Advances and perspectives of CVD-fabricated nano-scale Si-C anodes

Advances and perspectives of CVD-fabricated nano-scale Si-C anodes | Authorea try { document.documentElement.classList.add('js'); } catch (e) { } var _gaq = _gaq || []; _gaq.push(['_setAccount', 'G-8VDV14Y67G']); _gaq.push(['_trackPageview']); (function() { var ga = document.createElement('script'); ga.type = 'text/javascript'; ga.async = true; ga.src = ('https:' == document.location.protocol ? 'https://ssl' : 'http://www') + '.google-analytics.com/ga.js'; var s = document.getElementsByTagName('script')[0]; s.parentNode.insertBefore(ga, s); })(); Skip to main content Preprints Collections Wiley Open Research IET Open Research Ecological Society of Japan All Collections About About Authorea FAQs Contact Us Quick Search anywhere Search for preprint articles, keywords, etc. Search Search ADVANCED SEARCH SCROLL This is a preprint and has not been peer reviewed. Data may be preliminary. 14 October 2025 V1 Latest version Share on Advances and perspectives of CVD-fabricated nano-scale Si-C anodes Authors : Meng Fan , Jiajun Lin , Zhenxing Wang 0009-0004-6008-3183 , Xianyou Luo , Feng Yu , and Yong Chen 0000-0002-0419-7504 [email protected] Authors Info & Affiliations https://doi.org/10.22541/au.176047771.14061939/v1 297 views 159 downloads Contents Abstract Information & Authors Metrics & Citations View Options References Figures Tables Media Share Abstract The commercialization of nanoscale Si and SiOₓ anodes faces challenges like substantial volume expansion, extensive interfacial side reactions, and low initial Coulombic efficiency. Recently, Si-C anodes produced through chemical vapor deposition (CVD) by co-pyrolyzing silane and hydrocarbon gases on carbon scaffolds have attracted considerable attention from both academia and industry. The porous structure of carbon matrix facilitates the in-situ growth of Si particles, enhancing electrical conductivity and mechanical strength. This innovative design endows Si-C anodes with high initial Coulombic efficiency, large reversible capacity, minimal volume expansion, and stable cycling performance. However, comprehensive research on these CVD-derived anodes is still lacking, particularly regarding the structural-property-performance relationships. This review aims to highlight recent developments by examining the fabrication processes that influence electrochemical performance. Special attention is paid to various carbon materials, including Super P carbon, graphene, carbon nanotubes, and porous carbons with diverse pore size distributions and volumes. Factors affecting Si deposition, such as deposition model, precursor selection, temperature, atmosphere, and kinetics, are also discussed. Additionally, the review summarizes the use of carbon films on Si particles, considering aspects like layer thickness, hydrocarbon gas sources and temperatures. Finally, effective strategies are proposed to promote the industrial adoption of Si-C anodes. Review Lithium Ion Batteries Advances and perspectives of CVD-fabricated nano-scale Si-C anodes Meng Fan a , Jiajun Lin a Zhenxing Wang a *, Xianyou Luo a , Feng Yu a,b , Yong Chen a,b * M. F, J. L, Dr. Z. W, Dr. X. L, Prof. F. Y, Prof. Y. C a Engineering Technology Research Center for Green Energy Equipment and Materials of Guangdong Province, School of Materials and Energy, Foshan University, Foshan, 528225, China E-mail: [email protected] ; [email protected] Prof. Y. C b School of Materials Science and Engineering, Hainan University. Haikou, China. Keywords: silicon anode, chemical vapor deposition, coulombic efficiency, lithium-ion battery, volume expansion ABSTRACT: The commercialization of nanoscale Si and SiOₓ anodes faces challenges like substantial volume expansion, extensive interfacial side reactions, and low initial Coulombic efficiency. Recently, Si-C anodes produced through chemical vapor deposition (CVD) by co-pyrolyzing silane and hydrocarbon gases on carbon scaffolds have attracted considerable attention from both academia and industry. The porous structure of carbon matrix facilitates the in-situ growth of Si particles, enhancing electrical conductivity and mechanical strength. This innovative design endows Si-C anodes with high initial Coulombic efficiency, large reversible capacity, minimal volume expansion, and stable cycling performance. However, comprehensive research on these CVD-derived anodes is still lacking, particularly regarding the structural-property-performance relationships. This review aims to highlight recent developments by examining the fabrication processes that influence electrochemical performance. Special attention is paid to various carbon materials, including Super P carbon, graphene, carbon nanotubes, and porous carbons with diverse pore size distributions and volumes. Factors affecting Si deposition, such as deposition model, precursor selection, temperature, atmosphere, and kinetics, are also discussed. Additionally, the review summarizes the use of carbon films on Si particles, considering aspects like layer thickness, hydrocarbon gas sources and temperatures. Finally, effective strategies are proposed to promote the industrial adoption of Si-C anodes. 1. Introduction Silicon (Si) is recognized as a highly promising anode material for lithium-ion batteries (LIBs) due to its impressive theoretical specific capacity of 3579 mAh g -1 , natural abundance, and environmentally friendly properties. [1] However, the significant volume expansion (> 300%) that Si-based anodes undergo during lithiation and delithiation leads to considerable internal stress. [2] This stress can cause structural damage and loss of mechanical integrity within the active material, resulting in diminished electrical contact at the electrode/electrolyte interface and continuous formation of the solid electrolyte interphase (SEI). These interconnected failure mechanisms contribute to substantial irreversible capacity loss (initial Coulombic efficiency < 80%) and increased electrode polarization, posing major challenges to their commercialization. [3] Moreover, the low intrinsic electrical conductivity of Si (10 -4 S m -1 ) further limits its performance. [4] In the past two decades, extensive research has aimed to tackle the issues of volume expansion and low conductivity in Si-based anodes. Various strategies have been explored, including nano-structuring Si, [5-7] creating porous Si, [8-10] developing silicon oxides (SiO x ), [11-13] and applying carbon coatings. [14-16] Notably, nano-structuring Si has proven effective in alleviating volume expansion by reducing particle size. Studies suggest that a critical particle size of 150 nm or less can significantly suppress cracking and fragmentation during cycling, thereby mitigating the effects of volume expansion. [17] Additionally, the process of volume expansion occurs from the exterior to the interior of Si particles, leading to maximum stress concentrations within the particles. [18] Therefore, it is advantageous to produce Si particles below this critical size, ideally at the nanoscale, to minimize stress accumulation. While nano-structural approaches effectively improve the cycling stability of Si-based anodes, the inherent semiconducting nature of Si presents a fundamental challenge due to slow charge transfer kinetics. This limitation exacerbates electrode polarization and significantly restricts high-rate capability, emerging as a key hurdle in the advancement of nano-Si anodes. To address the low electrical conductivity of Si, researchers have turned to composite materials, with carbon being a favored component due to its excellent conductivity, flexibility, and cost-effectiveness. [19,20] As a result, silicon-carbon (Si-C) composites have become a prominent strategy for enhancing the performance of Si-based anodes. The evolution of Si-C anode technology can be categorized into three generations. The first generation focused on reducing Si particle size through mechanical ball milling to tackle volume expansion. The underlying concept was to utilize the voids between Si nanoparticles to accommodate the resulting volume changes. Theoretically, reducing Si particle sizes below 20 nm could effectively mitigate volume expansion. However, practical challenges arise, as mechanical ball milling struggles to achieve consistent particle sizes below this threshold without causing severe agglomeration, leading to larger particle sizes, impurity introduction, and rapid