Abstract

Mixed matrix membranes (MMMs) with one class of fillers always require high loadings to maximize gas permeability. The incompatibility between polymers and high content fillers causes non-selective interfacial voids in the MMMs and poor mechanical properties of MMMs. This work adopts two morphology distinct fillers with chemical similarity to achieve improved gas separation performance of Tröger’ base membranes without sacrificing their mechanical properties. The three-dimensional ZIF-8 nanoparticles are beneficial for membrane gas permeability. The addition of low content ZIF-8 nanosheets can greatly improve H2/CH4 and CO2/CH4 selectivities of the membranes. ZIF-8 particles and ZIF-8 nanosheets with similar chemical properties can mix more homogeneously and disperse well in the polymer matrix with expected hydrogen bonding interaction compared to mixed ZIF-8 and CuBDC nanosheets. Eventually, the resulting dual filler MMMs doped with 4 wt% ZIF-8 nanosheets and 10 wt% ZIF-8 nanoparticles have H2/CH4 ideal selectivity of 60 with H2 permeability of 426 Barrer, which is an increase of 18% and 102% over pure membranes, respectively. Moreover, the membrane has a significantly enhanced CO2/CH4 mixed gas selectivity of 68 at sub-ambient temperature, accompanied by temperature-dependent CO2-induced plasticization behavior. Mixing morphology distinct fillers with chemical similarity is proved to be an effective method to prepare a robust MMM at low filler amounts, and the synergistic effect on gas permeability and selectivity endows these dual filler MMMs with great H2/CH4 and CO2/CH4 separation performance.

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