The self-template synthesis of highly efficient hollow structure Fe/N/C electrocatalysts with Fe-N coordination for the oxygen reduction reaction.
The self-template synthesis of highly efficient hollow structure Fe/N/C electrocatalysts with Fe-N coordination for the oxygen reduction reaction.
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DOI：
10.1039/c8ra03672a
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发表时间：
2018-07-02
期刊：
影响因子：
3.9
通讯作者：
Zuo, Xia
中科院分区：
文献类型：
--
作者：
Yu, Yue;Xiao, Dejian;Ma, Jun;Chen, Changli;Li, Kai;Ma, Jie;Liao, Yi;Zheng, Lirong;Zuo, Xia
在M/N/C催化剂的基础上，寻找高效的催化剂来代替贵金属铂进行氧还原反应，具有重要的意义和挑战性。本文提出了一种利用自模板法合成高效、稳定的空心结构Fe/N/C催化剂的方法。在NaCl保护下制备的Fe/N/C催化剂具有独特的中空结构、多孔形貌和Fe-N配位活性中心，这些都显著赋予了材料优异的ORR性能，包括高电导率、长期耐久性和优异的抗甲醇能力。利用X射线吸收精细结构谱研究了Fe/N/C催化剂中心铁原子的化学状态和配位环境，阐明了NaCl保护对热解过程中Fe-N配位的促进作用。特别是，Fe/N/C催化剂表现出正半波电位（0.84 V vs. RHE）和Tafel斜率与20%商业Pt/C相当，具有四电子转移途径以及优异的长期稳定性和在碱性介质中的甲醇耐受性。在M/N/C催化剂的基础上，寻找高效的催化剂来代替贵金属铂进行氧还原反应，具有重要的意义和挑战性。
The exploration of highly efficient catalysts to replace noble metal platinum for the oxygen reduction reaction, on which M/N/C catalysts have shed brilliant light, is greatly significant but challenging. This paper presents a strategy for synthesizing highly efficient and stabilized hollow structure Fe/N/C catalysts with iron and nitrogen doped into the carbon layer by the self-template method. The prepared Fe/N/C catalysts with NaCl protection during pyrolysis are characterized by a unique hollow structure, porous morphology and Fe–N coordination as the active sites, all of which significantly endow the materials with excellent properties towards the ORR, including high electrical conductivity, long-term durability and outstanding capacity for methanol tolerance. We employed X-ray absorption fine structure spectrometry to investigate the chemical state and coordination environment of the central iron atoms of the Fe/N/C catalysts, which also clarified the promoting effect of the NaCl protection for Fe–N coordination during pyrolysis. In particular, the Fe/N/C catalysts exhibit positive half-wave potentials (0.84 V vs. RHE) and Tafel slope comparable to 20% commercial Pt/C, possessing four-electron transfer pathway as well as excellent long-term stability and methanol tolerance in alkaline medium. The exploration of highly efficient catalysts to replace noble metal platinum for the oxygen reduction reaction, on which M/N/C catalysts have shed brilliant light, is greatly significant but challenging.
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