Highly Stretchable Polyurethane Porous Membranes with Adjustable Morphology for Advanced Lithium Metal Batteries

A highly flexible, tunable morphology membrane with excellent thermal stability and ionic conductivity can endow lithium metal batteries with high power density and reduced dendrite growth. Herein, a porous Polyurethane (PU) membrane with an adjustable morphology was prepared by a simple nonsolvent–induced phase separation technique. The precise control of the final morphology of PU membranes can be achieved through appropriate selection of a nonsolvent, resulting a range of pore structures that vary from finger–like voids to sponge–like pores. The implementation of combinatorial DFT and experimental analysis has revealed that spongy PU porous membranes, especially PU−EtOH, show superior electrolyte wettability (472%), high porosity (75%), good mechanical flexibility, robust thermal dimensional stability (above 170 °C), and elevated ionic conductivity (1.38 mS cm⁻¹) in comparison to the polypropylene (PP) separator. The use of PU−EtOH in Li//Li symmetric cell results in a prolonged lifespan of 800 h, surpasing the longevity of PU or PP cells. Moreover, when subjected to a high rate of 5 C, the LiFePO₄/Li half-cell with a PU−EtOH porous membrane displayed better cycling performance (115.4 mAh g⁻¹) compared to the PP separator (104.4 mAh g⁻¹). Finally, the prepared PU porous membrane exhibits significant potential for improving the efficiency and safety of LMBs.