Nano/Microstructured Silicon–Graphite Composite Anode for High-Energy-Density Li-Ion Battery

With the ever-increasing demand for lithium-ion batteries (LIBs) with higher energy density, tremendous attention has been paid to design various silicon-active materials as alternative electrodes due to their high theoretical capacity (ca. 3579 mAh g^-1). However, totally replacing the commercially utilized graphite with silicon is still insurmountable owing to bottlenecks such as low electrode loading and insufficient areal capacity. Thus, in this study, we turn back to enhanced graphite electrode through the cooperation of modified silicon via a facile and scalable blending process. The modified nano/microstructured silicon with boron doping and carbon nanotube wedging (B-Si/CNT) can provide improved stability (88.2% retention after 200 cycles at 2000 mA g^-1) and high reversible capacity (∼2426 mAh g^-1), whereas the graphite can act as a tough framework for high loading. Owing to the synergistic effect, the resultant B-Si/CNT-graphite composite (B-Si/CNT@G) shows a high areal capacity of 5.2 mAh cm^-2 and excellent cycle retention of 83.4% over 100 cycles, even with ultrahigh active mass loading of 11.2 mg cm^-2,which could significantly surpass the commercially used graphite electrode. Notably, the composite also exhibits impressive application in Li-ion full battery using 2 mol % Al-doped full-concentration-gradient Li[Ni_0.76Co_0.09Mn_0.15]O₂ (Al2-FCG76) as the cathode with excellent capacity retention of 82.5% even after 300 cycles and an outstanding energy density (8.0 mWh cm^-2) based on the large mass loading of the cathode (12.0 mg cm^-2).