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

社会在放弃对化石燃料的依赖方面面临着巨大的挑战。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景观，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”的概念和一个依赖于可持续自然资源生物质的新化学部门。生物质由聚合物的混合物组成，与石油和天然气相比，生物质含有高比例的元素氧与元素碳。元素氧和碳形成强的碳-氧键，这对处理和将这些化学品转化为日常产品构成了障碍。为了使生物炼制的分子满足社会日益增长和复杂的需求，必须开发新的方法，通过破坏碳-氧键来去除可再生资源中的元素氧。我们的研究中心围绕开发新的基础方法，通过基于过渡金属和主族金属的催化剂活化，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醚转化为化学制造的化学构件的方法。具体来说，我们将通过破坏不反应的C-O键并用反应性C-B和C-Al键取代它们，将醚转化为C1-C9-烃结构单元。我们将展示这些构建模块在化学制造中的应用。

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.