Silicon-based anode materials for high-capacity lithium-ion batteries: recent advances and challenges

Sirou Li; Jianing Xie; Zirui Li; Zitong Wang; Xiaomin Wang

doi:10.1039/d6ra05647d

. 2026 Aug 28;16(41):47726–47759. doi: 10.1039/d6ra05647d

Silicon-based anode materials for high-capacity lithium-ion batteries: recent advances and challenges

Sirou Li ^a, Jianing Xie ^a, Zirui Li ^a, Zitong Wang ^a, Xiaomin Wang ^a,^✉

PMCID: PMC13523656 PMID: 42666654

Abstract

Silicon is a promising anode material for high-energy-density lithium-ion batteries because of its high theoretical capacity, low operating potential, and natural abundance. However, large volume changes, poor electronic conductivity, and sluggish lithium-ion transport cause particle pulverization, unstable solid-electrolyte interphase formation, loss of electrical contact, and rapid capacity fading. This review critically evaluates four major improvement strategies: material and structural design, interface engineering, multifunctional binders, and pre-lithiation. These strategies are comparatively evaluated in terms of their mechanisms, representative performance, limitations, manufacturing complexity, and scalability. Recent advances in fast-charging degradation and artificial-intelligence-assisted material screening, state estimation, and charging control are also summarized. Particular attention is given to commercially relevant conditions, including high areal loading, limited electrolyte, realistic N/P ratios, and full-cell validation. Finally, practical Si–graphite composites, stable interfaces, adaptive binders, and controllable pre-lithiation are identified as key directions for scalable silicon-based anodes.

This review evaluates silicon‑based anode strategies and links fast‑charging degradation and AI‑assisted battery management to commercial electrode–cell operating conditions. graphic file with name d6ra05647d-ga.webp

1. Introduction

Lithium-ion batteries (LIBs) are widely used in portable electronic devices, electric vehicles, and renewable energy storage systems due to their high energy density, excellent cycling stability, lack of memory effect, superior safety, and environmental friendliness.^1–5 However, with the development of electric vehicles, smart grids, and a wide range of portable electronic devices,^6–10 existing lithium-ion battery technologies are increasingly unable to meet growing market demands.^11–14 As one of the core components of LIBs, anode materials play a crucial role in overcoming the current energy-density limitations. Therefore, the development of next-generation anode materials is particularly important.

Beyond advances in electrode chemistry, recent progress in intelligent design and battery management is reshaping battery research. AI-assisted electrode-material screening, robust equivalent–circuit parameter identification, and temperature- and state-of-charge-dependent modeling enable more efficient material optimization and state-aware battery control.^15–17 Meanwhile, coordination-engineered ion-transport pathways and multiphysics analyses of lithium deposition highlight the importance of interfacial stability and safety under demanding operating conditions.^18,19 These developments provide useful methodological support for next-generation high-capacity lithium-ion batteries.

Graphite, currently the most widely used anode material, is limited by its relatively low theoretical capacity of only 372 mAh g⁻¹.^20,21 Consequently, the development of novel anode materials that outperform traditional graphite has become a central focus in the advancement of lithium-ion batteries.^22–26 Silicon (Si) is widely recognized as one of the most promising anode materials for lithium-ion batteries due to its high theoretical specific capacity of 4200 mAh g⁻¹, its relatively low operating potential of 0.4 V vs. Li⁺/Li, and its abundant reserves in the Earth's crust.^27–31 Despite these advantages, the practical application of silicon anodes still faces several key challenges.^32–35 First, silicon undergoes volume expansion of up to 300% during the electrochemical (de)lithiation process. This intrinsic property triggers a series of interlinked failure mechanisms, including the fracture and pulverization of active particles, the repeated formation and breakdown of the solid-electrolyte interphase (SEI), the collapse of the electrode conductive network, and the overall structural failure.^36–41 Second, the inherently low electrical conductivity (2.52 × 10⁻⁶ S m⁻¹) hinders electron transport through the fractured electrode structure, leading to rapid capacity decay. Furthermore, the low diffusion rate of lithium ions (Li⁺) within silicon creates concentration gradients between the particle surface and interior, thereby hindering complete lithiation and delithiation. The lithium-storage mechanism of silicon, the associated failure processes, and the major performance-improvement strategies are schematically summarized in Fig. 1.

To address these challenges, numerous material and electrode engineering strategies have been developed. Recent reviews have summarized nanostructured silicon architectures, Si–C composites, diverse silicon-based materials, and multidimensional structural design.^42,43 Functional binder engineering has also been systematically discussed.⁴⁴ Interfacial stability, scalable engineering, and laboratory-to-industrial commercialization pathways have been reviewed from practical perspectives.^45,46 However, the integration of these mitigation strategies with fast-charging degradation mechanisms and AI-enabled battery monitoring and control remains less systematically addressed. Therefore, this review integrates material design, interface engineering, multifunctional binders, and pre-lithiation with analyses of fast-charging behavior and AI-assisted material screening, state estimation, lifetime prediction, and charging control from a material–electrode–cell perspective.

To ensure the transparency and reproducibility of the literature selection process, the literature included in this review was identified primarily through searches of the Web of Science Core Collection and Google Scholar, supplemented by the X-MOL academic literature platform. The search covered publications available up to July 2026, with particular emphasis on studies published during the past five years. The search terms included combinations of “silicon anode”, “silicon-based anode”, “Si–C composite”, “interface engineering”, “solid electrolyte interphase”, “functional binder”, “pre-lithiation”, “fast charging”, and “artificial intelligence”. Peer-reviewed research articles and review papers directly related to the failure mechanisms, material design, electrochemical performance, and practical application of silicon-based anodes were included, whereas studies lacking sufficient electrochemical data or direct relevance to lithium-ion battery anodes were excluded. Earlier landmark studies were retained to provide historical and mechanistic context.

2. Strategies for improving the performance of silicon-based anodes in lithium-ion batteries

To address the major failure mechanisms of silicon-based anodes, the global research community has developed a multi-level, multi-dimensional strategy framework. These strategies do not operate independently but instead act synergistically to enhance cycling stability, rate capability, and safety while preserving silicon's inherent high-capacity advantage. This review provides a comprehensive evaluation of mainstream and cutting-edge strategies for optimizing the performance of silicon-based anodes across four dimensions: material and structural design, interface engineering, development of multifunctional binders, and pre-lithiation technology.

2.1. Material modification and structural design

Material modification and structural design are fundamental approaches to addressing the challenges associated with silicon-based anodes, and they represent the most direct and commonly used methods for enhancing the cycling stability and rate capability of such anodes. Through rational structural design and performance optimization, it is possible to effectively improve the structural stability, electrical conductivity, and ionic transport efficiency of the electrode, thereby enhancing the overall electrochemical performance of the silicon-based anode. Common approaches include nanostructuring, silicon-carbon composite design, and alloying; these modification techniques provide potential routes toward the practical application of silicon-based anodes.

2.1.1. Nanostructuring

Nanostructuring is a key method for mitigating silicon volume expansion and enhancing the performance of silicon-based lithium-ion battery anode materials.^47,48 Reducing silicon particles to the nanoscale not only accelerates electrolyte penetration and shortens the diffusion path of lithium ions within the silicon, thereby enabling faster charging and discharging rates,⁴⁹ but also improves the ability of nanoscale silicon particles to accommodate mechanical strain, allowing them to withstand greater volumetric strain without fracturing.^50,51 Ran Wang et al.⁵² proposed a method combining high-temperature disproportionation and carbonization with acid etching. By sintering a mixture of SiO and sucrose, they achieved carbon coating while forming Si nanocrystals and a SiO₂ matrix. Following HF acid etching for a controlled duration, they prepared a hierarchical Si/SiO_x@C composite with internal buffer voids (Fig. 2a) to buffer volume expansion and enhance ion transport. The intact and dense carbon shell enhances electronic conductivity and stabilizes the electrode–electrolyte interface. As an anode material, the optimized SSC-10 sample exhibited a capacity retention of 90% after 100 cycles and a reversible capacity of 1095.0 mAh g⁻¹, demonstrating excellent cycling stability (Fig. 2b); even at a high current density of 2.0 A g⁻¹, its capacity still reached 850 mAh g⁻¹ (Fig. 2c).

