Effect of Additive Gases on Light Alkanes Converting Under Dielectric Barrier Discharge

doi:10.7503/cjcu20120219

Abstract

Abstract:

At atmospheric pressure, the influences of different types of additive gases(N₂, He, Ar, H₂, NH₃, CO, CO₂) on the transformation of low carbon alkanes(CH₄, C₂H₆ and C₃H₈) to light alkenes via the dielectric barrier discharge non-equilibrium plasma(DBD plasma) method were investigated. Results show that the additive gases have different effects on the reaction. For CH₄ or C₂H₆, the conversion and selectivity of feedstock increase with the introduction of N₂, He, Ar, CO. While CO₂, NH₃ and H₂ have no obvious effect to conversion of feedstock but NH₃ and H₂ inhibit the selectivity obviously. As for C₃H₈ feedstock, the conversion can be enhanced by all the additive gases mentioned above, while the selectivity decreased in different degrees except CO. Among these additive gases, 80%(molar fraction) CO exhibits the best activity both for the feedstock conversion and selectivity of total alkenes. The conversion of CH₄, C₂H₆ and C₃H₈ increase by 14.4%, 17.6% and 42.8%, respectively, and the corresponding selectivity of total alkenes increase by 19.9%, 25.0% and 11.9%, respectively. Studies on in situ optical emission spectroscopy(OES) and current waveform of discharge show that the introduction of CO can not only increase the electron density of plasma, but also generate the excited oxygen atoms(777.5 and 844.7 nm), the latter can effectively facilitate the C-H cleavage of methane to the formation of ethylene. Therefore, the existence of excited oxygen atoms and the increased electron density of plasma may be the main reasons to cause the effective transformation of methane to light alkenes when CO as additive gas.

Key words: Light alkane, Additive gas, Plasma, Light alkene, Optical emission spectroscopy

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DONG Jie, WANG Li, ZHAO Yue, ZHANG Jia-Liang, GUO Hong-Chen. Effect of Additive Gases on Light Alkanes Converting Under Dielectric Barrier Discharge[J]. Chem. J. Chinese Universities, 2013, 34(1): 192.

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Effect of Additive Gases on Light Alkanes Converting Under Dielectric Barrier Discharge

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