Integrated Experimental and Theoretical Endeavor for Fundamental Understanding of Processes in Methane Dehydroaromatization

综合实验和理论研究对甲烷脱氢芳构化过程的基本理解

• 批准号: 2320059
• 负责人: Sheima Khatib
• 金额: $ 50.94万
• 依托单位: Virginia Polytechnic Institute and State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2022
• 资助国家: 美国
• 起止时间: 2022-10-01 至 2024-11-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2320059&HistoricalAwards=false
• 关键词: Integrated; Experimental; Theoretical; Endeavor; Fundamental

The West Texas Permian Basin holds trillions of cubic feet of natural gas resources predominantly comprised of methane, which constitutes an economic opportunity in the billions of dollars to upgrade this low-carbon fossil fuel to higher-value fuels and chemicals. The project advances catalytic processing technology that upgrades methane to higher-value chemicals in small plants located at or near the production wells, thus avoiding flaring or costly gas pipeline transport. The catalysts currently employed in this process do not fulfill the activity and stability requirements necessary to make the process economically viable. The study integrates experimental and theoretical methods to better understand the factors limiting current catalyst performance, and uses that knowledge to guide the design of improved catalysts and processing schemes. The project also promotes training of graduate and undergraduate students in technologies related to efficient, cost-effective, and low environmental impact utilization of hydrocarbon resources, while promoting outreach to predominantly minority schools to attract K-12 students to STEM fields.This project targets methane dehydroaromatization (MDA) which constitutes a path for the direct conversion of methane to benzene and hydrogen. Specifically, the project focuses on ZSM-5-supported molybdenum (Mo) catalysts. Previous work by the investigators has revealed that the specific processes by which a ZSM-5-supported Mo oxide precursor is activated to form Mo carbide species strongly affects the catalytic behavior. Thus, Mo-C-support interactions play a pivotal role in achieving the stable formation of aromatics. To further investigate those interactions, model catalysts, with active metals existing only on either the outer surface or within the zeolite channels, will be prepared and evaluated by a suite of experimental and computational tools. The structure, location, and evolution of the Mo species will be monitored by in situ and operando experiments using advanced characterization techniques, including X-ray absorption and high-resolution powder diffraction. The experimental data will be combined with density functional theory calculations to advance knowledge with respect to the structure-activity relationship of the catalysts and the reaction pathways involved in the complete MDA catalytic cycle (activation, reaction, deactivation, regeneration). The combination of kinetic tests, in situ structural characterization, and theoretical calculations will result in the determination of the reaction and deactivation pathways of MDA and will provide the basis for the rational design of catalysts. Beyond the research efforts, the investigators will develop a novel virtual reality (VR) technology module that will allow K-12 students to immerse themselves into a catalyst structure and allow them to directly interact with dynamic 3-D images of the molecules involved in a catalytic process.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

西德克萨斯二叠纪盆地拥有数万亿立方英尺的天然气资源，主要由甲烷组成，甲烷构成了数十亿美元的经济机会，以将这种低碳化石燃料升级为高价值燃料和化学物质。 该项目推进了催化加工技术，该技术将甲烷升级为位于生产井或附近的小型植物中的高价值化学物质，从而避免了膨胀或昂贵的气管运输。 当前在此过程中使用的催化剂无法满足使该过程在经济上可行的必要的活动和稳定要求。该研究集成了实验和理论方法，以更好地了解限制当前催化剂性能的因素，并使用该知识来指导改进的催化剂和加工方案的设计。 该项目还促进了与高效，具有成本效益和低环境影响的技术有关的培训，同时促进了主要是少数族裔学校，以吸引K-12学生进入STEM领域。该项目构成了甲烷脱氢疗法（MDA），该项目构成了甲烷甲烷的甲烷和甲烷甲烷的途径。具体而言，该项目着重于ZSM-5支持的钼（MO）催化剂。 研究人员的先前工作表明，激活ZSM-5支撑的Mo氧化物前体以形成Mo碳化物物质的特定过程会强烈影响催化行为。 因此，Mo-C-支持相互作用在实现芳香族的稳定形成中起着关键作用。 为了进一步研究这些相互作用，模型催化剂，仅在外表面或沸石通道内存在活性金属，将通过一套实验和计算工具进行准备和评估。 MO物种的结构，位置和演变将通过原位和Operando实验来监测高级表征技术，包括X射线吸收和高分辨率粉末衍射。 实验数据将与密度功能理论计算相结合，以促进催化剂的结构活性关系以及完全MDA催化循环中涉及的反应途径（激活，反应，反应，失活，再生）。 动力学测试的原位结构表征和理论计算的组合将导致MDA的反应和失活途径的确定，并将为催化剂的合理设计提供基础。 Beyond the research efforts, the investigators will develop a novel virtual reality (VR) technology module that will allow K-12 students to immerse themselves into a catalyst structure and allow them to directly interact with dynamic 3-D images of the molecules involved in a catalytic process.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.