Removal of VOCs by Ozone: n-Alkane Oxidation under Mild Conditions

Mytareva, Alina I.; Mashkovsky, Igor S.; Kanaev, S. A.; Bokarev, Dmitriy A.; Баева, Г. Н.; Kazakov, A. V.; Stakheev, A. Yu.

doi:10.3390/catal11040506

Cited by 14 publications

(2 citation statements)

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“…In contrast, the ozonation of alkanes has been reported at lower and even sub-ambient temperatures compared to those for oxidation with dioxygen. − Ozone readily oxidizes propane, n -butane, and isobutane in the gas phase at 50 °C and ambient pressure. Isobutane is oxidized to tert -butyl alcohol at ∼50% selectivity with a CO 2 selectivity of ∼16% .…”

Section: Introductionmentioning

confidence: 99%

Facile Ozonation of Light Alkanes to Oxygenates with High Atom Economy in Tunable Condensed Phase at Ambient Temperature

Zhu

Jackson

Subramaniam

2023

JACS Au

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We have demonstrated the oxidation of mixed alkanes (propane, nbutane, and isobutane) by ozone in a condensed phase at ambient temperature and mild pressures (up to 1.3 MPa). Oxygenated products such as alcohols and ketones are formed with a combined molar selectivity of >90%. The ozone and dioxygen partial pressures are controlled such that the gas phase is always outside the flammability envelope. Because the alkane−ozone reaction predominantly occurs in the condensed phase, we are able to harness the unique tunability of ozone concentrations in hydrocarbon-rich liquid phases for facile activation of the light alkanes while also avoiding over-oxidation of the products. Further, adding isobutane and water to the mixed alkane feed significantly enhances ozone utilization and the oxygenate yields. The ability to tune the composition of the condensed media by incorporating liquid additives to direct selectivity is a key to achieving high carbon atom economy, which cannot be achieved in gas-phase ozonations. Even in the liquid phase, without added isobutane and water, combustion products dominate during neat propane ozonation, with CO 2 selectivity being >60%. In contrast, ozonation of a propane+isobutane+water mixture suppresses CO 2 formation to 15% and nearly doubles the yield of isopropanol. A kinetic model based on the formation of a hydrotrioxide intermediate can adequately explain the yields of the observed isobutane ozonation products. Estimated rate constants for the formation of oxygenates suggest that the demonstrated concept has promise for facile and atom-economic conversion of natural gas liquids to valuable oxygenates and broader applications associated with C−H functionalization.

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Section: Introductionmentioning

confidence: 99%

Facile Ozonation of Light Alkanes to Oxygenates with High Atom Economy in Tunable Condensed Phase at Ambient Temperature

Zhu

Jackson

Subramaniam

2023

JACS Au

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“…The authors attributed this improved performance to the enhanced textural and redox properties of the modified red mud due to the better dispersion and higher enrichment of Fe oxides at their surface. Mytareva et al [8] investigated the ozone catalytic oxidation of alkanes by using an alumina-supported manganese oxide catalyst. They demonstrated that the presence of a small amount of ozone in air allowed to significantly decrease the temperature range of n-alkane oxidation, since 80-100% conversion is achievable in the temperature range 70-200 • C over Mn (10 wt.%)/Al 2 O 3 catalyst.…”

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confidence: 99%