Transition Metal and Main Group Organometallic Chemistry: Synthesis and Catalysis

化学催化是通过添加在反应中不消耗的物质-催化剂来提高有用反应的速率、选择性和效率的过程。基于过渡金属的催化剂通过提供用于形成和断开化学键的低能量路径而起作用。对于需要能量才能完成的反应，催化剂也可以从阳光中获取能量，以推动反应向前发展。 将CO2或H2O（两种高度丰富的小分子）转化为有用的产品或燃料的催化剂的发现是旨在为当今人类面临的主要环境（CO2利用）和能源（将水分解为H2和O2）问题找到解决方案的研究的关键。 我们的团队积极参与寻找新的催化剂和捕光材料，并探索它们运作的详细分子机制。 这些基础知识对于在工业上大规模开发这些反应的催化剂至关重要。 这项建议侧重于三个主要调查领域： 1)用于CO2转化的前过渡金属催化剂。 2)有机物分解水的方法。 3)含硼杂环化合物在材料中的应用。 虽然这些主题跨越了元素周期表，但我们在所有项目中的方法都是统一的，希望识别重要的反应并在分子水平上详细研究它们。 这涉及使用所有现代光谱，结构，计算和动力学技术进行深入的机理研究。这些详细信息的价值在于，通过精确的动力学和热力学数据而不是试错来开发改进的下一代催化剂。 该方法还为合成和机械化学提供了一个很好的培训基地，使毕业生具有良好的解决问题的能力以及现代化学技术的技术熟练程度。

Chemical catalysis is a process by which useful reactions are improved in rate, selectivity and efficiency by addition of a species that is not consumed in the reaction-the catalyst. Transition metal-based catalysts act by providing low energy pathways for making and breaking chemical bonds. For reactions that require energy to go to completion, catalysts may also harvest energy from sunlight to drive reactions forward. Discovery of catalysts that convert CO2 or H2O (two highly abundant small molecules) into useful products or fuels are at the crux of research aimed at finding solutions to major environmental (CO2 utilization) and energy (splitting of water into H2 and O2) problems that face humanity today. Our group is actively involved in the search for new catalysts and light harvesting materials and probing the detailed molecular mechanisms by which they operate. This fundamental knowledge is critical for the development of catalysts for these reactions on an industrially significant scale. This proposal focuses on three main areas of inquiry: 1) Early Transition Metal Catalysts for CO2 Conversion. 2) Organometallic Approaches to Water Splitting. 3) Boron Containing Heterocycles for Materials Applications. Although these topics span the periodic table, our approach in all projects is unified by the desire to identify important reactions and study them in great detail at the molecular level. This involves conducting in-depth mechanistic studies using all of the modern spectroscopic, structural, computational and kinetic techniques available. The value of such detailed information is that development of improved, next generation catalysts is informed by precise kinetic and thermodynamic data and not trial and error. The approach also provides an excellent training ground for synthetic and mechanistic chemistry, leaving graduates with sound problem-solving skills as well as technical proficiency in the techniques of modern chemistry.