Donor-acceptor engineered g-C₃N₄ enabling peroxymonosulfate photocatalytic conversion to ¹O₂ with nearly 100%...

Singlet oxygen (¹O₂) is a thrilling active species for selectively oxidating organic substances. However, the efficient and selective generation of ¹O₂ maintains a great challenge. Here, we develop a donor-acceptor structured g-C₃N₄ by covalently engineering benzenetricarboxaldehyde (BTA) onto the fringe of g-C₃N₄. The g-C₃N₄-BTA exerts high-efficiency ¹O₂ 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-C₃N₄. As such, PMS can be in-situ oxidated by the photogenerated holes to selectively produce ¹O₂. Besides, the g-C₃N₄-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.