Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO
[Display omitted] •Chalcone production over MgO sensitive to surface Lewis basicity (from CO2-TPD).•MgO Lewis basicity tuned by changes in synthesis method/calcination temperature.•Direct correlation of surface area with Lewis basicity for MgO catalysts proved.•Increase in Lewis basicity of MgO via...
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creator | Pischetola, Chiara Hesse, Fabian Bos, Jan-Willem G. Cárdenas-Lizana, Fernando |
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•Chalcone production over MgO sensitive to surface Lewis basicity (from CO2-TPD).•MgO Lewis basicity tuned by changes in synthesis method/calcination temperature.•Direct correlation of surface area with Lewis basicity for MgO catalysts proved.•Increase in Lewis basicity of MgO via Li+- and Cs+-incorporation by impregnation.•Efficient gas phase continuous chalcone production over novel Cs-MgO catalyst.
We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4−20 nm) and specific surface area (SSA = 58−246 m2 g−1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2− sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity. |
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•Chalcone production over MgO sensitive to surface Lewis basicity (from CO2-TPD).•MgO Lewis basicity tuned by changes in synthesis method/calcination temperature.•Direct correlation of surface area with Lewis basicity for MgO catalysts proved.•Increase in Lewis basicity of MgO via Li+- and Cs+-incorporation by impregnation.•Efficient gas phase continuous chalcone production over novel Cs-MgO catalyst.
We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4−20 nm) and specific surface area (SSA = 58−246 m2 g−1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2− sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.</description><identifier>ISSN: 0926-860X</identifier><identifier>EISSN: 1873-3875</identifier><identifier>DOI: 10.1016/j.apcata.2021.118277</identifier><language>eng</language><publisher>AMSTERDAM: Elsevier B.V</publisher><subject>Acetophenone ; Ammonia ; Basicity ; Benzaldehyde ; Benzaldehyde and acetophenone ; Benzylideneacetophenone ; Catalysts ; Chemical synthesis ; Chemistry ; Chemistry, Physical ; Condensates ; Crystal structure ; Environmental Sciences ; Environmental Sciences & Ecology ; Li- and Cs-promotion ; Life Sciences & Biomedicine ; Magnesium oxide ; MgO ; Physical Sciences ; Science & Technology ; Selective gas phase condensation ; Surface basicity ; Vapor phases</subject><ispartof>Applied catalysis. A, General, 2021-08, Vol.623, p.118277, Article 118277</ispartof><rights>2021 Elsevier B.V.</rights><rights>Copyright Elsevier Science SA Aug 5, 2021</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>true</woscitedreferencessubscribed><woscitedreferencescount>8</woscitedreferencescount><woscitedreferencesoriginalsourcerecordid>wos000694673700005</woscitedreferencesoriginalsourcerecordid><citedby>FETCH-LOGICAL-c264t-58b1467d5c209baea4a0ae58d67ac43a32dbf5544c4d64387c89004a4264d8ea3</citedby><cites>FETCH-LOGICAL-c264t-58b1467d5c209baea4a0ae58d67ac43a32dbf5544c4d64387c89004a4264d8ea3</cites><orcidid>0000-0003-3947-2024 ; 0000-0003-0008-0699 ; 0000-0003-4275-2529</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://dx.doi.org/10.1016/j.apcata.2021.118277$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>315,781,785,3551,27929,27930,39263,46000</link.rule.ids></links><search><creatorcontrib>Pischetola, Chiara</creatorcontrib><creatorcontrib>Hesse, Fabian</creatorcontrib><creatorcontrib>Bos, Jan-Willem G.</creatorcontrib><creatorcontrib>Cárdenas-Lizana, Fernando</creatorcontrib><title>Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO</title><title>Applied catalysis. A, General</title><addtitle>APPL CATAL A-GEN</addtitle><description>[Display omitted]
•Chalcone production over MgO sensitive to surface Lewis basicity (from CO2-TPD).•MgO Lewis basicity tuned by changes in synthesis method/calcination temperature.•Direct correlation of surface area with Lewis basicity for MgO catalysts proved.•Increase in Lewis basicity of MgO via Li+- and Cs+-incorporation by impregnation.•Efficient gas phase continuous chalcone production over novel Cs-MgO catalyst.
