Introducing a Pseudocapacitive Lithium Storage Mechanism into Graphite by Defect Engineering for Fast-Charging Lithium-Ion Batteries

ACS Appl Mater Interfaces. 2022 Apr 13;14(14):16279-16288. doi: 10.1021/acsami.2c02169. Epub 2022 Mar 29.

Abstract

The extreme fast-charging capability of lithium-ion batteries (LIBs) is very essential for electric vehicles (EVs). However, currently used graphite anode materials cannot satisfy the requirements of fast charging. Herein, we demonstrate that intrinsic lattice defect engineering based on a thermal treatment of graphite in CO2 is an effective method to improve the fast-charging capability of the graphite anode. The activated graphite (AG) exhibits a superior rate capability of 209 mAh g-1 at 10 C (in comparison to 15 mAh g-1 for the pristine graphite), which is attributed to a pseudocapacitive lithium storage behavior. Furthermore, the full cell LiFePO4||AG can achieve SOCs of 82% and 96% within 6 and 15 min, respectively. The intrinsic carbon defect introduced by the CO2 treatment succeeds in improving the kinetics of lithium ion intercalation at the rate-determining step during lithiation, which is identified by the distribution of relaxation times (DRT) and density functional theory (DFT) calculations. Therefore, this study provides a novel strategy for fast-charging LIBs. Moreover, this facile method is also suitable for activating other carbon-based materials.

Keywords: density functional theory calculation; distribution of relaxation times; fast charging; intrinsic carbon defects; pseudocapacitive.