Production of Stable Electrically Conductive PVDF Membranes Based on Polydopamine-Polyethyleneimine—Assisted Deposition of Carbon Nanotubes

Electrically conductive membranes (ECMs) have emerged as a multifunctional separation technology that integrates membrane filtration with electrochemical reactions. Physical stability remains a critical challenge for ECMs synthesized by coating polymer membranes with conductive materials. In this article, polydopamine (PDA) and polyethyleneimine (PEI) were used to facilitate the synthesis of significantly more stable ECMs using poly(vinylidene fluoride) (PVDF) ultrafiltration membranes and carbon nanotubes (CNTs). Four different synthesis methods were compared in terms of the final surface stability and separation properties: (1) CNTs deposited on PEI-crosslinked PDA-coated PVDF membranes, (2) PEI-crosslinked CNTs deposited on PDA-coated PVDF, (3) PDA, PEI and CNTs sequentially deposited layer-by-layer on PVDF, and (4) PEI-crosslinked PDA deposited on CNT-coated PVDF. The results revealed that method 1 generated ECMs with the greatest physical stability, highest electrical conductivity (18,518 S/m), and sufficient permeability (395.2 L/(m²·h·bar). In comparison, method 2 resulted in membranes with the highest permeability (2128.5 L/(m²·h·bar), but with low surface conductivity (502 S/m) and poor physical stability (i.e., 53–75% lower peel-off forces compared to other methods). Overall, methods 1, 3, and 4 can be used to make highly conductive membranes with a 97–99% removal of methyl orange by electrochemical degradation at −3 V.