Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China.
Key Laboratory of Industrial Ecology and Environmental Engineering (Ministry of Education), School of Environmental Science and Technology, Dalian University of Technology, Dalian, 116024, China.
Water Res. 2020 Jun 15;177:115798. doi: 10.1016/j.watres.2020.115798. Epub 2020 Apr 9.
Polymeric photocatalysts are promising candidates for water purification, however their catalytic performance are still unsatisfactory due to the fast charge recombination that leads to low reactive oxygen radicals production. In this study, a conceptual energy-transfer-mediated photocatalytic oxygen activation system over polymeric carbon nitride without the need of electron-hole separation is proposed, exhibiting remarkable singlet oxygen triggered bacteria inactivation performance as well as organic pollutants degradation. By structure and excitonic effect modulation, the oxygen activation process changes from the traditional electron-transfer mechanism to the final energy-transfer pathway, leading to the selective generation of singlet oxygen with high efficiency. The generated singlet oxygen is found to fervently attack the bacteria membrane, creating irreparable pores or holes on the cell membrane for cytoplasmic contents leaking out to accelerate bacteria destruction. The work demonstrated here offers a new photocatalytic oxygen activation pathway for achieving high-efficient reactive oxygen species generation performance without the need of charge separation.
聚合物光催化剂是水净化的有前途的候选者，然而，由于快速电荷复合导致产生的反应性氧自由基数量较少，其催化性能仍然不尽人意。在本研究中，提出了一种无需电子-空穴分离的聚合物氮化碳上的概念性能量转移介导的光催化氧活化系统，表现出显著的单重态氧触发细菌失活性能以及有机污染物降解性能。通过结构和激子效应调制，氧活化过程从传统的电子转移机制转变为最终的能量转移途径，从而高效选择性地生成单重态氧。研究发现，生成的单重态氧会猛烈攻击细菌膜，在细胞膜上造成不可挽回的孔或洞，使细胞质内容物泄漏出来，从而加速细菌的破坏。本工作为实现高效活性氧物种生成性能而无需电荷分离提供了一种新的光催化氧活化途径。
