期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 138, 期 17, 页码 5678-5684出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.6b02030
关键词
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资金
- NSF of China [21203022, 21261001, 21361001]
- Natural Science Foundation of Jiangxi Province of China [20143ACB20002]
- Young Scientist Training Program of Jiangxi Province of China [20142BCB23018]
- KAUST for the Competitive Research Funds [FCC/1/1972-02-01]
- Welch Foundation [AX-1730]
A new metal-organic framework Zn-2(H2O)-(dobdc)center dot 0.5(H2O) (UTSA-74, H4dobdc = 2,5-dioxido-1,4-benzenedicarboxylic acid), Zn-MOF-74/CPO-27-Zn isomer, has been synthesized and structurally characterized. It has a novel four coordinated fgl topology with one-dimensional channels of about 8.0 A. Unlike metal sites in the well established MOF-74 with a rod-packing structure in which each of them is in a five coordinate square pyramidal coordination geometry, there are two different Zn2+ sites within the binuclear secondary building units in UTSA-74 in which one of them (Znl) is in a tetrahedral while another (Zn2) in an octahedral coordination geometry. After activation, the two axial water molecules on Zn2 sites can be removed, generating UTSA-74a with two accessible gas binding sites per Zn2 ion. Accordingly, UTSA-74a takes up a moderately high and comparable amount of acetylene (145 cm(3)/cm(3)) to Zn-MOF-74. Interestingly, the accessible Zn2+ sites in UTSA-74a are bridged by carbon dioxide molecules instead of being terminally bound in Zn-MOF-74, so UTSA-74a adsorbs a much smaller amount of carbon dioxide (90 cm3/cm3) than Zn-MOF-74 (146 cm3/cm3) at room temperature and 1 bar,, leading to a superior MOF material for highly selective C2H2/CO2 separation. X-ray crystal structures, gas sorption isotherms, molecular modeling, and simulated and experimental breakthroughs comprehensively support this result.
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