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Features of the Mechanism of the Dimethyl Ether to Light Olefins Conversion over MgZSM-5/Al2O3: Study by Vibrational Spectroscopy Experimental and Theoretical Methods
Features of the mechanism of dimethyl ether (DME) conversion to olefins over ZSM-5 zeolite catalysts were studied using experimental and theoretical methods of vibrational spectroscopy. A catalytic activity comparison of the catalysts Mg-HZSM-5 without a binder and Mg-HZSM-5/Al 2 O 3 containing 1% M...
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| Published in: | Catalysis letters 2021-05, Vol.151 (5), p.1309-1319 |
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| container_start_page | 1309 |
| container_title | Catalysis letters |
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| creator | Bondarenko, G. N. Rodionov, A. S. Kolesnichenko, N. V. Batova, T. I. Khivrich, E. N. Maximov, A. L. |
| description | Features of the mechanism of dimethyl ether (DME) conversion to olefins over ZSM-5 zeolite catalysts were studied using experimental and theoretical methods of vibrational spectroscopy. A catalytic activity comparison of the catalysts Mg-HZSM-5 without a binder and Mg-HZSM-5/Al
2
O
3
containing 1% Mg (by weight) and 33% Al
2
O
3
(by weight) as a binder in the DME conversion was carried out. Using high-temperature diffuse reflectance IR (DRIR) spectroscopy in situ combined with quantum-chemical simulations in the temperature range of 25–450 °C in a stream of dry Ar and DME, the bands corresponding to OH bonds, including BAS and H
3
O
+
, were interpreted. Depending on the temperature and the presence of magnesium and a binder in the catalyst composition, the intensity and position of these bands maxima vary greatly. The intermediates of the catalytic DME conversion were discovered and identified. At low temperatures (below 200 °C), in a DME stream, methoxy groups (CH
3
O-Al-), ketene (CH
2
=C=O), and a carbocation (CH
3
+) were formed on the surface of the catalysts. As the temperature rises (above 300° C), the bands from ketene completely disappear in the spectra of catalysts, and bands from oxonium cations or ylide particles appear, leading the process of DME conversion by the oxonium-ylide mechanism. In the presence of H
3
O
+
, the conversion of DME on the zeolite catalyst surface was more effective; however, selectivity for olefins was lower.
Graphical Abstract |
| doi_str_mv | 10.1007/s10562-020-03399-2 |
| format | article |
| fullrecord | <record><control><sourceid>proquest_cross</sourceid><recordid>TN_cdi_proquest_journals_2510493750</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2510493750</sourcerecordid><originalsourceid>FETCH-LOGICAL-c400t-fc12793d7e9bd48c160e406688a8001249ef69ef79f9818e141f4ac3924939f43</originalsourceid><addsrcrecordid>eNp9kcFu1DAQhiMEEqXwApwscTYd20kcc6uWLSDtag9bUMUl8jrjTao0Dra3Ii_EczKwIG4cLM94vn_Go78oXgt4KwD0VRJQ1ZKDBA5KGcPlk-JCVFryRpu7pxSDEFxpefe8eJHSPQAYLcxF8eMGbT5FTCx4lntkW3S9nYb08Pfh_fCAuV9GtqYsshzYZjj2me1G9MOU2CpMjxjTECYWKGDb49f9lldX16PcqXdsn0_dwg4L-zIcos2E2ZHtZ3Q5huTCvLD19xkjDZkyVezUsdseQ8Q8OMq3NDt06WXxzNsx4as_92Xx-WZ9u_rIN7sPn1bXG-5KgMy9E1Ib1Wk0h65snKgBS6jrprENgJClQV_T0cabRjQoSuFL65ShijK-VJfFm3PfOYZvJ0y5vQ-nSF9OrawEEKUrIEqeKUc7pIi-nWkBG5dWQPvLj_bsR0t-tL_9aCWJ1FmUCJ6OGP-1_o_qJ6QVjtw</addsrcrecordid><sourcetype>Aggregation Database</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2510493750</pqid></control><display><type>article</type><title>Features of the Mechanism of the Dimethyl Ether to Light Olefins Conversion over MgZSM-5/Al2O3: Study by Vibrational Spectroscopy Experimental and Theoretical Methods</title><source>Springer Link</source><creator>Bondarenko, G. N. ; Rodionov, A. S. ; Kolesnichenko, N. V. ; Batova, T. I. ; Khivrich, E. N. ; Maximov, A. L.</creator><creatorcontrib>Bondarenko, G. N. ; Rodionov, A. S. ; Kolesnichenko, N. V. ; Batova, T. I. ; Khivrich, E. N. ; Maximov, A. L.</creatorcontrib><description>Features of the mechanism of dimethyl ether (DME) conversion to olefins over ZSM-5 zeolite catalysts were studied using experimental and theoretical methods of vibrational spectroscopy. A catalytic activity comparison of the catalysts Mg-HZSM-5 without a binder and Mg-HZSM-5/Al
2
O
3
containing 1% Mg (by weight) and 33% Al
2
O
3
