用于清洁能源应用的高孔隙率共价有机框架中氢气、甲烷和二氧化碳的储存
Storage of hydrogen, methane, and carbon dioxide in highly porous covalent organic frameworks for clean energy applications.
作者信息
Furukawa Hiroyasu, Yaghi Omar M
机构信息
Center for Reticular Chemistry, Department of Chemistry and Biochemistry, University of California-Los Angeles, Los Angeles, California 90095-1569, USA.
出版信息
J Am Chem Soc. 2009 Jul 1;131(25):8875-83. doi: 10.1021/ja9015765.
Dihydrogen, methane, and carbon dioxide isotherm measurements were performed at 1-85 bar and 77-298 K on the evacuated forms of seven porous covalent organic frameworks (COFs). The uptake behavior and capacity of the COFs is best described by classifying them into three groups based on their structural dimensions and corresponding pore sizes. Group 1 consists of 2D structures with 1D small pores (9 A for each of COF-1 and COF-6), group 2 includes 2D structures with large 1D pores (27, 16, and 32 A for COF-5, COF-8, and COF-10, respectively), and group 3 is comprised of 3D structures with 3D medium-sized pores (12 A for each of COF-102 and COF-103). Group 3 COFs outperform group 1 and 2 COFs, and rival the best metal-organic frameworks and other porous materials in their uptake capacities. This is exemplified by the excess gas uptake of COF-102 at 35 bar (72 mg g(-1) at 77 K for hydrogen, 187 mg g(-1) at 298 K for methane, and 1180 mg g(-1) at 298 K for carbon dioxide), which is similar to the performance of COF-103 but higher than those observed for COF-1, COF-5, COF-6, COF-8, and COF-10 (hydrogen at 77 K, 15 mg g(-1) for COF-1, 36 mg g(-1) for COF-5, 23 mg g(-1) for COF-6, 35 mg g(-1) for COF-8, and 39 mg g(-1) for COF-10; methane at 298 K, 40 mg g(-1) for COF-1, 89 mg g(-1) for COF-5, 65 mg g(-1) for COF-6, 87 mg g(-1) for COF-8, and 80 mg g(-1) for COF-10; carbon dioxide at 298 K, 210 mg g(-1) for COF-1, 779 mg g(-1) for COF-5, 298 mg g(-1) for COF-6, 598 mg g(-1) for COF-8, and 759 mg g(-1) for COF-10). These findings place COFs among the most porous and the best adsorbents for hydrogen, methane, and carbon dioxide.
在1-85巴和77-298K的条件下，对七种多孔共价有机框架（COF）的抽空形式进行了氢气、甲烷和二氧化碳等温线测量。根据COF的结构尺寸和相应的孔径将它们分为三组，这样能最好地描述COF的吸附行为和吸附容量。第一组由具有一维小孔（COF-1和COF-6的孔径均为9埃）的二维结构组成，第二组包括具有大的一维孔（COF-5、COF-8和COF-10的孔径分别为27、16和32埃）的二维结构，第三组由具有三维中等尺寸孔（COF-102和COF-103的孔径均为12埃）的三维结构组成。第三组COF的性能优于第一组和第二组COF，在吸附容量方面可与最佳金属有机框架和其他多孔材料相媲美。这一点以COF-102在35巴下的过量气体吸附为例（77K时氢气的吸附量为72mg g⁻¹，298K时甲烷的吸附量为187mg g⁻¹，298K时二氧化碳的吸附量为1180mg g⁻¹），其性能与COF-103相似，但高于COF-1、COF-5、COF-6、COF-8和COF-10所观察到的性能（77K时氢气的吸附量，COF-1为15mg g⁻¹，COF-5为36mg g⁻¹，COF-6为23mg g⁻¹，COF-8为35mg g⁻¹，COF-10为39mg g⁻¹；298K时甲烷的吸附量，COF-1为40mg g⁻¹，COF-5为89mg g⁻¹，COF-6为65mg g⁻¹，COF-8为87mg g⁻¹，COF-10为80mg g⁻¹；298K时二氧化碳的吸附量，COF-1为210mg g⁻¹，COF-5为779mg g⁻¹，COF-6为298mg g⁻¹，COF-8为598mg g⁻¹，COF-10为759mg g⁻¹）。这些发现使COF成为氢气、甲烷和二氧化碳最具多孔性且最佳的吸附剂之一。
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