期刊
INORGANIC CHEMISTRY
卷 60, 期 10, 页码 7070-7081出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c03688
关键词
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资金
- National Natural Science Foundation of China [21702038]
- China Postdoctoral Science Foundation [2020M670895]
- Shenzhen Fundamental Research Project [JCYJ20170811161344569]
- Natural Scientific Research Innovation Foundation in the Harbin Institute of Technology [HIT.NSRIF.2020061]
- Harbin Institute of Technology, Shenzhen
The synthesis of triazole-decorated silver(I)-based cationic metal-organic frameworks led to dimensional enhancement in MOFs, with fluoride groups aiding in the formation of highly electron-deficient internal pores. These 3D cationic MOFs demonstrated efficient dye adsorption and selective removal of anionic dyes, along with effective removal of oxoanions from water.
Four new triazole-decorated silver(I)-based cationic metal-organic frameworks (MOFs), {[Ag(L1)](BF4)}(n) (1), {[Ag(L1)](NO3)}(n) (2), {[Ag(L2)](BF4)}(n) (3), and {[Ag(L2)](NO3)}(n) (4), have been synthesized using two newly designed ligands, 3-fluoro-5-(4H-1,2,4-triazol-4-yl)pyridine (L1) and 3-(4H-1,2,4-triazol-4-yl)-5-(trifluoromethyl)pyridine (L2). When the fluorine atom was changed to a trifluoromethyl group at the same position, tremendous enhancement in the MOF dimensionality was achieved [two-dimensional to three-dimensional (3D)]. However, changing the metal salt (used for the synthesis) had no effect. The higher electron-withdrawing tendency of the trifluoromethyl group in L2 aided in the formation of higher-dimensional MOFs with different properties compared with those of the fluoro derivatives. The fluoride group was introduced in the ligand to make highly electron-deficient pores inside the MOFs that can accelerate the anion-exchange process. The concept was proved by density functional theory calculation of the MOFs. Both 3D cationic MOFs were used for dye adsorption, and a remarkable amount of dye was adsorbed in the MOFs. In addition, owing to their cationic nature, the MOFs selectively removed anionic dyes from a mixture of anionic, cationic, and neutral dyes in the aqueous phase. Interestingly, the present MOFs were also highly effective for the removal of oxoanions (MnO4- and Cr2O72-) from water.
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