In-situ self-templated preparation of porous core-shell Fe1-xS@N, S co-doped carbon architecture for highly efficient oxygen reduction reaction

In-situ self-templated preparation of porous core-shell Fe1-xS@N, S co-doped carbon architecture for highly efficient oxygen reduction reaction
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原位自模板制备多孔核壳Fe1xS@N、S共掺杂碳结构用于高效氧还原反应

DOI:
10.1016/j.jechem.2020.06.010
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发表时间:
2021-03-01
影响因子:
13.1
通讯作者:
Chen, Yangyang
Chen, Yangyang
中科院分区:
化学1区
文献类型:
--
作者:
Li, Zhi;Wang, Wei;Chen, Yangyang

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过渡金属化合物(TMC)/碳杂化材料作为一种新型的电催化剂,在氧还原反应(ORR)领域受到了广泛的关注。它们的形态、结构和组成通常在决定ORR性能方面起着至关重要的作用。本文首次报道了以Fe_3 O_4纳米球和吡咯为牺牲自模板,采用一种新颖的原位自模板诱导策略成功制备了核壳结构的Fe_(1-x)S @N,S共掺杂碳(Fe_(1-x)S @NSC-t,t代表刻蚀时间)。盐酸腐蚀Fe_3O_4释放出的Fe ~(3+)可实现吡咯的后聚合。因此,蚀刻时间对Fe 1-xS@NSC-t的形貌、结构、组成和ORR性能具有显著影响。通过表征发现,Fe 1-xS@NSC-24能够实现Fe 1-xS和NSC的有效平衡结合,具有多孔核壳结构、优化的结构缺陷、比表面积和杂原子掺杂构型(尤其是吡啶氮、石墨氮和Fe-N结构)。因此,这些特征导致对ORR的出色的催化活性和循环稳定性。该研究为设计具有独特稳定形貌和优化结构组成的TMC/碳基电极提供了很好的指导。(C)2020科学出版社、中国科学院大连化学物理研究所。由ELSEVIER B. V.和科学出版社出版。All rights reserved.
Transition metal compound (TMC)/carbon hybrids, as prospering electrocatalyst, have attracted great attention in the field of oxygen reduction reaction (ORR). Their morphology, structure and composition often play a crucial role in determining the ORR performance. In this work, we for the first time report the successful fabrication of porous core-shell Fe1-xS@N, S co-doped carbon (Fe1-xS@NSC-t, t represents etching time) by a novel in situ self-template induced strategy using Fe3O4 nanospheres and pyrrole as sacrificial self-template. The post-polymerization of pyrrole can be accomplished by the Fe3+ released through the etching of Fe3O4 by HCl acid. Thus, the etching time has a significant effect on the morphology, structure, composition and ORR performance of Fe1-xS@NSC-t. Based on the characterizations, we find Fe1-xS@NSC-24 can realize effective and balanced combination of Fe1-xS and NSC, possessing porous core-shell architecture, optimized structure defect, specific surface area and doped heteroatoms configurations (especially for pyridinic N, graphitic N and Fe-N structure). These features thus lead to outstanding catalytic activity and cycling stability towards ORR. Our work provides a good guidance on the design of TMC/carbon-based electrodes with unique stable morphology and optimized structure and composition. (C) 2020 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.