The role and performance of isolated zirconia sites on mesoporous silica for aldol condensation of furfural with acetone

Furfural is an important bio-based platform chemical in the production of valuable products such as biofuel intermediates and polymeric materials. In this work, isolated Zr on mesoporous silica catalysts at varied Zr loading were prepared and evaluated for aldol condensation of furfural with acetone...

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Veröffentlicht in:Applied catalysis. A, General General, 2022-11, Vol.648, p.118901, Article 118901
Hauptverfasser: Balaga, Ravi, Yan, Peifang, Ramineni, Kishore, Du, Hong, Xia, Zhi, Marri, Mahender Reddy, Zhang, Zongchao Conrad
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container_title Applied catalysis. A, General
container_volume 648
creator Balaga, Ravi
Yan, Peifang
Ramineni, Kishore
Du, Hong
Xia, Zhi
Marri, Mahender Reddy
Zhang, Zongchao Conrad
description Furfural is an important bio-based platform chemical in the production of valuable products such as biofuel intermediates and polymeric materials. In this work, isolated Zr on mesoporous silica catalysts at varied Zr loading were prepared and evaluated for aldol condensation of furfural with acetone to 4-(2-furyl)− 3-buten-2-one(FAc) and 1,5-bis-(2-furanyl)− 1,4-pentadien-3-one(F2Ac). A remarkable effect of the Zr loading on the catalyst performance is revealed. The catalysts are characterized by XRD, BET, NH3-TPD, Py-FTIR, XPS, UV–visible, and TGA. The connectivity of Zr was characterized by XPS and UV–visible spectroscopy. For the 25 wt% Zr loading, Zr is present predominantly as isolated monomeric species on mesoporous SiO2. The types and densities of different acid sites of the catalysts are measured with Py-FTIR analysis. The results show that isolated Zr on mesoporous SiO2 enhanced Lewis acid site densities and exhibited superior catalytic activity for aldol condensation between furfural and acetone to produce FAc and F2Ac. [Display omitted] •Highly dispersed Zr on m-SiO2 catalyst exhibited high activityfor aldol condensation of furfural with acetone.•The rate of aldol condensation correlated with the Lewis acidic sitedensity of Zr doped on m-SiO2.•The catalyst was stable and no leaching of active sites in recycled uses.
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In this work, isolated Zr on mesoporous silica catalysts at varied Zr loading were prepared and evaluated for aldol condensation of furfural with acetone to 4-(2-furyl)− 3-buten-2-one(FAc) and 1,5-bis-(2-furanyl)− 1,4-pentadien-3-one(F2Ac). A remarkable effect of the Zr loading on the catalyst performance is revealed. The catalysts are characterized by XRD, BET, NH3-TPD, Py-FTIR, XPS, UV–visible, and TGA. The connectivity of Zr was characterized by XPS and UV–visible spectroscopy. For the 25 wt% Zr loading, Zr is present predominantly as isolated monomeric species on mesoporous SiO2. The types and densities of different acid sites of the catalysts are measured with Py-FTIR analysis. The results show that isolated Zr on mesoporous SiO2 enhanced Lewis acid site densities and exhibited superior catalytic activity for aldol condensation between furfural and acetone to produce FAc and F2Ac. [Display omitted] •Highly dispersed Zr on m-SiO2 catalyst exhibited high activityfor aldol condensation of furfural with acetone.•The rate of aldol condensation correlated with the Lewis acidic sitedensity of Zr doped on m-SiO2.•The catalyst was stable and no leaching of active sites in recycled uses.