EFRI DCheM: One-step conversion of CH4 and CO2 to liquid fuels with the use of a multi-functional pseudo catalytic system

由于运输成本过高和储层规模小等经济限制，目前搁浅的天然气资源都是燃烧的。成功地将这些偏远分布的天然气资源转化为有用的能源产品，将对美国的能源经济和能源安全做出重大贡献。该项目的目标是开发一个小型模块化化学处理系统，将搁浅的天然气和二氧化碳转化为增值的液体燃料产品。所提出的这项技术具有变革性和环境可持续性，因为它既可以实现搁浅天然气资源的货币化，又可以在天然气转化过程中消耗二氧化碳作为原料。研究人员是俄亥俄州立大学（OSU）的教职员工，他们将使用数据驱动的方法集成反应器系统组件，并将通过确定有效的催化剂来促进反应，进一步了解气体升级化学的基本知识。这个跨学科的俄勒冈州立大学项目团队将与工业合作伙伴Velocys公司和Jan Lerou公司合作，利用他们的工业专业知识，使用先进的制造协议和最先进的计算工具来优化系统设计。 提议的项目 将促进对液体燃料转化过程的基本理解，并为K-12、本科生和研究生提供多种学习经验。该项目团队将与当地高中合作，促进将代表性不足的学生纳入其研究活动。本计划所产生的 基础知识 也将作为本科和研究生教育的科学、工程和技术导向的学习资源。提出的工作解决了建立热催化燃烧气重整（TC-FGR）系统以货币化搁浅天然气资源的技术和科学障碍。TC-FGR系统是一种小型模块化GTL（气转液）工艺，可加强天然气合成气的生产，并将商业演示的微通道F-T（费托合成）系统集成在一个反应堆容器中。此外，将开发一种新型的伪催化金属氧化物（PMO）材料，以减少传统小型F-T系统所需的单元操作。研究小组将使用第一性原理计算方法和实验参数测试来开发PMO材料。该团队还将开发一种机器学习信息集成、灵活的反应堆设计，以加强模块化GTL系统，并将评估拟议技术的经济可行性。PMO是一种铁基金属氧化物复合材料，能够表现出多种氧化态，允许CH4与PMO反应，提取晶格氧形成部分燃烧产物CO和H2。同时，CO2/H2O再氧化PMO生成额外的CO/H2。PMO作为氧介质的独特活化为工艺优化增加了额外的自由度，提高了合成气的生产率，并提供了一种控制其组成的方法。该项目的工业合作伙伴采用独特的微通道设计，增强了传热传质能力；再加上高活性催化剂，其生产效率是传统F-T系统的10-15倍。该项目将在每个项目步骤中协同使用多尺度模型和先进的优化/控制方法，以确保增强型TC-FGR系统在经济边际较小的分布式应用中是可行的。由此产生的集成模块化TC-FGR系统可以部署在几口井中，为目前浪费的天然气燃烧提供了一种革命性的替代方案。TC-FGR搁浅气工艺的广泛应用将通过二氧化碳转化进一步减少温室气体排放。TC-FGR等可持续技术为减少化石燃料的碳足迹搭建了一座桥梁。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。

Stranded natural gas resources are currently flared due to economic limitations associated with prohibitive transportation costs and small reservoir sizes. Successfully transforming these remotely distributed gas resources to useful energy products will contribute significantly to the U.S. energy economy and its energy security. The goal of this project is to develop a small-scale modular chemical processing system to convert stranded natural gas and carbon dioxide into value-added liquid fuel products. This technology as proposed is transformative and environmentally sustainable as it will achieve both the monetization of stranded gas resources and will consume carbon dioxide as a feedstock in the gas conversion process. The researchers are Ohio State University (OSU) faculty members who will use a data-driven approach to integrate the reactor system components and will further the fundamental understanding of the gas upgrading chemistry by identifying an efficient catalyst to promote the reactions. This interdisciplinary OSU project team will work with industrial partners Velocys, Inc. and Jan Lerou LLC. to leverage their industrial expertise to optimize the system design using an advanced manufacturing protocol and state-of-the-art computational tools. The proposed project will advance fundamental understanding of liquid fuel conversion processes as well as provide multiple learning experiences for K-12, undergraduate, and graduate students. The project team will work with local high schools to promote the inclusion of under-represented students in its research activities. The foundational knowledge generated by this project will also serve as a science, engineering, and technology-oriented learning resource for undergraduate and graduate education. The proposed work addresses the technological and scientific barriers to building a thermo-catalytic flared-gas reforming (TC-FGR) system for monetizing stranded gas resources. The TC-FGR system is a small-scale, modular GTL (gas to liquid) process that intensifies syngas production from natural gas and integrates a commercially demonstrated micro-channel F-T (Fischer-Tropsch) synthesis system in one reactor vessel. Furthermore, a novel pseudo-catalytic metal oxide (PMO) material will be developed to reduce the unit operations required for conventional small-scale F-T systems. The research team will develop the PMO material using first-principles computational methods and experimental parametric testing. The team also will develop a machine learning-informed integrated, flexible reactor design that intensifies modular GTL systems and will assess the economic feasibility of the proposed technology. The PMO is an iron-based metal oxide composite, capable of exhibiting several oxidation states, that allows CH4 to react with the PMO, abstracting the lattice oxygen to form partial-combustion products CO and H2. At the same time, CO2/H2O re-oxidizes the PMO forming additional CO/H2. This unique activation with the PMO acting as the oxygen mediator adds additional degrees of freedom for process optimization, enhancing the production rate of syngas as well as providing a means of controlling its composition. The unique microchannel design used by the industrial partner of this project results in enhanced heat and mass transfer capabilities; this coupled with a highly active catalyst allows for productivity that is 10-15 times higher than conventional F-T systems. The project will synergistically use multi-scale models and advanced optimization/control methods at every project step to ensure that the intensified TC-FGR system is viable in distributed applications with small economic margins. The resulting integrated, modular TC-FGR system can be deployed over several wells, providing a transformative alternative to the wasteful gas flaring that is current practice. Widespread applications of the TC-FGR stranded gas process will further mitigate greenhouse gas emissions through carbon dioxide conversion. Sustainable technology such as TC-FGR constitutes a bridge towards reducing the carbon footprint of fossil fuels.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.