One-Step Synthesis of Zeolite Membranes Containing Catalytic Metal Nanoclusters
Metal-loaded zeolitic membranes are promising candidates as catalytic membrane reactors. We report a one-step synthesis method to synthesize zeolite membranes containing metal nanoclusters, that has advantages in comparison to multistep methods such as impregnation and ion exchange. Pure-silica MFI...
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Veröffentlicht in: | ACS applied materials & interfaces 2016-09, Vol.8 (37), p.24671-24681 |
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creator | Kim, Seok-Jhin Tan, Shuai Taborga Claure, Micaela Briones Gil, Laura More, Karren L Liu, Yujun Moore, Jason S Dixit, Ravindra S Pendergast, John G Sholl, David S Jones, Christopher W Nair, Sankar |
description | Metal-loaded zeolitic membranes are promising candidates as catalytic membrane reactors. We report a one-step synthesis method to synthesize zeolite membranes containing metal nanoclusters, that has advantages in comparison to multistep methods such as impregnation and ion exchange. Pure-silica MFI zeolite-Pt hybrid membranes were prepared by hydrothermal synthesis with addition of 3-mercaptopropyl-trimethoxysilane (MPS) and a platinum precursor. Composition analysis and mapping by energy-dispersive X-ray spectroscopy (EDX) reveal that Pt ions/clusters are uniformly distributed along the membrane cross-section. High-magnification scanning transmission electron microscopy (STEM) analysis shows that Pt metal clusters in the hybrid zeolite membrane have a diameter distribution in the range of 0.5–2.0 nm. In contrast, a pure-silica MFI membrane synthesized from an MPS-free solution shows negligible incorporation of Pt metal clusters. To characterize the properties of the hybrid (zeolite/metal) membrane, it was used as a catalytic membrane reactor (CMR) for high-temperature propane dehydrogenation (PDH) at 600 °C and 1 atm. The results indicate that Pt metal clusters formed within the MFI zeolite membrane can serve as effective catalysts for high-temperature PDH reaction along with H2 removal via membrane permeation, thereby increasing both conversion and selectivity in relation to a conventional membrane reactor containing an equivalent amount of packed Pt catalyst in contact with an MFI membrane. The hybrid zeolite-Pt CMR also showed stable conversion and selectivity upon extended high-temperature operation (12 h), indicating that encapsulation in the zeolite allowed thermal stabilization of the Pt nanoclusters and reduced catalyst deactivation. |
doi_str_mv | 10.1021/acsami.6b06576 |
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We report a one-step synthesis method to synthesize zeolite membranes containing metal nanoclusters, that has advantages in comparison to multistep methods such as impregnation and ion exchange. Pure-silica MFI zeolite-Pt hybrid membranes were prepared by hydrothermal synthesis with addition of 3-mercaptopropyl-trimethoxysilane (MPS) and a platinum precursor. Composition analysis and mapping by energy-dispersive X-ray spectroscopy (EDX) reveal that Pt ions/clusters are uniformly distributed along the membrane cross-section. High-magnification scanning transmission electron microscopy (STEM) analysis shows that Pt metal clusters in the hybrid zeolite membrane have a diameter distribution in the range of 0.5–2.0 nm. In contrast, a pure-silica MFI membrane synthesized from an MPS-free solution shows negligible incorporation of Pt metal clusters. To characterize the properties of the hybrid (zeolite/metal) membrane, it was used as a catalytic membrane reactor (CMR) for high-temperature propane dehydrogenation (PDH) at 600 °C and 1 atm. The results indicate that Pt metal clusters formed within the MFI zeolite membrane can serve as effective catalysts for high-temperature PDH reaction along with H2 removal via membrane permeation, thereby increasing both conversion and selectivity in relation to a conventional membrane reactor containing an equivalent amount of packed Pt catalyst in contact with an MFI membrane. The hybrid zeolite-Pt CMR also showed stable conversion and selectivity upon extended high-temperature operation (12 h), indicating that encapsulation in the zeolite allowed thermal stabilization of the Pt nanoclusters and reduced catalyst deactivation.