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author:

Luo, Laiyu (Luo, Laiyu.) [1] | Wu, Qinglong (Wu, Qinglong.) [2] | Wang, Siyu (Wang, Siyu.) [3] | Song, Haojie (Song, Haojie.) [4] | Li, Jiaqi (Li, Jiaqi.) [5] | Zhang, Liping (Zhang, Liping.) [6] | Zhang, Qun (Zhang, Qun.) [7] | Fang, Yuanxing (Fang, Yuanxing.) [8] (Scholars:方元行) | Jiang, Baojiang (Jiang, Baojiang.) [9] | Wang, Xinchen (Wang, Xinchen.) [10]

Indexed by:

Scopus SCIE

Abstract:

Poly(heptazine imide) (PHI) is a promising photocatalyst for hydrogen peroxide (H2O2) production; however, enhancing its specific surface area to expose internal active sites and understanding their roles in key mechanistic steps for the H2O2 synthesis remain challenging. Here, we utilized organic cations to exfoliate bulk PHI and fabricate PHI nanosheets for producing H2O2 at a rate of 27.35 mmol g-1 h-1 under simulated solar light irradiation, outperforming most of the reported carbon nitride-based catalysts. Importantly, after 36 h of cyclic accumulation reactions in a self-created spiral flow reactor, the H2O2 concentration stabilized at 2.7 wt.%, close to medical sterilization levels. In situ spectroscopic characterizations and density functional theory calculations revealed that the exfoliation results in molecular reconfiguration of the PHI basal planes, forming the active sites to promote charge separation and electron localization. This new structure also creates midgap states, enabling direct H2O2 production via a one-step, two-electron pathway, bypassing the superoxide radical pathway. Theoretical calculations suggest that the localized electronic structure created by the active sites favors the protonation of adsorbed O2 and stabilizes the *OOH species, which converts to H2O2. This study elucidates and underscores the importance of active-site reconfiguration for efficient photocatalytic oxygen reduction reaction (ORR) pathways.

Keyword:

Electron transport Hydrogen peroxide synthesis Ion exchange Photocatalysis Poly(heptazine imide) nanosheets

Community:

  • [ 1 ] [Luo, Laiyu]Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China
  • [ 2 ] [Wang, Siyu]Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China
  • [ 3 ] [Song, Haojie]Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China
  • [ 4 ] [Li, Jiaqi]Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China
  • [ 5 ] [Jiang, Baojiang]Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China
  • [ 6 ] [Fang, Yuanxing]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 7 ] [Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 8 ] [Wu, Qinglong]Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Dept Chem Phys, Hefei 230026, Peoples R China
  • [ 9 ] [Zhang, Qun]Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Dept Chem Phys, Hefei 230026, Peoples R China
  • [ 10 ] [Wu, Qinglong]Univ Sci & Technol China, Hefei Natl Lab, Hefei 230088, Peoples R China
  • [ 11 ] [Zhang, Qun]Univ Sci & Technol China, Hefei Natl Lab, Hefei 230088, Peoples R China
  • [ 12 ] [Zhang, Liping]Shenzhen MSU BIT Univ, Fac Mat Sci, Shenzhen 518172, Peoples R China

Reprint 's Address:

  • 方元行

    [Jiang, Baojiang]Heilongjiang Univ, Key Lab Funct Inorgan Mat Chem, Minist Educ Peoples Republ China, Harbin 150080, Peoples R China;;[Fang, Yuanxing]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China;;[Wang, Xinchen]Fuzhou Univ, Coll Chem, State Key Lab Chem NBC Hazards Protect, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China;;[Zhang, Qun]Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Dept Chem Phys, Hefei 230026, Peoples R China;;[Zhang, Qun]Univ Sci & Technol China, Hefei Natl Lab, Hefei 230088, Peoples R China

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Source :

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

Year: 2025

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: 2

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