Effective Gas Separation Performance Enhancement Obtained by Constructing Polymorphous Core–Shell Metal–Organic Frameworks

We reported a new polymorphous core–shell metal–organic framework (MOF) in the form of a three-dimensional MOF core wrapped in a two-dimensional layered MOF shell by applying a general acid–solvent synergy synthesis. This hybrid material can achieve high adsorptive selectivity/capacity simultaneously, which is validated by the unary isotherms of CO2 and N2 conducted at 273 K (0–1 bar). The MOF-S@MOF-C with a 7-day exchange showed the highest CO2/N2 selectivity (32.7) among our samples and a moderate CO2 capacity (2.3 mmol/g), which are 3 times and 1.6 times those of the MOF-C and MOF-S, respectively. We attributed the enhanced selective adsorption performance to the negligible N2 uptake exhibited by the outer shell of MOF-S@MOF-C. This study provides a new route for elevating gas separation performance by constructing multifunctional core–shell materials.