Controlling Binder Adhesion to Impact Electrode Mesostructures and Transport

The complex three-phase composition of lithium-ion battery electrodes, containing an ion-conducting pore phase, a nanoporous electronconducting carbon binder domain (CBD) phase, and an active material (AM) phase, provides several avenues of mesostructural engineering to enhance battery performance. We demonstrate a promising strategy for engineering electrode mesostructures by controlling the strength of adhesion between the AM and CBD phases. Using high-fidelity, physics-based colloidal and granular dynamics simulations, we predict that this strategy can provide significant control over electrochemical transport-relevant properties such as ionic conductivity, electronic conductivity, and available AM-electrolyte interface area. Importantly, the proposed strategy could be experimentally realized through surface functionalization of the AM and CBD phases and would be compatible with traditional electrode manufacturing methods.