</description><identifier>ISSN: 1944-8244</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.6b06576</identifier><identifier>PMID: 27574979</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><ispartof>ACS applied materials & interfaces, 2016-09, Vol.8 (37), p.24671-24681</ispartof><rights>Copyright © 2016 American Chemical Society</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a330t-539f542c8b9400cdaec491bebe30fc89da47a7ae4b932cb8c60a863586f2c9233</citedby><cites>FETCH-LOGICAL-a330t-539f542c8b9400cdaec491bebe30fc89da47a7ae4b932cb8c60a863586f2c9233</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acsami.6b06576$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acsami.6b06576$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>314,776,780,2752,27053,27901,27902,56713,56763</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/27574979$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Kim, Seok-Jhin</creatorcontrib><creatorcontrib>Tan, Shuai</creatorcontrib><creatorcontrib>Taborga Claure, Micaela</creatorcontrib><creatorcontrib>Briones Gil, Laura</creatorcontrib><creatorcontrib>More, Karren L</creatorcontrib><creatorcontrib>Liu, Yujun</creatorcontrib><creatorcontrib>Moore, Jason S</creatorcontrib><creatorcontrib>Dixit, Ravindra S</creatorcontrib><creatorcontrib>Pendergast, John G</creatorcontrib><creatorcontrib>Sholl, David S</creatorcontrib><creatorcontrib>Jones, Christopher W</creatorcontrib><creatorcontrib>Nair, Sankar</creatorcontrib><title>One-Step Synthesis of Zeolite Membranes Containing Catalytic Metal Nanoclusters</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl. Mater. Interfaces</addtitle><description>Metal-loaded zeolitic membranes are promising candidates as catalytic membrane reactors. We report a one-step synthesis method to synthesize zeolite membranes containing metal nanoclusters, that has advantages in comparison to multistep methods such as impregnation and ion exchange. Pure-silica MFI zeolite-Pt hybrid membranes were prepared by hydrothermal synthesis with addition of 3-mercaptopropyl-trimethoxysilane (MPS) and a platinum precursor. Composition analysis and mapping by energy-dispersive X-ray spectroscopy (EDX) reveal that Pt ions/clusters are uniformly distributed along the membrane cross-section. High-magnification scanning transmission electron microscopy (STEM) analysis shows that Pt metal clusters in the hybrid zeolite membrane have a diameter distribution in the range of 0.5–2.0 nm. In contrast, a pure-silica MFI membrane synthesized from an MPS-free solution shows negligible incorporation of Pt metal clusters. To characterize the properties of the hybrid (zeolite/metal) membrane, it was used as a catalytic membrane reactor (CMR) for high-temperature propane dehydrogenation (PDH) at 600 °C and 1 atm. The results indicate that Pt metal clusters formed within the MFI zeolite membrane can serve as effective catalysts for high-temperature PDH reaction along with H2 removal via membrane permeation, thereby increasing both conversion and selectivity in relation to a conventional membrane reactor containing an equivalent amount of packed Pt catalyst in contact with an MFI membrane. The hybrid zeolite-Pt CMR also showed stable conversion and selectivity upon extended high-temperature operation (12 h), indicating that encapsulation in the zeolite allowed thermal stabilization of the Pt nanoclusters and reduced catalyst deactivation.</description><issn>1944-8244</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNp1kL1PwzAQxS0EoqWwMqKMCCnFsR3HHlHEl1ToUFhYLNu9QKp8FNsZ-t9jlNKN6Z50v_d09xC6zPA8wyS71dbrtp5zg3le8CM0zSRjqSA5OT5oxibozPsNxpwSnJ-iCSnygslCTtFy2UG6CrBNVrsufIGvfdJXyQf0TR0geYHWON2BT8q-C7ru6u4zKXXQzS7UNq6jSl5119tm8AGcP0cnlW48XOznDL0_3L-VT-li-fhc3i1STSkOaU5llTNihZEMY7vWYJnMDBiguLJCrjUrdKGBGUmJNcJyrAWnueAVsZJQOkPXY-7W9d8D-KDa2ltomnhsP3iVCUIYl5KLiM5H1LreeweV2rq61W6nMqx-S1RjiWpfYjRc7bMH08L6gP-1FoGbEYhGtekH18VX_0v7AYfwfO4</recordid><startdate>20160921</startdate><enddate>20160921</enddate><creator>Kim, Seok-Jhin</creator><creator>Tan, Shuai</creator><creator>Taborga Claure, Micaela</creator><creator>Briones Gil, Laura</creator><creator>More, Karren L</creator><creator>Liu, Yujun</creator><creator>Moore, Jason S</creator><creator>Dixit, Ravindra S</creator><creator>Pendergast, John G</creator><creator>Sholl, David