EAGER: Development of Atom Efficient Single Site Catalysts for Low Temperature Hydrocarbon and CO Emissions Removal

该项目将单位催化的计算进展与汽车催化的需求相结合，为低温活性和热稳定的下一代汽车催化剂的实验设计提供理论驱动的帮助。考虑到汽车催化剂复杂的反应环境和它们在使用寿命中所经历的广泛条件，这是一项雄心勃勃的任务。拟议的研究将有助于实施高效低温燃烧系统，使催化剂的设计能够在低温废气环境中满足严格的排放标准，同时还能最大限度地减少对昂贵贵金属的依赖。汽车催化剂的开发历来依赖于反复试验的催化剂筛选，几乎没有理论支持。这一建议有可能开发一种理论辅助的催化剂设计方法，从而在减少实验负担的同时开辟设计空间。该提案为建立一个全面的、可预测的、经过实验验证的一氧化碳和碳氢化合物低温汽车尾气氧化单位催化模型奠定了基础。它建立在催化方面的最新进展的基础上，这些进展表明了合成单位催化剂的能力，并在许多反应中展示了它们相对于负载金属簇或颗粒的优势。然而，将这些进展延伸到汽车催化领域并不是一帆风顺的。汽车催化比大多数催化应用更加复杂，因为尾气环境的复杂和动态变化，以及催化剂必须在较宽的工作温度范围内长时间发挥作用。该提案将建立在单位含钯催化剂合成实验进展的基础上，以及之前证明氧化镧稳定贵金属颗粒的有效性的工作的基础上。预测低温转化效率和高温耐久性所需的单点催化剂性质的双重推力代表着计算工作在以前工作基础上的雄心勃勃的扩展。由此产生的方法和理解应该可以推广到其他系统。这位研究人员还在提案中包括了将计算催化纳入一个面向高中生的教育项目的计划，该项目旨在说明基础化学对替代能源领域进展的重要性。这些方案将与教育机构和旨在为少数族裔提供机会的现有方案合作进行。

The project marries computational advances in "single site" catalysis with the demands of automotive catalysis to provide theory-driven aid to experimental design of low-temperature active and thermally stable next-generation automotive catalysts. This is an ambitious undertaking given the complex reaction environment of automotive catalysts and the broad range of conditions that they experience over their useful life. The proposed research will aid the implementation of high-efficiency low-temperature combustion systems by enabling the design of catalysts capable of meeting strict emission standards in a low-temperature exhaust environment, while also minimizing reliance on expensive noble metals. Development of automotive catalysts has historically relied on trial-and-error catalyst screening, with little theoretical underpinning. This proposal has the potential to develop a theory-aided approach to catalyst design, thereby opening up the design space while reducing the experimental burden. The proposal lays groundwork for a comprehensive, predictive, and experimentally validated model of single site catalysis for low-temperature automotive emission oxidation of carbon monoxide and hydrocarbons. It builds on recent advances in catalysis that speak to the ability to synthesize single site catalysts and demonstrate their advantages over supported metal clusters or particles in a number of reactions. The extension of these advances to automotive catalysis is not straight-forward, however. Automotive catalysis is more complicated than most catalytic applications because of the complex and dynamic changes in exhaust gas environment and broad operating temperature ranges under which the catalysts must function over a long life. The proposal will build on experimental progress in the synthesis of single site palladium-containing catalysts, as well as previous work demonstrating the effectiveness of lanthana for stabilizing noble metal particles. The dual thrust to predict single site catalyst properties needed for both low-temperature conversion efficiency and durability at high temperatures represents an ambitious extension of computational efforts over previous work. The resulting methods and understanding should be generalizable to other systems. The investigator has also included in the proposal plans to integrate computational catalysis into an educational program for high school students aimed at illustrating the importance of fundamental chemistry for advances in alternative energy fields. Those programs will be conducted in collaboration with educational institutions and existing programs that aim to provide opportunities for minorities.