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

EAGER：开发用于去除低温碳氢化合物和二氧化碳排放的原子效率单中心催化剂

• 批准号: 1552320
• 负责人: Jean-Sabin McEwen
• 金额: $ 10万
• 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: 2015
• 资助国家: 美国
• 起止时间: 2015-09-01 至 2017-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1552320&HistoricalAwards=false
• 关键词: EAGER; Development; Atom; Efficient; Single

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.

该项目将“单点”催化的计算进展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。这是一项雄心勃勃的事业，因为汽车催化剂的反应环境复杂，而且在使用寿命期间会经历各种各样的条件。拟议的研究将有助于实现高效低温燃烧系统，使催化剂的设计能够在低温排气环境中满足严格的排放标准，同时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试错催化剂筛选，几乎没有理论基础。这一建议有可能开发一种理论辅助的催化剂设计方法，从而打开了设计空间，同时减少了实验负担。该提案为一氧化碳和碳氢化合物的低温汽车排放氧化的单中心催化的综合，预测和实验验证模型奠定了基础。它建立在催化剂的最新进展之上，这些进展表明了合成单中心催化剂的能力，并在许多反应中证明了它们相对于负载金属簇或颗粒的优势。然而，将这些进展扩展到汽车催化并不是直截了当的。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起作用的宽操作温度范围。该提案将建立在合成单位点含钯催化剂的实验进展以及先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下耐久性所需的单位点催化剂性质的双重推力代表了对先前工作的计算努力的雄心勃勃的扩展。 由此产生的方法和理解应该推广到其他系统。研究人员还在提案中计划将计算催化纳入高中学生的教育计划，旨在说明基础化学对替代能源领域进步的重要性。这些方案将与教育机构和旨在为少数群体提供机会的现有方案合作进行。

项目成果

Structurally Accurate Model for the “29”-Structure of Cu x O/Cu(111): A DFT and STM Study

Cu x O/Cu(111) 的 29 结构的结构精确模型：DFT 和 STM 研究

• DOI: 10.1021/acs.jpcc.6b01284
• 发表时间: 2016
• 期刊: The Journal of Physical Chemistry C
• 作者: Therrien, Andrew J.;Zhang, Renqin;Lucci, Felicia R.;Marcinkowski, Matthew D.;Hensley, Alyssa;McEwen, Jean-Sabin;Sykes, E. Charles
• 通讯作者: Sykes, E. Charles