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author:

Tan, Yangyang (Tan, Yangyang.) [1] | Zhang, Zeyi (Zhang, Zeyi.) [2] | Chen, Suhao (Chen, Suhao.) [3] | Wu, Wei (Wu, Wei.) [4] | Yu, Liyue (Yu, Liyue.) [5] | Chen, Runzhe (Chen, Runzhe.) [6] | Guo, Fei (Guo, Fei.) [7] | Wang, Zichen (Wang, Zichen.) [8] | Cheng, Niancai (Cheng, Niancai.) [9] (Scholars:程年才)

Indexed by:

EI Scopus SCIE

Abstract:

Local geometric strain engineering is useful for modulating the performance of nitrogen-coordinated transition metal-carbon catalysts. However, realizing the nano-level strain is technically challenging. Additionally, the structure-property relationship between strain degree and performance remains poorly understood. Herein, it is conceptually predict that geometric bending induces more electron transfer from Zn to the coordinated N in ZnNC, leading to a positive shift of the d-band center of the Zn atom, which promotes the adsorption reduction process of the O-2 molecule and thus increases the intrinsic oxygen reduction reaction (ORR) activity. Moreover, a low-temperature non-saturated coordination strategy is proposed to prepare spherical porous carbon catalysts with surface-enriched geometrically bent (20-50(degrees)) ZnNC sites. Benefiting from the highly active ZnNC sites, large specific surface area and abundant pore structure, the optimized catalyst (SZnNC-950) exhibited excellent intrinsic alkaline ORR activity (half-wave potential E-1/2 = 0.89 V) and high zinc-air battery performance (peak power density of 229.2 mW cm(-2)), exceeding that of commercial Pt/C catalysts. Density functional theory (DFT) calculations show that when the geometrical bending angle is 30-45(degrees), Zn centers with suitable charge transfer to the surrounding N can produce a moderate adsorption strength to the oxygen intermediate state, resulting in optimal ORR activity.

Keyword:

bending strain DFT calculations low temperature unsaturated coordination oxygen reduction reaction ZnNx Sites

Community:

  • [ 1 ] [Tan, Yangyang]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 2 ] [Zhang, Zeyi]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 3 ] [Chen, Suhao]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 4 ] [Wu, Wei]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 5 ] [Yu, Liyue]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 6 ] [Chen, Runzhe]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 7 ] [Guo, Fei]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 8 ] [Wang, Zichen]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 9 ] [Cheng, Niancai]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China

Reprint 's Address:

  • [Cheng, Niancai]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China;;

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Source :

ADVANCED FUNCTIONAL MATERIALS

ISSN: 1616-301X

Year: 2024

Issue: 10

Volume: 34

1 8 . 5 0 0

JCR@2023

JCR Journal Grade:1

CAS Journal Grade:1

Cited Count:

WoS CC Cited Count: 19

SCOPUS Cited Count: 19

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 2

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