期刊
JOURNAL OF MATERIALS CHEMISTRY A
卷 5, 期 10, 页码 4861-4867出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c6ta10785k
关键词
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资金
- National Natural Science Foundation of China [21471134, 21571158, 21601160]
- Innovation Scientists and Technicians Troop Construction Projects of Henan Province [152101510003]
- Program for Science & Technology Innovative Research Team in University of Henan Province [15IRTSTHN-002]
- Plan for Scientific Innovation Talent of Henan Province [154200510011]
- Startup Fund for PhDs of Natural Scientific Research of Zhengzhou University of Light Industry [2015BSJJ042]
Metal-organic frameworks (MOFs), as a class of adjustable porous crystalline materials, have received considerable attention in recent years. In this study, starting from an unstable MIL-88 type Co(II)-MOF as the prototype structure, two isoreticular stabilized MOFs with similar structural features but different water/thermal stabilities and acetylene sorption behaviors were prepared, which can be modulated by incorporating different functional brackets in the pores. MOF 1 equipped with open metal sites (OMSs) decomposed quickly in water solution, while the free N-donor functionalized MOF 2 could be stable in water with improved thermostability. The gas sorption study reveals that activated material 2 has a significantly enhanced acetylene uptake capacity with a lower Qst value than those of activated 1, showing a 79% increase (242 vs. 135 cm(3) g(-1)) at 273 K and 91% increase (165 vs. 86 cm(3) g(-1)) at 298 K. The acetylene uptake capacity of activated material 2 is extraordinarily high among MOFs without OMSs, and is even comparable to some famous MOFs with much stronger C2H2 binding ability which however require considerably higher energy for regeneration. The experimental results were further confirmed by the molecular mechanics (MM) calculations, grand canonical Monte Carlo (GCMC) simulations and density functional theory (DFT) studies.
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