Architecting Sturdy Si/Graphite Composite with Lubricative Graphene Nanoplatelets for High‐Density Electrodes

Densification of the electrode by calendering is essential for achieving high-energy density in lithium-ion batteries. However, Si anode, which is regarded as the most promising high-energy substituent of graphite, is vulnerable to the crack during calendering process due to its intrinsic brittleness. Herein, a distinct strategy to prevent the crack and pulverization of Si nanolayer-embedded Graphite (Si/G) composite with graphene nanoplatelets (GNP) is proposed. The thickly coated GNP layer on Si/G by simple mechanofusion process imparts exceptional mechanical strength and lubricative characteristic to the Si/G composite, preventing the crack and pulverization of Si nanolayer against strong external force during calendering process. Accordingly, GNP coated Si/G (GNP-Si/G) composite demonstrates excellent electrochemical performances including superior cycling stability (15.6% higher capacity retention than P-Si/G after 300 cycles in the full-cell) and rate capability under the industrial testing condition including high electrode density (>1.6 g cm^-3) and high areal capacity (>3.5 mAh cm^-2). The material design provides a critical insight for practical approach to resolve the fragile properties of Si/G composite during calendering process.