Precursor Induced Assembly of Si Nanoparticles Encapsulated in Graphene/Carbon Matrices and the Influence of Al2O3 Coating on their Properties as Anode for Lithium‐Ion Batteries

Abstract The theoretical capacity of pristine silicon as anodes for lithium‐ion batteries (LIBs) can reach up to 4200 mAh g −1 , however, the low electrical conductivity and the huge volume expansion limit their practical application. To address this challenge, a precursor strategy has been explored to induce the curling of graphene oxide (GO) flakes and the enclosing of Si nanoparticles by selecting protonated chitosan as both assembly inducer and carbon precursor. The Si nanoparticles are dispersed first in a slurry of GO by ball milling, then the resulting dispersion is dried by a spray drying process to achieve instantaneous solution evaporation and compact encapsulation of silicon particles with GO. An Al 2 O 3 layer is constructed on the surface of Si@rGO@C‐SD composites by the atomic layer deposition method to modify the solid electrolyte interface. This strategy enhances obviously the electrochemical performance of the Si as anode for LIBs, including excellent long‐cycle stability of 930 mAh g −1 after 1000 cycles at 1000 mA g −1 , satisfied initial Coulomb efficiency of 76.7%, and high rate ability of 806 mAh g −1 at 5000 mA g −1 . This work shows a potential solution to the shortcomings of Si‐based anodes and provides meaningful insights for constructing high‐energy anodes for LIBs.