</description><identifier>ISSN: 0926-860X</identifier><identifier>EISSN: 1873-3875</identifier><identifier>DOI: 10.1016/j.apcata.2022.118901</identifier><language>eng</language><publisher>Amsterdam: Elsevier B.V</publisher><subject>Acetone ; Aldehyde and ketone condensation ; Aldehydes ; Aldol condensation ; Ammonia ; Biofuels ; Catalysts ; Catalytic activity ; Condensates ; Furfural ; Furfural and acetone ; Lewis acid ; Lewis acid site density ; Silicon dioxide ; X ray photoelectron spectroscopy ; Zirconia doped silica ; Zirconium dioxide</subject><ispartof>Applied catalysis. 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A, General</title><description>Furfural is an important bio-based platform chemical in the production of valuable products such as biofuel intermediates and polymeric materials. In this work, isolated Zr on mesoporous silica catalysts at varied Zr loading were prepared and evaluated for aldol condensation of furfural with acetone to 4-(2-furyl)− 3-buten-2-one(FAc) and 1,5-bis-(2-furanyl)− 1,4-pentadien-3-one(F2Ac). A remarkable effect of the Zr loading on the catalyst performance is revealed. The catalysts are characterized by XRD, BET, NH3-TPD, Py-FTIR, XPS, UV–visible, and TGA. The connectivity of Zr was characterized by XPS and UV–visible spectroscopy. For the 25 wt% Zr loading, Zr is present predominantly as isolated monomeric species on mesoporous SiO2. The types and densities of different acid sites of the catalysts are measured with Py-FTIR analysis. The results show that isolated Zr on mesoporous SiO2 enhanced Lewis acid site densities and exhibited superior catalytic activity for aldol condensation between furfural and acetone to produce FAc and F2Ac. [Display omitted] •Highly dispersed Zr on m-SiO2 catalyst exhibited high activityfor aldol condensation of furfural with acetone.•The rate of aldol condensation correlated with the Lewis acidic sitedensity of Zr doped on m-SiO2.•The catalyst was stable and no leaching of active sites in recycled uses.</description><subject>Acetone</subject><subject>Aldehyde and ketone condensation</subject><subject>Aldehydes</subject><subject>Aldol condensation</subject><subject>Ammonia</subject><subject>Biofuels</subject><subject>Catalysts</subject><subject>Catalytic activity</subject><subject>Condensates</subject><subject>Furfural</subject><subject>Furfural and acetone</subject><subject>Lewis acid</subject><subject>Lewis acid site density</subject><subject>Silicon dioxide</subject><subject>X ray photoelectron spectroscopy</subject><subject>Zirconia doped silica</subject><subject>Zirconium dioxide</subject><issn>0926-860X</issn><issn>1873-3875</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNp9kM1LxDAQxYMouK7-Bx4CnrsmTbtNL4IsfsGClxW8hdlkwmbpNjVJ_frrjdSzMDDweO8N8yPkkrMFZ3x5vV_AoCHBomRlueBctowfkRmXjSiEbOpjMmNtuSzkkr2ekrMY94yxsmrrGfnc7JAG3yGF3tABg_XhAL1G6i110XeQ0NBvF7TvHdDoEkbqe3rA6Acf_Biz1jkNNAcpdMZ3NFsN9hGSy8ZcY8eQBzr64dKOgsbkezwnJxa6iBd_e05e7u82q8di_fzwtLpdF1qIKhUWwVjcgkEupGW2YrVmICXWbcn11upKCgOtFlaC4G3LW25tk_W6ARCiEXNyNfUOwb-NGJPa-zH0-aQqm7piDWeyyq5qcungYwxo1RDcAcKX4kz9MlZ7NTFWv4zVxDjHbqYY5g_eHQYVtcNMz7iAOinj3f8FPz3UihM</recordid><startdate>20221125</startdate><enddate>20221125</enddate><creator>Balaga, Ravi</creator><creator>Yan, Peifang</creator><creator>Ramineni, Kishore</creator><creator>Du, Hong</creator><creator>Xia, Zhi</creator><creator>Marri, Mahender Reddy</creator><creator>Zhang, Zongchao Conrad</creator><general>Elsevier B.V</general><general>Elsevier Science SA</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope></search><sort><creationdate>20221125</creationdate><title>The role and performance of isolated zirconia sites on mesoporous silica for aldol condensation of furfural with acetone</title><author>Balaga, Ravi ; Yan, Peifang ; Ramineni, Kishore ; Du, Hong ; Xia, Zhi ; Marri, Mahender Reddy ; Zhang, Zongchao