Chemical vapour deposition of Fe–N–C oxygen reduction catalysts with full utilization of dense Fe–N4 sites
Abstract
Replacing scarce and expensive platinum (Pt) with metal–nitrogen–carbon (M–N–C) catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has largely been impeded by the low oxygen reduction reaction activity of M–N–C due to low active site density and site utilization. Herein, we overcome these limits by implementing chemical vapour deposition to synthesize Fe–N–C by flowing iron chloride vapour over a Zn–N–C substrate at 750 °C, leading to high-temperature trans-metalation of Zn–N4 sites into Fe–N4 sites. Characterization by multiple techniques shows that all Fe–N4 sites formed via this approach are gas-phase and electrochemically accessible. As a result, the Fe–N–C catalyst has an active site density of 1.92 × 1020 sites per gram with 100% site utilization. This catalyst delivers an unprecedented oxygen reduction reaction activity of 33 mA cm-2 at 0.90 V (iR-corrected; i, current; R, resistance) in a H2–O2 proton exchange membrane fuel cell at 1.0 bar and 80 °C.
- Authors:
-
[1];
[2];
[3];
[5];
[6];
[7];
[2];
[1]
- Northeastern Univ., Boston, MA (United States)
- Univ. Montpellier (France). Institute Charles Gerhardt of Montpellier (ICGM)
- Univ. of California, Los Angeles, CA (United States)
- Giner, Inc, Newton, MA (United States)
- Univ. of California, Los Angeles, CA (United States). California NanoSystems Institute (CNSI)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1813025
- Alternate Identifier(s):
- OSTI ID: 1846535
- Grant/Contract Number:
- AC02-06CH11357; SC0012704; EE0008416; EE0008075; AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 2021; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Jiao, Li, Li, Jingkun, Richard, Lynne LaRochelle, Sun, Qiang, Stracensky, Thomas, Liu, Ershuai, Sougrati, Moulay Tahar, Zhao, Zipeng, Yang, Fan, Zhong, Sichen, Xu, Hui, Mukerjee, Sanjeev, Huang, Yu, Cullen, David A., Park, Jae Hyung, Ferrandon, Magali, Myers, Deborah J., Jaouen, Frédéric, and Jia, Qingying. Chemical vapour deposition of Fe–N–C oxygen reduction catalysts with full utilization of dense Fe–N4 sites. United States: N. p., 2021.
Web. doi:10.1038/s41563-021-01030-2.
Jiao, Li, Li, Jingkun, Richard, Lynne LaRochelle, Sun, Qiang, Stracensky, Thomas, Liu, Ershuai, Sougrati, Moulay Tahar, Zhao, Zipeng, Yang, Fan, Zhong, Sichen, Xu, Hui, Mukerjee, Sanjeev, Huang, Yu, Cullen, David A., Park, Jae Hyung, Ferrandon, Magali, Myers, Deborah J., Jaouen, Frédéric, & Jia, Qingying. Chemical vapour deposition of Fe–N–C oxygen reduction catalysts with full utilization of dense Fe–N4 sites. United States. https://doi.org/10.1038/s41563-021-01030-2
Jiao, Li, Li, Jingkun, Richard, Lynne LaRochelle, Sun, Qiang, Stracensky, Thomas, Liu, Ershuai, Sougrati, Moulay Tahar, Zhao, Zipeng, Yang, Fan, Zhong, Sichen, Xu, Hui, Mukerjee, Sanjeev, Huang, Yu, Cullen, David A., Park, Jae Hyung, Ferrandon, Magali, Myers, Deborah J., Jaouen, Frédéric, and Jia, Qingying. Thu .
"Chemical vapour deposition of Fe–N–C oxygen reduction catalysts with full utilization of dense Fe–N4 sites". United States. https://doi.org/10.1038/s41563-021-01030-2. https://www.osti.gov/servlets/purl/1813025.
@article{osti_1813025,
title = {Chemical vapour deposition of Fe–N–C oxygen reduction catalysts with full utilization of dense Fe–N4 sites},
author = {Jiao, Li and Li, Jingkun and Richard, Lynne LaRochelle and Sun, Qiang and Stracensky, Thomas and Liu, Ershuai and Sougrati, Moulay Tahar and Zhao, Zipeng and Yang, Fan and Zhong, Sichen and Xu, Hui and Mukerjee, Sanjeev and Huang, Yu and Cullen, David A. and Park, Jae Hyung and Ferrandon, Magali and Myers, Deborah J. and Jaouen, Frédéric and Jia, Qingying},
abstractNote = {Replacing scarce and expensive platinum (Pt) with metal–nitrogen–carbon (M–N–C) catalysts for the oxygen reduction reaction in proton exchange membrane fuel cells has largely been impeded by the low oxygen reduction reaction activity of M–N–C due to low active site density and site utilization. Herein, we overcome these limits by implementing chemical vapour deposition to synthesize Fe–N–C by flowing iron chloride vapour over a Zn–N–C substrate at 750 °C, leading to high-temperature trans-metalation of Zn–N4 sites into Fe–N4 sites. Characterization by multiple techniques shows that all Fe–N4 sites formed via this approach are gas-phase and electrochemically accessible. As a result, the Fe–N–C catalyst has an active site density of 1.92 × 1020 sites per gram with 100% site utilization. This catalyst delivers an unprecedented oxygen reduction reaction activity of 33 mA cm-2 at 0.90 V (iR-corrected; i, current; R, resistance) in a H2–O2 proton exchange membrane fuel cell at 1.0 bar and 80 °C.},
doi = {10.1038/s41563-021-01030-2},
journal = {Nature Materials},
number = ,
volume = 2021,
place = {United States},
year = {Thu Jun 10 00:00:00 EDT 2021},
month = {Thu Jun 10 00:00:00 EDT 2021}
}
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