期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 314, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2022.121467
关键词
Redox-active; Donor-acceptor; Anthraquinone; Photoreduction uranium; Radioactive wastewater
资金
- National Natural Science Foundation of China [22105034, 21866004, 22066003]
- Jiangxi Provincial Natural Science Foundation [20202BABL213027]
- Research Foundation for Advanced Talents of East China University of Technology [DHBK2019138]
- National College Students Innovation and Entrepreneurship Training Program [202110405015]
This study reports a novel D-A type conjugated microporous polymer photocatalyst (ECUT-AQ) for photoreduction of uranium in strongly acidic radioactive wastewater. The ECUT-AQ photocatalyst, with its electron-rich perylene unit as donor and electron-deficient anthraquinone (AQ) as acceptor, exhibits excellent electron transport channels and redox activity. The photocatalyst effectively broadens the light absorption range, improves electron-hole pairs separation efficiency, and accelerates electron transfer to UO22+, achieving a high photoreduction rate.
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.
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