Conversion of [ 14C]methanol and propane mixtures with H-ZSM-5
One of the major discoveries in zeolite catalysis was the conversion of methanol to gasoline using H-ZSM-5 catalysts. While there have been many mechanistic studies, the reaction pathway and the C{sub 1} species involved in the reaction remain uncertain. The proposed mechanisms may be classified int...
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| Veröffentlicht in: | Journal of catalysis 1988-11, Vol.114 (1), p.190-195 |
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| creator | Tau, Li-Min Bao, Shiqi Davis, Burtron H. |
| description | One of the major discoveries in zeolite catalysis was the conversion of methanol to gasoline using H-ZSM-5 catalysts. While there have been many mechanistic studies, the reaction pathway and the C{sub 1} species involved in the reaction remain uncertain. The proposed mechanisms may be classified into three groups based upon the required intermediate: (a) mechanisms utilizing carbene (:CH{sub 2}), (b) mechanisms utilizing cations (e.g., CH{sub 3}{sup +}), and (c) mechanisms utilizing trimethyloxonium ions ((CH{sub 3}){sub 3}O{sup +}) or similar oxygen-containing species. Preliminary {sup 14}C tracer studies provided evidence that was consistent with the oxonium ion intermediate. Refinements in the {sup 14}C analytical procedures showed that the {sup 14}C added in propanol had completely scrambled with the methanol carbon and the data could therefore not define the intermediate species. Considering the importance of experiments with the methanol-propane mixture to an understanding of the methanol to gasoline conversion, the author has carried out studies using {sup 14}CH{sub 3}OH and unlabeled propane. |
| doi_str_mv | 10.1016/0021-9517(88)90021-8 |
| format | Article |
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While there have been many mechanistic studies, the reaction pathway and the C{sub 1} species involved in the reaction remain uncertain. The proposed mechanisms may be classified into three groups based upon the required intermediate: (a) mechanisms utilizing carbene (:CH{sub 2}), (b) mechanisms utilizing cations (e.g., CH{sub 3}{sup +}), and (c) mechanisms utilizing trimethyloxonium ions ((CH{sub 3}){sub 3}O{sup +}) or similar oxygen-containing species. Preliminary {sup 14}C tracer studies provided evidence that was consistent with the oxonium ion intermediate. Refinements in the {sup 14}C analytical procedures showed that the {sup 14}C added in propanol had completely scrambled with the methanol carbon and the data could therefore not define the intermediate species. Considering the importance of experiments with the methanol-propane mixture to an understanding of the methanol to gasoline conversion, the author has carried out studies using {sup 14}CH{sub 3}OH and unlabeled propane.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/0021-9517(88)90021-8</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>01 COAL, LIGNITE, AND PEAT ; ALCOHOLS ; ALKANES ; BETA DECAY RADIOISOTOPES ; BETA-MINUS DECAY RADIOISOTOPES ; CARBON 14 ; CARBON ISOTOPES ; CATALYTIC EFFECTS ; CHARGED PARTICLES ; CHEMICAL REACTION KINETICS ; CHEMICAL REACTIONS ; Chemistry ; DISPERSIONS ; EVEN-EVEN NUCLEI ; Exact sciences and technology ; FUELS ; GASOLINE ; HYDROCARBONS ; HYDROXY COMPOUNDS ; INORGANIC ION EXCHANGERS ; ION EXCHANGE MATERIALS ; IONS ; ISOTOPES ; KINETICS ; Kinetics and mechanisms ; LABELLED COMPOUNDS ; LIGHT NUCLEI ; LIQUID FUELS ; MATERIALS ; METHANOL ; MINERALS ; MIXTURES ; MOLECULAR IONS ; NUCLEI ; Organic chemistry ; ORGANIC COMPOUNDS ; OXONIUM IONS ; PETROLEUM PRODUCTS ; PROPANE ; RADIOISOTOPES ; REACTION INTERMEDIATES ; REACTION KINETICS ; Reactivity and mechanisms ; SYNTHESIS ; YEARS LIVING RADIOISOTOPES 010408 -- Coal, Lignite, & Peat-- C1 Processes-- (1987-) ; ZEOLITES</subject><ispartof>Journal of catalysis, 1988-11, Vol.114 (1), p.190-195</ispartof><rights>1988</rights><rights>1989 INIST-CNRS</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c398t-f09423d1fd4a4bed739005345adf263b36a844ad35a8fc8169fa5ac520bea03d3</citedby><cites>FETCH-LOGICAL-c398t-f09423d1fd4a4bed739005345adf263b36a844ad35a8fc8169fa5ac520bea03d3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/0021-9517(88)90021-8$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>230,314,780,784,885,3550,27924,27925,45995</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=7131422$$DView record in Pascal Francis$$Hfree_for_read</backlink><backlink>$$Uhttps://www.osti.gov/biblio/6845298$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Tau, Li-Min</creatorcontrib><creatorcontrib>Bao, Shiqi</creatorcontrib><creatorcontrib>Davis, Burtron H.