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

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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 °C. In O2-staturated 0.1 M KOH solution, the half-wave potential (E 1/2) 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.

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Authors and Affiliations

  1. State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai, 200050, China

    Ruguang Ma, Xiaodong Ren, Yao Zhou, Chi Sun, Qian Liu, Jianjun Liu & Jiacheng Wang

  2. Shanghai Institute of Materials Genome, 99 Shangda Road, Shanghai, 200444, China

    Ruguang Ma, Xiaodong Ren, Yao Zhou, Chi Sun, Qian Liu, Jianjun Liu & Jiacheng Wang

  3. School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore

    Bao Yu Xia

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  1. Ruguang Ma
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  2. Xiaodong Ren
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  3. Bao Yu Xia
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  4. Yao Zhou
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  6. Qian Liu
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Correspondence to Qian Liu, Jianjun Liu or Jiacheng Wang.

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Ma, R., Ren, X., Xia, B.Y. et al. Novel synthesis of N-doped graphene as an efficient electrocatalyst towards oxygen reduction. Nano Res. 9, 808–819 (2016). https://doi.org/10.1007/s12274-015-0960-2

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