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Pyrolysis and Oxidation of Methane in a RF Plasma Reactor

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Abstract

The chemical kinetic effects of RF plasma on the pyrolysis and oxidation of methane were studied experimentally and computationally in a laminar flow reactor at 100 Torr and 373 K with and without oxygen addition into He/CH4 mixtures. The formation of excited species as well as intermediate species and products in the RF plasma reactor was measured with optical emission spectrometer and Gas Chromatography and the data were used to validate the kinetic model. The kinetic analysis was performed to understand the key reaction pathways. The experimental results showed that H2, C2 and C3 hydrocarbon formation was the major pathways for plasma assisted pyrolysis of methane. In contrast, with oxygen addition, C2 and C3 formation dramatically decreased, and syngas (H2 and CO) became the major products. The above results revealed oxygen addition significantly modified the chemistry of plasma assisted fuel pyrolysis in a RF discharge. Moreover, an increase of E/n was found to be more beneficial for the formation of higher hydrocarbons while a small amount of oxygen was presented in a He/CH4 mixture. A reaction path flux analysis showed that in a RF plasma, the formation of active species such as CH3, CH2, CH, H, O and O (1D) via the electron impact dissociation reactions played a critical role in the subsequent processes of radical chain propagating and products formation. The results showed that the electronically excitation, ionization, and dissociation processes as well as the products formation were selective and strongly dependent on the reduced electric field.

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Acknowledgements

This work was supported by the ACEE grand challenge grants, the Exxon Mobile research grant, the U.S. Department of Energy, Office of Science (DE-SC0015735),and the National Natural Science Foundation of China (51373021).

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Authors and Affiliations

  1. Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ, 08544, USA

    Qi Chen & Yiguang Ju

  2. Department of Chemical and Biological Engineering, Princeton University, Princeton, NJ, 08544, USA

    Xiaofang Yang & Bruce E. Koel

  3. School of Mechanical and Electronic Control Engineering, Beijing Jiaotong University, Beijing, 100044, China

    Qi Chen, Jintao Sun, Xiaojun Zhang & Xingian Mao

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  1. Qi Chen
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Correspondence to Yiguang Ju.

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Chen, Q., Yang, X., Sun, J. et al. Pyrolysis and Oxidation of Methane in a RF Plasma Reactor. Plasma Chem Plasma Process 37, 1551–1571 (2017). https://doi.org/10.1007/s11090-017-9844-4

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