科研之友
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摘要
The efficient capture of SO2 is of great significance in gas-purification processes including flue-gas desulfurization and natural-gas purification, but the design of porous materials with high adsorption capacity and selectivity of SO2 remains very challenging. Herein, the selective recognition and dense packing of SO2 clusters through multiple synergistic host-guest and guest-guest interactions by controlling the pore chemistry and size in inorganic anion (SiF62-, SIFSIX) pillared metal-organic frameworks is reported. The binding sites of anions and aromatic rings in SIFSIX materials grasp every atom of SO2 firmly via S delta+center dot center dot center dot F delta- electrostatic interactions and O delta-center dot center dot center dot H delta+ dipole-dipole interactions, while the guest-guest interactions between SO2 molecules further promote gas trapping within the pore space, which is elucidated by first-principles density functional theory calculations and powder X-ray diffraction experiments. These interactions afford new benchmarks for the highly efficient removal of SO2 from other gases, even if at a very low SO2 concentration. Exceptionally high SO2 capacity of 11.01 mmol g(-1) is achieved at atmosphere pressure by SIFSIX-1-Cu, and unprecedented low-pressure SO2 capacity is obtained in SIFSIX-2-Cu-i (4.16 mmol g(-1) SO2 at 0.01 bar and 2.31 mmol g(-1) at 0.002 bar). More importantly, record SO2/CO2 selectivity (86-89) and excellent SO2/N-2 selectivity (1285-3145) are also achieved. Experimental breakthrough curves further demonstrate the excellent performance of these hybrid porous materials in removing low-concentration SO2.
- 出版日期2017-7-26
- 单位浙江大学
