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

从实验和第一性原理理论合成稳定单中心催化剂的设计规则

基本信息

批准号：
1800507
负责人：
Robert Rioux
金额：
$ 47.32万
依托单位：
Pennsylvania State Univ University Park
依托单位国家：
美国
项目类别：
Continuing Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-09-01 至 2022-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1800507&HistoricalAwards=false
关键词：
Design rules synthesis stable single

项目摘要

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.

在美国国家科学基金会化学部化学催化计划的资助下，博士。宾夕法尼亚州立大学的 Rioux 和 Janik 正在开发基本原理，以提供新的、更有效的催化剂。目前使用的大多数催化剂由载体材料上的金属原子聚集体组成。这些金属通常稀有且昂贵，并且聚集体内的金属原子不具有催化活性。如果这些昂贵的金属在载体上以单个原子而不是聚集体的形式使用，则可以更有效地利用它们。因此，制备单原子金属催化剂具有重要的意义。宾夕法尼亚州立大学团队正在使用实验和计算方法相结合来确定和了解可以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也被纳入这些研究工作中。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，以纳入针对学生和公众的外展活动。单原子催化剂代表了一类令人兴奋的新型催化剂，它们在相关化学反应中表现出高活性。在能源生产方面。 Robert Rioux 博士和 Michael Janik 博士的研究小组正在开发计算得出并经过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。该合成方法基于贵族金属前体的强静电吸附，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可以确定描述符，从而指导合成稳定的贵金属单原子催化剂的前体、载体和 pH 值的选择。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用于评估和预测形成稳定单原子催化剂的条件。二氧化铈上的钯系统由于其作为低温甲烷氧化催化剂的前景而被用作初始测试平台。该研究项目包括本科生通过少数族裔本科生研究经验和女性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，用于外展活动。该奖项反映了 NSF 的法定使命通过使用基金会的智力价值和更广泛的影响审查标准进行评估，并被认为值得支持。