State‐Of‐The‐Art Structural Regulation Methods and Quantum Chemistry for Carbon‐Based Single‐Atom Catalysts in Advanced Oxidation Process: Critical Perspectives into Molecular Level

Advanced oxidation processes (AOPs) by carbon-based single-atom catalysts (SACs) are recognized as an attractive scientific frontier for water treatment, with the outstanding benefits of ultra-effective and anti-interference capability. However, most of the research has paid more attention to the performance of SACs, while the in-depth understanding of catalytic regulation by molecular interaction is relatively deficient. This critical review delves into deciphering the catalytic mechanism through a micro-level, which makes it more convenient to interpret apparent catalytic phenomena. It first summarizes basic theories of quantum chemistry, which provide mechanism interpretation and prediction for molecular-oxidation systems. Additionally, corresponding oxidation pathways of common oxidants are underscored. Following the oxidants, state-of-the-art regulation methods are discussed with special attention to involved molecular interactions and pollutants. Particularly, the preliminary insights into the "oxidant-catalyst-pollutants" internal relationships are provided to help construct the SAC-AOP system from a molecular standpoint. Meanwhile, some cutting-edge laboratory devices and pilot-scale engineering are presented to illustrate the ultimate purpose of scientific molecular exploration. Eventually, relative challenges of SACs-AOPs upon the design of catalytic systems and investigation methods are provided. This review aims to promote the large-scale potential of SACs-based AOPs in practical water treatment by emphasizing the pivotal role of micro-insights.