Low-valent and low-coordinate main group chemistry

本提案中概述的研究计划需要开发和研究几种新的无机试剂系列。 特别是，这项研究的重点是主族的化学，其中包括元素周期表的s-和p-块的元素。 虽然这些元素是许多重要材料的组成部分，例如称为“铟锡氧化物”的透明半导体是触摸屏和太阳能电池板以及化合物（例如肥料和清洁产品中的磷酸盐）的关键组成部分，但与有机化学或过渡金属化学相比，这些元素的化学性质仍然知之甚少。** 我们的研究包括新主族化合物的合成以及通过使用计算化学对化学物种和反应进行精确建模。 目标化合物包括一类新的化学品，其中含有氧化态和配位数异常低的主族元素。 低氧化态化合物是富电子的，并且通常是高反应性的，许多具有低配位数的元素也是如此。 我们已经发现了方便的方法来介导这些化合物的几个主要类别的反应性，使得它们足够稳定以被分离，但仍然具有所需的反应性特征。 我们的化合物可以方便地合成许多使用传统方法难以或不可能合成的化合物，我们努力使用我们的新试剂来获得许多前所未有的化学品。 我们还将探索我们的试剂（以及从中衍生的化学品）作为形成新材料或重要材料的前体的实用性。 除了它们的合成效用之外，所研究的化合物还将为主族元素化学的基本方面提供许多新的见解。 这些研究提供的理解形成了合理设计和开发主族化合物衍生的化学品和材料所必需的基础。

The research program outlined in this proposal entails the development and investigation of several new families of inorganic reagents. In particular, this research is focused on the chemistry of the main group, which includes the elements of the s- and p-blocks of the periodic table. Although these elements are components in many important materials e.g. the transparent semi-conductor called "indium tin oxide" is a critical component of touch screens and solar panels and chemical compounds (e.g. phosphates in fertilizers and cleaning products), the chemistry of these elements remains poorly understood and controlled in comparison to those of organic chemistry or transition metal chemistry. ******Our studies include both the synthesis of new main group compounds and the accurate modeling of chemical species and reactions through the use of computational chemistry. The target compounds consist of new classes of chemicals that contain main group elements in unusually low oxidation states and coordination numbers. Low oxidation state compounds are electron-rich and are typically highly reactive as are many elements with low coordination numbers. We have discovered convenient approaches to mediate the reactivity of several major classes of these compounds so that they are stable enough to be isolated yet still possess the desired reactivity characteristics. Our compounds allow for the convenient synthesis of many compounds that are difficult or impossible to make using traditional methods and we endeavour to use our new reagents to obtain many unprecedented types of chemicals. We will also explore the utility of our reagents (and chemicals derived from them) as precursors for the formation of new or important materials. In addition to their synthetic utility, the compounds studied will provide many new insights into the fundamental aspects of the chemistry of the main group elements. The understanding provided by such studies form the foundation necessary for the rational design and development of chemicals and materials derived from main group compounds.