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

被引:350
作者
Luo, Fang [1 ]
Roy, Aaron [2 ]
Silvioli, Luca [3 ,4 ]
Cullen, David A. [5 ]
Zitolo, Andrea [6 ]
Sougrati, Moulay Tahar [2 ]
Oguz, Ismail Can [2 ]
Mineva, Tzonka [2 ]
Teschner, Detre [7 ,8 ]
Wagner, Stephan [9 ,10 ]
Wen, Ju [1 ]
Dionigi, Fabio [1 ]
Kramm, Ulrike, I [9 ,10 ]
Rossmeisl, Jan [3 ]
Jaouen, Frederic [2 ]
Strasser, Peter [1 ]
机构
[1] Tech Univ Berlin, Dept Chem, Chem Engn Div, Electrochem Energy Catalysis & Mat Sci Lab, Berlin, Germany
[2] Univ Montpellier, CNRS, ENSCM, ICGM, Montpellier, France
[3] Univ Copenhagen, Nanosci Ctr, Dept Chem, Copenhagen, Denmark
[4] Seaborg Technol, Copenhagen, Denmark
[5] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN USA
[6] Synchrotron SOLEIL, BP 48, Gif Sur Yvette, France
[7] Fritz Haber Inst Max Planck Gesell, Inorgan Chem Elect Struct Grp, Berlin, Germany
[8] Max Planck Inst Chem Energy Convers, Dept Heterogeneous React, Berlin, Germany
[9] Tech Univ Darmstadt, Grad Sch Excellence Energy Sci & Engn, Dept Chem, Darmstadt, Germany
[10] Tech Univ Darmstadt, Grad Sch Excellence Energy Sci & Engn, Dept Mat & Earth Sci, Darmstadt, Germany
基金
新加坡国家研究基金会; 欧盟地平线“2020”;
关键词
DENSITY-FUNCTIONAL THEORY; ACTIVE-SITES; FE/N/C CATALYSTS; ELECTROCATALYSTS; IRON; ELECTROREDUCTION; IDENTIFICATION; UNIVERSALITY; DEGRADATION; COMPLEXES;
D O I
10.1038/s41563-020-0717-5
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
This contribution reports the discovery and analysis of ap-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-NH(3)catalysts displayed a 40-50% higher current density than FeNC-NH(3)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. A range of analytical techniques combined with density functional theory calculations indicate that stannic Sn(iv)N(x)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 NH(3)activation treatment, makes them a promising alternative to today's state-of-the-art Fe-based catalysts. For oxygen reduction and hydrogen oxidation reactions, proton-exchange membrane fuel cells typically rely on precious-metal-based catalysts. Ap-block single-metal-site tin/nitrogen-doped carbon is shown to exhibit promising electrocatalytic and fuel cell performance.
引用
收藏
页码:1215 / +
页数:10
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