Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs)

Xin, Le; Yang, Fan; Qiu, Yang; Uzunoglu, Aytekin; Rockward, Tommy; Borup, Rodney L.; Stanciu, Lia A.; Li, Wenzhen; Xie, Jian

doi:10.1149/2.0921610jes

Title: Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs)

Abstract

Nanoscale graphenes were used as cathode catalyst supports in proton exchange membrane fuel cells (PEMFCs). Surface-initiated polymerization that covalently bonds polybenzimidazole (PBI) polymer on the surface of graphene supports enables the uniform distribution of the Pt nanoparticles, as well as allows the sealing of the unterminated carbon bonds usually present on the edge of graphene from the chemical reduction of graphene oxide. The nanographene effectively shortens the length of channels and pores for O₂ diffusion/water dissipation and significantly increases the primary pore volume. Further addition of p-phenyl sulfonic functional graphitic carbon particles as spacers, increases the specific volume of the secondary pores and greatly improves O₂ mass transport within the catalyst layers. The developed composite cathode catalyst of Pt/PBI-nanographene (50 wt%) + SO₃H-graphitic carbon black demonstrates a higher beginning of life (BOL) PEMFC performance as compared to both Pt/PBI-nanographene (50 wt%) and Pt/PBI-graphene (50 wt%) + SO₃H-graphitic carbon black (GCB). Accelerated stress tests show excellent support durability compared to that of traditional Pt/Vulcan XC72 catalysts, when subjected to 10,000 cycles from 1.0 V to 1.5 V. As a result, this study suggests the promise of using PBI-nanographene + SO₃H-GCB hybrid supports in fuel cells to achieve the 2020 DOE targetsmore » for transportation applications.« less

Authors:

Xin, Le ^[1]; Yang, Fan ^[2]; Qiu, Yang ^[3]; Uzunoglu, Aytekin ^[4]; Rockward, Tommy ^[5]; Borup, Rodney L. ^[5]; Stanciu, Lia A. ^[4]; Li, Wenzhen ^[3]; Xie, Jian ^[1]

Indiana Univ.-Purdue Univ. Indianapolis, Indianapolis, IN (United States)
Indiana Univ.-Purdue Univ. Indianapolis, Indianapolis, IN (United States); Purdue Univ., West Lafayette, IN (United States)
Iowa State Univ., Ames, IA (United States)
Purdue Univ., West Lafayette, IN (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Publication Date:: Thu Aug 25 00:00:00 EDT 2016

Research Org.:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Hydrogen Fuel Cell Technologies Office

OSTI Identifier:: 1344363

Report Number(s):: LA-UR-16-24680
Journal ID: ISSN 0013-4651

Grant/Contract Number:: AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Journal of the Electrochemical Society

Additional Journal Information:: Journal Volume: 163; Journal Issue: 10; Journal ID: ISSN 0013-4651

Publisher:: The Electrochemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 30 DIRECT ENERGY CONVERSION; energy Sciences; fuel cell; nanographene; graphene supports; mercury porosimetry; PEMFCs; polybenzimidazole polymer; support durability; surface functionalization

Citation Formats


                    Xin, Le, Yang, Fan, Qiu, Yang, Uzunoglu, Aytekin, Rockward, Tommy, Borup, Rodney L., Stanciu, Lia A., Li, Wenzhen, and Xie, Jian. Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs).  United States: N. p., 2016. 
Web.  doi:10.1149/2.0921610jes.

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                    Xin, Le, Yang, Fan, Qiu, Yang, Uzunoglu, Aytekin, Rockward, Tommy, Borup, Rodney L., Stanciu, Lia A., Li, Wenzhen, & Xie, Jian. Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs).  United States.  https://doi.org/10.1149/2.0921610jes

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                    Xin, Le, Yang, Fan, Qiu, Yang, Uzunoglu, Aytekin, Rockward, Tommy, Borup, Rodney L., Stanciu, Lia A., Li, Wenzhen, and Xie, Jian. Thu .  
"Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs)".  United States.  https://doi.org/10.1149/2.0921610jes.  https://www.osti.gov/servlets/purl/1344363.