capacity decline. To enhance battery capacity and rate capability, a second-generation approach emerged, incorporating silicon monoxide (SiO x ) in place of pure Si. This strategy involves precursors formed from pure Si and silicon dioxide (SiO 2 ) to create SiO x . During lithiation/delithiation, SiO x reacts with Li + to produce elemental Si, lithium oxide, and lithium silicates. The resultant elemental Si further interacts with lithium to form Li x Si alloys, contributing to reversible capacity. Importantly, the Li 2 O and lithium silicates produced are electrochemically inactive in subsequent cycles, preventing further volume expansion and allowing for greater accommodation of stress during cycling. Although SiO x has a lower theoretical specific capacity than first-generation Si materials, it experiences reduced volume expansion (~118%) during lithiation, leading to improved cycling performance. [21] Nevertheless, the formation of substantial amounts of inactive phases during charge/discharge processes results in significant irreversible capacity loss and a low initial Coulombic efficiency (around 70%). These challenges, particularly in large-scale production, lead to increased raw material costs of 15%-20%, impeding widespread commercial adoption. As the development of Si anodes reached this bottleneck, the next-generation chemical vapor deposition (CVD) Si-C technology emerged, recognized as the third generation of Si-based anode technology. This approach involves integrating Si within a porous carbon matrix, where silane gas (SiH 4 ) is introduced into the pores of carbon particles. High-temperature pyrolysis decomposes the SiH 4 , dispersing Si nanoparticles within the carbon framework. The subsequent pyrolysis of hydrocarbon gases generates a dense carbon coating around the Si nanoparticles, which not only protects them from electrolyte corrosion but also enhances the overall electrical conductivity of the composite. However, achieving uniformity at the nanoscale remains a significant challenge that limits the development of technology. A noteworthy advancement occurred in 2021 when Group14, a US company, announced the start of commercial production of its CVD-derived Si-C anode, SCC55TM (Si:C = 45:55). [22] The porous carbon framework effectively buffers the volume expansion of Si during lithiation, dissipating internal stress and significantly reducing electrode expansion. Additionally, the carbon skeleton contributes to increased energy density. This material has demonstrated exceptional performance metrics, achieving a specific capacity of 1800 mAh g -1 and a cycle life exceeding 1000 cycles. This advancement establishes CVD as the favored method for leading manufacturers in the production of next-generation Si-C composite anodes. While numerous reviews have covered the structural design and modifications of Si-based anodes, [1,23-48] SiO x -based anodes, [49-51] as well as binder, [52-56] electrolyte designs, [57-60] and advanced characterization techniques, [61-63] a detailed exploration of the connections between material structure and electrochemical performance specific to CVD-fabricated Si-C anodes has yet to be systematically discussed in the literature. This review aims to provide a timely and comprehensive analysis of the relationships between material fabrication and overall performance ( Figure 1 ). It begins with an examination of the inherent characteristics of Si produced via CVD techniques, including aspects such as structural characteristics, particle size, Coulombic efficiency, and volume expansion, especially in comparison to conventional Si. Next, the various factors influencing the fabrication processes are summarized. Special emphasis is placed on carbon matrices, with a focus on different carbon species, including Super P carbon, graphene, carbon nanotubes, and high-surface-area porous carbons with varying pore size distributions and volumes. The discussion also encompasses key considerations for Si deposition, such as deposition model, precursor selection, temperature, atmospheric conditions, and deposition methods. Moreover, the deposition of protective carbon films on Si particles is summarized, highlighting factors like layer thickness, hydrocarbon gas sources, and applied methods. Finally, the promising strategies to facilitate the practical industrial adoption of Si-C anodes are proposed. Drawing on existing research accomplishments, this review presents forward-looking insights into the future development trends of next-generation CVD Si-C anode materials. Figure 1. Issues of Si anode and the corresponding strategies based on CVD-fabricated Si-C anode. Reproduced with permission. [64] Copy right 2025, Springer Nature. 2. Fundamentals of CVD techniques The practical implementation of Si anodes faces significant challenges stemming from their substantial cyclic swelling and shrinkage and inherently low electrical conductivity during lithium insertion/extraction. These large volume fluctuations induce detrimental effects, including electrode fracture, particle disintegration, and detachment from the current collector. Consequently, this degradation manifests as compromised charge-discharge efficiency and rapid capacity fading. Furthermore, the mechanical stresses generated by repeated expansion not only damage the electrode structure over cycles but also pose potential safety risks. To address these issues arising from volume changes, combining Si with carbon-based materials has emerged as a highly effective strategy. Incorporating carbon not only helps mitigate the volume strain experienced by Si during cycling, but also significantly enhances electrical conductivity and prevents Si particle coalescence. Figure 2. Schematic of CVD-derived Si-C anodes. Numerous fabrication routes, including solution precipitation, [65,66] sol-gel synthesis, [67] layer-by-layer assembly, [68,69] , sputtering, [70,71] atomic layer deposition, [72,73] and CVD, [74,75] are actively pursued for synthesizing Si-C composites. Among these, CVD offers distinct advantages in nanometer-scale tailoring of Si particle dimensions, spatial distribution homogeneity, and carbon coating thickness. The CVD process for Si-C anodes fundamentally comprises three stages: (1) preparation of the carbon matrix, (2) Si deposition, and (3) carbon film encapsulation. This typically entails pyrolyzing Si-containing precursors onto a carbon substrate. The choice of carbon substrate profoundly impacts the resultant composite. Variations in the microstructure and physicochemical properties of carbon substrates govern Si deposition kinetics and critically determine Si-C interfacial bonding characteristics. These factors, in turn, exert a dominant influence on the electrochemical behavior of composites. While substrate structure is undoubtedly crucial for CVD-derived Si-C anodes, understanding the kinetics and atomistic mechanisms of Si deposition is equally essential. This deposition stage directly dictates active material loading, distribution uniformity, and the quality of the nascent Si-C interface, a primary determinant of overall electrode performance. Subsequent carbon film growth via CVD depends critically on process parameters: precursor gases, flow rates, temperature, pressure, and duration. Precise modulation of these variables enables the fabrication of carbon substrate-Si-carbon film architectures with customized properties, which is vital for enhancing battery performance. As illustrated in Figure 2, gaseous precursors (e.g., SiH 4 ) flow into the reaction chamber over the carbon substrate. Thermal activation drives precursor decomposition and adsorption onto the substrate, followed by dehydrogenation. Notably, catalytically active carbon substrates can lower the energy barrier and required temperature for this dehydrogenation step. Depending on substrate properties, temperature, duration, and flow rates, adsorbed SiH 4 species may diffuse to form either Si or SiC nuclei. Crucially, the carbon substrate steers the morphological evolution and properties of the Si deposited. Finally, gaseous precursor, such as CH 4 , C 2 H 2 , C 2 H 4 and C 3 H 6 , et al., is thermally decomposed at high temperature to deposit a thin carbon film onto Si nanoparticles, which effectively prevents the corrosion of electrolyte solvents and ensures high Coulombic efficiency and stable cycling stability. Through orchestrated optimization of the carbon substrate, Si deposition conditions, and