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Development of Molecular Sieving Inorganic Membranes and Separation System for High Temperature Gases

高温气体分子筛无机膜及分离系统的研制

基本信息

批准号：
05555214
负责人：
MOROOKA Shigeharu
金额：
$ 5.5万
依托单位：
KYUSHU UNIVERSITY
依托单位国家：
日本
项目类别：
Grant-in-Aid for Developmental Scientific Research (B)
财政年份：
1993
资助国家：
日本
起止时间：
1993 至 1994
项目状态：
已结题

项目摘要

Inorganic membranes can be used for gas separation at high temperature in an oxidative atmosphere where organic membranes are not resistant. In preparing molecular sieving inorganic membranes with high permeability, the pore structure should be strictly controlled. In this study, ceramic and palladium thin membranes were formed by novel preparation methods, and gas permeability and thermal and chemical stability of the membranes were examined.Palladium thin membrane was formed in macropores of an alpha-alumina support tube by cross-flow CVD method. Hydrogen permeance and selectivity to nitrogen were respectively higher than 10^<-6> mol・m^<-2>s^<-1>Pa^<-1> and 1000. The membrane was resistant against hydrogen embrittlement and sulfur poisoning. Silica membrane was also prepared by the same procedure using tetraethylorthosilicate. The membrane was stable in steam and showed a selectivity of hydrogen to nitrogen higher than 1000. Furthermore, Silica-based microporous membrane was prepared by controlled pyrolysis of polycarbosilane coated on a gamma-alumina-modified support tube. The membrane showed a permselectivity of hydrogen to nitrogen higher than the Knudsen value and was usable up to 400ﾟC.Perovskite oxide membrane was prepared by sol-gel methods and slicalite membrane formed by hydrothermal synthesis, respectively. Carbon dioxide was preferentially permeated through these membranes because of the surface diffusion, but the CO_2 permselectivity was insufficient. Further pore-size control is needed for the industrial uses.

无机膜可用于高温氧化气氛下的气体分离，而有机膜不耐氧化。在制备高渗透无机分子筛膜时，应严格控制孔隙结构。本研究采用新的制备方法制备了陶瓷和钯薄膜，并对膜的透气性、热稳定性和化学稳定性进行了测试。采用横流气相沉积法在α -氧化铝支撑管的大孔中制备了钯薄膜。氢透性和对氮选择性分别高于10^<-6> mol·m^<-2>s^<-1>Pa^<-1>和1000。该膜具有抗氢脆和抗硫中毒的特点。以四乙基硅酸盐为原料，用同样的方法制备了二氧化硅膜。该膜在蒸汽中稳定，对氢氮的选择性大于1000。在此基础上，通过控制热解将聚碳硅烷包覆在γ -氧化铝修饰的支撑管上，制备了硅基微孔膜。该膜对氢氮的选择性高于Knudsen值，使用温度高达400℃。采用溶胶-凝胶法制备了钙钛矿氧化膜，采用水热法制备了硅藻土氧化膜。由于膜的表面扩散作用，二氧化碳优先通过膜，但CO_2的选择性不够。工业用途需要进一步的孔径控制。