Skip to main content
SpringerLink
Log in

Low-Cost and Highly Efficient Metal-Free Electrocatalysts for Oxygen Reduction Reaction: Environment-Friendly Three-Dimensional B, N Co-doped Graphene Aerogels

  • Original Research
  • Published:
Electrocatalysis Aims and scope Submit manuscript

Abstract

Nitrogen (N) and boron (B) co-doped graphene materials have been certified as promising catalyst for oxygen reduction reaction (ORR), since the dual doping of foreign atoms could induce a unique electronic structure in graphene and create a synergistic coupling effect between heteroatoms. However, previously reported B, N co-doped graphene materials suffered from shortcomings such as needing highly toxic precursors or high cost or complex preparation procedures. Herein, one highly efficient metal-free ORR catalyst, three-dimensional graphene aerogels (GAs) co-doped with B and N using economical and environmentally friendly melamine and boric acid as heteroatom precursors, was prepared through a one-step hydrothermal method. The as-prepared microporous B, N co-doped GAs showed excellent electrochemical catalytic performances for ORR under alkaline condition (0.1 M KOH) with a much more positive onset potential (0.994 V vs. RHE) than most of the existing B, N co-doped ones, a dominant four-electron transfer mechanism (n = 3.73 at 0.6 V), as well as excellent stability.

ᅟ

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Scheme 1.
Fig. 1
Fig. 2
Fig. 3
Fig. 4