However, nanosized silicon also faces several practical limitations. Its high specific surface area increases direct contact with the electrolyte, thereby intensifying electrolyte decomposition, repeated SEI formation, irreversible lithium consumption, and initial coulombic efficiency loss. In addition, the low tap density of silicon nanoparticles limits the volumetric energy density of the electrode and makes it difficult to achieve commercially relevant areal capacities. Nanoparticle agglomeration may also cause non-uniform dispersion during slurry preparation, while the multistep size-control, etching, coating, and purification processes commonly used for nanosized silicon increase manufacturing costs and complicate large-scale production. In response to these limitations, porous and hierarchical silicon structures have been widely investigated. Porous silicon retains the kinetic advantages of nanomaterials, while its internal pores provide space to accommodate silicon volume expansion, thereby improving mechanical stability.^53,54 To date, numerous methods have been reported for preparing nanoporous silicon materials.^55–57 Yaodong Ma et al.⁵⁸ used low-cost silicon-aluminum alloy as the raw material to prepare micron-sized porous silicon via acid etching, which was then coated with amorphous hard carbon using a sol–gel self-assembly method. They successfully synthesized micron-sized P–Si@C with a synergistic porous silicon/carbon shell structure, as shown in Fig. 2d. Due to its porous structure, which mitigates volume expansion, and the carbon shell, which enhances conductivity, this material exhibits excellent cycling performance in half-cells (Fig. 2e), with an energy density of 795.1 Wh L⁻¹ in full-cell configurations. Bing Bai et al.⁵⁹ proposed a metal oxide thermal etching method for the preparation of nitrogen-doped porous layered silicon nanosheets (P–Si NFs), as shown in Fig. 2f. Through the in situ growth of FeOOH on Si NFs, followed by heat treatment and acid etching, a nitrogen-doped porous surface was created while preserving the two-dimensional layered structure, thereby buffering volume expansion and enhancing ion transport. When used as an anode material, the P–Si NFs exhibited a capacity retention of 89.6% after 500 cycles at 2 A g⁻¹, demonstrating excellent cycling stability (Fig. 2g). This work provides a pathway for the preparation of high-performance, low-cost silicon-based anode materials.

2.1.2. Silicon-carbon composite materials

The poor conductivity of silicon-based materials and their susceptibility to volume changes have long been a challenge for many researchers. Due to their structural stability, high electrochemical activity, and good compatibility with silicon-based materials,^60–62 composites incorporating carbon materials are currently one of the most common and effective strategies for addressing the issues of poor conductivity and volume expansion in silicon. Furthermore, carbon materials (such as carbon nanotubes and graphene) can form three-dimensional conductive networks that suppress the aggregation of silicon particles, thereby enhancing the overall conductivity of the electrode and enabling fast-charging capabilities.⁶³ Carbon-coated core–shell structures, hollow core–shell structures, and multilayer core–shell structures represent the current mainstream research directions for silicon-carbon composites.

Carbon-coated core–shell structures represent the most fundamental and widely applied silicon-based core–shell strategy. The key lies in introducing a continuous carbon layer onto the surface of silicon particles, which not only restricts the volumetric expansion of silicon and reduces mechanical stress,⁶⁴ but also prevents direct contact between silicon and the electrolyte, thereby minimizing side reactions and promoting the formation of a stable SEI film.^65,66 The effectiveness of this strategy has been validated in numerous studies. SMG@C, prepared by Bo Ding et al.,⁶⁷ is a representative example of this approach. As shown in Fig. 3a, in this system, high-energy ball milling first induces an in situ reaction between Mg and SiO to form a Si/MgO composite; graphite is then introduced, and the outer carbon coating is completed through the carbonization of pitch, ultimately forming a core–shell composite consisting of Si, MgO, graphite, and amorphous carbon. Unlike pure Si@C, the MgO and graphite in this system simultaneously serve as a buffering matrix and a conductive framework, while the outer carbon shell further enhances structural integrity and interfacial stability. The results show that the material retains a capacity of 1124 mAh g⁻¹ after 75 cycles at 100 mA g⁻¹, and the capacity recovers after rate cycling, reflecting the synergistic effect of carbon coating and the composite buffer phase Fig. 3b and c). Similarly, Jian Shi et al.⁶⁸ prepared recycled silicon-based core–uniform carbon shell composites (m-RWSi@PMMA-C) using a surface engineering-assisted method, as shown in Fig. 3d. In this work, KH550 was used to surface-functionalize the recycled silicon particles, guiding the uniform polymerization of MMA on the silicon surface, followed by carbonization to form a uniform carbon shell. The authors noted that the uniform and dense carbon layer not only helps isolate the electrolyte and promote the formation of a stable SEI, but also improves electron and lithium-ion transport through its lower specific surface area and higher degree of graphitization. Benefiting from this structural design, the material maintained a reversible capacity of 1083 mAh g⁻¹ after 200 cycles at 200 mA g⁻¹, with an initial discharge capacity of 3176.2 mAh g⁻¹ and an initial coulombic efficiency of 75.6% (Fig. 3e and f). These results demonstrate that controlling the uniformity of the carbon shell and the density of the interface is key to enhancing the cycling stability of traditional Si@C systems. However, a single carbon shell cannot fully restrain the volume expansion of silicon during cycling; as the number of cycles increases, this leads to repeated rupture and reconstruction of the SEI, thereby affecting the overall electrochemical performance.

In hollow core–shell structures, a certain void is typically left between the silicon core and the shell, allowing the volume expansion of silicon during lithiation to be released primarily into the internal cavity; this design generally outperforms conventional dense core–shell structures in terms of suppressing particle pulverization and maintaining SEI stability.⁶⁹ The granadilla-like porous/hollow composite structure proposed by Peng Guan et al.⁷⁰ is a typical example of this class of structures. In this work, multiple yolk–shell Si/C nanobeads are dispersed within a three-dimensional porous carbon framework, with the voids between the cores and shells and the external porous network working together to buffer volume changes (Fig. 4a and b). A similar approach is also reflected in the Si@Void@C structures reported by Pan et al.⁷¹ In this work, a carbon layer was first formed on the surface of Si nanoparticles, followed by partial removal of the core via alkaline etching, resulting in a yolk–shell structure with distinct core–cavity–shell features (Fig. 4c and d). The authors explicitly state that the void between the core and the carbon shell must be large enough to accommodate the volume change resulting from the complete lithiation of silicon; accordingly, the cavity size in their design exceeds 30 nm to accommodate a volume expansion of approximately 300–400%. This structure combines the advantages of both yolk–shell and porous carbon scaffold architectures, releasing the expansion stress of silicon while enhancing conductivity and facilitating Li⁺ diffusion. Compared to conventional carbon-coated core–shell structures, this approach better accommodates the intrinsic property of silicon anodes—namely, their significant volume change. The carbon shell no longer bears the full expansion stress directly; instead, stress is released through the internal cavity, thereby more effectively maintaining the integrity of the shell and the stability of the interface. However, parameters such as the cavity ratio and shell thickness are often difficult to control, and the excessive length of the ion transport path can lead to a decrease in conductivity.

Multilayer core–shell structures enhance overall stability through hierarchical synergy,^72–74 emphasizing the functional division of labor among the different shell layers. The representative double-layer core–shell structure Si@AlF₃@C, proposed by Hyungmin Park et al.⁷⁵ involves first introducing an AlF₃ layer onto the Si surface, followed by coating it with an outer layer of amorphous carbon (Fig. 5a). AlF₃ is used to enhance mechanical strength and interfacial stability, suppress electrolyte decomposition, and promote the formation of a more stable SEI. The outer carbon layer is responsible for improving conductivity and enhancing compatibility with the conductive agent (Fig. 5b). Experimental results show (Fig. 5c–e) that Si@C, which consists solely of a carbon layer, exhibits significant capacity decay after 125 cycles, whereas Si@AlF₃@C achieved a capacity retention of 75.8% after 125 cycles at 25 °C and maintained 73.7% capacity retention after 150 cycles at 60 °C, while still delivering a capacity exceeding 1600 mAh g⁻¹ at 5C. In addition, Shuwu Liu et al.⁷⁶ employed an “electrospinning-secondary carbon coating” strategy to prepare silicon-based composite nanofiber anodes (CNFs/Si@C) (Fig. 5f and g). In this bilayer carbon structure, the inner layer of carbon nanofibers provides a continuous conductive network, while the outer carbon layer effectively suppresses the pulverization and shedding of silicon particles during charging and discharging, thereby jointly buffering silicon volume expansion and stabilizing the SEI (Fig. 5h). This significantly enhances the electrochemical performance of the self-supporting, binder-free electrode (Fig. 5i–j).

A comparison of these architectures shows that they accommodate silicon volume expansion through different mechanisms. Dense carbon-coated core–shell structures rely mainly on mechanical confinement by the outer shell and offer relatively simple, compact designs, but the shell directly bears the expansion stress and may fracture during prolonged cycling. Hollow and yolk–shell structures provide internal void space, thereby reducing stress transfer to the outer shell and improving particle and SEI stability; however, excessive voids and poorly controlled cavity dimensions may lower electrode density and hinder ion transport. Multilayer core–shell structures assign mechanical support, interface stabilization, and electronic conduction to different functional layers, providing more comprehensive protection, but their additional interfaces and fabrication steps increase structural complexity and may introduce transport resistance. Therefore, dense core–shell structures favor simplicity and compactness, hollow or yolk–shell structures offer greater expansion accommodation, and multilayer structures provide multifunctional protection at the cost of higher manufacturing complexity.

To provide a clear comparison of the differences in electrochemical performance among various core–shell silicon-carbon composites, the key parameters of representative materials are summarized in Table 1.

Table 1. Electrochemical performance of representative core–shell Si–C anodes^a.

