Homogeneous Catalysts for the Activation and Functionalization of Carbon Oxygen Sigma Bonds in Ethers from Biomass

在放弃对化石燃料的依赖方面，社会面临着巨大的挑战。虽然二氧化碳水平和石油价格继续上升，但石油分子继续主导着我们的格局，并为我们的化学工业提供燃料。作为解决这一危机的一种方法，许多人提倡“生物炼油厂”的概念和依赖于可持续自然资源生物质的新的化学部门。生物质是由聚合物的混合物组成的，与石油和天然气相比，这种聚合物含有高比例的元素氧和元素碳。元素氧和碳形成强大的碳氧键，这为将这些化学品加工和转化为日常产品提供了障碍。为了使生物精炼中的分子满足日益增长和复杂的社会需求，必须开发新的方法，通过打破碳-氧键来去除可再生资源中的元素氧。我们的研究重点是开发新的支撑方法，通过以过渡金属和主族金属为基础的催化剂活化，将碳-氧键转化为碳-碳和碳-氮键。通过发现和开发新的催化剂系统，我们将发现将生物质中的乙醚转化为化学制造的化学构件的方法。具体地说，我们将通过打断未反应的C-O键并用活性C-B和C-Al键取代它们，将醚转化为C1-到C9-烃的构建基块。我们将演示这些构建块在化学制造中的使用。

Society faces a monumental challenge in relinquishing its dependence on fossil fuels. While CO2 levels and the price of petroleum continue to rise, molecules from oil continue to dominate the landscape and fuel our chemical industries. As one approach to solving this crisis, many have promoted the concept of "The Biorefinery" and a new chemical sector dependent upon the sustainable natural resource biomass. Biomass is made up of a mixture of polymers which, when compared to petroleum and natural gas, contain a high ratio of elemental oxygen to elemental carbon. The elemental oxygen and carbon form strong carbon-oxygen bonds which present an obstacle for processing and transforming these chemicals into everyday products. In order for molecules from biorefineries to meet the growing and complex demands of Society, new methods will have to be developed that remove the elemental oxygen from renewable resources by breaking carbon-oxygen bonds.Our research centers around developing new underpinning methods for the transformation of carbon-oxygen bonds to carbon-carbon and carbon-nitrogen bond by activation with catalysts based on transition and main-group metals. By discovering and exploiting new catalyst systems we will uncover methods for turning ethers from biomass into chemical building blocks for chemical manufacture. Specifically, we will convert ethers into C1- to C9-hydrocarbon building blocks by breaking the unreactive C-O bonds and replacing them with reactive C-B and C-Al bonds. We will demonstrate the use of these building blocks in chemical manufacture.