School of Material Science and Engineering, Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion, Hunan University of Science and Technology, Xiangtan, 411201, China.
College of Materials and Chemical Engineering, Hunan Provincial Key Laboratory of Environmental Catalysis & Waste Recycling, Hunan Institute of Engineering, Xiangtan, 411104, China.
Chemosphere. 2024 Sep;364:143236. doi: 10.1016/j.chemosphere.2024.143236. Epub 2024 Aug 31.
The misuse and inevitable release of antibiotics can cause significant harm to both human health and the environment, and the use of polymeric semiconductors for photodegradation of antibiotics in aqueous environments is one of the most effective strategies to alleviate the current dilemma. Nevertheless, the inherently high exciton binding energy (E) and low photogenerated carrier transfer efficiency for most photocatalysts results in unsatisfactory photodegradation performance. Hence, this work proposes a donor polarization strategy to regulate the exciton dissociation of conjugated microporous polymers (CMPs) by minimizing their E. Results exhibited that the introduction of the strong donor unit 3,4-ethylenedioxythiophene (EDOT) not only reduces the E and effectively promotes exciton dissociation, but also broadens the visible light absorption of CMP. Among them, EdtTz-CMP with the lowest E (99 meV) delivered an efficiency of 94.6% in photocatalytic degradation of tetracycline (TC) with in 90 min, significantly higher than those of its analogues. This work provides a viable approach to design CMPs by tuning the intrinsic dipole of the donor for efficient environmental purification.
抗生素的滥用和不可避免的释放会对人类健康和环境造成重大危害，而在水相环境中使用聚合半导体进行抗生素的光降解是缓解这一困境的最有效策略之一。然而，大多数光催化剂的本征激子结合能 (E) 较高且光生载流子转移效率较低，导致光降解性能不理想。因此，本工作提出了一种施主极化策略，通过最小化共轭微孔聚合物 (CMP) 的 E 来调节激子的离解。结果表明，引入强施主单元 3,4-亚乙基二氧噻吩 (EDOT) 不仅降低了 E，有效地促进了激子的离解，而且还拓宽了 CMP 的可见光吸收。其中，具有最低 E（99 meV）的 EdtTz-CMP 在 90 分钟内对四环素 (TC) 的光催化降解效率达到 94.6%，明显高于其类似物。这项工作通过调整供体的固有偶极子为高效的环境净化提供了一种可行的设计 CMP 的方法。
