Oxygen transport through La1-xSrxFeO3-delta membranes .2. Permeation in air/CO, CO2 gradients

被引:154
作者
tenElshof, JE
Bouwmeester, HJM
Verweij, H
机构
关键词
oxygen permeation; mixed conductor; lanthanum strontium iron oxide; perovskite; carbon monoxide oxidation;
D O I
10.1016/0167-2738(96)00255-X
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Oxygen permeation measurements were performed on dense La1-xSrxFeO3-delta (n = 0.1-0.4) membranes in large oxygen activity gradients, i.e. air/CO, CO2, in the temperature range 1173-1323 K, yielding fluxes up to 25 mmol m(-2) s(-1) at 1273 K. The oxygen semipermeability was linearly proportional with the CO partial pressure and the strontium content. It was concluded that the fluxes are limited by the surface exchange kinetics. Two simple models are proposed for the oxygen exchange reaction in the presence of CO. In both models oxygen vacancies at the phase boundary play a definite role in the exchange process. XPS and SEM analysis of the perovskite/CO, CO2 interfaces indicated segregation of strontium, being present at the surface mostly in the form of SrCO3 and/or SrO. The enhanced oxygen fluxes in air/He gradients as they were observed after exposure of the membrane surface to CO are probably (indirectly) related to the level of strontium segregation. Based on SEM analysis and surface profile measurements, it is suggested that the segregation process is accompanied by an enlargement of the specific surface area, which may promote the speed of the overall permeation process under exchange-controlled conditions.
引用
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页码:81 / 92
页数:12
相关论文
共 39 条
[31]   OXYGEN-TRANSPORT THROUGH LA1-XSRXFEO3-DELTA MEMBRANES .1. PERMEATION IN AIR/HE GRADIENTS [J].
TENELSHOF, JE ;
BOUWMEESTER, HJM ;
VERWEIJ, H .
SOLID STATE IONICS, 1995, 81 (1-2) :97-109
[32]   OXIDATIVE COUPLING OF METHANE IN A MIXED-CONDUCTING PEROVSKITE MEMBRANE REACTOR [J].
TENELSHOF, JE ;
BOUWMEESTER, HJM ;
VERWEIJ, H .
APPLIED CATALYSIS A-GENERAL, 1995, 130 (02) :195-212
[33]   ACTIVATION OF METHANE USING SOLID OXIDE MEMBRANES [J].
TENELSHOF, JE ;
VANHASSEL, BA ;
BOUWMEESTER, HJM .
CATALYSIS TODAY, 1995, 25 (3-4) :397-402
[34]   XPS SPECTRA OF CA, SR, BA AND THEIR OXIDES [J].
VANDOVEREN, H ;
VERHOEVEN, JAT .
JOURNAL OF ELECTRON SPECTROSCOPY AND RELATED PHENOMENA, 1980, 21 (03) :265-273
[35]   OXYGEN PERMEATION FLUX THROUGH LA1-YSRYFEO3 LIMITED BY CARBON-MONOXIDE OXIDATION RATE [J].
VANHASSEL, BA ;
TENELSHOF, JE ;
BOUWMEESTER, HJM .
APPLIED CATALYSIS A-GENERAL, 1994, 119 (02) :279-291
[36]  
VOORHOEVE RJH, 1976, ANN NY ACAD SCI, V3, P3
[37]  
WACHOWSKI L, 1988, Z PHYS CHEM-LEIPZIG, V269, P743
[38]   ELECTRICAL-CONDUCTIVITY AND CHEMICAL DIFFUSION-COEFFICIENT OF SR-DOPED LANTHANUM CHROMITES [J].
YASUDA, I ;
HISHINUMA, M .
SOLID STATE IONICS, 1995, 80 (1-2) :141-150
[39]   PRECISE DETERMINATION OF THE CHEMICAL DIFFUSION-COEFFICIENT OF CALCIUM-DOPED LANTHANUM CHROMITES BY MEANS OF ELECTRICAL-CONDUCTIVITY RELAXATION [J].
YASUDA, I ;
HIKITA, T .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 1994, 141 (05) :1268-1273