Unveiling singlet oxygen spin trapping in catalytic oxidation processes using in situ kinetic EPR analysis
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-indep...
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| Vydané v: | Proceedings of the National Academy of Sciences - PNAS Ročník 120; číslo 30; s. e2305706120 |
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| Hlavní autori: | , , , |
| Médium: | Journal Article |
| Jazyk: | English |
| Vydavateľské údaje: |
United States
25.07.2023
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| Predmet: | |
| ISSN: | 1091-6490, 1091-6490 |
| On-line prístup: | Zistit podrobnosti o prístupe |
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| Shrnutí: | 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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| Bibliografia: | ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
| ISSN: | 1091-6490 1091-6490 |
| DOI: | 10.1073/pnas.2305706120 |