Highly Stable Germanium Microparticle Anodes with a Hybrid Conductive Shell for High Volumetric and Fast Lithium Storage

ACS Appl Mater Interfaces. 2022 Jan 12;14(1):750-760. doi: 10.1021/acsami.1c18607. Epub 2021 Dec 22.

Abstract

The ability to realize a highly capacitive/conductive electrode is an essential factor in large-scale devices, requiring a high-power/energy density system. Germanium is a feasible candidate as an anode material of lithium-ion batteries to meet the demands. However, the application is constrained due to low charge conductivity and large volume change on cycles. Here, we design a hybrid conductive shell of multi-component titanium oxide on a germanium microstructure. The shell enables facile hybrid ionic/electronic conductivity for swift charge mobility in the germanium anode, revealed through computational calculation and consecutive measurement of electrochemical impedance spectroscopy. Furthermore, a well-constructed electrode features a high initial Coulombic efficiency (90.6%) and stable cycle life for 800 cycles (capacity retention of 90.4%) for a fast-charging system. The stress-resilient properties of dense microparticle facilitate to alleviate structural failure toward high volumetric (up to 1737 W h L-1) and power density (767 W h L-1 at 7280 W L-1) of full cells, paired with highly loaded NCM811 in practical application.

Keywords: core−shell structure; fast charging; germanium microparticle; hybrid conductivity; sequential reduction reaction; volumetric energy density.