(by weight) as a binder in the DME conversion was carried out. Using high-temperature diffuse reflectance IR (DRIR) spectroscopy in situ combined with quantum-chemical simulations in the temperature range of 25–450 °C in a stream of dry Ar and DME, the bands corresponding to OH bonds, including BAS and H
3
O
+
, were interpreted. Depending on the temperature and the presence of magnesium and a binder in the catalyst composition, the intensity and position of these bands maxima vary greatly. The intermediates of the catalytic DME conversion were discovered and identified. At low temperatures (below 200 °C), in a DME stream, methoxy groups (CH
3
O-Al-), ketene (CH
2
=C=O), and a carbocation (CH
3
+) were formed on the surface of the catalysts. As the temperature rises (above 300° C), the bands from ketene completely disappear in the spectra of catalysts, and bands from oxonium cations or ylide particles appear, leading the process of DME conversion by the oxonium-ylide mechanism. In the presence of H
3
O
+
, the conversion of DME on the zeolite catalyst surface was more effective; however, selectivity for olefins was lower.
Graphical Abstract</description><identifier>ISSN: 1011-372X</identifier><identifier>EISSN: 1572-879X</identifier><identifier>DOI: 10.1007/s10562-020-03399-2</identifier><language>eng</language><publisher>New York: Springer US</publisher><subject>Alkenes ; Aluminum oxide ; Catalysis ; Catalysts ; Catalytic activity ; Catalytic converters ; Chemistry ; Chemistry and Materials Science ; Conversion ; Dimethyl ether ; High temperature ; Industrial Chemistry/Chemical Engineering ; Infrared spectroscopy ; Low temperature ; Magnesium ; Organometallic Chemistry ; Physical Chemistry ; Quantum chemistry ; Selectivity ; Spectrum analysis ; Weight ; Zeolites</subject><ispartof>Catalysis letters, 2021-05, Vol.151 (5), p.1309-1319</ispartof><rights>Springer Science+Business Media, LLC, part of Springer Nature 2020</rights><rights>Springer Science+Business Media, LLC, part of Springer Nature 2020.</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c400t-fc12793d7e9bd48c160e406688a8001249ef69ef79f9818e141f4ac3924939f43</citedby><cites>FETCH-LOGICAL-c400t-fc12793d7e9bd48c160e406688a8001249ef69ef79f9818e141f4ac3924939f43</cites><orcidid>0000-0001-9297-4950</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,780,784,27924,27925</link.rule.ids></links><search><creatorcontrib>Bondarenko, G. N.</creatorcontrib><creatorcontrib>Rodionov, A. S.</creatorcontrib><creatorcontrib>Kolesnichenko, N. V.</creatorcontrib><creatorcontrib>Batova, T. I.</creatorcontrib><creatorcontrib>Khivrich, E. N.</creatorcontrib><creatorcontrib>Maximov, A. L.</creatorcontrib><title>Features of the Mechanism of the Dimethyl Ether to Light Olefins Conversion over MgZSM-5/Al2O3: Study by Vibrational Spectroscopy Experimental and Theoretical Methods</title><title>Catalysis letters</title><addtitle>Catal Lett</addtitle><description>Features of the mechanism of dimethyl ether (DME) conversion to olefins over ZSM-5 zeolite catalysts were studied using experimental and theoretical methods of vibrational spectroscopy. A catalytic activity comparison of the catalysts Mg-HZSM-5 without a binder and Mg-HZSM-5/Al
2
O
3
containing 1% Mg (by weight) and 33% Al
2
O
3
(by weight) as a binder in the DME conversion was carried out. Using high-temperature diffuse reflectance IR (DRIR) spectroscopy in situ combined with quantum-chemical simulations in the temperature range of 25–450 °C in a stream of dry Ar and DME, the bands corresponding to OH bonds, including BAS and H
3
O
+
, were interpreted. Depending on the temperature and the presence of magnesium and a binder in the catalyst composition, the intensity and position of these bands maxima vary greatly. The intermediates of the catalytic DME conversion were discovered and identified. At low temperatures (below 200 °C), in a DME stream, methoxy groups (CH
3
O-Al-), ketene (CH
2
=C=O), and a carbocation (CH
3
+) were formed on the surface of the catalysts. As the temperature rises (above 300° C), the bands from ketene completely disappear in the spectra of catalysts, and bands from oxonium cations or ylide particles appear, leading the process of DME conversion by the oxonium-ylide mechanism. In the presence of H
3
O
+
, the conversion of DME on the zeolite catalyst surface was more effective; however, selectivity for olefins was lower.
