Sekine Yuma, Sakai Motomu, Matsukata Masahiko
Department of Applied Chemistry, Waseda University, 513 Wasedatsurumaki-cho, Shinjuku-ku, Tokyo 162-0041, Japan.
Research Organization for Nano & Life Innovation, Waseda University, 513 Wasedatsurumaki-cho, Shinjuku-ku, Tokyo 162-0041, Japan.
Membranes (Basel). 2023 Jan 14;13(1):111. doi: 10.3390/membranes13010111.
AEI-type zeolite membrane for dehydration was prepared, and a flow-type membrane reactor for the esterification of acetic acid and ethanol by AEI membrane was developed. A synthesized AEI membrane had suitable molecular sieving property for gas separation (H/-butane and CO/CH) and pervaporation (HO/acetic acid). AEI membrane showed HO permeance of 6.2 × 10 mol m s Pa with a separation factor of 67 at 363 K for the equimolar mixture of HO/acetic acid. AEI membrane maintained stable performance under acidic conditions. The yield of ethyl acetate at 363 K in a flow-type membrane reactor with AEI membrane successfully exceeded the equilibrium of 69.1%, reaching 89.0%. The flow rate of feed solution strongly affected the conversion of acetic acid and the space-time yield (STY) of ethyl acetate. Due to the more significant proportion of water selectively removed from the reaction system at a lower feed flow rate, the thermodynamic equilibrium shifted significantly, resulting in higher conversions. In contrast, STY increased with increasing feed flow rate. Our flow-type membrane reactor exhibited a relatively large STY of 430 kg m h compared with the batch-type membrane reactor previously reported.
制备了用于脱水的AEI型沸石膜,并开发了一种使用AEI膜进行乙酸和乙醇酯化反应的流动型膜反应器。合成的AEI膜对气体分离(H₂/正丁烷和CO/CH₄)和渗透汽化(H₂O/乙酸)具有合适的分子筛性能。对于H₂O/乙酸等摩尔混合物,AEI膜在363 K时显示出6.2×10⁻⁶ mol m⁻² s⁻¹ Pa的H₂O渗透率和67的分离因子。AEI膜在酸性条件下保持稳定性能。在带有AEI膜的流动型膜反应器中,363 K时乙酸乙酯的产率成功超过了69.1%的平衡产率,达到89.0%。进料溶液的流速强烈影响乙酸的转化率和乙酸乙酯的时空产率(STY)。由于在较低进料流速下从反应体系中选择性去除的水比例更大,热力学平衡显著移动,导致转化率更高。相比之下,STY随进料流速增加而增加。与先前报道的间歇式膜反应器相比,我们的流动型膜反应器表现出相对较大的430 kg m⁻³ h⁻¹的STY。