A proposed reaction mechanism for the selective oxidation of methane with nitrous oxide over Co-ZSM-5 catalyst forming synthesis gas (CO + H2)

作者: Naseer A. Khan , Eric M. Kennedy , Bogdan Z. Dlugogorski , Adesoji A. Adesina , Michael Stockenhuber

DOI: 10.1016/J.IJHYDENE.2018.05.026

关键词:

摘要: Abstract Probable reaction intermediates and mechanistic steps involved for the selective oxidation of methane (CH4) with nitrous oxide (N2O) forming synthesis gas (CO + H2) over Co-ZSM-5 was examined. To assess kinetics reactions were conducted within a temperature range 300 °C–550 °C at atmospheric pressure, composition reactant feed (N2O/CH4) varied between three fixed ratios (5, 3, 1). TPD, XRD, TEM FT-IR techniques used catalyst characterization studies. It found, that H2 selectivity is higher feeds lower N2O concentration. Furthermore, CO formation commences temperatures in comparison to which result methanol (CH3OH) carbon oxides (CO CO2) low CH4 conversions. Based on conditions, literature proposes direct an indirect route formation. Our catalytic study suggests formation; i.e. formed by decomposition intermediate species (methoxy CH2O). This supported spectroscopic investigation. Under favourable conditions catalyst, first oxidizes CH3OH, active intermediate, then subsequently converted into (formaldehyde) CH2O H2. highly reactive decomposes

参考文章(103)
Andrew PE York, Tiancun Xiao, Malcom LH Green, Brief Overview of the Partial Oxidation of Methane to Synthesis Gas Topics in Catalysis. ,vol. 22, pp. 345- 358 ,(2003) , 10.1023/A:1023552709642
H.Y. Wang, E. Ruckenstein, Conversions of Methane to Synthesis Gas over Co/γ-Al2O3 by CO2 and/or O2 Catalysis Letters. ,vol. 75, pp. 13- 18 ,(2001) , 10.1023/A:1016719703118
A. V. Kiselev, V. I. Lygin, Infrared spectra of surface compounds Wiley : distributed by Halsted Press. ,(1975)
Jinghuan Chen, Hamidreza Arandiyan, Xiang Gao, Junhua Li, Recent Advances in Catalysts for Methane Combustion Catalysis Surveys From Asia. ,vol. 19, pp. 140- 171 ,(2015) , 10.1007/S10563-015-9191-5
V.D. Sokolovskii, J.C. Jeannot, N.J. Coville, D. Glasser, D. Hildebrandt, M. Makoa, High yield syngas formation by partial oxidation of methane over Co-alumina catalysts Studies in Surface Science and Catalysis. ,vol. 107, pp. 461- 465 ,(1997) , 10.1016/S0167-2991(97)80377-1
A.G. Steghuis, J.G. van Ommen, K. Seshan, J.A. Lercher, New highly active catalysts in direct partial oxidation of methane to synthesis gas Studies in Surface Science and Catalysis. ,vol. 107, pp. 403- 408 ,(1997) , 10.1016/S0167-2991(97)80368-0
T.S. Christensen, I.I. Primdahl, Improve syngas production using autothermal reforming Hydrocarbon Processing. ,vol. 73, pp. 39- 46 ,(1994)
S. S. Goryashenko, Y. K. Park, D. S. Kim, S. -E. Park, Mechanistic study of the SCR of NO with propylene over Co/ZSM-5 using in-situ FT-IR Research on Chemical Intermediates. ,vol. 24, pp. 933- 951 ,(1998) , 10.1163/156856798X00636