protective carbon film growth, CVD-synthesized Si-C composites achieve superior properties. This integrated approach effectively mitigates failure mechanisms inherent to Si lithiation/delithiation, leading to significantly enhanced electrochemical performance. Characteristics of Si anode derived by CVD technique 3.1 Structural characteristics. As shown in Figure 3a, the X-ray diffraction (XRD) patterns exhibit no detectable characteristic diffraction peaks of crystalline Si (c-Si), indicating that the CVD-synthesized nanoscale Si embedded in the carbon matrix is amorphous. [64] Furthermore, the high-resolution transmission electron microscopy (HRTEM) images acquired at lower magnification reveal no discernible crystalline domains in the Si, consistent with its amorphous nature (Figure 3b). Whether it is crystalline or amorphous phases, the lithiation can be described by the following reaction: Si + x Li + + x e - → Li x Si (1) Critically, the lithiation pathways of c-Si and amorphous Si (a-Si) diverge significantly, profoundly impacting electrochemical performance. Thermodynamically, distinct driving forces govern their lithiation behavior. Initial lithium insertion into c-Si is thermodynamically hindered, promoting phase segregation between the crystalline core and the forming amorphous lithiated Si (a-Li x Si). Conversely, a-Si undergoes homogeneous lithiation via the stable growth of a single a-LiₓSi alloy phase. This fundamental contrast in phase evolution dictates differences in structural integrity and stress accumulation within Si anodes. Kinetically, room-temperature lithium diffusion coefficients ( D Li + ) differ markedly. Computational studies reveal D Li + for c-Si is s -1 , compared to s -1 for a-Si, indicating approximately 100-fold faster lithium transport in the amorphous phase. [76,77] This kinetic advantage underscores the suitability of a-Si for high-rate applications. Furthermore, in widely used c-Si, lithiation-induced swelling exhibits pronounced anisotropy, occurring predominantly on planes. [78] The swelling rate on these planes can exceed that on other orientations by up to a factor of eight, leading to localized stress concentrations detrimental to electrode integrity. In contrast, the isotropic expansion characteristic of a-Si inherently circumvents this limitation of c-Si. [79] Analysis of reported lithiation potentials indicates that c-Si lithiates at approximately 0.2 V lower than a-Si. This voltage differential stems fundamentally from their divergent microstructural evolution pathways during lithiation, which consequently governs kinetic behavior and stress distribution within the electrode. Critically, the subsequent phase transformation from a-Li x Si to crystalline Li 15 Si 4 generates substantial internal stress, severely compromising Si anode integrity. However, within a suitably engineered CVD-derived Si-C composite anode, the carbon matrix provides effective mechanical confinement. This confinement suppresses the characteristic delithiation plateau of crystalline Li 15 Si 4 near 0.45 V. Consequently, the intrinsic amorphous nature of CVD-fabricated Si, coupled with this constraint, facilitates superior redox kinetics. Particle size. Departing from conventional methods that yield large, agglomerated Si nanoparticles, a-Si was synthesized via high-temperature thermal decomposition of SiH 4 vapor directly onto a conductive porous carbon substrate. This approach facilitated in-situ infiltration of a-Si along micropore walls, forming an integrated Si-C composite anode. Progressive Si deposition substantially reduced micropore volume in the carbon substrate, achieving near-complete micropore filling. N 2 physisorption analysis quantitatively assessed deposited Si dimensions through characterization of residual pore architecture and specific surface area evolution. [80] HRTEM analysis confirms dense Si infilling within the carbon matrix. Images reveal a-Si occupying pore volumes without observable interfacial voids or interparticle gaps, demonstrating intimate Si-C interfacial contact. Preferential SiH 4 deposition within carbon micropores, rather than superficial film growth, stems from nanoconfinement effects. The micropore architecture of substrate facilitates enhanced physisorption of small molecules like SiH 4 through collective van der Waals interactions along curved pore walls. This generates adsorption potentials exceeding those of planar surfaces, thermodynamically favoring pore-filling deposition. Consequently, Si dimensions are precisely dictated by host pore morphology. TEM further reveals uniformly dispersed spherical nanoparticles with diameters constrained below 2 nm (Figure 3c). [64] For example, the microporous activated carbon with 89% microporous volume proportion can form sub-nano Si (< 1 nm). [80] Replacing the porous carbon substrate with graphitized carbon black yields spherical Si nanoparticles 10-30 nm in diameter. [81] Also, a size distribution range from 5 to 20 nm was formed onto graphite when simultaneous pyrolysis of C 2 H 2 and SiH 4. [74] In conclusion, the deposited Si derived from CVD technique ranges from several tens of nano-meter to sub-nano scale. As the previous reports, if the size of Si nanoparticles is smaller than 150 nm, the nanoparticles will no longer be able to fracture against the volume expansion. Such size distributions are beneficial for the long-term cycling of Si anodes. Coulombic efficiency. Coulombic efficiency critically governs active material utilization and energy density in Si anodes, representing a fundamental barrier to commercialization. Initial Coulombic efficiency proves particularly decisive, quantifying first-cycle electrochemical reversibility. The low initial Coulombic efficiency of Si anode (50-80%) primarily originates from irreversible lithium consumption during SEI formation at the anode-electrolyte interface. During initial lithiation, c-Si undergoes phase transformation to amorphous Li x Si accompanied by anisotropic swelling (>300%), while delithiation induces drastic contraction. This cyclic dilatation fractures particles, continuously exposing fresh surfaces that promote parasitic SEI growth. Although nanostructuring and porosity engineering mitigate fracture, their high specific surface area exacerbates SEI-related lithium losses. Graphite anodes contrastingly achieve >94% initial Coulombic efficiency due to minimal volume change. In CVD-fabricated Si-C composites, conformal carbon coatings prevent nanoparticle detachment and suppress electrolyte penetration. Recent pore-engineering via CVD achieved a high initial Coulombic efficiency of 93.6% through precise spatial confinement of Si deposition (Figure 3d). [64] Conformal carbon encapsulation of Si nanoparticles promotes inorganic-dominated SEI formation, creating topological constraints that mechanically stabilize pore-confined Si. This generates a stress-voltage coupling phenomenon which effectively suppresses deleterious crystalline Li 15 Si 4 phase evolution. The architecture enables ultralow cycling fade (0.015% per cycle), establishing CVD as a critical enabler for high-efficiency Si anodes. Volume expansion. Bulk Si particles undergo extreme volumetric expansion (>300%) during lithiation, generating tensile hoop stresses that initiate surface cracking, particle fracture, and eventual pulverization. These cyclic dilatations produce unstable SEI that progressively thicken through continuous reformation. The resulting mechanical degradation and SEI instability cause electrical disconnection, reduced reversibility, and accelerated capacity fade. Integration with microporous carbon substrates resolves these limitations through engineered void spaces. Consider a-Si ( ρ = 2.23 g cm -3 ) infiltrated at 49 wt% into carbon with 0.85 cm 3 g -1 pore volume: the residual void fraction (0.64 cm 3 g -1 ) exceeds the theoretical expansion volume (0.63 cm 3 g -1 for 300% growth). While geometrically sufficient, practical constraints arise from: (i) morphological mismatch between nanopore cavities and expanding Li x Si phases; (ii) bidirectional stress transfer at Si/C interfaces. Through nanovoid architectural control, electrode expansion is constrained to 57% at full lithiation, demonstrating effective strain confinement (Figure 3e). [64] Figure 3. (a) Operando XRD patterns comparing CVD-derived Si-C composite and c-Si anodes lithiated to 0.01 V vs Li/Li⁺. (b) HRTEM micrograph illustrating conformal a-Si deposition via CVD (scale bar: 2 nm). (c) Phase-transformed c-Si nanoparticles after 900 °C annealing with corresponding diffractogram inset. (d) Correlation between initial Coulombic efficiency and capacity decay rate for benchmarked anode architectures. (e) Electrode expansion metrics at 4 mAh cm -2 areal capacity, demonstrating superior dimensional stability in pore-engineered Si-C anodes (57%). Reproduced with permission. [64] Copyright 2025, Springer Nature. Latest understanding in the process of CVD-fabricated Si-C anodes Establishing structure-performance relationships in Si-C anodes necessitates systematic analysis of fabrication parameters. This review synthesizes recent advances with emphasis on: (i) carbon substrate selection criteria; (ii) Si deposition dynamics; (iii) carbon coating engineering. This section particularly elucidate how carbon nanoscale architecture, including surface topology, pore geometry, and size distribution, governs SiH 4 decomposition pathways. Kinetic analysis further resolves deposition mechanisms through precursor adsorption/desorption energetics. Carbon matrix Si-C composite anode materials are fabricated through precise Si source and carbonaceous material proportioning, rational structural design, and subsequent forming/sintering or deposition. CVD preparation specifically involves pyrolytic deposition of Si-containing precursors onto carbon substrates. The choice of carbon substrate critically influences the process: variations in microstructure and physicochemical properties significantly impact Si deposition behavior and Si-C interfacial bonding characteristics, leading to marked differences in the final electrochemical performance. This section provides a comparative analysis of key carbon substrates, including Super carbon, carbon nanofiber, and graphite used in CVD for Si-C anodes, outlining their essential characteristics. It further examines SiH 4 application across these substrates and analyzes the influence of substrate on Si deposition kinetics. Reflecting recent commercial advancements, particular emphasis is placed on porous carbon substrates. The section compares precursor sources for various porous carbons, detailing their respective advantages and disadvantages, and analyzes the impact of critical porous carbon parameters, such as pore structure and specific surface area, on Si deposition. Findings indicate that porous carbons exhibiting appropriate pore volume, high specific surface area (about 2000 m 2 g -1 ), and a high microporosity fraction are optimal precursors for SiH 4 deposition. Based on this analysis, recommendations are provided for selecting suitable carbon substrates for CVD-derived Si-C composites. 4.1.1 Graphite-Si Graphite serves as the dominant commercial anode for LIBs owing to its low cost, structural stability, and high electrical conductivity. However, its theoretical capacity is limited to 372 mAh g -1 , falling short of the demands for next-generation high-energy-density LIBs. Crucially, the excellent conductivity of graphite can effectively compensate for the intrinsic poor conductivity of Si anodes. Consequently, forming Si-graphite composites represents a promising strategy. Petrat et al. demonstrated this approach by synthesizing nanoscale Si via SiH 4 pyrolysis and compositing it with graphite. [82] The material forms highly structured aggregates composed of ~50 nm primary particles featuring an amorphous surface layer. Utilizing CVD, Si particles can be embedded within graphite interlayers. In this configuration, graphite fulfills three key roles: contributing to a stable SEI layer, preventing Si particle aggregation, and enhancing electronic conduction throughout the anode. Scanning electron microscopy (SEM) imaging confirms a homogeneous distribution of nano-Si particles (20 wt%) within the graphite matrix. This composite delivers an initial discharge capacity of 1350 mAh g -1 with a Coulombic efficiency of 74%. Notably, it retains a capacity of 1000 mAh g -1 after 100 cycles at 74 mA g -1 . This relatively gradual capacity fade is attributed to the uniform dispersion of Si nanoparticles on graphite and their strong interfacial adhesion, demonstrating the effectiveness of graphite in buffering Si volume changes. However, cycling performance improvements remain constrained by the low initial Coulombic efficiency and limited tapping density. To address these limitations, a novel Si-graphite composite design (Si: 10 wt%) was developed. This material not only enhances Li + kinetics but also meets critical industrial electrode requirements. [83] As shown in Figure 4a, the composite integrates an edge-plane-activated graphite core with an a-Si nanolayer, synthesized via Ni-catalyzed hydrogenation and CVD using C 2 H 2 and SiH 4 gases. This design offers four key advantages: (1) enhanced graphite reactivity: the catalytic reaction activates Li + -reactive edge planes on the graphite; (2) improved conductivity and catalysis: residual Ni nanoparticles act as catalysts for ongoing activation and enhance overall electrical conductivity; (3) mechanical robustness: the graphite core serves as a structural framework, maintaining high tap density and withstanding mechanical pressure during electrode calendaring; (4) high capacity and fast kinetics: the nanoscale Si coating boosts energy density and enables rapid Li + transport. Electrochemical performance of this optimized Si-graphite anode was evaluated under industrial conditions, including high areal capacity of 3.4 mAh cm -2 and high electrode density of 1.6 g cm -3 (Figure 4b). The Si-graphite anode delivers a high specific capacity of 525 mAh g -1 , remarkable initial Coulombic efficiency of 93.8%, and excellent capacity retention of 99.3% after 50 cycles (Figure 4c). Separately, Cui et al. developed Si-nanolayer-embedded graphite/carbon hybrids using minimal SiH 4 , scaling production to 5 kg/batch while achieving dense a-Si deposition (Figures 5a-b). [74] This hybrid anode exhibits a high reversible capacity of 517 mAh g -1 and 92% initial Coulombic efficiency (Figures 5c-d). Critically, it suppresses electrode expansion even at high electrode density (>1.6 g cm -3 ) and areal capacity (>3.3 mAh cm -2 ). However, such composites face inherent limitations: constrained Si content restricts specific capacity, while excessive Si deposition thickens the nanolayer, accelerating capacity fade and negating nanoscale benefits. To increase Si loading, porous graphite, engineered via CO 2 etching heat treatment, has been proposed. This method creates internal pores/channels within spherical natural graphite, enabling higher Si incorporation. [84] Compared to conventional Si-graphite-C composites, this porous graphite substrate enables preferential Si deposition within its expanded pore network. This results in a thinner surface Si layer and more uniform distribution throughout the matrix. Consequently, anodes incorporating 15 wt% Si on porous graphite deliver a high reversible capacity of 817 mAh g -1 and maintain a capacity retention of 83.6% after 200 cycles. Complementing this approach, Cho et al. designed an advanced high-energy anode featuring an ultrathin Si coating on microporous carbon-graphite, protected by an outermost carbon layer. [85] This novel structure withstands calendering pressure without pore/Si-layer fracture while maintaining high energy density. Consequently, the composite delivers: (1) high volumetric capacity of 1064 mAh cm -3 ; (2) excellent initial Coulombic efficiency of 90.9%; (3) stable cycling at 3.6 mAh cm -2 areal capacity. Furthermore, emerging carbon substrates like biomass-derived and resin-derived carbons show promise as graphite alternatives. [86] Biomass-derived carbon often exhibits irregular morphology and structural non-uniformity, limiting electrochemical performance. In contrast, resin-derived carbon delivers superior advantages for Si-C anodes due to its well-defined morphology and tunable porosity. Recently, Yu et al. developed monodisperse spherical Si-C composites by converting phenolic resin spheres through controlled carbonization and activation into modified porous carbon substrates. [87] Monodisperse spherical carbon substrates enable uniform Si deposition within their porous networks via CVD. This nanoconfinement controls Si particle size while mitigating volume expansion during cycling. The obtained Si-C composites retain 93.3% of its initial capacity after 800 cycles in half cell, along with minimal volume expansion. 