Zirconium Catalyst Grafted on Ceria‐Coated Silica for Transformation of Carbon Dioxide to Diethyl Carbonate
A heterogeneous zirconium catalyst was grafted on a ceria‐coated silica support, denoted as Zr(OEt)x/CeO2/SiO2. It exhibited higher catalytic activity compared to its homogeneous counterpart, Zr(OEt)4, in the conversion of carbon dioxide to diethyl carbonate using tetraethyl orthosilicate as a regen...
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creator | Nagae, Haruki Koizumi, Hiroki Takeuchi, Katsuhiko Hamura, Satoshi Yamamoto, Toshihide Matsumoto, Kazuhiro Kamimura, Yoshihiro Kataoka, Sho Fukaya, Norihisa Choi, Jun‐Chul |
description | A heterogeneous zirconium catalyst was grafted on a ceria‐coated silica support, denoted as Zr(OEt)x/CeO2/SiO2. It exhibited higher catalytic activity compared to its homogeneous counterpart, Zr(OEt)4, in the conversion of carbon dioxide to diethyl carbonate using tetraethyl orthosilicate as a regenerable agent in the absence of any dehydrating agents under non‐protic conditions. We found that the ceria‐coated silica (CeO2/SiO2) support not only improved the catalytic activity of Zr(OEt)4 but also inhibited catalyst deactivation during catalyst recycling tests. Furthermore, we analyzed the surface of the Zr(OEt)x/CeO2/SiO2 catalysts by FE‐SEM and EDX.
The grafting of Zr(OEt)4 onto ceria‐coated silica not only enhanced the catalytic activity for the conversion of carbon dioxide to diethyl carbonate but also improved reusability. The heterogeneous Zr(OEt)x/CeO2/SiO2 catalyst demonstrated superior catalytic activity, maintaining its effectiveness even after being recycled 10 times, in comparison to the homogeneous Zr(OEt)4 catalyst. Furthermore, we investigated the surface of the catalysts and conducted kinetic studies to determine the reaction order based on the concentration of CO2. |
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The grafting of Zr(OEt)4 onto ceria‐coated silica not only enhanced the catalytic activity for the conversion of carbon dioxide to diethyl carbonate but also improved reusability. The heterogeneous Zr(OEt)x/CeO2/SiO2 catalyst demonstrated superior catalytic activity, maintaining its effectiveness even after being recycled 10 times, in comparison to the homogeneous Zr(OEt)4 catalyst. Furthermore, we investigated the surface of the catalysts and conducted kinetic studies to determine the reaction order based on the concentration of CO2.</description><identifier>ISSN: 1867-3880</identifier><identifier>EISSN: 1867-3899</identifier><identifier>DOI: 10.1002/cctc.202400673</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Carbon dioxide ; Catalysts ; Catalytic activity ; Catalytic converters ; Ceria-coated silica support ; Cerium oxides ; CO2 ; Dehydration ; Diethyl carbonate ; Heterogeneous catalyst ; Silicon dioxide ; Tetraethyl orthosilicate ; Zirconium</subject><ispartof>ChemCatChem, 2024-11, Vol.16 (21), p.n/a</ispartof><rights>2024 Wiley-VCH GmbH</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><cites>FETCH-LOGICAL-c2023-73dc6b1f38c9f421dd94152fe60c55a3bde2c66130b05197ec5fc66656b02bff3</cites><orcidid>0000-0003-1580-8822 ; 0000-0002-5589-7375 ; 0000-0001-8319-803X ; 0000-0002-7049-5032 ; 0000-0002-2720-5394 ; 0000-0003-3954-7292 ; 0000-0002-3518-5944 ; 0000-0002-0210-6488</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%2Fcctc.202400673$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fcctc.202400673$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids></links><search><creatorcontrib>Nagae, Haruki</creatorcontrib><creatorcontrib>Koizumi, Hiroki</creatorcontrib><creatorcontrib>Takeuchi, Katsuhiko</creatorcontrib><creatorcontrib>Hamura, Satoshi</creatorcontrib><creatorcontrib>Yamamoto, Toshihide</creatorcontrib><creatorcontrib>Matsumoto, Kazuhiro</creatorcontrib><creatorcontrib>Kamimura, Yoshihiro</creatorcontrib><creatorcontrib>Kataoka, Sho</creatorcontrib><creatorcontrib>Fukaya, Norihisa</creatorcontrib><creatorcontrib>Choi, Jun‐Chul</creatorcontrib><title>Zirconium Catalyst Grafted on Ceria‐Coated Silica for Transformation of Carbon Dioxide to Diethyl Carbonate</title><title>ChemCatChem</title><description>A heterogeneous zirconium catalyst was grafted on a ceria‐coated silica support, denoted as Zr(OEt)x/CeO2/SiO2. It exhibited higher catalytic activity compared to its homogeneous counterpart, Zr(OEt)4, in the conversion of carbon dioxide to diethyl carbonate using tetraethyl orthosilicate as a regenerable agent in the absence of any dehydrating agents under non‐protic conditions. We found that the ceria‐coated silica (CeO2/SiO2) support not only improved the catalytic activity of Zr(OEt)4 but also inhibited catalyst deactivation during catalyst recycling tests. Furthermore, we analyzed the surface of the Zr(OEt)x/CeO2/SiO2 catalysts by FE‐SEM and EDX.
