Tartaric acid anion intercalated layered double hydroxides constructed a CO2-favorable transport channel in PIM-1 mixed matrix membranes for CO2/N2 separation

As a unique polymer of intrinsic microporosity, PIM-1 has great potential in mixed matrix membranes (MMMs) for gas separation with ultra-high permeability. However, the separation performance, e.g. CO2/N2 separation, is still limited by its poor selectivity. In this work, PIM-1-based MMMs containing tartaric acid anion intercalated layered double hydroxides (TA-LDH) nanofillers are successfully prepared. The uniformly dispersed TA-LDH in the PIM-1 matrix contributes to optimizing the stacking of polymer chains for accessible pores, which is conducive to CO2 diffusion. In addition, the assistant experiment and theoretical calculation point out that the -COO-, –OH between the TA-LDH layers had an affinity for CO2, creating a two-dimensional fast transport channel between the enlarged interlayer space. Compared with the pristine PIM-1 membrane, the CO2 permeability and CO2/N2 selectivity of 0.7 % TA-LDH/PIM-1 membrane is increased by 43.19 % and 105.48 %. The excellent gas separation performance with CO2 permeability of 8343.18 Barrer and CO2/N2 selectivity of 39.02 exceeds the 2019 Robson upper limit. This paves a new way to improve the gas separation performance of PIM-1-based MMMs and suggests high perspectives for real applications. [Display omitted] •Tartaric acid anion increased LDH layer spacing and had an affinity for CO2.•A specific CO2 fast transport channel was designed to improve the rate of CO2 diffusion.•Molecular simulation and dissolution-diffusion mechanism studied separation mechanism.•0.7 % TA-LDH/PIM-1 MMM showed significant CO2 permeability and CO2/N2 selectivity.