4.1.2 Carbon nanotube-Si However, Si-graphite composites typically have low Si content, resulting in unsatisfactory battery energy densities. To develop Si-C composites with high Si content, carbon materials featuring high surface areas or exposed pore structures have attracted significant interest. Carbon nanotubes (CNTs) are frequently employed as additives to enhance electrode electrochemical performance, leveraging their superior electrical conductivity, excellent mechanical strength, high aspect ratio, and low tortuosity. Therefore, integrating CNTs with Si represents a rational strategy. Recently, a high-strength, flexible, and highly conductive carbon skeleton composed of graphene and CNTs was constructed using CVD technique. [88] The unique combination of electrical, mechanical, and porous properties in this composite contributes to its excellent electrochemical performance. Specifically, the Si-based anode delivered a capacity of 802 mAh g -1 at 1000 mA g -1 , retaining 90.7% of its capacity after 500 cycles. Furthermore, porous carbon and soft carbon are also employed as carbon substrates due to their distinct structural advantages. [89] The micro-hard carbon matrix supports nano-Si particles while maintaining structural stability during cycling. The composite delivers a high discharge capacity of 1625 mAh g -1 with 86.8% initial Coulombic efficiency. Additionally, interconnected carbon-black particles with open structures serve as alternative substrates. Their high specific surface area (80 m 2 g -1 ) provides abundant deposition sites for Si. Annealing at 2000 °C induces graphitization, interconnects adjacent particles, and achieves >99.9% purification. [81] TEM analysis reveals spherical Si nanoparticles of 10-30 nm diameter deposited on annealed carbon black (Figure 5e), predominantly exhibiting amorphous microstructures. The nanoparticles densely coat the carbon surface, frequently anchoring to graphitic edge sites. Their spherical morphology minimizes Si/carbon-black contact area. When assembled into coin cells, the composite containing about 50 wt% Si delivers a high reversible capacity of 1950 mAh g -1 at C/20 (Figure 5f), exceeding the theoretical capacity of graphite by over fivefold. This indicates highly accessible active Si for Li + insertion in the designed architecture. Despite inherent sluggish kinetics in Si anodes, the composite maintains 1590 mAh g -1 at 1 C. Figure 4. (a) SEAG fabrication: Adsorbed Ni penetrated graphite via catalytic hydrogenation at 1000 °C, activating edge-plane sites on graphite surfaces. SEAG: edge-plane-activated graphite and a-Si nanolayer. (b) Tap density of different anodes. EAG: edge-plane-activated graphite. Commercial NG: commercial natural graphite. (c) Cycling performance: reversible capacity and Coulombic efficiency for different anodes over 50 cycles. Reproduced with permission. [83] Copy right 2017, Springer Nature. Figure 5. (a) SGC hybrid fabrication schematic: SiH 4 /C 2 H 2 gases adsorb and diffuse across PG surfaces and subsurface pores, enabling homogeneous Si/C coating. (b) HR-TEM of SGC interfacial region (insets: FFT patterns). Yellow dashed curves demarcate graphite, a-Si, and carbon boundaries. (c) Galvanostatic charge/discharge profiles of PG, SG, SGC and B-Si/G measured at 0.1 C. (d) Coulombic efficiency stabilization: Cycling evolution toward 99.5% CE from initial formation (five materials). PG: pristine graphite. SGC: Si-nanolayer-embedded graphite/carbon hybrids. SG: Si-nanolayer-embedded graphite. B-Si/G: physically blended nano-Si/graphite. Reproduced with permission. [74] Copyright 2016, Springer Nature. (e) Hierarchical assembly schematic: Bottom-up fabrication of Si-C composite granules. (f) Cycling performance: Reversible capacity and CE of C-Si granules vs. the theoretical capacity of graphite. Reproduced with permission. [81] Copyright 2010, Springer Nature. 4.1.3 Porous carbon-Si Porous carbon dominates CVD-fabricated Si-C anodes due to its abundance, hierarchical porosity, and cost-effectiveness. Produced through precursor pyrolysis with subsequent activation, this carbon matrix offers high specific surface area and interconnected pore networks ideal for CVD-based Si-C composites. Nano-Si deposition within internal pores accommodates volume expansion during cycling, significantly enhancing electrode stability. Mechanically, the low Young’s modulus of porous carbon (1-10 GPa) enables plastic deformation under stress, maintaining structural integrity without fracture. While its 3D network facilitates rapid Li + diffusion, reducing ionic resistance and improving rate capability. Recent work utilizes low-cost activated carbon (AC) with high microporosity as a CVD template for synthesizing highly dispersed sub-nano Si from SiH 4. [80] Commercial AC was loaded into a rotary furnace as a scaffold. Nano-Si was then incorporated via SiH 4 thermal decomposition at 430 °C, achieving uniform pore deposition (Figure 6a). Subsequent carbon encapsulation spatially isolated Si from the electrolyte, mitigating parasitic reduction. By controlling SiH 4 flow rate and duration, composites with tunable Si content/distribution were obtained. The AC scaffold provides both continuous conductivity and mechanical buffering for Si volume changes. Ultra-small a-Si particles enable isotropic expansion, enhancing structural stability. Nitrogen adsorption and desorption experiments were performed to indirectly assess the size of the deposited Si. The pores in AC primarily consist of mesopores approximately 4 nm and micropores around 0.7 nm, with micropore volume constituting 89% of the total pore volume. The extensive micropore volume facilitates the achievement of a significant amount of highly dispersed sub-nanoscale Si. After Si deposition, the composite decreases from 2274 m 2 g -1 to 18 m 2 g -1 . Moreover, there are no detectable 4 nm mesopores, and the volume of 0.7 nm micropores experiences a notable reduction from 0.83 cm 3 g -1 to 0.01 cm 3 g -1 . The micropore volume decreases to 1.2% of its pre-deposition level, indicating near-complete filling of the micropores of Si. This preferential pore filling, attributed to strong adsorption potentials in nanoconfined spaces, yielded highly dispersed sub-nano Si. The dramatic pore volume reduction and size distribution shift confirm the sub-nanoscale dimensions of Si. Consequently, ACS 0.48 C (48% Si) delivered 1500 mAh g -1 at 0.5C (1C = 1700 mAh g -1 ), outperforming ball-milled Si/AC electrodes (Figure 6b). For the porous carbon substrate, the influence of porosity on Si-C performance is important. To investigate the relationship between the pore structure and key electrochemical performance metrics, including initial Coulombic efficiency, rate capability and cycling stability. Recently, Yu et al. synthesized a series of porous activating carbon substrates to produce varying ratios of micropores and mesopores. [90] Figure 6c illustrates CO 2 activation of coconut shell carbon in a tube furnace, creating enhanced porosity to accommodate more Si. Adjusting activation time yielded carbon supports with controlled porosity. These underwent CVD processing: SiH 4 decomposition at 430 °C deposited Si nanoparticles within pores, followed by C 2 H 2 decomposition at 600 °C forming protective carbon encapsulation that isolates Si from electrolyte. To investigate the impact of microporous to mesoporous ratios on the performance of the Si-C materials, the deposition time of SiH 4 was controlled to achieve approximately uniform Si content. The samples are denoted as follows: AC 0.68 for the highest micropore-to-total pore ratio, AC 0.44 for the intermediate ratio, and AC 0.29 for the lowest ratio. To minimize the influence of other pore characteristics, the BET surface area was maintained at approximately 1735 m 2 g -1 , and the pore volume was controlled at around 0.88 cm 3 g -1 . Figure. 