Similar content being viewed by others

References

  1. M.K. Debe, Nature 43, 486 (2012)

  2. M. Zhou, HL. Wang, S.Guo, Chem. Soc. Rev. 1273, 45 (2016)

  3. H. Woo, J. Kang, J. Kim, C. Kim, S. Nam, B. Park, Electron. Mater. Lett. 1, 12 (2016)

    Google Scholar 

  4. J. Suntivich, H. Gasteiger, N. Yabuuchi, H. Nakanishi, J.B. Goodenough, Y. Shao-Horn, Nat. Chem. 546, 3 (2011)

    Google Scholar 

  5. W. Ai, Z. Luo, J. Jiang, J. Zhu, Z. Du, Z. Fan, L. Xie, H. Zhang, W. Huang, T. Yu, Adv. Mater. 6186, 26 (2014)

    Google Scholar 

  6. Q. Liu, Z. Pu, C. Tang, A. Asiri, A. Qusti, A. Al-Youbi, X. Sun, Electrochem. Commun. 57, 36 (2013)

    Google Scholar 

  7. Z.W. Liu, F. Peng, H.J. Wang, H. Yu, W.X. Zheng, J. Yang, Angew. Chem. Int. Ed. 3257, 50 (2011)

  8. Z.S. Wu, S. Yang, Y. Sun, K. Parvez, X. Feng, K. Müllen, J. Am, Chem. Soc. 9082, 134 (2012)

    Google Scholar 

  9. W. Yang, X. Liu, X. Yue, J.Jia, S. Guo, J. Am. Chem. Soc.14, 137(2015)

  10. Z. Pu, Q. Liu, C. Tang, A. Asiri, A. Qusti, A. Al-Youbi, X. Sun, J. Power Sources 257, 170 (2014)

    Article  CAS  Google Scholar 

  11. Z. Wen, S. Ci, F. Zhang, X. Feng, S. Cui, S. Mao, S. Luo, Z. He, J. Chen, Adv. Mater. 1399, 24 (2012)

    Google Scholar 

  12. S. Guo, S. Zhang, L. Wu, S. Sun, Angew. Chem. Int. Ed. 11770, 51 (2012)

    Google Scholar 

  13. W. Xia, R. Zou, L. An, D. Xia, S. Guo, Energy Environ. Sci. 568, 8 (2015)

    Google Scholar 

  14. J. Tian, R. Ning, Q. Liu, A.M. Asiri, A. Al-Youbi, X. Sun, ACS Appl. Mater. Interfaces 1011, 6 (2014)

    Google Scholar 

  15. Y.K. Choi, K.H. Chjo, S.M. Park, J. Electrochem. Soc. 4107, 142 (1995)

    Google Scholar 

  16. Y. Shimizu, K. Uemura, N. Miura, N. Yamazoe, Chem. Lett. 1979, 12 (1988)

    Google Scholar 

  17. M.R. Gao, J. Jiang, S.H. Yu, Small 13, 8 (2012)

    Google Scholar 

  18. S. Ye, A.K. Vijh, Electrochem. Commun. 272, 5 (2003)

    Google Scholar 

  19. H. Ghanbarlou, S. Rowshanzamir, M.J. Parnian, F. Mehri, Int. J. Hydrog. Energy 14665, 41 (2016)

    Google Scholar 

  20. D. Higgins, F.M. Hassan, H.S. Min, J.Y. Choi, M.A. Hoque, U.L. Dong, Z. Chen, J. Mater. Chem. A6340, 3 (2015)

    Google Scholar 

  21. S. Rojas-Carbonell, S. Babanova, A. Serov, Y. Ulyanova, S. Singhal, P. Atanassov, Electrochim. Acta 504, 190 (2016)

    Google Scholar 

  22. K. Gong, F. Du, Z. Xia, M. Durstock, L. Dai, Science 760, 323 (2009)

    Google Scholar 

  23. L. Yang, S. Jiang, Y. Zhao, L. Zhu, S. Chen, X. Wang, Q. Wu, J. Ma, Y. Ma, Z. Hu, Angew. Chem. Int. Ed. 7270, 123 (2011)

    Google Scholar 

  24. K.N. Wood, R. O’Hayre, S. Pylypenko, Energy Environ. Sci. 1212, 7 (2014)

    Google Scholar 

  25. Y. Zhou, C.H. Yen, S. Fu, G. Yang, C. Zhu, D. Du, P.C. Wo, X. Chen, J. Yang, C.M. Wai, Green Chem. 3552, 17 (2015)

    Google Scholar 

  26. A. Ramadoss, S.J. Kim, Carbon 63, 434 (2013)

    Article  CAS  Google Scholar 

  27. L. Shi, K. Chen, R. Du, A. Bachmatiuk, M. Rümmeli, K. Xie, Y. Huang, Y. Zhang, Z. Liu, J. Am. Chem. Soc. 6360, 138 (2016)

    Google Scholar 

  28. L. Chen, R. Du, J. Zhu, Y. Mao, C. Xue, N. Zhang, Y. Hou, J. Zhang, T. Yi, Small 1423, 11 (2015)

    Google Scholar 

  29. Z. Hou, Y. Jin, X. Xin, H. Tao, D. Wu, P. Xu, R. Liu, J. Colloid Interface Sci. 317, 488 (2016)

    Google Scholar 

  30. R. Liu, X. Xi, X. Xing, D. Wu, Rsc Advances 83613, 6 (2016)

    Google Scholar 

  31. L. Zhang, J. Niu, L. Dai, Z. Xia, Langmuir 7542, 28 (2012)

    Google Scholar 

  32. J. Liu, P. Song, Z. Ning, W. Xu, Electrocatalysis 132, 6 (2015)

    Google Scholar 

  33. R. Gokhale, Y. Chen, A. Serov, K. Artyushkova, P. Atanassov, Electrochem. Commun. 140, 72 (2016)

    Google Scholar 

  34. T. Huang, S. Mao, M. Qiu, O. Mao, C. Yuan, J. Chen, Electrochim. Acta 481, 222 (2016)

    Google Scholar 

  35. J. Zhu, C. He, Y. Li, S. Kang, P. Shen, J. Mater. Chem. A14700, 1 (2013)

    Google Scholar 

  36. Y. Liu, S. Chen, X. Quan, H. Yu, H. Zhao, Y. Zhang, G. Chen, J. Phys. Chem. C14992, 117 (2013)

    Google Scholar 

  37. Y. Zhang, X. Zhuang, Y. Su, F. Zhang, X. Feng, J. Mater. Chem. A7742, 2 (2014)

    Google Scholar 

  38. Y. Xue, D. Yu, L. Dai, R. Wang, D. Li, A. Roy, F. Lu, H. Chen, Y. Liu, J. Qu, Phys. Chem. Chem. Phys. 12220, 15 (2013)

