Wang Lintao, Yang Jing
School of Urban Planning and Municipal Engineering, Xi'an Polytechnic University, Xi'an 710048, China.
Nanomaterials (Basel). 2022 Jun 23;12(13):2159. doi: 10.3390/nano12132159.
In order to obtain a steam-stable hydrogen permselectivity membrane, with tetraethylorthosilicate (TEOS) as the silicon source, zirconium nitrate pentahydrate (Zr(NO)·5HO) as the zirconium source, and methyltriethoxysilane (MTES) as the hydrophobic modifier, the methyl-modified ZrO-SiO (ZrO-MSiO) membranes were prepared via the sol-gel method. The microstructure and gas permeance of the ZrO-MSiO membranes were studied. The physical-chemical properties of the membranes were characterized by Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscope (SEM), and N adsorption-desorption analysis. The hydrogen permselectivity of ZrO-MSiO membranes was evaluated with Zr content, temperature, pressure difference, drying control chemical additive (glycerol) content, and hydrothermal stability as the inferred factors. XRD and pore structure analysis revealed that, as n increased, the MSiO peak gradually shifted to a higher 2θ value, and the intensity gradually decreased. The study found that the permeation mechanism of H and other gases is mainly based on the activation-diffusion mechanism. The separation of H is facilitated by an increase in temperature. The ZrO-MSiO membrane with n = 0.15 has a better pore structure and a suitable ratio of micropores to mesopores, which improved the gas permselectivities. At 200 °C, the H permeance of MSiO and ZrO-MSiO membranes was 3.66 × 10 and 6.46 × 10 mol·m·s·Pa, respectively. Compared with the MSiO membrane, the H/CO and H/N permselectivities of the ZrO-MSiO membrane were improved by 79.18% and 26.75%, respectively. The added amount of glycerol as the drying control chemical additive increased from 20% to 30%, the permeance of H decreased by 11.55%, and the permselectivities of H/CO and H/N rose by 2.14% and 0.28%, respectively. The final results demonstrate that the ZrO-MSiO membrane possesses excellent hydrothermal stability and regeneration capability.
为了获得具有蒸汽稳定性的氢选择性渗透膜，以正硅酸乙酯（TEOS）为硅源、五水合硝酸锆（Zr(NO₃)₂·5H₂O）为锆源、甲基三乙氧基硅烷（MTES）为疏水改性剂，通过溶胶-凝胶法制备了甲基改性的ZrO₂-SiO₂（ZrO₂-MSiO₂）膜。研究了ZrO₂-MSiO₂膜的微观结构和气体渗透性能。通过傅里叶变换红外光谱（FTIR）、X射线光电子能谱（XPS）、X射线衍射（XRD）、透射电子显微镜（TEM）、扫描电子显微镜（SEM）和N₂吸附-脱附分析对膜的物理化学性质进行了表征。以Zr含量、温度、压差、干燥控制化学添加剂（甘油）含量和水热稳定性为推断因素，对ZrO₂-MSiO₂膜的氢选择性渗透性能进行了评估。XRD和孔结构分析表明，随着n的增加，MSiO₂峰逐渐向更高的2θ值移动，强度逐渐降低。研究发现，H₂和其他气体的渗透机制主要基于活化扩散机制。温度升高有利于H₂的分离。n = 0.15的ZrO₂-MSiO₂膜具有更好的孔结构和合适的微孔与介孔比例，提高了气体渗透选择性。在200℃时，MSiO₂和ZrO₂-MSiO₂膜的H₂渗透率分别为3.66×10⁻⁷和6.46×10⁻⁷mol·m⁻²·s⁻¹·Pa⁻¹。与MSiO₂膜相比，ZrO₂-MSiO₂膜的H₂/CO₂和H₂/N₂渗透选择性分别提高了79.18%和26.75%。作为干燥控制化学添加剂的甘油添加量从20%增加到30%，H₂渗透率下降了11.55%，H₂/CO₂和H₂/N₂渗透选择性分别提高了2.14%和0.28%。最终结果表明，ZrO₂-MSiO₂膜具有优异的水热稳定性和再生能力。
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