Fundamental Reactions Relevant to Selective Hydrocarbon Functionalization with Late-Transition Metals

通过这一奖项，化学系的化学催化计划资助华盛顿大学的Karen I.Goldberg教授提高对关键反应的一般机理的理解，这些反应是设计催化剂所需的，使碳氢化合物能够实现节能、环保和经济高效的转化。新的催化方法选择性地将碳氢化合物的碳氢键转化为更高价值的产品，可能会影响大规模的化学生产。新的工艺可能最终允许工业化学家通过在生产中使用可用的和未得到重视的碳原料，以及大量的无毒试剂来实现更可持续的工艺。在这个项目中，碳氢功能化所涉及的特定反应步骤的机理，如碳氢键断裂和从空气中掺入氧，正在被仔细研究，以期在选择性催化中得到最佳应用。一群不同的研究生和本科生正在接受研究催化和机械的现代方法的培训。鼓励学生从事科学事业，强调需要一支强大的有效的独立科学家队伍。计划向高中生和普通公众宣传催化研究在寻找新的能源效率和环境友好的方法制造从塑料到油漆再到制药等许多日常产品方面的重要作用。戈德伯格教授正在详细了解基本的有机金属反应的机理，以及在碳氢化合物碳氢键功能化方面的潜在应用，包括选择性甲烷氧化。人们正在研究激活碳-氢键、选择性地激活氧并将氧结合到金属-烷基键以及区域选择性烯烃氢芳基化转化的新策略。目前正在研究关键的模型反应，通过对这些化学计量和催化反应的研究，正在确定促进这些转变的关键变量。对有利于特定反应步骤的特定配位环境、金属和配体选择、底物要求和反应条件等方面的见解进行了设想。从这些研究中收集的机械信息可能会对催化研究产生明显更广泛的影响，无论是在学术上还是在工业环境中。

With this award, the Chemical Catalysis Program of the Division of Chemistry is funding Professor Karen I. Goldberg of the University of Washington to improve the general mechanistic understanding of key reactions needed to design catalysts that enable an energy efficient, environmentally benign and cost-effective transformation of hydrocarbons. New catalytic methods that selectively convert the carbon-hydrogen bonds of hydrocarbons to yield higher value products have the potential to impact large-scale chemical production. New processes may eventually permit industrial chemists to achieve more sustainable processes by employing available and underappreciated carbon feedstocks, and abundant, non-toxic reagents in production. Within this project, the mechanisms of specific reaction steps involved in hydrocarbon functionalization, such as carbon-hydrogen bond cleavage and incorporation of oxygen from air, are being carefully investigated for their optimal application in selective catalysis. A diverse group of graduate and undergraduate students is being trained in modern methods for studying catalysis and mechanism. Students are encouraged to pursue careers in science, with emphasis on the need for a strong workforce of effective independent scientists. Outreach to high school students and the general public is being planned to communicate the vital role of catalysis research in finding new energy efficient and environmentally benign methods for making many everyday products from plastics, to paints, to pharmaceuticals.Professor Goldberg is developing a detailed mechanistic understanding of fundamental organometallic reactions with potential applications in the functionalization of carbon-hydrogen bonds of hydrocarbons, including selective methane oxidation. New strategies for activating carbon-hydrogen bonds, for selectively activating and incorporating oxygen into metal-alkyl bonds, and for regioselective olefin hydroarylation transformations are being investigated. Key model reactions are being studied, and through investigations of these stoichiometric and catalytic reactions, critical variables for promoting these transformations are being determined. Insights concerning specific coordination environments, metal and ligand options, substrate requirements and reaction conditions that favor particular reaction steps are envisaged. The mechanistic information gleaned from these studies may have a distinctly broader impact on catalysis research, in both academic and industrial settings.