Three new derivatives of hexavanadate with remote methacryl,phthalyl and tetrahydrophthalyl groups,respectively,were synthesized by esterification of pentaerythritol-derivatized hexavanadate.These new compounds were c...Three new derivatives of hexavanadate with remote methacryl,phthalyl and tetrahydrophthalyl groups,respectively,were synthesized by esterification of pentaerythritol-derivatized hexavanadate.These new compounds were characterized by FT-IR,^(1)H NMR,UV-vis,elemental analysis and single-crystal X-ray diffraction.Their thermal stabilities were also tested by TGA analyses.Through such syntheses,we have successfully introduced the carbon-carbon double bond and/or carboxylic groups into the polyoxovanadates which could be utilized to build more complex structures.We also discuss the influence of anhydrides with different functional groups on the esterification of the pentaerythritol derivatized hexavanadate.展开更多
Chemical fixation of CO_(2)into C1 source, as a general approach, can effectively alleviate the emission of greenhouse gasses. Whereas, the challenge posed by the need for efficient catalysts with high catalytic activ...Chemical fixation of CO_(2)into C1 source, as a general approach, can effectively alleviate the emission of greenhouse gasses. Whereas, the challenge posed by the need for efficient catalysts with high catalytic active sites still exists. In this work, we reported a series of new hexavanadate clusters, [(C6H6ON)2(C2H8N2)2(CH3O)6VIV6O8](V6–1), [(C6H6ON)2(C3H10N2)2(CH3O)6VIV6O8](V6–2), [(C6H6ON)2(C6H14N2)2(CH3O)6VIV6O8](V6–3) and [(C6H6ON)2(C4H11N2O)2(CH3O)4VIV6O8](V6–4), assembled by 2-aminophenol and four different kinds of Lewis bases(LB), ethanediamine(en), 1,2-diaminopropane, 1,2-cyclohexanediamine and N-(2-hydroxyethyl)ethylenediamine(ben) together. Among them, the basic unit {V6} cluster featured Z-shaped configuration represents a brand-new example of hexanuclear vanadium clusters. Remarkably, the catalytic tests demonstrated that V6–1 as catalyst displays high catalytic activity in the cycloaddition for the CO_(2)fixation into cyclic carbonates by virtue of open V sites. As expected, for oxidative desulfurization of sulfides, V6–1 also exhibits satisfied catalytic effectiveness. Furthermore, the recycling test confirmed that catalyst V6–1 may be a bifunctional heterogeneous catalyst with great promise for both CO_(2)cycloaddition and oxidative desulfurization reactions.展开更多
基金supported by the National Natural Science Foundation of China(no.21271068,21401050 and 21471087)the Natural Science Foundation of Hubei Province(no.2015CFA131)the Wuhan Applied Basic Research Program(no.2014010101010020).
文摘Three new derivatives of hexavanadate with remote methacryl,phthalyl and tetrahydrophthalyl groups,respectively,were synthesized by esterification of pentaerythritol-derivatized hexavanadate.These new compounds were characterized by FT-IR,^(1)H NMR,UV-vis,elemental analysis and single-crystal X-ray diffraction.Their thermal stabilities were also tested by TGA analyses.Through such syntheses,we have successfully introduced the carbon-carbon double bond and/or carboxylic groups into the polyoxovanadates which could be utilized to build more complex structures.We also discuss the influence of anhydrides with different functional groups on the esterification of the pentaerythritol derivatized hexavanadate.
基金supported by Natural Science Foundation of Jiangsu (No. BK20191359)the Natural Science Foundation of China (No. 21571103)the Postgraduate Research & Practice Innovation Program of Jiangsu Province (No. KYCX22_1343)。
文摘Chemical fixation of CO_(2)into C1 source, as a general approach, can effectively alleviate the emission of greenhouse gasses. Whereas, the challenge posed by the need for efficient catalysts with high catalytic active sites still exists. In this work, we reported a series of new hexavanadate clusters, [(C6H6ON)2(C2H8N2)2(CH3O)6VIV6O8](V6–1), [(C6H6ON)2(C3H10N2)2(CH3O)6VIV6O8](V6–2), [(C6H6ON)2(C6H14N2)2(CH3O)6VIV6O8](V6–3) and [(C6H6ON)2(C4H11N2O)2(CH3O)4VIV6O8](V6–4), assembled by 2-aminophenol and four different kinds of Lewis bases(LB), ethanediamine(en), 1,2-diaminopropane, 1,2-cyclohexanediamine and N-(2-hydroxyethyl)ethylenediamine(ben) together. Among them, the basic unit {V6} cluster featured Z-shaped configuration represents a brand-new example of hexanuclear vanadium clusters. Remarkably, the catalytic tests demonstrated that V6–1 as catalyst displays high catalytic activity in the cycloaddition for the CO_(2)fixation into cyclic carbonates by virtue of open V sites. As expected, for oxidative desulfurization of sulfides, V6–1 also exhibits satisfied catalytic effectiveness. Furthermore, the recycling test confirmed that catalyst V6–1 may be a bifunctional heterogeneous catalyst with great promise for both CO_(2)cycloaddition and oxidative desulfurization reactions.
