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author:

Zeng, Yuan (Zeng, Yuan.) [1] | Tan, Xin (Tan, Xin.) [2] (Scholars:谈鑫) | Zhuang, Zewen (Zhuang, Zewen.) [3] (Scholars:庄泽文) | Chen, Chen (Chen, Chen.) [4] | Peng, Qing (Peng, Qing.) [5]

Indexed by:

EI Scopus SCIE

Abstract:

The two-electron oxygen reduction reaction (2e- ORR) is a pivotal pathway for the distributed production of hydrogen peroxide (H2O2). In nature, enzymes containing manganese (Mn) centers can convert reactive oxygen species into H2O2. However, Mn-based heterogeneous catalysts for 2e- ORR are scarcely reported. Herein, we developed a nature-inspired single-atom electrocatalyst comprising N, O co-coordinated Mn sites, utilizing carbon dots as the modulation platform (Mn CD/C). As-synthesized Mn CD/C exhibited exceptional 2e- ORR activity with an onset potential of 0.786 V and a maximum H2O2 selectivity of 95.8 %. Impressively, Mn CD/C continuously produced 0.1 M H2O2 solution at 200 mA/cm2 for 50 h in the flow cell, with negligible loss in activity and H2O2 faradaic efficiency, demonstrating practical application potential. The enhanced activity was attributed to the incorporation of Mn atomic sites into the carbon dots. Theoretical calculations revealed that the N, O co-coordinated structure, combined with abundant oxygen-containing functional groups on the carbon dots, optimized the binding strength of intermediate *OOH at the Mn sites to the apex of the catalytic activity volcano. This work illustrates that carbon dots can serve as a versatile platform for modulating the microenvironment of single-atom catalysts and for the rational design of nature-inspired catalysts.

Keyword:

carbon dots electrocatalysis hydrogen peroxide interfacial regulation single-atom catalysts

Community:

  • [ 1 ] [Zeng, Yuan]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China
  • [ 2 ] [Tan, Xin]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China
  • [ 3 ] [Chen, Chen]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China
  • [ 4 ] [Peng, Qing]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China
  • [ 5 ] [Tan, Xin]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 6 ] [Zhuang, Zewen]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China

Reprint 's Address:

  • 庄泽文

    [Chen, Chen]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China;;[Peng, Qing]Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Beijing 100084, Peoples R China;;[Zhuang, Zewen]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

ISSN: 1433-7851

Year: 2024

Issue: 4

Volume: 64

1 6 . 1 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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