Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of Education, School of Ecology, Environment and Resources, Guangdong University of Technology, Guangzhou 510006, PR China.
Key Laboratory for City Cluster Environmental Safety and Green Development of the Ministry of Education, School of Ecology, Environment and Resources, Guangdong University of Technology, Guangzhou 510006, PR China.
J Hazard Mater. 2023 Apr 15;448:130869. doi: 10.1016/j.jhazmat.2023.130869. Epub 2023 Jan 25.
Singlet oxygen (O) is a thrilling active species for selectively oxidating organic substances. However, the efficient and selective generation of O maintains a great challenge. Here, we develop a donor-acceptor structured g-CN by covalently engineering benzenetricarboxaldehyde (BTA) onto the fringe of g-CN. The g-CN-BTA exerts high-efficiency O generation with nearly 100% selectivity via peroxymonosulfate (PMS) photocatalytic activation upon visible light illumination, exhibiting obviously boosted efficiency for selective elimination of atrazine (ATZ). The consequences of experiments and theoretical calculations demonstrate that BTA units serve as electron-withdrawing sites to trap photogenerated electrons and facilitate the adsorption of PMS on the electron-deficient heptazine rings of g-CN. As such, PMS can be in-situ oxidated by the photogenerated holes to selectively produce O. Besides, the g-CN-BTA/PMS system delivers high stability and strong resistance to the coexisting organic ions and natural organic matter, demonstrating great potential for selectively removing targeted organic contaminants with high efficiency.
单线态氧（O）是一种用于选择性氧化有机物质的令人兴奋的活性物质。然而，高效和选择性地产生 O 仍然是一个巨大的挑战。在这里，我们通过将苯三甲醛（BTA）共价修饰到 g-CN 的边缘，开发了一种给体-受体结构的 g-CN。g-CN-BTA 在可见光照射下通过过一硫酸盐（PMS）光催化活化，高效地产生近 100%选择性的 O，对莠去津（ATZ）的选择性消除表现出明显的增强效率。实验和理论计算的结果表明，BTA 单元作为吸电子位点来捕获光生电子，并促进 PMS 在电子缺陷的 heptazine 环上的吸附。因此，PMS 可以被光生空穴原位氧化，以选择性地产生 O。此外，g-CN-BTA/PMS 体系具有高稳定性和对共存有机离子和天然有机物的强抵抗力，展示了高效选择性去除目标有机污染物的巨大潜力。