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@article{osti_1344363,

  title        = {Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs)},

  author       = {Xin, Le and Yang, Fan and Qiu, Yang and Uzunoglu, Aytekin and Rockward, Tommy and Borup, Rodney L. and Stanciu, Lia A. and Li, Wenzhen and Xie, Jian},

  abstractNote = {Nanoscale graphenes were used as cathode catalyst supports in proton exchange membrane fuel cells (PEMFCs). Surface-initiated polymerization that covalently bonds polybenzimidazole (PBI) polymer on the surface of graphene supports enables the uniform distribution of the Pt nanoparticles, as well as allows the sealing of the unterminated carbon bonds usually present on the edge of graphene from the chemical reduction of graphene oxide. The nanographene effectively shortens the length of channels and pores for O2 diffusion/water dissipation and significantly increases the primary pore volume. Further addition of p-phenyl sulfonic functional graphitic carbon particles as spacers, increases the specific volume of the secondary pores and greatly improves O2 mass transport within the catalyst layers. The developed composite cathode catalyst of Pt/PBI-nanographene (50 wt%) + SO3H-graphitic carbon black demonstrates a higher beginning of life (BOL) PEMFC performance as compared to both Pt/PBI-nanographene (50 wt%) and Pt/PBI-graphene (50 wt%) + SO3H-graphitic carbon black (GCB). Accelerated stress tests show excellent support durability compared to that of traditional Pt/Vulcan XC72 catalysts, when subjected to 10,000 cycles from 1.0 V to 1.5 V. As a result, this study suggests the promise of using PBI-nanographene + SO3H-GCB hybrid supports in fuel cells to achieve the 2020 DOE targets for transportation applications.},

  doi          = {10.1149/2.0921610jes},

  journal      = {Journal of the Electrochemical Society},

  number       = 10,

  volume       = 163,

  place        = {United States},

  year         = {Thu Aug 25 00:00:00 EDT 2016},

  month        = {Thu Aug 25 00:00:00 EDT 2016}

}

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Title: Polybenzimidazole (PBI) functionalized nanographene as highly stable catalyst support for polymer Electrolyte membrane fuel cells (PEMFCs)

Abstract

Citation Formats

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

Polymer supports for low-temperature fuel cell catalysts journal, August 2009

The role of carbon in fuel cells journal, June 2006

Investigation of Carbon Corrosion Behavior and Kinetics in Proton Exchange Membrane Fuel Cell Cathode Electrodes journal, January 2013

Low temperature operation and influence parameters on the cold start ability of portable PEMFCs journal, March 2006

PEM fuel cell cathode carbon corrosion due to the formation of air/fuel boundary at the anode journal, August 2006

A Reverse-Current Decay Mechanism for Fuel Cells journal, January 2005

Durable PEM Fuel Cell Electrode Materials: Requirements and Benchmarking Methodologies conference, January 2006

Effect of operating conditions on carbon corrosion in polymer electrolyte membrane fuel cells journal, September 2009

PEM fuel cell electrocatalyst durability measurements journal, December 2006

Ex Situ and In Situ Stability Studies of PEMFC Catalysts journal, January 2005

Accelerated Stress Testing by Rotating Disk Electrode for Carbon Corrosion in Fuel Cell Catalyst Supports journal, January 2015

Understanding and approaches for the durability issues of Pt-based catalysts for PEM fuel cell journal, September 2007

Study of the effect of temperature on Pt dissolution in polymer electrolyte membrane fuel cells via accelerated stress tests journal, January 2014

Characterization of Vulcan Electrochemically Oxidized under Simulated PEM Fuel Cell Conditions journal, January 2004

Transmission Electron Microscopy Observation of Corrosion Behaviors of Platinized Carbon Blacks under Thermal and Electrochemical Conditions journal, January 2010

Non-destructive transmission electron microscopy study of catalyst degradation under electrochemical treatment journal, December 2008

Initial Stages of Oxidation on Graphitic Surfaces: Photoemission Study and Density Functional Theory Calculations journal, April 2009

The influence of the electrochemical stressing (potential step and potential-static holding) on the degradation of polymer electrolyte membrane fuel cell electrocatalysts journal, October 2008

Surface oxidation of carbon supports due to potential cycling under PEM fuel cell conditions journal, June 2010

Investigation of the Carbon Corrosion Process for Polymer Electrolyte Fuel Cells Using a Rotating Disk Electrode Technique journal, January 2010

Enhancing the catalytic performance of Pt/C catalysts using steam-etched carbon blacks as a catalyst support journal, January 2011

Electrochemical and Raman spectroscopic evaluation of Pt/graphitized carbon black catalyst durability for the start/stop operating condition of polymer electrolyte fuel cells journal, May 2012

Graphitic Carbon as Durable Cathode-Catalyst Support for PEFCs journal, May 2011

Comparative investigation of the resistance to electrochemical oxidation of carbon black and carbon nanotubes in aqueous sulfuric acid solution journal, August 2006

Pristine and graphitized-MWCNTs as durable cathode-catalyst supports for PEFCs journal, November 2013

Corrosion resistance and sintering effect of carbon supports in polymer electrolyte membrane fuel cells journal, November 2009

Use of a carbon nanocage as a catalyst support in polymer electrolyte membrane fuel cells journal, June 2009

Nanoscale graphite-supported Pt catalysts for oxygen reduction reactions in fuel cells journal, February 2011

Graphitic mesoporous carbon as a durable fuel cell catalyst support journal, October 2008

