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| Design and synthesis of hybrid solids based on the tetravanadate core toward improved catalytic properties |
| Yan-Hong Niu, Song Yang, Ji-Kun Li, Yan-Qing Xu, Chang-Wen Hu |
| Key Laboratory of Cluster Science, Ministry of Education of China, Beijing Key Laboratory of Photoelectronic/Electrophotonic, School of Chemistry, Beijing Institute of Technology, Beijing 100081, China |
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Abstract Five inorganic-organic hybrid vanadates based on tetravanadate cores, transition metals and N-donor ligands have been designed and synthesized under hydrothermal conditions, namely, [Zn(eIM)3]2V4O12(1),[Zn(pIM)3]2V4O12·H2O(2),[Zn(ipIM)3]2V4O12(3),[Co(eIM)3]2V4O12·H2O(4),[Cu(eIM)2(H2O)]2V4O12(5) (eIM=1-ethylimidazole, pIM=1-propylimidazole, ipIM=isopropylimidazole). All compounds were fully characterized by single-crystal XRD, powder XRD, elemental analysis, TGA, and FT-IR spectroscopy. The hybrid zinc vanadates (1-3) and cobalt vanadate (4) exhibit interesting 2D folded structures and the hybrid copper vanadate (5) presents a 1D chain configuration. All compounds can catalyze olefin epoxidation reactions when using TBHP (TBHP=tert-butyl hydroperoxide) as an oxidant in acetonitrile. The introduction of transition metal ions into tetravanadate cores not only improved the catalytic activity but also fulfilled the heterogeneous catalytic behavior. 1-5 all exhibit extraordinary efficiency in converting olefins to the corresponding epoxides with high conversion and selectivity (particularly, conv. up to 97.1%, sele. up to 100% for 1). Leaching test was also carried out to prove the heterogeneous behavior.
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Received: 26 October 2015
Published: 13 January 2016
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| Fund:This work was financially supported by the National Natural Science Foundation of China (Nos. 21173021, 21231002, 21271025 and 21276026), 973 Program (No. 2014CB932103), the 111 Project (No. B07012) and Beijing Higher Education Youth Elite Teacher Project (No. 1209). |
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Corresponding Authors:
Yan-Qing Xu, Chang-Wen Hu
E-mail: xyq@bit.edu.cn;cwhu@bit.edu.cn
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