Generation of Single Cation Sites Supported on Oxides

在化学系化学催化项目的支持下，加州大学河滨分校的Matthew Conley博士正在研究使用设计的多相催化剂加速化学反应的方法。这些新型催化剂经过设计，可以提供比传统方法更节能的反应条件。康利教授和他的研究团队致力于开发专门的高表面积材料，这种材料可以与金属试剂反应，形成具有可理解结构和可调节催化活性的表面支撑金属位点。这个灵活的系统将被用来研究各种重要的过程，以产生对日常生活很重要的商品和特种化学品。康利博士将让莫雷诺谷高中的学生参与这项研究计划，以帮助培养对STEM学科的兴趣，并鼓励对STEM职业道路的兴趣。单原子催化剂（SACs）为非均相催化提供了一种比贵金属纳米颗粒更有效的原子效率策略，后者只有表面原子暴露于试剂中。SACs的生成涉及到极少量贵金属原子在氧化还原活性氧化物载体上的分散。康利博士和他的研究团队正在开发一种制备单阳离子位点催化剂（scs）的新方法，并研究这些新材料的催化反应活性，这些新材料对精细化工和大宗化工行业都很重要。该团队将使用这种合成技术来获得高表面积的氧化物，这些氧化物支持非常强的硅路易斯酸作为目标scs的前体。硅包覆氧化物将在有机金属配合物中用金属卤化物键处理，在明确的配位环境中形成单阳离子位（scs）。该方法被用于将单个过渡金属阳离子均匀分散在掺杂弱配位阴离子的氧化物表面上，并且是生成sac的已知方法的补充。由于这种生成SCSs的方法可以与多种有机金属试剂配对，Conley小组正在研究这些材料支持的一系列催化活性，包括烯烃聚合、氢胺化和硅氢化化学，以及甲烷的部分氧化。这些开发多相催化超临界流体的努力也将为研究生、本科生和高中生的多样化群体提供一个强大的训练环境。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

With the support of the Chemical Catalysis Program in the Division of Chemistry, Dr. Matthew Conley of the University of California – Riverside is studying ways to accelerate chemical reactions using designer heterogeneous catalysts. These new catalysts are engineered to provide more energy-efficient reaction conditions than traditional approaches. Professor Conley and his research team are invested in developing specialized high surface area materials that can react with metal reagents to form surface-supported metal sites with understandable structures and tunable catalytic activity. This flexible system will be employed to investigate a variety of important processes to generate commodity and specialty chemicals that are important to everyday life. Dr. Conley will be involving students from a Moreno Valley high school in this research program to help foster interest in STEM disciplines and encourage interest in STEM career paths. Single atom catalysts (SACs) provide a more atom-efficient strategy for heterogeneous catalysis than noble metal nanoparticles where only surface atoms are exposed to reagents. The generation of SACs involves the dispersion of very small quantities of noble metal atoms onto a redox active oxide support. Dr. Conley and his research team are developing a new approach to preparing single cation site catalysts (SCSs) and studying the catalytic reactivity of these new materials towards transformations that are important to both the fine and commodity chemical industries. The team will be using this synthetic technology to access high surface area oxides that support very strong silylium Lewis acids as precursors for the targeted SCSs. The silylium-coated oxides will be treated with metal-halide bonds in organometallic complexes to form single cation sites (SCSs) in well-defined coordination environments. This methodology is being used to install single transition metal cations uniformly dispersed on oxide surfaces doped with weakly coordinating anions and is complementary to known methods that generate SACs. Because this approach to generating SCSs can be paired with a variety of organometallic reagents, the Conley group is investigating a range of catalytic activity supported by these materials including olefin polymerization, hydroamination, and hydrosilylation chemistry, as well as the partial oxidation of methane. These efforts to develop SCSs for heterogeneous catalysis also will serve as a strong training environment for a diverse group of graduate, undergraduate, and high school students.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.