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计划的资助下，宾夕法尼亚州立大学的Rioux博士和Janik博士正在开发基本原理，以提供新的、更有效的催化剂。今天使用的大多数催化剂都是由载体材料上的金属原子聚集体组成的。金属通常是稀有和昂贵的，聚集体中的金属原子在催化中不活跃。如果这些昂贵的金属在载体上作为单原子而不是聚集体使用，那么它们的使用效率可能会高得多。因此，制备单原子金属催化剂具有重要的动机。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了解成功制备单原子催化剂的条件。来自科学和工程领域代表性不足的群体的本科生被纳入这些研究努力。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，以包括在针对学生和公众的推广活动中。单原子催化剂代表了一种令人兴奋的新催化剂类别，已显示出与能源生产相关的化学反应的高活性。Robert Rioux博士和Michael Janik博士的研究小组正在开发通过计算推导和实验验证的设计规则，用于稳定可还原氧化物上的单原子基序。合成方法是基于贵族金属前驱体的强烈静电吸附，这将定义氧化物载体上金属负载的上限。计算和实验技术的结合使得能够确定用于指导合成稳定的贵金属单原子催化剂的前体、载体和pH的描述符。等温滴定量热法、固-液界面吸附测量和密度泛函理论计算被用来评估和预测导致稳定单原子催化剂形成的条件。由于Pd-on-CeO2体系有望成为低温甲烷氧化催化剂，该催化剂正被用作初始试验床。该研究项目包括通过少数民族本科生研究经验和女性参与科学和工程研究计划的本科生参与研究，并正在生成教学模块，展示能源生产对我们环境的影响，用于外展活动。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。

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.