6d illustrates the difference in pore size distribution among the pristine coconut carbon, AC 0.68 and Si/AC 0.68 . The micropores in pristine coconut shell carbon are centered at 0.65 nm. The activated samples retain this micropore size of 0.65 nm but subsequently shift to a broader range of 0.75 nm to 1.25 nm in the Si/AC 0.68 sample. The mesopores, as calculated by the BJH desorption model, are centered at 4 nm, maintaining a similar pore size distribution to that of the carbon material. The broadening of the micropore size distribution is attributed to the filling of the original micropores with Si nanoparticles and carbon coating during the CVD process. Additionally, the mesopores present in the precursor material undergo shrinkage during Si deposition, further contributing to the observed broadening of the pore size distribution. The electrochemical performance of Si-C composite materials was evaluated by using assembled coin cells. As shown in Fig. 6e, the initial discharge capacities of Si/AC 0.68 , Si/AC 0.44 and Si/AC 0.29 were determined to be 1746, 1643, 1626 mAh g -1 , respectively. The initial Coulombic efficiencies were calculated to be 89.7%, 84.7% and 84.4%. These results indicate that Si/AC 0.68 , which has a high micropore ratio, exhibits superior initial Coulombic efficiency. This outstanding performance can be ascribed to two main factors: (1) the micropores effectively constrain the size of the deposited Si nanoparticles, limiting their growth and reducing volumetric expansion during Li insertion and extraction. In contrast, larger Si particles tend to form with an increase in mesopores leading to greater volume expansion during lithiation. (2) The increase in mesopores results in wider existing pores and a reduced pore wall thickness making the carbon framework more vulnerable to damage during volume expansion. The structural differences observed among these samples likely contribute to the variations in performance, which align with the measured initial Coulombic efficiency. Cycling stability tests show that Si/AC 0.68 retained 66.04% of its initial capacity, Si/AC 0.44 retained 77.30%, and Si/AC 0.29 retained 66.15% after 200 cycles. Notably, the sample with the highest micropore content demonstrated the best capacity retention (Figure 6f). Overall, the design and synthesis of this composite structure, where Si is deposited into the pores, effectively limit the Si particle size and further restrict expansion, giving rise to superior capacity retention during cycling. Critically, pore volume, distinct from porosity, serves as a vital design parameter for Si-C anodes. Recent studies systematically investigate carbon matrices with engineered pore volumes to elucidate their impact on electrochemical performance. [91] Figure 7a illustrates the CVD synthesis route. Carbon matrices exhibit characteristic hard carbon features: short-range ordered microstructures with randomly stacked graphitic nanodomains. N 2 adsorption-desorption isotherms display type Ⅰ isotherms with obvious sorption at the low-pressure region, demonstrating the presence of micropore (Figure 7b). Based on the BET method, the specific surface area values of the HC-1, HC-0.8, and HC-0.6 are 1836, 1678, 1593 m 2 g -1 , with the total volume of 0.91, 0.78, and 0.69 cm 3 g -1 , respectively (Figure. 7c). Here, HC-x: x = 1, 0.8, 0.6, x is the total pore volume. The results based on the Dubinin-Astakhov model in Figure 7c display that the pore size distributions of HC-1, HC-0.8, and HC-0.6 are mostly dominated by micropores, which is consistent with the average pore diameter results. Electrochemically, HC-0.8@Si@C delivers optimal cycling stability: 1335 mAh g -1 at 0.2C after 65 cycles (Figure 7d). To maximize performance, HC@Si@C precursors (12% content) were blended with graphite. Figure 7e shows HC-0.6@Si@C/Graphite experiences rapid capacity decay versus counterparts, indicating structural degradation during cycling. Figure 6. (a) Schematic illustration of synthetic methodologies of the Si-C composites. (b) Cycle performance of ACS 0.48 C and ball-milled nano-Si/carbon anode. (1C = 1700 mA g -1 ). Reproduced with permission. [80] Copyright 2024, Elsevier. (c) Synthesis procedure of Si-AC. (d) Micropore distribution and mesopore distribution of coconut shell carbon, AC 0.68 and Si/AC 0.68 . (d) Initial discharge capacities and initial coulombic efficiencies (ICE) of Si/AC 0.68 , Si/AC 0.44 , and Si/AC 0.29 . (e) Cycling stability of Si/AC 0.68 , Si/AC 0.44 , and Si/AC 0.29 over 200 cycles. Reproduced with permission. [90] Copyright 2025, Royal Society of Chemistry. Figure 7. (a) Schematic illustrating the synthesis of the HC-0.8@Si@C composite. (b) N 2 adsorption-desorption isotherms of the HC-1, HC-0.8, and HC-0.6. (c) Micropore size distributions of the HC-1, HC-0.8, and HC-0.6. (d) cycling performance at 0.2 C. (e) Long-term cycling performance of the HC@Si@C/Graphite//NCM811 full coin cells at 0.5 mA. HC-x: x = 1, 0.8, 0.6, x is the total pore volume. Reproduced with permission. [91] Copyright 2024, Wiley. For the novel CVD-derived Si-C composites with carbon matrices, elucidating structure-performance relationships between carbon architecture and deposition behavior holds fundamental scientific importance. Key porous carbon parameters, pore size distribution, volume, and specific surface area, critically govern Si deposition kinetics, nucleation mechanisms, and uniformity. These structural features dictate precursor diffusion/adsorption while controlling deposited Si morphology and spatial distribution. Consequently, fundamental mechanistic studies spanning molecular to microscale regimes are essential to establish quantitative structure-deposition correlations. Si deposition Despite the prevalence of SiH 4 as the primary gaseous Si source for CVD-based Si-C anodes, its deposition mechanisms remain incompletely understood. Research reveals SiH 4 pyrolysis involves complex intermediate species and surface reaction pathways critically governed by temperature, pressure, and gas flow dynamics. Furthermore, deposition methodologies, such as plasma-enhanced CVD (PECVD), dictate Si morphology, crystallinity, and distribution uniformity through kinetic modulation. These processing-structure relationships ultimately determine electrochemical performance. Consequently, elucidating SiH 4 reaction mechanisms and optimizing deposition parameters are critical for fabricating high-performance Si-C anodes. Figure 8. Schematic of SiH 4 decomposition into nano-porous carbon particles by a CVD process. Reproduced with permission. [92] Copyright 2024, American Association for the Advancement of Science. 4.2.1 Deposition model Conformal CVD of Si within nanoporous carbon is particularly advantageous for precise thickness control while leveraging the conductivity and stability of carbon. However, the precise relationships governing how deposition conditions and pore architecture dictate Si morphology remain unclear. Recently, a predictive model was developed to correlate deposition parameters and nanoporous carbon properties with Si thickness and uniformity, accounting for SiH 4 reactant transport through porous media. [92] Figure 8 illustrates three key transport processes of the model: (1) SiH 4 transport in the furnace (gas advection/diffusion); (2) SiH 4 diffusion within μm-scale nanoporous carbon particles; (3) SiH 4 pyrolysis forming solid Si inside particles. Deposition temperatures were optimized to 485-535 °C. Beyond 550 °C, substantial Si self-nucleation occurs, impeding uniform deposition; below 450 °C, SiH 4 decomposition becomes insufficient for practical deposition. Pressure effects were subsequently investigated across 0.2-2 atm. Lower pressures reduce deposition rates: achieving 40% coverage requires 17.4 min at 0.2 atm versus 4.7 min at 2 atm. This stems from higher SiH 4 concentrations at elevated pressures accelerating deposition. Counterintuitively, lower pressures enhance total Si deposition. Zone length variations (0.05-0.4 m) negligibly affect deposition rates. Conversely, carbon loading significantly impacts kinetics: 100 g carbon requires 9.7 min versus 5.1 min for 25 g. Reduced loading improves deposition uniformity. Beyond process parameters, pore characteristics (surface area, volume, size) critically influence deposition behavior. For nanoporous carbon, specific surface area (500-2000 m 2 g -1 ) inversely correlates with deposition kinetics: 500 m 2 g -1 requires 4.6 min versus 7.6 min at 2000 m 2 g -1 . Conversely, pore volume of 0.5-1.5 cm 3 g -1 exhibits positive correlation, deposition accelerates from 9.9 min (0.5 cm 3 g -1 ) to 3.3 min (1.5 cm 3 g -1 ). Pore size of 1-2 nm inversely affects deposition rate (4.4 min at 1 nm vs. 8.7 min at 2 nm), as smaller pores yield higher Si content per unit thickness. Optimal uniform deposition occurs at 485 °C with: (1) low pressure; (2) extended deposition zones; (3) reduced carbon loading. Low surface area and pore volume further enhance uniformity across the deposition zone, while pore size exhibits negligible