Highly Selective Adsorption of Para‐Xylene, Ethylbenzene, and Explicit Exclusion of Ortho‐Xylene from Xylene Isomers Using a Pillar‐Layered MOF with Tuned Pore Channels

W4412492967 · 수집 2026-10-04 18:16:38

T11362 Membrane Separation and Gas Transport

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Xylene isomer separation is a long-standing challenge due to the nearly identical properties of para-xylene (PX), meta-xylene (MX), ortho-xylene (OX), and ethylbenzene (EB). Here, we report a rationally designed pillar-layered metal-organic framework (MOF), Ni-HDB, incorporating a cylindrical 1,4-diazabicyclo[2.2.2]octane (DABCO) pillar that blocks lateral channels and directs molecular transport through elliptical windows (3.2 × 6.7 Å<sup>2</sup>). These apertures closely match the dimensions of PX and EB, enabling kinetic sieving. As a result, Ni-HDB exhibits high selectivity for PX and EB, moderate selectivity for MX, and exclusion of OX under ambient conditions. It achieves record liquid-phase selectivities for EB/OX (1943), PX/OX (951), and MX/OX (158), along with high PX and MX adsorption capacities. Comparative studies with isoreticular analogues confirm that DABCO-driven confinement is key to enhancing size-based selectivity. Density functional theory calculations indicate kinetic preference for PX and EB, thermodynamic favorability for MX, and exclusion of OX. Ni-HDB also shows excellent thermal and structural stability, with no performance loss over ten cycles. These results highlight the importance of channel geometry in MOFs and provide a framework for developing next-generation adsorbents for energy-efficient hydrocarbon separations.

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