Size-Controlled Synthesis of Metallosilicates with MTW Structure and Catalytic Performance for Methanol-to-Propylene Reaction

The synthesis of metallosilicates with a MTW structure was achieved using tetraethylammonium bromide (TEABr) and methyltriethylammonium chloride (MTEACl) as organic structure-directing agents (OSDAs). MTW zeolites (Al-MTW, Si-MTW, Fe-MTW and (Al, Fe)-MTW) were obtained by hydrothermal synthesis. The...

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Veröffentlicht in:Catalysis letters 2016-03, Vol.146 (3), p.666-676
Hauptverfasser: Taniguchi, Taichi, Nakasaka, Yuta, Yoneta, Keitaro, Tago, Teruoki, Masuda, Takao
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Nakasaka, Yuta
Yoneta, Keitaro
Tago, Teruoki
Masuda, Takao
description The synthesis of metallosilicates with a MTW structure was achieved using tetraethylammonium bromide (TEABr) and methyltriethylammonium chloride (MTEACl) as organic structure-directing agents (OSDAs). MTW zeolites (Al-MTW, Si-MTW, Fe-MTW and (Al, Fe)-MTW) were obtained by hydrothermal synthesis. The crystal size of the resulting MTW zeolite strongly depended on the type of OSDA, in which the column-like and agglomerated nano-sized crystals could be produced by using MTEACl and TEABr, respectively as an OSDA. Isomorphous substitution of Fe for Si was demonstrated by UV–vis spectra and ac -NH 3 -TPD profiles. These analyses indicated that Fe atoms were incorporated into the lattice framework and that almost all of the Fe species were well-dispersed without forming bulky iron oxide particles. The ac -NH 3 -TPD profiles showed that the acid strength of the Fe-MTW zeolite was weaker than that of the Al-MTW zeolite. Al-MTW zeolites with different crystal sizes were applied to methanol-to-propylene reactions. The nano-sized Al-MTW zeolite exhibited a longer catalyst life time compared to the macro-sized Al-MTW zeolite. Since decreasing the acid strength of the MTW zeolite inhibited excessive reactions followed by the formation of aromatics, the (Al, Fe)-MTW zeolite exhibited higher yields of propylene and butenes and a lower yield of aromatics compared with the Al-MTW zeolite. Graphical Abstract
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MTW zeolites (Al-MTW, Si-MTW, Fe-MTW and (Al, Fe)-MTW) were obtained by hydrothermal synthesis. The crystal size of the resulting MTW zeolite strongly depended on the type of OSDA, in which the column-like and agglomerated nano-sized crystals could be produced by using MTEACl and TEABr, respectively as an OSDA. Isomorphous substitution of Fe for Si was demonstrated by UV–vis spectra and ac -NH 3 -TPD profiles. These analyses indicated that Fe atoms were incorporated into the lattice framework and that almost all of the Fe species were well-dispersed without forming bulky iron oxide particles. The ac -NH 3 -TPD profiles showed that the acid strength of the Fe-MTW zeolite was weaker than that of the Al-MTW zeolite. Al-MTW zeolites with different crystal sizes were applied to methanol-to-propylene reactions. The nano-sized Al-MTW zeolite exhibited a longer catalyst life time compared to the macro-sized Al-MTW zeolite. Since decreasing the acid strength of the MTW zeolite inhibited excessive reactions followed by the formation of aromatics, the (Al, Fe)-MTW zeolite exhibited higher yields of propylene and butenes and a lower yield of aromatics compared with the Al-MTW zeolite. 