influence. This model provides critical insights for tubular reactor optimization and advances deposition process design. Figure 9. (a) Calculated heat of reaction (∆ E ) for the reaction of the SiH 3 radical with ethylene (C 2 H 4 ) and SiH 4 . (b-c) High-resolution TEM images of Si-G (c) and C(5)Si-G with inset FFT images. The orange dotted curves indicate the boundaries between graphite and the Si or CSi layer, and the parallel lines show the d-spacing of each material. (d) Discharging capacity retention of Si-G/LCO and C(5)Si-G/LCO when cycled at 1 C (discharge) and 0.5 C (charge) at 25 °C using 1 Ah full-cell. Reproduced with permission. [93] Copyright 2021, Springer Nature. (e) Schematic illustrating the synthesis of CS-CNG particles. CS-CNG: SiC chemical bonding between Si and grphite/open-edge structure of carbon nanotube. Reproduced with permission. [94] Copyright 2023, Wiley. (f) Schematic of the synthesis of SiC x micro-sized particles. (g) Cycling performance of Si-C1-C, Si-C2-C, and Si-C3-C at 0.1C in the first cycle, and 0.2 C in the following. (h) Coulombic efficiency of Si-C1-C, Si-C2-C, and Si-C3-C. Here, SiH 4 and C 2 H 4 were mixed at volume ratios of 10:3, 10:5, and 10:7, donated as Si-C1-C, Si-C2-C, and Si-C3-C. Reproduced with permission. [95] Copyright 2024, Wiley. 4.2.2 Si precursor Beyond controlled SiH 4 decomposition for a-Si anodes, the co-pyrolysis of SiH 4 /C 2 H 4 via CVD was introduced to synthesize subnanoscale (<1 nm) Si embedded within a stable dual-phase carbon/Si carbide matrix. [93] Figure. 9a illustrates DFT-calculated thermal decomposition pathways for the SiH 4 /C 2 H 4 gas mixture. Calculations reveal SiH 3 radicals (from SiH₄ decomposition) preferentially react with C 2 H 4 rather than monosilane. This C 2 H 4 -mediated reaction interrupts continuous Si growth through Si-C bond formation, yielding subnanoscale (<1 nm) Si encapsulated within SiC/amorphous carbon matrices, unlike pure SiH 4 decomposition. The resulting SiC phase possesses high strength and toughness, significantly enhancing Si-based anode electrochemical performance. [96] Adjusting SiH 4 : C 2 H 4 ratios (10:0, 10:1.5, 10:5, 10:7; denoted Si, C(1.5)Si, C(5)Si, C(7)Si) significantly alters Si particle growth. Increasing C 2 H 4 reduces Si-Si bonds while increasing Si-C bonds. Carbon atoms adsorbed on Si surfaces inhibit Si-Si bond formation, suppressing cluster growth and yielding subnanoscale Si within SiC/amorphous-C matrices. Figures 9b and c showed high-angle annular dark-field scanning transmission electron microscopy (HAADF) images of the cross-sectional pristine Si and C(5)Si layer. The thickness of the C(5)Si layer (22 nm) was slightly greater than that of the pristine Si layer (15 nm) due to the existence of SiC/amorphous-C in the C(5)Si layer. As the amount of crystal growth inhibitor increased, the size of the Si crystals substantially decreased in the C(1.5)Si layer with the emergence of the SiC phase. Higher inhibitor concentration of C(1.5)Si further reduces Si crystal size with emergent SiC phase. This carbon-coated architecture enables 99.96% Coulombic efficiency after 50 cycles. As a result, a battery pack (107 kWh) containing 110 Ah full-cells was fabricated to verify the practical application of this anode, which demonstrated cycling stability of 91% after 2,875 cycles and a good calendar life of 97.6% for 365 days (Figure 9d). Beyond gas-phase co-pyrolysis, elevated temperatures promote beneficial nanoscale SiC formation. Conventional SiC synthesis requires temperatures >1400 °C, where annealing not only nucleates SiC at Si/C interfaces but also drives bulk crystallization, converting all Si to SiC. DFT reveals carbon edge structures enable SiC formation at significantly reduced temperatures versus graphitic carbon. [94] Figure 9c shows Ni catalysts restructure graphene into stacked oblique layers (10°-15°). These angled graphene domains provide highly reactive sites enabling SiC formation at 900 °C with a-Si nanolayers deposited via CVD. The resulting Si-graphite composite with interfacial SiC delivers 79.5% capacity retention after 300 cycles. Complementarily, Figure 9d demonstrates that CVD co-pyrolysis of SiH 4 /C 2 H 4 produces electrochemically tunable SiC x phases. [95] In this design, the fundamental SiC 4 tetrahedral units critically govern microstructural optimization and electrochemical enhancement. The optimized architecture delivers 1455 mAh g -1 with 95.8% capacity retention after 100 cycles. Pouch-type full-cell demonstrates that the composite possesses excellent cycling stability with capacity retentions of 82.5% after 500 cycles at 25 °C and 84.0% after 400 cycles at 45 °C. As a safer alternative to highly flammable SiH 4 for Si deposition, octamethyltrisiloxane (OMTS), featuring low decomposition temperature, has been employed. During vaporization at 130 °C, OMTS vapor was delivered into the tube furnace. [97] Figure 10a illustrates Si-C nanolayers deposited on commercial graphite via OMTS thermal decomposition under H 2 atmosphere. This architecture features three key advantages: (1) homogeneous amorphous C-Si nanolayers with isotropic Li + diffusion paths and ultrathin morphology enable rapid ion transport and high energy density; (2) the integrated 3D carbon skeleton suppresses subnanometer Si aggregation/volume change while enhancing Si-C electrical contact for accelerated electron/Li + transport; (3) the robust framework of graphite ensures 93.1% initial Coulombic efficiency, high tap density, and mechanical resilience during calendering. As a result, the composite exhibits a superior rate capability of 760.3 mAh g -1 at 5C, and a capacity retention of 85.3% after 1,000 cycles at 1 C, as well as a high initial Coulombic efficiency of 93.1% (Figure 10b). Beyond graphite substrates, Yu et al. employed engineered interconnected macroporous carbon architectures as conductive scaffolds, achieving superior electrochemical performance. [98] A controlled OMTS evaporation unit was integrated with the gas inlet of the box furnace. OMTS vapor concentration was precisely regulated via flow meter and switching valves. The resulting composite anode exhibits exceptional low-strain characteristics and fast-charging capability, featuring five key advantages: (1) uniform stress distribution enables minimal cumulative stress and isotropic expansion during lithiation, effectively eliminating stress concentration. (2) Intrinsic low-strain behavior accommodates volume changes of ultrasmall Si nanoparticles without macroscopic composite deformation. (3) Superior fast-charging performance resolves interfacial electron transfer limitations in conventional void-containing core-shell structures while providing aligned continuous pathways for accelerated Li + diffusion. (4) Structural robustness engineered interconnected macroporous carbon architecture suppresses Si agglomeration and enhances mechanical stability. (5) High energy density achieves high electrode compaction density coupled with high specific capacity. Benefiting from these advantages, the composite anode exhibits high specific capacity of 1301.4 mAh g -1 at 1 A g -1 after 1,000 cycles without apparent decay, and high-rate capacity of 910.3 mAh g -1 at 20 A g -1 . Except for the low temperature handling of OTMS, high temperature over 1000 ℃ can produce SiO x (1< x < 2) species. [99] Figure 10c illustrates the synthesis: (1) SiO x -C nanospheres (0<x<2) prepared via OMTS CVD at 1000 °C; (2) aluminothermic reduction yields Si-C nanospheres; (3) CH 4 /H 2 CVD grows secondary composites on nanospheres. The TEM image indicates that SiO x particles have a size number of less than 1 nm and are uniformly dispersed in the skeleton consisting of subnanoscale carbon. Based on this unique architecture design, the composites deliver a high capacity of 1279.6 mAh g -1 at 0.1 A g -1 , a high initial Coulombic efficiency of 91.2%, and a long cycling life of 81.3% after 1,000 cycles at 5 A g -1 . Besides, methyltrichlorosilane (CH 3 SiCl 3 ) was used as both Si and C precursor, which is a cheap byproduct in the organosilane industry. [100] The synthesized a-Si-C nanospheres demonstrate superior lithium storage performance compared to graphite. More importantly, CH 3 SiCl 3 is less toxic and flammable than SiH 4 , and significantly more cost-effective. Its use is expected to substantially reduce the production costs of Si-C composite materials, enabling the industrial-scale production of Si-C anode materials. Figure 10. (a) Schematic diagram of synthesis process of C-Si@graphite. (b) Long-term cycling performances at g 1.0 C and h 2.0 C of graphite and C-Si@graphite. [97] Permission with Springer Rare metals, 2023. (c) Schematic of the synthesis process of samples. (d) Long-term cycling performances at 1 A g -1 . Reproduced with permission. [98] Copyright 2024, Springer Nano-Micro Letters. (e) Synthesis diagram of C/VGSs@Si-C. C/VGSs@Si-C: a micron‐sized Si/C composite by anchoring vertical graphene sheets. (f) Cycling curves at 1 A g -1 . (g) Cycling curves at 5 A g -1 . Reproduced with permission. [99] Copyright 2024, Wiley. 