De novo assembly of frustrated Lewis pair bearing metal-organic frameworks for atmospheric CO₂ cycloaddition

Porous frustrated Lewis pairs (FLPs) have been demonstrated as cutting-edge heterogeneous catalysts in acidic-basic catalysis, which, yet faces great challenges in synthesis. Herein, we propose a one-step de novo assembly strategy for constructing porous FLPs by capping monodentate ionic liquids (ILs) on metal clusters during the synthesis of metal-organic frameworks (MOFs). The capping of ILs makes adjacent metal sites on MOFs transforming to coordinatively-unsaturated metal Lewis acids, producing FLPs containing Lewis basic Cl- ions from ILs and metal sites. The distribution of ILs on the framework of MOFs endows the catalysts with large surface areas (up to 2125 m(2) g(-1)), open channels and good stability. The porous FLPs behave unprecedented activity for atmospheric CO2 activation and coupling with epoxides (25-40(degrees)C, 1 bar, without cocatalyst). This de novo assembly strategy exhibits good universality for synthesizing porous FLPs from different kinds of ILs, paving a facile approach for designing high-efficiency acidic-basic catalysts.