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Author:

Hou, Jixiang (Hou, Jixiang.) | Wang, Kaiwen (Wang, Kaiwen.) | Zhang, Xu (Zhang, Xu.) | Wang, Yang (Wang, Yang.) | Su, Hui (Su, Hui.) | Yang, Chenyu (Yang, Chenyu.) | Zhou, Xiyuan (Zhou, Xiyuan.) | Liu, Wenning (Liu, Wenning.) | Hu, Hanwei (Hu, Hanwei.) | Wang, Jiaxing (Wang, Jiaxing.) | Li, Chen (Li, Chen.) | Ma, Peijie (Ma, Peijie.) | Zhang, Rui (Zhang, Rui.) | Wei, Zhen (Wei, Zhen.) | Sun, Zaicheng (Sun, Zaicheng.) | Liu, Qinghua (Liu, Qinghua.) | Zheng, Kun (Zheng, Kun.) (Scholars:郑坤)

Indexed by:

EI Scopus SCIE

Abstract:

The photocatalytic two-electron O-2 reduction reaction (2e(-) ORR) for high-value hydrogen peroxide (H2O2) production is attracting widespread attention as a green and promising research pathway. Despite multiple optimization strategies, the current 2e(-) ORR systems remain constrained by photogenerated carrier recombination and slow O-2 reduction kinetics. Therefore, a refined photocatalyst design is urgently needed to overcome these constraints, enabling enhanced H2O2 activity and deeper exploration of reaction mechanisms. Here, we design surface defect sites (N vacancies) and oxygen-affine CoOx nanoclusters on polymeric carbon nitride (CN) to break through the above limitations for enhanced photocatalytic H2O2 production. The introduction of N vacancies significantly enhances the photogenerated carrier separation, and highly active CoOx nanoclusters optimize the surface reaction process from O-2 to H2O2, synergistically improving the activity and selectivity of H2O2 production. The designed photocatalyst (CoOx-NvCN) achieves a H2O2 production rate of 244.8 mu mol L-1 h(-1) in pure water, with an apparent quantum yield (AQY) of 5.73% at 420 nm and a solar-to-chemical energy conversion (SCC) efficiency of 0.47%, surpassing previously reported CN-based photocatalysts. Importantly, experiments and theoretical calculations reveal that N vacancies optimize the photoelectronic response characteristics of the CN substrate, while the CoOx nanoclusters promote O-2 adsorption and activation, reducing the formation energy barrier for crucial intermediate *OOH, thereby accelerating H2O2 generation. This work provides a feasible approach to the photocatalyst design strategy that simultaneously facilitates photogenerated carrier separation and effective active sites for high-performance H2O2 production.

Keyword:

polymeric carbon nitride photocatalytic H2O2 production metaloxide nanocluster oxygen reduction reaction nitrogen defect

Author Community:

  • [ 1 ] [Hou, Jixiang]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 2 ] [Zhang, Xu]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 3 ] [Zhou, Xiyuan]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 4 ] [Hu, Hanwei]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 5 ] [Wang, Jiaxing]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 6 ] [Li, Chen]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 7 ] [Ma, Peijie]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 8 ] [Zhang, Rui]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 9 ] [Zheng, Kun]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China
  • [ 10 ] [Wang, Kaiwen]Barcelona Inst Sci & Technol, ICFO Inst Ciencies Foton, Castelldefels 08860, Barcelona, Spain
  • [ 11 ] [Wang, Yang]Chongqing Univ Posts & Telecommun, Sch Optoelect Engn, Chongqing 400065, Peoples R China
  • [ 12 ] [Su, Hui]Hunan Normal Univ, Key Lab Light Energy Convers Mat Hunan Prov Coll, Coll Chem & Chem Engn, Changsha 410081, Hunan, Peoples R China
  • [ 13 ] [Yang, Chenyu]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
  • [ 14 ] [Liu, Qinghua]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
  • [ 15 ] [Liu, Wenning]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 16 ] [Wei, Zhen]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China
  • [ 17 ] [Sun, Zaicheng]Beijing Univ Technol, Beijing Key Lab Green Catalysis & Separat, Beijing 100124, Peoples R China

Reprint Author's Address:

  • [Zhang, Xu]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China;;[Zheng, Kun]Beijing Univ Technol, Beijing Key Lab Microstruct & Properties Solids, Beijing 100124, Peoples R China;;

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Source :

ACS CATALYSIS

ISSN: 2155-5435

Year: 2024

Issue: 14

Volume: 14

Page: 10893-10903

1 2 . 9 0 0

JCR@2022

Cited Count:

WoS CC Cited Count: 9

SCOPUS Cited Count: 21

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 3

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