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Overall solar H2O2 generation in water and real seawater by covalent organic frameworks with kgd topology.

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Title: Overall solar H2O2 generation in water and real seawater by covalent organic frameworks with kgd topology.
Authors: Yue, Jie-Yu1 (AUTHOR) yuejieyu@sdnu.edu.cn, Song, Li-Ping1 (AUTHOR), Pan, Zi-Xian1 (AUTHOR), Cheng, Min2 (AUTHOR), Wang, Xuan2 (AUTHOR), Xu, Qing1,3 (AUTHOR) xuqing@sari.ac.cn, Yang, Peng1 (AUTHOR) yangpeng@sdnu.edu.cn
Source: Chemical Engineering Journal. Jan2025, Vol. 504, pN.PAG-N.PAG. 1p.
Subjects: Oxidation-reduction reaction, Escherichia coli, Activation energy, Oxidation of water, Oxygen reduction
Abstract: Two innovative covalent organic frameworks (COFs) with kgd topology are constructed for photocatalytic H 2 O 2 formation for the first time, realizing overall H 2 O 2 generation in water and real seawater with high production rates via the oxygen reduction reaction and the water oxidation reaction among the best COF-based photocatalysts, inspiring the photocatalytic performance modulation by topology design. [Display omitted] • Two novel COFs with kgd topology (TPT-COF and TPB-COF) were constructed for H 2 O 2 generation for the first time. • In pure water and real seawater, TPT-COF and TPB-COF exhibited superior H 2 O 2 generation rates, among the best organic photocatalysts, manifesting a potential sustainable blueprint for making H 2 O 2. • Experimental and theoretical investigations proved that TPT-COF and TPB-COF can drive the overall solar H 2 O 2 generation via O 2 -O 2 −-H 2 O 2 , O 2 -O 2 −-O 2 1-H 2 O 2 , and H 2 O-H 2 O 2 three pathways. • The seawater-produced H 2 O 2 can be utilized for E. coli sterilization, providing a guide for the sustainable use of seawater for high-value chemical production. Applying covalent organic frameworks (COFs) for photosynthesizing H 2 O 2 has garnered significant research interest due to their customizable structures and functions. Nevertheless, there is still much room to tailor the structures of COFs to achieve high H 2 O 2 yields, fulfilling the future industrial requirements for massive and green H 2 O 2 generation. Herein, by topology design, we fabricate two novel COFs with kgd topology for H 2 O 2 production. In pure water and O 2 , the non-sacrificial H 2 O 2 evolution rates of TPT-COF and TPB-COF are 5903 and 7874 μmol g−1h−1 (4006 and 5696 μmol g−1h−1 in real seawater), outperforming their counterparts with hcb topology, ranking ahead of COF-based photocatalysts. Thorough experimental and computational inspections corroborate the indirect 2e− oxygen reduction and direct 2e− water oxidation paths of TPT-COF and TPB-COF for overall H 2 O 2 photogeneration. The boosted charge carrier separation, easier adsorption of O 2 and water, and lower energy barriers of the formation of *OOH and *OH intermediates in TPB-COF make it a superior photocatalyst for producing H 2 O 2 than TPT-COF. This is the first time COFs with kgd topology are constructed towards H 2 O 2 synthesis, inspiring the photocatalytic performance modulation by topology design. Additionally, the seawater-produced H 2 O 2 can be exploited for sterilization, enlightening a blueprint for sustainable utilizing seawater for high-value chemicals. [ABSTRACT FROM AUTHOR]
Copyright of Chemical Engineering Journal is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Label: Title
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  Data: Overall solar H2O2 generation in water and real seawater by covalent organic frameworks with kgd topology.
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  Data: <searchLink fieldCode="AR" term="%22Yue%2C+Jie-Yu%22">Yue, Jie-Yu</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> yuejieyu@sdnu.edu.cn</i><br /><searchLink fieldCode="AR" term="%22Song%2C+Li-Ping%22">Song, Li-Ping</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Pan%2C+Zi-Xian%22">Pan, Zi-Xian</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Cheng%2C+Min%22">Cheng, Min</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Wang%2C+Xuan%22">Wang, Xuan</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Xu%2C+Qing%22">Xu, Qing</searchLink><relatesTo>1,3</relatesTo> (AUTHOR)<i> xuqing@sari.ac.cn</i><br /><searchLink fieldCode="AR" term="%22Yang%2C+Peng%22">Yang, Peng</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> yangpeng@sdnu.edu.cn</i>
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  Data: <searchLink fieldCode="JN" term="%22Chemical+Engineering+Journal%22">Chemical Engineering Journal</searchLink>. Jan2025, Vol. 504, pN.PAG-N.PAG. 1p.
