Challenging fabrication of hollow ceramic fiber supported Cu3(BTC)2 membrane for hydrogen separation
Challenging fabrication of hollow ceramic fiber supported Cu3(BTC)2 membrane for hydrogen separation
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DOI：
10.1039/c2jm16371c
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发表时间：
2012-05
影响因子：
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通讯作者：
Shuyuan Zhou;Xiaoqin Zou;F. Sun;Feng Zhang;Songjie Fan;Huijun Zhao;T. Schiestel;G. Zhu
中科院分区：
文献类型：
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作者：
Shuyuan Zhou;Xiaoqin Zou;F. Sun;Feng Zhang;Songjie Fan;Huijun Zhao;T. Schiestel;G. Zhu
采用二次生长法在壳聚糖修饰的α-Al_2O_3中空陶瓷纤维上成功制备了高性能的连续Cu3(Btc)_2膜。采用改进的溶剂热法可以方便地合成Cu3(BTC)2纳米晶。得到了稳定、均匀的Cu3(BTC)2晶种前驱体，其粒径为300 nm，适合于种下羟基磷灰石，而不会堵塞羟基磷灰石载体的孔洞(羟基磷灰石的孔径为200 nm)。引入一种新的底物HCFS作为Cu3(BTC)2膜的支撑体。此外，壳聚糖因其丰富的氨基和羟基首次被用于改善种子与载体之间的结合力。对所制备的Cu3(BTC)2膜进行了H2/N2、H2/CO2和H2/CH4二元气体渗透分离氢的研究。合成膜对H2/N2、H2/CO2和H2/CH4混合气体的分离系数分别为8.66、13.56和6.19，具有较高的H2选择性。由于Cu3(−)2MOF材料的独特性质，在3.2 3×10−8~4.1×10−8molm−2 4.1×10−8molm−2−1PaMOF 1范围内，获得了H2在二元混合气体中的较好磁导率，有望在工业氢回收中得到潜在应用。
High-performance and continuous Cu3(BTC)2 membranes have been successfully fabricated using a secondary growth approach on pre-seeded α-Al2O3 hollow ceramic fibers (HCFs) modified with chitosan. Facile synthesis of Cu3(BTC)2 nanocrystals can be achieved by a modified solvothermal protocol. A stable and homogeneous Cu3(BTC)2 seed precusor obtained with particle size of 300 nm, the size of which is suitable for seeding HCFs without any pore jam of HCFs supports (pore size of 200 nm for HCFs). A new substrate HCFs was introduced as the support of Cu3(BTC)2 membranes. Moreover, for the first time, chitosan is used to improve the binding force between seeds and the support owing to its abundance of both amino and hydroxyl groups. As-prepared Cu3(BTC)2 membrane is studied for hydrogen separation by binary gas permeation of H2/N2, H2/CO2 and H2/CH4. The synthesized membrane shows high H2 selectivity with separation factors of 8.66, 13.56 and 6.19 for the gas mixtures of H2/N2, H2/CO2 and H2/CH4 respectively. A preferred permeance for H2 in the binary gas mixture is obtained in the range of 3.23 × 10−8 to 4.1 × 10−8 mol m−2 s−1 Pa−1 due to the unique properties of the Cu3(BTC)2 MOF material, which is expected in the potential applications of industrial hydrogen recycling.