Bulletin of the American Physical Society
75th Annual Gaseous Electronics Conference
Volume 67, Number 9
Monday–Friday, October 3–7, 2022;
Sendai International Center, Sendai, Japan
The session times in this program are intended for Japan Standard Time zone in Tokyo, Japan (GMT+9)
Session FT2: Plasma Chemical Synthesis and Conversion |
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Chair: Masaharu Shiratani, Kyushu University Room: Sendai International Center Shirakashi 1 |
Tuesday, October 4, 2022 10:00AM - 10:15AM |
FT2.00001: Self-limiting trade-off between CO yield and CO2 conversion energy efficiency in atmospheric pressure radio-frequency plasmas: picosecond laser spectroscopy James Dedrick, Alex Foote, Andrew R Gibson, Kari Niemi, Steven Thomas, Jüri Raud, Joshua Boothroyd, Zaenab Abd-Allah, Jérôme Bredin, Michael North, Deborah O'Connell, Timo Gans Non-thermal atmospheric pressure plasmas are of interest for producing CO from CO2. We have measured ground-state CO and O densities in rf driven argon and helium plasmas admixed with CO2 using picosecond two-photon absorption laser induced fluorescence. CO and O densities in the far-effluent show quantitative agreement with Fourier-transform infrared spectroscopy, enabling the study of CO yield and CO2 conversion energy-efficiency with respect to CO2 admixture and total flow rate. The CO density increases with distance from the outlet, which can be explained in terms of electron power deposition into CO vibrational states and self-limiting trade-off between the yield and energy efficiency in high-conversion regimes. |
Tuesday, October 4, 2022 10:15AM - 10:30AM |
FT2.00002: Thermocatalytic Plasma-Assisted Dry Reforming of Methane Over Heterogeneous Ni/Al2O3 Catalyst. Tyler Wong, Daniel E Guerrero, Setrak Tanielyan, Jose L Lopez A very promising area of plasma catalysis is the dry reforming of methane, whose symbiotic use of CH4 and CO2 mitigates the environmental impact of both greenhouse gases by transforming them into valuable syngas which can be used to produce petrochemicals. Because of the high carbon content in the feedstocks and harsh industrial reaction conditions, the dry reforming of methane is prone to coke formation, making the catalyst deactivation a severe problem for larger-scale industrial applications. |
Tuesday, October 4, 2022 10:30AM - 11:00AM |
FT2.00003: The role of reactive oxygen and nitrogen species on the conversion of volatile organic compounds in a twin surface dielectric barrier discharge Invited Speaker: Lars Schücke In consideration of the increasing consciousness for environmental protection, energy efficient processes for the purification of exhaust gas streams, e.g. in industrial plants, are growing in demand. These gas streams can be contaminated with pollutants such as fine particles, volatile organic compounds (VOCs), and various microorganisms, depending on the industry and application. |
Tuesday, October 4, 2022 11:00AM - 11:15AM |
FT2.00004: Nonthermal plasma assisted CO2 hydrogenation over intermetallic Pd2Ga/SiO2 Daeyeong Kim, Shinya Furukawa, Tomohiro Nozaki Coupling nonthermal plasma (NTP) with heterogeneous catalysis has been applied in C1 chemistry and is attracting more attention as an alternative to conventional thermal catalysis.1, 2 However, the fundamental reaction pathway in NTP-activated CO2 hydrogenation has not been fully explored and are still not clear. Here, we investigated the NTP-assisted CO2 hydrogenation in Pd2Ga/SiO2 catalyst and compared to thermal catalysis. To gain mechanistic insight between NTP-activated species and intermetallic catalysts, we performed in situ transmission IR spectroscopy. In addition, chemical and structure transition of catalysis during NTP-activated CO2 hydrogenation were conducted by in situ X-ray absorption fine structure (XAFS) analysis. In situ characterizations indicate that NTP-assisted CO2 hydrogenation improved compared to thermal catalysis. In particularly, bending mode of vibrationally-excited CO2 can react with hydrogen adsorbed on the catalyst surface to promote formate formation. This work provides a fundamental mechanism for the interacting NTP-activated species and intermetallic catalysts and sheds light on the rational design of NTP-assisted catalysis. |
Tuesday, October 4, 2022 11:15AM - 11:30AM |
FT2.00005: Reaction Mechanism for the Atmospheric Pressure Plasma Jet Treatment of Cysteine in Solution Jordyn Polito, Sanjana J Kerketta, María J Herrera Quesada, katharina Stapelmann, Mark J Kushner Atmospheric-pressure-plasma-jets (e.g., KINpen, COST-jet) are a source of reactive oxygen and nitrogen species (RONS) for applications in biology and medicine. Recent fundamental investigations utilizing these devices have focused on plasma-liquid interactions of RONS with simple biologically-relevant amino acids (e.g., cysteine, glycine) in solution. Experimental studies have shown RONS are depleted in reactions with simple amino acids in solution, producing oxidation products that are similar to those formed by treatment of organic molecules with gas-phase plasmas [1]. Reaction mechanisms for plasma-liquid interactions are generally available for solutions that do not contain organic molecules and materials. Development of these mechanisms based on analogous reactions of gas-phase plasmas with organic molecules could provide insight for biological applications. |
Tuesday, October 4, 2022 11:30AM - 11:45AM |
FT2.00006: Plasma catalysis in fluidized-bed reactor for reverse water gas shift reaction Xiaozhong Chen, Shinya Furukawa, Tomohiro Nozaki Plasma catalysis for valorization of gas, i.e., CO2, is attracting increasing attention. High value-added chemicals, i.e., CO, CH3OH, are possible to be formed under mild conditions. However, plasma-catalyst interaction is typically limited in conventional packed-bed DBD reactors. Herein, a fluidized-bed DBD reactor was newly proposed. Powdered catalyst was fluidized directly in plasma, yielding an enhanced plasma-catalyst coupling and heat transfer. Reverse water gas shift reaction over Pd2Ga/SiO2 was selected as a model, by which we confirmed plasma catalysis yielded more than doubled CO2 conversion compared to thermal catalysis. Further promotion was achieved by increasing discharge frequency, where, interestingly, we found thermal equilibrium was well beyond. Meanwhile, linear Arrhenius behavior for plasma catalysis was experimentally obtained, by which a dramatic decrease of activation energy from 75 kJ/mol of thermal to 43 kJ/mol was observed. Lissajous plot analysis and electron collision kinetics further suggested increasing low-energy electron concentration is the key, where vibrational excitation contributed to a kinetically and thermodynamically favored CO2 conversion. A green plasma technology assisted by catalysis for energy conversion was developed successfully. |
Tuesday, October 4, 2022 11:45AM - 12:00PM |
FT2.00007: Powderization behavior of uranium dioxide solid by non-equilibrium plasma oxidation ZhuoRan Ma, Takaharu Tatsuno, Yoshiya Homma, Kenji Konashi, Tatsuya Suzuki The amounts of actinide and isotope ratios of actinides in the nuclear fuel debris from the Fukushima accident are required to known for the determination of the plan of the treatment and disposal of nuclear fuel debris. For these analyses, the dissolution of debris, and the nuclide separation are necessary. |
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