Soluble polyimide binder for silicon electrodes in lithium secondary batteries

Abstract

A solvent-soluble polyimide (PI) polymeric binder was synthesized by a two-step reaction for silicon (Si) anodes for lithium-ion batteries. Polyamic acid was first prepared through ring opening between two monomers, bicyclo[2,2,2]oct-7-ene-2,3,5,6-tetracarboxylic dianhydride (BCDA) and 4,4-oxydianiline (ODA), followed by condensation reaction. Using the synthesized PI polymeric binder (molecular weight = ~10,945), the coating slurry was then prepared and Si anode was fabricated. For the control system, Si anode based on polyvinylidene fluoride (PVDF, molecular weight = ~350,000) having the same constituent ratio was prepared. During precycling, PI polymeric binder revealed much improved discharge capacity (2,167 mAh g-1) compared to that of using PVDF polymeric binder (1,740 mAh g-1), while the Coulombic efficiency of two systems were similar. PI polymeric binder improved the cycle retention ability during cycles compared to that of using PVDF, which is attributed to an improved adhesion property inside Si anode diminishing the dimensional stress during Si volume changes. The adhesion property of each polymeric binder in Si anode was confirmed by surface and interfacial cutting analysis system (SAICAS) (Si anode based on PI polymeric binder = 0.217 kN m-1 and Si anode based on PVDF polymeric binder = 0.185 kN m-1).