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Research Article

Novel synthesis of N-doped graphene as an efficient electrocatalyst towards oxygen reduction

Ruguang Ma1,2, Xiaodong Ren1,2, Bao Yu Xia3, Yao Zhou1,2, Chi Sun1,2, Qian Liu1,2( ), Jianjun Liu1,2( ), Jiacheng Wang1,2( )
State Key Laboratory of High Performance Ceramics and Superfine MicrostructureShanghai Institute of CeramicsChinese Academy of Sciences1295 Dingxi RoadShanghai200050China
Shanghai Institute of Materials Genome99 Shangda RoadShanghai200444China
School of Chemical and Biomedical EngineeringNanyang Technological University62 Nanyang DriveSingapore637459Singapore
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Graphical Abstract

Abstract

Nitrogen-doped graphene (NG) was successfully synthesized by a novel, facile, and scalable bottom-up method. The annealed NG (NG-A) possessed high specific surface area and a hierarchical porous texture, and exhibited remarkably improved electrocatalytic activity in the oxygen reduction reaction in both alkaline and acidic media. Ab initio molecular dynamic simulations indicated that rapid H transfer and the thermodynamic stability of six-membered N structures promoted the transformation of N-containing species from pyrrolic to pyridinic at 600 ℃. In O2-staturated 0.1 M KOH solution, the half-wave potential (E1/2) of NG-A was only 62 mV lower than that of a commercial Pt/C catalyst, and the limiting current density of NG-A was 0.5 mA·cm–2 larger than that of Pt/C. Koutecky–Levich (K–L) plots and rotating ring-disk electrode measurement indicated a four-electron-transfer pathway in NG-A, which could be ascribed to its high content of pyridinic N.

Keywords

oxygen reduction reactiongraphenenitrogen dopingmolecular dynamic simulation

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Nano Research
Volume 9 Issue 3,
March 2016
Pages 808-819
DOI: 10.1007/s12274-015-0960-2
Cite this article:
Ma R, Ren X, Xia BY, et al. Novel synthesis of N-doped graphene as an efficient electrocatalyst towards oxygen reduction. Nano Research, 2016, 9(3): 808-819. https://doi.org/10.1007/s12274-015-0960-2

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Received: 13 August 2015
Revised: 24 September 2015
Accepted: 29 November 2015
Published: 14 January 2016
© Tsinghua University Press and Springer-Verlag Berlin Heidelberg 2015
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