Molybdenum(VI) network polymers based on anion–π interaction and hydrogen bonding: Synthesis, crystal structures and oxidation catalytic application |
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Authors: | Jia Li Ge Wang Zhan Shi Mu Yang Rudy L Luck |
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Institution: | aSchool of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, PR China;bState Key Laboratory of Inorganic Synthesis & Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, PR China;cDepartment of Chemistry, Michigan Technological University, Houghton, MI 49931, USA |
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Abstract: | A crystallographic investigation of anion–π interactions and hydrogen bonds on the preferred structural motifs of molybdenum(VI) complexes has been carried out. Two molybdenum(VI) network polymers MoO2F4·(Hinca)2 (1) and MoO2F3(H2O)·(Hinpa) (2), where inca = isonicotinamide and inpa = isonipecotamide, have been synthesized, crystallographically characterized and successfully applied to alcohol oxidation reaction. Complex 1 crystallizes in the monoclinic space C2/c: a = 16.832(3) Å, b = 8.8189(15) Å, c = 12.568(2) Å, β = 118.929(3)°, V = 1560.1(5) Å3, Z = 4. Complex 2 crystallizes in the triclinic space P-1: a = 5.459(2) Å, b = 9.189(4) Å, c = 12.204(5) Å, α = 71.341(6)°, β = 81.712(7)°, γ = 77.705(7)°, V = 564.8(4) Å3, Z = 2. Complex 1 consists of hydrogen bonding and anion–π interactions, both of which are considered as important factors for controlling the geometric features and packing characteristics of the crystal structure. The geometry of the sandwich complex of MoO2F4]2− with two pyridine rings indicates that the anion–π interaction is an additive and provides a base for the design and synthesis of new complexes. For complex 2, the anions and the protonated inpa ligands form a 2D supramolecular network by four different types of hydrogen contacts (N–HF, N–HO, O–HF and O–HO). The catalytic ability of complexes 1 and 2 has also been evaluated by applying them to the oxidation of benzyl alcohol with TBHP as oxidant. |
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Keywords: | Hydrogen bonds Anion– π interaction X-ray structures Molybdenum |
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