Microporous Adsorbent-Based Mixed Matrix Membranes for CO2/N2 Separation

Abstract

As the atmospheric carbon dioxide (CO2) concentration rapidly rises, carbon capture, utilization, and storage (CCUS) is an emerging field for climate change mitigation. Various carbon capture technologies are in development with the help of adsorbents, membranes, solvent-based systems, etc. One of the main challenges in this field is the removal of CO2 from nitrogen (N2) gas. This paper focuses on mixed matrix membrane technology, for which the CO2/N2 separation performance is based on differences in gas permeations. Membrane separation and purification technologies are widely studied for carbon capture. Microporous adsorbents such as zeolites and metal organic frameworks (MOFs) for carbon capture have been attracting researchers’ attention due to their highly porous structures, high selectivity values, and tunable porosities. Utilizing microporous adsorbents dispersed within a novel, blended polymer matrix, fourteen membranes were prepared with the commercial MOF ZIF-8, zeolite 13X, and kaolin, with methyl cellulose (MC) and polyvinyl alcohol (PVA), which were tested using a single gas permeation setup in this study. The addition of polyallylamine (PAH) as a chemisorbent was also investigated. These membranes were synthesized both with and without a polyacrylonitrile (PAN) support to compare their performances. MC was found to be an ideal polymeric matrix component to develop free-standing MMMs. At 24 °C and a relatively low feed pressure of 2.36 atm, a free-standing zeolite-13X-based membrane (MC/PAH/13X/PVA) exhibited the highest N2/CO2 selectivity of 2.8, with a very high N2 permeability of 6.9 × 107 Barrer. Upon the optimization of active layer thickness and filler weight percentages, this easily fabricated free-standing MMM made of readily available materials is a promising candidate for CO2 purification through nitrogen removal.