Collaborative Research: A New Class of Chemical Potential Driven Plug Flow Membrane Reactors for Combined Gas Separation and Direct Natural Gas Conversion

页岩革命使大量生产低成本天然气成为可能。这些资源的大部分仍在燃烧以取暖和发电，向大气中释放二氧化碳，进一步加重了碳捕获努力的负担。同时，由于低成本天然气带来的潜在利润率，直接将天然气转化为有价值的化学品受到了学术界和工业界的极大关注。这项研究项目旨在利用一种新型的化学势驱动(无电)、陶瓷基催化推流膜反应器(PFMR)作为平台，进一步了解与二氧化碳捕获、天然气转化机理和催化剂开发有关的基础科学知识。将气体分离和天然气转化统一在一个反应器中，以提高能源效率和成本效益。正在进行的二氧化碳捕获和天然气转化技术的科学进步的重要性和潜在影响将在南卡罗来纳大学(USC)的年度“爱迪生系列讲座”节目中向公众展示。南加州大学将与本尼迪克特学院合作，举办一次关于能源研究主题的联合夏季研讨会，以促进STEM领域代表性不足的学生的教育和劳动力发展。本尼迪克特学院工程专业的本科生将通过提供暑期实习和学年兼职工作，以及获得南加州大学和马萨诸塞大学洛厄尔分校(UML)现有的本科课程，从事这些研究课题。两门关于气体分离/转化和电化学系统计算分析的新课程将独立开发，并为南加州大学和联合大学的研究生提供。本研究项目旨在开发两种特定类型的全氟化氢化合物。第一种是基于碳酸盐离子、氧化物离子和电子导体的三重体系，在这个反应器中，甲烷将在合适的催化剂存在下，利用共捕获的二氧化碳/氧气混合物进行催化氧化偶联，将天然气转化为乙烯。第二种类型的PFMR是基于一个三氧离子、质子和电子导体，在这个反应器中，甲烷的催化非氧化脱氢将与同时提取氢以将天然气转化为乙烯。对于这两种PFMR，从进料侧流入的二氧化碳和/或氧气有助于显著减少结焦，从而延长膜/催化剂的寿命。该项目的基本组成部分包括通过实验和理论相结合的方法开发新的膜组合物和特定于转化的催化剂/载体。将使用同位素交换技术和原位拉曼光谱研究控制甲烷氧化和非氧化转化以及焦炭形成的基本机制，并将通过内部催化反应器、多物理和系统建模来进行PFMR的设计、测试和建模。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

The shale revolution has enabled large volume production of low-cost natural gas. The majority of this resource is still being burned for heat and power, releasing carbon dioxide into the atmosphere and further burdening carbon capture efforts. Meanwhile, directly converting natural gas into valuable chemicals has received significant interest from academia and industry due to the potential profit margin brought by low-cost natural gas. This research project aims to further fundamental scientific knowledge related to carbon dioxide capture, natural gas conversion mechanisms, and catalyst development using a new class of chemical-potential driven (electricity-free), ceramic-based, catalytic plug flow membrane reactors (PFMRs) as a platform. The gas separation and natural gas conversion are unified in a single reactor to be energy efficient and cost-effective. The importance and potential impact of the ongoing scientific advances in carbon dioxide capture and natural gas conversion technologies will be presented to the public during the annual "Edison Lecture Series" program at the University of South Carolina (USC). USC will team up with Benedict College to host a joint summer workshop on energy research topics to promote education and workforce development for students underrepresented in STEM fields. Undergraduate students at Benedict College in engineering majors will be engaged in these research topics by offering summer internships and academic-year part-time jobs, along with having access to USC's and University of Massachusetts at Lowell's (UML) existing undergraduate programs. Two new courses on the topics of gas separation / conversion and computational analysis for electrochemical systems will be independently developed and offered for graduate students at both USC and UML. This research project seeks to develop two specific types of PFMRs. The first is based on a triple carbonate-ion, oxide-ion and electron conductor, and within this reactor the catalytic oxidative coupling of methane will take place using the co-captured carbon dioxide / oxygen mixture to convert natural gas into ethylene in the presence of a suitable catalyst. The second type of PFMR is based on a triple oxide-ion, proton and electron conductor, and within this reactor the catalytic non-oxidative dehydrogenation of methane will be undertaken with the concurrent extraction of hydrogen to convert natural gas into ethylene. For both PFMRs, the influx of carbon dioxide and / or oxygen from the feed side helps significantly mitigate coke formation, thus prolonging the membrane / catalyst life. The fundamental components of the project include developing new membrane compositions and conversion-specific catalysts / supports through a combined experimental and theoretical approach. The fundamental mechanisms governing the methane oxidative and non-oxidative conversions and coke formation will be studied using an isotopic exchange technique and in situ Raman spectroscopy, and the design, testing and modeling of PFMRs via in-house catalytic reactors, multiphysics and system modeling will be performed.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.