Engineering Dual CO2‐ and Photothermal‐Responsive Membranes for Switchable Double Emulsion Separation

Abstract Stimulus‐responsive membranes demonstrate promising applications in switchable oil/water emulsion separations. However, they are unsuitable for the treatment of double emulsions like oil‐in‐water‐in‐oil (O/W/O) and water‐in‐oil‐in‐water (W/O/W) emulsions. For efficient separation of these complicated emulsions, fine control over the wettability, response time, and aperture structure of the membrane is required. Herein, dual‐coated fibers consisting of primary photothermal‐responsive and secondary CO 2 ‐responsive coatings are prepared by two steps. Automated weaving of these fibers produces membranes with photothermal‐ and CO 2 ‐responsive characteristics and narrow pore size distributions. These membranes exhibit fast switching wettability between superhydrophilicity (under CO 2 stimulation) and high hydrophobicity (under near‐infrared stimulation), achieving on‐demand separation of various O/W/O and W/O/W emulsions with separation efficiencies exceeding 99.6%. Two‐dimensional low‐field nuclear magnetic resonance and correlated spectra technique are used to clarify the underlying mechanism of switchable double emulsion separation. The approach can effectively address the challenges associated with the use of stimulus‐responsive membranes for double emulsion separation and facilitate the industrial application of these membranes.