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

Journal Article · · Nature Materials
 [1];  [2];  [3];  [4];  [5];  [2];  [2];  [2];  [6];  [7];  [1];  [1];  [7];  [8];  [2];  [1]
  1. Technical Univ. of Berlin (Germany)
  2. Montpellier Univ. (France)
  3. Copenhagen Univ. (Denmark); Seabourg Technologies, Copenhagen (Denmark)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. Synchrotron SOLEIL, Gif-sur-Yvette (France)
  6. Max Planck Society, Berlin (Germany). Fritz Haber Institute; Max Planck Inst. for Chemical Energy Conversion, Berlin (Germany)
  7. Technical Univ. of Darmstadt (Germany)
  8. Copenhagen Univ. (Denmark)
+ Show Author Affiliations
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.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
Danish National Research Foundation; Federal Ministry of Education and Research (BMBF); Graduate School of Excellence Energy Science and Engineering; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
1756269
Journal Information:
Nature Materials, Journal Name: Nature Materials Journal Issue: 11 Vol. 19; ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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25 ENERGY STORAGE