Synergistic Effects between Atomically Dispersed Fe-N-C and C-S-C for the Oxygen Reduction Reaction in Acidic Media
Synergistic Effects between Atomically Dispersed Fe-N-C and C-S-C for the Oxygen Reduction Reaction in Acidic Media
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DOI：
10.1002/anie.201706602
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发表时间：
2017-10-23
影响因子：
16.6
通讯作者：
Guo, Shaojun
中科院分区：
文献类型：
--
作者：
Shen, Hangjia;Gracia-Espino, Eduardo;Guo, Shaojun
近年来，人们设计了多种基于硫掺杂Fe/N/C材料的先进催化剂用于氧还原反应（ORR）;然而，活性的增强仍然存在争议，通常归因于表面积的差异，电导率的提高或不确定的协同效应。本文中，通过牺牲模板的方法获得硫掺杂的Fe/N/C催化剂（表示为Fe/SNC）。掺入的硫产生噻吩样结构（C-S-C），减少了Fe中心周围的电子局域化，改善了与含氧物种的相互作用，因此促进了酸性溶液中的完全4 e（-）ORR。由于这些协同效应，Fe/SNC催化剂在0.5m H2SO 4中表现出比无硫变体（Fe/NC）好得多的ORR活性。
Various advanced catalysts based on sulfur-doped Fe/N/C materials have recently been designed for the oxygen reduction reaction (ORR); however, the enhanced activity is still controversial and usually attributed to differences in the surface area, improved conductivity, or uncertain synergistic effects. Herein, a sulfur-doped Fe/N/C catalyst (denoted as Fe/SNC) was obtained by a template-sacrificing method. The incorporated sulfur gives a thiophene-like structure (C-S-C), reduces the electron localization around the Fe centers, improves the interaction with oxygenated species, and therefore facilitates the complete 4e(-) ORR in acidic solution. Owing to these synergistic effects, the Fe/SNC catalyst exhibits much better ORR activity than the sulfur-free variant (Fe/NC) in 0.5m H2SO4.