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An unprecedented oxalate-functionalized Ta/W polyoxometalate enabling the self-assembly of a 2D composite for catalytic hydrogenation
An oxalate-functionalized polyoxometalate Na2H38[P8W60Ta12O242(C2O4)4]·56H2O (C2O4-POM) was synthesized by the reaction of the Ta/W mixed-addenda precursor [P2W15Ta3O62]9− with oxalic acid and fully characterized using various techniques. The C2O4-POM polyanion is a tetragonal cluster composed of fo...
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Published in: | Inorganic chemistry frontiers 2024-10, Vol.11 (21), p.7324-7332 |
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creator | Li, Shujun Meng-Yao, Huang Cheng, Weiyi Waqas Ali Shah Xu-Sheng, Dai Ma, Nana Zhao, Qianyi Chen, Xuenian |
description | An oxalate-functionalized polyoxometalate Na2H38[P8W60Ta12O242(C2O4)4]·56H2O (C2O4-POM) was synthesized by the reaction of the Ta/W mixed-addenda precursor [P2W15Ta3O62]9− with oxalic acid and fully characterized using various techniques. The C2O4-POM polyanion is a tetragonal cluster composed of four Wells–Dawson {P2W15Ta3O62} fragments and four oxalate ligands (C2O42−), with each oxalate chelating a Ta atom in a bidentate fashion. The stability of C2O4-POM was studied using phosphorus nuclear magnetic resonance spectroscopy, solid-state and liquid-state infrared spectroscopy, and ultraviolet spectroscopy, which reveal that C2O4-POM can maintain its structure for at least six months over a pH range of 0.5 to 3.0. Based on the planar structure with an oxalate “antenna” and the high stability of C2O4-POM, a composite material (Pd/(C2O4-POM)@rGO) was synthesized by loading C2O4-POM and Pd particles into graphene through a one-pot photoreduction strategy. TEM measurements indicate the uniform distribution of C2O4-POM and palladium nanoparticles on the graphene. Theoretical calculations indicate that C2O4-POM may interact with graphene through covalent bonding. Pd/(C2O4-POM)@rGO showed good catalytic performance as a heterogeneous catalyst for the hydrogenation of olefin under mild conditions. The hydrogen spillover effect was found to play a crucial role in enhancing its catalytic activity. |
doi_str_mv | 10.1039/d4qi01551g |
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The C2O4-POM polyanion is a tetragonal cluster composed of four Wells–Dawson {P2W15Ta3O62} fragments and four oxalate ligands (C2O42−), with each oxalate chelating a Ta atom in a bidentate fashion. The stability of C2O4-POM was studied using phosphorus nuclear magnetic resonance spectroscopy, solid-state and liquid-state infrared spectroscopy, and ultraviolet spectroscopy, which reveal that C2O4-POM can maintain its structure for at least six months over a pH range of 0.5 to 3.0. Based on the planar structure with an oxalate “antenna” and the high stability of C2O4-POM, a composite material (Pd/(C2O4-POM)@rGO) was synthesized by loading C2O4-POM and Pd particles into graphene through a one-pot photoreduction strategy. TEM measurements indicate the uniform distribution of C2O4-POM and palladium nanoparticles on the graphene. Theoretical calculations indicate that C2O4-POM may interact with graphene through covalent bonding. Pd/(C2O4-POM)@rGO showed good catalytic performance as a heterogeneous catalyst for the hydrogenation of olefin under mild conditions. The hydrogen spillover effect was found to play a crucial role in enhancing its catalytic activity.