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) 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 LiFePO/Li half-cell with a PU-EtOH porous membrane displayed better cycling performance (115.4 mAh g) compared to the PP separator (104.4 mAh g). Finally, the prepared PU porous membrane exhibits significant potential for improving the efficiency and safety of LMBs.