Unraveling the Oxygen‐Reduction Sites in Graphitic‐Carbon Co–N–C‐Type Electrocatalysts Prepared by Single‐Precursor Pyrolysis

作者: Palaniappan Subramanian , Roopathy Mohan , Alex Schechter

DOI: 10.1002/CCTC.201700324

关键词:

摘要: Metal- and nitrogen-doped carbon-based hybrid materials (M–N–C) are widely regarded as promising alternative to platinum for catalyzing the oxygen-reduction reaction (ORR) in fuel-cell cathodes. The two important steps involved preparation of these catalysts acid washing a second heat treatment pyrolyzed mixture made carbon, nitrogen, metal precursors (M). We have explored detail changes induced by post-treatment on structure, composition, activity new prepared prolonged pyrolysis single well-defined organometallic precursor. marginal increase nitrogen content, apparent BET surface area, porosity, defects, higher degree graphitization positively contribute substantial improvement ORR post-treated alkaline solution, whereas this procedure is found weaker influence solution. findings from study suggest that both free nitrogen-coordinated sites, specifically, “Co2N” which present catalyst bulk protected graphitic carbon layer, most likely active sites Co–N–C catalysts. Based experimental results, we propose model will assist improving understanding plausible functioning

参考文章(37)
Andrea Zitolo, Vincent Goellner, Vanessa Armel, Moulay-Tahar Sougrati, Tzonka Mineva, Lorenzo Stievano, Emiliano Fonda, Frédéric Jaouen, Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials. Nature Materials. ,vol. 14, pp. 937- 942 ,(2015) , 10.1038/NMAT4367
Xiaogang Su, Jianguo Liu, Yingfang Yao, Yong You, Xiang Zhang, Canyun Zhao, Hong Wan, You Zhou, Zhigang Zou, Solid phase polymerization of phenylenediamine toward a self-supported FeNx/C catalyst with high oxygen reduction activity Chemical Communications. ,vol. 51, pp. 16707- 16709 ,(2015) , 10.1039/C5CC06413A
Ping Song, Ying Wang, Jing Pan, Weilin Xu, Lin Zhuang, Structure-activity relationship in high-performance iron-based electrocatalysts for oxygen reduction reaction Journal of Power Sources. ,vol. 300, pp. 279- 284 ,(2015) , 10.1016/J.JPOWSOUR.2015.09.081
Shaohong Liu, Yanfeng Dong, Zhiyu Wang, Huawei Huang, Zongbin Zhao, Jieshan Qiu, Towards efficient electrocatalysts for oxygen reduction by doping cobalt into graphene-supported graphitic carbon nitride Journal of Materials Chemistry. ,vol. 3, pp. 19657- 19661 ,(2015) , 10.1039/C5TA05776K
Alexey Serov, Urszula Tylus, Kateryna Artyushkova, Sanjeev Mukerjee, Plamen Atanassov, Mechanistic studies of oxygen reduction on Fe-PEI derived non-PGM electrocatalysts Applied Catalysis B: Environmental. ,vol. 150-151, pp. 179- 186 ,(2014) , 10.1016/J.APCATB.2013.12.009
Shenlong Zhao, Huajie Yin, Lei Du, Liangcan He, Kun Zhao, Lin Chang, Geping Yin, Huijun Zhao, Shaoqin Liu, Zhiyong Tang, Carbonized nanoscale metal-organic frameworks as high performance electrocatalyst for oxygen reduction reaction. ACS Nano. ,vol. 8, pp. 12660- 12668 ,(2014) , 10.1021/NN505582E
RAYMOND JASINSKI, A New Fuel Cell Cathode Catalyst Nature. ,vol. 201, pp. 1212- 1213 ,(1964) , 10.1038/2011212A0
Galina V. Zhutaeva, Vera A. Bogdanovskaya, Elena S. Davydova, Leonid P. Kazanskii, Michail R. Tarasevich, Kinetics and mechanism of oxygen electroreduction on Vulcan XC72R carbon black modified by pyrolysis products of cobalt 5,10,15,20-tetrakis(4-methoxyphenyl)porphyrine in a broad pH interval Journal of Solid State Electrochemistry. ,vol. 18, pp. 1319- 1334 ,(2014) , 10.1007/S10008-013-2233-X
Guo-Liang Chai, Zhufeng Hou, Da-Jun Shu, Takashi Ikeda, Kiyoyuki Terakura, Active Sites and Mechanisms for Oxygen Reduction Reaction on Nitrogen-Doped Carbon Alloy Catalysts: Stone–Wales Defect and Curvature Effect Journal of the American Chemical Society. ,vol. 136, pp. 13629- 13640 ,(2014) , 10.1021/JA502646C