Silicon (Si) anodes, despite their exceptional theoretical capacity (~ 4200 mAh·g⁻¹), face critical challenges, including severe volumetric expansion (> 300%) during lithiation and poor intrinsic conductivity, resulting in structural pulverization and unstable solid electrolyte interphase (SEI) formation. This work demonstrates a hierarchical confinement strategy integrating self-assembly and chemical vapor deposition (CVD) to construct microporous silicon-based composite anode material (mpSi-MGC) synergistically encapsulated by few-layer Ti₃C₂T_x (T = F, O, and OH) MXene, reduced graphene oxide (rGO), and CVD carbon coating. The multi-confinement architecture not only enhances mechanical stability but also optimizes electron (e⁻)/lithium ions (Li⁺) transport kinetics. Systematic ex situ analysis reveals that fluorine-functionalized groups in Ti₃C₂T_x significantly boost Li⁺ diffusion coefficients by promoting LiF-rich SEI formation, while the exterior CVD-carbon coating further stabilizes the hybrid structure. The optimized mpSi-MGC delivers exceptional Li storage performance: a high reversible initial capacity of 1800 mAh·g⁻¹ at 0.2 A·g⁻¹, remarkable cyclability with 992 mAh·g⁻¹ retained after 200 cycles at 1.0 A·g⁻¹, and superior rate capability (818 mAh·g⁻¹ at 3 A·g⁻¹). This multi-scale confinement design effectively mitigates volume expansion in micron-sized Si while enhancing e⁻/Li⁺ conductivity, offering a promising paradigm for developing high-energy-density lithium-ion batteries (LIBs) through rational structural engineering and interfacial optimization.

Compared to nanostructured Si/C materials, micro-sized Si/C anodes for lithium-ion batteries (LIBs) have gained significant attention in recent years due to their higher volumetric energy density, reduced side reactions and low costs. However, they suffer from more severe volume expansion effects, making the construction of stable micro-sized Si/C anode materials crucial. In this study, we proposed a simple wet chemistry method to obtain porous micro-sized silicon (μP-Si) from waste AlSi alloys. Then, the μP-Si@carbon nanotubes (CNT)@C composite anode with high tap density was prepared by wrapping with CNT and coated with polyvinylpyrrolidone (PVP)-derived carbon. Electrochemical tests and finite element (FEM) simulations revealed that the introduction of CNTs and PVP-derived carbon synergistically optimize the stability and overall performance of the μP-Si electrode via construction of tough composite interface networks. As an anode material for LIBs, the μP-Si@CNT@C electrode exhibits boosted reversible capacity (~ 3500 mAh·g⁻¹ at 0.2 A·g⁻¹), lifetime and rate performance compared to pure μP-Si. Further full cell assembly and testing also indicates that μP-Si@CNT@C is a highly promising anode, with potential applications in future advanced LIBs. It is expected that this work can provide valuable insights for the development of micro-sized Si-based anode materials for high-energy-density LIBs.

Silicon anodes have been extensively studied as a potential alternative to graphite ones for Li-ion batteries. However, their commercial application is limited by the issues of the poor structural and interfacial stability. In this regard, one of the key strategies for fully exploiting the capacity potential of Si-based anodes is to design robust conductive binder networks. Although the amount of binder in the electrode is small, it is, however, considered as a critical component of Si-based anodes for Li-ion batteries. In this review, a brief summary is given from the structural and functional aspects of the existing binders for Si anodes. In particular, three-dimensional and multifunctional polymeric binders with excellent electrical conductivity, flexibility, and adhesion prepared by chemical bonding, electrostatic and coordination interactions have become the focus of research, and are expected to accelerate the practical application of silicon anodes. Lastly, some suggestions for the future development of Si anodic binders are put forward.