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Author:

Wang, Yifei (Wang, Yifei.) | Li, Beibei (Li, Beibei.) | Chen, Guangheng (Chen, Guangheng.) | Wu, Yuhan (Wu, Yuhan.) | Tian, Meng (Tian, Meng.) | Peng, Yongzhen (Peng, Yongzhen.) | Dou, Shixue (Dou, Shixue.) | Li, Laiquan (Li, Laiquan.) | Sun, Jingyu (Sun, Jingyu.)

Indexed by:

EI Scopus SCIE

Abstract:

Hydrogen peroxide (H2O2) electrosynthesis using metal-free carbon materials via the 2e(-) oxygen reduction pathway has sparked considerable research interest. However, the scalable preparation of carbon electrocatalysts to achieve satisfactory H2O2 yield in acidic media remains a grand challenge. Here, we present the design of a carbon nanoreactor series that integrates precise O/N codoping alongside well-regulated geometric structures targeting high-efficiency electrosynthesis of H2O2. Theoretical computations reveal that strategic N/O codoping facilitates partial electron transfer from C sites to O sites, realizing electronic rearrangement that optimizes C-site adsorption of *OOH. Concurrently, the O-O bond in *OOH is strengthened by charge transfer from antibonding to pi-orbitals, stabilizing the O-O bond and preventing its dissociation. The carbon nanoreactor with a hollow bowl geometry also facilitates the mass transport of O-2 and H2O2, achieving an H2O2 selectivity of 96% in acidic media. Furthermore, a flow cell integrated with the refined nanoreactor catalyst achieves an impressive H2O2 production rate of 2942.4 mg L-1 h(-1), coupled with stable operation of nearly 80 h, surpassing the state-of-the-art metal-free analogs. The feasibility of the electro-synthesized H2O2 is further demonstrated to be highly efficient in wastewater remediation.

Keyword:

H2O2 electrosynthesis Water remediation Metal-free carbon catalyst Geometricmodification N-O codoping

Author Community:

  • [ 1 ] [Wang, Yifei]Beijing Univ Technol, Natl Engn Lab Adv Municipal Wastewater Treatment &, Key Lab Beijing Water Qual Sci & Water Environm Re, Beijing 100124, Peoples R China
  • [ 2 ] [Li, Beibei]Beijing Univ Technol, Natl Engn Lab Adv Municipal Wastewater Treatment &, Key Lab Beijing Water Qual Sci & Water Environm Re, Beijing 100124, Peoples R China
  • [ 3 ] [Chen, Guangheng]Beijing Univ Technol, Natl Engn Lab Adv Municipal Wastewater Treatment &, Key Lab Beijing Water Qual Sci & Water Environm Re, Beijing 100124, Peoples R China
  • [ 4 ] [Peng, Yongzhen]Beijing Univ Technol, Natl Engn Lab Adv Municipal Wastewater Treatment &, Key Lab Beijing Water Qual Sci & Water Environm Re, Beijing 100124, Peoples R China
  • [ 5 ] [Wu, Yuhan]Soochow Univ, Soochow Inst Energy & Mat Innovat, Coll Energy, Key Lab Adv Carbon Mat & Wearable Energy Technol J, Suzhou 215006, Peoples R China
  • [ 6 ] [Sun, Jingyu]Soochow Univ, Soochow Inst Energy & Mat Innovat, Coll Energy, Key Lab Adv Carbon Mat & Wearable Energy Technol J, Suzhou 215006, Peoples R China
  • [ 7 ] [Tian, Meng]Nanjing Univ Sci & Technol, Sch New Energy, Jiangyin 214443, Jiangsu, Peoples R China
  • [ 8 ] [Dou, Shixue]Univ Shanghai Sci & Technol, Inst Energy Mat Sci, Shanghai 200093, Peoples R China
  • [ 9 ] [Li, Laiquan]Univ Shanghai Sci & Technol, Inst Energy Mat Sci, Shanghai 200093, Peoples R China

Reprint Author's Address:

  • 王艺霏

    [Wang, Yifei]Beijing Univ Technol, Natl Engn Lab Adv Municipal Wastewater Treatment &, Key Lab Beijing Water Qual Sci & Water Environm Re, Beijing 100124, Peoples R China;;[Sun, Jingyu]Soochow Univ, Soochow Inst Energy & Mat Innovat, Coll Energy, Key Lab Adv Carbon Mat & Wearable Energy Technol J, Suzhou 215006, Peoples R China;;[Tian, Meng]Nanjing Univ Sci & Technol, Sch New Energy, Jiangyin 214443, Jiangsu, Peoples R China;;[Li, Laiquan]Univ Shanghai Sci & Technol, Inst Energy Mat Sci, Shanghai 200093, Peoples R China

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Source :

ENVIRONMENTAL SCIENCE & TECHNOLOGY

ISSN: 0013-936X

Year: 2024

Issue: 49

Volume: 58

Page: 21893-21903

1 1 . 4 0 0

JCR@2022

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: 14

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