Hollow fiber thin-film composite membrane regulated by macrocyclic polyamine molecules for high performance organic solvent nanofiltration

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Organic solvent nanofiltration (OSN) technology has the potential to separate and purify organic solvents in high efficiency. The self-supporting structure and ease scaling-up merit of hollow fiber (HF) type membrane make it an attractive option for OSN application. Nevertheless, low solvent permeance is one of technical limitation in conventional HF OSN membranes due to their excessively dense separation layer and limited free volume. Herein, we propose a straightforward methodology to fabricate HF thin-film composite (TFC) OSN membranes having exceptional solvent permeance and solute rejection. This methodology is conducted through the incorporation of macrocyclic molecules, 1,4,7,10-tetraazacyclododecane (Cyclen), into the aqueous monomer solution of m-Phenylenediamine (MPD) during the interfacial polymerization to modulate the separation layer. In this way, the average pore size of the separation layer could be precisely enlarged and narrowed on a sub-nanometer scale. Consequently, the Cyclen-modulated HF TFC OSN membrane exhibits excellent separation performance, with a pure methanol permeance of 76.7 L m−2 h−1 MPa−1 and a pure ethanol permeance of 26.5 L m−2 h−1 MPa−1, which is nearly 60 % increase compared with the baseline TFC membrane, while the Rhodamine B (RDB) rejection only shows a neglectable decrease from 99.7 % to 99.6 % at optimal fabrication conditions. Furthermore, the optimal membrane exhibits remarkable solvent resistance, withstanding a 35 d immersion in N, N-dimethylformamide (DMF) at room temperature without a significant decline in RDB rejection. Additionally, the optimal membrane shows higher than 99 % rejection for Rifampicin (823 Da), which is considerable potential for applications in the separation and recovery of pharmaceuticals. In summary, incorporating macrocyclic polyamine Cyclen into the polyamide layer is a viable method for regulating the physical structure and strengthening the performance of HF OSN membrane.