The grafting of Zr(OEt)4 onto ceria‐coated silica not only enhanced the catalytic activity for the conversion of carbon dioxide to diethyl carbonate but also improved reusability. The heterogeneous Zr(OEt)x/CeO2/SiO2 catalyst demonstrated superior catalytic activity, maintaining its effectiveness even after being recycled 10 times, in comparison to the homogeneous Zr(OEt)4 catalyst. Furthermore, we investigated the surface of the catalysts and conducted kinetic studies to determine the reaction order based on the concentration of CO2.</description><subject>Carbon dioxide</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Catalytic converters</subject><subject>Ceria-coated silica support</subject><subject>Cerium oxides</subject><subject>CO2</subject><subject>Dehydration</subject><subject>Diethyl carbonate</subject><subject>Heterogeneous catalyst</subject><subject>Silicon dioxide</subject><subject>Tetraethyl orthosilicate</subject><subject>Zirconium</subject><issn>1867-3880</issn><issn>1867-3899</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNqFkL1OwzAUhS0EEqWwMkdiTvFP48QjMlCQKjFQFhbLcWzhKomL7Qqy8Qg8I0-Co1ZlZPLx9XfOtQ4AlwjOEIT4WqmoZhjiOYS0JEdggipa5qRi7PigK3gKzkJYJ4SRspiA7tV65Xq77TIuo2yHELOFlybqJnN9xrW38ufrmzs5Tp5ta5XMjPPZyss-JNHJaBPoTPL7Oqlb6z5to7PoktTxbWj3LynhHJwY2QZ9sT-n4OX-bsUf8uXT4pHfLHOV_k_ykjSK1siQSjEzx6hp2BwV2GgKVVFIUjcaK0oRgTUsECu1Kky604LWENfGkCm42uVuvHvf6hDF2m19n1YKgnAJCSsrlKjZjlLeheC1ERtvO-kHgaAYKxVjpeJQaTKwneHDtnr4hxacr_if9xdIB3xE</recordid><startdate>20241111</startdate><enddate>20241111</enddate><creator>Nagae, Haruki</creator><creator>Koizumi, Hiroki</creator><creator>Takeuchi, Katsuhiko</creator><creator>Hamura, Satoshi</creator><creator>Yamamoto, Toshihide</creator><creator>Matsumoto, Kazuhiro</creator><creator>Kamimura, Yoshihiro</creator><creator>Kataoka, Sho</creator><creator>Fukaya, Norihisa</creator><creator>Choi, Jun‐Chul</creator><general>Wiley Subscription Services, Inc</general><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0003-1580-8822</orcidid><orcidid>https://orcid.org/0000-0002-5589-7375</orcidid><orcidid>https://orcid.org/0000-0001-8319-803X</orcidid><orcidid>https://orcid.org/0000-0002-7049-5032</orcidid><orcidid>https://orcid.org/0000-0002-2720-5394</orcidid><orcidid>https://orcid.org/0000-0003-3954-7292</orcidid><orcidid>https://orcid.org/0000-0002-3518-5944</orcidid><orcidid>https://orcid.org/0000-0002-0210-6488</orcidid></search><sort><creationdate>20241111</creationdate><title>Zirconium Catalyst Grafted on Ceria‐Coated Silica for Transformation of Carbon Dioxide to Diethyl Carbonate</title><author>Nagae, Haruki ; Koizumi, Hiroki ; Takeuchi, Katsuhiko ; Hamura, Satoshi ; Yamamoto, Toshihide ; Matsumoto, Kazuhiro ; Kamimura, Yoshihiro ; Kataoka, Sho ; Fukaya, Norihisa ; Choi, Jun‐Chul</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c2023-73dc6b1f38c9f421dd94152fe60c55a3bde2c66130b05197ec5fc66656b02bff3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Carbon dioxide</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Catalytic converters</topic><topic>Ceria-coated silica support</topic><topic>Cerium oxides</topic><topic>CO2</topic><topic>Dehydration</topic><topic>Diethyl carbonate</topic><topic>Heterogeneous catalyst</topic><topic>Silicon dioxide</topic><topic>Tetraethyl