Material	Structure designs	Initial specific (mAh g⁻¹)	Current density	Number of cycles	Residual reversible capacity (mAh g⁻¹)	Capacity retention (%)	Ref.
SMG@C	Core–shell structure with carbon	2222	100 mA g⁻¹	75	1124	87.4%	67
m-RWSi@PMMA-C	Core–shell structure with carbon	3176	200 mA g⁻¹	200	1083	34.1%	68
PSi/C-400	Yolk–shell structure	1357	100 mA g⁻¹	100	933	86.5%	70
Si@Void@C	Yolk–shell structure	2258	1 A g⁻¹	50	804	83.0%	71
Si@AlF₃@C	Multi-layer core–shell structure	2457	0.5C	125	1001	75.8%	75
CNFs/Si@C	Multi-layer core–shell structure	936	100 mA g⁻¹	100	753	80.5%	76
Si@C–Ni	Core–shell structure with carbon	3317	0.1C	360	2514.8	75.8%	77
CNTs/Si/C	Multi-layer core–shell structure	1933.6	500 mA g⁻¹	1000	1508.5	78.0%	78
C@Si@C	Multi-layer core–shell structure	4130	0.07C	60	2246	54.4%	79
P–Si/C@C	Core–shell structure with carbon	1269.6	1000 mA g⁻¹	820	708.6	87.1%	80
Si@void@N–C	Yolk–shell structure	1282.3	100 mA g⁻¹	100	994.2	77.5%	81
Si@void@NCN-1	Yolk–shell structure	1245.5	500 mA g⁻¹	500	402.5	68.66%	82

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Note: capacity–retention values are reported according to the definitions used in the original studies and may be referenced to different baseline cycles.

2.1.3. Alloying

Alloying involves the use of metallic components to induce the formation of new alloy phases, silicide phases, or composite phases, thereby simultaneously regulating the material's electronic transport, stress distribution, and electrochemical reaction pathways.⁸³ Depending on whether the introduced metallic elements can undergo reversible reactions with lithium, silicon alloy systems are typically classified into two categories: active metal alloying and inert metal alloying.

An active metal alloying system refers to a system in which elements such as Mg, Ge, and Zn form silicides or single-phase alloys with silicon and undergo reversible reactions with lithium during cycling, thereby providing additional capacity to mitigate volume expansion.^84–86 Yinghui Yang et al.⁸⁷ prepared three-dimensional nanoporous Si–Ge alloys using a chemical dealloying method. The resulting materials exhibit a continuous ribbon-like structure and a uniform coral-like morphology characterized by a hierarchical micro-/mesoporous structure (Fig. 6a). This structure not only ensures the uniform dispersion of Si and Ge within the alloy and reduces the agglomeration of active particles, but also provides an effective buffer space to accommodate volume expansion during cycling. The incorporation of Ge significantly enhanced electrical conductivity and lithium-ion migration rates, enabling the Si₁₂Ge₈ electrode to maintain a reversible specific capacity of 1158 mAh g⁻¹ after 150 cycles at 1000 mA g⁻¹, with an initial coulombic efficiency of 75.6%. This work demonstrates that the benefits of active metal alloying extend beyond additional capacity to include synergistic improvements in reaction kinetics and structural reversibility. Zizhong Chen et al.⁸⁸ prepared a dendritic, multi-level porous Si/Zn composite anode material via a one-step selective dealloying process Fig. 6b). This material forms a three-dimensionally interconnected dendritic porous network, which not only increases the number of active sites for lithium-ion insertion and extraction but also effectively buffers the volume change of silicon through open channels. Meanwhile, the high electrical conductivity of the Zn phase further promotes electron transport and lithium-ion migration. Thanks to this synergistic structural design, the optimal composition NP-Si₈₀Zn₂₀ maintained a reversible specific capacity of 901.8 mAh g⁻¹ after 1000 cycles at 1000 mA g⁻¹, with an initial coulombic efficiency of 66.4%. It maintained 792.3 mAh g⁻¹ at 3000 mA g⁻¹, and the capacity recovered to 1732.4 mAh g⁻¹ when the current density was reduced to 100 mA g⁻¹.

An inert metal alloying system refers to a mixture formed by combining silicon with elements such as Fe, Co, Ni, Cu, and Ti to create a blend of active silicon phases and electrochemically inert phases. The inert components typically do not directly participate in the charge–discharge process.^89–91 Instead, they sacrifice some specific capacity in exchange for greater structural stability, enhance the conductivity of the silicon anode, and mitigate volume changes.^92,93 Mirco Ruttert et al.⁹⁴ prepared Fe_xSi_y alloy anode materials (Fig. 6c) by ball-milling micron-sized Fe and Si elemental powders as precursors under an argon atmosphere. The study demonstrated that varying the ball-milling time and Fe/Si ratio can effectively modulate the microstructure of the alloy. The optimal composition, Fe₁₄Si₈₆, exhibited an initial coulombic efficiency of 92.0% in a half-cell and a capacity retention of 48% after 50 cycles at 1000 mA g⁻¹, outperforming pure Si electrodes; in a full cell assembled with an NMC-111 cathode, the material retained 37–40% of its initial capacity even at a high rate of 3C. The electrode density of this material reaches 1.0–2.0 g cm⁻³, indicating its potential advantages in the preparation of electrodes with high areal capacity and high packing density. In the inert metal system, Ti–Si and Ni–Si alloys further demonstrate the concept that an inert framework can modulate reaction pathways. Wang et al.⁹⁵ prepared nanostructured Si_1−xTi (0 ≤ x ≤ 0.3) alloys using a ball-milling method. As the Ti content increased, Ti reacted with Si to form nanocrystalline C₄₉-phase TiSi₂ with a high defect density, consisting primarily of amorphous Si and C₄₉-phase TiSi₂. The electrochemically inert TiSi₂ framework in this material limits lithium-induced volume expansion to below 135% and effectively suppresses the formation of the Li₁₅Si₄ phase, thereby significantly improving the structural integrity of the electrode. These results indicate that the inert phase is not merely a passive diluent but can actively alter the failure behavior of silicon anodes by regulating phase composition and phase transformation processes. Furthermore, Zhang et al.⁹⁶ fabricated a Si/Ni₃Si-coated carbon nanofiber composite anode material (Fig. 6d) using silicon nanoparticles and nickel acetate as precursors via a one-step electrospinning process. In this composite, Ni₃Si acts as an inert, rigid buffer matrix that effectively mitigates the severe volume expansion of silicon during lithiation, thereby suppressing electrode pulverization and flaking, while the carbon nanofiber network provides continuous electron transport pathways and enhances the overall mechanical strength of the electrode, thereby maintaining the integrity of the one-dimensional fiber structure during cycling. Studies have shown that after 200 cycles, the charge transfer resistance of this electrode decreased to 73.88 Ω, and it retained its complete fiber morphology even after cycling. When the inert alloy phase is further coupled with the carbon scaffold, a synergistic system comprising a buffering matrix, a conductive network, and structural support is formed. This also indicates that inert metal alloys do not necessarily exist as standalone alloys; they can be further integrated with nanostructured, fibrous, and coated designs to construct more stable composite lithium storage frameworks. To systematically compare the electrochemical performance of silicon-based anodes doped with different metals, the key parameters of typical alloy systems are summarized in Table 2.

Table 2. Electrochemical performance of representative Si–metal and silicide anodes^a.

Material	Initial specific capacity (mAh g⁻¹)	Current density	Number of cycles	Residual reversible capacity (mAh g⁻¹)	Capacity retention (%)	Ref.
3D-NP-Si-Ge	2582	1000 mA g⁻¹	150	1158	59.4%	87
NP–Si₈₀Zn₂₀	2651.4	1000 mA g⁻¹	1000	901.8	34.0%	88
Fe₁₄Si₈₆	1528	1000 mA g⁻¹	50	733	48.0%	94
Si_0.85Ti_0.15	1372	0.2C	50	1317	96.0%	95
Si/Ni₃Si@C	1179.8	0.1C	200	1132.4	95.9%	96
FeSi₆/C	1758	100 mA g⁻¹	50	615	77.4%	97
Si@Cu₃Si@C	2052	400 mA g⁻¹	200	1477	71.9%	98
Si–Cu₃Si–Cu	2907.4	1.0 A g⁻¹	200	1401.2	74.9%	99
NCNTs-Ni₂Si@Si	2418	358 mA g⁻¹	600	1311	85%	100
ST + GBP	1088.4	0.1 mA cm⁻²	50	443.7	60%	101
Si/Ni/Si/Ni	1992	0.05 mA cm⁻²	200	1647	82%	102
Cu@Si CSNWF	3193	0.1C	500	948	29.7%	103

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Note: capacity–retention values are reported according to the definitions used in the original studies and may be referenced to different baseline cycles.

The strategy for silicon alloying does not simply involve suppressing silicon's volume changes through the addition of a second element; rather, it simultaneously regulates reactivity, the conductive network, and mechanical response within a multiphase coupling framework. Alloying with reactive metals emphasizes providing additional capacity while mitigating volume effects, whereas alloying with inert metals focuses more on enhancing structural stability and conductive continuity through an inactive framework. Future research should not focus solely on achieving higher specific capacity per half-cell, but should also examine alloy phase distribution, interface evolution, packing density, and overall performance under full-cell conditions, thereby advancing the practical application of silicon alloy anodes.

