Systematic Regulation of C2H2/CO2 Separation by 3p-Block Open Metal Sites in a Robust Metal–Organic Framework Platform
| Autor: | Hong-Juan Lv, Yong-Peng Li, Ying-Ying Xue, Yucheng Jiang, Shu-Ni Li, Mancheng Hu, Quan-Guo Zhai |
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| Rok vydání: | 2020 |
| Předmět: |
010405 organic chemistry
Chemistry 010402 general chemistry Block (periodic table) 01 natural sciences 0104 chemical sciences Inorganic Chemistry Metal Chemical engineering visual_art visual_art.visual_art_medium Tetrahedron Chemical stability Metal-organic framework Gas separation SBus Physical and Theoretical Chemistry Porosity |
| Zdroj: | Inorganic Chemistry. 59:4825-4834 |
| ISSN: | 1520-510X 0020-1669 |
| Popis: | 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. |
| Databáze: | OpenAIRE |
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