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摘要: 采用二次生长法在多孔α-Al2O3载体上制备MFI型（ZSM-5和silicate-1）分子筛膜；通过XRD和SEM检测，证明所合成的分子筛膜为致密、交联和无取向的MFI型分子筛膜，厚度为5 μm；单组分气体渗透实验检测中，所制备样品膜的N2渗透量均小于10-11 mol/（m2·s·Pa），可认为其无缺陷；同时，考察了样品分子筛膜对H2S/CH4混合气的分离效果，在渗透压分别为0.3和0.5 MPa时，silicate-1分子筛膜的H2S/CH4的分离因子分别为1.99和4.44，而ZSM-5分子筛膜的CH4/H2S的分离因子分别为6.71和12.85。Abstract: The MFI (ZSM-5 and silicate-1) membranes with porous α-Al2O3 substrates were synthesized by secondary growth method. The results of scanning electron microscopy (SEM) and X-ray diffraction (XRD) indicate that the membranes with 5 μm thickness are composed of well-intergrown MFI crystals, which completely covers on the α-Al2O3 substrates in random orientation. The gas permeation measurements reveal that the resulting membranes are of high quality with few non-zeolitic pores. In addition, the separation properties of H2S/CH4 through the synthesized MFI membranes were investigated. Under the osmotic pressure of 0.3 and 0.5 MPa, the separation factors of H2S/CH4 by silicate-1 zeolite membrane are 1.99 and 4.44, and the separation factors of CH4/H2S by ZSM-5 zeolite membrane are 6.71 and 12.85, respectively.
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Key words:
- MFI zeolite membrane /
- H2S/CH4 separation /
- secondary growth method
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图 1 所制备的silicate-1和ZSM-5晶种分子筛的XRD谱图
Figure 1 XRD patterns of as-synthesized silicate-1 and ZSM-5 zeolites seed
a: silicate-1; b: ZSM-5
图 2 silicate-1和ZSM-5晶种分子筛的SEM照片
Figure 2 SEM images of silicalite-1 and ZSM-5 zeolites seed
(a): silicate-1; (b): ZSM-5
图 3 所制备的silicate-1和ZSM-5分子筛膜的XRD谱图
Figure 3 XRD patterns of as-synthesized silicate-1 and ZSM-5 zeolite membranes
a: silicate-1 zeolite membrane; b: ZSM-5 zeolite membrane
图 4 silicate-1和ZSM-5分子筛膜的SEM照片: silicate-1分子筛膜的平面(a)和断面图(b)；ZSM-5分子筛膜的平面(c)和断面图(d)
Figure 4 SEM images of silicate-1 and ZSM-5 zeolite membranes: top view (a) and cross-sectional view (b) of silicate-1 zeolite membrane; top view (c) and cross-sectional view (d) of ZSM-5 zeolite membrane
表 1 在不同压降下H2S/CH4混合气在silicalite-1和ZSM-5分子筛膜分离
Table 1 H2S/CH4 separating results for synthesized silicalite-1 zeolite membrane at different pressure drops
Zeolite membrane Osmotic pressure difference p/MPa Feed gas volume fraction/% Separation gas volume fraction/% Separation factor β H2S CH4 H2S CH4 Silicalite-1 0.3 30.51 69.49 18.24 82.76 1.99(H2S/CH4) 0.5 30.51 69.49 9.00 91.00 4.44(H2S/CH4) ZSM-5 0.3 44.37 55.63 84.25 15.75 6.71(CH4/H2S) 0.5 44.37 55.63 91.11 8.89 12.85(CH4/H2S) 
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