p-Phenylenediamine-Bridged Binder-Electrolyte-Unified Supramolecules for Versatile Lithium Secondary Batteries

The binder is an essential component in determining the structural integrity and ionic conductivity of Li-ion battery electrodes. However, conventional binders are not sufficiently conductive and durable to be used with solid-state electrolytes. In this study, a novel system is proposed for a Li secondary battery that combines the electrolyte and binder into a unified structure, which is achieved by employing para-phenylenediamine (pPD) moiety to create supramolecular bridges between the parent binders. Due to a partial crosslinking effect and charge-transferring structure of pPD, the proposed strategy improves both the ionic conductivity and mechanical properties by a factor of 6.4 (achieving a conductivity of 3.73 x 10-4 S cm-1 for poly(ethylene oxide)-pPD) and 4.4 (reaching a mechanical strength of 151.4 kPa for poly(acrylic acid)-pPD) compared to those of conventional parent binders. As a result, when the supramolecules of pPD are used as a binder in a pouch cell with a lean electrolyte loading of 2 mu L mAh-1, a capacity retention of 80.2% is achieved even after 300 cycles. Furthermore, when it is utilized as a solid-state electrolyte, an average Coulombic efficiency of 99.7% and capacity retention of 98.7% are attained under operations at 50 degrees C without external pressure or a pre-aging process. A binder-electrolyte integrated solid-state battery (SSB) system exploiting a new synergistic ionic conduction mechanism through supramolecular bridging with p-phenylenediamine molecules is proposed. As such, the contact issue in SSBs can be minimized, enabling the implementation of high loading SSB systems. These achievements are expected to provide a strong foundation for the development of SSB systems with exceptional energy density.image