Department of Chemistry, Uppsala Biocenter, Swedish University of Agricultural Sciences, P.O. Box 7015, SE-75007 Uppsala, Sweden.
Inorg Chem. 2012 Sep 17;51(18):9598-609. doi: 10.1021/ic300202f. Epub 2012 Sep 5.
The coordination chemistry of hydrated and solvated vanadium(III), oxovanadium(IV), and dioxovanadium(V) ions in the oxygen-donor solvents water, dimethyl sulfoxide (DMSO), and N,N'-dimethylpropyleneurea (DMPU) has been studied in solution by extended X-ray absorption fine structure (EXAFS) and large-angle X-ray scattering (LAXS) and in the solid state by single-crystal X-ray diffraction and EXAFS. The hydrated vanadium(III) ion has a regular octahedral configuration with a mean V-O bond distance of 1.99 Å. In the hydrated and DMSO-solvated oxovanadium(IV) ions, vanadium binds strongly to an oxo group at ca. 1.6 Å. The solvent molecule trans to the oxo group is very weakly bound, at ca. 2.2 Å, while the remaining four solvent molecules, with a mean V-O bond distance of 2.0 Å, form a plane slightly below the vanadium atom; the mean O═V-O(perp) bond angle is ca. 98°. In the DMPU-solvated oxovanadium(IV) ion, the space-demanding properties of the DMPU molecule leave no solvent molecule in the trans position to the oxo group, which reduces the coordination number to 5. The O═V-O bond angle is consequently much larger, 107°, and the mean V═O and V-O bond distances decrease to 1.58 and 1.97 Å, respectively. The hydrated and DMSO-solvated dioxovanadium(V) ions display a very distorted octahedral configuration with the oxo groups in the cis position with a mean V═O bond distance of 1.6 Å and a O═V═O bond angle of ca. 105°. The solvent molecules trans to the oxo groups are weakly bound, at ca. 2.2 Å, while the remaining two have bond distances of 2.02 Å. The experimental studies of the coordination chemistry of hydrated and solvated vanadium(III,IV,V) ions are complemented by summarizing previously reported crystal structures to yield a comprehensive description of the coordination chemistry of vanadium with oxygen-donor ligands.
水、二甲基亚砜 (DMSO) 和 N,N'-二甲基丙烯脲 (DMPU) 等含氧溶剂中,水合和溶剂化的钒(III)、氧钒(IV)和二氧钒(V)离子的配位化学通过扩展 X 射线吸收精细结构 (EXAFS) 和大角度 X 射线散射 (LAXS) 在溶液中以及通过单晶 X 射线衍射和 EXAFS 在固态中进行了研究。水合钒(III)离子具有规则的八面体构型,平均 V-O 键距离为 1.99 Å。在水合和 DMSO 溶剂化的氧钒(IV)离子中,钒与氧原子强烈结合,距离约为 1.6 Å。与氧原子处于反式位置的溶剂分子结合非常弱,距离约为 2.2 Å,而其余四个溶剂分子与钒原子形成一个平面,距离约为 2.0 Å,平均 V-O 键距离为 2.0 Å;平均 O=V-O(perp)键角约为 98°。在 DMPU 溶剂化的氧钒(IV)离子中,DMPU 分子的空间需求特性使得在氧原子的反式位置没有溶剂分子,从而将配位数降低至 5。因此,O=V-O 键角大得多,为 107°,平均 V=O 和 V-O 键距离分别减小至 1.58 和 1.97 Å。水合和 DMSO 溶剂化的二氧钒(V)离子呈现非常扭曲的八面体构型,氧原子处于顺式位置,平均 V=O 键距离为 1.6 Å,O=V=O 键角约为 105°。与氧原子处于反式位置的溶剂分子结合较弱,距离约为 2.2 Å,而其余两个具有 2.02 Å 的键距离。对水合和溶剂化的钒(III、IV、V)离子配位化学的实验研究通过总结以前报道的晶体结构进行了补充,从而全面描述了钒与含氧配体的配位化学。