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

通过这一奖项，化学系的化学催化项目资助了华盛顿大学的Karen I. Goldberg教授，以提高对设计催化剂所需的关键反应的一般机理理解，从而实现节能、环保和成本效益高的碳氢化合物转化。新的催化方法选择性地转化碳氢化合物的碳氢键以产生更高价值的产品，这有可能影响大规模的化学生产。新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被充分利用的碳原料以及丰富的无毒试剂来实现更可持续的工艺。在这个项目中，正在仔细研究碳氢化合物功能化过程中特定反应步骤的机制，如碳氢键裂解和空气中氧气的掺入，以便在选择性催化中获得最佳应用。一群多样化的研究生和本科生正在接受研究催化和机理的现代方法的培训。鼓励学生从事科学事业，重点是需要一支强大的有效的独立科学家队伍。正在计划向高中学生和一般公众宣传催化研究在寻找新的节能和无害环境的方法以制造从塑料、油漆到药品等许多日常用品方面的重要作用。Goldberg教授正在发展对基本有机金属反应的详细机理理解，这些反应在碳氢化合物碳氢键功能化方面有潜在的应用，包括选择性甲烷氧化。目前正在研究激活碳氢键、选择性地激活和结合氧到金属-烷基键以及区域选择性烯烃氢芳基化转化的新策略。研究人员正在研究关键的模型反应，并通过对这些化学计量和催化反应的研究，确定了促进这些转化的关键变量。展望了特定的配位环境、金属和配体选择、底物要求和有利于特定反应步骤的反应条件。从这些研究中收集到的机理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.