Design of interchain hydrogen bond in polyimide membrane for improved gas selectivity and membrane stability

Polyimide has been widely investigated as a potential material for gas separation. The post-crosslinking of polyimide could increase gas selectivity and membrane stability due to increase of chain-packing density and chain stiffness. However, common crosslinking strategies tend to destroy the chemical structure of polyimide. In this work, a strong hydrogen bond among polymer chains of 6FDA-durene polyimide (Du-PI) membranes is designed by introducing isophthalic dihydrazide (IPD) molecules as cross-linker. The formation of hydrogen bond between Du-PI and IPD strengthens the polymer interchain interaction and regulates interchain spacing but without breaking the chemical structure of Du-PI. The resulting IPD/Du-PI membranes exhibit largely enhanced mechanical strength and anti-plasticization property in comparison with pristine Du-PI membranes. In addition, due to the increased packing density of polymer chains, the membranes show obviously increased gas perm-selectivity by 296%, 505%, 125%, 66%, and 171% for H2/N2, H2/CH4, H2/CO2, O2/N2, and CO2/CH4 gas pair in the case of 20% IPD/Du-PI membrane. The use of IPD as cross-linker has demonstrated herein to be a facile and effective strategy to strengthen the inter-polymer chain interaction and simultaneously improve membrane stability in a mild way.