Heterometallic Polyhydride Compounds: Synthesis and Reactivity (Chemistry)

氢化，即将氢加到其他原子或分子上，是一个极其重要的化学过程。例如，在将玉米油转化为人造黄油和利用煤进行化学合成方面，氢化作用是涉及的，毫无疑问，它也将参与未来太阳能利用的实际计划。本课题的研究重点是金属-氢化合物的合成，它可以使其他化合物加氢或催化加氢反应。该项目涉及合成和研究氢转移到CO、二氧化碳和烯烃等可还原底物上的优化化合物的反应性。这种化合物包含两种不同的金属，或者两种过渡金属或一种过渡金属和一种高电性金属(锌，Y，Sm……)，以及许多氢化物配体。三种不同类型的合成程序将用于这些异金属氢化物。在初步工作中，观察到了一种异质双金属聚氢化物对二氧化碳的还原。由于可以从动力学和热力学的角度论证未成对的电子密度应该促进这种氢化反应，因此具有未成对电子的单体金属多氢化物也将被合成。单体和异双金属多氢化合物都将根据它们的动态过程(例如，通过EPR光谱)和它们的化学反应活性来表征。

Hydrogenation, the addition of hydrogen to other atoms or molecules, is an extremely important chemical process. For example, hydrogenation is involved in the conversion of corn oil to margarine and in the utilization of coal for chemical synthesis, and will undoubtedly be involved also in future practical schemes for the utilization of solar energy. The focus of this research project is the synthesis of metal-hydrogen compounds of metals which can hydrogenate other compounds or catalyze hydrogenation reactions. This project involves the synthesis and investigation of the reactivity of compounds optimized for hydrogen transfer to reducible substrates such as CO, carbon dioxide and olefins. Such compounds contain two different metals, either two transition metals or a transition metal and a highly electropositive metal (Zn, Y, Sm ....), as well as numerous hydride ligands. Three different classes of synthetic procedures will be used for these heterometallic hydrides. In preliminary work the reduction of carbon dioxide by one heterobimetallic polyhydride has been observed. Since it can be argued that unpaired electron density should promote such hydrogenations from both a kinetic and a thermodynamic point of view, monomeric metallic polyhydrides with unpaired electrons will also be synthesized. Both monomeric and heterobimetallic polyhydrides will be characterized in terms of their dynamic processes ( e.g. by EPR spectroscopy ) and their chemical reactivity.