Pressure‐Induced Dense and Robust Ge Architecture for Superior Volumetric Lithium Storage

Abstract

The germanium (Ge) anode attains wide attention in lithium‐ion batteries because of its high theoretical volumetric capacity (8646 mAh cm−3). However, the huge volume expansion (≈230%) results in its poor electrochemical performances. The strategies reported in the literature to solve the issue often cause a low packing density, lowering the volumetric capacity. Here, a pressure‐induced route is proposed to fabricate a Ge architecture, in which nano‐sized Ge (≈15 nm) is encapsulated by robust TiO2 and highly conductive carbon, which offer the advantages of a low stress–strain characteristic, low volume expansion in thickness change, high electrical conductivity (463.2 S m−1), high Li‐ion diffusion coefficient (9.55 × 10−9–8.51 × 10−12 cm2 s−1), and high tapping density (1.79 g cm−3). As a result, the dense architecture obtains outstanding volumetric capacities of 3559.8 mAh cm−3 at 0.1 A g−1 and 2628.2 mAh cm−3 at 20 A g−1, along with excellent cycling life over 5000 cycles at 10 A g−1. Remarkably, the full cell achieves a high volumetric energy density of 1760.1 Wh L−1, along with impressive fast‐charging performances and long cycling life. This work provides a new synthesis strategy and deep insight into the design of high‐volumetric capacity alloy‐based lithium‐ion‐battery anodes.