Direct Catalytic Conversion of Methane to Methanol in an Aqueous Medium by using Copper‐Promoted Fe‐ZSM‐5

Hammond, Ceri; Forde, Michael M.; Rahim, Mohd Hasbi Ab.; Thetford, Adam; He, Qian; Jenkins, Robert L.; Dimitratos, Nikolaos; López-Sánchez, José Antonio; Dummer, Nicholas F.; Murphy, Damien M.; Carley, Albert Frederick; Taylor, Stuart H.; Willock, David J.; Stangland, Eric E.; Kang, Jun-Koo; Hagen, Henk; Kiely, Christopher J.; Hutchings, Graham J.

doi:10.1002/ange.201108706

Cited by 112 publications

(104 citation statements)

References 36 publications

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“…0.5 M and there was no requirement for a PPh3 additive. In line with analogous studies of the ZSM-5 catalysed oxidation of methane within the same group [98], the catalytic conversion of both ethane and H2O2 was attributed to extraframework iron sites. Indeed, whilst H-ZSM-5 (30) showed a rate of 2.8 molethane converted•kgcat −1 •h −1 , post synthesis deposition of 1.1 wt % Fe increased the rate to 47.1 molethane converted•kgcat −1 •h −1 under the same conditions [7].…”

Section: C2h6 + 4•ohsupporting

confidence: 77%

An Overview of Recent Advances of the Catalytic Selective Oxidation of Ethane to Oxygenates

2016

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Abstract:The selective partial oxidation of short chain alkanes is a key challenge within catalysis research. Direct ethane oxidation to oxygenates is a difficult aim, but potentially rewarding, and it could lead to a paradigm shift in the supply chain of several bulk chemicals. Unfortunately, low C-H bond reactivity and kinetically labile products are just some reasons affecting the development and commercialisation of such processes. Research into direct ethane oxidation is therefore disparate, with approaches ranging from oxidation in the gas phase at high temperatures to enzyme catalysed hydroxylation under ambient conditions. Furthermore, in overcoming the barrier posed by the chemically inert C-H bond a range of oxidants have been utilised. Despite years of research, this remains an intriguing topic from both academic and commercial perspectives. Herein we describe some recent developments within the field of catalytic ethane oxidation focusing on the formation of oxygenated products, whilst addressing the key challenges which are still to be overcome.

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Section: C2h6 + 4•ohsupporting

confidence: 77%

An Overview of Recent Advances of the Catalytic Selective Oxidation of Ethane to Oxygenates

2016

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“…Such homogeneous processes have been extensively reviewed by Periana et al and Shilov et al [22,23] and heterogenised by Schüth and co-workers [24,25]. A number of homogeneously [26][27][28] and heterogeneously [29][30][31][32] catalysed aqueous processes for the direct oxidation of methane with H 2 O 2 have recently been reported. These benefit from the clean decomposition of the oxidant to H 2 O as an environmentally benign byproduct.…”

Section: Introductionmentioning

confidence: 95%

“…It has previously been reported that ZSM-5 materials containing trace amounts of iron (as dimeric -oxo-hydroxo iron species) can catalyse the direct conversion of methane and ethane to oxygenated products, utilising hydrogen peroxide as the oxidant [31,32,[38][39][40]. The oxidation of methane to methanol was shown to proceed via formation of methylhydroperoxide (CH 3 OOH), and deep oxidation to formic acid and CO 2 was observed [31].…”

Section: Introductionmentioning

confidence: 95%

“…Unfortunately despite extensive research in the field, no approach has yet been deemed commercially viable, with methanol J. Xu et al / Catalysis Today xxx (2015) xxx-xxx Scheme 1. Reaction scheme for methane oxidation over ZSM-5 (30) catalysts as proposed by previous studies [31,41]. still produced through an energy intensive two-step process which proceeds via synthesis gas.…”

Section: Introductionmentioning

confidence: 99%

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Continuous selective oxidation of methane to methanol over Cu- and Fe-modified ZSM-5 catalysts in a flow reactor

et al. 2016

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Please cite this article in press as: J. Xu, et al., Continuous selective oxidation of methane to methanol over Cu-and Fe-modified ZSM-5 catalysts in a flow reactor, Catal. Today (2015), http://dx. a b s t r a c tThe selective oxidation of methane to methanol is a key challenge in catalysis. Iron and copper modified ZSM-5 catalysts are shown to be effective for this reaction using H 2 O 2 as the oxidant under continuous flow operation. Co-impregnation of ZSM-5 with Fe and Cu by chemical vapour impregnation yielded catalysts that showed high selectivity to methanol (>92% selectivity, 0.5% conversion), as the only product in the liquid phase. The catalysts investigated did not deactivate during continuous reaction, and methanol selectivity remained high. The effect of reaction pressure, temperature, hydrogen peroxide concentration and catalyst mass were investigated. An increase in any of these led to increased methane conversion, with high methanol selectivity (≥73%) maintained throughout. Catalysts were characterised using DR-FTIR, DR-UV-Vis and 27 Al MAS-NMR spectroscopy.

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“…Even the oxidation power of artificial Fenton and photoFenton systems is known to be high enough to hydroxylate aliphatic C-H bonds, inclusing CH 4 hydroxylation to methanol (Gopakumar et al, 2011;Hammond et al, 2012;Yoshizawa et al, 2000).…”

Section: Oxidation Of Organic Aerosol Particles Containing Black and mentioning

confidence: 99%

Climate engineering by mimicking natural dust climate control: the iron salt aerosol method

et al. 2017

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Abstract. Power stations, ships and air traffic are among the most potent greenhouse gas emitters and are primarily responsible for global warming. Iron salt aerosols (ISAs), composed partly of iron and chloride, exert a cooling effect on climate in several ways. This article aims firstly to examine all direct and indirect natural climate cooling mechanisms driven by ISA tropospheric aerosol particles, showing their cooperation and interaction within the different environmental compartments. Secondly, it looks at a proposal to enhance the cooling effects of ISA in order to reach the optimistic target of the Paris climate agreement to limit the global temperature increase between 1.5 and 2 • C.Mineral dust played an important role during the glacial periods; by using mineral dust as a natural analogue tool and by mimicking the same method used in nature, the proposed ISA method might be able to reduce and stop climate warming. The first estimations made in this article show that by doubling the current natural iron emissions by ISA into the troposphere, i.e., by about 0.3 Tg Fe yr −1 , artificial ISA would enable the prevention or even reversal of global warming. The ISA method proposed integrates technical and economically feasible tools.

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Direct Catalytic Conversion of Methane to Methanol in an Aqueous Medium by using Copper‐Promoted Fe‐ZSM‐5

Cited by 112 publications

References 36 publications

An Overview of Recent Advances of the Catalytic Selective Oxidation of Ethane to Oxygenates

An Overview of Recent Advances of the Catalytic Selective Oxidation of Ethane to Oxygenates

Continuous selective oxidation of methane to methanol over Cu- and Fe-modified ZSM-5 catalysts in a flow reactor

Climate engineering by mimicking natural dust climate control: the iron salt aerosol method

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