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Reactivity of methoxy species towards methylation and oligomerization in Cu-zeolite systems.

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Title: Reactivity of methoxy species towards methylation and oligomerization in Cu-zeolite systems.
Authors: Solemsli, Bjørn Gading1 (AUTHOR), Berdiell, Izar Capel1 (AUTHOR), Prodinger, Sebastian1 (AUTHOR), Kvande, Karoline1 (AUTHOR), Deplano, Gabriele2 (AUTHOR), Olsbye, Unni1 (AUTHOR), Beato, Pablo3 (AUTHOR), Bordiga, Silvia2 (AUTHOR), Svelle, Stian1 (AUTHOR) stian.svelle@kjemi.uio.no
Source: Catalysis Today. Jun2024, Vol. 436, pN.PAG-N.PAG. 1p.
Subjects: Oligomerization, Partial oxidation, Methylation, Brønsted acids, Copper, Zeolites, Species, Toluene
Abstract: Ethylene, propylene, and benzene were investigated as molecules for extracting methoxy intermediate species formed during the cyclic partial oxidation of methane in Cu-exchanged zeolites, promising materials for the step-wise methane-to-methanol (MTM) reaction. 13C-labeled reaction studies reveal that alkenes preferentially undergo oligomerization followed by cracking, while benzene is successfully methylated, forming toluene. Benzene methylation further showcases the methyl species to behave similar to surface methoxy species formed on Brønsted acid sites in methanol-to-hydrocarbon (MTH) reaction. However, benzene is only able to extract a fraction of the methyl species compared to the methanol produced with water extraction, indicating either steric or intrinsic mechanistic effects to limit the full potential of the methyl pool inside the framework. We infer the presence of reactive methoxy species on Brønsted acid sites generated under reaction conditions, revealing their potential as a synthetic platform to form additional products from methane. • Benzene reacts with the methoxy intermediate in the Cu-zeolite forming toluene. • Benzene and water access different amounts of methoxy; more than one type of methoxy. • Cu(I)-species formed after methane activation affect ethylene oligomerization. • Propylene oligomerizes independently of Cu species, BAS, or methoxy presence. [ABSTRACT FROM AUTHOR]
Copyright of Catalysis Today is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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DbLabel: Engineering Source
An: 177372660
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  Data: Reactivity of methoxy species towards methylation and oligomerization in Cu-zeolite systems.
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  Data: <searchLink fieldCode="AR" term="%22Solemsli%2C+Bjørn+Gading%22">Solemsli, Bjørn Gading</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Berdiell%2C+Izar+Capel%22">Berdiell, Izar Capel</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Prodinger%2C+Sebastian%22">Prodinger, Sebastian</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Kvande%2C+Karoline%22">Kvande, Karoline</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Deplano%2C+Gabriele%22">Deplano, Gabriele</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Olsbye%2C+Unni%22">Olsbye, Unni</searchLink><relatesTo>1</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Beato%2C+Pablo%22">Beato, Pablo</searchLink><relatesTo>3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Bordiga%2C+Silvia%22">Bordiga, Silvia</searchLink><relatesTo>2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Svelle%2C+Stian%22">Svelle, Stian</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> stian.svelle@kjemi.uio.no</i>
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  Data: <searchLink fieldCode="JN" term="%22Catalysis+Today%22">Catalysis Today</searchLink>. Jun2024, Vol. 436, pN.PAG-N.PAG. 1p.
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  Data: <searchLink fieldCode="DE" term="%22Oligomerization%22">Oligomerization</searchLink><br /><searchLink fieldCode="DE" term="%22Partial+oxidation%22">Partial oxidation</searchLink><br /><searchLink fieldCode="DE" term="%22Methylation%22">Methylation</searchLink><br /><searchLink fieldCode="DE" term="%22Brønsted+acids%22">Brønsted acids</searchLink><br /><searchLink fieldCode="DE" term="%22Copper%22">Copper</searchLink><br /><searchLink fieldCode="DE" term="%22Zeolites%22">Zeolites</searchLink><br /><searchLink fieldCode="DE" term="%22Species%22">Species</searchLink><br /><searchLink fieldCode="DE" term="%22Toluene%22">Toluene</searchLink>
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  Data: Ethylene, propylene, and benzene were investigated as molecules for extracting methoxy intermediate species formed during the cyclic partial oxidation of methane in Cu-exchanged zeolites, promising materials for the step-wise methane-to-methanol (MTM) reaction. 13C-labeled reaction studies reveal that alkenes preferentially undergo oligomerization followed by cracking, while benzene is successfully methylated, forming toluene. Benzene methylation further showcases the methyl species to behave similar to surface methoxy species formed on Brønsted acid sites in methanol-to-hydrocarbon (MTH) reaction. However, benzene is only able to extract a fraction of the methyl species compared to the methanol produced with water extraction, indicating either steric or intrinsic mechanistic effects to limit the full potential of the methyl pool inside the framework. We infer the presence of reactive methoxy species on Brønsted acid sites generated under reaction conditions, revealing their potential as a synthetic platform to form additional products from methane. • Benzene reacts with the methoxy intermediate in the Cu-zeolite forming toluene. • Benzene and water access different amounts of methoxy; more than one type of methoxy. • Cu(I)-species formed after methane activation affect ethylene oligomerization. • Propylene oligomerizes independently of Cu species, BAS, or methoxy presence. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
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  Data: <i>Copyright of Catalysis Today is the property of Elsevier B.V. and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1016/j.cattod.2024.114729
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              Text: Jun2024
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