Controlling Binder Adhesion to Impact Electrode Mesostructure and Transport

The complex three-phase composition of lithium-ion battery electrodes - containing an ion-conducting pore phase, a nanoporous electron-conducting 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 surface 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.