These strategies offer different benefits and limitations. Nanostructuring shortens lithium-ion diffusion pathways and reduces particle fracture, but its high surface area and low tap density increase side reactions and lower volumetric energy density. Porous structures accommodate silicon expansion and relieve stress, although excessive porosity can reduce electrode density and hinder ion transport. Carbon coatings and Si–C networks improve conductivity and SEI stability, but inactive carbon lowers overall capacity and the shell may still fracture during long-term cycling. Alloying redistributes stress and enhances structural or electronic stability, while additional inactive phases and complex processing may reduce practical energy density and increase manufacturing difficulty. Therefore, practical electrode design requires a balance among capacity, initial coulombic efficiency, areal loading, cycling stability, and scalability.

2.2. Interface engineering: creating a stable electrode/electrolyte interface

Interface instability is a major cause of capacity decay in silicon-based anodes. Interface engineering regulates the composition, mechanical stability, and ion-transport properties of the SEI through artificial interphase construction and electrolyte optimization, thereby reducing electrolyte decomposition, active-lithium loss, and impedance growth during repeated volume changes.

2.2.1. Construction of artificial SEI films: active control of interface stability

During initial lithiation, electrolyte reduction produces a heterogeneous SEI containing inorganic species, such as LiF, Li₂O, and Li₂CO₃, together with organic and polymeric species. The inorganic-rich components generally provide electronic insulation, chemical stability, and mechanical strength, whereas the organic-rich components contribute flexibility and interfacial contact. Therefore, long-term performance depends not only on whether an SEI is formed, but also on its composition, uniformity, ionic conductivity, and mechanical robustness. Because silicon repeatedly expands and contracts during cycling, a brittle or compositionally non-uniform SEI can crack and expose fresh silicon surfaces, triggering further electrolyte decomposition and SEI regrowth. This repeated process continuously consumes active lithium and electrolyte, thickens the interphase, increases charge-transfer resistance, isolates active particles, and ultimately reduces coulombic efficiency and capacity retention. A dense inorganic-rich SEI can suppress parasitic reactions and improve mechanical stability; however, excessive inorganic content may impede lithium-ion transport. An effective SEI must therefore balance chemical stability, mechanical adaptability, and ionic conductivity. In contrast, a synthetic SEI involves pre-forming a stable protective layer on the silicon surface during the material synthesis stage. This transforms the interface—which would otherwise form passively and become increasingly unstable—into a functional interface that can be designed and controlled. By establishing a balance between ion transport, electrical insulation, mechanical confinement, and interfacial chemical stability, this approach fundamentally enhances the cycling stability of silicon-based anodes.

Currently, vapor deposition and wet chemical methods are the two representative approaches for synthesizing artificial SEI. In vapor deposition, gaseous precursor molecules pass through the powder at a sufficiently high flow rate, causing the solid material to reach a state of equilibrium and exhibit liquid-like properties. This ensures uniform operating conditions and precursor concentration distribution, ultimately resulting in a uniform coating thickness.^104–106 B. H. Shen et al.¹⁰⁷ used initiated chemical vapor deposition (iCVD) to deposit the pV₄D₄ polymer onto the surface of a silicon thin-film electrode, thereby constructing a nanoscale artificial SEI layer. The siloxane rings facilitate Li⁺ migration, while the highly cross-linked structure endows the film with good mechanical strength, electrolyte barrier properties, and electrical insulation, thereby simultaneously suppressing electrolyte reduction and excessive SEI growth. Further analysis indicates that this coating can also regulate the composition of the SEI, promoting the formation of a LiF-enriched and denser interfacial layer, as shown in Fig. 7, thereby effectively suppressing interface instability and active lithium loss induced by volume expansion. It can thus be seen that the artificial SEI constructed via vapor deposition is no longer merely a simple physical coating, but rather a composite interfacial layer that combines both interfacial chemical regulation and mechanical stabilization functions.

In addition to vapor deposition, wet chemical methods are also widely used to construct artificial SEI layers, as they offer process flexibility and can be easily combined with various composite modification strategies. Hyungmin Park et al.¹⁰⁸ developed a dual-coating interface modification strategy in which an amorphous BaTiO_x layer was first deposited onto the surface of silicon nanoparticles via the sol–gel method, followed by the introduction of an outer carbon layer via chemical vapor deposition, resulting in a Si@BaTiO_x@C core–shell structure (Fig. 8a). In this system, the inner BaTiO_x layer primarily provides mechanical support and induces the formation of a more stable SEI, while the outer carbon layer constructs a continuous conductive network, thereby achieving synergistic optimization of mechanical confinement, interfacial stability, and enhanced conductivity. Unlike a single carbon layer, this dual–layer interface design more effectively suppresses the volume expansion of silicon particles and the accumulation of side reactions, enabling the electrode to retain its spherical morphology (Fig. 8b). In terms of electrochemical performance, this structure maintains a specific capacity of 1300 mAh g⁻¹ and a capacity retention of 65% after 600 cycles at 60 °C and 1C, while effectively suppressing excessive SEI growth and self-discharge (Fig. 8c–e). This indicates that the development of artificial SEI is no longer limited to single-interface passivation but has gradually evolved into a composite protective layer that integrates mechanical buffering, interface regulation, and transport optimization functions.

The core value of artificial SEI lies in transforming the inherently dynamic and difficult-to-control interfacial processes in silicon anodes into a stable interface that can be actively regulated through material design. Vapor deposition methods offer distinct advantages in terms of film uniformity, conformality, and thickness control, making them more suitable for precise interface engineering; wet chemical methods, on the other hand, hold greater potential in terms of process flexibility and the fabrication of composite structures. However, both methods have their own limitations: vapor deposition typically relies on costly equipment and process conditions, which limits its large-scale application; wet chemical methods, on the other hand, are susceptible to the evaporation rate of solvents, liquid-phase parameters, and reaction time, leading to uneven distribution of film thickness, local composition, and mechanical properties. It is evident, therefore, that further optimization of artificially engineered SEI should not be limited to the question of “whether a film can be formed”, but should instead focus on achieving a comprehensive balance among ionic conductivity, electrical insulation, mechanical toughness, and process scalability. This is also the key to advancing silicon-based anode interface engineering from laboratory research to practical application.

2.2.2. Electrolyte optimization: inducing the formation of a stable SEI layer

The electrolyte is the direct source of the SEI film, and its composition largely determines the chemical composition, microstructure, and long-term stability of the interface layer. Therefore, developing compatible electrolytes capable of inducing the formation of a stable SEI is a key approach to enhancing the cycling life and practical performance of silicon-based anodes. Among existing optimization strategies, electrolyte additives are widely adopted due to their low dosage, low cost, and direct controllability. Their function goes beyond merely “modifying the interface”; rather, through preferential reduction or decomposition behavior, they regulate the solvation structure and interfacial reaction pathways, thereby actively guiding the formation of a more stable SEI film.

Among the many additives, fluoroethylene carbonate (FEC) has become one of the most commonly used organic carbonate film-forming additives due to its excellent reductive stability.^109–111 FEC typically decomposes before the main solvent, inducing the formation of a LiF-rich inorganic–organic composite SEI layer on the silicon surface.^112–114 Such an interface layer not only helps improve the chemical stability of the SEI but also enhances interfacial mechanical strength and suppresses ongoing side reactions through the inorganic-enriched phase. Gaopan Liu et al.¹¹⁵ designed a dual-salt (LiFSi–LiPF₆) ether-based locally high-concentration electrolyte (D-LHCE-F) containing FEC, using a DME/TTE solvent system, and optimized the lithium-ion solvation structure by introducing 20 mol% FEC (Fig. 9a and b). The study demonstrated that this system effectively promotes the formation of a LiF-rich composite SEI and endows the interface with a higher mechanical modulus and better volume change adaptability, with a Young's modulus reaching 8.9 GPa and the irreversible electrode expansion rate decreasing from 221% to 175%. Additionally, the use of the main salt LiFSi helps prevent HF generation, thereby mitigating interfacial corrosion. Consequently, the SiO_x/C electrode exhibits excellent cycling stability, with a capacity retention of 78.5% after 500 cycles at 0.5C and 30 °C (Fig. 9c and d). Thus, the role of FEC is no longer limited to conventional film formation but can synergize with the dual-salt system and the localized high-concentration solvated environment to systematically optimize the interfacial composition and cycling behavior of silicon-based electrodes.

In addition to FEC, lithium salt-based additives are another key focus in the design of silicon-based anode electrolytes. These additives not only provide an additional source of lithium ions for the system but also contribute to the formation of a stable interface through preferential decomposition; their effects are often reflected simultaneously in multiple aspects, including SEI composition, ion transport, and the suppression of side reactions. M. Graf et al.¹¹⁶ introduced lithium nitrate (LiNO₃) and lithium nitrite (LiNO₂) into a 1 M LiPF₆/EC-DEC carbonate electrolyte to improve the interfacial stability of silicon-based electrodes. The study demonstrated that LiNO₃ can generate inorganic components such as Li₂O and Li₃N through multi-step reduction reactions (Fig. 9e), thereby forming a more stable SEI; among these, LiNO₂ serves as an intermediate product and can be further reduced to ultimately convert into Li₃N, thereby further enhancing the mechanical stability and lithium-ion transport capacity of the interface. Unlike traditional additives that primarily rely on local surface reactions, this type of lithium salt additive can diffuse with the electrolyte to achieve more uniform regulation of the entire electrode interface and significantly suppress side reactions caused by EC reduction, reducing ethylene gas evolution by 75% (Fig. 9f). Consequently, interfacial impedance growth is effectively suppressed, and the number of cycles required for the Si‖NCM622 full cell to reach an 80% capacity retention at 25 °C increases from 104 to 225 cycles; its performance at 45 °C also outperforms that of FEC-based electrolytes. More importantly, this system can partially compensate for additive consumption through regeneration reactions, demonstrating sustained interfacial regulation. This indicates that the role of lithium salt additives is no longer limited to initial film formation but lies in maintaining long-term interfacial stability through dynamic participation during cycling.

