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Title: High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells

Abstract

Low cost and high-performing platinum group metal-free (PGM-free) cathodes have the potential to transform the economics of polymer electrolyte fuel cell (PEFC) commercialization. Significant advancements have been made recently in terms of PGM-free catalyst activity and stability. However, before PGM-free catalysts become viable in PEFCs, several technical challenges must be addressed including cathode’s fabrication, ionomer integration, and transport losses. Here we present an integrated optimization of cathode performance that was achieved by simultaneously optimizing the catalyst morphology and electrode structure for high power density. The chemically-doped metal-organic framework (MOF) derived Fe-N-C catalyst we used allows precise tuning of particle size over a wide range, enabling this unique study. Our results demonstrate the careful interplay between the catalyst primary particle size and the polymer electrolyte ionomer integration. The primary particles must be sufficiently large to permit uniform ionomer thin-films throughout the surrounding pores, but not so large as to impact intraparticle transport to the active sites. Here, the content of ionomer must be carefully balanced between sufficient loading for complete catalyst coverage and adequate proton conductivity, while not being excessive and inducing large oxygen transport losses and liquid water flooding. With the optimal 100 nm size catalyst and ionomer loading, wemore » achieved a high power density of 410 mW/cm2 at rated voltage and a peak power density of 610 mW/cm2 in an automotive-relevant operating condition.« less

Authors:
 [1];  [1];  [2];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Carnegie Mellon Univ., Pittsburgh, PA (United States)
  2. Univ. at Buffalo, The State Univ. of New York, NY (United States)
Publication Date:
Research Org.:
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Fuel Cell Technologies Office
OSTI Identifier:
1901983
Grant/Contract Number:  
EE0008076
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 12; Journal Issue: 2; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; polymer electrolyte fuel cell; platinum group metal-free; metal−organic framework; Fe−N−C catalyst; computed tomography; ionomer; atmospheric chemistry; catalysts; electrodes; fuel cells; ionomers

Citation Formats

Uddin, Aman, Dunsmore, Lisa, Zhang, Hanguang, Hu, Leiming, Wu, Gang, and Litster, Shawn. High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells. United States: N. p., 2019. Web. doi:10.1021/acsami.9b13945.
Uddin, Aman, Dunsmore, Lisa, Zhang, Hanguang, Hu, Leiming, Wu, Gang, & Litster, Shawn. High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells. United States. https://doi.org/10.1021/acsami.9b13945
Uddin, Aman, Dunsmore, Lisa, Zhang, Hanguang, Hu, Leiming, Wu, Gang, and Litster, Shawn. Wed . "High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells". United States. https://doi.org/10.1021/acsami.9b13945. https://www.osti.gov/servlets/purl/1901983.
@article{osti_1901983,
title = {High Power Density Platinum Group Metal-free Cathodes for Polymer Electrolyte Fuel Cells},
author = {Uddin, Aman and Dunsmore, Lisa and Zhang, Hanguang and Hu, Leiming and Wu, Gang and Litster, Shawn},
abstractNote = {Low cost and high-performing platinum group metal-free (PGM-free) cathodes have the potential to transform the economics of polymer electrolyte fuel cell (PEFC) commercialization. Significant advancements have been made recently in terms of PGM-free catalyst activity and stability. However, before PGM-free catalysts become viable in PEFCs, several technical challenges must be addressed including cathode’s fabrication, ionomer integration, and transport losses. Here we present an integrated optimization of cathode performance that was achieved by simultaneously optimizing the catalyst morphology and electrode structure for high power density. The chemically-doped metal-organic framework (MOF) derived Fe-N-C catalyst we used allows precise tuning of particle size over a wide range, enabling this unique study. Our results demonstrate the careful interplay between the catalyst primary particle size and the polymer electrolyte ionomer integration. The primary particles must be sufficiently large to permit uniform ionomer thin-films throughout the surrounding pores, but not so large as to impact intraparticle transport to the active sites. Here, the content of ionomer must be carefully balanced between sufficient loading for complete catalyst coverage and adequate proton conductivity, while not being excessive and inducing large oxygen transport losses and liquid water flooding. With the optimal 100 nm size catalyst and ionomer loading, we achieved a high power density of 410 mW/cm2 at rated voltage and a peak power density of 610 mW/cm2 in an automotive-relevant operating condition.},
doi = {10.1021/acsami.9b13945},
journal = {ACS Applied Materials and Interfaces},
number = 2,
volume = 12,
place = {United States},
year = {Wed Dec 18 00:00:00 EST 2019},
month = {Wed Dec 18 00:00:00 EST 2019}
}

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