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

该项目将“单位点”催化的计算进步与汽车催化的需求结合起来，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以及它们在使用寿命期间所经历的广泛条件，这是一项雄心勃勃的任务。这项研究将通过设计能够在低温排气环境中满足严格排放标准的催化剂，帮助实现高效低温燃烧系统，同时也最大限度地减少对昂贵贵金属的依赖。汽车催化剂的发展历来依赖于催化剂筛选的反复试验，几乎没有理论基础。这一建议有可能发展出一种理论辅助的催化剂设计方法，从而开辟了设计空间，同时减少了实验负担。该建议为建立一个全面、预测和实验验证的汽车排放一氧化碳和碳氢化合物低温氧化单位点催化模型奠定了基础。它建立在催化的最新进展上，说明了合成单位点催化剂的能力，并在许多反应中证明了它们比支撑金属团簇或颗粒的优势。然而，将这些先进技术推广到汽车催化领域并非易事。汽车催化比大多数催化应用更复杂，因为废气环境的复杂和动态变化以及催化剂必须在长寿命下工作的广泛工作温度范围。该提案将建立在单位点含钯催化剂合成的实验进展，以及先前证明镧稳定贵金属颗粒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位点催化剂性质的双重推力代表了对以前工作的雄心勃勃的计算努力的扩展。由此产生的方法和理解应该可以推广到其他系统。研究人员还在提案中计划将计算催化整合到高中学生的教育计划中，旨在说明基础化学对替代能源领域进步的重要性。这些项目将与旨在为少数民族提供机会的教育机构和现有项目合作开展。

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.