Regulating the distance of electron transfer in anthraquinone-based covalent organic framework for efficient photocatalytic U(VI) reduction
摘要
Driven by the dual impetus of environmental protection and resource recycling, photocatalytic U(VI) reduction has emerged as a pivotal supporting technology for radioactive uranium treatment in the nuclear industry. In this work, anthraquinone-based covalent organic frameworks (COFs) with donor-acceptor (D-A) architectures were successfully constructed, using 2,4,6-triformylphloroglucinol (TP) as the donor and 1,4-diaminoanthraquinone (1,4-DQ) along with 1,5-diaminoanthraquinone (1,5-DQ) as the acceptor. This design strategy eliminates the need for introducing extra specific functional groups and avoids altering the core structures of D-donors and A-acceptors. By adjusting the connection mode of building units, the transport distance of photogenerated electrons is significantly extended, which efficiently suppresses the electron-hole pair recombination and ultimately enables high-performance photocatalytic reduction. Among the COFs tested, ECUT-COF-152 demonstrated the optimal catalytic activity under visible light, achieving 100% U(VI) removal with a maximum reduction capacity as high as 1950 mg g−1. This work offers valuable insights into the design of efficient materials for photocatalytic reduction of U(VI) by precisely tuning the D-A structure.