Selective oxidation of methane by molecular oxygen catalyzed by a bridged binuclear ruthenium complex at moderate pressures and ambient temperature

Khokhar, Munir D.; Shukla, Ram S.; Jasra, Raksh V.

doi:10.1016/j.molcata.2008.10.023

Cited by 29 publications

(5 citation statements)

References 39 publications

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“…Jasra and co-workers 158 reported that a Ru 3+ −salen dimer [(HSalen) 2 Ru 2 (μ-O)(μ-CH 3 COO) 2 ], shown in Figure 6, where one of the Hsalen ligands remains tridentate with a dangling phenol group, was competent to catalyze the hydroxylation of methane. Up to 58 TONs were observed at 30 °C with 5 bar of O 2 (the gas chromatography study did not mention CO 2 or other oxygenated derivatives).…”

Section: Rutheniummentioning

confidence: 99%

Homogeneous Functionalization of Methane

et al. 2017

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One of the remaining "grand challenges" in chemistry is the development of a next generation, less expensive, cleaner process that can allow the vast reserves of methane from natural gas to augment or replace oil as the source of fuels and chemicals. Homogeneous (gas/liquid) systems that convert methane to functionalized products with emphasis on reports after 1995 are reviewed. Gas/solid, bioinorganic, biological, and reaction systems that do not specifically involve methane functionalization are excluded. The various reports are grouped under the main element involved in the direct reactions with methane. Central to the review is classification of the various reports into 12 categories based on both practical considerations and the mechanisms of the elementary reactions with methane. Practical considerations are based on whether or not the system reported can directly or indirectly utilize O as the only net coreactant based only on thermodynamic potentials. Mechanistic classifications are based on whether the elementary reactions with methane proceed by chain or nonchain reactions and with stoichiometric reagents or catalytic species. The nonchain reactions are further classified as CH activation (CHA) or CH oxidation (CHO). The bases for these various classifications are defined. In particular, CHA reactions are defined as elementary reactions with methane that result in a discrete methyl intermediate where the formal oxidation state (FOS) on the carbon remains unchanged at -IV relative to that in methane. In contrast, CHO reactions are defined as elementary reactions with methane where the carbon atom of the product is oxidized and has a FOS less negative than -IV. This review reveals that the bulk of the work in the field is relatively evenly distributed across most of the various areas classified. However, a few areas are only marginally examined, or not examined at all. This review also shows that, while significant scientific progress has been made, greater advances, particularly in developing systems that can utilize O, will be required to develop a practical process that can replace the current energy and capital intensive natural gas conversion process. We believe that this classification scheme will provide the reader with a rapid way to identify systems of interest while providing a deeper appreciation and understanding, both practical and fundamental, of the extensive literature on methane functionalization. The hope is that this could accelerate progress toward meeting this "grand challenge."

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Section: Rutheniummentioning

confidence: 99%

Homogeneous Functionalization of Methane

et al. 2017

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“…The rest three components of Fe 2+ (d 6 ; 5 D) make the next quintet states around ∼20 kcal/ mol higher. These split in a pseudo 4 Π and 4 Σ + branches.…”

Section: Resultsmentioning

confidence: 99%

“…Industrially, the conversion of methane to commodity chemicals and liquid fuels goes through the synthetic gas route. It is first decomposed to CO + H 2 (syngas), which is then exposed to harsh conditions (15–40 atm pressure and 700–1000 °C temperature), to make methanol. , An overview of available direct methane to methanol (MTM) conversion techniques avoiding the syngas path has been given recently. , These involve gas-phase and solution-phase homogeneous catalysis, heterogeneous catalysis, photocatalysis, biocatalysts (enzymes), plasma technologies, frustrated Lewis-pairs, , MOFs, − and others. Their drawbacks and limitations are discussed in ref .…”

Section: Introductionmentioning

confidence: 99%

Methane to Methanol Conversion Facilitated by Transition-Metal Methyl and Methoxy Units: The Cases of FeCH₃⁺ and FeOCH₃⁺

Khan

Miliordos

2019

J. Phys. Chem. A

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The conversion of methane to methanol (MTM) catalyzed by FeOCH 3 + and FeCH 3 + is investigated by means of multireference configuration interaction (MRCI), single-reference coupled clusters (CC), and density functional theory (DFT) approaches. Our dual purpose is the assessment of the applied methodologies and the performance of the proposed catalytic cycle, which involves both of the titled units. The investigated cycle aims to bypass the limitations of metal-oxide catalysts and offers an alternative promising method for efficient MTM transformation. From the technical viewpoint, we found that generally accurate electron correlation treatment is more important than accurately calculated geometries. The combination of optimal DFT geometries with MRCI and CC energetics provides a good compromise between accuracy and efficiency, although there are cases where multireference calculations must be used to obtain correct structures.

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“…However, selective oxidations of alkanes or arylalkanes to partially oxidized products are accompanied by many difficulties due to their low reactivities compared to alkenes and dienes. Selective oxidation of hydrocarbons by O2 has been the subject of many researches (Bettahar et al, 1996;Khokhar et al, 2009;Ma et al, 2007;Min and Mizuno, 2001;Misono et al, 1997;Mizuno et al, 1996). A large number of papers have been devoted to the study of the oxidative dehydrogenation (ODH) reaction of paraffin on metals oxides which may be an attractive alternative route as compared to the conventional thermal dehydrogenation process (Kung and Kung, 1991;Madeira and Portela, 1998;Mamedov and Corberan, 1995).…”

Section: Introductionmentioning

confidence: 99%

Catalytic activation of C–H bonds of hydrocarbons by heteropolycompounds

Benlounes

Cheknoun

Mansouri

et al. 2011

Journal of the Taiwan Institute of Chemical Engineers

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Selective oxidation of methane by molecular oxygen catalyzed by a bridged binuclear ruthenium complex at moderate pressures and ambient temperature

Cited by 29 publications

References 39 publications

Homogeneous Functionalization of Methane

Homogeneous Functionalization of Methane

Methane to Methanol Conversion Facilitated by Transition-Metal Methyl and Methoxy Units: The Cases of FeCH₃⁺ and FeOCH₃⁺

Catalytic activation of C–H bonds of hydrocarbons by heteropolycompounds

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Selective oxidation of methane by molecular oxygen catalyzed by a bridged binuclear ruthenium complex at moderate pressures and ambient temperature

Cited by 29 publications

References 39 publications

Homogeneous Functionalization of Methane

Homogeneous Functionalization of Methane

Methane to Methanol Conversion Facilitated by Transition-Metal Methyl and Methoxy Units: The Cases of FeCH3+ and FeOCH3+

Catalytic activation of C–H bonds of hydrocarbons by heteropolycompounds

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Product

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Methane to Methanol Conversion Facilitated by Transition-Metal Methyl and Methoxy Units: The Cases of FeCH₃⁺ and FeOCH₃⁺