orthosilicate</topic><topic>Zirconium</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Nagae, Haruki</creatorcontrib><creatorcontrib>Koizumi, Hiroki</creatorcontrib><creatorcontrib>Takeuchi, Katsuhiko</creatorcontrib><creatorcontrib>Hamura, Satoshi</creatorcontrib><creatorcontrib>Yamamoto, Toshihide</creatorcontrib><creatorcontrib>Matsumoto, Kazuhiro</creatorcontrib><creatorcontrib>Kamimura, Yoshihiro</creatorcontrib><creatorcontrib>Kataoka, Sho</creatorcontrib><creatorcontrib>Fukaya, Norihisa</creatorcontrib><creatorcontrib>Choi, Jun‐Chul</creatorcontrib><collection>CrossRef</collection><jtitle>ChemCatChem</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Nagae, Haruki</au><au>Koizumi, Hiroki</au><au>Takeuchi, Katsuhiko</au><au>Hamura, Satoshi</au><au>Yamamoto, Toshihide</au><au>Matsumoto, Kazuhiro</au><au>Kamimura, Yoshihiro</au><au>Kataoka, Sho</au><au>Fukaya, Norihisa</au><au>Choi, Jun‐Chul</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Zirconium Catalyst Grafted on Ceria‐Coated Silica for Transformation of Carbon Dioxide to Diethyl Carbonate</atitle><jtitle>ChemCatChem</jtitle><date>2024-11-11</date><risdate>2024</risdate><volume>16</volume><issue>21</issue><epage>n/a</epage><issn>1867-3880</issn><eissn>1867-3899</eissn><abstract>A heterogeneous zirconium catalyst was grafted on a ceria‐coated silica support, denoted as Zr(OEt)x/CeO2/SiO2. It exhibited higher catalytic activity compared to its homogeneous counterpart, Zr(OEt)4, in the conversion of carbon dioxide to diethyl carbonate using tetraethyl orthosilicate as a regenerable agent in the absence of any dehydrating agents under non‐protic conditions. We found that the ceria‐coated silica (CeO2/SiO2) support not only improved the catalytic activity of Zr(OEt)4 but also inhibited catalyst deactivation during catalyst recycling tests. Furthermore, we analyzed the surface of the Zr(OEt)x/CeO2/SiO2 catalysts by FE‐SEM and EDX.
The grafting of Zr(OEt)4 onto ceria‐coated silica not only enhanced the catalytic activity for the conversion of carbon dioxide to diethyl carbonate but also improved reusability. The heterogeneous Zr(OEt)x/CeO2/SiO2 catalyst demonstrated superior catalytic activity, maintaining its effectiveness even after being recycled 10 times, in comparison to the homogeneous Zr(OEt)4 catalyst. Furthermore, we investigated the surface of the catalysts and conducted kinetic studies to determine the reaction order based on the concentration of CO2.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/cctc.202400673</doi><tpages>6</tpages><orcidid>https://orcid.org/0000-0003-1580-8822</orcidid><orcidid>https://orcid.org/0000-0002-5589-7375</orcidid><orcidid>https://orcid.org/0000-0001-8319-803X</orcidid><orcidid>https://orcid.org/0000-0002-7049-5032</orcidid><orcidid>https://orcid.org/0000-0002-2720-5394</orcidid><orcidid>https://orcid.org/0000-0003-3954-7292</orcidid><orcidid>https://orcid.org/0000-0002-3518-5944</orcidid><orcidid>https://orcid.org/0000-0002-0210-6488</orcidid></addata></record> |
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subjects | Carbon dioxide Catalysts Catalytic activity Catalytic converters Ceria-coated silica support Cerium oxides CO2 Dehydration Diethyl carbonate Heterogeneous catalyst Silicon dioxide Tetraethyl orthosilicate Zirconium |
title | Zirconium Catalyst Grafted on Ceria‐Coated Silica for Transformation of Carbon Dioxide to Diethyl Carbonate |
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