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MTW zeolites (Al-MTW, Si-MTW, Fe-MTW and (Al, Fe)-MTW) were obtained by hydrothermal synthesis. The crystal size of the resulting MTW zeolite strongly depended on the type of OSDA, in which the column-like and agglomerated nano-sized crystals could be produced by using MTEACl and TEABr, respectively as an OSDA. Isomorphous substitution of Fe for Si was demonstrated by UV–vis spectra and ac -NH 3 -TPD profiles. These analyses indicated that Fe atoms were incorporated into the lattice framework and that almost all of the Fe species were well-dispersed without forming bulky iron oxide particles. The ac -NH 3 -TPD profiles showed that the acid strength of the Fe-MTW zeolite was weaker than that of the Al-MTW zeolite. Al-MTW zeolites with different crystal sizes were applied to methanol-to-propylene reactions. The nano-sized Al-MTW zeolite exhibited a longer catalyst life time compared to the macro-sized Al-MTW zeolite. Since decreasing the acid strength of the MTW zeolite inhibited excessive reactions followed by the formation of aromatics, the (Al, Fe)-MTW zeolite exhibited higher yields of propylene and butenes and a lower yield of aromatics compared with the Al-MTW zeolite. Graphical Abstract</description><subject>Aluminum</subject><subject>Ammonia</subject><subject>Analysis</subject><subject>Butenes</subject><subject>Catalysis</subject><subject>Chemical synthesis</subject><subject>Chemistry</subject><subject>Chemistry and Materials Science</subject><subject>Crystals</subject><subject>Hydrothermal crystal growth</subject><subject>Industrial Chemistry/Chemical Engineering</subject><subject>Iron oxides</subject><subject>Methanol</subject><subject>Organometallic Chemistry</subject><subject>Physical Chemistry</subject><subject>Propylene</subject><subject>Silicon</subject><subject>Substitution reactions</subject><subject>Zeolites</subject><issn>1011-372X</issn><issn>1572-879X</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><sourceid>BENPR</sourceid><recordid>eNp1kU1rGzEQhpeSQvP1A3oT9JSDUkmr3dUeg2nTgEODnZLchKwd2Qqy5EhaWhfy3yOzhZJDmMMM4nlmBG9VfabkkhLSfU2UNC3DhDaYtqLG_EN1TJuOYdH1j0dlJpTiumOPn6qTlJ4IIX1H--PqZWn_Ap4Fn2NwDga03Pu8gWQTCgbdQlbOhWSd1SpDQr9t3qDb-we0zHHUeYyAlB_QTBVun61GdxBNiFvlNaAyHDZslA8O54DvYtjtHXhAC1A62-DPqo9GuQTn__pp9ev7t_vZDzz_eX0zu5pj3VKSMbAOVsJ0nAJb8YFx3TDB2l6YVpmaKD0MK6BCAdUGgPHaKCKaoW4NMy2pWX1afZn27mJ4HiFl-RTG6MtJyVgjhCC87Qp1OVFr5UBab0KOSpcaYGt18GBseb_ivG5E33BahIs3QmEy_MlrNaYkb5aLtyydWB1DShGM3EW7VXEvKZGHCOUUoSwRykOEkheHTU4qrF9D_P_t96VXVZygIA</recordid><startdate>20160301</startdate><enddate>20160301</enddate><creator>Taniguchi, Taichi</creator><creator>Nakasaka, Yuta</creator><creator>Yoneta, Keitaro</creator><creator>Tago, Teruoki</creator><creator>Masuda, Takao</creator><general>Springer US</general><general>Springer</general><general>Springer Nature B.V</general><scope>AAYXX</scope><scope>CITATION</scope><scope>ISR</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></search><sort><creationdate>20160301</creationdate><title>Size-Controlled Synthesis of Metallosilicates with MTW Structure and Catalytic Performance for Methanol-to-Propylene Reaction</title><author>Taniguchi, Taichi ; 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Since decreasing the acid strength of the MTW zeolite inhibited excessive reactions followed by the formation of aromatics, the (Al, Fe)-MTW zeolite exhibited higher yields of propylene and butenes and a lower yield of aromatics compared with the Al-MTW zeolite. Graphical Abstract</abstract><cop>New York</cop><pub>Springer US</pub><doi>10.1007/s10562-015-1683-4</doi><tpages>11</tpages></addata></record>
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subjects Aluminum
Ammonia
Analysis
Butenes
Catalysis
Chemical synthesis
Chemistry
Chemistry and Materials Science
Crystals
Hydrothermal crystal growth
Industrial Chemistry/Chemical Engineering
Iron oxides
Methanol
Organometallic Chemistry
Physical Chemistry
Propylene
Silicon
Substitution reactions
Zeolites
title Size-Controlled Synthesis of Metallosilicates with MTW Structure and Catalytic Performance for Methanol-to-Propylene Reaction
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