Graphical Abstract</description><subject>Alkenes</subject><subject>Aluminum oxide</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Catalytic converters</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Conversion</subject><subject>Dimethyl ether</subject><subject>High temperature</subject><subject>Industrial Chemistry/Chemical Engineering</subject><subject>Infrared spectroscopy</subject><subject>Low temperature</subject><subject>Magnesium</subject><subject>Organometallic Chemistry</subject><subject>Physical Chemistry</subject><subject>Quantum chemistry</subject><subject>Selectivity</subject><subject>Spectrum analysis</subject><subject>Weight</subject><subject>Zeolites</subject><issn>1011-372X</issn><issn>1572-879X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><recordid>eNp9kcFu1DAQhiMEEqXwApwscTYd20kcc6uWLSDtag9bUMUl8jrjTao0Dra3Ii_EczKwIG4cLM94vn_Go78oXgt4KwD0VRJQ1ZKDBA5KGcPlk-JCVFryRpu7pxSDEFxpefe8eJHSPQAYLcxF8eMGbT5FTCx4lntkW3S9nYb08Pfh_fCAuV9GtqYsshzYZjj2me1G9MOU2CpMjxjTECYWKGDb49f9lldX16PcqXdsn0_dwg4L-zIcos2E2ZHtZ3Q5huTCvLD19xkjDZkyVezUsdseQ8Q8OMq3NDt06WXxzNsx4as_92Xx-WZ9u_rIN7sPn1bXG-5KgMy9E1Ib1Wk0h65snKgBS6jrprENgJClQV_T0cabRjQoSuFL65ShijK-VJfFm3PfOYZvJ0y5vQ-nSF9OrawEEKUrIEqeKUc7pIi-nWkBG5dWQPvLj_bsR0t-tL_9aCWJ1FmUCJ6OGP-1_o_qJ6QVjtw</recordid><startdate>20210501</startdate><enddate>20210501</enddate><creator>Bondarenko, G. N.</creator><creator>Rodionov, A. S.</creator><creator>Kolesnichenko, N. V.</creator><creator>Batova, T. I.</creator><creator>Khivrich, E. N.</creator><creator>Maximov, A. L.</creator><general>Springer US</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>8FE</scope><scope>8FG</scope><scope>ABJCF</scope><scope>AFKRA</scope><scope>BENPR</scope><scope>BGLVJ</scope><scope>CCPQU</scope><scope>D1I</scope><scope>DWQXO</scope><scope>HCIFZ</scope><scope>KB.</scope><scope>PDBOC</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>PRINS</scope><orcidid>https://orcid.org/0000-0001-9297-4950</orcidid></search><sort><creationdate>20210501</creationdate><title>Features of the Mechanism of the Dimethyl Ether to Light Olefins Conversion over MgZSM-5/Al2O3: Study by Vibrational Spectroscopy Experimental and Theoretical Methods</title><author>Bondarenko, G. N. ; Rodionov, A. S. ; Kolesnichenko, N. V. ; Batova, T. I. ; Khivrich, E. N. ; Maximov, A. L.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c400t-fc12793d7e9bd48c160e406688a8001249ef69ef79f9818e141f4ac3924939f43</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Alkenes</topic><topic>Aluminum oxide</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Catalytic converters</topic><topic>Chemistry</topic><topic>Chemistry and Materials Science</topic><topic>Conversion</topic><topic>Dimethyl ether</topic><topic>High temperature</topic><topic>Industrial Chemistry/Chemical Engineering</topic><topic>Infrared spectroscopy</topic><topic>Low temperature</topic><topic>Magnesium</topic><topic>Organometallic Chemistry</topic><topic>Physical Chemistry</topic><topic>Quantum chemistry</topic><topic>Selectivity</topic><topic>Spectrum analysis</topic><topic>Weight</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Bondarenko, G. N.</creatorcontrib><creatorcontrib>Rodionov, A. S.</creatorcontrib><creatorcontrib>Kolesnichenko, N. V.</creatorcontrib><creatorcontrib>Batova, T. I.</creatorcontrib><creatorcontrib>Khivrich, E. N.</creatorcontrib><creatorcontrib>Maximov, A. L.