Continuous methanol synthesis directly from methane and steam over Cu(II)-exchanged mordenite

Lee, Sae Ha; Kang, Jong Kyu; Park, Eun Duck

doi:10.1007/s11814-018-0150-5

Cited by 26 publications

(23 citation statements)

References 13 publications

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“…Cu‐exchanged zeolites are probably the most studied zeolites in the field of DMTM conversion, because they are considered the most promising for industrial application . Just as Fe, Cu is believed to form the active sites in methane monooxygenase (MMO), which is an enzyme able to convert CH 4 to CH 3 OH at ambient conditions with a high selectivity.…”

Section: Direct Ch4 To Ch3oh Conversion Over Zeolitesmentioning

confidence: 99%

Advanced X‐ray Absorption Spectroscopy Analysis to Determine Structure‐Activity Relationships for Cu‐Zeolites in the Direct Conversion of Methane to Methanol

et al. 2020

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An industrial process for direct conversion of methane to methanol (DMTM) would revolutionize methane as feedstock for the chemical industry and it would be a cherished contribution to climate change mitigation. At the present stage, it is a rather remote perspective, but the search for the materials that would make it possible and economically viable, is very active. Cu‐exchanged zeolites have been shown to cleave the C−H bond of methane at low temperatures (≤200 °C), and has been extensively studied for the stepwise DMTM conversion over the last decades. The determination of the speciation of CuxOy‐species in zeolites and the understanding of their role in the reaction mechanism has been heavily debated. Lately, advanced X‐ray absorption spectroscopy (XAS) analysis has been standing out as a powerful technique for investigating the behavior of Cu in zeolites. In this review we focus on the in situ and operando studies of changes in the electronic and structural properties of Cu, during the different steps of the DMTM conversion uncovered by XAS, which have led to new and insightful information about the complex behavior of Cu‐zeolites in the DMTM process.

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Section: Direct Ch4 To Ch3oh Conversion Over Zeolitesmentioning

confidence: 99%

Advanced X‐ray Absorption Spectroscopy Analysis to Determine Structure‐Activity Relationships for Cu‐Zeolites in the Direct Conversion of Methane to Methanol

et al. 2020

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“…Also, it has been reported that methanol can be continuously produced from the simultaneous introduction of methane and steam without any oxidant by the oxidizing ability of H 2 O (Sushkevich et al, 2017; Lee et al, 2018). The produced methanol was not excessively oxidized since steam has lower oxidizing power than oxygen.…”

Section: Continuous Methanol Production Over a Cu-zeolite Systemmentioning

confidence: 99%

“…Although many studies on the direct conversion of methane over a zeolite containing transition metal ions of Fe, Co, Ni, Cu, and Zn and using N 2 O, H 2 O 2 , O 2 , and recently H 2 O as oxidants have been reported, the Cu-zeolite system with O 2 or H 2 O has been regarded to be most promising for industrial application (Sushkevich et al, 2017; Lee et al, 2018). Cu-zeolites can be activated by both N 2 O and O 2 , unlike the Fe-zeolites on which methane activation sites cannot be formed with O 2 .…”

Section: Introductionmentioning

confidence: 99%

Recent Progress in Direct Conversion of Methane to Methanol Over Copper-Exchanged Zeolites

Park

Ahn

2019

Front. Chem.

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The conversion of methane into an easily transportable liquid fuel or chemicals has become a highly sought-after goal spurred by the increasing availability of cheap and abundant natural gas. While utilization of methane for the production of syngas and its subsequent conversion via an indirect route is typical, it is cost-intensive, and alternative direct conversion routes have been investigated actively. One of the most promising directions among these is the low-temperature partial oxidation of methane to methanol over a metal-loaded zeolite, which mimics facile enzymatic chemistry of methane oxidation. Thus mono-, bi-, and trinuclear oxide compounds of iron and copper stabilized on ZSM-5 or mordenite, which are structurally analogous to those found in methane monooxygenases, have demonstrated promising catalytic performances. The two major problems of theses metal-loaded zeolites are low yield to methanol and batch-like non-catalytic reaction systems challenging to extend to an industrial scale. In this mini-review, attention was given to the direct methane oxidation to methanol over copper-loaded zeolite systems. A brief introduction on the catalytic methane direct oxidation routes and current status of the applied metal-containing zeolites including the ones with copper ions are given. Next, by analyzing the extensive experimental and theoretical data available, the consensus among the researchers to achieve the target of high methanol yield is discussed in terms of zeolite topology, active species, and reaction parameters. Finally, the recent efforts on continuous methanol production from the direct methane oxidation aiming for an industrial process are summarized.

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“…The gas‐phase partial oxidation of methane has been reported over Fe‐ or Cu‐zeolites using N 2 O, O 2 , and H 2 O as oxidants. However, most reactions can only proceed at relatively high temperatures (>200 °C) resulting in low product yields .…”

Section: Catalytic Performance For the Selective Oxidation Of Methanementioning

confidence: 99%

Aqueous‐Phase Selective Oxidation of Methane with Oxygen over Iron Salts and Pd/C in the Presence of Hydrogen

Kang

Park

2019

ChemCatChem

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Direct conversion of methane into value‐added chemicals is a challenging but worthwhile subject. In this communication, the direct conversion of methane into methane oxygenates was achieved in an aqueous solution at room temperature using iron salts and Pd/C as catalysts and hydrogen peroxide as an oxidant. The hydrogen peroxide can be directly added or generated in situ from hydrogen and oxygen. The Pd/C catalyst greatly enhanced the reaction rate together with the iron salts. The effect of some parameters such as reaction temperature, reaction time, pH, acid type, and catalyst amount on the yields of the methane oxygenates was also investigated. When hydrogen peroxide was directly added, the turnover frequency (TOF), defined as the moles of methane oxygenates per moles of Fe per unit time, at 293 K was 29 h−1 at pH=2.3. The TOF at 293 K was 42 h−1 at pH=1.3 with in situ generated hydrogen peroxide from hydrogen and oxygen.

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Continuous methanol synthesis directly from methane and steam over Cu(II)-exchanged mordenite

Cited by 26 publications

References 13 publications

Advanced X‐ray Absorption Spectroscopy Analysis to Determine Structure‐Activity Relationships for Cu‐Zeolites in the Direct Conversion of Methane to Methanol

Advanced X‐ray Absorption Spectroscopy Analysis to Determine Structure‐Activity Relationships for Cu‐Zeolites in the Direct Conversion of Methane to Methanol

Recent Progress in Direct Conversion of Methane to Methanol Over Copper-Exchanged Zeolites

Aqueous‐Phase Selective Oxidation of Methane with Oxygen over Iron Salts and Pd/C in the Presence of Hydrogen

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