Nitrogen and Sulfur Co-doped Mesoporous Carbon Materials as Highly Efficient Electrocatalysts for Oxygen Reduction Reaction

被引:57
作者
Shi, Jingjing [1 ]
Zhou, Xuejun [1 ]
Xu, Pan [1 ]
Qiao, Jinli [1 ]
Chen, Zhongwei [2 ]
Liu, Yuyu [3 ]
机构
[1] Donghua Univ, Coll Environm Sci & Engn, Shanghai 201620, Peoples R China
[2] Univ Waterloo, Dept Chem Engn, Waterloo, ON N2L 3G1, Canada
[3] Tohoku Univ, Grad Sch Environm Studies, Multidisciplinary Res Circulat Waste Resources, Aoba Ku, Sendai, Miyagi 9808579, Japan
基金
中国国家自然科学基金;
关键词
Mesoporous carbon material; N and S co-doping; Oxygen reduction reaction; Proton-exchange membrane fuel cell; NONPRECIOUS METAL ELECTROCATALYSTS; CELL CATHODE CATALYST; FUEL-CELLS; ALKALINE-SOLUTIONS; GRAPHENE; NANOTUBES; ELECTROREDUCTION; ELECTRODES; IRON; GRAPHITE;
D O I
10.1016/j.electacta.2014.08.091
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
Nitrogen and sulfur co-doped mesoporous carbon materials are synthesized by pyrolyzing FeSO4+ poly (ethyleneimine) + template SiO2 mixture at a high temperature without additional dopant precursors. For post-treatment, acid leaching is used to remove the metal, and the heat-treatment is tailored to optimize the catalytic activity of the catalysts toward the oxygen reduction reaction (ORR) in acidic solution. Scanning electron microscopy, X-ray diffraction, low-temperature N-2 adsorption, X-ray photoelectron spectroscopy and inductively coupled plasma are used to characterize the catalysts' morphologies, structures, and compositions. Rotating disk electrode and rotating ring-disk electrode techniques are employed to quantitatively obtain the ORR kinetic constants and determine the reaction mechanisms. The ORR activity is highly improved by reheating the catalyst after H2SO4 leaching with improved half-wave potential of 0.68 V vs. RHE, and ORR electron number larger than 3.76. Moreover, increasing the catalyst loading of 800 mu g cm(-2) exhibits only 36 mV deviation from Pt/C. It is believed that the synergetic effect between the Fe-, N- and S-containing active sites and the modified carbon matrix structure due to H2SO4 leaching and reheating should make contribution to the high ORR activity. (C) 2014 Elsevier Ltd. All rights reserved.
引用
收藏
页码:259 / 269
页数:11
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