</creatorcontrib><collection>CrossRef</collection><collection>ProQuest SciTech Collection</collection><collection>ProQuest Technology Collection</collection><collection>Materials Science & Engineering Collection</collection><collection>ProQuest Central</collection><collection>ProQuest Central</collection><collection>Technology Collection</collection><collection>ProQuest One Community College</collection><collection>ProQuest Materials Science Collection</collection><collection>ProQuest Central</collection><collection>SciTech Premium Collection</collection><collection>Materials Science Database</collection><collection>Materials science collection</collection><collection>ProQuest One Academic Eastern Edition (DO NOT USE)</collection><collection>ProQuest One Academic</collection><collection>ProQuest One Academic UKI Edition</collection><collection>ProQuest Central China</collection><jtitle>Catalysis letters</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Bondarenko, G. N.</au><au>Rodionov, A. S.</au><au>Kolesnichenko, N. V.</au><au>Batova, T. I.</au><au>Khivrich, E. N.</au><au>Maximov, A. L.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Features of the Mechanism of the Dimethyl Ether to Light Olefins Conversion over MgZSM-5/Al2O3: Study by Vibrational Spectroscopy Experimental and Theoretical Methods</atitle><jtitle>Catalysis letters</jtitle><stitle>Catal Lett</stitle><date>2021-05-01</date><risdate>2021</risdate><volume>151</volume><issue>5</issue><spage>1309</spage><epage>1319</epage><pages>1309-1319</pages><issn>1011-372X</issn><eissn>1572-879X</eissn><abstract>Features of the mechanism of dimethyl ether (DME) conversion to olefins over ZSM-5 zeolite catalysts were studied using experimental and theoretical methods of vibrational spectroscopy. A catalytic activity comparison of the catalysts Mg-HZSM-5 without a binder and Mg-HZSM-5/Al
2
O
3
containing 1% Mg (by weight) and 33% Al
2
O
3
(by weight) as a binder in the DME conversion was carried out. Using high-temperature diffuse reflectance IR (DRIR) spectroscopy in situ combined with quantum-chemical simulations in the temperature range of 25–450 °C in a stream of dry Ar and DME, the bands corresponding to OH bonds, including BAS and H
3
O
+
, were interpreted. Depending on the temperature and the presence of magnesium and a binder in the catalyst composition, the intensity and position of these bands maxima vary greatly. The intermediates of the catalytic DME conversion were discovered and identified. At low temperatures (below 200 °C), in a DME stream, methoxy groups (CH
3
O-Al-), ketene (CH
2
=C=O), and a carbocation (CH
3
+) were formed on the surface of the catalysts. As the temperature rises (above 300° C), the bands from ketene completely disappear in the spectra of catalysts, and bands from oxonium cations or ylide particles appear, leading the process of DME conversion by the oxonium-ylide mechanism. In the presence of H
3
O
+
, the conversion of DME on the zeolite catalyst surface was more effective; however, selectivity for olefins was lower.
Graphical Abstract</abstract><cop>New York</cop><pub>Springer US</pub><doi>10.1007/s10562-020-03399-2</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0001-9297-4950</orcidid><oa>free_for_read</oa></addata></record> |
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| ispartof | Catalysis letters, 2021-05, Vol.151 (5), p.1309-1319 |
| issn | 1011-372X 1572-879X |
| language | eng |
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| source | Springer Link |
| subjects | Alkenes Aluminum oxide Catalysis Catalysts Catalytic activity Catalytic converters Chemistry Chemistry and Materials Science Conversion Dimethyl ether High temperature Industrial Chemistry/Chemical Engineering Infrared spectroscopy Low temperature Magnesium Organometallic Chemistry Physical Chemistry Quantum chemistry Selectivity Spectrum analysis Weight Zeolites |
| title | Features of the Mechanism of the Dimethyl Ether to Light Olefins Conversion over MgZSM-5/Al2O3: Study by Vibrational Spectroscopy Experimental and Theoretical Methods |
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