Keys to methane conversion technologies

Lange, Jean‐Paul; Jong, Krijn P. de; Ansorge, J.; Tijm, P.J.A.

doi:10.1016/s0167-2991(97)80320-5

Cited by 37 publications

(41 citation statements)

References 9 publications

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“…First, the reaction of methane with CuMOR(6), activated in oxygen at 673 Kt oe xclude the reduction with carbonaceous impurities, [43] was studied at elevated temperature. 1 HMAS NMR spectra (Figures S9 and S10) display the progressive development of the signal at 4.1 ppm due to the Brønsted acid sites,inline with our previous study,confirming that the reaction of Cu II species in the zeolite pores with methane leads to the transfer of ahydrogen atom from CH 4 to the framework as ap roton. [23] Simultaneously,t he formation of Cu I species is observed in Cu K-edge XANES spectra acquired during the temperature-programmed reaction with methane ( Figure S11).…”

Section: Resultssupporting

confidence: 88%

“…Thes earch for novel pathways for the conversion of methane to valuable chemicals nowadays attracts enormous interest from the industrial and scientific communities. [1][2][3][4][5] There is an abundance of natural gas,m ostly methane,a nd its price is relatively low,when calculated per carbon fraction. However,methane is the least active of all the alkanes,and its selective transformation to the desired product is challenging.…”

Section: Introductionmentioning

confidence: 99%

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Pathways of Methane Transformation over Copper‐Exchanged Mordenite as Revealed by In Situ NMR and IR Spectroscopy

2019

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The reaction of methane with copper‐exchanged mordenite with two different Si/Al ratios was studied by means of in situ NMR and infrared spectroscopies. The detection of NMR signals was shown to be possible with high sensitivity and resolution, despite the presence of a considerable number of paramagnetic CuII species. Several types of surface‐bonded compounds were found after reaction, namely molecular methanol, methoxy species, dimethyl ether, mono‐ and bidentate formates, CuI monocarbonyl as well as carbon monoxide and dioxide, which were present in the gas phase. The relative fractions of these species are strongly influenced by the reaction temperature and the structure of the copper sites and is governed by the Si/Al ratio. While methoxy species bonded to Brønsted acid sites, dimethyl ether and bidentate formate species are the main products over copper‐exchange mordenite with a Si/Al ratio of 6; molecular methanol and monodentate formate species were observed mainly over the material with a Si/Al ratio of 46. These observations are important for understanding the methane partial oxidation mechanism and for the rational design of the active materials for this reaction.

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Section: Resultssupporting

confidence: 88%

Section: Introductionmentioning

confidence: 99%

Pathways of Methane Transformation over Copper‐Exchanged Mordenite as Revealed by In Situ NMR and IR Spectroscopy

2019

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“…To avoid this waste, converting this methane to more valuable molecules like methanol could be a win‐win situation for economics and the environment . Directly converting methane to methanol has its share of scientific challenges that have given it a reputation as the “dream reaction.” The methane must be stabilized in a partially oxidized state rather than undergo much more favorable complete oxidation to carbon dioxide ,. Copper exchanged zeolites can do just that when a stepwise looping procedure is applied .…”

Section: Figurementioning

confidence: 99%

Copper‐Exchanged Omega (MAZ) Zeolite: Copper‐concentration Dependent Active Sites and its Unprecedented Methane to Methanol Conversion

et al. 2018

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The direct conversion of methane to methanol may provide a way to utilize methane that is otherwise wasted. Here we have explored one of the most promising copper zeolite materials to date, copper‐exchanged omega (MAZ) zeolite. With highly crystalline and uniform zeolite omega, we can produce 150 umol‐methanol/gram‐zeolite under 1 bar methane and as high as 200 umol‐methanol/gram‐zeolite under 30 bar methane, the highest yield ever reported. Furthermore, zeolite omega's ability to convert methane to methanol has a distinct copper‐concentration dependent behavior. At lower copper loadings, Cu–MAZ is inactive, and once a minimum copper loading is reached, Cu–MAZ converts methane to methanol more selective than the widely studied Cu‐mordenite. With the unprecedented high conversion and selectivity, Cu–MAZ provides insight into the active copper phase and its mechanism which was quantified as two electrons per molecule of methanol produced.

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“…Direct methane to methanol conversion is difficult, because the higher reactivity of methanol than methane sets a limit to the yield that can be obtained. [5][6][7][8] Currently, research in this area is at a transition point where scientific refocusing towards processes with more industrial feasibility are needed. 9 One promising system using copper-exchanged zeolites is a stoichiometric stepwise (''chemical looping'') procedure.…”

mentioning

confidence: 99%

Comparative performance of Cu-zeolites in the isothermal conversion of methane to methanol

et al. 2019

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Keys to methane conversion technologies

Cited by 37 publications

References 9 publications

Pathways of Methane Transformation over Copper‐Exchanged Mordenite as Revealed by In Situ NMR and IR Spectroscopy

Pathways of Methane Transformation over Copper‐Exchanged Mordenite as Revealed by In Situ NMR and IR Spectroscopy

Copper‐Exchanged Omega (MAZ) Zeolite: Copper‐concentration Dependent Active Sites and its Unprecedented Methane to Methanol Conversion

Comparative performance of Cu-zeolites in the isothermal conversion of methane to methanol

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