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，具有很强的反应性，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，同时提供二氧化碳的捕获。非平衡等离子体催化（NEPC）用于化学环和甲烷处理可以对能量转换基础设施产生全球性影响，例如用于化学合成的小型反应堆、发电厂、气转液技术、石油勘探和燃料电池等。该项目将研究铈载体催化剂（CuOx和RuOx）的形状（如棒状、立方体、八面体和纤维）对非平衡低温等离子体增强化学环水中制氢的性能和选择性的影响，以二氧化碳、水和天然气为原料。拟议的研究可能会导致经济上可行的方法，从直接从发电厂、水和天然气原料中获得的二氧化碳合成可持续燃料，从而提供化石燃料的替代品，同时减少温室气体排放。拟议的研究将测试假设气体非平衡低温等离子体包含之电子和电子兴奋物种/自由基/热等一起支持的金属氧化物催化剂在不同二氧化铈nano-shapes可以协同增强异构反应导致产品低温性能和选择性可以包括合成气(CO + H2)和更大的碳氢化合物(C2H4 C2H6,还原循环中的C2H2和氧化循环中的H2。等离子体-催化协同作用可以提高低温下的产率，也有助于对产物选择性催化剂设计的理解。例如，等离子体可以在低温下将CH4分解成CH3+H。如果在催化剂或界面上有合适的对接位点，两个CH3自由基可以在失去H2后结合形成C2H4。射频放电等离子体可以持续利用太阳能或风能，可以开发出新的高效表面放电技术。拟议的推广计划将针对阿拉巴马州农村地区的教师和学生，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、反应工程和分子热力学以及促进竞争研究的既定计划（EPSCoR）共同资助。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。

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.