Outstanding Low-Temperature Performance of Structure-Controlled Graphene Anode Based on Surface-Controlled Charge Storage Mechanism

The energy and power performance of lithium (Li)-ion batteries is significantly reduced at low-temperature conditions, which is mainly due to the slow diffusion of Li-ions in graphite anode. Here, it is demonstrated that the effective utilization of the surface-controlled charge storage mechanism through the transition from layered graphite to 3D crumpled graphene (CG) dramatically improves the Li-ion charge storage kinetics and structural stability at low-temperature conditions. The structure-controlled CG anode prepared via a one-step aerosol drying process shows a remarkable rate-capability by delivering ≈206 mAh g^–1 at a high current density of 10 A g^–1 at room temperature. At an extremely low temperature of −40 °C, CG anode still exhibits a high capacity of ≈154 mAh g^–1 at 0.01 A g^–1 with excellent rate-capability and cycling stability. A combination of electrochemical studies and density functional theory (DFT) reveals that the superior performance of CG anode stems from the dominant surface-controlled charge storage mechanism at various defect sites. This study establishes the effective utilization of the surface-controlled charge storage mechanism through structure-controlled graphene as a promising strategy to improve the charge storage kinetics and stability under low-temperature conditions.