Mapping the Methanol‐to‐Gasoline Process Over Zeolite Beta
Decarbonizing the transportation sector is among the biggest challenges in the fight against climate change. CO2‐neutral fuels, such as those obtained from renewable methanol, have the potential to account for a large share of the solution, since these could be directly compatible with existing powe...
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Veröffentlicht in: | Angewandte Chemie International Edition 2023-06, Vol.62 (24), p.e202303124-n/a |
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creator | Ye, Yiru Abou‐Hamad, Edy Gong, Xuan Shoinkhorova, Tuiana B. Dokania, Abhay Gascon, Jorge Chowdhury, Abhishek Dutta |
description | Decarbonizing the transportation sector is among the biggest challenges in the fight against climate change. CO2‐neutral fuels, such as those obtained from renewable methanol, have the potential to account for a large share of the solution, since these could be directly compatible with existing power trains. Although discovered in 1977, the zeolite‐catalyzed methanol‐to‐gasoline (MTG) process has hardly reached industrial maturity, among other reasons, because maximizing the production of gasoline range hydrocarbons from methanol has proved complicated. In this work, we apply multimodal operando UV/Vis diffuse reflectance spectroscopy coupled with an online mass spectrometer and “mobility‐dependent” solid‐state NMR spectroscopy to better understand the reaction mechanism over zeolites H‐Beta and Zn‐Beta. Significantly, the influential co‐catalytic role of oxymethylene species is linked to gasoline formation, which impacts the MTG process more than carbonylated species.
A multimodal and complementary spectroscopic strategy (involving operando UV/Visible spectroscopy coupled to online mass spectrometry and solid‐state NMR spectroscopy) delivers a mechanistic blueprint of the zeolite‐catalyzed methanol‐to‐gasoline process by elucidating the impact of carbonylated and oxymethylene species. |
doi_str_mv | 10.1002/anie.202303124 |
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A multimodal and complementary spectroscopic strategy (involving operando UV/Visible spectroscopy coupled to online mass spectrometry and solid‐state NMR spectroscopy) delivers a mechanistic blueprint of the zeolite‐catalyzed methanol‐to‐gasoline process by elucidating the impact of carbonylated and oxymethylene species.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202303124</identifier><identifier>PMID: 37040129</identifier><language>eng</language><publisher>Germany: Wiley Subscription Services, Inc</publisher><subject>Carbon dioxide ; Carbonyls ; Climate change ; Decarbonization ; Diffuse reflectance spectroscopy ; Gasoline ; Magnetic resonance spectroscopy ; Methanol ; Methanol-to-Gasoline ; Methanol-to-Hydrocarbon ; NMR ; NMR spectroscopy ; Nuclear magnetic resonance ; Operando Study ; Powertrain ; Reaction Mechanism ; Reaction mechanisms ; Spectroscopy ; Transportation industry ; Zeolite ; Zeolites</subject><ispartof>Angewandte Chemie International Edition, 2023-06, Vol.62 (24), p.e202303124-n/a</ispartof><rights>2023 Wiley‐VCH GmbH</rights><rights>2023 Wiley-VCH GmbH.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c3734-f26da2dbbff0fa9200a1480a0d9fdfa0455278173aa9fa8cc32dd9a42333e32f3</citedby><cites>FETCH-LOGICAL-c3734-f26da2dbbff0fa9200a1480a0d9fdfa0455278173aa9fa8cc32dd9a42333e32f3</cites><orcidid>0000-0002-4121-7375</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.202303124$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.202303124$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/37040129$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Ye, Yiru</creatorcontrib><creatorcontrib>Abou‐Hamad, Edy</creatorcontrib><creatorcontrib>Gong, Xuan</creatorcontrib><creatorcontrib>Shoinkhorova, Tuiana B.</creatorcontrib><creatorcontrib>Dokania, Abhay</creatorcontrib><creatorcontrib>Gascon, Jorge</creatorcontrib><creatorcontrib>Chowdhury, Abhishek Dutta</creatorcontrib><title>Mapping the Methanol‐to‐Gasoline Process Over Zeolite Beta</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>Decarbonizing the transportation sector is among the biggest challenges in the fight against climate change. CO2‐neutral fuels, such as those obtained from renewable methanol, have the potential to account for a large share of the solution, since these could be directly compatible with existing power trains. Although discovered in 1977, the zeolite‐catalyzed methanol‐to‐gasoline (MTG) process has hardly reached industrial maturity, among other reasons, because maximizing the production of gasoline range hydrocarbons from methanol has proved complicated. In this work, we apply multimodal operando UV/Vis diffuse reflectance spectroscopy coupled with an online mass spectrometer and “mobility‐dependent” solid‐state NMR spectroscopy to better understand the reaction mechanism over zeolites H‐Beta and Zn‐Beta. Significantly, the influential co‐catalytic role of oxymethylene species is linked to gasoline formation, which impacts the MTG process more than carbonylated species.
