We describe a new strategy to prepare thermally- and electrochemically-stable polyimide (PI) nanofiber membranes by the hot-press treatment of polyamic acid (PAA) nanofiber sheets in situ and examine their performance as Li-ion battery separators. Typical thermal imidization of PAA to PI membranes using sequential high temperature treatments in an oven takes a long time, but our method readily completes this conversion process at a mild temperature in 30 min while generating a high probability of inter-nanofiber imidization. Along with the improved electrolyte uptake capability and uniform distribution of the pore size and porosity caused by the dense and compact arrangements, the hot-press-induced PI membrane exhibits relatively thin sheets and a much greater mechanical strength than the membrane prepared by the thermal treatment. Subsequently, these PI-based membranes are installed in Li-ion full coin cells as battery separators whose C-rate (charging and discharging) performances are comparable to a commercial polyethylene (PE) separator. In addition, the highly improved thermal stabilities of these PI separators over PE separators are observed during thermal shrinkage and hot-box tests. Overall, our strategy can allow for the manufacture of diverse PI-based membranes with minimal preparation time and cost that can be utilized in high power portable devices requiring thermal and electrochemical stability.
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