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A Defect-Driven Metal-free Electrocatalyst for Oxygen Reduction in Acidic Electrolyte

Journal Article


Abstract


  • Newly N-S-C coordination-structured active sites, originating from the integrity of edged thiophene S, graphitic N, and pentagon defects, were reconstructed by N-modified S defects in carbon aerogel with a 3D hierarchical macro-meso-microporous structure. This metal-free material exhibited outstanding oxygen reduction reaction (ORR) activity (e.g., half-wave potentials of 0.76 V in 0.5 M H2SO4 and 0.1 M HClO4; 0.85 V in 0.1 M KOH) with good stability and high current density in both acidic and alkaline electrolytes. The experimental and computational results reveal that the pentagon S defect is essential for the ORR in acidic electrolytes because it provides a remarkable increase in reactivity. One graphitic-type N in the meta-position of the pentagon defect further significantly improves the reactivity as a result of locally precise control of the electronic structure, thus forming highly active sites for ORR in acid.

Authors


  •   Li, Daohao (external author)
  •   Jia, Yi (external author)
  •   Chang, Guojing (external author)
  •   Chen, Jun
  •   Liu, Hongwei (external author)
  •   Wang, Jiancheng (external author)
  •   Hu, Yongfeng (external author)
  •   Xia, Yanzhi (external author)
  •   Yang, Dongjiang (external author)
  •   Yao, Xiangdong (external author)

Publication Date


  • 2018

Published In


Citation


  • Li, D., Jia, Y., Chang, G., Chen, J., Liu, H., Wang, J., Hu, Y., Xia, Y., Yang, D. & Yao, X. (2018). A Defect-Driven Metal-free Electrocatalyst for Oxygen Reduction in Acidic Electrolyte. Chem, 4 (10), 2345-2356.

Ro Metadata Url


  • http://ro.uow.edu.au/aiimpapers/3344

Number Of Pages


  • 11

Start Page


  • 2345

End Page


  • 2356

Volume


  • 4

Issue


  • 10

Place Of Publication


  • United States

Abstract


  • Newly N-S-C coordination-structured active sites, originating from the integrity of edged thiophene S, graphitic N, and pentagon defects, were reconstructed by N-modified S defects in carbon aerogel with a 3D hierarchical macro-meso-microporous structure. This metal-free material exhibited outstanding oxygen reduction reaction (ORR) activity (e.g., half-wave potentials of 0.76 V in 0.5 M H2SO4 and 0.1 M HClO4; 0.85 V in 0.1 M KOH) with good stability and high current density in both acidic and alkaline electrolytes. The experimental and computational results reveal that the pentagon S defect is essential for the ORR in acidic electrolytes because it provides a remarkable increase in reactivity. One graphitic-type N in the meta-position of the pentagon defect further significantly improves the reactivity as a result of locally precise control of the electronic structure, thus forming highly active sites for ORR in acid.

Authors


  •   Li, Daohao (external author)
  •   Jia, Yi (external author)
  •   Chang, Guojing (external author)
  •   Chen, Jun
  •   Liu, Hongwei (external author)
  •   Wang, Jiancheng (external author)
  •   Hu, Yongfeng (external author)
  •   Xia, Yanzhi (external author)
  •   Yang, Dongjiang (external author)
  •   Yao, Xiangdong (external author)

Publication Date


  • 2018

Published In


Citation


  • Li, D., Jia, Y., Chang, G., Chen, J., Liu, H., Wang, J., Hu, Y., Xia, Y., Yang, D. & Yao, X. (2018). A Defect-Driven Metal-free Electrocatalyst for Oxygen Reduction in Acidic Electrolyte. Chem, 4 (10), 2345-2356.

Ro Metadata Url


  • http://ro.uow.edu.au/aiimpapers/3344

Number Of Pages


  • 11

Start Page


  • 2345

End Page


  • 2356

Volume


  • 4

Issue


  • 10

Place Of Publication


  • United States