Abstract
This paper describes the results of an experimental study on the usage of high-frequency, high-voltage, low direct current spark discharge plasma to examine the catalytic role of chlorine (Cl2) gas on the selective and rapid conversion of light hydrocarbons in the natural gas stream. Our results indicate that the cold DC-spark discharge method in the presence of small amount of chlorine gas is a useful method for decomposition of methane into gaseous constituents and carbon at relatively low power consumption (10 W). Presence of Cl2 boosts the conversion rate of methane (the main constituent of natural gas) to C2 hydrocarbons, as well as formation of nano-graphene, and apparently, molecular hydrogen. Our results indicate that conversion of methane increases by a factor of ~3 in the presence of 6–8 % of chlorine gas. This method is adopted as an efficient and selective routine for the formation of nano-carbons such as graphene using natural gas along with a trace amount of Cl2 in an inert atmosphere such as argon bath gas.
Similar content being viewed by others
References
Y. Koga, S. Tsuneizumi, M. Tabata, H. Mizutani, H. Yamamoto, T.Amari. Mitsubishi Heavy Industries, Ltd. Technical Review. 44 (2), (2007)
Z. Liu, Z. Jiang, B. Fei, X. Liu, Bio. Resour. 8, 5014 (2013)
T.V. Choudhary, E. Aksoylu, D.W. Goodman, Catal. Rev. 45, 151–203 (2003)
Y.-G. Cho, K.-H. Choi, Y.-R. Kim, S.-H. Lee, Bull. Kor. Chem. Soc. 29, 1609 (2008)
H. Shuanghui, W. Baowei, L. Yijun, Y. Wenjuan, Plasma. Sci. Technol. 15, 555 (2013)
B. Wang, W. Yan, W. Ge, X.J. Duan, Energy. Chem. 22, 876–882 (2013)
T. Kolb, J.H. Voigt, K.-H. Gericke, Plasma. Chem. Plasma. Process. 33, 631–646 (2013)
Q. Liu, H. Zheng, F. Pan, G. Pan, R. Yang. ASME, Power Conference, Boston, Massachusetts, USA, July 29–August 1 2013
T. Nozaki, N. Mute, S. Kado, K. Okazaki, Catal. Today. 89, 57–65 (2004)
I.E. Makerov, A.V. Ponomarev, B.G. Ershov, High. Energy. Chem. 4, 55 (2007)
T. Hammer, T. Kappes, M. Baldauf, Catal. Today. 89, 5 (2004)
H.K. Song, J.-W. Choi, S.H. Yue, H. Lee, B.-K. Na, Catal. Today. 89, 27 (2004)
W. Kangjun, L. I. LI Xiaosong, Z. H. U. Aimin. PST. 13, pp 77–81(2011)
X.-S. Li, C.-K. Lin, C. Shi, Y. Xu, Y.-N. Wang, A.-M. Zhu, J. Phys. D Appl. Phys. 41, 175203 (2008)
H. Le, L.L. Lobban, R.G. Mallinson, Pap. Am. Chem. Soc. Div. Fuel. Chem. 49, 173 (2004)
C. Liu, A. Marafee, B. Hill, G. Xu, R. Mallinson, L.L. Lobban, Ind. Eng. Chem. Res. 35, 3295 (1996)
S. Kado, K. Urasaki, Y. Sekine, Fuel. Chem. Div. Prepr. 47, 327 (2002)
Y. Sekine, M. Haraguchi, M. Tomioka, M. Matsukata, E. Kikuchi, J. Phys. Chem. A. 114, 3824–3833 (2010)
W. Kangjun, L. Xiaosong, Z. Aimin, Plasma. Sci. Technol. 13, 77 (2011)
N. Chintala, R. Meyer, A. Hicks, A. Bao, J. W. Rich, W. R. Lempert, I. V. Adamovich. J. Propuls. Power. 21, 583(2005)
J. Kriegseis, B. Möller, S. Grundmann, C. Tropea, J. Electrost. 69, 302 (2011)
