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

该项目研究了新兴的“单中心”催化领域对低温汽车尾气催化的潜在适用性，从而为高效稳定的汽车催化剂铺平了道路，该催化剂主要由地球上丰富的过渡金属组成，辅之以低浓度的原子分散贵金属，如铂。 该研究还将产生改进的计算方法，用于对基于负载型催化剂的广泛化学过程的单中心催化机会和限制进行一般预测。 该研究将与塔夫茨大学的实验表面科学和催化研究以及针对高中到研究生院水平的代表性不足的群体（包括美洲印第安人）的相关教育和推广计划相结合。将开发一个多尺度模型来预测低温排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行过渡金属氧化物进行化学改性将显示出比纯贵金属催化剂优越的上级理论效率，并且这些高效率将与载体控制原子分散的金属的氧化态的能力有关。为此，一个全面的模型-从高品质的表征数据从其他团体获得-将被用来预测废气相关的反应，如CO氧化和水煤气变换反应，原子分散的铂与明确的铜表面氧化物支持。教育和推广目标将展示计算建模工具如何与实验数据结合使用，以加速新催化剂材料和结构的发现。 PI将使用讲故事的方法向高中生解释汽车尾气催化，以使他们对STEM学科的高等教育机会感到兴奋。

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.