The regulatory role of electrolyte additives on silicon-based anodes has evolved from early-stage, simple interface modification to active restructuring of the SEI formation mechanism. Organic additives, such as FEC, emphasize the formation of an inorganic-enriched SEI through preferential reduction, whereas lithium salt additives, such as LiNO₃/LiNO₂, exhibit characteristics of “sustained participation” in interface regulation. The design of compatible electrolytes should not focus solely on the efficacy of a single additive but should place greater emphasis on its systematic impact on solvation structures, decomposition pathways, and interfacial evolution behavior. Future optimization efforts should not be limited to improving initial coulombic efficiency or single-cycle capacity, but should instead focus on the mechanical and thermal stability of the SEI, gas-related side reactions, and long-term compatibility under full-cell conditions. This will drive the design of electrolytes for silicon-based anodes from an empirical screening approach toward mechanism–driven interface engineering.

2.3. Development of multifunctional binders

Although binders account for a small proportion of lithium-ion battery electrodes, typically less than 10 wt%,^117–119 and do not directly contribute to capacity, they play a critical role in maintaining the structural integrity of the electrode and ensuring ionic and electronic transport.¹²⁰ Traditional binders are typically single-component natural or synthetic polymers, such as PVDF,¹²¹ CMC/SBR,¹²² SA,¹²³ PAA,¹²⁴ PVA,¹²⁵ CS,¹²⁶ GG,¹²⁷ GA,¹²⁸ PI,¹²⁹ and PAN.¹³⁰ However, these materials typically rely primarily on weak van der Waals forces and/or hydrogen bonds to maintain network connectivity,¹³¹ making them ill-equipped to withstand the immense volumetric stress generated by silicon anodes during long-term cycling. Consequently, they are prone to phase separation, structural degradation, and capacity decay.^132,133 Therefore, the development of novel binders with multiple synergistic effects has become a key direction for optimizing silicon-based anodes. Currently, based on their working mechanisms, multifunctional binders can be broadly classified as mechanically robust binders, conductive polymer binders, self-healing binders, and other functionalized binders.¹³⁴Fig. 10 summarizes the structural characteristics and key performance features of traditional silicon-based anode binders.

To enhance the overall mechanical strength, elasticity, dimensional stability, adhesion, and wettability of electrodes, in situ cross-linking has become one of the common strategies for developing high-performance polymer binders.¹²⁰ The core of this approach lies in constructing a continuous network capable of maintaining particle contact, transferring local stresses, and suppressing structural instability during the significant volume changes induced by charging and discharging of silicon anodes. Based on the fundamental nature of the cross-linking mechanism, these strategies are typically classified into two categories: chemical (covalent) cross-linking and physical (dynamic) cross-linking.

The advantage of chemical (covalent) cross-linking systems lies in their ability to firmly couple polymer chains to the surfaces of active particles via stable chemical bonds, thereby significantly enhancing the electrode's structural integrity and resistance to swelling. Bonjae Koo et al.¹³⁵ thermoset polyacrylic acid (PAA) with sodium carboxymethyl cellulose (CMC) under vacuum at 150 °C, constructing a highly cross-linked three-dimensional interconnecting network binder, c-PAA-CMC, through a dehydration condensation reaction, as shown in Fig. 11a. In this system, the cross-linked network not only provides high mechanical strength and deformation resistance but also enables the carboxyl groups in PAA to form covalent ester bonds with the hydroxyl groups on the silicon surface oxide layer (SiO₂), thereby further enhancing the interfacial bonding between the binder and the silicon particles. The synergistic effect of the three-dimensional network support and interfacial covalent anchoring not only effectively suppresses the irreversible migration of silicon particles during cycling but also reduces the binder's tendency to swell in the electrolyte, while promoting the formation of a more stable SEI film. The significance of chemically cross-linked binders lies not merely in “stronger adhesion”, but in maintaining the structural integrity of the electrode through the combined action of a rigid network and interfacial anchoring. Similarly, Wenqiang Zhu et al.¹³⁶ modulated the interactions between polyacrylic acid (PAA), sodium alginate (SA), and a silicon dendritic structure via a simple esterification reaction. After reacting at 150 °C for 2 h, they synthesized a moderately cross-linked PAA-SA binder, as shown in Fig. 11b. Compared to pure PAA or SA, the PAA carboxyl groups and SA hydroxyl groups in this system can form covalent ester bonds with the silanol groups on the silica surface, while hydrogen bonding also exists between the molecular chains. Consequently, the system maintains strong bonding capacity while retaining a certain degree of flexibility. The authors noted that this binder possesses both high mechanical strength and a certain degree of ductility, with a tensile strength of 47.8 MPa and a strain at break of 15.1%, enabling it to effectively accommodate the volumetric expansion of silicon; simultaneously, its contact angle is only 1.28° and its swelling ratio is 69.89%, indicating that it also exhibits good electrolyte wettability and chemical stability. More importantly, the esterification reaction reduces the polar groups on the surface of silicon particles, thereby suppressing interfacial side reactions and promoting the formation of a stable SEI film rich in LiF and Li₂CO₃. This suggests that chemical cross-linking does not necessarily mean that “harder” is better; rather, a more important design principle lies in achieving a balance between network rigidity, interfacial bonding, and electrolyte compatibility.

Unlike chemical cross-linking, physical (dynamic) cross-linking primarily enhances the mechanical stability of electrodes through reversible noncovalent interactions, such as hydrogen bonding, van der Waals forces, ionic interactions, metal ion coordination, host–guest interactions, π–π interactions, and chain entanglement effects.^137,138 The strength of these interactions typically falls between that of covalent bonds and weak intermolecular forces; they are characterized by reversible formation and breaking, thereby enabling dynamic stress release and network restructuring as the volume of the silicon particles changes repeatedly. The advantage of physical cross-linking lies not in constructing an absolutely rigid constraint framework, but in endowing the binder with the ability to “recover” and maintain the interface, thereby enhancing mechanical adaptability under long-term cycling conditions. Dejian Cheng et al.¹³⁹ prepared the water-based binder AMNG using acrylic acid (AA), acrylamide (AM), and acrylonitrile (AN) as raw materials via a one-pot aqueous radical polymerization process, as shown in Fig. 11c. This system combines strong stress dissipation capabilities with good ionic conductivity. It forms strong interfacial interactions with the hydroxyl groups on the surface of silica particles and significantly enhances the adhesion strength between the electrode material and the copper current collector. The role of the dynamically cross-linked network is not merely to strengthen inter-particle bonding, but also to establish continuous and tunable stress transfer pathways between the active material, binder, and current collector, thereby mitigating localized delamination and structural fracture during cycling. Li Deng et al.¹⁴⁰ prepared the supramolecular polymer binder poly (N-acryloylglycinamide) (PNAGA) via radical polymerization using N-acryloylglycinamide (NAGA), which contains diamide groups, as the monomer, as shown in Fig. 11d. The diamide groups on both ends of the binder's molecular chains can form stable intermolecular and intramolecular hydrogen bonds between the diamide groups, thereby constructing a supramolecular network that combines mechanical strength with interfacial bonding capability. Because these hydrogen bonds possess reversible reorganization properties, PNAGA not only effectively buffers the stress concentration caused by silicon particle expansion but also slows down the delamination between the active material and the binder during cycling. Compared to traditional rigid binders, this type of supramolecular network better embodies the essence of dynamic cross-linking, namely, maintaining electrode structure and interfacial integrity through the continuous reorganization of noncovalent interactions.

Multifunctional binders exhibit distinct trade-offs. Covalently cross-linked binders provide strong adhesion and mechanical reinforcement, but excessive rigidity and thermal curing may limit stress relaxation and processing flexibility. Dynamically cross-linked and self-healing binders accommodate volume changes through reversible bonds and repair interfacial damage, although their load-bearing strength and long-term stability require further validation. Ionically or electronically conductive binders improve charge transport and may reduce the demand for conductive additives, but excessive electrolyte uptake or complex functionalization can compromise mechanical integrity and increase manufacturing cost. For commercial electrodes, water-based processing, low binder content, rapid drying, high areal loading, and compatibility with calendaring and roll-to-roll coating are also important. Therefore, practical binder design must balance mechanical strength, self-healing capability, transport performance, and manufacturing compatibility. Representative binders and their electrochemical performance are summarized in Table 3.

Table 3. Comparison of representative multifunctional binders for silicon anodes.

