
Journal of the Chemical Society - Faraday Transactions p. 4419 - 4422 (1995)
Update date:2022-08-16
Topics:
Hibino, Takashi
Sato, Teruyuki
Ushiki, Ken-ichi
Kuwahara, Yoshitaka
A membrane reactor for the oxidative coupling of CH4 has been constructed with an oxide ion-electron hole mixed conductor, BaCe0.8Gd0.2=3-α. 10percent CH4 diluted with Ar and an O2-Ar mixture at a given ratio were fed into opposite sides of the membrane at 1173 K.The formation rate of C2-hydrocarbons (ethane and especially ethene) in CH4 compartment increased with PO2 in the O2-Ar compartment.This enhancement was due to electrochemical oxygen permeation, causing the conductor to short-circuit itself, resulting from the mixed conduction.For comparison, 10percent CH4 and a small amount of O2 were co-fed into one side of the membrane.The membrane operation gave a C2 selectivity two times that of the co-feed operation for all CH4 conversions.From a catalytic study using BaCe1-xGdxO3-α powders as catalyst, it was found that increasing both the oxide-ion and electron-hole conductivities enhanced the formation of C2 hydrocarbons, but reduced that of CO2.On the basis of these results, a mechanism for the oxidative coupling of CH4 of the mixed-conductor membrane was proposed.
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