</creatorcontrib><title>Conversion of [ 14C]methanol and propane mixtures with H-ZSM-5</title><title>Journal of catalysis</title><description>One of the major discoveries in zeolite catalysis was the conversion of methanol to gasoline using H-ZSM-5 catalysts. While there have been many mechanistic studies, the reaction pathway and the C{sub 1} species involved in the reaction remain uncertain. The proposed mechanisms may be classified into three groups based upon the required intermediate: (a) mechanisms utilizing carbene (:CH{sub 2}), (b) mechanisms utilizing cations (e.g., CH{sub 3}{sup +}), and (c) mechanisms utilizing trimethyloxonium ions ((CH{sub 3}){sub 3}O{sup +}) or similar oxygen-containing species. Preliminary {sup 14}C tracer studies provided evidence that was consistent with the oxonium ion intermediate. Refinements in the {sup 14}C analytical procedures showed that the {sup 14}C added in propanol had completely scrambled with the methanol carbon and the data could therefore not define the intermediate species. Considering the importance of experiments with the methanol-propane mixture to an understanding of the methanol to gasoline conversion, the author has carried out studies using {sup 14}CH{sub 3}OH and unlabeled propane.</description><subject>01 COAL, LIGNITE, AND PEAT</subject><subject>ALCOHOLS</subject><subject>ALKANES</subject><subject>BETA DECAY RADIOISOTOPES</subject><subject>BETA-MINUS DECAY RADIOISOTOPES</subject><subject>CARBON 14</subject><subject>CARBON ISOTOPES</subject><subject>CATALYTIC EFFECTS</subject><subject>CHARGED PARTICLES</subject><subject>CHEMICAL REACTION KINETICS</subject><subject>CHEMICAL REACTIONS</subject><subject>Chemistry</subject><subject>DISPERSIONS</subject><subject>EVEN-EVEN NUCLEI</subject><subject>Exact sciences and technology</subject><subject>FUELS</subject><subject>GASOLINE</subject><subject>HYDROCARBONS</subject><subject>HYDROXY COMPOUNDS</subject><subject>INORGANIC ION EXCHANGERS</subject><subject>ION EXCHANGE MATERIALS</subject><subject>IONS</subject><subject>ISOTOPES</subject><subject>KINETICS</subject><subject>Kinetics and mechanisms</subject><subject>LABELLED COMPOUNDS</subject><subject>LIGHT NUCLEI</subject><subject>LIQUID FUELS</subject><subject>MATERIALS</subject><subject>METHANOL</subject><subject>MINERALS</subject><subject>MIXTURES</subject><subject>MOLECULAR IONS</subject><subject>NUCLEI</subject><subject>Organic chemistry</subject><subject>ORGANIC COMPOUNDS</subject><subject>OXONIUM IONS</subject><subject>PETROLEUM PRODUCTS</subject><subject>PROPANE</subject><subject>RADIOISOTOPES</subject><subject>REACTION INTERMEDIATES</subject><subject>REACTION KINETICS</subject><subject>Reactivity and mechanisms</subject><subject>SYNTHESIS</subject><subject>YEARS LIVING RADIOISOTOPES 010408 -- Coal, Lignite, & Peat-- C1 Processes-- (1987-)</subject><subject>ZEOLITES</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>1988</creationdate><recordtype>article</recordtype><recordid>eNp9kE1LAzEURYMoWKv_wEUQF7oYzec0synIoFZQXKgbRUKaDxppkyEZq_57ZzrSpatH4Ny8-w4AxxhdYITLS4QILiqOJ2dCnFebl9gBI4wqVJCyYrtgtEX2wUHOHwhhzLkYgWkdw9qm7GOA0cE3iFn9vrLtQoW4hCoY2KTYqGDhyn-3n8lm-OXbBZwVr08PBT8Ee04tsz36m2PwcnP9XM-K-8fbu_rqvtC0Em3hUMUINdgZptjcmgntWnLKuDKOlHROSyUYU4ZyJZwWuKyc4kpzguZWIWroGJwM_8bcepm1b61e6BiC1a0sBeOkEh3EBkinmHOyTjbJr1T6kRjJXpTsLcjeghRCbkTJPnY6xBqVtVq6pIL2eZudYIoZIR02HTDb3bn2NvU1bNDW-NS3MNH_v-cXsYJ58g</recordid><startdate>19881101</startdate><enddate>19881101</enddate><creator>Tau, Li-Min</creator><creator>Bao, Shiqi</creator><creator>Davis, Burtron H.</creator><general>Elsevier Inc</general><general>Elsevier</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>OTOTI</scope></search><sort><creationdate>19881101</creationdate><title>Conversion of [ 14C]methanol and propane mixtures with H-ZSM-5</title><author>Tau, Li-Min ; Bao, Shiqi ; Davis, Burtron H.