Tough Germanium Nanoparticles under Electrochemical Cycling

Abstract

Mechanical degradation of the electrode materials during electrochemical cycling remains a serious issue that critically limits the capacity retention and cyclability of rechargeable lithium-ion batteries. Here we report the highly reversible expansion and contraction of germanium nanoparticles under lithiation–delithiation cycling with <i>in situ</i> transmission electron microscopy (TEM). During multiple cycles to the full capacity, the germanium nanoparticles remained robust without any visible cracking despite ∼260% volume changes, in contrast to the size-dependent fracture of silicon nanoparticles upon the first lithiation. The comparative <i>in situ</i> TEM study of fragile silicon nanoparticles suggests that the tough behavior of germanium nanoparticles can be attributed to the weak anisotropy of the lithiation strain at the reaction front. The tough germanium nanoparticles offer substantial potential for the development of durable, high-capacity, and high-rate anodes for advanced lithium-ion batteries