</description><identifier>ISSN: 2052-1545</identifier><identifier>EISSN: 2052-1553</identifier><identifier>DOI: 10.1039/d4qi01551g</identifier><language>eng</language><publisher>London: Royal Society of Chemistry</publisher><subject>Catalysis ; Catalytic activity ; Chelation ; Chemical synthesis ; Composite materials ; Graphene ; Hydrogenation ; Infrared spectroscopy ; NMR spectroscopy ; Oxalic acid ; Palladium ; Planar structures ; Polyelectrolytes ; Polyoxometallates ; Self-assembly ; Spectrum analysis ; Stability</subject><ispartof>Inorganic chemistry frontiers, 2024-10, Vol.11 (21), p.7324-7332</ispartof><rights>Copyright Royal Society of Chemistry 2024</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27900,27901</link.rule.ids></links><search><creatorcontrib>Li, Shujun</creatorcontrib><creatorcontrib>Meng-Yao, Huang</creatorcontrib><creatorcontrib>Cheng, Weiyi</creatorcontrib><creatorcontrib>Waqas Ali Shah</creatorcontrib><creatorcontrib>Xu-Sheng, Dai</creatorcontrib><creatorcontrib>Ma, Nana</creatorcontrib><creatorcontrib>Zhao, Qianyi</creatorcontrib><creatorcontrib>Chen, Xuenian</creatorcontrib><title>An unprecedented oxalate-functionalized Ta/W polyoxometalate enabling the self-assembly of a 2D composite for catalytic hydrogenation</title><title>Inorganic chemistry frontiers</title><description>An oxalate-functionalized polyoxometalate Na2H38[P8W60Ta12O242(C2O4)4]·56H2O (C2O4-POM) was synthesized by the reaction of the Ta/W mixed-addenda precursor [P2W15Ta3O62]9− with oxalic acid and fully characterized using various techniques. The C2O4-POM polyanion is a tetragonal cluster composed of four Wells–Dawson {P2W15Ta3O62} fragments and four oxalate ligands (C2O42−), with each oxalate chelating a Ta atom in a bidentate fashion. The stability of C2O4-POM was studied using phosphorus nuclear magnetic resonance spectroscopy, solid-state and liquid-state infrared spectroscopy, and ultraviolet spectroscopy, which reveal that C2O4-POM can maintain its structure for at least six months over a pH range of 0.5 to 3.0. Based on the planar structure with an oxalate “antenna” and the high stability of C2O4-POM, a composite material (Pd/(C2O4-POM)@rGO) was synthesized by loading C2O4-POM and Pd particles into graphene through a one-pot photoreduction strategy. TEM measurements indicate the uniform distribution of C2O4-POM and palladium nanoparticles on the graphene. Theoretical calculations indicate that C2O4-POM may interact with graphene through covalent bonding. Pd/(C2O4-POM)@rGO showed good catalytic performance as a heterogeneous catalyst for the hydrogenation of olefin under mild conditions. The hydrogen spillover effect was found to play a crucial role in enhancing its catalytic activity.</description><subject>Catalysis</subject><subject>Catalytic activity</subject><subject>Chelation</subject><subject>Chemical synthesis</subject><subject>Composite materials</subject><subject>Graphene</subject><subject>Hydrogenation</subject><subject>Infrared spectroscopy</subject><subject>NMR spectroscopy</subject><subject>Oxalic acid</subject><subject>Palladium</subject><subject>Planar structures</subject><subject>Polyelectrolytes</subject><subject>Polyoxometallates</subject><subject>Self-assembly</subject><subject>Spectrum analysis</subject><subject>Stability</subject><issn>2052-1545</issn><issn>2052-1553</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2024</creationdate><recordtype>article</recordtype><recordid>eNo9j0trwzAQhEVpoSHNpb9A0LMbrWXZ0TGkjxQCvQR6DKtX4qJYjiVD3Hv_d90HPe3s8O0sQ8gtsHtgXM5NcaoZCAH7CzLJmcizceGX_7oQ12QWY63YaDAJrJqQz2VD-6btrLbGNskaGs7oMdnM9Y1OdWjQ1x-jvcX5G22DH8I5HG36YahtUPm62dN0sDRa7zKM0R6VH2hwFGn-QHU4tiHWI-xCRzWOl0OqNT0Mpgv7MeD7xw25cuijnf3NKdk-PW5X62zz-vyyWm4ynRcsZcDBAlNCCsml0ZwXsgJVGlEiOOa0YkZiDhVHXQAirxZcM1UutDJYipxPyd1vbNuFU29j2r2Hvhsbxh0HkGzBBOT8C5szZSc</recordid><startdate>20241022</startdate><enddate>20241022</enddate><creator>Li, Shujun</creator><creator>Meng-Yao, Huang</creator><creator>Cheng, Weiyi</creator><creator>Waqas Ali Shah</creator><creator>Xu-Sheng, Dai</creator><creator>Ma, Nana</creator><creator>Zhao, Qianyi</creator><creator>Chen, Xuenian</creator><general>Royal Society of Chemistry</general><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope></search><sort><creationdate>20241022</creationdate><title>An unprecedented oxalate-functionalized Ta/W polyoxometalate enabling the self-assembly of a 2D composite for catalytic hydrogenation</title><author>Li, Shujun ; Meng-Yao, Huang ; Cheng, Weiyi ; Waqas Ali Shah ; Xu-Sheng, Dai ; Ma, Nana ; Zhao, Qianyi ; Chen, Xuenian</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c240t-131e10b595939dc334971b6d56a1f0fcb0d9a2173ac41aa3783c0b68cbda6523</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2024</creationdate><topic>Catalysis</topic><topic>Catalytic activity</topic><topic>Chelation</topic><topic>Chemical synthesis</topic><topic>Composite materials</topic><topic>Graphene</topic><topic>Hydrogenation</topic><topic>Infrared spectroscopy</topic><topic>NMR spectroscopy</topic><topic>Oxalic acid</topic><topic>Palladium</topic><topic>Planar structures</topic><topic>Polyelectrolytes</topic><topic>Polyoxometallates</topic><topic>Self-assembly</topic><topic>Spectrum analysis</topic><topic>Stability</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Li, Shujun</creatorcontrib><creatorcontrib>Meng-Yao, Huang</creatorcontrib><creatorcontrib>Cheng, Weiyi</creatorcontrib><creatorcontrib>Waqas Ali Shah</creatorcontrib><creatorcontrib>Xu-Sheng, Dai</creatorcontrib><creatorcontrib>Ma, Nana</creatorcontrib><creatorcontrib>Zhao, Qianyi</creatorcontrib><creatorcontrib>Chen, Xuenian</creatorcontrib><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><jtitle>Inorganic chemistry frontiers</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Li, Shujun</au><au>Meng-Yao, Huang</au><au>Cheng, Weiyi</au><au>Waqas Ali Shah</au><au>Xu-Sheng, Dai</au><au>Ma, Nana</au><au>Zhao, Qianyi</au><au>Chen, Xuenian</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>An unprecedented oxalate-functionalized Ta/W polyoxometalate enabling the self-assembly of a 2D composite for catalytic hydrogenation</atitle><jtitle>Inorganic chemistry frontiers</jtitle><date>2024-10-22</date><risdate>2024</risdate><volume>11</volume><issue>21</issue><spage>7324</spage><epage>7332</epage><pages>7324-7332</pages><issn>2052-1545</issn><eissn>2052-1553</eissn><abstract>An oxalate-functionalized polyoxometalate Na2H38[P8W60Ta12O242(C2O4)4]·56H2O (C2O4-POM) was synthesized by the reaction of the Ta/W mixed-addenda precursor [P2W15Ta3O62]9− with oxalic acid and fully characterized using various techniques. The C2O4-POM polyanion is a tetragonal cluster composed of four Wells–Dawson {P2W15Ta3O62} fragments and four oxalate ligands (C2O42−), with each oxalate chelating a Ta atom in a bidentate fashion. The stability of C2O4-POM was studied using phosphorus nuclear magnetic resonance spectroscopy, solid-state and liquid-state infrared spectroscopy, and ultraviolet spectroscopy, which reveal that C2O4-POM can maintain its structure for at least six months over a pH range of 0.5 to 3.0. Based on the planar structure with an oxalate “antenna” and the high stability of C2O4-POM, a composite material (Pd/(C2O4-POM)@rGO) was synthesized by loading C2O4-POM and Pd particles into graphene through a one-pot photoreduction strategy. TEM measurements indicate the uniform distribution of C2O4-POM and palladium nanoparticles on the graphene. Theoretical calculations indicate that C2O4-POM may interact with graphene through covalent bonding. Pd/(C2O4-POM)@rGO showed good catalytic performance as a heterogeneous catalyst for the hydrogenation of olefin under mild conditions. The hydrogen spillover effect was found to play a crucial role in enhancing its catalytic activity.</abstract><cop>London</cop><pub>Royal Society of Chemistry</pub><doi>10.1039/d4qi01551g</doi><tpages>9</tpages></addata></record> |
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subjects | Catalysis Catalytic activity Chelation Chemical synthesis Composite materials Graphene Hydrogenation Infrared spectroscopy NMR spectroscopy Oxalic acid Palladium Planar structures Polyelectrolytes Polyoxometallates Self-assembly Spectrum analysis Stability |
title | An unprecedented oxalate-functionalized Ta/W polyoxometalate enabling the self-assembly of a 2D composite for catalytic hydrogenation |
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