Cylindrical-type cells have been widely adopted by major battery and electric vehicle manufacturers owing to their price competitiveness, safety, and easy expandability. However, placement of electrodes at the core of cylindrical cells is currently restricted because of high electrode curvature and the lack of specialized electrodes and electrode materials. Here, we report the realization of highly flexible high-energy-density electrodes (active material loading of >98.4%) that can be used at the cores of cylindrical cells. The improved properties result from the introduction of a multifunctional poly(melamine-co-formaldehyde) (MF copolymer) additive, which yields a relatively more fluidic and well-dispersed slurry using only 0.08 wt %. MF copolymer-mediated formation of completely wrapped CNT/PVDF networks on LiCoO2 (LCO) and accompanying contact enhancement between LCO and carbon nanotubes (CNTs) resulted in an increase of electrical and mechanical properties of the two types (composites with or without collectors) of electrodes compared with those of additive-free electrodes. Flexibility tests were carried out by rolling electrodes onto cylinder substrates (diameters of ca. 1 and 10 mm); this process resulted in relatively lower resistance changes of the MF copolymer-containing electrodes than for the reference electrodes. In addition, capacity retention after 100 cycles for cells with and without MF copolymers was approximately 10-20% better for the samples with the MF copolymer than for those without. CNT/PVDF networks with MF copolymers were proven to induce a relatively thin and stable cathode electrolyte interface layer accompanying the chemical bond formation during cycling.
Keywords: composite interfaces; conductive additive/binder networks; electrode additives; high-energy-density electrodes; lithium-ion batteries.