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Stepwise Construction of New Different Heterometallic-Organic Frameworks (HMOFs) for Highly Efficient CO2 Fixation.

Coordination preference of different metal ions and ligands push forward immense influence on the constructions of functional MOF materials. In this work, two new monometallic complexes, namely [Ag(HL)(bipy)0.5] (1), and {[Tb(L)1.5(H2O)]∙4H2O}n (2) (bipy = 4,4-bipyridine), have been firstly synthesized successfully by employing a bifunctional 2-(imidazol-1-yl)terephthalic acid (H2L) ligand. After that, two new different heterometallic-organic frameworks (HMOFs), namely {[TbAg(L)2(H2O)3]∙H2O}n (3), and [TbAg(L)2(H2O)]n (4), were obtained by complexes 1 and 2 as the precursors based on the rational stepwise construction strategy and theory of hard and soft acids and bases (HSAB principle), respectively. The HMOFs bearing dual metallic catalytic sites (Tb and Ag) can be used as heterogeneous catalysts without losing performance for the chemical fixation of CO2 with epoxides including the sterically hindered epoxides, demonstrating some of the highest reported catalytic activity values. This work may build up a new synthetic route toward tailoring more new HMOFs with excellent catalytic activity.