Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process

After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the “direct mechanism”‐derived molecules (that is, methyl acetate) during MTH, and su...

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Vydáno v:	Angewandte Chemie International Edition Ročník 57; číslo 27; s. 8095 - 8099
Hlavní autoři:	Chowdhury, Abhishek Dutta, Paioni, Alessandra Lucini, Houben, Klaartje, Whiting, Gareth T., Baldus, Marc, Weckhuysen, Bert M.
Médium:	Journal Article
Jazyk:	angličtina
Vydáno:	Germany Wiley Subscription Services, Inc 02.07.2018 John Wiley and Sons Inc
Vydání:	International ed. in English
Témata:	Acetic acid Carbon Catalysis Communication Communications Diffuse reflectance spectroscopy heterogeneous catalysis hydrocarbon pool Hydrocarbons Magnetic resonance spectroscopy Methanol Methyl acetate Molecular chains NMR spectroscopy Organic chemistry Reaction centers reaction mechanisms solid-state NMR Spectroscopy zeolites reaction mechanisms solid-state NMR zeolites heterogeneous catalysis hydrocarbon pool
ISSN:	1433-7851, 1521-3773, 1521-3773
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Abstract	After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the “direct mechanism”‐derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H‐SAPO‐34 catalyst, using a combination of advanced solid‐state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on‐line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C−C bond‐containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon‐based co‐catalytic organic reaction centers. Like a MTH to a flame: The direct mechanism of the zeolite‐catalyzed methanol‐to‐hydrocarbon (MTH) process directly generates co‐catalytic hydrocarbon reaction centers in the hydrocarbon pool. Advanced solid‐state NMR spectroscopy, mass spectrometry, and UV/Vis diffuse reflectance spectroscopy provide evidence for the formation of olefinic and aromatic species in the hydrocarbon pool.
AbstractList	After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the “direct mechanism”‐derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H‐SAPO‐34 catalyst, using a combination of advanced solid‐state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on‐line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C−C bond‐containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon‐based co‐catalytic organic reaction centers. After a prolonged effort over many years, the route for the formation of a direct carbon-carbon (C-C) bond during the methanol-to-hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the "direct mechanism"-derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H-SAPO-34 catalyst, using a combination of advanced solid-state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on-line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C-C bond-containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon-based co-catalytic organic reaction centers.After a prolonged effort over many years, the route for the formation of a direct carbon-carbon (C-C) bond during the methanol-to-hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the "direct mechanism"-derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H-SAPO-34 catalyst, using a combination of advanced solid-state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on-line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C-C bond-containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon-based co-catalytic organic reaction centers. After a prolonged effort over many years, the route for the formation of a direct carbon-carbon (C-C) bond during the methanol-to-hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the "direct mechanism"-derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H-SAPO-34 catalyst, using a combination of advanced solid-state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on-line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C-C bond-containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon-based co-catalytic organic reaction centers. After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has very recently been unveiled. However, the relevance of the “direct mechanism”‐derived molecules (that is, methyl acetate) during MTH, and subsequent transformation routes to the conventional hydrocarbon pool (HCP) species, are yet to be established. This important piece of the MTH chemistry puzzle is not only essential from a fundamental perspective, but is also important to maximize catalytic performance. The MTH process was probed over a commercially relevant H‐SAPO‐34 catalyst, using a combination of advanced solid‐state NMR spectroscopy and operando UV/Vis diffuse reflectance spectroscopy coupled to an on‐line mass spectrometer. Spectroscopic evidence is provided for the formation of (olefinic and aromatic) HCP species, which are indeed derived exclusively from the direct C−C bond‐containing acetyl group of methyl acetate. New mechanistic insights have been obtained from the MTH process, including the identification of hydrocarbon‐based co‐catalytic organic reaction centers. Like a MTH to a flame: The direct mechanism of the zeolite‐catalyzed methanol‐to‐hydrocarbon (MTH) process directly generates co‐catalytic hydrocarbon reaction centers in the hydrocarbon pool. Advanced solid‐state NMR spectroscopy, mass spectrometry, and UV/Vis diffuse reflectance spectroscopy provide evidence for the formation of olefinic and aromatic species in the hydrocarbon pool.
Author	Chowdhury, Abhishek Dutta Baldus, Marc Weckhuysen, Bert M. Paioni, Alessandra Lucini Houben, Klaartje Whiting, Gareth T.
AuthorAffiliation	3 Current address: DSM Food Specialties DSM Biotechnology Center R&D analysis Alexander Flemminglaan 1 2613 AX Delft The Netherlands 1 Inorganic Chemistry and Catalysis Group Debye Institute for Nanomaterials Science Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands 2 NMR Spectroscopy group Bijvoet Center for Biomolecular Research Utrecht University Padualaan 8 3584 CH Utrecht The Netherlands
AuthorAffiliation_xml	– name: 1 Inorganic Chemistry and Catalysis Group Debye Institute for Nanomaterials Science Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands – name: 3 Current address: DSM Food Specialties DSM Biotechnology Center R&D analysis Alexander Flemminglaan 1 2613 AX Delft The Netherlands – name: 2 NMR Spectroscopy group Bijvoet Center for Biomolecular Research Utrecht University Padualaan 8 3584 CH Utrecht The Netherlands
Author_xml	– sequence: 1 givenname: Abhishek Dutta surname: Chowdhury fullname: Chowdhury, Abhishek Dutta organization: Utrecht University – sequence: 2 givenname: Alessandra Lucini surname: Paioni fullname: Paioni, Alessandra Lucini organization: Utrecht University – sequence: 3 givenname: Klaartje surname: Houben fullname: Houben, Klaartje organization: Current address: DSM Food Specialties – sequence: 4 givenname: Gareth T. surname: Whiting fullname: Whiting, Gareth T. organization: Utrecht University – sequence: 5 givenname: Marc surname: Baldus fullname: Baldus, Marc organization: Utrecht University – sequence: 6 givenname: Bert M. orcidid: 0000-0001-5245-1426 surname: Weckhuysen fullname: Weckhuysen, Bert M. email: b.m.weckhuysen@uu.nl organization: Utrecht University
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/29710435$$D View this record in MEDLINE/PubMed
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Snippet	After a prolonged effort over many years, the route for the formation of a direct carbon−carbon (C−C) bond during the methanol‐to‐hydrocarbon (MTH) process has... After a prolonged effort over many years, the route for the formation of a direct carbon-carbon (C-C) bond during the methanol-to-hydrocarbon (MTH) process has...
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SubjectTerms	Acetic acid Carbon Catalysis Communication Communications Diffuse reflectance spectroscopy heterogeneous catalysis hydrocarbon pool Hydrocarbons Magnetic resonance spectroscopy Methanol Methyl acetate Molecular chains NMR spectroscopy Organic chemistry Reaction centers reaction mechanisms solid-state NMR Spectroscopy zeolites
Title	Bridging the Gap between the Direct and Hydrocarbon Pool Mechanisms of the Methanol‐to‐Hydrocarbons Process
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