金属有机骨架
选择性
化学
甲酸
苯甲酸
邻氨基苯甲酸
表面改性
锆
吸附
多孔性
苯胺
配体(生物化学)
吡啶
组合化学
无机化学
有机化学
催化作用
物理化学
受体
生物化学
作者
Athanasios Koutsianos,Ewa Kazimierska,Andrew R. Barron,Marco Taddei,Enrico Andreoli
出处
期刊:Dalton Transactions
[The Royal Society of Chemistry]
日期:2019-01-01
卷期号:48 (10): 3349-3359
被引量:63
摘要
Zirconium-based metal-organic frameworks (Zr-MOFs) are a subclass of MOFs known for their remarkable stability, especially in the presence of water. This makes them extremely attractive for practical applications, including CO2 capture from industrial emission sources; however, the CO2 adsorption capacity of Zr-MOFs is moderate compared to that of the best performing MOFs reported to date. Functionalization of Zr-MOFs with amino groups has been demonstrated to increase their affinity for CO2. In this work, we assessed the potential of post-synthetic defect exchange (PSDE) as an alternative approach to introduce amino functionalities at missing-cluster defective sites in formic acid modulated UiO-66. Both pyridine-containing (picolinic acid and nicotinic acid) and aniline-containing (3-aminobenzoic acid and anthranilic acid) monocarboxylates were integrated within defective UiO-66 with this method. Non-defective UiO-66 modified with linkers bearing the same amino groups (2,5-pyridinedicarboxylic acid and 2-aminoterephthalic acid) were prepared by classical post-synthetic ligand exchange (PSE), in order to compare the effect of introducing functionalities at defective sites versus installing them on the backbone. PSDE reduces the porosity of defective UiO-66, but improves both the CO2 uptake and the CO2/N2 selectivity, whereas PSE has no effect on the porosity of non-defective UiO-66, improving the CO2 uptake but leaving selectivity unchanged. Modification of defective UiO-66 with benzoic acid reveals that pore size reduction is the main factor responsible for the observed uptake improvement, whereas the presence of nitrogen atoms in the pores seems to be beneficial for increasing selectivity.
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