期刊
INORGANIC CHEMISTRY
卷 59, 期 6, 页码 4030-4036出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c00003
关键词
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资金
- National Natural Science Foundation of China [21661014, 21861020, 21561015, 21922810]
- Jiangxi Provincial Natural Science Foundation [20181BAB203001, 20171ACB20008]
A novel fluorinated biphenyldicarboxylate ligand of 3,3',5,5'-tetrafluorobipheny1-4,4'-dicarboxylic acid (H-2-TFBPDC) and its terbium metal-organic framework, {[Tb-2(TFBPDC)(3)(H2O)]center dot 4.5DMF center dot 0.5H(2)O}(n) (denoted as JXNU-6), were synthesized. JXNU-6 exhibits a three-dimensional (3D) framework built from one-dimensional (1D) terbium carboxylate helical chains bridged by TFBPDC2- linkers. The 3D framework of JXNU-6 features 1D fluorine-lined channels. The gas adsorption experiments show that the activated JXNU-6 (JXNU-6a) displays distinct adsorption behavior for propyne (C3H4) and propylene (C3H6) gases. The effective removal of a trace amount of C3H4 from C3H6 was achieved by JXNU-6a under ambient conditions, which is demonstrated by the column-breakthrough experiments. The modeling studies show that the preferential binding sites for C3H4 are the exposed F atoms on the pore surface in 1D channels. The strong C-H-F hydrogen bonds between C3H4 molecules and F atoms of TFBPDC2- ligands dominate the host-guest interactions, which mainly account for the excellent C3H4/C3H6 separation performance of JXNU-6a. This work provides a strategy for specific recognition toward C3H4 over C3H6 through the C-H center dot center dot center dot F hydrogen bond associated with the fluorinated organic ligand.
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