diffusion of ions in sea water and in deep-sea sediments journal, May 1974

Durability of PEM fuel cell cathode in the presence of Fe3+ and Al3+ journal, December 2010

Distributed effects of calcium ion contaminant on polymer electrolyte fuel cell performance journal, November 2015

The Effect of Impurity Cations on the Transport Characteristics of Perfluorosulfonated Ionomer Membranes journal, April 1999

PEMFC contaminant tolerance limit – Foreign cations in ionomers journal, May 2011

Accelerated Testing of Carbon Corrosion and Membrane Degradation in PEM Fuel Cells journal, March 2013

Evaluation of cathode contamination with Ca2+ in proton exchange membrane fuel cells journal, January 2018

The Maxwell-Stefan approach to mass transfer journal, March 1997

Transport and equilibrium properties of Nafion® membranes with H+ and Na+ ions journal, January 1998

A review of PEM hydrogen fuel cell contamination: Impacts, mechanisms, and mitigation journal, March 2007

Effect of hydrophobicity of gas diffusion layer in calcium cation contamination in polymer electrolyte fuel cells journal, September 2016

Effect of cations (Na+, Ca2+, Fe3+) on the conductivity of a Nafion membrane journal, November 2010

On the Maxwell−Stefan Approach to Diffusion: A General Resolution in the Transient Regime for One-Dimensional Systems journal, January 2010

Ion and water transport characteristics of Nafion membranes as electrolytes journal, August 1998

A Half Cell Model to Study Performance Degradation of a PEMFC due to Cationic Contamination conference, January 2007

Nafion degradation in PEFCs from end plate iron contamination journal, May 2003

In situ metal ion contamination and the effects on proton exchange membrane fuel cell performance journal, November 2011

Permeability of solutes through hydrated polymer membranes. Part I. Diffusion of sodium chloride journal, November 1968

Contaminant absorption and conductivity in polymer electrolyte membranes journal, August 2005

Kinetic model of the electrochemical oxidation of graphitic carbon in acidic environments
journal, January 2009

Carbon Corrosion in PEM Fuel Cell Dead-Ended Anode Operations
journal, January 2011

Effect of Chloride on PEFCs in Presence of Various Cations
journal, January 2015

Conductivity of polymer electrolyte membranes by impedance spectroscopy with microelectrodes
journal, August 2005

Theory for water management in membranes for polymer electrolyte fuel cells
journal, April 1999

Modeling the steady-state effects of cationic contamination on polymer electrolyte membranes
journal, February 2009

A Carbon Corrosion Model to Evaluate the Effect of Steady State and Transient Operation of a Polymer Electrolyte Membrane Fuel Cell
journal, January 2013

Degradation of polymer electrolyte membranes
journal, October 2006

Fuel Cell Perfluorinated Sulfonic Acid Membrane Degradation Correlating Accelerated Stress Testing and Lifetime
journal, September 2012

Modeling the cation transport in an operating polymer electrolyte fuel cell (PEFC)
journal, June 2010

Effect of cationic contaminants on polymer electrolyte fuel cell performance
journal, July 2015

Scientific Aspects of Polymer Electrolyte Fuel Cell Durability and Degradation
journal, October 2007

Cation and Water Diffusion in Nafion Ion Exchange Membranes: Influence of Polymer Structure
journal, January 1981

Theory for water management in membranes for polymer electrolyte fuel cells
journal, April 1999

Effect of Al ³⁺ Contaminant on Polymer Electrolyte Fuel Cell Performance
journal, January 2013

Ion and Water Transport Characteristics in Membranes for Polymer Electrolyte Fuel Cells Containing H[sup +] and Ca[sup 2+] Cations
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Investigation of Pt catalytic effects on carbon support corrosion of the cathode catalyst in PEM fuel cells using DEMS spectra
journal, June 2009

Ca ²⁺ as an Air Impurity in Polymer Electrolyte Membrane Fuel Cells
journal, January 2014

A Comprehensive Model for Carbon Corrosion during Fuel Cell Start-Up
journal, January 2015

Mechanisms of Ion and Water Transport in Perfluorosulfonated Ionomer Membranes for Fuel Cells
journal, October 2004

Understanding the mechanism of membrane electrode assembly degradation by carbon corrosion by analyzing the microstructural changes in the cathode catalyst layers and polarization losses in proton exchange membrane fuel cell
journal, November 2012

Study of Self-Diffusion of Monovalent and Divalent Cations in Nafion-117 Ion-Exchange Membrane
journal, September 2001

Computational Modeling of Foreign Cation Contamination in PEFCs
journal, January 2014

Cationic Contamination Effects on Polymer Electrolyte Membrane Fuel Cell Performance
journal, January 2011

Distributed cation contamination from cathode to anode direction in polymer electrolyte fuel cells
journal, October 2015

Carbon Corrosion in PEM Fuel Cells during Drive Cycle Operation
journal, September 2015

Carbon corrosion induced by membrane failure: The weak link of PEMFC long-term performance
journal, December 2014

Polymer Electrolyte Fuel Cell Model
journal, January 1991

The influence of metal ions on the conductivity of Nafion 112 in polymer electrolyte membrane fuel cell
journal, September 2008

Diffusion of ions in sea water and in deep-sea sediments
journal, May 1974

Durability of PEM fuel cell cathode in the presence of Fe3+ and Al3+
journal, December 2010

Distributed effects of calcium ion contaminant on polymer electrolyte fuel cell performance
journal, November 2015

The Effect of Impurity Cations on the Transport Characteristics of Perfluorosulfonated Ionomer Membranes
journal, April 1999

PEMFC contaminant tolerance limit – Foreign cations in ionomers
journal, May 2011

Accelerated Testing of Carbon Corrosion and Membrane Degradation in PEM Fuel Cells
journal, March 2013

Evaluation of cathode contamination with Ca2+ in proton exchange membrane fuel cells
journal, January 2018

The Maxwell-Stefan approach to mass transfer
journal, March 1997

Transport and equilibrium properties of Nafion® membranes with H+ and Na+ ions
journal, January 1998

A review of PEM hydrogen fuel cell contamination: Impacts, mechanisms, and mitigation
journal, March 2007

Effect of hydrophobicity of gas diffusion layer in calcium cation contamination in polymer electrolyte fuel cells
journal, September 2016

Effect of cations (Na+, Ca2+, Fe3+) on the conductivity of a Nafion membrane
journal, November 2010

On the Maxwell−Stefan Approach to Diffusion: A General Resolution in the Transient Regime for One-Dimensional Systems
journal, January 2010

Ion and water transport characteristics of Nafion membranes as electrolytes
journal, August 1998

A Half Cell Model to Study Performance Degradation of a PEMFC due to Cationic Contamination
conference, January 2007

Nafion degradation in PEFCs from end plate iron contamination
journal, May 2003

In situ metal ion contamination and the effects on proton exchange membrane fuel cell performance
journal, November 2011

Permeability of solutes through hydrated polymer membranes. Part I. Diffusion of sodium chloride
journal, November 1968

Contaminant absorption and conductivity in polymer electrolyte membranes
journal, August 2005