A multimodal and complementary spectroscopic strategy (involving operando UV/Visible spectroscopy coupled to online mass spectrometry and solid‐state NMR spectroscopy) delivers a mechanistic blueprint of the zeolite‐catalyzed methanol‐to‐gasoline process by elucidating the impact of carbonylated and oxymethylene species.</description><subject>Carbon dioxide</subject><subject>Carbonyls</subject><subject>Climate change</subject><subject>Decarbonization</subject><subject>Diffuse reflectance spectroscopy</subject><subject>Gasoline</subject><subject>Magnetic resonance spectroscopy</subject><subject>Methanol</subject><subject>Methanol-to-Gasoline</subject><subject>Methanol-to-Hydrocarbon</subject><subject>NMR</subject><subject>NMR spectroscopy</subject><subject>Nuclear magnetic resonance</subject><subject>Operando Study</subject><subject>Powertrain</subject><subject>Reaction Mechanism</subject><subject>Reaction mechanisms</subject><subject>Spectroscopy</subject><subject>Transportation industry</subject><subject>Zeolite</subject><subject>Zeolites</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><recordid>eNqFkDtLxEAQxxdRfLeWErCxybk7k7i7jaCHL_BVaGOzzCWzGsklZzan2PkR_Ix-ElfOB9jYzAzDb34MfyE2lBwoKWGHmooHIAElKsjmxLLKQaWoNc7HOUNMtcnVklgJ4SHyxsjdRbGEWmZSgV0We-c0mVTNXdLfc3LO_T01bf3--ta3sRxTaOuq4eSqawsOIbl84i655bjsOTngntbEgqc68PpXXxU3R4fXw5P07PL4dLh_lhaoMUs97JYE5WjkvfRkQUpSmZEkS-tLTzLLc9BGaSSynkxRIJSlpQwQkRE8rortmXfStY9TDr0bV6HguqaG22lwoK01oHWOEd36gz60066J3zkwoHJl0KpIDWZU0bUhdOzdpKvG1L04Jd1nsu4zWfeTbDzY_NJOR2Muf_DvKCNgZ8BzVfPLPzq3f3F6-Cv_ANu1hVs</recordid><startdate>20230612</startdate><enddate>20230612</enddate><creator>Ye, Yiru</creator><creator>Abou‐Hamad, Edy</creator><creator>Gong, Xuan</creator><creator>Shoinkhorova, Tuiana B.</creator><creator>Dokania, Abhay</creator><creator>Gascon, Jorge</creator><creator>Chowdhury, Abhishek Dutta</creator><general>Wiley Subscription Services, Inc</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-4121-7375</orcidid></search><sort><creationdate>20230612</creationdate><title>Mapping the Methanol‐to‐Gasoline Process Over Zeolite Beta</title><author>Ye, Yiru ; Abou‐Hamad, Edy ; Gong, Xuan ; Shoinkhorova, Tuiana B. ; Dokania, Abhay ; Gascon, Jorge ; Chowdhury, Abhishek Dutta</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3734-f26da2dbbff0fa9200a1480a0d9fdfa0455278173aa9fa8cc32dd9a42333e32f3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Carbon dioxide</topic><topic>Carbonyls</topic><topic>Climate change</topic><topic>Decarbonization</topic><topic>Diffuse reflectance spectroscopy</topic><topic>Gasoline</topic><topic>Magnetic resonance spectroscopy</topic><topic>Methanol</topic><topic>Methanol-to-Gasoline</topic><topic>Methanol-to-Hydrocarbon</topic><topic>NMR</topic><topic>NMR spectroscopy</topic><topic>Nuclear magnetic resonance</topic><topic>Operando Study</topic><topic>Powertrain</topic><topic>Reaction Mechanism</topic><topic>Reaction mechanisms</topic><topic>Spectroscopy</topic><topic>Transportation industry</topic><topic>Zeolite</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ye, Yiru</creatorcontrib><creatorcontrib>Abou‐Hamad, Edy</creatorcontrib><creatorcontrib>Gong, Xuan</creatorcontrib><creatorcontrib>Shoinkhorova, Tuiana B.</creatorcontrib><creatorcontrib>Dokania, Abhay</creatorcontrib><creatorcontrib>Gascon, Jorge</creatorcontrib><creatorcontrib>Chowdhury, Abhishek Dutta</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ye, Yiru</au><au>Abou‐Hamad, Edy</au><au>Gong, Xuan</au><au>Shoinkhorova, Tuiana B.</au><au>Dokania, Abhay</au><au>Gascon, Jorge</au><au>Chowdhury, Abhishek Dutta</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Mapping the Methanol‐to‐Gasoline Process Over Zeolite Beta</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2023-06-12</date><risdate>2023</risdate><volume>62</volume><issue>24</issue><spage>e202303124</spage><epage>n/a</epage><pages>e202303124-n/a</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>Decarbonizing the transportation sector is among the biggest challenges in the fight against climate change. 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subjects | Carbon dioxide Carbonyls Climate change Decarbonization Diffuse reflectance spectroscopy Gasoline Magnetic resonance spectroscopy Methanol Methanol-to-Gasoline Methanol-to-Hydrocarbon NMR NMR spectroscopy Nuclear magnetic resonance Operando Study Powertrain Reaction Mechanism Reaction mechanisms Spectroscopy Transportation industry Zeolite Zeolites |
title | Mapping the Methanol‐to‐Gasoline Process Over Zeolite Beta |
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