Synthesis and Characterization of an Amino Functionalized MIL-101(Al): Separation and Catalytic Properties

被引:468
|
作者
Serra-Crespo, Pablo [1 ]
Ramos-Fernandez, Enrique V. [1 ]
Gascon, Jorge [1 ]
Kapteijn, Freek [1 ]
机构
[1] Delft Univ Technol, Dept Chem Engn, NL-2628 BL Delft, Netherlands
基金
美国国家科学基金会;
关键词
metal organic framework; MIL-101 (Al); amine; catalysis; CO(2) separation; Knoevenagel condensation; METAL-ORGANIC FRAMEWORKS; PROTON SPONGE; ADSORPTION; MIL-53; CO2; ENCAPSULATION; PERFORMANCE; STABILITY; MIXTURES; CARRIERS;
D O I
10.1021/cm103644b
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A new MIL-101 material based on aluminum and containing amine functional groups has been synthesized. The pure phase NH(2)-MIL-101(Al) can only be formed in very specific synthesis conditions, where both the metal source and the solvent used play a key role. The resulting porous solid shows a high thermal and chemical stability, decomposing at temperatures above 650 K in air. The NH(2)-MIL-101(Al) framework offers an excellent trade off for separation of CO(2): the combination of high stability, acceptable capacity at low adsorbate partial pressures, high selectivity, and fast regenerability makes this new material a very attractive candidate for applications like natural gas or biogas upgrading. CO(2) capacities up to 62 wt % are obtained at room temperature and 3 MPa. In addition to an excellent separation performance, the NH(2)MIL-101(Al) shows a high activity in the basic catalyzed Knoevenagel condensation of benzaldehyde with ethyl cyanoacetate at 313 K even in an as apolar a solvent as toluene (turn over frequency, TOF = 1.8 h(-1)).
引用
收藏
页码:2565 / 2572
页数:8
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