Chinese Journal of Catalysis ›› 2018, Vol. 39 ›› Issue (4): 790-799.DOI: 10.1016/S1872-2067(17)62982-6

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Paper-derived cobalt and nitrogen co-doped carbon nanotube@porous carbon as a nonprecious metal electrocatalyst for the oxygen reduction reaction

Gaopeng Liua, Bin Wanga, Li Xua, Penghui Dinga, Pengfei Zhangb,c, Jiexiang Xiaa,b, Huaming Lia, Junchao Qiand   

  1. a School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, Jiangsu, China;
    b Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge 37830, USA;
    c School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;
    d Jiangsu Key Laboratory for Environment Functional Materials, Suzhou University of Science and Technology, Suzhou 215009, Jiangsu, China
  • Received:2017-11-21 Revised:2017-12-23 Online:2018-04-18 Published:2018-04-08
  • Contact: 10.1016/S1872-2067(17)62982-6
  • Supported by:

    This work was supported by the National Nature Science Foundation of China (21476098, 21471069, 21576123) and International Postdoctoral Exchange Fellowship Program of China Postdoctoral Council (20150060).

Abstract:

The oxygen reduction reaction (ORR) is a vitally important process in fuel cells. The development of high-performance and low-cost ORR electrocatalysts with outstanding stability is essential for the commercialization of the electrochemical energy technology. Herein, we report a facile synthesis of cobalt (Co) and nitrogen (N) co-doped carbon nanotube@porous carbon (Co/N/CNT@PC-800) electrocatalyst through a one-step pyrolysis of waste paper, dicyandiamide, and cobalt(Ⅱ) acetylacetonate. The surface of the hierarchical porous carbon supported a large number of carbon nanotubes (CNTs), which were derived from dicyandiamide through the catalysis of Co. The addition of Co resulted in the formation of a hierarchical micro/mesoporous structure, which was beneficial for the exposure of active sites and rapid transportation of ORR-relevant species (O2, H+, OH-, and H2O). The doped N and Co formed more active sites to enhance the ORR activity of the electrocatalyst. The Co/N/CNT@PC-800 material exhibited optimal ORR performance with an onset potential of 0.005 V vs. Ag/AgCl and a half-wave potential of -0.173 V vs. Ag/AgCl. Meanwhile, the electrocatalyst showed an excellent methanol tolerance and a long-term operational durability than that of Pt/C, as well as a quasi-four-electron reaction pathway. The low-cost and simple synthesis approach makes the Co/N/CNT@PC-800 a prospective electrocatalyst for the ORR. Furthermore, this work provides an alternative approach for exploring the use of biomass-derived electrocatalysts for renewable energy applications.

Key words: Oxygen reduction reaction, Waste paper, Biomass, Porous carbon, Cobalt