X.-S. Li, A.-M. Zhu, K.-J. Wang, Y. Xu, Z.-M. Song, Catal. Today. 98, 617 (2004)
S. Kado, Y. Sekine, T. Nozaki, K. Okazaki, Catal. Today. 89, 47 (2004)
A. Kirubakaran, S. Jain, R.K. Nema, Renew. Sustain. Energy Rev. 13, 2430–2440 (2009)
A.I. Pushkarev, A.-M. Zhub, X.-S. Li, R.V. Sazonov, High. Energy Chem. 43, 156–162 (2009)
R.-F. Horng, Y.-P. Chang, H.-H. Huang, M.-P. Lai, Fuel 86, 81–89 (2007)
M. Matsushima, G. Kalita, K. Kato, M. Noda, H. Uchida, K. Wakita, M. Umeno, M. Tanemura, J. Nanosci. Nanotechnol. 14, 2614–2619 (2014). (references there in)
For instance see the following reports: http://www.corrosion-doctors.org/Pipeline/Carlsbad-explosion.htm, http://www.gascape.org/, http://www.piedmontng.com/files/pdfs/safety/Material Safety Data Sheet_92404.pdf
M.A. Malik, F. Lian-Mei, J.J. Xuan-Zhen, Nat. Gas. Chem. 8, 9–17 (1999)
M.M. Moshrefi, F. Rashidi, H.R. Bozorgzadeh, S.M. Zekordi, Plasma. Chem. Plasma. Process. 32, 1157–1168 (2012)
S. Kado, Y. Sekine, K. Urasaki, K. Okazaki, T. Nozaki. Stud. Surf. Sci. Catal. 147, 577–658(2004)
R-F. Horng, Y-P. Chang, H-H. Huang, M-P. Ming-Pin Lai. Fuel. 86, 81–89(2007)
G. Musa, N. Ekem, T. Akan, S. Pat, M.Z. Balbag, M.I. Cenik, R. Vladoiu, M. Tanisli, O. Ozen, Phys. Stat. Sol. c. 4, 521–523 (2007)
A.N. Obraztsov, A.A. Zolotukhin, A.O. Ustinov, A.P. Volkov, Y. Svirkob, K. Jefimovs, Diam. Relat. Mater. 12, 917–920 (2003)
M. Okumoto, A. Mizuno, Catal. Today. 71, 211–217 (2001)
V.N. Rozanov, Y.A. Treger, Kinet. Catal. 51, 635–643 (2010)
Y.D. Gao, R.G. MacDonald, J. Phys. Chem. A 110, 977–989 (2006)
C. Murray, B. Retail, A.J. Orr-Ewing, Chem. Phys. 301, 239–249 (2004). and references therein
N. Choi, M.J. Pilling, P.W. Seakins, L. Wang, Phys. Chem. Chem. Phys. 8, 2172–2178 (2006). and references therein
K. Takahashi, O. Yamamot, T. Inomata, Proc. Combust. Inst. 29, 2447–2453 (2002). (references there in)
D.W. Chang, E.K. Lee, E.Y. Park, H. Yu, H.-J. Choi, I.-Y. Jeon, G.-J. Sohn, D. Shin, N. Park, J.H. Oh, L. Dai, J.-B. Baek, J. Am. Chem. Soc. 135, 8981 (2013)
A.V. Kirikov, V.V. Ryzhov, A.I. Suslov, Tech. Phys. Lett. 25, 794–795 (1999)
Z. Zhao, D.T. Huskey, K.J. Olsen, J.M. Nicovich, M.L. McKee, P.H. Wine, Phys. Chem. Chem. Phys. 9, 4383–4394 (2007)
Acknowledgments
The financial support from the Research Council of Shiraz University is acknowledged. SHM would like to thank the Department of Chemistry at the SQU for its hospitality during the preparation of this manuscript.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Mousavipour, S.H., Doroodmand, M.M., Zarin Hamedani, S.M.A. et al. Conversion of natural gas into the gaseous constituents and nano-graphene in the presence of chlorine as homogeneous promoter by DC-spark discharge. J IRAN CHEM SOC 12, 1303–1311 (2015). https://doi.org/10.1007/s13738-015-0595-y
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s13738-015-0595-y