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Introduction of functionality into a Tb(III)-organic framework via mixed-ligand strategy for selective C2H2 capture and ratiometric Cr(VI) detection

Chen Di-Ming,Han-Dong Qiao,Shao-Ming Fang

Introduction of porosity and fluorescent properties into lanthanide metal–organic frameworks (MOFs) with rational design to achieve multifunctional use is of great significance from the energy and environmental viewpoint. In this study, a microporous Tb(III)-based MOF with the formula of {[Tb 2 (oba) 3 (Phen) 2 ](DMF) 2 (H 2 O) 4 } n ( 1 ) was solvothermally prepared via using the mixed ligands of 1,10-phenanthroline (Phen) and 4,4′-oxybis(benzoic acid) (H 2 oba) as organic connecters. The structural evaluation results indicate that complex 1 is composed of binuclear Tb 2 (CO 2 ) 6 (Phen) 2 clusters which are extended by the oba 2− ligands to afford a two-fold interpenetrated framework with one-dimensional microporous channels along the b -axis. Gas sorption studies show that the activated 1 demonstrates a high ideal adsorption solution theory (IAST) sorption selectivity of 7.4 toward C 2 H 2 in a C 2 H 2 /CO 2 gas mixture, which are further supported by the dynamic breakthrough experiments. The grand canonical Monte Carlo (GCMC) simulation results indicate that the synergistic effects of the H-bond interactions of C 2 H 2 with oba 2− ligands and the C–H···π interactions with Phen ligand contribute to the strong binding of the framework toward C 2 H 2 molecules. What's more, the luminescent measurements reveal that the emission of 1 features both the characteristic peaks of Phen ligand and Tb(III) ion, which could be further applied as a self-calibrating sensor for the Cr(VI) detection in water. To the best of our knowledge, complex 1 represents the first example of Tb-MOF holding such a high C 2 H 2 /CO 2 selectivity together with ratiometric Cr(VI) detection performances.