EFRI DCheM: Engineering Interfaces between Plasma, Catalysts, and Reactor Design for Natural Gas Conversion to Liquid Products

传统的大型化工厂和炼油厂严重依赖高温催化将碳氢化合物原料转化为燃料和化学品。这些过程需要大量的能源，通常由天然气燃烧提供，同时产生大量的二氧化碳。该项目研究了另一种方法——等离子体催化——它可以由可再生电力提供动力，并设计成能够从搁浅和燃烧的天然气中分布式生产化学品和液体燃料。该项目将普林斯顿大学、南卡罗来纳大学和斯坦福大学的研究人员与催化、等离子体物理和化学以及纳米制造方面的专业知识结合起来，与国家实验室和行业合作，提供各种研究和教育计划，培养未来美国能源和工程科学与技术领域的领导者和创新者。该项目得到了一个扩大参与计划的支持，以吸引代表性不足的少数民族学生（如高中生、本科生和研究生）参加暑期校园学习计划、工业实习和论文研究。这种强调与团队的教育目标一致，即为从高中到大学和高级学位的学生创造一条科学和工程方面的管道。此外，与国家实验室和工业的合作以及中心咨询委员会和工业联盟的成立将促进创新和技术向市场的转移。来自太阳能和风能的可再生电力为使用低温、非平衡大气雾状等离子体催化的分布式反应堆提供了前所未有的机会。该项目的总体目标是研究等离子体辅助催化甲烷转化为高阶液态碳氢化合物和含氧燃料和化学品。解决的主要挑战是：(i)理解等离子体催化中物质的非平衡能量转移和转化；（ii）确定稳定等离子体而不影响其效率的方法；（iii）等离子体特性与化学转化的催化活性、选择性和稳定性之间的协调；（iv）为新型等离子体催化剂和反应器协同设计开发实验验证的预测动力学和输运模型；阐明优化等离子体和催化剂集成的反应器设计和制造标准。这些研究将通过对非平衡等离子体特性、激发态和化学进行先进的激光诊断，并通过开发实验验证的等离子体化学和等离子体催化中物质转化的预测多尺度建模工具，推进对等离子体催化的基本理解。此外，混合等离子体控制、催化剂设计和增材制造的元素将被用于开发一种创新的微气溶胶等离子体催化反应器（MAPCAR），作为一种模块化设备，能够将大量的原料（如滞留天然气和二氧化碳）高效和选择性地转化为液体燃料和含氧化学前体。时间分辨同步等离子体特性和化学诊断将被用来加强对非平衡等离子体状态、能量转移、化学动力学和等离子体催化中物质转化的基本理解。这些数据将用于开发和实验验证模型以及用于MAPCAR优化的多尺度等离子体催化建模工具。该研究不仅将促进对等离子体催化基本物理和化学过程的科学认识，而且还将为等离子体催化设计提供新的预测工具，为实现均匀大气等离子体提供新的控制方法，并为制造用于化学处理的分布式等离子体催化反应器提供新技术。该奖项反映了美国国家科学基金会的法定使命，并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，被认为值得支持。

Traditional large-scale chemical plants and refineries rely heavily on high-temperature catalysis to transform hydrocarbon feedstocks to fuels and chemicals. Such processes carry high energy demands, which are typically provided by natural gas combustion with a large associated generation of CO2. This project investigates an alternative approach – plasma catalysis – that can be powered by renewable electricity and engineered to enable distributed production of chemicals and liquid fuels from otherwise stranded and flared natural gas. This project combines researchers at Princeton University, University of South Carolina, and Stanford University with expertise in catalysis, plasma physics and chemistry, and nanomanufacturing with national laboratories and industry to provide a variety of research and educational initiatives that will nurture future U.S. leaders and innovators in energy and engineering sciences and technology. The project is supported by a broadening participation plan to attract underrepresented minority (URM) students (e.g. high-school, undergraduate, and graduate students) for summer on-campus learning programs, industrial internships, and thesis research. Such emphasis aligns with the team’s educational goal of creating a pipeline in science and engineering for students from high school through college and advanced degrees. Further, collaborations with national laboratories and industry and the formation of the Center Advisory Board and Industrial Consortium will facilitate the innovation and technology transfer to market. Renewable electricity from solar and wind provides unprecedented opportunities for distributed reactors using low-temperature, non-equilibrium atmospheric misty plasma catalysis. The overarching project goal is to investigate the plasma-assisted catalytic conversion of methane to higher-order liquid hydrocarbons and oxygenated fuels and chemicals. Key challenges addressed are: (i) understanding non-equilibrium energy transfer and transformation of matters in plasma catalysis; (ii) identifying methods to stabilize plasma without impacting its efficiency; (iii) coordination between plasma properties and catalytic activity, selectivity, and stability in chemical conversion; (iv) development of experimentally validated, predictive kinetic and transport models for novel plasma catalysts and reactor co-design; and (v) elucidating reactor design and manufacturing criteria that optimize plasma and catalyst integration. The studies will advance fundamental understanding of plasma catalysis by conducting advanced laser diagnostics of non-equilibrium plasma properties, excited states, and chemistry, and by developing experimentally validated predictive multiscale modeling tools for plasma chemistry and transformation of matter in plasma catalysis. Moreover, elements of hybrid plasma control, catalyst design, and additive manufacturing will be employed to develop an innovative micro-aerosol plasma catalytic reactor (MAPCAR) as a modular device to enable efficient and selective conversion of abundant feedstocks such as stranded natural gas and CO2, to liquid fuels and oxygenated chemical precursors. Time-resolved simultaneous plasma properties and chemistry diagnostics will be employed to enhance fundamental understanding of the non-equilibrium plasma states, energy transfer, chemical kinetics, and transformation of matters in plasma-catalysis. The data will be used to develop and experimentally validate models and multiscale plasma catalysis modeling tools for MAPCAR optimization. The research will not only advance the scientific understanding of the elementary physical and chemical processes in plasma catalysis, but also develop a new predictive tool for plasma catalysis design, new control methods for achieving uniform atmospheric plasma, and new techniques to manufacture distributed plasma catalytic reactors for chemical 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.