Controlled organosilica networks via metal doping for improved dehydration membranes with layered hybrid structures
Controlled organosilica networks via metal doping for improved dehydration membranes with layered hybrid structures
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DOI：
10.1016/j.seppur.2021.119561
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发表时间：
2022
影响因子：
8.6
通讯作者：
Takashi Terao;Hiroki Nagasawa;M. Kanezashi;H. Yanagishita;T. Tsuru
中科院分区：
文献类型：
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作者：
Takashi Terao;Hiroki Nagasawa;M. Kanezashi;H. Yanagishita;T. Tsuru
利用掺杂金属离子（Al和Zr）的双（三乙氧基硅基）乙烷（BTESE）衍生的有机硅溶胶，在纳米多孔聚合物衬底上成功制备了有机硅顶层的层状杂化膜。这些膜应用于甲醇（MeOH）、乙醇（EtOH）和异丙醇（IPA）等乙醇水溶液的脱水。通过动态光散射分析（DLS）、傅里叶变换红外光谱（FT-IR）、x射线光电子能谱（XPS）、n2吸附等温线、激光扫描共聚焦显微镜（LSM）和扫描电子显微镜（SEM）对金属掺杂的BTESE溶胶和凝胶进行了表征。在105℃的IPA溶液脱水过程中，Al-BTESE衍生膜和zr -BTESE衍生膜的分离因子分别达到8,000和10,000，超过了未掺杂BTESE膜的分离因子，表明掺杂金属离子提高了层状杂化膜的脱水性能。此外，通过漂洗法制备的zr - btese衍生膜的透水性为1.8 × 10-6mol m−2s−1Pa−1，与聚合物基底相比具有足够高的透水性。这些膜的分离系数也高于10,000。利用改进的气体转化（mGT）和双峰孔隙模型成功预测了H2O/MeOH、H2O/EtOH和H2O/IPA渗透率比之间的相关性。
A layered hybrid membrane consisting of an organosilica top layer on a polymeric nanoporous substrate was successfully fabricated using bis(triethoxysilyl)ethane (BTESE)-derived organosilica sols doped with metal ions (Al and Zr). These membranes were applied to the dehydration of aqueous alcohol solutions including methanol (MeOH), ethanol (EtOH) and isopropanol (IPA). Metal-doped BTESE sols and gels were characterized via dynamic light scattering analysis (DLS), Fourier Transform Infrared spectroscopy (FT-IR), X-ray Photoelectron Spectroscopy (XPS), the isotherms of N2sorption, laser scanning confocal microscopy (LSM), and scanning electron microscopy (SEM). During the dehydration of an IPA solution at 105 °C, the separation factors for Al-BTESE- and Zr-BTESE-derived membranes reached 8,000 and 10,000, respectively, which exceeded the separation factor for undoped BTESE membranes and indicates that doping with metal ions improves the dehydration performance of layered-hybrid membranes. In addition, Zr-BTESE-derived membranes prepared via the rinse method showed water permeance of 1.8 × 10-6mol m−2s−1Pa−1, which is sufficiently high and compares favorably to that of polymer substrates. These membranes also showed a separation factor that was higher than 10,000. Correlations among the permeance ratios for H2O/MeOH, H2O/EtOH, and H2O/IPA were successfully predicted using modified gas translation (mGT) and bimodal pore models.