Revisiting the Roles of Natural Graphite in Ongoing Lithium‐Ion Batteries

Graphite, commonly including artificial graphite and natural graphite (NG), possesses a relatively high theoretical capacity of 372 mA h g–1 and appropriate lithiation/de‐lithiation potential, and has been extensively used as the anode of lithium‐ion batteries (LIBs). With the requirements of reducing CO2 emission to achieve carbon neutral, the market share of NG anode will continue to grow due to its excellent processability and low production energy consumption. NG, which is abundant in China, can be divided into flake graphite (FG) and microcrystalline graphite (MG). In the past 30 years, many researchers have focused on developing modified NG and its derivatives with superior electrochemical performance, promoting their wide applications in LIBs. Here, a comprehensive overview of the origin, roles, and research progress of NG‐based materials in ongoing LIBs is provided, including their structure, properties, electrochemical performance, modification methods, derivatives, composites, and applications, especially the strategies to improve their high‐rate and low‐temperature charging performance. Prospects regarding the development orientation as well as future applications of NG‐based materials are also considered, which will provide significant guidance for the current and future research of high‐energy‐density LIBs. A comprehensive overview of natural graphite‐based materials in ongoing lithium‐ion batteries is presented, covering fundamental mechanisms, detailed applications, and an outlook of natural graphite‐based materials, from not only the aspects of structure and properties, modifications, derivatives, and composites, but also perspectives in terms of natural graphite in hybrid lithium‐ion/lithium‐metal cells and all‐solid‐state lithium batteries.