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.

该项目调查了新兴的“单点”催化领域对低温汽车尾气催化的潜在适用性，从而铺平了一条通往高效和稳定的汽车催化剂的道路，该催化剂主要由富含稀土的过渡金属组成，辅以低浓度的原子分散的贵金属，如铂。这项研究还将改进计算方法，用于基于负载型催化剂的广泛化学过程的单点催化机会和限制的一般预测。这项研究将与塔夫茨大学的实验表面科学和催化研究以及相关的教育和推广项目相结合，这些项目针对高中到研究生水平的代表不足的群体(包括美国印第安人)。将开发一个多尺度模型来预测低温废气催化剂在现实世界条件下的催化行为。中心假设是，用原子分散的贵金属对第一排过渡金属氧化物进行化学修饰将显示出优于纯贵金属催化剂的理论效率，并且这些高效率将与载体控制原子分散的金属的氧化状态的能力有关。为此，一个从其他组获得的高质量表征数据开发的综合模型将用于预测废气相关反应，如CO氧化和水-气变换反应，在原子分散的铂上，具有明确定义的铜表面氧化物载体。教育和推广目标将展示如何结合实验数据使用计算建模工具，以加速发现新的催化剂材料和结构。PI将使用讲故事的方式向高中生解释汽车尾气催化作用，以使他们对STEM学科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

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

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.

Assessing factors that determine adatom migration and clustering on a thin film oxide; Pt1 and Rh1 on the “29” CuxO/Cu(1 1 1) surface

评估决定吸附原子在薄膜氧化物上迁移和聚集的因素；

• DOI: 10.1016/j.apsusc.2023.157145
• 发表时间: 2023
• 期刊: Applied Surface Science
• 影响因子: 6.7
• 作者: Ulumuddin, Nisa;Çınar, Volkan;Schilling, Alex C.;Hunt, Adrian;Waluyo, Iradwikanari;Sykes, E. Charles;McEwen, Jean-Sabin
• 通讯作者: McEwen, Jean-Sabin