CAREER: Supports as steric and electronic modifiers of catalysis at single atom metal active sites

1554112 Christopher，Phillip通过孤立的金属原子促进催化反应负载的金属催化剂，特别是那些使用昂贵的贵金属如铑（Rh）的催化剂，通常在贵金属以极小的颗粒分散时最有效地利用-并且在极限情况下作为孤立的金属原子。 本研究在基础水平上考察了如何设计支持氧化物材料和活性贵金属之间的相互作用，以控制孤立Rh原子的稳定性和活性。 从工作的见解将被用来设计催化剂，丙烯加氢的高选择性-一个重要的工业反应，目前在均相液相催化条件下运行。 一种异质的气相类似物--如这里所寻求的--将提供一种成本较低、环境友好的替代品。 此外，该研究将为加州大学滨江分校广泛多样的学生提供机会，以培养成功的技术职业所需的分析和沟通技能。该项目的重点是控制选择性，反应性，通过改变氧化物载体和通过用有机硅烷部分以产生复制的电子和空间结构的方式官能化载体，单金属原子均相催化剂的那些。 该研究的核心是一系列涉及合成，原位催化剂转化和分析方法的技术，这些技术将用于创建，确认和表征孤立的原子位点并控制其活性和稳定性。 基础实验将使用探针分子光谱学，探针反应动力学，原位光谱学和显微镜，密度泛函理论计算进行。 虽然当前的重点将是丙烯加氢，但相关的基本理解将通过设计比均相工艺更具能源和环境友好性的多相催化工艺而造福社会。 该项目的高度多学科性质将为学生提供大量的机会，在这个西班牙裔服务机构发展技能，提出技术信息的基础上仔细推理和结构化的科学论据。

1554112 Christopher, PhillipPromoting Catalytic Reactions Via Isolated Metal AtomsSupported metal catalysts, especially those utilizing expensive noble metals such as rhodium (Rh), are often most effectively utilized when the noble metal is dispersed as extremely small particles - and in the limit as isolated metal atoms. This study examines at a fundamental level how interactions between the supporting oxide material and the active noble metal can be engineered to control the stability and activity of isolated Rh atoms. Insights from the work will be used to design catalysts with high selectivity in propylene hydroformylation - an important industrial reaction currently operated under homogeneous liquid-phase catalytic conditions. A heterogeneous, gas-phase analog - as sought here - would offer a lower cost, environmentally friendly alternative. Additionally, the research will provide opportunities for a broadly diverse student body at UC Riverside to develop both the analytical and communication skills needed for successful technical careers.The project focuses on controlling the selectivity, reactivity, and stability of isolated metal atom catalysts by varying the oxide support and by functionalizing the support with organosilane moieties in ways that create electronic and steric structures that replicate those of single-metal-atom homogeneous catalysts. Central to the study are a host of techniques involving synthesis, in-situ catalyst transformations, and analytical methods that will be utilized to create, confirm, and characterize the isolated atom sites and control their activity and stability. Fundamental experiments will be carried out using probe molecule spectroscopy, probe reaction kinetics, in-situ spectroscopy and microscopy, and density functional theory calculations. While the immediate focus will be on propylene hydroformylation, the associated fundamental understanding will benefit society through the design of heterogeneous catalytic processes that are more energy and environmentally friendly than homogeneous processes. The highly multidisciplinary nature of the project will provide plentiful opportunities for students at this Hispanic serving institution to develop skills in presenting technical information based on carefully reasoned and structured scientific arguments.