Ultrathin polymer membranes on porous substrates exhibit excellent gas and ion permeability and have important applications in many fields, such as membrane separation and batteries. However, there is still a lack of facile and general methods for the direct preparation of ultrathin polymer membranes on porous substrates, especially from polymer solutions. Within this work, a new strategy to fabricate centimeter-size ultrathin polymer membranes (thickness down to 16nm) is presented directly on porous supports by using the liquid-liquid interfacial spin-coating technique. The method allows the preparation of ultrathin polymer membranes with a wide range of polymers, and the membranes are smooth and intact without cracks. The helium/methane separation performance is evaluated. As the membrane thickness increased from 40 to 180nm, the He/CH4 selectivity increased and then decreased. The ultrathin membrane provides a good He/CH4 selectivity of 8.8 and He permeance of 1 × 105 GPU, which is the highest value reported so far and more than 150 times higher than that of membranes with He/CH4 selectivity above eight in the literature. This new approach provides the possibility to explore the great potential of ultrathin membranes for separation.
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