小型商用车
化学
块(置换群论)
金属有机骨架
金属
热稳定性
气体分离
多孔性
四面体
结晶学
纳米技术
化学工程
物理化学
有机化学
材料科学
吸附
生物化学
几何学
数学
膜
工程类
作者
Hong-Juan Lv,Yongpeng Li,Yingying Xue,Yucheng Jiang,Shu-Ni Li,Shu-Ni Li,Quan‐Guo Zhai
出处
期刊:Inorganic Chemistry
[American Chemical Society]
日期:2020-03-18
卷期号:59 (7): 4825-4834
被引量:38
标识
DOI:10.1021/acs.inorgchem.0c00115
摘要
The separation of a mixture of C2H2 and CO2 is a great challenge due to their similar molecular sizes and shapes. Al-based metal–organic frameworks (Al-MOFs) have great promise for gas separation applications due to their light weight, high stability, and low cost. However, the cultivation of suitable Al-MOF single crystals is extremely difficult and has limited their explorations up to now. Since In, Ga, and Al are all 3p-block metal elements, a systematic application of the periodic law to investigate 3p-MOFs will undoubtedly help in the understanding and development of worthy Al-MOF materials. Herein, we report the design of a robust 3p metal–organic framework platform (SNNU-150) and the systematic regulation of C2H2/CO2 separation by open 3p-block metal sites. X-ray single-crystal diffraction analysis reveals that SNNU-150 is a 3,6-connected 3D framework consisting of [M3O(COO)6] trinuclear secondary building units (SBUs) and tritopic nitrilotribenzoate (NTB) linkers. Small {[M3O(COO)6]4(NTB)6} tetrahedral cages and extra-large {[M3O(COO)6]10(NTB)14} polyhedral cages connect with each other to generate a hierarchically porous architecture. These 3p-MOFs present very high water, thermal, and chemical stability, especially for SNNU-150-Al, which can maintain its framework at 85 °C in water for 24 h and in a room-temperature environment for more than 30 days. IAST calculations, breakthrough experiments, and GCMC simulations all show that SNNU-150 MOFs have top-level C2H2/CO2 separation performance and follow the order Al-MOF > Ga-MOF > In-MOF.
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