The low initial Coulombic efficiency (ICE) and insufficient cycling lives of silicon (Si)‐based anodes seriously hinder their eventual introduction into next‐generation high‐energy‐density lithium–ion batteries (LIBs). Herein, an engineering prelithiation binder strategy based on polyacrylic acid (LixPAA) is proposed for representative SiOx anodes. The ICEs and cycling lives of SiOx anodes are significantly improved by precisely controlling the lithiation degree of PAA binder. The ICE of the high‐loading (3.0 mg cm−2) SiOx electrode increases by 10.9% when the Li0.75PAA binder replaces the PAA binder. Moreover, the working mechanism of the lithiation binder strategy to improve the electrochemical performances (especially for ICE) is systematically investigated, which is universally applied to other Si anodes such as Si nanoparticles and Si/graphite. This universal binder strategy and proposed working mechanism provide enlightenment on constructing high‐ICE, high‐energy‐density, and long‐life Si‐based anodes.

The development of high-performance cathode material is the key to realize commercial application of zinc-ion batteries (ZIBs). Vanadium-based materials have been used as cathode candidate for ZIBs due to their...

The large volume expansion hinders the commercial application of silicon oxide (SiO x ) anodes in lithium-ion batteries. Recent studies show that binders play a vital role in mitigating the volume change of SiO x electrodes. Herein, we introduce the small molecule tannic acid (TA) with high branching into the linear poly(acrylic acid) (PAA) binder for SiO x anodes. The three-dimensional (3D) crosslinked network with multiple hydrogen bonds is formed by the incorporation of abundant hydroxyl groups with unique carboxyl groups, which increases the interfacial adhesive strength with SiO x particles. As a consequence, SiO x electrodes based on the PAA-TA binder show an excellent cycling performance with a high specific capacity of 1025 mA h g–1 at 500 mA g–1 after 250 cycles. Moreover, the SiO x ||NCM811 full cell exhibits a reversible capacity of 143 mA h g–1 corresponding to 87.4% capacity retention after 100 cycles.

Micron-sized silicon oxide (SiO x ) has been regarded as a promising anode material for new-generation lithium-ion batteries due to its high capacity and low cost. However, the distinct volume expansion during the repeated (de)lithiation process and poor conductivity can lead to structural collapse of the electrode and capacity fading. In this study, SiO x anode materials coated with TiO 0.6 N 0.4 layers are fabricated by a facile solvothermal and thermal reduction technique. The TiO 0.6 N 0.4 layers are homogeneously dispersed on SiO x particles and form an intimate contact. The TiO 0.6 N 0.4 layers can enhance the conductivity and suppress volume expansion of the SiO x anode, which facilitate ion/electron transport and maintain the integrity of the overall electrode structure. The as-prepared SiO x -TiON-200 composites demonstrate a high reversible capacity of 854 mAh g −1 at 0.5 A g −1 with a mass loading of 2.0 mg cm −2 after 250 cycles. This surface modification technique could be extended to other anodes with low conductivity and large volume expansion for lithium-ion batteries.