Chen Lisong, Cui Xiangzhi, Wang Yongxia, Wang Min, Cui Fangming, Wei Chenyang, Huang Weimin, Hua Zile, Zhang Lingxia, Shi Jianlin
State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295# Dingxi Rd., Shanghai, 200050 (P.R. China).
Chem Asian J. 2014 Oct;9(10):2915-20. doi: 10.1002/asia.201402334. Epub 2014 Aug 5.
A high amount of heteroatom doping in carbon, although favorable for enhanced density of catalytically active sites, may lead to substantially decreased electroconductivity, which is necessary for the electrochemical oxygen reduction reaction. Herein, a relatively low amount of nitrogen was successfully doped into carbon nanotubes (CNTs) by a hydrothermal approach in one step, and the synthesized nitrogen-doped CNT (CNT-N) materials retained most of the original, excellent characteristics, such as the graphitic structure, tubular morphology, and high surface area, of CNTs. The resultant CNT-N materials, although containing a relatively low amount of nitrogen doping, exhibited high electrocatalytic ORR activity, comparable to that of 20 wt% Pt/C; long durability; and, more importantly, largely inhibited methanol crossover effect.
碳中大量的杂原子掺杂，虽然有利于提高催化活性位点的密度，但可能会导致电导率大幅下降，而电导率对于电化学氧还原反应是必需的。在此，通过水热法一步成功地将相对少量的氮掺杂到碳纳米管（CNT）中，合成的氮掺杂碳纳米管（CNT-N）材料保留了碳纳米管的大部分原始优异特性，如石墨结构、管状形态和高比表面积。所得的CNT-N材料虽然氮掺杂量相对较低，但表现出高电催化氧还原反应（ORR）活性，与20 wt%的Pt/C相当；具有长耐久性；更重要的是，很大程度上抑制了甲醇渗透效应。
