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Research Article

Facile synthesis of porous nitrogen-doped holey graphene as an efficient metal-free catalyst for the oxygen reduction reaction

Li Qin1,2,5, Ruimin Ding1,2, Huixiang Wang1,2,5, Jianghong Wu1,2,5, Conghui Wang1,2,5, Chenghua Zhang1,3, Yao Xu4, Liancheng Wang1,2( ), Baoliang Lv1,2( )
State Key Laboratory of Coal Conversion,Institute of Coal Chemistry, Chinese Academy of Sciences,Taiyuan,030001,China;
Key Laboratory of Carbon Materials,Institute of Coal Chemistry, Chinese Academy of Sciences,Taiyuan,030001,China;
Synfuels China Technology Co. Ltd., Beijing 101407, China
State Key Laboratory of Transient Optics and Photonics,Xi'an Institute of Optics and Precision Mechanics, Chinese Academy of Sciences,Xi'an,710119,China;
University of Chinese Academy of Sciences, Beijing 100049, China
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Abstract

Nitrogen-doped graphene is a promising candidate for the replacement of noble metal-based electrocatalysts for oxygen reduction reactions (ORRs). The addition of pores and holes into nitrogen-doped graphene enhances the ORR activity by introducing abundant exposed edges, accelerating mass transfer, and impeding aggregation of the graphene sheets. Herein, we present a straightforward but effective strategy for generating porous holey nitrogen-doped graphene (PHNG) via the pyrolysis of urea and magnesium acetate tetrahydrate. Due to the combined effects of the in situ generated gases and MgO nanoparticles, the synthesized PHNGs featured not only numerous out-of-plane pores among the crumpled graphene sheets, but also interpenetrated nanoscale (5-15 nm) holes in the assembled graphene. Moreover, the nitrogen doping configurations of PHNG were optimized by post-thermal treatments at different temperatures. It was found that the overall content of pyridinic and quaternary nitrogen positively correlates with the ORR activity; in particular, pyridinic nitrogen generates the most desirable characteristics for the ORR. This work reveals new routes for the synthesis of PHNG-based materials and elucidates the contributions of various nitrogen species to ORRs.

Keywords

porous holey N-doped graphenein situ templatespost-thermal treatmentoxygen reduction reaction

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Nano Research
Volume 10 Issue 1,
January 2017
Pages 305-319
DOI: 10.1007/s12274-016-1293-5
Cite this article:
Qin L, Ding R, Wang H, et al. Facile synthesis of porous nitrogen-doped holey graphene as an efficient metal-free catalyst for the oxygen reduction reaction. Nano Research, 2017, 10(1): 305-319. https://doi.org/10.1007/s12274-016-1293-5

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Received: 22 June 2016
Revised: 13 September 2016
Accepted: 19 September 2016
Published: 20 October 2016
© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2016
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