As fast-charging lithium-ion batteries turn into increasingly important components in forthcoming applications, various strategies have been devoted to the development of high-rate anodes. However, despite vigorous efforts, the low initial Coulombic efficiency and poor volumetric energy density with insufficient electrode conditions remain critical challenges that have to be addressed. Herein, we demonstrate a hybrid anode via incorporation of a uniformly implanted amorphous silicon nanolayer and edge-site-activated graphite. This architecture succeeds in improving lithium ion transport and minimizing initial capacity losses even with increase in energy density. As a result, the hybrid anode exhibits an exceptional initial Coulombic efficiency (93.8%) and predominant fast-charging behavior with industrial electrode conditions. As a result, a full-cell demonstrates a higher energy density (≥1060 Wh l⁻¹) without any trace of lithium plating at a harsh charging current density (10.2 mA cm⁻²) and 1.5 times faster charging than that of conventional graphite.

To achieve the urgent requirement for high volumetric energy density in lithium-ion batteries, alloy-based anodes have been spotlighted as next-generation alternatives. Nonetheless, for the veritable accomplishment with regards to high-energy demand, alloy-based anodes must be evaluated considering several crucial factors that determine volumetric capacity. In particular, the electrode swelling upon cycling must be contemplated if these anodes are to replace conventional graphite anodes in terms of volumetric capacity. Herein, we propose macropore-coordinated graphite-silicon composite by incorporating simulation and mathematical calculation of numerical values from experimental data. This unique structure exhibits minimized electrode swelling comparable to conventional graphite under industrial electrode fabrication conditions. Consequently, this hybrid anode, even with high specific capacity (527 mAh g⁻¹) and initial coulombic efficiency (93%) in half-cell, achieves higher volumetric capacity (493.9 mAh cm⁻³) and energy density (1825.7 Wh L⁻¹) than conventional graphite (361.4 mAh cm⁻³ and 1376.3 Wh L⁻¹) after 100 cycles in the full-cell configuration.

Lithium metal is the most promising anode for next-generation lithium batteries. Nonetheless, its non-uniform Li nucleation, dendritic growth, and infinite volume variation lead to rapid cell failure and hinder its practical application. Here, we propose a defective graphene shell grown on a carbon matrix as a stable lithium metal host via carbide-mediated catalytic hydrogenolysis. It has numerous nano-channels with defective graphene shells on its surface, which can effectively guide the dendrite-free Li deposition and accommodate a rational amount of metallic Li without severe cell volume change. Due to these features, the host exhibits good cycle stability (87.2% after 500 cycles) and low dimension variation (9 μm) in carbonate electrolyte full-cell evaluations. In addition to its good performances in the carbonate electrolyte, our versatile Li host, acting as a Li-ion flux regulating interlayer, also achieves an improved cycling performance in the argyrodite Li₆PS₅Cl based high energy density all-solid-state battery full-cell configuration.

Silicon (Si) is considered a potential alternative anode for next-generation Li-ion batteries owing to its high theoretical capacity and abundance. However, the commercial use of Si anodes is hindered by their large volume expansion (∼ 300%). Numerous efforts have been made to address this issue. Among these efforts, Si-graphite co-utilization has attracted attention as a reasonable alternative for high-energy anodes. A comparative study of representative commercial Si-based materials, such as Si nanoparticles, Si suboxides, and Si–Graphite composites (SiGC), was conducted to characterize their overall performance in high-energy lithium-ion battery (LIB) design by incorporating conventional graphite. Nano-Si was found to exhibit poor electrochemical performance, with severe volume expansion during cycling. Si suboxide provided excellent cycling stability in a full-cell evaluation with stable volume variation after 50 cycles, but had a large irreversible capacity and remarkable volume expansion during the first cycle. SiGC displayed a good initial Coulombic efficiency and the lowest volume change in the first cycle owing to the uniformly distributed nano-Si layer on graphite; however, its long-term cycling stability was relatively poor. To complement each disadvantage of Si suboxide and SiGC, a new combination of these Si-based anodes was suggested and a reasonable improvement in overall battery performance was successfully achieved.