S</creator><creator>Jones, Christopher W</creator><creator>Nair, Sankar</creator><general>American Chemical Society</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope></search><sort><creationdate>20160921</creationdate><title>One-Step Synthesis of Zeolite Membranes Containing Catalytic Metal Nanoclusters</title><author>Kim, Seok-Jhin ; Tan, Shuai ; Taborga Claure, Micaela ; Briones Gil, Laura ; More, Karren L ; Liu, Yujun ; Moore, Jason S ; Dixit, Ravindra S ; Pendergast, John G ; Sholl, David S ; Jones, Christopher W ; Nair, Sankar</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a330t-539f542c8b9400cdaec491bebe30fc89da47a7ae4b932cb8c60a863586f2c9233</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2016</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Kim, Seok-Jhin</creatorcontrib><creatorcontrib>Tan, Shuai</creatorcontrib><creatorcontrib>Taborga Claure, Micaela</creatorcontrib><creatorcontrib>Briones Gil, Laura</creatorcontrib><creatorcontrib>More, Karren L</creatorcontrib><creatorcontrib>Liu, Yujun</creatorcontrib><creatorcontrib>Moore, Jason S</creatorcontrib><creatorcontrib>Dixit, Ravindra S</creatorcontrib><creatorcontrib>Pendergast, John G</creatorcontrib><creatorcontrib>Sholl, David S</creatorcontrib><creatorcontrib>Jones, Christopher W</creatorcontrib><creatorcontrib>Nair, Sankar</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><jtitle>ACS applied materials & interfaces</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Kim, Seok-Jhin</au><au>Tan, Shuai</au><au>Taborga Claure, Micaela</au><au>Briones Gil, Laura</au><au>More, Karren L</au><au>Liu, Yujun</au><au>Moore, Jason S</au><au>Dixit, Ravindra S</au><au>Pendergast, John G</au><au>Sholl, David S</au><au>Jones, Christopher W</au><au>Nair, Sankar</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>One-Step Synthesis of Zeolite Membranes Containing Catalytic Metal Nanoclusters</atitle><jtitle>ACS applied materials & interfaces</jtitle><addtitle>ACS Appl. Mater. Interfaces</addtitle><date>2016-09-21</date><risdate>2016</risdate><volume>8</volume><issue>37</issue><spage>24671</spage><epage>24681</epage><pages>24671-24681</pages><issn>1944-8244</issn><eissn>1944-8252</eissn><abstract>Metal-loaded zeolitic membranes are promising candidates as catalytic membrane reactors. We report a one-step synthesis method to synthesize zeolite membranes containing metal nanoclusters, that has advantages in comparison to multistep methods such as impregnation and ion exchange. Pure-silica MFI zeolite-Pt hybrid membranes were prepared by hydrothermal synthesis with addition of 3-mercaptopropyl-trimethoxysilane (MPS) and a platinum precursor. Composition analysis and mapping by energy-dispersive X-ray spectroscopy (EDX) reveal that Pt ions/clusters are uniformly distributed along the membrane cross-section. High-magnification scanning transmission electron microscopy (STEM) analysis shows that Pt metal clusters in the hybrid zeolite membrane have a diameter distribution in the range of 0.5–2.0 nm. In contrast, a pure-silica MFI membrane synthesized from an MPS-free solution shows negligible incorporation of Pt metal clusters. To characterize the properties of the hybrid (zeolite/metal) membrane, it was used as a catalytic membrane reactor (CMR) for high-temperature propane dehydrogenation (PDH) at 600 °C and 1 atm. The results indicate that Pt metal clusters formed within the MFI zeolite membrane can serve as effective catalysts for high-temperature PDH reaction along with H2 removal via membrane permeation, thereby increasing both conversion and selectivity in relation to a conventional membrane reactor containing an equivalent amount of packed Pt catalyst in contact with an MFI membrane. The hybrid zeolite-Pt CMR also showed stable conversion and selectivity upon extended high-temperature operation (12 h), indicating that encapsulation in the zeolite allowed thermal stabilization of the Pt nanoclusters and reduced catalyst deactivation.</abstract><cop>United States</cop><pub>American Chemical Society</pub><pmid>27574979</pmid><doi>10.1021/acsami.6b06576</doi><tpages>11</tpages></addata></record> |
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title | One-Step Synthesis of Zeolite Membranes Containing Catalytic Metal Nanoclusters |
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