Durability of Pt/C and Pt/MC-PEDOT Catalysts under Simulated Start-Stop Cycles in Polymer Electrolyte Fuel Cells journal, March 2013

Development of highly-active and stable Pt/C catalyst for polymer electrolyte membrane fuel cells under simulated start-up/shut-down cycling journal, January 2016

Development of catalytically active and highly stable catalyst supports for polymer electrolyte membrane fuel cells journal, January 2015

Development of Highly Active and Durable Hybrid Cathode Catalysts for Polymer Electrolyte Membrane Fuel Cells journal, January 2014

The rise of graphene journal, March 2007

Graphene for energy conversion and storage in fuel cells and supercapacitors journal, July 2012

Ultraflat graphene journal, November 2009

Highly Active Platinum Nanoparticles on Graphene Nanosheets with a Significant Improvement in Stability and CO Tolerance journal, February 2012

Graphene/carbon nanospheres sandwich supported PEMfuel cell metal nanocatalysts with remarkably high activity and stability journal, January 2013

Exfoliated Graphene Separated by Platinum Nanoparticles journal, November 2008

Stabilization of High-Performance Oxygen Reduction Reaction Pt Electrocatalyst Supported on Reduced Graphene Oxide/Carbon Black Composite journal, July 2012

Graphene and Graphene Oxide: Synthesis, Properties, and Applications journal, June 2010

Electronic Transport Properties of Individual Chemically Reduced Graphene Oxide Sheets journal, November 2007

Hierarchical polybenzimidazole-grafted graphene hybrids as supports for Pt nanoparticle catalysts with excellent PEMFC performance journal, September 2015

Understanding Pt Nanoparticle Anchoring on Graphene Supports through Surface Functionalization journal, March 2016

Preparation of Graphitic Oxide journal, March 1958

A highly durable fuel cell electrocatalyst based on polybenzimidazole-coated stacked graphene journal, January 2014

Porosimetry of MEAs Made by “Thin Film Decal” Method and Its Effect on Performance of PEFCs journal, January 2004

Investigation of the Microstructure in the Catalyst Layer and Effects of Both Perfluorosulfonate Ionomer and PTFE-Loaded Carbon on the Catalyst Layer of Polymer Electrolyte Fuel Cells journal, January 1995

Structural evolution of water swollen perfluorosulfonated ionomers from dry membrane to solution journal, July 2000

Colloidal structure of ionomer solutions in polar solvents journal, September 1996

Investigation of a Catalyst Ink Dispersion Using Both Ultra-Small-Angle X-ray Scattering and Cryogenic TEM journal, December 2010

Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs journal, March 2005

Covalent Electron Transfer Chemistry of Graphene with Diazonium Salts journal, September 2012

Electrochemical Glucose Detection Using PdAg Nanoparticles Anchored on rGO/MWCNT Nanohybrids journal, July 2019

Phosphoric Acid Doped Crosslinked Polybenzimidazole/Modified Graphene Oxide Composite Membranes for High Temperature Proton Exchange Membrane Applications journal, January 2018

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

Polymer supports for low-temperature fuel cell catalysts
journal, August 2009

The role of carbon in fuel cells
journal, June 2006

Investigation of Carbon Corrosion Behavior and Kinetics in Proton Exchange Membrane Fuel Cell Cathode Electrodes
journal, January 2013

Low temperature operation and influence parameters on the cold start ability of portable PEMFCs
journal, March 2006

PEM fuel cell cathode carbon corrosion due to the formation of air/fuel boundary at the anode
journal, August 2006

A Reverse-Current Decay Mechanism for Fuel Cells
journal, January 2005

Durable PEM Fuel Cell Electrode Materials: Requirements and Benchmarking Methodologies
conference, January 2006

Effect of operating conditions on carbon corrosion in polymer electrolyte membrane fuel cells
journal, September 2009

PEM fuel cell electrocatalyst durability measurements
journal, December 2006

Ex Situ and In Situ Stability Studies of PEMFC Catalysts
journal, January 2005

Accelerated Stress Testing by Rotating Disk Electrode for Carbon Corrosion in Fuel Cell Catalyst Supports
journal, January 2015

Understanding and approaches for the durability issues of Pt-based catalysts for PEM fuel cell
journal, September 2007

Study of the effect of temperature on Pt dissolution in polymer electrolyte membrane fuel cells via accelerated stress tests
journal, January 2014

Characterization of Vulcan Electrochemically Oxidized under Simulated PEM Fuel Cell Conditions
journal, January 2004

Transmission Electron Microscopy Observation of Corrosion Behaviors of Platinized Carbon Blacks under Thermal and Electrochemical Conditions
journal, January 2010

Non-destructive transmission electron microscopy study of catalyst degradation under electrochemical treatment
journal, December 2008

