Nano-ceria shape effects on non-equilibrium plasma-catalysis for chemical looping CO2 reuse

非平衡等离子体，也称为低温等离子体，具有高反应性，可用于催化化学过程。 化学循环过程可以将天然气转化为电力，液体燃料，氢气或化学品，同时捕获二氧化碳（CO2）。 利用非平衡态等离子体催化（NEPC）进行化学循环和甲烷处理，可以对能源转换基础设施产生全球性影响，如化学合成的小型反应器、发电厂、气液转化技术、石油勘探和燃料电池等。（如棒状、立方体、八面体和纤维）的氧化铈负载的催化剂（CuOx和RuOx）在非平衡低温等离子体增强化学链制氢中的性能和选择性，使用CO2，水和天然气作为原料。拟议的研究可能会导致经济上可行的方法，用于从发电厂直接获得的二氧化碳，水和天然气原料合成可持续燃料，从而提供化石燃料的替代品，同时减少温室气体排放。拟议的研究将测试以下假设：含有振动和电子激发的物种/自由基/热电子等与负载在不同二氧化铈纳米形状上的金属氧化物催化剂一起可以协同地增强多相反应，导致低温性能和产物的选择性，所述产物可以包括合成气（CO+H2）和较大的烃（C2 H4、C2 H6、C2 H2）和氧化循环期间的H2。等离子体-催化协同作用可以提高低温下的产率，并且还导致对产物选择性的催化剂设计的理解。例如，等离子体可以在低温下将CH 4解离成CH 3 +H。通过在催化剂或界面上的正确对接位点，两个CH 3自由基可以在失去H2后联合收割机形成C2 H4。利用太阳能或风能可以维持射频放电等离子体，并可以开发新型的高效表面放电技术。拟议的外展计划将针对亚拉巴马农村的教师和学生，以增加代表性不足的少数民族学生参与科学和工程研究。该项目由过程系统公司联合资助，反应工程和分子热力学以及刺激竞争研究的既定计划（EPSCoR）该奖项反映了NSF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。

Non-equilibrium plasmas, also known as low-temperature plasmas, are highly reactive and can be used in catalytic chemical processes. Chemical looping processes can convert natural gas into electricity, liquid fuels, hydrogen, or chemicals while providing capture of carbon dioxide (CO2). The use of non-equilibrium plasma-catalysis (NEPC) for chemical looping and methane processing can have a global impact on energy conversion infrastructure such as small-scale reactors for chemical synthesis, power plants, gas-to-liquid technology, oil exploration, and fuel cells, etc. This project will study the shape effects (such as rods, cubes, octahedra, and fibers) of ceria-supported catalysts (CuOx and RuOx) on performance and selectivity in non-equilibrium low-temperature plasma-enhanced chemical looping hydrogen production from water, using CO2, water and natural gas as feedstock. The proposed research could lead to economically viable approaches for synthesis of sustainable fuels from CO2 obtained directly from power plants, water and natural gas feedstock, thus providing alternatives to fossil fuels while mitigating greenhouse gas emissions.The proposed research will test the hypothesis that gaseous non-equilibrium low temperature plasma containing vibrationally and electronically excited species/radicals/hot electrons etc. together with the metal oxide catalysts supported on different ceria nano-shapes can synergistically enhance heterogeneous reactions leading to low temperature performance and selectivity in products which can include syngas (CO+H2) and larger hydrocarbons (C2H4, C2H6, C2H2) during the reduction cycle and H2 during the oxidation cycle. The plasma-catalysis synergy can enhance the yield at low temperatures and also lead to understanding towards catalyst design for product selectivity. For example, the plasma can dissociate CH4 to CH3+H at low temperatures. With the right docking sites on catalysts or interfaces, two CH3 radicals can combine to form C2H4 after losing H2. The RF discharge plasma can by sustained using solar energy or wind energy and novel high efficiency surface discharge techniques can be developed. The proposed outreach program will be aimed at teachers and students in rural Alabama to increase participation of underrepresented minority students in science and engineering research.This project is jointly funded by Process Systems, Reaction Engineering and Molecular Thermodynamics and the Established Program to Stimulate Competitive Research (EPSCoR).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.