P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction
Abstract
This contribution reports the discovery and analysis of a p-block Sn-based catalyst for the electroreduction of molecular oxygen in acidic conditions at fuel cell cathodes; the catalyst is free of platinum-group metals and contains single-metal-atom actives sites coordinated by nitrogen. The prepared SnNC catalysts meet and exceed state-of-the-art FeNC catalysts in terms of intrinsic catalytic turn-over frequency and hydrogen–air fuel cell power density. The SnNC-NH3 catalysts displayed a 40–50% higher current density than FeNC-NH3 at cell voltages below 0.7 V. Additional benefits include a highly favourable selectivity for the four-electron reduction pathway and a Fenton-inactive character of Sn. Here, a range of analytical techniques combined with density functional theory calculations indicate that stannic Sn(iv)Nx single-metal sites with moderate oxygen chemisorption properties and low pyridinic N coordination numbers act as catalytically active moieties. The superior proton-exchange membrane fuel cell performance of SnNC cathode catalysts under realistic, hydrogen–air fuel cell conditions, particularly after NH3 activation treatment, makes them a promising alternative to today’s state-of-the-art Fe-based catalysts.
- Authors:
-
[4];
[5];
[2];
[2];
[7];
[8];
[2];
[1]
- Technical Univ. of Berlin (Germany)
- Montpellier Univ. (France)
- Copenhagen Univ. (Denmark); Seabourg Technologies, Copenhagen (Denmark)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Synchrotron SOLEIL, Gif-sur-Yvette (France)
- Max Planck Society, Berlin (Germany). Fritz Haber Institute; Max Planck Inst. for Chemical Energy Conversion, Berlin (Germany)
- Technical Univ. of Darmstadt (Germany)
- Copenhagen Univ. (Denmark)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; Federal Ministry of Education and Research (BMBF); Danish National Research Foundation; Graduate School of Excellence Energy Science and Engineering
- OSTI Identifier:
- 1756269
- Grant/Contract Number:
- AC05-00OR22725; 05K16RD1; DNRF 149; GRC1070
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Materials
- Additional Journal Information:
- Journal Volume: 19; Journal Issue: 11; Journal ID: ISSN 1476-1122
- Publisher:
- Springer Nature - Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE
Citation Formats
Luo, Fang, Roy, Aaron, Silvioli, Luca, Cullen, David A., Zitolo, Andrea, Sougrati, Moulay Tahar, Oguz, Ismail Can, Mineva, Tzonka, Teschner, Detre, Wagner, Stephan, Wen, Ju, Dionigi, Fabio, Kramm, Ulrike I., Rossmeisl, Jan, Jaouen, Frédéric, and Strasser, Peter. P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction. United States: N. p., 2020.
Web. doi:10.1038/s41563-020-0717-5.
Luo, Fang, Roy, Aaron, Silvioli, Luca, Cullen, David A., Zitolo, Andrea, Sougrati, Moulay Tahar, Oguz, Ismail Can, Mineva, Tzonka, Teschner, Detre, Wagner, Stephan, Wen, Ju, Dionigi, Fabio, Kramm, Ulrike I., Rossmeisl, Jan, Jaouen, Frédéric, & Strasser, Peter. P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction. United States. https://doi.org/10.1038/s41563-020-0717-5
Luo, Fang, Roy, Aaron, Silvioli, Luca, Cullen, David A., Zitolo, Andrea, Sougrati, Moulay Tahar, Oguz, Ismail Can, Mineva, Tzonka, Teschner, Detre, Wagner, Stephan, Wen, Ju, Dionigi, Fabio, Kramm, Ulrike I., Rossmeisl, Jan, Jaouen, Frédéric, and Strasser, Peter. Mon .
"P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction". United States. https://doi.org/10.1038/s41563-020-0717-5. https://www.osti.gov/servlets/purl/1756269.
@article{osti_1756269,
title = {P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction},
author = {Luo, Fang and Roy, Aaron and Silvioli, Luca and Cullen, David A. and Zitolo, Andrea and Sougrati, Moulay Tahar and Oguz, Ismail Can and Mineva, Tzonka and Teschner, Detre and Wagner, Stephan and Wen, Ju and Dionigi, Fabio and Kramm, Ulrike I. and Rossmeisl, Jan and Jaouen, Frédéric and Strasser, Peter},
abstractNote = {This contribution reports the discovery and analysis of a p-block Sn-based catalyst for the electroreduction of molecular oxygen in acidic conditions at fuel cell cathodes; the catalyst is free of platinum-group metals and contains single-metal-atom actives sites coordinated by nitrogen. The prepared SnNC catalysts meet and exceed state-of-the-art FeNC catalysts in terms of intrinsic catalytic turn-over frequency and hydrogen–air fuel cell power density. The SnNC-NH3 catalysts displayed a 40–50% higher current density than FeNC-NH3 at cell voltages below 0.7 V. Additional benefits include a highly favourable selectivity for the four-electron reduction pathway and a Fenton-inactive character of Sn. Here, a range of analytical techniques combined with density functional theory calculations indicate that stannic Sn(iv)Nx single-metal sites with moderate oxygen chemisorption properties and low pyridinic N coordination numbers act as catalytically active moieties. The superior proton-exchange membrane fuel cell performance of SnNC cathode catalysts under realistic, hydrogen–air fuel cell conditions, particularly after NH3 activation treatment, makes them a promising alternative to today’s state-of-the-art Fe-based catalysts.},
doi = {10.1038/s41563-020-0717-5},
journal = {Nature Materials},
number = 11,
volume = 19,
place = {United States},
year = {Mon Jul 13 00:00:00 EDT 2020},
month = {Mon Jul 13 00:00:00 EDT 2020}
}
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