    Google Scholar 

  39. W.S.H. Jr, R.E. Offeman, J. Am, Chem. Soc. 1339, 80 (1958)

    Google Scholar 

  40. H.C. Chang, S.H. Park, S.I. Woo, Green Chem. 406, 13 (2010)

    Google Scholar 

  41. W. Wei, H. Liang, K. Parvez, X. Zhuang, X. Feng, K. Müllen, Angew. Chem. Int. Ed. 1570, 53 (2014)

    Google Scholar 

  42. Z.Q. Liu, H. Cheng, N. Li, T.Y. Ma, Y.Z. Su, Adv. Mater. 3777, 28 (2016)

    Google Scholar 

  43. Y. Liu, H. Feng, Y. Wu, L. Joshi, X. Zeng, J. Li, Biosens. Bioelectron. 63, 35 (2012)

    Google Scholar 

  44. X. Tu, S. Luo, G. Chen, J. Li, Chemistry 14359, 18 (2012)

  45. S. Kabir, K. Artyushkova, A. Serov, P. Atanassov, ACS Appl. Mater. Interfaces 11623, 10 (2018)

  46. Y. Zheng, Y. Jiao, M. Jaroniec, Y. Jin, S.Z. Qiao, Small 3550, 8 (2012)

    Google Scholar 

  47. L. Zhang, Z. Xia, J. Phys. Chem. C11170, 115 (2011)

    Google Scholar 

  48. E. Iyyamperumal, S. Wang, L. Dai, ACS Nano 5259, 6 (2012)

    Google Scholar 

  49. H. Fei, R. Ye, G. Ye, Y. Gong, Z. Peng, X. Fan, E.L. Samuel, P.M. Ajayan, J.M. Tour, ACS Nano 10837, 8 (2014)

    Google Scholar 

  50. L. Yang, S. Jiang, Y. Zhao, L. Zhu, S. Chen, X. Wang, Q. Wu, J. Ma, Y. Ma, Z. Hu, Angew. Chem. Int. Ed. 7132, 50 (2011)

    Google Scholar 

Download references

Acknowledgements

This work was supported by the National Nature Science Foundation of China (No 21575071), Qingdao Innovation Leading Expert Program, Qingdao Basic & Applied Research Project (15-9-1-100-jch), Open Funds of the State Key Laboratory of Electroanalytical Chemistry (SKLEAC201601) and Science & Technology Fund Planning Project of Shandong Colleges and Universities (J16LA13), and Training Programme for Outstanding Young Teachers in Higher Education Institutions of Guangdong Province (No. YQ2015203).

Author information

Author notes

  1. Jingrui Han and Yanlin Zhang contributed equally to this work.

Authors and Affiliations

  1. College of Life Sciences, College of Materials Science and Engineering, College Institute for Graphene Applied Technology Innovation, Qingdao University, Qingdao, 266071, China

    Jingrui Han, Fushuang Niu, Tao Chen, Jingquan Liu & Yuanhong Xu

  2. Department of Environmental Monitoring, Guangdong Polytechnic of Environmental Protection Engineering, Foshan, 528216, China

    Yanlin Zhang

Authors
  1. Jingrui Han
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yanlin Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Fushuang Niu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Tao Chen
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Jingquan Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Yuanhong Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Jingquan Liu or Yuanhong Xu.

Electronic Supplementary Material

ESM 1

(DOC 1662 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Han, J., Zhang, Y., Niu, F. et al. Low-Cost and Highly Efficient Metal-Free Electrocatalysts for Oxygen Reduction Reaction: Environment-Friendly Three-Dimensional B, N Co-doped Graphene Aerogels. Electrocatalysis 10, 56–62 (2019). https://doi.org/10.1007/s12678-018-0494-y

Download citation

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s12678-018-0494-y

Keywords

Search

Navigation