Protecting Silicon Film Anodes in Lithium-Ion Batteries Using an Atomically Thin Graphene Drape

Silicon (Si) shows promise as an anode material in lithium-ion batteries due to its very high specific capacity. However, Si is highly brittle, and in an effort to prevent Si from fracturing, the research community has migrated from the use of Si films to Si nanoparticle based electrodes. However, such a strategy significantly reduces volumetric energy density due to the porosity of Si nanoparticle electrodes. Here we show that contrary to conventional wisdom, Si films can be stabilized by two strategies: (a) anchoring the Si films to a carbon nanotube macrofilm (CNM) current collector and (b) draping the films with a graphene monolayer. After electrochemical cycling, the graphene-coated Si films on CNM resembled a tough mud-cracked surface in which the graphene capping layer suppresses delamination and stabilizes the solid electrolyte interface. The graphene-draped Si films on CNM exhibit long cycle life (>1000 charge/discharge steps) with an average specific capacity of ∼806 mAh g^-1. The volumetric capacity averaged over 1000 cycles of charge/discharge is ∼2821 mAh cm^-3, which is 2 to 5 times higher than what is reported in the literature for Si nanoparticle based electrodes. The graphene-draped Si anode could also be successfully cycled against commercial cathodes in a full-cell configuration.