The permeability and stability of Sm_(0.7)Sr_(0.3)CoO_(3-δ)(SSCO) regarding the special requirements for carbon capture and storage(CCS) application were investigated.Pure CO_ was used as the sweep gas at 900 °C,leading to that the oxygen permeation flux decreases by about 34 %.Several cycles of changing the sweep gas between helium and CO_2 indicate the good reversibility of this degradation.Both carbonate formation and adsorption of CO_2 on the membrane surface are responsible for the degradation of the membrane performance.The better CO_2 resistance results from the substitution of Sm for Sr due to the higher acidity of Sm_2O_3(1.278) than that of Sr O(0.978) and a discontinuous layer of carbonate.
Yu-Wen ZhangFan-Lin ZengChen-Chen YuCheng-Zhang WuWei-Zhong DingXiong-Gang Lu
利用固相合成法制备了A位La掺杂Ba Co0.88Nb0.12O3-δ[BLCN-x,x为La的掺杂量(摩尔分数)]钙钛矿透氧膜材料,采用X射线衍射(XRD)、扫描电子显微镜(SEM)、热重分析(TG)及程序升温脱附-质谱(TPD-MS)等方法研究了CO2气氛静态处理及动态透氧条件BLCN-x系列材料的结构稳定性.研究结果表明,随着La掺杂量的增加,BLCN-x膜片材料抗CO2腐蚀的性能明显提高.当La含量高于0.5时,在850℃纯CO2气氛静态处理或透氧条件下均未观察到碳酸盐衍射峰.尽管La掺杂会降低BLCN-x膜片的初始透氧量,但在CO2气氛吹扫时透氧量的降低速率明显减慢,其中BLCN-0.5膜片在纯CO2气氛下10 h后的透氧量仍可达到0.46 m L·cm-2·min-1.通过容差因子和平均金属-氧键能计算可知,良好的结构稳定性和增强的金属-氧键能是导致La掺杂样品抗CO2腐蚀的主要因素.
Ba1.0Co0.7Fe0.2Nb0.1O3-δ(BCFN) oxide with perovskite cubic structure was synthesized by solid state reaction method. CO2 corrosion of BCFN membrane was investigated by X-ray diffraction(XRD), scanning electron microscopy(SEM), diffuse reflectance infrared Fouriertransformed spectroscopy(DRIFT) and X-ray absorption fine structure spectroscopy(XAFS). Cobalt(Co) K-edge absorption spectra of BCFN annealed in CO2 reveal that the oxidation states of Co in all the samples were larger than +3 and they decreased with the increase of calcination time. At 800℃, 1% CO2 introduced into He could speed up the reduction of Co cations in comparison with pure He. In addition, sulfate ions in the bulk of BCFN membrane preferred to migrate to the surface under CO2 calcination and form monoclinic Ba(CO3)0.9(SO4)0.1besides orthorhombic witherite. Moreover, SEM results indicate that the nucleation and growth of carbonates grains started at the grain boundary of the membrane.
Chengzhang WuHe WangXingxing ZhangYuwen ZhangWeizhong DingChenghua Sun
