Activation of Carbon-Hydrogen Bonds at Multinuclear Metal Sites

甲烷和乙烷等简单碳氢化合物现在可以从充足的天然气供应中获得。然而，由于这些材料不容易转化为其他产品，它们不是化学工业的良好原料。在很大程度上，这种困难的出现是因为碳氢化合物中的碳氢(C-H)键相对不活跃。在这个由化学系化学合成计划资助的项目中，南卡罗来纳大学化学和生物化学系理查德·D·亚当斯教授正在开发激活碳氢C-H键的方法。具有两个或多个金属原子的金属络合物被设计成使碳氢化合物中的几个C-H键与金属相互作用。这些相互作用激活了键，并允许碳氢化合物转化为有价值的产品，如醇、醛和羧酸。这些导致了生产工业材料的新工艺。除了科学部分，该项目还涉及研究生和本科生，包括来自代表性不足的群体的学生，为他们在科学和技术领域的职业生涯做准备。贵金属元素的多核配合物，如Ru、Rh、Re、Ir和Plu，被评估它们激活碳氢C-H键的能力。通过使用具有两个或多个金属原子的金属络合物，实现了多个CH活化，并在单个碳氢化合物上引入了几个官能团。这些研究针对的是C-C和C-O键的形成过程，并包括机理研究，以揭示这些转变的细节。新的双金属络合物被转化为双金属纳米颗粒，从而创造出新一代高活性的多相催化剂。更广泛的影响包括开发新的工艺，将简单碳氢化合物和相关资源转化为用作工业原料的有价值的化学品。研究生和本科生接受最新的科学探究和分析方法的培训。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

Simple hydrocarbons such as methane and ethane are now available from abundant supplies of natural gas. However, since these materials cannot easily be converted into other products, they are not good feedstocks for the chemical industry. In large part, this difficulty arises because the carbon-hydrogen (C-H) bonds in hydrocarbons are relatively unreactive. In this project, funded by the Chemical Synthesis Program of the Chemistry Division, Professor Richard D. Adams, Department of Chemistry and Biochemistry at the University of South Carolina, is developing methods to activate hydrocarbon C-H bonds. Metal complexes having two or more metal atoms are designed so that several C-H bonds in a hydrocarbon interact with the metals. These interactions activate the bonds and allow the hydrocarbons to be converted into valuable products, such as alcohols, aldehydes and carboxylic acids. These lead to new processes for the production of industrial materials. In addition to the scientific component, the project involves both graduate and undergraduate students, including ones from underrepresented groups and prepares them for careers in science and technology.Multinuclear complexes of precious metal elements, such as ruthenium, rhodium, rhenium, iridium, and platinum, are evaluated for their ability to activate hydrocarbon C-H bonds. By using metal complexes having two or more metal atoms, multiple CH activations are achieved and several functionalities are introduced on a single hydrocarbon. The studies target C-C and C-O bond forming processes and include mechanistic investigations to uncover details of the transformations. New bimetallic complexes are converted into bimetallic nanoparticles to create a new generation of high activity heterogeneous catalysts. Broader impacts include the development of new processes for the conversion of simple hydrocarbons and related resources into valuable chemicals for use as industrial feedstocks. Graduate and undergraduate students are trained in the latest methods of scientific inquiry and analysis.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.