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  Data: <searchLink fieldCode="DE" term="%22Oxidation-reduction+reaction%22">Oxidation-reduction reaction</searchLink><br /><searchLink fieldCode="DE" term="%22Escherichia+coli%22">Escherichia coli</searchLink><br /><searchLink fieldCode="DE" term="%22Activation+energy%22">Activation energy</searchLink><br /><searchLink fieldCode="DE" term="%22Oxidation+of+water%22">Oxidation of water</searchLink><br /><searchLink fieldCode="DE" term="%22Oxygen+reduction%22">Oxygen reduction</searchLink>
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: Two innovative covalent organic frameworks (COFs) with kgd topology are constructed for photocatalytic H 2 O 2 formation for the first time, realizing overall H 2 O 2 generation in water and real seawater with high production rates via the oxygen reduction reaction and the water oxidation reaction among the best COF-based photocatalysts, inspiring the photocatalytic performance modulation by topology design. [Display omitted] • Two novel COFs with kgd topology (TPT-COF and TPB-COF) were constructed for H 2 O 2 generation for the first time. • In pure water and real seawater, TPT-COF and TPB-COF exhibited superior H 2 O 2 generation rates, among the best organic photocatalysts, manifesting a potential sustainable blueprint for making H 2 O 2. • Experimental and theoretical investigations proved that TPT-COF and TPB-COF can drive the overall solar H 2 O 2 generation via O 2 -O 2 −-H 2 O 2 , O 2 -O 2 −-O 2 1-H 2 O 2 , and H 2 O-H 2 O 2 three pathways. • The seawater-produced H 2 O 2 can be utilized for E. coli sterilization, providing a guide for the sustainable use of seawater for high-value chemical production. Applying covalent organic frameworks (COFs) for photosynthesizing H 2 O 2 has garnered significant research interest due to their customizable structures and functions. Nevertheless, there is still much room to tailor the structures of COFs to achieve high H 2 O 2 yields, fulfilling the future industrial requirements for massive and green H 2 O 2 generation. Herein, by topology design, we fabricate two novel COFs with kgd topology for H 2 O 2 production. In pure water and O 2 , the non-sacrificial H 2 O 2 evolution rates of TPT-COF and TPB-COF are 5903 and 7874 μmol g−1h−1 (4006 and 5696 μmol g−1h−1 in real seawater), outperforming their counterparts with hcb topology, ranking ahead of COF-based photocatalysts. Thorough experimental and computational inspections corroborate the indirect 2e− oxygen reduction and direct 2e− water oxidation paths of TPT-COF and TPB-COF for overall H 2 O 2 photogeneration. The boosted charge carrier separation, easier adsorption of O 2 and water, and lower energy barriers of the formation of *OOH and *OH intermediates in TPB-COF make it a superior photocatalyst for producing H 2 O 2 than TPT-COF. This is the first time COFs with kgd topology are constructed towards H 2 O 2 synthesis, inspiring the photocatalytic performance modulation by topology design. Additionally, the seawater-produced H 2 O 2 can be exploited for sterilization, enlightening a blueprint for sustainable utilizing seawater for high-value chemicals. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Chemical Engineering Journal is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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RecordInfo BibRecord:
  BibEntity:
    Identifiers:
      – Type: doi
        Value: 10.1016/j.cej.2024.158983
    Languages:
      – Code: eng
        Text: English
    PhysicalDescription:
      Pagination:
        PageCount: 1
        StartPage: N.PAG
    Subjects:
      – SubjectFull: Oxidation-reduction reaction
        Type: general
      – SubjectFull: Escherichia coli
        Type: general
      – SubjectFull: Activation energy
        Type: general
      – SubjectFull: Oxidation of water
        Type: general
      – SubjectFull: Oxygen reduction
        Type: general
    Titles:
      – TitleFull: Overall solar H2O2 generation in water and real seawater by covalent organic frameworks with kgd topology.
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            NameFull: Yue, Jie-Yu
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            NameFull: Song, Li-Ping
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            NameFull: Pan, Zi-Xian
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            NameFull: Wang, Xuan
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              M: 01
              Text: Jan2025
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              Y: 2025
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