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Identification of active sites for acidic oxygen reduction on carbon catalysts with and without nitrogen doping

Journal Article


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Abstract


  • Owing to the difficulty in controlling the dopant or defect types and their homogeneity in carbon materials, it is still a controversial issue to identify the active sites of carbon-based metal-free catalysts. Here we report a proof-of-concept study on the active-site evaluation for a highly oriented pyrolytic graphite catalyst with specific pentagon carbon defective patterns (D-HOPG). It is demonstrated that specific carbon defect types (an edged pentagon in this work) could be selectively created via controllable nitrogen doping. Work-function analyses coupled with macro and micro-electrochemical performance measurements suggest that the pentagon defects in D-HOPG served as major active sites for the acidic oxygen reduction reaction, even much superior to the pyridinic nitrogen sites in nitrogen-doped highly oriented pyrolytic graphite. This work enables us to elucidate the relative importance of the specific carbon defects versus nitrogen-dopant species and their respective contributions to the observed overall acidic oxygen reduction reaction activity.

Authors


  •   Jia, Yi (external author)
  •   Zhang, Longzhou (external author)
  •   Zhuang, Linzhou (external author)
  •   Liu, Hongli (external author)
  •   Yan, Xuecheng (external author)
  •   Wang, Xin (external author)
  •   Liu, Jiandang (external author)
  •   Wang, Jiancheng (external author)
  •   Zheng, Yarong (external author)
  •   Xiao, Zhaohui (external author)
  •   Taran, Elena (external author)
  •   Chen, Jun
  •   Yang, Dongjiang (external author)
  •   Zhu, Zhonghua (external author)
  •   Wang, Shuangyin (external author)
  •   Dai, Liming (external author)
  •   Yao, Xiangdong (external author)

Publication Date


  • 2019

Citation


  • Jia, Y., Zhang, L., Zhuang, L., Liu, H., Yan, X., Wang, X., Liu, J., Wang, J., Zheng, Y., Xiao, Z., Taran, E., Chen, J., Yang, D., Zhu, Z., Wang, S., Dai, L. & Yao, X. (2019). Identification of active sites for acidic oxygen reduction on carbon catalysts with and without nitrogen doping. Nature Catalysis, 2 688-695.

Scopus Eid


  • 2-s2.0-85068052512

Ro Full-text Url


  • https://ro.uow.edu.au/context/aiimpapers/article/4816/type/native/viewcontent

Ro Metadata Url


  • http://ro.uow.edu.au/aiimpapers/3761

Has Global Citation Frequency


Number Of Pages


  • 7

Start Page


  • 688

End Page


  • 695

Volume


  • 2

Place Of Publication


  • United Kingdom

Abstract


  • Owing to the difficulty in controlling the dopant or defect types and their homogeneity in carbon materials, it is still a controversial issue to identify the active sites of carbon-based metal-free catalysts. Here we report a proof-of-concept study on the active-site evaluation for a highly oriented pyrolytic graphite catalyst with specific pentagon carbon defective patterns (D-HOPG). It is demonstrated that specific carbon defect types (an edged pentagon in this work) could be selectively created via controllable nitrogen doping. Work-function analyses coupled with macro and micro-electrochemical performance measurements suggest that the pentagon defects in D-HOPG served as major active sites for the acidic oxygen reduction reaction, even much superior to the pyridinic nitrogen sites in nitrogen-doped highly oriented pyrolytic graphite. This work enables us to elucidate the relative importance of the specific carbon defects versus nitrogen-dopant species and their respective contributions to the observed overall acidic oxygen reduction reaction activity.

Authors


  •   Jia, Yi (external author)
  •   Zhang, Longzhou (external author)
  •   Zhuang, Linzhou (external author)
  •   Liu, Hongli (external author)
  •   Yan, Xuecheng (external author)
  •   Wang, Xin (external author)
  •   Liu, Jiandang (external author)
  •   Wang, Jiancheng (external author)
  •   Zheng, Yarong (external author)
  •   Xiao, Zhaohui (external author)
  •   Taran, Elena (external author)
  •   Chen, Jun
  •   Yang, Dongjiang (external author)
  •   Zhu, Zhonghua (external author)
  •   Wang, Shuangyin (external author)
  •   Dai, Liming (external author)
  •   Yao, Xiangdong (external author)

Publication Date


  • 2019

Citation


  • Jia, Y., Zhang, L., Zhuang, L., Liu, H., Yan, X., Wang, X., Liu, J., Wang, J., Zheng, Y., Xiao, Z., Taran, E., Chen, J., Yang, D., Zhu, Z., Wang, S., Dai, L. & Yao, X. (2019). Identification of active sites for acidic oxygen reduction on carbon catalysts with and without nitrogen doping. Nature Catalysis, 2 688-695.

Scopus Eid


  • 2-s2.0-85068052512

Ro Full-text Url


  • https://ro.uow.edu.au/context/aiimpapers/article/4816/type/native/viewcontent

Ro Metadata Url


  • http://ro.uow.edu.au/aiimpapers/3761

Has Global Citation Frequency


Number Of Pages


  • 7

Start Page


  • 688

End Page


  • 695

Volume


  • 2

Place Of Publication


  • United Kingdom