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Superior oxidation of MO within the presence of Cu(II) primarily based on redox biking: a mixed experimental and DFT research.
Polycyclic fragrant hydrocarbons (PAHs) and aliphatic hydrocarbons (AH) are among the many most plentiful chemical pollution within the atmosphere. Aqueous chemistry could also be a significant however nonetheless elusive supply of their bioavailability within the atmosphere. Whereas they’re typically extremely reactive to ozone, they seem to have restricted reactivity with ·OH. On this work, liquid-liquid microextraction (LLME) coupled with chromatographic separation and subsequent evaluation by GC-MS was used to review the response of 4 aliphatic OH-acids (AOHAc) with tert-butyl hydroxylperoxide (TBHOO), an artificial mannequin for the oxidation of AH by ·OH. Among the many 4 examined OH-acids, 2-chloropropanoic acid (HACr) was discovered to react most effectively with TBHOO, with 95% conversion (2-oxo-propyl-alcohol (HAPol) yields) in lower than 10 min at pH 7.4. An in depth research on the response mechanism primarily based on MALDI-TOF-MS-MS and deuterium-labeling, mixed with DFT calculations, allowed for the identification of two potential response pathways, the place the HO-Cl intermediate is at first oxidized after which hydrogenated to a secondary alcohol. The response might be subsequently accomplished by a extremely oxidizing (and consequently quick) OH-hydrogenation, which regenerates the dad or mum OH-acid. The DFT calculations have been additional discovered to be in good settlement with experimental outcomes. The end result of this research present the ability of this method for the research of response mechanisms within the presence of Cu(II) and due to this fact opens up for promising new approaches for the superior oxidation of OH-acids by ·OH.import {
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