Initial Stages of Oxidation on Graphitic Surfaces: Photoemission Study and Density Functional Theory Calculations
journal, April 2009

The influence of the electrochemical stressing (potential step and potential-static holding) on the degradation of polymer electrolyte membrane fuel cell electrocatalysts
journal, October 2008

Surface oxidation of carbon supports due to potential cycling under PEM fuel cell conditions
journal, June 2010

Investigation of the Carbon Corrosion Process for Polymer Electrolyte Fuel Cells Using a Rotating Disk Electrode Technique
journal, January 2010

Enhancing the catalytic performance of Pt/C catalysts using steam-etched carbon blacks as a catalyst support
journal, January 2011

Electrochemical and Raman spectroscopic evaluation of Pt/graphitized carbon black catalyst durability for the start/stop operating condition of polymer electrolyte fuel cells
journal, May 2012

Graphitic Carbon as Durable Cathode-Catalyst Support for PEFCs
journal, May 2011

Comparative investigation of the resistance to electrochemical oxidation of carbon black and carbon nanotubes in aqueous sulfuric acid solution
journal, August 2006

Pristine and graphitized-MWCNTs as durable cathode-catalyst supports for PEFCs
journal, November 2013

Corrosion resistance and sintering effect of carbon supports in polymer electrolyte membrane fuel cells
journal, November 2009

Use of a carbon nanocage as a catalyst support in polymer electrolyte membrane fuel cells
journal, June 2009

Nanoscale graphite-supported Pt catalysts for oxygen reduction reactions in fuel cells
journal, February 2011

Graphitic mesoporous carbon as a durable fuel cell catalyst support
journal, October 2008

Durability of Pt/C and Pt/MC-PEDOT Catalysts under Simulated Start-Stop Cycles in Polymer Electrolyte Fuel Cells
journal, March 2013

Development of highly-active and stable Pt/C catalyst for polymer electrolyte membrane fuel cells under simulated start-up/shut-down cycling
journal, January 2016

Development of catalytically active and highly stable catalyst supports for polymer electrolyte membrane fuel cells
journal, January 2015

Development of Highly Active and Durable Hybrid Cathode Catalysts for Polymer Electrolyte Membrane Fuel Cells
journal, January 2014

The rise of graphene
journal, March 2007

Graphene for energy conversion and storage in fuel cells and supercapacitors
journal, July 2012

Ultraflat graphene
journal, November 2009

Highly Active Platinum Nanoparticles on Graphene Nanosheets with a Significant Improvement in Stability and CO Tolerance
journal, February 2012

Graphene/carbon nanospheres sandwich supported PEMfuel cell metal nanocatalysts with remarkably high activity and stability
journal, January 2013

Exfoliated Graphene Separated by Platinum Nanoparticles
journal, November 2008

Stabilization of High-Performance Oxygen Reduction Reaction Pt Electrocatalyst Supported on Reduced Graphene Oxide/Carbon Black Composite
journal, July 2012

Graphene and Graphene Oxide: Synthesis, Properties, and Applications
journal, June 2010

Electronic Transport Properties of Individual Chemically Reduced Graphene Oxide Sheets
journal, November 2007

Hierarchical polybenzimidazole-grafted graphene hybrids as supports for Pt nanoparticle catalysts with excellent PEMFC performance
journal, September 2015

Understanding Pt Nanoparticle Anchoring on Graphene Supports through Surface Functionalization
journal, March 2016

Preparation of Graphitic Oxide
journal, March 1958

A highly durable fuel cell electrocatalyst based on polybenzimidazole-coated stacked graphene
journal, January 2014

Porosimetry of MEAs Made by “Thin Film Decal” Method and Its Effect on Performance of PEFCs
journal, January 2004

Investigation of the Microstructure in the Catalyst Layer and Effects of Both Perfluorosulfonate Ionomer and PTFE-Loaded Carbon on the Catalyst Layer of Polymer Electrolyte Fuel Cells
journal, January 1995

Structural evolution of water swollen perfluorosulfonated ionomers from dry membrane to solution
journal, July 2000

Colloidal structure of ionomer solutions in polar solvents
journal, September 1996

Investigation of a Catalyst Ink Dispersion Using Both Ultra-Small-Angle X-ray Scattering and Cryogenic TEM
journal, December 2010

Activity benchmarks and requirements for Pt, Pt-alloy, and non-Pt oxygen reduction catalysts for PEMFCs
journal, March 2005

Covalent Electron Transfer Chemistry of Graphene with Diazonium Salts
journal, September 2012

Electrochemical Glucose Detection Using PdAg Nanoparticles Anchored on rGO/MWCNT Nanohybrids
journal, July 2019

Phosphoric Acid Doped Crosslinked Polybenzimidazole/Modified Graphene Oxide Composite Membranes for High Temperature Proton Exchange Membrane Applications
journal, January 2018