Synthesis of cobalt and nitrogen co-doped carbon nanotubes and its ORR activity as the catalyst used in hydrogen fuel cells

Synthesis of cobalt and nitrogen co-doped carbon nanotubes and its ORR activity as the catalyst used in hydrogen fuel cells
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钴氮共掺杂碳纳米管的合成及其氢燃料电池催化剂的ORR活性

DOI:
10.1016/j.ijhydene.2019.03.271
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发表时间:
2019
影响因子:
7.2
通讯作者:
An Baigang
An Baigang
中科院分区:
工程技术2区
文献类型:
--
作者:
Zhao Hongwei;Xing Tianyu;Li Lixiang;Geng Xin;Guo Ke;Sun Chengguo;Zhou Weimin;Yang Haiming;Song Renfeng;An Baigang

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在氢燃料电池中,缓慢的氧还原反应(ORR)需要使用催化剂。不幸的是,在商业氢燃料电池中,贵重的铂基催化剂仍然表现出最好的ORR活性。因此,开发非贵金属催化剂成为氢燃料电池利用氢能的一个重要方面。为了开发非贵金属催化剂,了解其催化剂的ORR活性中心,本文分别制备了钴氮共掺杂、氮掺杂和钴掺杂的碳纳米管,并测试和比较了它们对ORR的催化性能。采用X射线衍射(XRD)、X射线光电子能谱(XPS)、孔/比表面分析仪和电化学方法对样品的表面组成、微观结构和氧化还原性能进行了研究。结果表明,钴氮共掺杂的碳纳米管作为催化剂时,具有最高的ORR极限电流密度、最正的ORR起始电位和最大的转移电子数(接近4),表现出比氮掺杂和钴掺杂的碳纳米管更好的ORR催化性能。钴氮共掺杂碳纳米管的良好ORR性能可归因于其含氮官能团、钴或钴氧化物、Co-Nx结构的活性位点以及这些位点对ORR的协同作用。
In hydrogen fuel cells, the sluggish oxygen reduction reaction (ORR) requires the catalysts used. Unfortunately, the precious platinum based catalysts still exhibit the best ORR activity in the commercial hydrogen fuel cells. Therefore, developing non-precious metal catalysts ORR become an important aspect for the utilization of hydrogen energy by using hydrogen fuel cells to develop non-precious catalysts and understand their active sites of ORR, herein the cobalt and nitrogen co-doped CNTs, nitrogen-doped CNTs and cobalt doped CNTs were prepared, respectively, and their catalytic properties toward ORR were tested and compared. The surface composition, microstructure and ORR performance of the samples were examined by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), pore/specific surface analyzer and electrochemical methods. The results demonstrate that as the catalyst, the cobalt and nitrogen co-doped CNTs owns the highest ORR limiting current density, the most positive ORR onset potential and the largest transfer electron number close to four, and thus exhibits the better ORR catalytic performance compared to the other two samples of the nitrogen-doped CNTs and the cobalt doped CNTs. The good ORR performance of cobalt and nitrogen co-doped CNTs can be attributed to its active sites of nitrogen containing functional groups, cobalt or cobalt oxides, Co-Nxstructure, and the synergistic effect of these sites on ORR.