Zp. Shao et al., Performance of a mixed-conducting ceramic membrane reactor with high oxygen permeability for methane conversion, J MEMBR SCI, 183(2), 2001, pp. 181-192
A mixed-conducting perovskite-type Ba0.5Sr0.5Co0.8Fe0.2O3-delta (BSCFO) cer
amic membrane reactor with high oxygen permeability was applied for the act
ivation of methane. The membrane reactor has intrinsic catalytic activities
for methane conversion to ethane and ethylene. C-2 selectivity up to 40-70
% was achieved, albeit that conversion rate were low, typically 0.5-3.5% at
800-900 degreesC with a 50% helium diluted methane inlet stream at a flow
rate of 34 ml/min. Large amount of unreacted molecular oxygen was detected
in the eluted gas and the oxygen permeation flux improved only slightly com
pared with that under non-reactive air/He experiments. The partial oxidatio
n of methane to syngas in a BSCFO membrane reactor was also performed by pa
cking LiLaNiO/gamma -Al2O3 with 10% Ni loading as the catalyst. At the init
ial stage, oxygen permeation flux, methane conversion and CO selectivity we
re closely related with the state of the catalyst. Less than 21 h was neede
d for the oxygen permeation flux to reach its steady state. 98.5% CH4 conve
rsion, 93.0% CO selectivity and 10.45 ml/cm(2) min oxygen permeation flux w
ere achieved under steady state at 850 degreesC. Methane conversion and oxy
gen permeation flux increased with increasing temperature, No fracture of t
he membrane reactor was observed during syngas production. However, H-2-TPR
investigation demonstrated that the BSCFO was unstable under reducing atmo
sphere, yet the material was found to have excellent phase reversibility. A
membrane reactor made from BSCFO was successfully operated for the POM rea
ction at 875 degreesC for more than 500h without failure, with a stable oxy
gen permeation flux of about 11.5 ml/cm(2) min. (C) 2001 Elsevier Science B
.V. All rights reserved.