Design rules for synthesis of stable single-site catalysts from experiment and first principles theory

在美国国家科学基金会化学部化学催化项目的资助下。宾夕法尼亚州立大学的Rioux和Janik正在研究提供新的、更有效的催化剂的基本原理。目前使用的大多数催化剂都是由金属原子聚集在支撑材料上构成的。这些金属通常是稀有和昂贵的，并且聚集体中的金属原子在催化作用中不活跃。如果把这些昂贵的金属作为单个原子，而不是作为载体上的聚集体来使用，就有可能更有效地利用它们。因此，制备单原子金属催化剂具有重要的动力。宾夕法尼亚州立大学的研究小组正在使用实验和计算方法相结合的方法来确定和理解单原子催化剂可以成功制备的条件。来自在科学和工程领域未被充分代表的群体的本科生正在被纳入这些研究工作。此外，学生研究人员正在开发教学模块，展示能源生产如何影响我们的环境，并将其纳入针对学生和公众的推广活动中。单原子催化剂是一类令人兴奋的新型催化剂，在与能源生产有关的化学反应中表现出高活性。Robert Rioux博士和Michael Janik博士的研究小组正在开发计算推导和实验验证的设计规则，以稳定可还原氧化物上的单原子基序。该合成方法是基于贵金属族金属前驱体的强静电吸附，这将确定金属在氧化物载体上负载的上限。计算和实验技术的结合允许确定描述符，指导前体，支持和pH值的选择，以合成稳定的贵金属单原子催化剂。固液界面吸附的等温滴定量热法测量和密度泛函理论计算被用于评价和预测导致形成稳定的单原子催化剂的条件。由于钯铈体系有望成为低温甲烷氧化催化剂，因此被用作初始测试平台。该研究项目包括本科生通过少数民族本科生研究经验和科学与工程研究项目参与研究，并正在生成教学模块，展示能源生产对我们环境的影响，用于推广活动。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 funding from the Chemical Catalysis Program of the NSF Division of Chemistry, Drs. Rioux and Janik of Penn State University are developing fundamental principles to provide new, more effective catalysts. Most catalysts used today consist of aggregates of metal atoms on a support material. The metals are often rare and expensive, and the metal atoms inside the aggregates are not active in catalysis. Much more efficient use of these expensive metals is possible if they are used as single atoms, and not aggregates, on the support. Thus, there is significant motivation for preparing single atom metal catalysts. The Penn State team is using a combination of experimental and computational methods to determine and understand the conditions under which single atom catalysts can be successfully prepared. Undergraduates from groups underrepresented in science and engineering are being included in these research efforts. In addition, student researchers are developing teaching modules that demonstrate how energy production impacts our environment for inclusion in outreach activities directed at students and the general public.Single-atom catalysts represent an exciting new class of catalysts that have demonstrated high activity for chemical reactions relevant in energy production. The research groups of Dr. Robert Rioux and Dr. Michael Janik are developing computationally derived and experimentally validated design rules for the stabilization of single-atom motifs on reducible oxides. The synthesis approach is based on the strong electrostatic adsorption of precious group metal precursors that will define the upper boundary for metal loading on oxide supports. The combination of computational and experimental techniques is allowing the determination of descriptors that guide the choice of precursors, support, and pH for the synthesis of stable precious metal single atom catalysts. Isothermal titration calorimetry measurements of adsorption at the solid-liquid interface and density functional theory calculations are being used to evaluate and predict conditions leading to formation of stable single atom catalysts. The Pd on ceria system is being used as an initial testbed due to its promise as a low-temperature methane oxidation catalyst. The research project includes undergraduate involvement in research through the Minority Undergraduate Research Experience and Women in Science and Engineering Research programs, and is generating teaching modules that demonstrate the impact of energy production on our environment for use in outreach activities.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.