Interlayer Expansion in a Layered Metal-Organic Framework Enhances CO 2 Capture and CO 2 /N 2 Separation.

Developing efficient CO 2 adsorbent materials and technologies is significant to reduce the increasing greenhouse gases concentration in the atmosphere. Herein, a layered MOF with a porous kagomé lattice (kgm), which owned three phases (kgm-1, kgm-2, and kgm-3) via interlayer expansion, was evaluated as a promising CO 2 capture and separation material by using grand canonical Monte Carlo simulations. Results showed that the interlayer expansion provided additional pore volume, which played a considerable role in CO 2 adsorption and separation. The CO 2 adsorption capacity and CO 2 /N 2 selectivity followed the sequence kgm-3>kgm-2>kgm-1, and kgm-3 exhibited an excellent CO 2 adsorption capacity of 8.7 mmol g -1 at 1 bar with a CO 2 /N 2 selectivity of 130.3 at 20 bar and 298 K. Gas distribution analysis showed that CO 2 and N 2 are adsorbed only in the channels in kgm-1, whereas they could be adsorbed between layers in kgm-2 and kgm-3 due to the interlayer expansion. The adsorption heat and interactions between CO 2 and frameworks were analyzed to elucidate the effect of interlayer expansion. Results of this work highlighted that appropriate interlayer expansion can be an effective approach for framework adsorbents to improve CO 2 capture ability and separation performance at the same time.