A redox-active perylene-anthraquinone donor-acceptor conjugated microporous polymer with an unusual electron delocalization channel for photocatalytic reduction of uranium (VI) in strongly acidic solution

Achieving photoreduction uranium with D-A type conjugated microporous polymers in strongly acidic radioactive wastewater holds great promise but is extremely challenging, as it requires proper electron transport channels. Herein, a redox-active perylene-anthraquinone D−A conjugated microporous polym...

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Published in:Applied catalysis. B, Environmental Environmental, 2022-10, Vol.314, p.121467, Article 121467
Main Authors: Yu, Fengtao, Zhu, Zhiqiang, Li, Chuangye, Li, Wanru, Liang, Renping, Yu, Shanshan, Xu, Zhenzhen, Song, Fangru, Ren, Qiang, Zhang, Zhibin
Format: Article
Language:English
Subjects:
Anthraquinone
Anthraquinones
Charge transfer
Donor−acceptor
Electric fields
Electromagnetic absorption
Electron transfer
Electron transport
Holes (electron deficiencies)
Irradiation
Photocatalysis
Photocatalysts
Photoreduction
Photoreduction uranium
Polymers
Radiation
Radioactive wastewater
Radioactive wastewaters
Redox-active
Uranium
Uranium dioxide
Wastewater
Wastewater purification
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Summary:Achieving photoreduction uranium with D-A type conjugated microporous polymers in strongly acidic radioactive wastewater holds great promise but is extremely challenging, as it requires proper electron transport channels. Herein, a redox-active perylene-anthraquinone D−A conjugated microporous polymer photocatalyst (ECUT-AQ) which electron-rich perylene unit as donor and electron-deficient anthraquinone (AQ) as acceptor is innovatively reported. The results clearly demonstrates that AQ with dual characteristics of electron deficiency and redox activity plays a key role in photocatalytic reduction of UO22+ to UO2. On one hand, the constructed D-A structure induces the formation of a huge built-in electric field, which enhances the intramolecular charge transfer, thus significantly broadening visible light absorption range and improving electron-hole pairs separation efficiency. On the other hand, and very significantly, the redox-active AQ acts as a matched electron transfer channel, which further accelerates the photogenerated electrons transfer from the photocatalyst to the UO22+. Consequently, the ECUT-AQ achieves 86% photoreduction UO22+ removal within two hours irradiation and obtains an impressive reduction rate constant (k = 0.015 min-1, pH=1 and T = 293.15 K). Encouragingly, the current work can enlighten a whole new direction for the subsequent cultivation of more practical metal-free photocatalysts for purification radioactive wastewater. Herein, a redox-active perylene-anthraquinone D−A conjugated microporous polymer photocatalyst (ECUT-AQ) which perylene as donor and anthraquinone (AQ) as acceptor is innovatively reported. As a result, the ECUT-AQ exhibits highly AQ-dependent activity of visible-light-driven photoreduction of U(VI) to U(IV), realizing an impressive reduction rate constant (k = 0.015 min-1) in strong acid solution (pH=1). Such ECUT-AQ photocatalyst can not only broaden the absorption spectrum but also significantly boost photogenerated carrier separation, owing to the AQ unit has the dual characteristics of strong electron deficiency and redox activity, which separately induces a giant built-in electric field and builds an efficient electron delocalization channel. [Display omitted] •A redox-active D-A-type CMPs photocatalyst is innovatively applied to photoreduction of U(VI).•AQ with dual characteristics of electron deficiency and redox activity plays a key role in the photoreduction of UO22+ to UO2.•The integrated AQ can induce
ISSN:0926-3373
1873-3883
DOI:10.1016/j.apcatb.2022.121467