Reinforcing Germanium Electrode with Polymer Matrix Decoration for Long Cycle Life Rechargeable Lithium Ion Batteries

Germanium is a promising anode material for lithium ion batteries because of its high theoretical specific capacity and low operation voltage. However, a significant challenge in using Ge-based anodes is the large volume variation during cycling that causes pulverization and capacity fade. Despite intense studies in the past decade, unsatisfactory cycling stability of the Ge-based electrodes still impedes their widespread applications. In this study, we demonstrate a high-performance electrode through the synergistic combination of a high-capacity Ge film grown on a three-dimensional current collector and an in situ formed poly(vinylidene fluoride)-hexafluoropropene/SiO₂ protective layer. Specifically, the polymer matrix is in continuous contact with the surface of the Ge shell, which provides improved mechanical and ionic transport properties. As a highlight, we present impressive cycling stability over 3000 cycles at 1 C rate with a capacity retention as high as 95.7%. Furthermore, the LiCoO₂-Ge full battery operates at an average voltage of 3.3 V at 0.5 C and maintains good electrochemical performance, suggesting great potential for applications in energy storage and conversion devices.