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Title: Understanding how single-atom site density drives the performance and durability of PGM-free Fe–N–C cathodes in anion exchange membrane fuel cells

Abstract

One of the most important needs for the future of low-cost fuel cells is the development of highly active platinum group metal (PGM)-free catalysts. For the oxygen reduction reaction, Fe–N–C materials have been widely studied in both acid and alkaline media. However, reported catalysts in the literature show quite different intrinsic activity and in-cell performance, despite similar synthesis routes and precursors. Here, two types of Fe–N–C are prepared from the same precursor and procedure – the main difference is how the precursor was handled prior to use. It is shown that in one case Fe overwhelmingly existed as highly active single-metal atoms in FeN4 coordination (preferred), while in the other case large Fe particles coexisting with few single metal atoms were obtained. As a result, there were drastic differences in the catalyst structure, activity, and especially in their performance in an operating anion exchange membrane fuel cell (AEMFC). Additionally, it is shown that catalyst layers created from single-atom-dominated Fe–N–C can have excellent performance and durability in an AEMFC using H2/O2 reacting gases, achieving a peak power density of 1.8 W cm-2 – comparable to similar AEMFCs with a Pt/C cathode – and being able to operate stably for more thanmore » 100 h. Finally, the Fe–N–C cathode was paired with a low-loading PtRu/C anode electrode to create AEMFCs (on H2/O2) with a total PGM loading of only 0.135 mg cm-2 (0.090 mgPt cm-2) that was able to achieve a very high specific power of 8.4 W mgPGM-1 (12.6 W mgPt<sup>-1).« less

Authors:
 [1];  [2]; ORCiD logo [1];  [1];  [3];  [3];  [3]; ORCiD logo [3];  [1]; ORCiD logo [2];  [4];  [5];  [1]; ORCiD logo [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. University of South Carolina, Columbia, SC (United States)
  2. Montpellier University (France)
  3. Technion-Israel Institute of Technology, Haifa (Israel)
  4. Synchrotron SOLEIL, L'orme des Merisiers, Gif-sur-Yvette (France)
  5. University of Surrey, Guildford (United Kingdom)
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States); Univ. of South Carolina, Columbia, SC (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Hydrogen Fuel Cell Technologies Office (HFTO); Engineering and Physical Sciences Research Council (EPSRC); Center of Catalysis for Renewable Fuels(CReF); European Union's Horizon 2020; Ministry of National Infrastructure, Energy and Water Resources of Israel; Mauerberger Foundation Fund (MFF)
OSTI Identifier:
1977473
Grant/Contract Number:  
EE0008433; EP/M014371/1; 721065; 3-15578; 3-16686 (219-11-135)
Resource Type:
Accepted Manuscript
Journal Name:
Materials Today Advances
Additional Journal Information:
Journal Volume: 12; Journal Issue: C; Journal ID: ISSN 2590-0498
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; PGM-free; AEM; fuel cell; oxygen reduction; high performance; Fe–N–C; single-atom

Citation Formats

Adabi, Horie, Santori, Pietro Giovanni, Shakouri, Abolfazl, Peng, Xiong, Yassin, Karam, Rasin, Igal G., Brandon, Simon, Dekel, Dario R., Hassan, Noor Ul, Sougrati, Moulay-Tahar, Zitolo, Andrea, Varcoe, John R., Regalbuto, John R., Jaouen, Frédéric, and Mustain, William E. Understanding how single-atom site density drives the performance and durability of PGM-free Fe–N–C cathodes in anion exchange membrane fuel cells. United States: N. p., 2021. Web. doi:10.1016/j.mtadv.2021.100179.
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Adabi, Horie, Santori, Pietro Giovanni, Shakouri, Abolfazl, Peng, Xiong, Yassin, Karam, Rasin, Igal G., Brandon, Simon, Dekel, Dario R., Hassan, Noor Ul, Sougrati, Moulay-Tahar, Zitolo, Andrea, Varcoe, John R., Regalbuto, John R., Jaouen, Frédéric, & Mustain, William E. Understanding how single-atom site density drives the performance and durability of PGM-free Fe–N–C cathodes in anion exchange membrane fuel cells. United States. https://doi.org/10.1016/j.mtadv.2021.100179
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Adabi, Horie, Santori, Pietro Giovanni, Shakouri, Abolfazl, Peng, Xiong, Yassin, Karam, Rasin, Igal G., Brandon, Simon, Dekel, Dario R., Hassan, Noor Ul, Sougrati, Moulay-Tahar, Zitolo, Andrea, Varcoe, John R., Regalbuto, John R., Jaouen, Frédéric, and Mustain, William E. Wed . "Understanding how single-atom site density drives the performance and durability of PGM-free Fe–N–C cathodes in anion exchange membrane fuel cells". United States. https://doi.org/10.1016/j.mtadv.2021.100179. https://www.osti.gov/servlets/purl/1977473.
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@article{osti_1977473,
title = {Understanding how single-atom site density drives the performance and durability of PGM-free Fe–N–C cathodes in anion exchange membrane fuel cells},
author = {Adabi, Horie and Santori, Pietro Giovanni and Shakouri, Abolfazl and Peng, Xiong and Yassin, Karam and Rasin, Igal G. and Brandon, Simon and Dekel, Dario R. and Hassan, Noor Ul and Sougrati, Moulay-Tahar and Zitolo, Andrea and Varcoe, John R. and Regalbuto, John R. and Jaouen, Frédéric and Mustain, William E.},
abstractNote = {One of the most important needs for the future of low-cost fuel cells is the development of highly active platinum group metal (PGM)-free catalysts. For the oxygen reduction reaction, Fe–N–C materials have been widely studied in both acid and alkaline media. However, reported catalysts in the literature show quite different intrinsic activity and in-cell performance, despite similar synthesis routes and precursors. Here, two types of Fe–N–C are prepared from the same precursor and procedure – the main difference is how the precursor was handled prior to use. It is shown that in one case Fe overwhelmingly existed as highly active single-metal atoms in FeN4 coordination (preferred), while in the other case large Fe particles coexisting with few single metal atoms were obtained. As a result, there were drastic differences in the catalyst structure, activity, and especially in their performance in an operating anion exchange membrane fuel cell (AEMFC). Additionally, it is shown that catalyst layers created from single-atom-dominated Fe–N–C can have excellent performance and durability in an AEMFC using H2/O2 reacting gases, achieving a peak power density of 1.8 W cm-2 – comparable to similar AEMFCs with a Pt/C cathode – and being able to operate stably for more than 100 h. Finally, the Fe–N–C cathode was paired with a low-loading PtRu/C anode electrode to create AEMFCs (on H2/O2) with a total PGM loading of only 0.135 mg cm-2 (0.090 mgPt cm-2) that was able to achieve a very high specific power of 8.4 W mgPGM-1 (12.6 W mgPt<sup>-1).},
doi = {10.1016/j.mtadv.2021.100179},
journal = {Materials Today Advances},
number = C,
volume = 12,
place = {United States},
year = {Wed Nov 10 00:00:00 EST 2021},
month = {Wed Nov 10 00:00:00 EST 2021}
}
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