In recent times, commercially available lithium ion batteries (LIBs) employ graphite, with a theoretical capacity of 372 mAh g^-1, as their anode material. To enhance the energy density of LIBs, alternative anode materials with higher capacities, such as Li metal, Si, and various alloys, have been extensively exploited. With its advantages of a higher theoretical capacity (4200 mAh g^-1), environmental friendliness, and terrestrial abundance, Si is particularly well-suited as an anode material for this purpose. Nevertheless, Si suffers from large volume variations (up to 300%) during lithiation/delithiation processes, leading to pulverization, low cycling efficiency, unstable solid electrolyte interphases (SEI), and permanent capacity losses.

There have been several scientific investigations and strategies to solve the issues related to the large volume changes in Si. Relevant breakthroughs have been made with the help of advanced nanotechnologies in terms of enhancing the cycle life and improving the cycle rate performance. Notable among them is the use of binding materials with improved adhesive properties, such as copolyimide, alginate, poly(acrylic acid) (PAA), carboxymethyl cellulose, polyamide-imide, polyimide, and polymers that form cross-linked networks. Moreover, enhancing the adhesive strength between the Si composite electrode and Cu current collector by coating the latter’s surface with a very thin polymeric layer has significantly enhanced the electrochemical performance of Si anodes. However, the mechanism underlying this improvement in performance was not clearly addressed.

In this presentation, a coupled chemo-mechanical model which considers the contact resistance as well as the influence of the attractive forces inside the contact area between the electrode and current collector was developed to study the effects of the adhesive strength of a binding material on the electrochemical performance of silicon-based lithium-ion batteries. The model predictions were validated with experimental data from coin-type half-cells composed of Li metal, Si electrodes, and Cu current collectors coated with binding materials with different adhesive strengths. The proposed model was used to investigate the effects of the adhesive strength and various cell design parameters on the specific capacity of the Si-based Li-ion cells.