Effects of the Formulations of Silicon‐Based Composite Anodes on their Mechanical, Storage, and Electrochemical Properties

In this work, the effects of the formulation of silicon‐based composite anodes on their mechanical, storage, and electrochemical properties were investigated. The electrode formulation was changed through the use of hydrogenated or modified (through the covalent attachment of a binding additive such as polyacrylic acid) silicon and acetylene black or graphene sheets as conducting additives. A composite anode with a covalently grafted binder had the highest elongation without breakages and strong adhesion to the current collector. These mechanical properties depend significantly on the conductive carbon additive used and the use of graphene sheets instead of acetylene black can improve elongation and adhesion significantly. After 180 days of storage under ambient conditions, the electronic conductivity and discharge capacity of the modified silicon electrode showed much smaller decreases in these properties than those of the hydrogenated silicon composite electrode, indicating that the modification can result in passivation and a constant composition of the active material. Moreover, the composite Si anode has a high packing density. Consequently, thin‐film electrodes with very high material loadings can be prepared without decreased electrochemical performance. In a bind: The modification of silicon surfaces for use in anodes through the covalent attachment of binder molecules has multiple effects, such as improved adhesion strength to the current collector, passivation, ease of electrode processability, enhanced nanoparticle packing density, improved resistance to stress during volume changes, and reduced parasitic material in the electrode formulation.