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Title: Oxidative coupling of methane in solid oxide fuel cell tubular membrane reactor with high ethylene yield

Authors:
; ; ; ; ;
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1415344
Grant/Contract Number:
SC0015202
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Catalysis Communications
Additional Journal Information:
Journal Volume: 96; Journal Issue: C; Related Information: CHORUS Timestamp: 2018-01-02 19:59:55; Journal ID: ISSN 1566-7367
Publisher:
Elsevier
Country of Publication:
Netherlands
Language:
English

Citation Formats

Liu, Kefeng, Zhao, Jing, Zhu, Di, Meng, Fei, Kong, Fanhua, and Tang, Yongchun. Oxidative coupling of methane in solid oxide fuel cell tubular membrane reactor with high ethylene yield. Netherlands: N. p., 2017. Web. doi:10.1016/j.catcom.2017.03.010.
Liu, Kefeng, Zhao, Jing, Zhu, Di, Meng, Fei, Kong, Fanhua, & Tang, Yongchun. Oxidative coupling of methane in solid oxide fuel cell tubular membrane reactor with high ethylene yield. Netherlands. doi:10.1016/j.catcom.2017.03.010.
Liu, Kefeng, Zhao, Jing, Zhu, Di, Meng, Fei, Kong, Fanhua, and Tang, Yongchun. 2017. "Oxidative coupling of methane in solid oxide fuel cell tubular membrane reactor with high ethylene yield". Netherlands. doi:10.1016/j.catcom.2017.03.010.
@article{osti_1415344,
title = {Oxidative coupling of methane in solid oxide fuel cell tubular membrane reactor with high ethylene yield},
author = {Liu, Kefeng and Zhao, Jing and Zhu, Di and Meng, Fei and Kong, Fanhua and Tang, Yongchun},
abstractNote = {},
doi = {10.1016/j.catcom.2017.03.010},
journal = {Catalysis Communications},
number = C,
volume = 96,
place = {Netherlands},
year = 2017,
month = 6
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on March 27, 2018
Publisher's Accepted Manuscript

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  • The oxidative coupling of methane (OCM) has been studied using the 1 wt% Sr/La{sub 2}O{sub 3}-Bi{sub 2}O{sub 3}-Ag-YSZ solid oxide membrane reactor. The effects of oxygen flux, temperature and feed concentration on the performance of oxidative coupling of methane reaction have been investigated. Two mathematical models based on well-mixed flow (CSTM) or plug flow (PFM) in the reactor have been developed to describe the behavior of the solid oxide membrane reactors. The simulation results show good agreement with experimental data. However, the simulation results of the CSTM fit experimental data much better than that of PFM over a broad rangemore » of experimental conditions. The simulation results also show it is very important to match reaction conditions and reactor parameters.« less
  • Tetragonal LaOBr is a better catalyst than La{sub 2}O{sub 3} for the oxidative coupling of methane (OCM), whereas BaCO{sub 3} is a good promoter for LaOBr. With contact time equal to 0.2 g s ml{sup -1} and a CH{sub 4}:O{sub 2}:N{sub 2}ratio of 1:1:12, a C{sub 2} yield of 26.3% with a C{sub 2}H{sub 4}/C{sub 2}H{sub 6} ratio of 4.3 could be achieved over the 50 mol% BaCO{sub 3}/LaOBr catalyst at 800{degrees}C. When the CH{sub 4}:O{sub 2}:N{sub 2} ratio was 0.5:1:12 and the contact time was 0.6 g s ml{sup -1}, the C{sub 2} yield became 18.9% and C{sub 2}H{submore » 4} was the sole C{sub 2} product. Fixing the CH{sub 4}:O{sub 2}:N{sub 2} ratio to 2.6:1:12 and contact time to 0.6 g s ml{sup -1}, the C{sub 2}H{sub 4}/C{sub 2}H{sub 6} ratios over the LaOF, LaOBr, and 30 mol% BaCO{sub 3}/LaOBr catalysts were, respectively, 1.6, 3.3, and 11.3 at 800{degrees}C. The authors suggest that for a mixed catalyst like BaCO{sub 3}/LaOBr, nonstochiometric behavior is expected and defects such as O{sup -} centers and trapped electrons which would bring about the generation of surface dioxygen species could be present within the constituent structures of at the interfaces. The authors suggest that the direct interaction of CH{sub 4} with O{sub 2}{sup 2-} is an efficient way of producing carbene, and the coupling of carbene, rather than methyl radical, could be the major step for C{sub 2}H{sub 4} generation over these highly C{sub 2}H{sub 4} selective BaCO{sub 3}/LaOBr catalysts. 36 refs., 9 figs., 5 tabs.« less
  • Oxidative coupling of methane was conducted by using membrane reactors. The nonporous membrane film that consisted of PbO modified by alkaline or alkaline earth compound was supported on porous SiO[sub 2]-Al[sub 2]O[sub 3] tube. Higher hydrocarbons were successfully synthesized with high selectivity (about 90%). A kinetic analysis was conducted to clarify whether oxide ion transportation through PbO film participated in the oxidative coupling of methane. The evaluated value of the diffusion coefficient of oxide ion transport based on the methane oxidation agreed well with that of published data. The simulated gradient of the oxide ion concentration through the PbO membranemore » agreed well with that measured by electron probe X-ray microanalyzer. A transient response simulated by using kinetic parameters evaluated from steady-state analysis also agreed well with the experiment. These results prove the validity of the reaction model that consists of surface reactions of methane with oxide ion which is transferred from inside to outside of the membrane reactor. Alkali modifiers on the PbO membrane surface exhibited a promotional effect on the surface reaction of methane coupling. Another membrane reactor containing Bi[sub 2]O[sub 3] showed higher activity than the PbO membrane.« less
  • Catalytic performances of lead oxide supported on MgO which has been discovered to exhibit excellent characteristics for the oxidative coupling of methane to C/sub 2/ hydrocarbons have been studied. A 20 wt % PbO/MgO catalyst gave 13% methane conversion, 98% oxygen conversion, and 71% C/sub 2/ selectivity at 800/sup 0/C, a time factor of 1.0 g . h/mol, a feed gas composition for CH/sub 4/ of 14% and for O/sub 2/ of 1.6%, and atmospheric pressure. Significant changes of catalyst performance were observed with time. The methane conversion rate and C/sub 2/ selectivity as a function of PbO loading weremore » examined to clarify that 5 wt % PbO loading was the best. It was also clarified that ethylene and carbon dioxide were made successively from ethane and carbon monoxide, respectively.« less
  • Oxidative coupling of methane was conducted by using membrane reactors. The nonporous membrane film that consisted of PbO modified by alkali-metal or alkaline earth compound was supported on a porous tube or nonporous tube of stabilized zirconia. Oxide ion was transported from the oxygen (air) side to the methane side through PbO film. C[sub 2] hydrocarbons were obtained with high selectivity (>90 %), but the activity was influenced by alkali-metal compounds and the supports on which the membrane was formed. The temperature characteristics of the activity indicated that the C[sub 2] formation rate was controlled by O[sup 2[minus]] transportation whenmore » the support had low O[sup 2[minus]] conductivity, while it was controlled by both of the catalytic reaction and oxide ion transportation on other supports.« less