Bulletin of the American Physical Society
76th Annual Gaseous Electronics Conference
Volume 68, Number 9
Monday–Friday, October 9–13, 2023; Michigan League, Ann Arbor, Michigan
Session HW1: Plasma Chemical Synthesis and Conversion |
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Chair: Yiguang Ju, Princeton University Room: Michigan League, Michigan |
Wednesday, October 11, 2023 8:00AM - 8:15AM |
HW1.00001: Exploring the Fundamentals of Catalyst Development in Non-Thermal Plasma CO2 Hydrogenation for Sustainable Aviation Fuels Stefano Dell'Orco, Nico Dwarica, Susan Habas, Noemi Leick, Hariswaran Sitaraman, Daniel Ruddy, Calvin Mukarakate Sustainable aviation fuels (SAFs) are crucial for achieving GHG emission reduction targets by 2050. The SAF Grand Challenge in the US aims to produce 35 billion gallons of SAF annually, while the ReFuelEU Aviation initiative in the EU proposes to mandate airports to supply 70% of SAF. E-fuels have emerged as a promising solution for decarbonizing the aviation sector by using renewable electricity, green H2, and CO2 to produce synthetic fuels. Among pathways at lower TRL, non-thermal plasma (NTP) has the potential to enable thermodynamically unfavorable reactions by energizing electrons. However, NTP CO2 hydrogenation requires catalysts to tune reactions towards selective hydrocarbon formation. Currently, there is still a lack of fundamental understanding of how catalyst properties influence conversion, selectivity, and yields under NTP conditions. Our work aims to improve understanding of the catalysts structure-function relationship in NTP CO2 hydrogenation through experiments and computational models. To this end, we employ point-source DBD in a packed-bed DRIFTS cell for in-operando measurements of surface species. NTP CO2 hydrogenation over modified metal oxides and zeolites has exhibited activity in CO and CHx formation on the catalyst surfaces at lower temperatures. These observations are key to understanding the interrelatedness of NTP and catalyst properties, as well as establish an initial pathway for future optimized catalyst design to enhance conversion and hydrocarbon selectivity. |
Wednesday, October 11, 2023 8:15AM - 8:30AM |
HW1.00002: Plasma assisted dry reforming of methane: Syngas and hydrocarbons formation mechanisms. Manuel Oliva Ramirez, Paula Navascués, José Cotrino, Agustín Rodríguez González-Elipe, Ana M Gómez-Ramírez |
Wednesday, October 11, 2023 8:30AM - 8:45AM |
HW1.00003: Kinetics of High-Pressure CO2 Splitting in Nanosecond Pulsed Discharges Hongtao Zhong, Taemin Yong, Mark A Cappelli We investigate CO2 splitting using nanosecond repetitively pulsed discharges (NRP) in a high-pressure (5-12 bar) batch reactor. Product species were measured using gas chromatography. The yield and energy efficiency were determined for a range of processing times, pulse energy, and fill pressures. A zero-dimensional kinetic model was developed to understand the key reaction pathways for CO2 conversion. Experimental results reveal, for long processing times, a saturation in yield and drop in efficiency, attributed to the increasing role of three-body recombination reactions. Detailed modeling reveals the presence of three-stage kinetics between pulses, controlled by electron-impact CO2 dissociation, vibrational relaxation, and reversible neutral elementary kinetics. Transport effects are shown to be important at high pressures. Enhancing mixing at high pressures can avoid dissociating generated CO and increase efficiency. For fill pressures beyond 10 bar, CO2 may transit into local supercritical states, where the plasma kinetics may bypass atomic oxygen pathways and directly convert CO2 into O2. This work provides an analysis of plasma-based high-pressure CO2 conversion, which is of great relevance to future large-scale sustainable carbon capture, utilization, and storage. |
Wednesday, October 11, 2023 8:45AM - 9:00AM |
HW1.00004: Kinetics of CO2/N2 Discharges Investigated by Laser Diagnostics Christian A Busch, Nikita D Lepikhin, Jan Kuhfeld, Tsanko V Tsankov, Dirk Luggenhölscher, Uwe Czarnetzki
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Wednesday, October 11, 2023 9:00AM - 9:15AM |
HW1.00005: Solving Multi-Scale Plasma Chemistry Using Physics-Informed Neural Network Li Lin, Sophia Gershman, Yevgeny Raitses, Michael Keidar Cold atmospheric plasma (CAP) is a non-thermal plasma exposed in the open air, which is now applied to cancer therapy, wound treatment, sterilizations, agriculture, air and water purification, etc. All these applications are intensively relying on CAP chemistry, especially the reactive oxygen and nitrogen species. However, due to the complexity of CAP chemistry which contains hundreds of species and thousands of dynamic chemical reactions, it is challenging to measure the full picture of species concentrations through experiments. Numerical simulations are also at high computational cost because of the sub-nanosecond time scale of inelastic collisions (chemical reactions) compared with the millisecond to the minutes time scale of the CAP working period. Therefore, we developed physics-informed data-driven modeling to solve such a multi-scale problem using modern machine learning techniques. The physics-informed neural network (PINN) is trained under the constraints of chemical rate equations with a complete kinetic scheme, conservation laws, and the experimental measurement of a few species concentrations. After the training, PINN can provide us with the full picture of all the species' concentrations which agrees with the physical laws and observations in reality. In other words, an experiment and machine learning-assisted numerical simulation is developed, as a general method that can solve a multi-scale problem of microscopic plasma chemistry coupling with macroscopic gas flows. |
Wednesday, October 11, 2023 9:15AM - 9:30AM |
HW1.00006: Understanding Temperature Inhibition of Methane Conversion in DBD Plasma Systems Ibukunoluwa Akintola, Gerardo Rivera-Castro, Jinyu Yang, Jeffrey Secrist, Jason C Hicks, Felipe Veloso, David B Go Low-temperature non-thermal plasmas (LTPs) are known to produce highly reactive chemical environments. The combination of these reactive species with a catalyst can help drive thermodynamically unfavorable reactions and produce a synergistic conversion effect. There is appreciable promise in the direct coupling of methane (CH4) with nitrogen (N2) to produce value-added chemicals using plasma catalysis. In order to create effective plasma catalytic systems, it is important to understand the fundamentals of plasma-phase chemistry alone. Much research has gone into understanding how certain operating conditions affect the plasma, but there is limited knowledge of how bulk reaction temperature affects the plasma and ensuing plasma chemistry. In this work, we use a dielectric barrier discharge (DBD) to investigate the effects of operating conditions, specifically temperature, on the chemical transformation of methane species and correlate these to the plasma’s electrical and optical properties in various methane-gas mixtures. Results show an increase in temperature leads to a reduction in the conversion of methane. This can be attributed to two possible causes: an increase in the conductivity of the gas prior to plasma ignition affecting plasma electrical properties and changes to the thermal chemical reaction kinetics. Both situations then lead to a plasma environment where methane conversion is limited. We also observe a positive correlation between key electrical plasma properties (average charge and lifetime per filament) and conversion at various operating conditions, which provide insight into a relationship between plasma properties and chemical transformations. |
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