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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Addition of H_2O and O_2 to Acetone and Dimethylsulfoxide Ligated Uranyl(V) Dioxocations
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Addition of H_2O and O_2 to Acetone and Dimethylsulfoxide Ligated Uranyl(V) Dioxocations

机译：将H_2O和O_2添加到丙酮和二甲基亚砜连接的Uranyl（V）二氧肟酸中

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摘要

Gas-phase complexes of the formula [UO2(lig)]+ (lig ) acetone (aco) or dimethylsulfoxide (dmso)) were generated by electrospray ionization (ESI) and studied by tandem ion-trap mass spectrometry to determine the general effect of ligand charge donation on the reactivity of UO2 + with respect to water and dioxygen.The original hypothesis that addition of O2 is enhanced by strong -donor ligands bound to UO2 + is supported by results from competitive collision-induced dissociation (CID) experiments, which show near exclusive loss of H2O from [UO2(dmso)(H2O)(O2)]+, whereas both H2O and O2 are eliminated from the corresponding [UO2(aco)(H2O)(O2)]+ species. Ligand-addition reaction rates were investigated by monitoring precursor and product ion intensities as a function of ion storage time in the ion-trap mass spectrometer: these experiments suggest that the association of dioxygen to the UO2+ complex is enhanced when the more basic dmso ligandwas coordinated to the metal complex. Conversely, addition of H2O is favored for the analogous complex ion that contains an aco ligand. Experimental rate measurements are supported by density function theory calculations of relative energies, which how stronger bonds between UO2 + and O2 when dmso is the coordinating ligand, whereas bonds to H2O are stronger for the aco complex.
机译：通过电喷雾电离（ESI）生成式[UO2（lig）] +（lig）丙酮（aco）或二甲基亚砜（dmso）的气相络合物，并通过串联离子阱质谱法研究以确定配体电荷对UO2 +与水和二氧的反应性的贡献。竞争性碰撞诱导解离（CID）实验的结果支持了最初的假说，即与UO2 +结合的强供体配体会增强O2的添加。显示[UO2（dmso）（H2O）（O2）] +中几乎没有H2O损失，而H2O和O2都从相应的[UO2（aco）（H2O）（O2）] +种中消除。通过监测离子阱质谱仪中前体离子和产物离子的强度与离子存储时间的关系，研究了配体加成反应速率：这些实验表明，当更基本的dmso配体配位时，双氧与UO2 +络合物的缔合会增强。到金属络合物。相反，对于含有aco配体的类似络合物离子，加入H2O是有利的。相对能量的密度函数理论计算支持实验速率测量，当dmso是配位配体时，UO2 +和O2之间的键有多强，而aco络合物与H2O的键更强。

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