Key Takeaways & Executive Findings
- •• • ECUT-COF-152 achieves 100% U(VI) removal and a maximum reduction capacity of 1950 mg g−1 under visible light, outperforming many reported photocatalysts and enabling efficient uranium recovery from wastewater. • • The D-A architecture with TP as donor and 1,4-DQ/1,5-DQ as acceptors extends electron transfer distance, reducing electron-hole recombination and boosting photocatalytic efficiency. • • The design eliminates the need for additional functional groups, simplifying synthesis while maintaining high crystallinity and porosity, which is critical for scalable production. • • The work provides a clear structure-property relationship: adjusting the connection mode of building units directly modulates electron transport, offering a general strategy for designing high-performance COF photocatalysts.
Abstract
Photocatalytic reduction of soluble U(VI) to insoluble U(IV) is a pivotal technology for uranium remediation and resource recovery. However, conventional covalent organic frameworks (COFs) suffer from short-range electron transport, leading to rapid electron-hole recombination and limited efficiency. Here, we report the rational design of anthraquinone-based COFs with donor-acceptor (D-A) architectures, employing 2,4,6-triformylphloroglucinol (TP) as the donor and 1,4-diaminoanthraquinone (1,4-DQ) or 1,5-diaminoanthraquinone (1,5-DQ) as the acceptor. By varying the connection mode of the building units, the electron transfer distance is systematically extended, effectively suppressing charge recombination. Among the synthesized COFs, ECUT-COF-152 exhibits optimal photocatalytic activity under visible light, achieving 100% U(VI) removal with a maximum reduction capacity of 1950 mg g−1. This work demonstrates that precise tuning of the D-A structure and electron transfer pathways is an effective strategy to enhance the photocatalytic performance of COFs for uranium reduction, offering insights for the design of efficient materials for nuclear waste treatment.
1. Introduction
Nuclear energy, despite its high energy density and low carbon emissions, generates uranium-containing wastewater throughout its lifecycle, posing severe environmental and health risks due to uranium's radioactivity and chemical toxicity. Conventional remediation technologies such as adsorption and electrochemical extraction face limitations in selectivity, energy consumption, or secondary waste generation. Photocatalytic reduction of soluble U(VI) to insoluble U(IV) has emerged as a promising green approach, but its efficiency is often constrained by the rapid recombination of photogenerated electron-hole pairs in conventional photocatalysts.
Covalent organic frameworks (COFs) offer tunable crystallinity, porosity, and functionalization, making them attractive for photocatalysis. However, their inherent short-range electron transport limits charge separation. This work addresses this bottleneck by constructing anthraquinone-based COFs with donor-acceptor architectures, where the electron transfer distance is deliberately extended by altering the connection mode of building units. This design suppresses recombination and significantly enhances U(VI) photoreduction, achieving near-complete removal and record capacity, thereby advancing the practical application of COFs in nuclear waste treatment.
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Tianhao Lei, Xianqing Xie, Zhongsheng Chen, Zhiwu Yu, Feng Luo (2026). Regulating the Distance of Electron Transfer in Anthraquinone-Based Covalent Organic Framework for Efficient Photocatalytic U(VI) Reduction. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3971-6
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Frequently Asked Questions
What is the maximum U(VI) reduction capacity of ECUT-COF-152 and under what conditions?
ECUT-COF-152 achieves a maximum reduction capacity of 1950 mg g−1 under visible light irradiation, with 100% U(VI) removal. The exact conditions (e.g., pH, initial concentration, catalyst dosage) are detailed in the full paper, but this capacity is among the highest reported for COF-based photocatalysts.
How does the electron transfer distance affect the photocatalytic performance in these COFs?
By varying the connection mode of the anthraquinone acceptors (1,4-DQ vs. 1,5-DQ), the distance over which photogenerated electrons travel is extended. This reduces the probability of electron-hole recombination, as evidenced by enhanced photocatalytic activity. ECUT-COF-152, with the optimal electron transfer distance, shows the highest U(VI) reduction efficiency.
What is the role of the donor-acceptor architecture in the COF design?
The D-A architecture facilitates charge separation by promoting electron transfer from the donor (TP) to the acceptor (anthraquinone). This spatial separation of charges reduces recombination and enhances the availability of electrons for U(VI) reduction. The design avoids the need for additional functional groups, simplifying synthesis.
How does the performance of ECUT-COF-152 compare to other reported photocatalysts for U(VI) reduction?
ECUT-COF-152 achieves a reduction capacity of 1950 mg g−1, which is significantly higher than many previously reported materials, such as traditional TiO2-based photocatalysts or other COFs. This performance is attributed to the optimized electron transfer distance and the robust D-A structure.
What are the potential scalability and stability concerns for practical application?
The synthesis of these COFs involves simple Schiff-base reactions under solvothermal conditions, which are scalable. The COFs exhibit good crystallinity and chemical stability, as indicated by their sustained performance. However, long-term stability under continuous irradiation and in complex wastewater matrices requires further investigation, though the initial results are promising.
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