Unveiling singlet oxygen spin trapping in catalytic oxidation processes using in situ kinetic EPR analysis.
Proceedings of the National Academy of Sciences of the United States of America(2023)
摘要
Singlet oxygen (O) plays a pivotal role in numerous catalytic oxidation processes utilized in water purification and chemical synthesis. The spin-trapping method based on electron paramagnetic resonance (EPR) analysis is commonly employed for O detection. However, it is often limited to time-independent acquisition. Recent studies have raised questions about the reliability of the O trapper, 2,2,6,6-tetramethylpiperidine (TEMP), in various systems. In this study, we introduce a comprehensive, kinetic examination to monitor the spin-trapping process in EPR analysis. The EPR intensity of the trapping product was used as a quantitative measurement to evaluate the concentration of O in aqueous systems. This in situ kinetic study was successfully applied to a classical photocatalytic system with exceptional accuracy. Furthermore, we demonstrated the feasibility of our approach in more intricate O-driven catalytic oxidation processes for water decontamination and elucidated the molecular mechanism of direct TEMP oxidation. This method can avoid the false-positive results associated with the conventional 2D O detection techniques, and provide insights into the reaction mechanisms in O-dominated catalytic oxidation processes. This work underscores the necessity of kinetic studies for spin-trapping EPR analysis, presenting an avenue for a comprehensive exploration of the mechanisms governing catalytic oxidation processes.
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关键词
singlet oxygen spin,catalytic oxidation processes
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