P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction

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

doi:10.1038/s41563-020-0717-5

Title: P-block single-metal-site tin/nitrogen-doped carbon fuel cell cathode catalyst for oxygen reduction reaction

Journal Article · Mon Jul 13 00:00:00 EDT 2020 · Nature Materials

DOI:https://doi.org/10.1038/s41563-020-0717-5· OSTI ID:1756269

Luo, Fang ^[1]; Roy, Aaron ^[2]; Silvioli, Luca ^[3];

^[4];

^[5];

^[2]; Oguz, Ismail Can ^[2];

^[2]; Teschner, Detre ^[6]; Wagner, Stephan ^[7]; Wen, Ju ^[1]; Dionigi, Fabio ^[1];

^[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)

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.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: 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

Grant/Contract Number:: AC05-00OR22725; 05K16RD1; DNRF 149; GRC1070

OSTI ID:: 1756269

Journal Information:: Nature Materials, Vol. 19, Issue 11; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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