High-density silicon composite anodes show large volume changes upon charging/discharging triggering the reformation of the solid electrolyte interface (SEI), an interface initially formed at the silicon surface. The question remains how the reformation process and accompanied material evolution, in particular for industrial up-scalable cells, impacts cell performance. Here, we develop a correlated workflow incorporating X-ray microscopy, field-emission scanning electron microscopy tomography, elemental imaging and deep learning-based microstructure quantification suitable to witness the structural and chemical progression of the silicon and SEI reformation upon cycling. The nanometer-sized SEI layer evolves into a micron-sized silicon electrolyte composite structure at prolonged cycles. Experimental-informed electrochemical modelling endorses an underutilisation of the active material due to the silicon electrolyte composite growth affecting the capacity. A chemo-mechanical model is used to analyse the stability of the SEI/silicon reaction front and to investigate the effects of material properties on the stability that can affect the capacity loss.

Polymer nanocomposites are increasingly important in food packaging sectors. Biopolymer pullulan is promising in manufacturing packaging films or coatings due to its excellent optical clarity, mechanical strength, and high water-solubility as compared to other biopolymers. This work aims to enhance its oxygen barrier properties and overcome its intrinsic brittleness by utilizing two-dimensional planar graphene oxide (GO) nanoplatelets. It has been found that the addition of only 0.2 wt% of GO enhanced the tensile strength, Young’s modulus, and elongation at break of pullulan films by about 40, 44 and 52%, respectively. The light transmittance at 550 nm of the pullulan/GO films was 92.3% and haze values were within 3.0% threshold, which meets the general requirement for food packaging materials. In particular, the oxygen permeability coefficient of pullulan was reduced from 6337 to 2614 mL μ m m ⁻² (24 h ⁻¹ ) atm ⁻¹ with as low as 0.05 wt% of GO loading and further to 1357 mL μ m m ⁻² (24 h ⁻¹ ) atm ⁻¹ when GO concentration reached 0.3 wt%. The simultaneous improvement of the mechanical and oxygen barrier properties of pullulan was ascribed to the homogeneous distribution and prevalent unidirectional alignment of GO nanosheets, as determined from the characterization and theoretical modelling results. The exceptional oxygen barrier properties of pullulan/GO nanocomposites with enhanced mechanical flexibility and good optical clarity will add new values to high performance food packaging materials.