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Edge-Rich Fe−N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis

Journal Article


Abstract


  • © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Controllably constructing nitrogen-modified divacancies (ND) in carbon substrates to immobilize atomic Fe species and unveiling the advantageous configuration is still challenging, but indispensable for attaining optimal Fe−N−C catalysts for the oxygen reduction reaction (ORR). Herein, a fundamental investigation of unfolding intrinsically superior edge-ND trapped atomic Fe motifs (e-ND−Fe) relative to an intact center model (c-ND−Fe) in ORR electrocatalysis is reported. Density functional theory calculations reveal that local electronic redistribution and bandgap shrinkage for e-ND−Fe endow it with a lower free-energy barrier toward direct four-electron ORR. Inspired by this, a series of atomic Fe catalysts with adjustable ND−Fe coordination are synthesized, which verify that ORR performance highly depends on the concentration of e-ND−Fe species. Remarkably, the best e-ND−Fe catalyst delivers a favorable kinetic current density and halfwave potential that can be comparable to benchmark Pt−C under acidic conditions. This work will guide to develop highly active atomic metal catalysts through rational defect engineering.

Authors


  •   Wang, Xin (external author)
  •   Jia, Yi (external author)
  •   Mao, Xin (external author)
  •   Liu, Daobin (external author)
  •   He, Wenxiang (external author)
  •   Li, Jia (external author)
  •   Liu, Jianguo (external author)
  •   Yan, Xuecheng (external author)
  •   Chen, Jun
  •   Song, Li (external author)
  •   Du, Aijun (external author)
  •   Yao, Xiangdong (external author)

Publication Date


  • 2020

Citation


  • Wang, X., Jia, Y., Mao, X., Liu, D., He, W., Li, J., Liu, J., Yan, X., Chen, J., Song, L., Du, A. & Yao, X. (2020). Edge-Rich Fe−N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis. Advanced Materials,

Scopus Eid


  • 2-s2.0-85080940834

Place Of Publication


  • Germany

Abstract


  • © 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim Controllably constructing nitrogen-modified divacancies (ND) in carbon substrates to immobilize atomic Fe species and unveiling the advantageous configuration is still challenging, but indispensable for attaining optimal Fe−N−C catalysts for the oxygen reduction reaction (ORR). Herein, a fundamental investigation of unfolding intrinsically superior edge-ND trapped atomic Fe motifs (e-ND−Fe) relative to an intact center model (c-ND−Fe) in ORR electrocatalysis is reported. Density functional theory calculations reveal that local electronic redistribution and bandgap shrinkage for e-ND−Fe endow it with a lower free-energy barrier toward direct four-electron ORR. Inspired by this, a series of atomic Fe catalysts with adjustable ND−Fe coordination are synthesized, which verify that ORR performance highly depends on the concentration of e-ND−Fe species. Remarkably, the best e-ND−Fe catalyst delivers a favorable kinetic current density and halfwave potential that can be comparable to benchmark Pt−C under acidic conditions. This work will guide to develop highly active atomic metal catalysts through rational defect engineering.

Authors


  •   Wang, Xin (external author)
  •   Jia, Yi (external author)
  •   Mao, Xin (external author)
  •   Liu, Daobin (external author)
  •   He, Wenxiang (external author)
  •   Li, Jia (external author)
  •   Liu, Jianguo (external author)
  •   Yan, Xuecheng (external author)
  •   Chen, Jun
  •   Song, Li (external author)
  •   Du, Aijun (external author)
  •   Yao, Xiangdong (external author)

Publication Date


  • 2020

Citation


  • Wang, X., Jia, Y., Mao, X., Liu, D., He, W., Li, J., Liu, J., Yan, X., Chen, J., Song, L., Du, A. & Yao, X. (2020). Edge-Rich Fe−N4 Active Sites in Defective Carbon for Oxygen Reduction Catalysis. Advanced Materials,

Scopus Eid


  • 2-s2.0-85080940834

Place Of Publication


  • Germany