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Title: Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells

Abstract

Here, the design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e- due to peroxide/radicals scavenging effect of Mn.

Authors:
 [1];  [2];  [3];  [1];  [1];  [4];  [5]; ORCiD logo [5]; ORCiD logo [5]; ORCiD logo [5];  [6]
  1. Univ. of Hawaii, Honolulu, HI (United States)
  2. IRD Fuel Cells, Albuquerque, NM (United States)
  3. GRandalytics, Honolulu, HI (United States)
  4. Pajarito Powder LLC, Albuquerque, NM (United States)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  6. Forschungszentrum Jülich GmbH (Germany)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); US Department of the Navy, Office of Naval Research (ONR); Hawaiian Electric Company; USDOE Office of Science (SC)
OSTI Identifier:
1866686
Alternate Identifier(s):
OSTI ID: 1864607
Grant/Contract Number:  
AC05-00OR22725; N00014-18-1-2127; N00014-19-1-2159; EE0008419
Resource Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 312; Journal Issue: NA; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; PEM fuel cell; PGM-free electrode; proton conductivity; electron conductivity; impedance; modeling

Citation Formats

Reshetenko, Tatyana, Odgaard, Madeleine, Randolf, Günter, Ohtaki, Kenta K., Bradley, John P., Zulevi, Barr, Lyu, Xiang, Cullen, David A., Jafta, Charl J., Serov, Alexey, and Kulikovsky, Andrei. Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells. United States: N. p., 2022. Web. doi:10.1016/j.apcatb.2022.121424.
Reshetenko, Tatyana, Odgaard, Madeleine, Randolf, Günter, Ohtaki, Kenta K., Bradley, John P., Zulevi, Barr, Lyu, Xiang, Cullen, David A., Jafta, Charl J., Serov, Alexey, & Kulikovsky, Andrei. Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells. United States. https://doi.org/10.1016/j.apcatb.2022.121424
Reshetenko, Tatyana, Odgaard, Madeleine, Randolf, Günter, Ohtaki, Kenta K., Bradley, John P., Zulevi, Barr, Lyu, Xiang, Cullen, David A., Jafta, Charl J., Serov, Alexey, and Kulikovsky, Andrei. Wed . "Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells". United States. https://doi.org/10.1016/j.apcatb.2022.121424. https://www.osti.gov/servlets/purl/1866686.
@article{osti_1866686,
title = {Design of PGM-free cathodic catalyst layers for advanced PEM fuel cells},
author = {Reshetenko, Tatyana and Odgaard, Madeleine and Randolf, Günter and Ohtaki, Kenta K. and Bradley, John P. and Zulevi, Barr and Lyu, Xiang and Cullen, David A. and Jafta, Charl J. and Serov, Alexey and Kulikovsky, Andrei},
abstractNote = {Here, the design of cathodic catalysts layer (CCL) consisted of Platinum Group Metal-free (PGM-free) electrocatalysts was done by catalyst coated membrane approach. Three different Fe-Mn-N-C compounds were synthesized with Fe:Mn ratio of 1:1, 2:1 and 2:1 with modified heat treatment profile. The catalysts were characterized by X-ray photoelectron spectroscopy, X-ray powder diffraction, pore and particle size distribution, zeta potential and transmission electron microscopy. Electrocatalysts were integrated into membrane electrode assembly and evaluated by electrochemical methods. Electrochemical impedance spectroscopy in combination with modeling were used for estimation of proton conductivity of CCL and its oxygen diffusivity. It was found that all CCLs possess extremely high proton conductivity, which was demonstrated for the first time for these types of PGM-free catalysts. The observed ORR mechanism was predominantly 4e- due to peroxide/radicals scavenging effect of Mn.},
doi = {10.1016/j.apcatb.2022.121424},
journal = {Applied Catalysis. B, Environmental},
number = NA,
volume = 312,
place = {United States},
year = {Wed Apr 20 00:00:00 EDT 2022},
month = {Wed Apr 20 00:00:00 EDT 2022}
}

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