Pd掺杂量对有机无机杂化SiO2膜H2/CO2分离性能和水热稳定性能的影响  

Pd Doping on H_2/CO_2 Separation Performance and Hydrothermal Stability of Organic-inorganic Hybrid SiO_2 Membranes

作　　者：张恒飞 刘为 雷姣姣 宋华庭 漆虹[1] ZHANG Heng-Fei;LIU Wei;LEI Jiao-Jiao;SONG Hua-Ting;QI Hong(State Key Laboratory of Materials-Oriented Chemical Engineering, Membrane Science and Technology Research Center, Nanjing Tech University, Nanjing 210009, China)

机构地区：[1]南京工业大学膜科学技术研究所,材料化学工程国家重点实验室,南京210009

出　　处：《无机材料学报》2018年第12期1316-1322,共7页Journal of Inorganic Materials

基　　金：国家自然科学基金(21490581); 中国石油化工股份有限公司资助项目(317008-6); 广西创新驱动发展专项资金(桂科 AA17204092).

摘　　要：以1,2-二(三乙氧基硅基)乙烷(BTESE)为前驱体、PdCl_2为钯源,制备Pd掺杂有机无机杂化SiO_2(POS)溶胶,涂膜后在水蒸气氛围中煅烧,制备得到POS膜。采用X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、N_2吸附-脱附和透射电子显微镜(TEM)对POS粉体的微观结构进行表征。考察了钯/硅摩尔比(n(Pd/Si)=0.1、0.5和1)对POS膜的气体分离性能与水热稳定性能的影响。结果表明:随着Pd掺杂量的增加,POS膜的H_2渗透率逐渐增大,H_2/CO_2的理想选择性逐渐下降。经100 kPa水蒸气处理180 h后,采用n(Pd/Si)=1制备的POS膜的H_2渗透率达到1.62×10^(–7) mol·m^(–2)·s^(–1)·Pa^(–1),H_2/CO_2理想分离因子达到13.6,表明该膜具有较好的H_2渗透性能、H_2/CO_2分离性能和水热稳定性能。Pd-doped organic-inorganic hybrid SiO 2 (POS) sols were synthesized by using 1,2-bis(triethoxysilyl) ethane (BTESE) and palladium chloride as precursors. POS membranes were fabricated via dip-coating process fol- lowed by calcination in the water vapor environment. The microstructure of POS powders was characterized by X-ray diffraction (XRD), Fourier transform infrared spectra (FT-IR), N 2 adsorption-desorption, and transmission electron microscope (TEM). Effect of the molar ratio of Pd to Si (n (Pd/Si)=0.1, 0.5 and 1) on separation performance and hydrothermal stability of POS membranes was investigated. Results showed that with the increase of Pd doping amount, H 2 permeance of POS membranes increased while the permselectivity of H 2 /CO 2 decreased. After exposing to 100 kPa steam atmosphere for 180 h, H 2 permeance and H 2 /CO 2 permselectivity of the POS membrane prepared with n (Pd/Si) of 1 reached 1.62×10^–7 mol·m^–2 ·s^–1 ·Pa^–1 and 13.6, respectively. This result indicated that as-prepared POS membrane exhibited good H 2 permeance, H 2 /CO 2 permselectivity and hydrothermal stability.

关 键 词：有机无机杂化SiO2膜 Pd掺杂 气体分离 水热稳定性 

分 类 号：TQ174[化学工程—陶瓷工业]