Binder	Binder type	Current density	Cycle number	Capacity (mAh g⁻¹)	Rate capability	Binder ratio (wt%)	Initial coulombic efficiency (%)	Ref.
PAA-CMC	Mechanical performance	0.3 A g⁻¹	100	2100	30 A g⁻¹: 1600 mAh g⁻¹	20	88	135
PAA-SA	Binders mechanical performance binders	0.2 A g⁻¹	70	1300	—	20	89	136
AMNG	Mechanical performance binders	0.5C	120	2220.3	—	10	89.95	139
PNAGA	Mechanical performance binders	1.26 A g⁻¹	400	1942.6	1.2C: 1590 mAh g⁻¹	20	81	140
CG	Conductive polymer binders	0.84 A g⁻¹	700	1500	2C: 737 mAh g⁻¹	10	80	141
PAA-TUEG	Conductive polymer binders	0.5C	150	2250	2C: 1000 mAh g⁻¹	10	87.2	142
SHPET	Self-healing binders	4.2 A g⁻¹	250	870	4.2 A g⁻¹: 1594 mAh g⁻¹	20	88	143
xPAA-DABBF	Self-healing binders	0.5C	500	1774.45	5C: 1831 mAh g⁻¹	20	77.89	144
PDPP	Other-type binders	0.5C	100	2312	5C: 2084 mAh g⁻¹	15	94	145
PAA-FREP	Other-type binders	1 A g⁻¹	330	2300	2C: 2039 mAh g⁻¹	15	85.7	146
ACD	Mechanical performance binders	0.5C	400	1429	4C: 1274 mAh g⁻¹	10	92.8	147

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2.4. Pre-lithiation technology

Silicon-based anodes undergo significant volume expansion during lithiation, causing the solid-electrolyte interphase (SEI) on the surface of lithiated silicon to repeatedly rupture and reform. This phenomenon often leads to the formation of “dead lithium”, ultimately resulting in poor cycling stability, lithium dendrite growth, continuous thickening of the SEI film, and low initial coulombic efficiency (ICE). Pre-lithiation technology compensates for the loss of active lithium during the first cycle by introducing an additional lithium source into the anode or cell before normal cycling, serving as an effective method to enhance initial coulombic efficiency and battery energy density.^148–153 Pre-lithiation of anode materials primarily includes electrochemical methods, chemical methods, and active material-assisted pre-lithiation methods.¹⁵⁴

2.4.1. Electrochemical pre-lithiation

Electrochemical pre-lithiation uses a galvanic cell or electrolytic cell to actively incorporate lithium ions into the anode material. This method allows for precise control of the pre-lithiation degree and forms an initial SEI layer on the anode surface, thereby suppressing particle fracture and side reactions. For example, Kim et al.¹⁵⁵ constructed an external circuit by introducing a separator, electrolyte, and a 100 Ω current-limiting resistor between the C-SiO_x electrode and a lithium metal foil, and used the potential difference between the electrodes to pre-lithiate the C-SiO_x electrode, as shown in Fig. 12a. The pre-lithiation process enables precise control over the degree of pre-lithiation through real-time voltage monitoring and short-circuit duration control. It offers advantages such as high precision and structural stability, effectively addressing the core issue of low initial coulombic efficiency (ICE) in SiO_x electrodes Fig. 12b), ultimately increasing the initial coulombic efficiency for the first three cycles to 94.9%, 95.7%, and 97.2%, respectively—significantly higher than the 73.6% achieved by non-pre-lithiated electrodes. Lulu Guo et al.¹⁵⁶ proposed a perovskite-type anode pre-lithiation method using Li₂OHCl as a solid-state Li⁺ conductor. This method releases Li⁺ through the controlled electrolysis of Li₂OHCl, achieving a lithium release capacity as high as 810 mAh g⁻¹ and precisely compensating for lithium loss caused by the initial SEI formation on the Si@C anode (Fig. 12c and d). Meanwhile, the HCl generated during the process can be absorbed and recovered using a LiOH solution for the regeneration of Li₂OHCl, creating a sustainable cycle. This approach provides a pre-lithiation solution for high-energy-density silicon-based batteries that combines high capacity, controllability, and sustainability. However, electrochemical methods also have certain limitations; they typically require the battery to be disassembled and reassembled, which is a complex process, and they carry the potential risk of thermal runaway in metallic lithium, making them unsuitable for large-scale industrial applications.

Another strategy for electrochemical lithiation involves bringing the anode into contact with metallic lithium or stabilized lithium metal powder (SLMP), allowing lithium to be driven by an electric field to intercalate into the active material. However, uneven contact between silicon-based materials and metallic lithium can lead to uneven pre-lithiation. Therefore, to improve contact uniformity, researchers have employed buffer interface layers, applied pressure, or utilized nanostructure designs. For example, Qinghai Meng et al.¹⁵⁷ regulated the pre-lithiation process in a vacuum environment by inserting a resistance buffer layer (RBL) composed of a polyvinyl butyral (PVB)-coated carbon nanotube film between the lithium foil and the SiO_x electrode (Fig. 13a). As shown in Fig. 13b, the use of this RBL layer resulted in a more uniform distribution of lithium and carbon in the RBL-modified samples, leading to a significant improvement in the initial coulombic efficiency (ICE) of the SiO_x anode—from 79% to 89% in half-cells and from 68% to 87% in NCM622/SiO_x full cells. Yao et al.¹⁵⁸ prepared Si/GONRs composites consisting of silicon nanoparticles coated with graphene oxide nanoribbons (GONRs) via an electrostatic self-assembly method (Fig. 13c), which enhances conductivity and mitigates volume expansion. To improve the initial coulombic efficiency (ICE), they employed a direct-contact pre-lithiation strategy, applying a pressure of 1 kg cm⁻² between the Si/GONRs electrode and the lithium foil in an argon atmosphere, and precisely controlling the degree of pre-lithiation by adjusting the contact time. Thanks to the excellent conductivity and flexibility of GONRs, lithium ions and electrons are uniformly transported within the electrode, effectively avoiding issues such as local over-lithiation or insufficient pre-lithiation; simultaneously, a stable solid-electrolyte interphase (SEI) film forms in situ during the pre-lithiation process, with no obvious cracks or powdering observed on the surface of the silicon particles (Fig. 13d). However, the high cost and uneven distribution of SLMPs remain obstacles to their industrialization.

2.4.2. Pre-lithiation assisted by active materials

Active material-assisted pre-lithiation involves the reaction of a solid-state lithium source with inert components in the anode material to generate reversible or irreversible lithiated products, thereby eliminating active lithium loss while compensating for lithium loss during the initial cycles. Researchers have already applied this method to SiO_x materials to compensate for lithium loss caused by the formation of lithium silicate. For example, Angathevar Veluchamy et al.¹⁵⁹ produced Li₄SiO₄ particles by heat-treating SiO with LiOH at 550 °C, which effectively improved ICE and promoted Li⁺ diffusion while maintaining the structural integrity of the anode. Zhao et al.¹⁶⁰ directly synthesized Li_xSi alloys by mechanically stirring silicon nanoparticles and lithium metal foil at 200 °C for 6 hours. During this process, trace amounts of oxygen in the glove box naturally formed a dense Li₂O passivation layer on the surface of the alloy particles, resulting in a core–shell structure with an Li_xSi core and a Li₂O shell. This yields a high-performance pre-lithiation agent—Li_xSi-Li₂O core–shell nanoparticles (Fig. 14a). Due to its low potential and high specific capacity of 2000 mAh g⁻¹, this material effectively compensates for the initial irreversible capacity loss caused by the formation of the solid electrolyte interphase (SEI), thereby significantly increasing the first-cycle coulombic efficiency of the silicon nanoparticle anode from 74% to 94%.

However, this reagent still faces two major challenges on the path to commercial application. As shown in Fig. 14b, Li_xSi-Li₂O nanoparticles are only compatible with slurries prepared using low-polarity solvents such as 1,3-dioxolane (DOL) or toluene, in which they can release a lithium capacity as high as 1200–1400 mAh g⁻¹. In contrast, they are virtually incompatible with highly polar solvents such as N-methyl-2-pyrrolidone (NMP) or diethyl carbonate (DEC), rendering them ineffective, which limits their applicability in existing battery manufacturing processes. In addition, there is the issue of the reagent's chemical stability. Although the Li₂O coating confers good short-term stability in dry air (with a dew point of −50 °C)—with a capacity retention rate of approximately 70% after 5 days of exposure and the ability to effectively pre-lithiate graphite—it remains relatively sensitive to humidity and converts to LiOH in humid air (Fig. 14c). Therefore, its stability during long-term storage and practical processing requires further improvement. To address the humidity sensitivity of these Li_xSi nanoparticles, Zhao et al.¹⁶¹, inspired by the mechanism of SEI formation in batteries, developed a surface passivation method. This method involves reacting Li_xSi with 1-fluorodecane (eqn (1) and (2)) to form a uniform composite coating in situ on the nanoparticle surface (Fig. 14d). This coating significantly suppresses side reactions between Li_xSi and oxygen and moisture in the environment, substantially improving the material's storage stability in dry air while also demonstrating excellent moisture resistance, making it better suited for practical electrode preparation environments (Fig. 14e and f).

