ORS6-0185
Functional Primer Design Formulating Energy-dense Battery Electrodes
When and Where
Nov 30, -0001
12:00am - 12:00am
Presenter(s)
Jaegeon Ryu (Sogang University)
Co-Author(s)
Abstract
Silicon (Si) anodes are among the most promising candidates for next-generation lithium-ion batteries owing to their exceptionally high theoretical capacity (~3500 mAh g⁻¹). However, their practical implementation is severely hampered by the enormous volumetric expansion (~400%) during cycling, which leads to particle pulverization, continuous SEI reconstruction, and rapid capacity decay — particularly at high active material contents. Conventional interfacial strategies have provided only limited improvements, failing to simultaneously address mechanical, ionic, and chemical demands at the electrode level. Herein, we report an interfacially tunable functional primer designed to serve as a multifunctional bridging agent within the Si electrode matrix. The primer is constructed from a thermally crosslinked polyarylene backbone combined with soft segments, enabling both mechanical rigidity and elastic adaptability. Upon thermal curing, a conformal and robust polymeric network forms on the Si surface via ring-opening polymerization, establishing strong Si–O–C anchoring bonds. The primer fulfills three synergistic roles. First, the dynamic soft chain exchange accommodates volumetric expansion while maintaining interfacial continuity with the binder, as confirmed by SAICAS and rheological analyses demonstrating superior cohesive strength even under electrolyte-wetted conditions. Second, the π-conjugated polyarylene backbone promotes strong π–π interactions with conductive carbon additives, yielding a homogeneous electron percolation network with reduced electrode resistance. Third, the ionophoric carbonyl and hydroxyl groups within the primer facilitate Li⁺ desolvation and accelerate interfacial ion transport — approximately 20 times faster than conventional binder interfaces — without immobilizing ions, thereby suppressing concentration polarization and enabling stable high-rate cycling. These synergistic effects enabled stable electrochemical operation of a nearly binder-free electrode with an unprecedented nearly all active material content (~99 wt%) representing the lowest reported binder content among Si-based anodes. This concept has been further validated in the ultrathick formulation and high-energy full cell configuration.