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c398t-f09423d1fd4a4bed739005345adf263b36a844ad35a8fc8169fa5ac520bea03d3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>1988</creationdate><topic>01 COAL, LIGNITE, AND PEAT</topic><topic>ALCOHOLS</topic><topic>ALKANES</topic><topic>BETA DECAY RADIOISOTOPES</topic><topic>BETA-MINUS DECAY RADIOISOTOPES</topic><topic>CARBON 14</topic><topic>CARBON ISOTOPES</topic><topic>CATALYTIC EFFECTS</topic><topic>CHARGED PARTICLES</topic><topic>CHEMICAL REACTION KINETICS</topic><topic>CHEMICAL REACTIONS</topic><topic>Chemistry</topic><topic>DISPERSIONS</topic><topic>EVEN-EVEN NUCLEI</topic><topic>Exact sciences and technology</topic><topic>FUELS</topic><topic>GASOLINE</topic><topic>HYDROCARBONS</topic><topic>HYDROXY COMPOUNDS</topic><topic>INORGANIC ION EXCHANGERS</topic><topic>ION EXCHANGE MATERIALS</topic><topic>IONS</topic><topic>ISOTOPES</topic><topic>KINETICS</topic><topic>Kinetics and mechanisms</topic><topic>LABELLED COMPOUNDS</topic><topic>LIGHT NUCLEI</topic><topic>LIQUID FUELS</topic><topic>MATERIALS</topic><topic>METHANOL</topic><topic>MINERALS</topic><topic>MIXTURES</topic><topic>MOLECULAR IONS</topic><topic>NUCLEI</topic><topic>Organic chemistry</topic><topic>ORGANIC COMPOUNDS</topic><topic>OXONIUM IONS</topic><topic>PETROLEUM PRODUCTS</topic><topic>PROPANE</topic><topic>RADIOISOTOPES</topic><topic>REACTION INTERMEDIATES</topic><topic>REACTION KINETICS</topic><topic>Reactivity and mechanisms</topic><topic>SYNTHESIS</topic><topic>YEARS LIVING RADIOISOTOPES 010408 -- Coal, Lignite, & Peat-- C1 Processes-- (1987-)</topic><topic>ZEOLITES</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Tau, Li-Min</creatorcontrib><creatorcontrib>Bao, Shiqi</creatorcontrib><creatorcontrib>Davis, Burtron H.</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><collection>OSTI.GOV</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Tau, Li-Min</au><au>Bao, Shiqi</au><au>Davis, Burtron H.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Conversion of [ 14C]methanol and propane mixtures with H-ZSM-5</atitle><jtitle>Journal of catalysis</jtitle><date>1988-11-01</date><risdate>1988</risdate><volume>114</volume><issue>1</issue><spage>190</spage><epage>195</epage><pages>190-195</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>One of the major discoveries in zeolite catalysis was the conversion of methanol to gasoline using H-ZSM-5 catalysts. While there have been many mechanistic studies, the reaction pathway and the C{sub 1} species involved in the reaction remain uncertain. The proposed mechanisms may be classified into three groups based upon the required intermediate: (a) mechanisms utilizing carbene (:CH{sub 2}), (b) mechanisms utilizing cations (e.g., CH{sub 3}{sup +}), and (c) mechanisms utilizing trimethyloxonium ions ((CH{sub 3}){sub 3}O{sup +}) or similar oxygen-containing species. Preliminary {sup 14}C tracer studies provided evidence that was consistent with the oxonium ion intermediate. Refinements in the {sup 14}C analytical procedures showed that the {sup 14}C added in propanol had completely scrambled with the methanol carbon and the data could therefore not define the intermediate species. Considering the importance of experiments with the methanol-propane mixture to an understanding of the methanol to gasoline conversion, the author has carried out studies using {sup 14}CH{sub 3}OH and unlabeled propane.</abstract><cop>Amsterdam</cop><pub>Elsevier Inc</pub><doi>10.1016/0021-9517(88)90021-8</doi><tpages>6</tpages></addata></record> |
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| ispartof | Journal of catalysis, 1988-11, Vol.114 (1), p.190-195 |
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| subjects | 01 COAL, LIGNITE, AND PEAT ALCOHOLS ALKANES BETA DECAY RADIOISOTOPES BETA-MINUS DECAY RADIOISOTOPES CARBON 14 CARBON ISOTOPES CATALYTIC EFFECTS CHARGED PARTICLES CHEMICAL REACTION KINETICS CHEMICAL REACTIONS Chemistry DISPERSIONS EVEN-EVEN NUCLEI Exact sciences and technology FUELS GASOLINE HYDROCARBONS HYDROXY COMPOUNDS INORGANIC ION EXCHANGERS ION EXCHANGE MATERIALS IONS ISOTOPES KINETICS Kinetics and mechanisms LABELLED COMPOUNDS LIGHT NUCLEI LIQUID FUELS MATERIALS METHANOL MINERALS MIXTURES MOLECULAR IONS NUCLEI Organic chemistry ORGANIC COMPOUNDS OXONIUM IONS PETROLEUM PRODUCTS PROPANE RADIOISOTOPES REACTION INTERMEDIATES REACTION KINETICS Reactivity and mechanisms SYNTHESIS YEARS LIVING RADIOISOTOPES 010408 -- Coal, Lignite, & Peat-- C1 Processes-- (1987-) ZEOLITES |
| title | Conversion of [ 14C]methanol and propane mixtures with H-ZSM-5 |
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