We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4−20 nm) and specific surface area (SSA = 58−246 m2 g−1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2− sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.</description><subject>Acetophenone</subject><subject>Ammonia</subject><subject>Basicity</subject><subject>Benzaldehyde</subject><subject>Benzaldehyde and acetophenone</subject><subject>Benzylideneacetophenone</subject><subject>Catalysts</subject><subject>Chemical synthesis</subject><subject>Chemistry</subject><subject>Chemistry, Physical</subject><subject>Condensates</subject><subject>Crystal structure</subject><subject>Environmental Sciences</subject><subject>Environmental Sciences & Ecology</subject><subject>Li- and Cs-promotion</subject><subject>Life Sciences & Biomedicine</subject><subject>Magnesium oxide</subject><subject>MgO</subject><subject>Physical Sciences</subject><subject>Science & Technology</subject><subject>Selective gas phase condensation</subject><subject>Surface basicity</subject><subject>Vapor phases</subject><issn>0926-860X</issn><issn>1873-3875</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2021</creationdate><recordtype>article</recordtype><sourceid>HGBXW</sourceid><recordid>eNqNkU1r3DAQhkVpodsk_6AHQY_FW8mWZPlSKEv6AVtySSE3MZbGsZat5Fpylu2vrxKHHktPGsT7SDPPEPKWsy1nXH04bGGykGFbs5pvOdd1274gG67bpmp0K1-SDetqVWnF7l6TNykdGGO16OSGHK-HAW2mcaB7PPlEe0je-nymMdA8IrUxZB-WuCR6D4lOI6SnS4chQfYlVdAew284OhzPDunJ55GCxRynEUMMSOMDzvT7_c0leTXAMeHV83lBfny-vt19rfY3X77tPu0rWyuRK6l7LlTrpK1Z1wOCAAYotVMtWNFAU7t-kFIIK5wSZUCrO8YEiEI7jdBckHfru9Mcfy2YsjnEZQ7lS1PLtpFcqU6XlFhTdo4pzTiYafY_YT4bzsyjV3Mwq1fz6NWsXgv2fsVO2MchWY_B4l-0iFVdab5pS8VkSev_T-98flK6i0vIBf24olhUPXiczTPu_FxWZlz0_-70D8qJpIg</recordid><startdate>20210805</startdate><enddate>20210805</enddate><creator>Pischetola, Chiara</creator><creator>Hesse, Fabian</creator><creator>Bos, Jan-Willem G.</creator><creator>Cárdenas-Lizana, Fernando</creator><general>Elsevier B.V</general><general>Elsevier</general><general>Elsevier Science SA</general><scope>BLEPL</scope><scope>DTL</scope><scope>HGBXW</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><orcidid>https://orcid.org/0000-0003-3947-2024</orcidid><orcidid>https://orcid.org/0000-0003-0008-0699</orcidid><orcidid>https://orcid.org/0000-0003-4275-2529</orcidid></search><sort><creationdate>20210805</creationdate><title>Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO</title><author>Pischetola, Chiara ; Hesse, Fabian ; Bos, Jan-Willem G. ; Cárdenas-Lizana, Fernando</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c264t-58b1467d5c209baea4a0ae58d67ac43a32dbf5544c4d64387c89004a4264d8ea3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2021</creationdate><topic>Acetophenone</topic><topic>Ammonia</topic><topic>Basicity</topic><topic>Benzaldehyde</topic><topic>Benzaldehyde and acetophenone</topic><topic>Benzylideneacetophenone</topic><topic>Catalysts</topic><topic>Chemical synthesis</topic><topic>Chemistry</topic><topic>Chemistry, Physical</topic><topic>Condensates</topic><topic>Crystal structure</topic><topic>Environmental Sciences</topic><topic>Environmental Sciences & Ecology</topic><topic>Li- and Cs-promotion</topic><topic>Life Sciences & Biomedicine</topic><topic>Magnesium oxide</topic><topic>MgO</topic><topic>Physical Sciences</topic><topic>Science & Technology</topic><topic>Selective gas phase condensation</topic><topic>Surface basicity</topic><topic>Vapor phases</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Pischetola, Chiara</creatorcontrib><creatorcontrib>Hesse, Fabian</creatorcontrib><creatorcontrib>Bos, Jan-Willem G.