F−(CH₂)₉CH₃ + Li_xSi → LiF + Li−(CH₂)₉CH₃

Li–(CH₂)₉CH₃ + O₂/CO₂ → Li−OC( O)O−(CH₂)₉CH₃

2.4.3. Chemical pre-lithiation

Chemical pre-lithiation is a pre-lithiation method that utilizes the reaction between organic lithium or lithium-aromatic complexes in solution and the anode material to restore the radical anion to its initial state, thereby embedding lithium into the anode. Currently, researchers have employed chemical pre-lithiation agents such as Li-BP, Li-NP, and Li–FIr, which can achieve efficient lithium embedding within minutes and form a uniform SEI layer, significantly improving ICE and cycling performance. For example, Shen et al.¹⁶² developed a chemical pre-lithiation strategy using lithium naphthalene (Li-Naph) as the pre-lithiation agent. This method leverages the reducing properties of lithium naphthalene in dimethoxyethane (DME) solvent to successfully pre-lithiate the sulfur-polyacrylonitrile (S-PAN) composite into a Li₂S-PAN cathode and partially pre-lithiate silicon nanopowder into a Li_xSi anode, as shown in Fig. 15a. The resulting silicon/sulfur lithium-ion battery enables reversible lithium-ion shuttling between the sulfur cathode and the silicon anode, completely avoiding the issues of polysulfide dissolution and lithium dendrite growth found in conventional lithium-sulfur batteries. The pre-lithiated Si/Li₂S-PAN battery exhibits a high specific energy of 710 Wh kg⁻¹ and a first-cycle coulombic efficiency of 93.5% (Fig. 15b), along with excellent cycling performance. Yan et al.¹⁶³ used a tetrahydrofuran (THF) solution of the lithium-biphenyl (LiBp) complex to uniformly pretreat SiO/C microparticles in the liquid phase. The specific process involved immersing the SiO/C particles in the LiBp solution and stirring to allow LiBp to adsorb uniformly onto the particle surfaces. This was followed by a series of steps including centrifugation, washing, preheating (70 °C), and high-temperature calcination (750 °C), ultimately yielding the pre-lithiated product (LiBp-SiO/C), as shown in Fig. 15c. The key to this method lies in the combination of solution-phase and high-temperature solid-phase reactions, which successfully and uniformly pre-form crystalline lithium silicate within the SiO/C particles (characterized primarily as Li₂Si₂O₅, as shown in Fig. 15d. This preformed Li_xSiO_y phase replaces the active lithium supplied by the cathode during the battery's first charge cycle, directly “offsetting” the significant lithium-ion consumption caused by the formation of the solid-electrolyte interphase (SEI) and irreversible phase transitions. Consequently, the ICE of the half-cell is significantly improved from 75.6% for the original SiO/C to 90.0%. Zhang et al.¹⁶⁴ reported a new organolithium compound, Li-9,9-dimethyl-9H-fluorene-tetrahydrofuran (FIr). Using Li–FIr to pre-lithiate SiO anodes enables highly efficient chemical lithiation of silicon-based materials in just a few minutes, effectively improving the initial coulombic efficiency (ICE) and reducing the occurrence of side reactions. Furthermore, the pre-lithiation performance of Li–FIr is superior to that of Li-NP and Li-BP, and it effectively mitigates lithium loss during cycling. Chemical pre-lithiation methods are stable, safe, and suitable for roll-to-roll industrial production; however, it is necessary to select an appropriate solvent to ensure a low reduction potential for the lithium-aromatic compound and compatibility with the anode components.

From a practical perspective, the major pre-lithiation routes involve different trade-offs. Electrochemical pre-lithiation offers precise control of the lithium dosage, but cell disassembly, additional electrolyte and separator handling, and lithium-metal safety risks limit throughput and large-scale integration. Direct-contact lithium and SLMP methods simplify lithium delivery, yet uneven contact, local over-lithiation, high material cost, and moisture sensitivity remain important concerns. Active-material-assisted routes provide high lithium compensation, but many lithiated agents require strict dry-room handling and may be incompatible with conventional polar-solvent slurry processing. Chemical pre-lithiation enables rapid and relatively uniform lithiation and may be suitable for continuous processing, although highly reducing reagents, flammable solvents, washing and drying steps, and residual-reagent removal increase safety requirements and process complexity. Therefore, industrially viable pre-lithiation should combine controllable lithium dosage, storage stability, low-cost processing, and compatibility with slurry mixing, coating, drying, calendaring, and cell assembly.

3. Trends in silicon-based anode materials for lithium-ion batteries

With the growing demand for short charging times, long cycle life, and low cost, fast charging has become a key performance metric for lithium-ion batteries used in electric vehicles and portable electronic devices, with the core objective being to enable efficient recharging in a short period of time. Consequently, the development of lithium-ion battery technologies tailored to fast-charging requirements has emerged as a major research direction for silicon-based anodes.

Fast charging intensifies concentration polarization, charge-transfer polarization, and heat generation in silicon-based anodes. Repeated silicon expansion and contraction fracture the SEI, increase interfacial resistance, and produce non-uniform current distribution. When lithium-ion transport through the electrolyte and SEI cannot match the applied current, the anode potential approaches the lithium-deposition potential, increasing the risk of lithium plating, particularly at high state of charge, low temperature, and high charging rates. Meanwhile, polarization and ohmic heating accelerate electrolyte decomposition, SEI thickening, particle fracture, and conductive-network degradation, resulting in rapid capacity loss and increased safety risks. Therefore, fast-charging performance requires the coordinated optimization of interfacial kinetics, mechanical stability, and thermal management.

Recent studies have identified complementary routes to fast-charging silicon anodes. Tu et al. regulated the interfacial solvation structure to form a compact LiF-rich SEI, enabling rapid Li⁺ transport and 6 min charging in Ah-level pouch cells.¹⁶⁵ Hasan et al. showed that the fast-charging behavior of Si–graphite composite anodes strongly depends on temperature, state of charge, and current distribution, which jointly affect lithium plating and mechanical degradation.¹⁶⁶ In sulfide-based all-solid-state batteries, Cao et al. identified interfacial charge transfer as the dominant kinetic limitation and highlighted the trade-off between conductive additives and energy density.¹⁶⁷ These studies demonstrate that fast charging requires coordinated control of interfacial kinetics, reaction uniformity, and mechanical stability.

Future fast-charging technology for lithium-ion batteries will aim to achieve breakthroughs in high-rate performance, enhanced safety, extended lifespan, and compatibility across a wide temperature range. Efforts will focus on three key areas: innovation in materials systems, upgrades in intelligent control, and optimization of system integration. This will drive the large-scale adoption of fast-charging batteries in electric vehicles, energy storage facilities, and the aerospace sector, thereby supporting the transition of the transportation and energy systems toward greater efficiency and sustainability.

3.1. Innovations in materials systems

The design of electrolytes for core components compatible with fast charging will shift from concentration optimization to molecular engineering, with the aim of simultaneously enhancing ionic conduction rates, interfacial stability, and mechanical compatibility. Future research should explore the molecular design of PAEC-type solvents to reduce the charge transfer energy barrier by optimizing the orbital coupling between the solvent and lithium ions, thereby inhibiting lithium dendrite growth. Concurrently, multidimensional models could be used to screen wide-temperature-range solvents with low melting points, high boiling points, and weak solvation effects, enabling the electrolyte to maintain low viscosity and high ionic conductivity over the temperature range from −70 °C to 60 °C, thereby improving fast-charging performance under extreme conditions.

SEI films will evolve toward integrating toughness, conductivity, and self-healing capabilities, overcoming the limitations of traditional SEI films, which are hard, brittle, and prone to cracking. The incorporation of tough inorganic components such as Ag₂S/AgF can significantly enhance the mechanical stability of the SEI film, enabling it to withstand long-term cycling at high current densities without cracking; the in situ formation of asymmetric SEI films can substantially reduce the lithium-ion diffusion energy barrier and improve interfacial transport efficiency; simultaneously, self-healing SEI designs can dynamically repair cracks formed during cycling, reduce active lithium loss, and achieve an ultra-thin, dense, and high-strength interfacial structure.

In addition, silicon-based anodes will further advance the dual regulation of structure and composition. Through the design of a multi-level structure—featuring a macroscopically dense, microscopically porous, and nanoscale conductive network—they will balance volumetric energy density with fast-charging performance. For example, a gradient carbon shell structure can effectively mitigate volumetric expansion and establish continuous conductive pathways.

3.2. AI-driven dynamic charging strategies

Artificial intelligence can support silicon-anode batteries at the levels of material screening, state estimation, and charging control. For material screening, Yilmaz et al. constructed a literature-derived dataset of silicon thin-film anodes and used a Random Forest model to predict discharge capacity, achieving an R² of 0.86 and a mean absolute error of 174.1 mAh g⁻¹. Feature analysis identified working pressure, cycle number, and C-rate as major performance-related variables.¹⁶⁸ For state estimation, Li and Wu combined electrochemical features with a self-attention network to estimate battery state of health under different aging conditions, obtaining root-mean-square errors below 0.0033.¹⁶⁹ For battery control, Cao et al. integrated meta-learning with deep deterministic policy-gradient reinforcement learning to design fast-charging protocols using voltage, temperature, and state of charge as feedback. By transferring experience across different batteries, the model reduced the training requirements and improved adaptation to new cells.¹⁷⁰

These examples demonstrate that machine learning can connect material-property prediction, online battery diagnosis, and adaptive charging control. However, practical implementation remains limited by inconsistent datasets, insufficient cross-chemistry validation, poor model interpretability, and the difficulty of enforcing safety constraints. For silicon-rich batteries, future physics-informed models should incorporate stress evolution, SEI growth, lithium plating, thermal gradients, and aging-dependent parameter changes. Uncertainty quantification and experimental validation under practical cell conditions are also required before AI-derived charging policies can be reliably implemented in battery-management systems.

