CAREER: Developing Multi-Scale Models for the Effective Design of Hydrothermally Stable Single-Site Catalysts for Low-Temperature CO Emissions Removal

职业：开发多尺度模型，用于有效设计用于低温二氧化碳减排的水热稳定单中心催化剂

• 批准号: 1653561
• 负责人: Jean-Sabin McEwen
• 金额: $ 51.2万
• 依托单位: Washington State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2017
• 资助国家: 美国
• 起止时间: 2017-06-01 至 2025-05-31
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1653561&HistoricalAwards=false
• 关键词: CAREER; Developing; Multi; Scale; Models

The project investigates the potential applicability of the emerging area of "single-site" catalysis to low-temperature automotive exhaust catalysis, thereby paving a path toward efficient and stable automotive catalysts comprised primarily of earth-abundant transition metals aided by low concentrations of atomically-dispersed noble metals such as platinum. The study will also yield improved computational methods for general predictions of single-site catalysis opportunities and limitations for a broad range of chemical processes based on supported catalysts. The research will be integrated both with experimental surface science and catalysis studies at Tufts and related educational and outreach programs targeting underrepresented groups (including American Indians) at the high school through graduate school levels.A multi-scale model will be developed to predict the catalytic behavior of low-temperature exhaust catalysts in real-world conditions. The central hypothesis is that the chemical modification of a first-row transition metal oxide with an atomically dispersed precious metal will display theoretical efficiencies that are superior to pure-precious-metal catalysts, and that these high efficiencies will be connected to the support's ability to control the oxidation state of the atomically dispersed metal. To this end, a comprehensive model - developed from high quality characterization data obtained from other groups - will be used to predict exhaust-gas related reactions such as CO oxidation and the water-gas shift reaction, on atomically dispersed platinum with a well-defined copper surface oxide support. The educational and outreach objectives will demonstrate how computational modeling tools can be used in conjunction with experimental data to accelerate the discovery of new catalyst materials and structures. The PI will use a story-telling approach to explain automotive exhaust catalysis to high-school students in a way that excites them about higher education opportunities in STEM disciplines.

该项目调查了“单位点”催化新兴区域对低温汽车排气催化的潜在适用性，从而铺平了一条通往高效且稳定的自动催化剂的道路，主要由地球上余丰的过渡金属组成，由低浓度的原子质降低的无含量的不含量的不含量的无磷酸金属（例如铂）提供了帮助。 该研究还将产生改进的计算方法，以基于支持的催化剂的广泛化学过程的单位催化机会的一般预测。 这项研究将与实验性的表面科学和塔夫茨的实验表面科学和催化研究融合，以及针对高中通过研究生院级别的代表性不足的群体（包括美国印第安人）的相关教育和外展计划。将开发多尺度模型，以预测现实情况下低温排气催化剂的催化行为。中心假设是，具有原子分散的珍贵金属的第一行过渡金属氧化物的化学修饰将显示出理论上的效率，这些效率优于纯粹的金属催化剂，并且这些高效率将与支撑物控制原子分散金属的氧化状态有关。为此，将使用从其他组获得的高质量表征数据开发的综合模型，用于预测与排气总和相关的反应，例如CO氧化和水和气偏移反应，并在原子分散的铂和铜表面氧化物支撑的原子分散的铂上。教育和外展目标将证明如何与实验数据结合使用计算建模工具来加速发现新的催化剂材料和结构。 PI将使用讲故事的方法向高中生解释汽车排气催化，以使他们对STEM学科中的高等教育机会感到兴奋。

项目成果

Templated Growth of a Homochiral Thin Film Oxide

同手性薄膜氧化物的模板化生长

• DOI: 10.1021/acsnano.0c00398
• 发表时间: 2020
• 期刊: ACS Nano
• 影响因子: 17.1
• 作者: Schilling, Alex C.;Therrien, Andrew J.;Hannagan, Ryan T.;Marcinkowski, Matthew D.;Kress, Paul L.;Patel, Dipna A.;Balema, Tedros A.;Larson, Amanda M.;Lucci, Felicia R.;Coughlin, Benjamin P.
• 通讯作者: Coughlin, Benjamin P.

Probing Active-Site Relocation in Cu/SSZ-13 SCR Catalysts during Hydrothermal Aging by In Situ EPR Spectroscopy, Kinetics Studies, and DFT Calculations

• DOI: 10.1021/acscatal.0c01590
• 发表时间: 2020-06
• 期刊: ACS Catalysis
• 影响因子: 12.9
• 作者: Yani Zhang;Yue Peng;Junhua Li;Kyle Groden;Jean-Sabin McEwen;E. Walter;Ying Chen;Yong Wang;F. Gao

An atomic-scale view of single-site Pt catalysis for low-temperature CO oxidation

• DOI: 10.1038/s41929-018-0028-2
• 发表时间: 2018-03-01
• 期刊: NATURE CATALYSIS
• 影响因子: 37.8
• 作者: Therrien, Andrew J.;Hensley, Alyssa J. R.;Sykes, E. Charles H.
• 通讯作者: Sykes, E. Charles H.

Developing single-site Pt catalysts for the preferential oxidation of CO: A surface science and first principles-guided approach

• DOI: 10.1016/j.apcatb.2020.119716
• 发表时间: 2021-05
• 期刊: Applied Catalysis B: Environmental
• 作者: Jilei Liu;Alyssa J. R. Hensley;G. Giannakakis;A. Therrien;A. Sukkar;A. Schilling;Kyle Groden;Nisa Ulumuddin;Ryan T. Hannagan;M. Ouyang;M. Flytzani-Stephanopoulos;Jean-Sabin McEwen;E. Sykes

Water activation by single Pt atoms supported on a Cu2O thin film

• DOI: 10.1016/j.jcat.2018.04.024
• 发表时间: 2018-08
• 期刊: Journal of Catalysis
• 影响因子: 7.3
• 作者: A. Therrien;Kyle Groden;Alyssa J. R. Hensley;A. Schilling;Ryan T. Hannagan;Matthew D. Marcinkowski;Alex Pronschinske;F. Lucci;E. Sykes;Jean-Sabin McEwen