The performance of lithium (Li)-ion batteries (LIBs) significantly decreases at low temperatures, primarily due to the slow diffusion of Li ions within the graphite anode. This issue often necessitates the use of complex thermal control systems to safeguard the batteries, enhancing their cost, mass, and volume, especially under extreme conditions. Here, we introduce both structure-controlled graphene and graphite composite anodes, which employ controlled charge storage mechanisms to accelerate Li-ion charge storage kinetics and maintain structural stability under low-temperature conditions. [1-3] By transitioning from layered graphite to crumpled graphene or expanded graphite (composite), we effectively utilize diffusion- and surface-controlled charge storage mechanisms. These structure-controlled anodes exhibit superior rate capability and exceptional performance at temperatures as low as -50 °C. Through comprehensive low-temperature analyses, this research provides a detailed understanding of the relationships between anode structure, charge storage mechanisms, and performance under low-temperature conditions. Our findings offer valuable insights for the development of advanced energy storage devices optimized for low-temperature operation.
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