A trade‐off behavior is noteworthy between protein rejection and pure water flux (PWF) for ultrafiltration membranes; it is recommendable to increase flux without reducing selectivity. The poly (meta‐phenylene isophthalamide) (PMIA) ultrafiltration membrane was modified via incorporating 1,3,5‐benzene tricarboxylic chloride (TMC) to optimize the performance for the first time. Molecular dynamics (MD) simulation was applied to probe the mechanism of the effects of the concentrations of cosolvent LiCl and addition TMC on the dissolving process. It was turned out that a suitable concentration of TMC in the dope solution markedly enhanced the PWF (from 276.22 to 566.20 m−2 h−1 bar−1) with an increasing bovine serum albumin rejection (from 92.05% to 94.64%). Besides, the optimized membrane also possesses excellent anti‐fouling and mechanical performance. These improvements can be due to the crosslinking between PMIA and TMC and enlarged average pore diameter. This work broadens the application of PMIA and TMC in ultrafiltration and provides a novel methodology for PMIA modification.
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