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Published on: April 28, 2023
Covalent-Organic Framework with Unconventional D-D Structure for Efficient Photocatalytic Uranium Extraction
Dongyang Xu1,2, Xin Du2, Bingyue Zhou2
1Key Laboratory of Nuclear Facility Decommissioning and Ecological Restoration of the Ministry of Ecology and Environment, School of Resources Environment and Safety Engineering, Hunan Provincial Engineering Research Center for Safety Control and Recycling of Radioactive Heavy Metal Pollutants, University of South China, 28 Changsheng West Road, Hengyang 421001, China.
A novel donor-donor covalent-organic framework (D-D COF) efficiently removes uranium from wastewater. This D-D COF shows high uranium uptake capacity and removal efficiency, offering a new strategy for nuclear wastewater treatment.
Area of Science:
- Environmental Science
- Materials Science
- Chemistry
Background:
- Photocatalytic uranium extraction from radioactive wastewater is vital for environmental safety and nuclear energy.
- Donor-acceptor (D-A) and D-π-A photocatalysts are known for efficient charge separation and performance.
- Donor-donor (D-D) photocatalysts are typically considered less active, posing a challenge for uranium recovery.
Purpose of the Study:
- To present a counterintuitive design of a D-D covalent-organic framework (COF) for efficient photocatalytic uranium extraction.
- To challenge the conventional understanding of D-D COF activity in photocatalysis.
- To develop an effective strategy for uranium recovery from nuclear wastewater.
Main Methods:
- Synthesis of a twisted D-D COF (COF-BCTB-Py) using bicarbazole and pyrene via solvothermal condensation.
- Characterization of the COF's structure, surface area, band gap, and stability (chemical, thermal, radiation).
- Evaluation of photocatalytic uranium extraction efficiency in complex water matrices with methanol as a co-reductant.
Main Results:
- The synthesized COF-BCTB-Py exhibited an AA-stacked porous structure, high surface area (963 m²·g⁻¹), a 2.44 eV band gap, and excellent stability.
- Achieved an ultrahigh uranium uptake capacity of 4278 mg·g⁻¹ with >97% removal efficiency and fast kinetics.
- Mechanistic studies indicated U(VI) conversion to crystalline (UO₂)O₂·2H₂O via in situ generated hydrogen peroxide.
Conclusions:
- The D-D COF design is an unconventional and effective strategy for uranium recovery.
- This work demonstrates high photocatalytic activity for D-D COFs, overcoming previous limitations.
- The developed photocatalyst offers a promising solution for safe and efficient uranium extraction from nuclear wastewater.