Conrad</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c334t-feadfebade138f0f405c0a88e5921cbfc483da9c3f8a3199191ff7bfc57aa3373</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Acetone</topic><topic>Aldehyde and ketone condensation</topic><topic>Aldehydes</topic><topic>Aldol condensation</topic><topic>Ammonia</topic><topic>Biofuels</topic><topic>Catalysts</topic><topic>Catalytic activity</topic><topic>Condensates</topic><topic>Furfural</topic><topic>Furfural and acetone</topic><topic>Lewis acid</topic><topic>Lewis acid site density</topic><topic>Silicon dioxide</topic><topic>X ray photoelectron spectroscopy</topic><topic>Zirconia doped silica</topic><topic>Zirconium dioxide</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Balaga, Ravi</creatorcontrib><creatorcontrib>Yan, Peifang</creatorcontrib><creatorcontrib>Ramineni, Kishore</creatorcontrib><creatorcontrib>Du, Hong</creatorcontrib><creatorcontrib>Xia, Zhi</creatorcontrib><creatorcontrib>Marri, Mahender Reddy</creatorcontrib><creatorcontrib>Zhang, Zongchao Conrad</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><jtitle>Applied catalysis. A, General</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Balaga, Ravi</au><au>Yan, Peifang</au><au>Ramineni, Kishore</au><au>Du, Hong</au><au>Xia, Zhi</au><au>Marri, Mahender Reddy</au><au>Zhang, Zongchao Conrad</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>The role and performance of isolated zirconia sites on mesoporous silica for aldol condensation of furfural with acetone</atitle><jtitle>Applied catalysis. A, General</jtitle><date>2022-11-25</date><risdate>2022</risdate><volume>648</volume><spage>118901</spage><pages>118901-</pages><artnum>118901</artnum><issn>0926-860X</issn><eissn>1873-3875</eissn><abstract>Furfural is an important bio-based platform chemical in the production of valuable products such as biofuel intermediates and polymeric materials. In this work, isolated Zr on mesoporous silica catalysts at varied Zr loading were prepared and evaluated for aldol condensation of furfural with acetone to 4-(2-furyl)− 3-buten-2-one(FAc) and 1,5-bis-(2-furanyl)− 1,4-pentadien-3-one(F2Ac). A remarkable effect of the Zr loading on the catalyst performance is revealed. The catalysts are characterized by XRD, BET, NH3-TPD, Py-FTIR, XPS, UV–visible, and TGA. The connectivity of Zr was characterized by XPS and UV–visible spectroscopy. For the 25 wt% Zr loading, Zr is present predominantly as isolated monomeric species on mesoporous SiO2. The types and densities of different acid sites of the catalysts are measured with Py-FTIR analysis. The results show that isolated Zr on mesoporous SiO2 enhanced Lewis acid site densities and exhibited superior catalytic activity for aldol condensation between furfural and acetone to produce FAc and F2Ac. [Display omitted] •Highly dispersed Zr on m-SiO2 catalyst exhibited high activityfor aldol condensation of furfural with acetone.•The rate of aldol condensation correlated with the Lewis acidic sitedensity of Zr doped on m-SiO2.•The catalyst was stable and no leaching of active sites in recycled uses.</abstract><cop>Amsterdam</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcata.2022.118901</doi></addata></record>
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subjects Acetone
Aldehyde and ketone condensation
Aldehydes
Aldol condensation
Ammonia
Biofuels
Catalysts
Catalytic activity
Condensates
Furfural
Furfural and acetone
Lewis acid
Lewis acid site density
Silicon dioxide
X ray photoelectron spectroscopy
Zirconia doped silica
Zirconium dioxide
title The role and performance of isolated zirconia sites on mesoporous silica for aldol condensation of furfural with acetone
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