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author:

Wang, Feiteng (Wang, Feiteng.) [1] | Zhou, Yipeng (Zhou, Yipeng.) [2] | Lin, Sen (Lin, Sen.) [3] (Scholars:林森) | Yang, Lijun (Yang, Lijun.) [4] | Hu, Zheng (Hu, Zheng.) [5] | Xie, Daiqian (Xie, Daiqian.) [6]

Indexed by:

EI Scopus SCIE

Abstract:

Iron and nitrogen co-doped carbons (Fe-N-C) have comparable activity to Pt-based catalysts for oxygen reduction reaction (ORR), but with much poorer durability in acidic electrolytes. Recently, regulating the coordination environment of Fe center (in-plane or axially) to boost the ORR activity of Fe-N-C has attracted many interests, and the axial OH ligand is even regarded as a necessary part of a highly-active structure. However, the influence of these regulations on the stability is still not clear. Herein, we performed kinetic and thermodynamic calculations based on density functional theory with explicit consideration of electrode potential to study the OH axial ligand effect on the stability of Fe-N-C electrocatalysts. We found that although the OH ligand can enhance the ORR onset potential to some extent, it substantially increases the H2O2 selectivity, pushing ORR diverted to the 2e+ 2e-pathway. In the latter 2e-process (H2O2 reduction), harmful hydroxyl radicals could be produced upon H2O2 dissociation. Therefore, from the perspective of catalysts' stability, OH ligand coordination on the metal center is not a good way to develop stable ORR catalysts.

Keyword:

Fe-N-C electrocatalysts First-principle modeling Oxygen reduction reaction Potential dependent kinetic study Stability

Community:

  • [ 1 ] [Wang, Feiteng]Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
  • [ 2 ] [Zhou, Yipeng]Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
  • [ 3 ] [Yang, Lijun]Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
  • [ 4 ] [Hu, Zheng]Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
  • [ 5 ] [Xie, Daiqian]Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China
  • [ 6 ] [Lin, Sen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350002, Peoples R China

Reprint 's Address:

  • [Yang, Lijun]Nanjing Univ, Sch Chem & Chem Engn, Key Lab Mesoscop Chem MOE, Nanjing 210023, Peoples R China

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Source :

NANO ENERGY

ISSN: 2211-2855

Year: 2020

Volume: 78

1 7 . 8 8 1

JCR@2020

1 6 . 8 0 0

JCR@2023

ESI Discipline: MATERIALS SCIENCE;

ESI HC Threshold:196

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 78

SCOPUS Cited Count: 76

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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