Mechanism and applications of homogeneous catalysis in main group chemistry

在有机分子和材料的生产中，催化在大宗和精细化学品工业中的重要性怎么强调都不为过。尽管我们通常认为催化剂只是简单地加速了缓慢的反应，但它们的真正价值在于选择性地制造所需形状和配方的单一产品，其中非催化过程将产生多个产品，所需的分子必须从这些产品中分离出来。 在无机分子和材料的生产中，催化提供的选择性严重得不到充分利用。我们的研究旨在纠正这一点。我们专注于P-H和Si-H键的催化转化产生的丰富的反应活性，并确定了磷或硅的化学、区域和立体结合具有显著价值的合成目标。这些包括：用于不对称有机合成的对映膦配体；用于光学和/或电子器件的坚固的聚硅烷塑料；以及用于制备各种含硅材料的独特的活性硅氧烷前体。 为了实现这些合成，我们需要对潜在的反应机理建立良好的理解，以便我们能够选择合适的催化剂和条件。我们将对基于过渡金属络合物(Ru、Rh等)和Lewis酸(有机硼烷)的简单催化剂体系进行详细研究。这些将包括使用一系列光谱、光谱和色谱技术对化学计量反应和催化反应进行全面的产品分析，以及动力学研究，以及仔细改变催化剂结构以观察活性的差异。

The importance of catalysis in the production of organic molecules and materials for the bulk and fine chemicals industries cannot be overstated. Although we typically think of catalysts as simply speeding up slow reactions, their real value is in selectively making single products of desired shapes and formulae, where non-catalytic processes would give multiple products from which the desired molecules must be separated. The selectivity afforded by catalysis is seriously under-exploited in the production of inorganic molecules and materials. Our research aims to remedy this. We have focused on the rich reactivity arising from catalytic transformations of P-H and Si-H bonds, and have identified synthetic targets for which the chemo-, regio-, and stereospecific incorporation of phosphorus or silicon adds significant value. These include: enantiopure phosphine ligands for use in asymmetric organic syntheses; robust polysilane plastics for incorporation in optical and/or electronic devices; and uniquely reactive siloxane precursors for the preparation of diverse silicone-containing materials. To achieve these syntheses, we need to establish a good understanding of the underlying reaction mechanisms, so that we can choose appropriate catalysts and conditions. We will carry out detailed studies of simple catalyst systems based both on transition metal complexes (Ru, Rh, and others) and on Lewis acids (organoboranes). These will involve comprehensive product analysis of both stoichiometric and catalytic reactions using a range of spectroscopic, spectrometric and chromatographic techniques, as well as kinetic studies, and careful variation of catalyst structure to observe differences in activity.