Unraveling Plasma-Assisted Catalysis: Toward Understanding Fundamental Molecule-Surface Interactions and Energy Partitioning Synergisms

拟议的项目旨在探索低温等离子体（LTP）中发生的基本化学，用于旨在去除大气污染物的等离子体辅助催化（PAC）过程。等离子体含有广谱的反应性物质，其可以与催化剂协同作用，以增强对污染物（例如氮氧化物（NOx）和挥发性有机化合物（VOC））的总体消除。然而，这些合作行动的机制并不十分清楚。拟议的工作将联合收割机电子结构计算与多种光谱分析工具相结合，以揭示该系统中发生的反应的复杂性。拟议的研究将结合联合收割机的实验和理论方法来破译能量分配和相互作用的反应，以得出预测的结果。这些研究旨在阐明解决与LTP过程相关的关键基础科学挑战的关键因素，包括确定能量如何在LTP中分配以及活性物质如何在这些系统中形成。在分子水平上，该项目旨在确定基底结构（包括微米和纳米结构）如何影响等离子体-表面相互作用以及等离子体-基底相互作用的机制。拟议的实验将提供强大的实验数据，以改善计算机模型的相关LTP，目前依赖于不完整的数据或外推的信息等离子体属性。一个关键因素是一个全面的方法，连接气相化学与分子表面相互作用，以阐明PAC系统的基本化学与增强性能。空间和时间分辨的吸收和发射光谱沿着质谱将用于探测LTP中化学过程之间的动力学、能量分配和协同作用。 为拟议的研究选择的基板和等离子体处理系统的设计，以提高性能的等离子体催化去除大气污染物。PI在传统上在STEM中代表性不足的指导小组方面有着良好的记录，目前正在努力在科罗拉多州立大学建立一个跨学院、多学科的先进材料发现学院（SAMD）。SAMD将容纳跨学科学位课程，并作为材料相关教育和推广的伞式组织。根据建议的工作，PI和她的学员将进一步开发用于K-12教室和演示的以材料为重点的套件，强调材料化学和等离子体处理。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的知识价值和更广泛的影响审查标准进行评估来支持。

The proposed project seeks to explore the fundamental chemistry occurring in low temperature plasmas (LTPs) used for plasma-assisted catalytic (PAC) processes designed to remove atmospheric pollutants. Plasmas contain a broad spectrum of reactive species that can work synergistically with a catalyst to enhance the overall elimination of contaminants such as nitrogen oxides (NOx) and volatile organic compounds (VOCs). The mechanisms for these cooperative actions, however, are not well understood. The proposed work will combine electronic structure calculations with multiple spectroscopic analysis tools to unravel the complexity of reactions occurring in this system. The proposed research will combine experimental and theoretical approaches to decipher energy partitioning and inter-twined reactions to elicit predictive outcomes. These studies are designed to illuminate key factors that address critical foundational science challenges associated with LTP processes, including determining how energy is partitioned in LTPs and how reactive species are formed in these systems. On a molecular level, the project seeks to determine how substrate architecture (including micro- and nanostructure) affects plasma-surface interactions as well as the mechanisms for plasma-substrate interactions. The proposed experiments will provide robust experimental data to improve computer models of relevant LTPs that currently rely on either incomplete data or extrapolated information for plasma properties. A key element is a comprehensive approach that connects gas-phase chemistry with molecule-surface interactions to elucidate the underlying chemistry in PAC systems with enhanced performance. Spatially- and temporally-resolved absorption and emission spectroscopies along with mass spectrometry will be used to probe dynamics, energy partitioning and synergisms among chemical processes in LTPs. Substrates and plasma processing systems selected for the proposed study are designed to improve performance of plasma-catalytic removal of atmospheric pollutants. The PI has a strong track record of mentoring groups traditionally underrepresented in STEM and is currently leading efforts to establish a cross-college, multidisciplinary School of Advanced Materials Discovery (SAMD) at Colorado State University. SAMD will house interdisciplinary degree programs and serve as an umbrella organization for materials-related education and outreach. Based on the proposed work, the PI and her trainees will further develop materials-focused kits for use in K-12 classrooms and demonstrations that emphasize materials chemistry and plasma processing.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.