7th Asia-Pacific Conference on Plasma Physics, 12-17 Nov, 2023 at Port Messe Nagoya

Investigation of synergic response on low temperature plasma catalytic C1
conversion for the production of platform chemicals
Yuan Gao1, Liguang Dou1, Bin Li1, Yuxuan Xu1, 2, Tao Shao1, 2*1
Beijing International S&T Cooperation Base for Plasma Science and Energy Conversion, Instituteof Electrical Engineering, Chinese Academy of Sciences
2
University of Chinese Academy of Sciencese-mail (speaker): yuangao@mail.iee.ac.cn
CH4, the major feedstock in platform chemicals
synthesis and hydrogen production, has gradually drawn
energy safety and environmental concerns in fossil fuelutilization owing to its rapid increase in global demand[1]. Under the goal of carbon neutralization, it is anurgent need to develop environmental-friendly
approaches of in-situ CH4 conversion to platformchemicals at mild condition with high energy andresources utilization efficiency.
The Non-thermal plasma (NTP) technology ishighlighted as a promising new frontier to overcome theabove challenges associated with its non-equilibrium
characters, it could be easy to activate the chemicallyinert gases (CH4, CO2, etc.) at room temperature andatmospheric pressure with the energetic electrons. Basedon application background of the distributed clean
energy and natural gas in-situ utilization, this talkfocuses on the plasma enabled C1 conversion forvalue-added chemicals. Several plasma sources are
employed to directly convert the CH4 into platformchemicals (e.g. syngas, CH3OH, C2+ alcohols) withspecialized plasma reactor.
Firstly, this talk aims at the regulating effects of pulsed
parameters on the discharge properties, transient species
evolution and the gaseous products distribution inplasma enabled CH4 dry reforming process, while themaximum conversion of CH4 and CO2 could respectively
arrive at 39.6% and 22.9%. The result showed that shortpulse rise & fall times promoted CH4 and CO2
conversions, as well as the energy conversion
efficiencies [2].
Secondly, this talk will introduce a promising plasma
approach for the partial oxidation of CH4 into hydrogenand value-added oxygenates (alcohol, acetic acid, andaldehydes) using the dielectric barrier discharge,achieving the maximum H2 selectivity (46.3%) and totalliquid selectivity (76.8 %) under different operating
conditions [3]. An adjustable pulsed power source wasemployed to directly convert CH4 into hydrogen andliquid chemicals with the addition of specializedgaseous/aqueous contents. Thus, the parameterized
pulsed discharge allowed us to subtly customize theoxidation within the micro time scale, moving toward theperformance limit of this promising process which wasrarely explored before. The investigation and decouplingof plasma-catalysis synergic effects is another main key
scientific problem. Based on the experimental evaluationof plasma-enabled catalytic system, high-resolution
spectroscopic techniques and theoretical calculations are
employed to elucidate the interface regulation
mechanism for directional conversion and mass-transfer,for the further process optimization and realize thein-situ high-value utilization of CH4.
At last, we would like to introduce our work on thesingle step synthesis of C2-C4 alcohols by plasma
enabled CH4-CH3OH conversion [4]. Here, an innovativesynthesis of higher alcohols from CH4-CH3OH wasdriven by a highly flexible nanosecond pulsed plasma.
Experimental results showed that the products
distribution was strongly correlated with the electric field
variation and reactants composition, and the maximum
conversion of CH4 (35.9%) and CH3OH (77.4%) wereobtained at the CH4/Ar ratio of 1:2. optical diagnostics
were used to obtain the active species distribution andintegrated insights into the C-C coupling of higher
alcohols generation.
References[1] X. Li, C. Pei, J. Gong. Shale gas revolution: catalytic
conversion of C1-C3 light alkanes to value-added
chemicals. Chem, 2021, 7: 1755-801.
[2] X. Wang, Y. Gao, S. Zhang, H. Sun, J. Li, T. Shao.
Nanosecond pulsed plasma assisted dry reforming of
CH4: the effect of plasma operating parameters. Appl.
Energy, 2019, 243: 132-144.
[3] Y. Gao, L. Dou, B. Feng, C. Zhang, T. Shao.
Catalyst-free activation of CH4 and air into platformchemicals and H2 using parametrized nanosecond pulsed
plasma, Energ. Convers. Manage., 2023, 276, 116750.
[4] J. Li, Y. Gao, L. Dou, C. Zhang, J. Du, T. Shao.
Parametricinvestigationsonplasma-activatedconversion of CH4-CH3OH to C2-C4 alcohols bynanosecond pulsed discharge, 2023, 20(2): 2200162.