Mechanical insight into direct singlet oxygen generation pathway: The significance of Co-O-X bond formation anchored by cobalt single atoms on mesoporous oxides
The understanding of how single atoms anchoring on oxides contribute to high-activity catalysis in the sulfate radical-advanced oxidation process (SR-AOP) remains obscure. Here we presented a new strategy for regulating singlet oxygen ( 1 O 2 ) generation in peroxymonosulfate-based advanced oxidation processes (PMS-AOPs) by engineering the Co-O-X active sites on oxide supports in this study. The Co single atoms supported on mesoporous oxides (Co SA -XO 2 ) were first successfully developed using a modified sol–gel solvent vaporization self-assembly method. We found that Co SA -XO 2 catalysts served as efficient PMS activators for pollutant decomposition over a wide pH range. Notably, Co SA -TiO 2 exhibited exceptional performance, achieving nearly 100% removal of sulfasalazine (SSZ) within 10 min. Furthermore, evidenced by experimental results and density functional theory (DFT) calculations, 1 O 2 was confirmed to be predominately active oxidizing species by the unique Co-O-X bonds for activating PMS in Co SA -XO 2 /PMS system, resulting in an excellent pollution degradation. This study provides valuable insights into the construction of highly loaded single-atom catalysts using oxide substrates in the PMS-AOP system, along with the mechanism of regulating reactive oxygen species (ROS) formation through interfacial bonding between active metal and support.
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