3.3. System integration optimization

Future system-level designs should focus on establishing efficient end-to-end ion-transport pathways to overcome internal transport limitations. Multiscale particle-size engineering of the cathode, AI-assisted electrolyte optimization, and low-tortuosity anode architectures could reduce internal resistance and heat generation. Dynamic interfacial regulation may further reduce interfacial impedance and improve ion-transport stability under fast-charging conditions.

Fast-charging technology will evolve toward low-cost, mass-producible solutions that are adaptable to a wide range of applications. By optimizing key processes such as solvent selection and electrode preparation, the cost of wide-temperature-range electrolytes can be reduced, and the preparation processes for structures such as artificial SEI and gradient electrodes can be simplified. At the same time, customized designs will be developed for various application scenarios—including electric vehicles in extremely cold climates, aerospace, polar equipment, and energy storage systems—to enhance low-temperature adaptability, reliability in extreme environments, and compatibility with long-cycle fast charging, thereby enabling rapid and efficient charging of distributed energy storage systems.

A clear distinction should be made between laboratory-level performance and commercially relevant conditions. Silicon-anode studies are often conducted in lithium-metal half-cells with low mass loading, thin electrodes, and excess electrolyte, which can underestimate irreversible lithium loss, electrolyte depletion, and transport limitations. Under high areal loading and lean-electrolyte conditions, increased electrode thickness, concentration polarization, non-uniform lithiation, repeated SEI formation, and mechanical degradation become more severe. Low N/P ratios further reduce the available lithium inventory, making initial coulombic efficiency and long-term lithium retention critical. Therefore, practical evaluation should include high areal capacity, controlled electrolyte-to-capacity ratio, realistic N/P ratio and electrode density, and long-term full-cell or pouch-cell testing. Areal and volumetric capacity, swelling, coulombic efficiency, and cell-level energy density should be reported in addition to gravimetric capacity.

4. Conclusions and outlook

With an ultra-high theoretical specific capacity of 4200 mAh g⁻¹, a low operating potential, and abundant crustal reserves, silicon-based anodes have emerged as a key candidate material for overcoming the energy density bottleneck in lithium-ion batteries. However, inherent defects such as severe volume expansion, low intrinsic conductivity, and slow lithium-ion diffusion rates during lithiation and delithiation can trigger a chain reaction of failures, including the pulverization of active particles, repeated rupture of the SEI film, and the breakdown of the conductive network, severely limiting their practical application.

To address these challenges, a series of solutions have been developed, including material and structural design, interface engineering, multifunctional binders, and pre-lithiation technology. At the material structure level, volume expansion buffering and enhanced conductivity are achieved through nanoscale processing, the construction of porous structures, silicon-carbon composites, and alloying. At the interface level, side reactions are suppressed and ionic transport efficiency is improved through the formation of artificial SEI films and electrolyte optimization. Multifunctional binders reinforce the structural integrity of the electrodes, while pre-lithiation technology effectively compensates for lithium loss during the first cycle and improves initial coulombic efficiency. The synergistic effect of these strategies has significantly enhanced the cycling stability and rate performance of silicon-based anodes, with some materials already achieving over 1000 cycles and demonstrating high-rate charging and discharging capabilities. Overall, the most promising route toward high-capacity lithium-ion batteries is the coordinated integration of practical Si–graphite composites, stable interphases, mechanically adaptive binders, and controllable pre-lithiation. These strategies should be validated under high areal loading, lean-electrolyte conditions, realistic N/P ratios, and full-cell configurations, with emphasis on initial coulombic efficiency, areal and volumetric capacity, electrode swelling, cycle life, safety, and cell-level energy density.

Beyond electrochemical performance, the safety and sustainability of silicon-anode technologies require equal attention. Unstable SEI formation, lithium plating, reactive pre-lithiation agents, and flammable solvents may increase thermal and manufacturing risks. Multistep nanostructuring, high-temperature treatment, solvent-intensive processing, and atmosphere control can also raise energy consumption and environmental burden. Recycling is further complicated by the heterogeneous composition of Si–C composites, strong binder adhesion, and accumulated interphase products. Nevertheless, recycled silicon from photovoltaic waste demonstrates the potential for circular material use. Future development should therefore combine safer and lower-solvent processing, design for recycling, direct material regeneration, and life-cycle assessment covering raw-material sourcing, electrode production, service life, and end-of-life recovery.

Despite substantial progress, several limitations still hinder the practical deployment of silicon-based anodes. Many reported high capacities are obtained in low-loading half-cells with excess electrolyte and cannot be directly translated to high-loading full cells. Nanostructuring, porous architectures, and multilayer coatings improve cycling stability but may reduce tap density, increase inactive mass, and complicate large-scale manufacturing. Artificial interphases, multifunctional binders, and pre-lithiation can mitigate lithium loss and mechanical degradation, but their long-term stability, process compatibility, dosage uniformity, cost, and safety require further validation. Future research should prioritize micron-scale Si–graphite composites with controlled silicon content, high areal capacity, lean electrolyte, realistic N/P ratios, and long-term pouch-cell testing. Scalable aqueous or dry-electrode processing, operando characterization, physics-informed artificial intelligence, and standardized reporting of cell-level energy density, swelling, safety, cost, and life-cycle impact will also be essential for laboratory-to-industry translation.

Conflicts of interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

This work was supported by the following grants: “Tianchi Talent” Introduction Program. Kashi University High-Level Talent Research Start-up Project (Grant No.: 022024173).

Biographies

Biography

Sirou Li is currently a graduate student in the class of 2025 at the School of Chemistry and Environmental Sciences, Kashi University. Her primary research focus is the modification of silicon-based anodes for lithium-ion batteries.

Biography

Jianing Xie is currently a graduate student in the class of 2024 at the School of Chemistry and Environmental Science, Kashi University. His primary research focus is on energy storage technology for new-energy lithium-ion batteries.

Biography

Zirui Li is currently a graduate student in the class of 2025 at the School of Chemistry and Environmental Sciences, Kashi University. His primary research focus is on energy storage technology involving electrode modification for new-energy flow batteries.

Biography

Zitong Wang is currently a student in the class of 2025 majoring in Chemical Engineering and Technology at the School of Chemistry and Environmental Sciences, Kashi University. His primary research focus is on energy storage technology involving electrode modification for new energy flow batteries.

Biography

Xiaomin Wang is currently a professor at the College of Chemistry and Environmental Science, Kashi University. He obtained his PhD degree from Northeastern University, China in 2010. His main research focuses on new energy materials and energy storage technologies.

Data availability

No primary research results, software or code have been included, and no new data were generated or analysed as part of this review.

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PERMALINK

Silicon-based anode materials for high-capacity lithium-ion batteries: recent advances and challenges

Sirou Li

Jianing Xie

Zirui Li

Zitong Wang

Xiaomin Wang

Abstract

1. Introduction

Fig. 1. Lithium storage mechanism in lithium-ion batteries (a), failure mechanisms (b), and strategies for improving silicon anode performance (c).

2. Strategies for improving the performance of silicon-based anodes in lithium-ion batteries

2.1. Material modification and structural design

2.1.1. Nanostructuring

2.1.2. Silicon-carbon composite materials

Table 1. Electrochemical performance of representative core–shell Si–C anodesa.

2.1.3. Alloying

Table 2. Electrochemical performance of representative Si–metal and silicide anodesa.

2.2. Interface engineering: creating a stable electrode/electrolyte interface

2.2.1. Construction of artificial SEI films: active control of interface stability

2.2.2. Electrolyte optimization: inducing the formation of a stable SEI layer

2.3. Development of multifunctional binders

Fig. 10. Structure and key characteristics of traditional silicon-based anode binders.

Table 3. Comparison of representative multifunctional binders for silicon anodes.

2.4. Pre-lithiation technology

2.4.1. Electrochemical pre-lithiation

2.4.2. Pre-lithiation assisted by active materials

2.4.3. Chemical pre-lithiation

3. Trends in silicon-based anode materials for lithium-ion batteries

3.1. Innovations in materials systems

3.2. AI-driven dynamic charging strategies

3.3. System integration optimization

4. Conclusions and outlook

Conflicts of interest

Acknowledgments

Biographies

Biography

Sirou Li.

Biography

Jianing Xie.

Biography

Zirui Li.

Biography

Zitong Wang.

Biography

Xiaomin Wang.

Data availability

References

Associated Data

Data Availability Statement

ACTIONS

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RESOURCES

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Table 1. Electrochemical performance of representative core–shell Si–C anodes^a.

Table 2. Electrochemical performance of representative Si–metal and silicide anodes^a.