</creatorcontrib><creatorcontrib>Cárdenas-Lizana, Fernando</creatorcontrib><collection>Web of Science Core Collection</collection><collection>Science Citation Index Expanded</collection><collection>Web of Science - Science Citation Index Expanded - 2021</collection><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>Pischetola, Chiara</au><au>Hesse, Fabian</au><au>Bos, Jan-Willem G.</au><au>Cárdenas-Lizana, Fernando</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO</atitle><jtitle>Applied catalysis. A, General</jtitle><stitle>APPL CATAL A-GEN</stitle><date>2021-08-05</date><risdate>2021</risdate><volume>623</volume><spage>118277</spage><pages>118277-</pages><artnum>118277</artnum><issn>0926-860X</issn><eissn>1873-3875</eissn><abstract>[Display omitted]
•Chalcone production over MgO sensitive to surface Lewis basicity (from CO2-TPD).•MgO Lewis basicity tuned by changes in synthesis method/calcination temperature.•Direct correlation of surface area with Lewis basicity for MgO catalysts proved.•Increase in Lewis basicity of MgO via Li+- and Cs+-incorporation by impregnation.•Efficient gas phase continuous chalcone production over novel Cs-MgO catalyst.
We have investigated the effect of Lewis basicity in the continuous gas phase condensation of acetophenone + benzaldehyde over MgO. The catalysts were prepared by ammonia precipitation, hydration and calcination to generate MgO with modified Lewis basicity (from CO2-TPD), dXRD (4−20 nm) and specific surface area (SSA = 58−246 m2 g−1); a direct correlation between SSA and Lewis basicity is presented. The introduction of Li+ and Cs+ served to decrease SSA and increase dXRD and Lewis basicity, linked to diffusion of the cations within the crystal structure (confirmed by XRD/STEM-EDX). All MgO systems delivered the exclusive and time invariant formation of target benzylideneacetophenone. Benzylideneacetophenone production rate is sensitive to the specific (per m2) Lewis basicity. The Cs10MgO_H(773) catalyst delivered the highest rate, attributed to high density of (Lewis basic) -O2− sites involved in the rate-determining step. Our results establish the feasibility of continuous chalcone synthesis using MgO catalysts with controlled Lewis basicity.</abstract><cop>AMSTERDAM</cop><pub>Elsevier B.V</pub><doi>10.1016/j.apcata.2021.118277</doi><tpages>11</tpages><orcidid>https://orcid.org/0000-0003-3947-2024</orcidid><orcidid>https://orcid.org/0000-0003-0008-0699</orcidid><orcidid>https://orcid.org/0000-0003-4275-2529</orcidid></addata></record> |
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subjects | Acetophenone Ammonia Basicity Benzaldehyde Benzaldehyde and acetophenone Benzylideneacetophenone Catalysts Chemical synthesis Chemistry Chemistry, Physical Condensates Crystal structure Environmental Sciences Environmental Sciences & Ecology Li- and Cs-promotion Life Sciences & Biomedicine Magnesium oxide MgO Physical Sciences Science & Technology Selective gas phase condensation Surface basicity Vapor phases |
title | Effect of Lewis basicity on the continuous gas phase condensation of benzaldehyde with acetophenone over MgO |
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