Abnormal electrochemical behavior of rounded graphite

Round-shaped natural graphite is commonly used as anode material for rechargeable lithium-ion batteries. We report atypical electrochemical behavior of round-shaped graphite anodes in Li-ion batteries: an intriguing phenomenon whereby substantial progressive increase in capacity is observed over tens of cycles. To understand the reasons underlying this abnormal behavior, we investigated the surface and bulk structure properties using HRSEM, XRD and Raman spectroscopy. Graphite particles with tense structure undergo exfoliation and fracture due to multiple transformations in intercalation/deintercalation processes. The increased capacity may result from enhanced particle exfoliation, compared with non-rounded graphite, which is accompanied by appearance of graphene sheets and fracture.