Holey graphite: A promising anode material with ultrahigh storage for lithium-ion battery

Abstract Recently, the 2019 Nobel prize in chemistry awards to three pioneers in the lithium-ion batteries (LIBs). However, the most commercially used anode for LIBs is still graphite, which suffers from the limited Li-ion storage of 372 mAh/g. To improve the performance of the intrinsic graphite anode (IGA), we use the ab initio calculations to examine the holey graphite anodes (HGAs) with three hole densities (35%: HGA35, 46%: HGA46 and 61%: HGA61) for LIBs. Remarkably, the maximum Li-ion storages of HGAs are up to 714–1689 mAh/g, which are about 2–4.5 times as high as that of the IGA (372 mAh/g). Besides, the in-plane diffusion barrier for Li-ions is also reduced from 0.57 eV (IGA) to 0.35–0.42 eV (HGAs), suggesting a higher Li-ion diffusion rate. The holey structures could open an extra out-plane Li-ions diffusing channel with only one-fifth of the diffusion barrier of that in the IGA, implying an accelerated charge/discharge process in the applications. We also demonstrate the relatively small surface area change ratio of less than 3%–14% in the HGAs upon adsorption of the maximum Li concentration. Therefore, the holey structure is a promising strategy to improve the graphite anode for LIBs significantly.