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The polydimethylsiloxane (PDMS) membrane commonly used for separation of biobutanol from fermentation broth fails to meet demand owing to its discontinuous and polluting thermal fabrication. Now, an UV‐induced polymerization strategy is proposed to realize the ultrafast and continuous fabrication of the PDMS membrane. UV‐crosslinking of synthesized methacrylate‐functionalized PDMS (MA‐PDMS) is complete within 30 s. The crosslinking rate is three orders of magnitude larger than the conventional thermal crosslinking. The MA‐PDMS membrane shows a versatile potential for liquid and gas separations, especially featuring an excellent pervaporation performance for n‐butanol. Filler aggregation, the major bottleneck for the development of high‐performance mixed matrix membranes (MMMs), is overcome, because the UV polymerization strategy demonstrates a freezing effect towards fillers in polymer, resulting in an extremely high‐loading silicalite‐1/MA‐PDMS MMM with uniform particle distribution.

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