4.2.3 Deposition method Furthermore, the choice of deposition method significantly impacts Si deposition morphology, crystallinity, and distribution uniformity by altering reaction kinetics. These factors ultimately determine the composite material’s electrochemical performance. Consequently, gaining an in-depth understanding of the SiH 4 deposition reaction mechanism and optimizing process parameters are crucial for preparing high-performance Si-C anode materials. CVD is a traditional technique for depositing thin films onto substrates via the decomposition of gaseous precursors. However, conventional CVD often requires high temperatures, making it unsuitable for non-catalytic and chemically unstable anode materials. Plasma-enhanced chemical vapor deposition (PECVD) is a widely used technique that utilizes plasma to activate chemical reactions during deposition. This enables the production of high-quality films at significantly lower temperatures than conventional CVD. In PECVD, SiH 4 is introduced into a reaction chamber. An applied electric field generates plasma, ionizing the gas and creating reactive species. These species interact with the substrate surface, decomposing SiH₄ and depositing Si nanoparticles. By adjusting process parameters, particle sizes can be controlled within the 10-200 nm range. The resulting Si nanoparticles exhibit good dimensional stability, low reaction temperatures, and faster deposition times. Laser-induced chemical vapor deposition (LICVD) is an advanced technique utilizing laser energy to initiate and control deposition reactions precisely. Gaseous precursors are introduced into the chamber, and a focused laser beam provides localized heating on the substrate surface. The laser energy excites the precursors, facilitating their decomposition and enabling the deposition of Si nanoparticles or carbon-based films. Compared to PECVD, LICVD offers a higher concentration of energy and a larger temperature gradient. This facilitates the preparation of amorphous or c-Si nanoparticles below 10 nm in size, with uniform particle size distribution and minimal contamination or by-product formation. For example, an original two-stage LICVD setup was designed specifically to synthesize Si-C core-shell nanoparticles. [101] Here, Si cores are synthesized in the lower stage of the reactor and are immediately conveyed by a carrier gas to the upper stage. In this second reaction zone, a carbon shell is deposited onto the Si core. This unique configuration is inherently safer as it eliminates the need for nanomaterial manipulation between the core and shell synthesis steps. This integrated process also ensures the protection of the Si surface against oxidation upon exposure to air. Consequently, the resulting Si-C composites deliver a high specific capacity of 2400 mAh g -1 at 0.1 C and maintain up to 500 mAh g -1 over 500 cycles at 2 C. Precise optimization of SiH 4 CVD parameters, including reaction kinetics, temperature, gas composition (particularly SiH 4 /C 2 H 2 or C 2 H 4 ratios), and deposition method, is critical. This process governs Si nanoparticle size, crystallinity, morphology, and surface properties, thereby determining key electrochemical performance indicators for Si-C anodes: initial Coulombic efficiency, specific capacity, cycling stability, and rate capability. 4.3 Carbon films Carbon films synthesized via CVD have garnered significant attention for rechargeable battery applications, where enhanced stability and capacity are critical for next-generation electronics and electric vehicles. Beyond inherent advantages, including high electrical conductivity, mechanical robustness, chemical stability, and flexibility, CVD offers exceptional versatility in tailoring carbon film architectures. This enables conformal coatings with engineered structures that precisely tune electrical and mechanical properties for battery optimization. [102] In this section, the CVD-grown carbon films are highlighted in the Si-C composite anodes, enabling them to overcome critical issues, such as volume expansion, sluggish kinetics, and unstable interfaces. [103] The growth of carbon films via CVD is influenced by various processing parameters, such as gaseous precursors, temperature, deposition time, and processing methods. By fine-tuning these parameters, carbon films with tailored properties can be produced, which is crucial for enhancing the electrochemical performance of Si-C composite anodes. Figure 11. (a) Effects of CVD-based carbon coating derived from CH 4 or C 2 H 2 . (b) Cycling performance at 0.75 A g -1 for 100 cycles. Reproduced with permission. [104] Copyright 2025, American Chemical Society. (c) Schematic illustration of synthesis process of Si-C hybrid composite material. (d) Magnified TEM image at the interfacial region of the Si-C particle. The yellow dotted curves indicate the boundaries between graphitic and amorphous C. (e) Long-term cycling stability at 0.2 C. SN-MCB: Si nanocrystal-micro carbon ball. Reproduced with permission. [86] Copyright 2025, American Chemical Society. (f) Schematic illustrating the fabrication of the Si-graphene via CVD. (g) Schematic illustrating the mechanism of SEI on Si-graphene. Reproduced with permission. [105] Copyright 2025, Wiley. 4.3.1 Gaseous precursor Gaseous precursors, such as CH 4 , C 2 H 2 , C 2 H 4 , and C 3 H 6 , are introduced into the reaction chamber and flow over the substrate. [84,86,104,106,107] The activation and decomposition of these precursors are driven by thermal or plasma energy. Then carbon species adsorb on the substrate, followed by dehydrogenation. The temperature and precursor show strong connection on the effect of carbon coating layer. Recently, Chio et al. explored the effects of carbon source and temperature on the CVD process. [104] As shown in Figure 11a, CH 4 and C 2 H 2 were selected as representative carbon sources. Results indicate that Si-based anodes coated with CH 4 -derived carbon at elevated temperatures exhibit superior electrochemical performance compared to those using C 2 H 2 . CH 4 yields a vertically aligned carbon coating, while C 2 H 2 produces a smooth carbon layer. The vertical microstructure enhances physical interparticle connectivity, facilitating electron transport and maintaining electrical contact during active material volume changes. Conversely, the smooth carbon layer reduces electrode surface area, mitigating electrolyte decomposition. These morphology-dependent functionalities are governed by carbon source selection. The optimized CH 4 -1000 sample (CH 4 -CVD coating at 1000 °C) demonstrated exceptional performance, delivering 778 mAh g -1 at 0.75 A g -1 with 92.8% capacity retention after 100 cycles (Figure 11b). When C 3 H 6 served as carbon source at 800 °C, it formed a thin graphitic carbon layer on Si nanoparticles (Figures 11c-d). This nanostructure simultaneously provides high electronic conductivity with shortened ion/electron transfer paths, while suppressing pulverization and accommodating volume changes during lithiation/delithiation. The composite anode maintained 80% capacity retention over 500 cycles at 0.2 C with >99.8% Coulombic efficiency (Figure 11e). Recent work employed CVD to grow vertical graphene nanosheets on Si nanoparticles and within internal pores (Figure 11f). [105] This flexible vertical graphene nanosheet layer establishes a robust conductive network with oriented channels, enabling stable operation under high areal mass loading (11.0 mg cm -2 ) while mitigating volume expansion. Cryogenic TEM analysis reveals a thin, continuous LiF-rich SEI formed on the nanosheets, ensuring cycling stability. Consequently, the composite anode maintains 641.9 mAh g -1 after 1,000 cycles with 95.9% capacity retention. Figure 12. (a-f) TEM images of Si, Si@C-1, Si@C-2, Si@C-3, Si@C-4 and Si@C-5, respectively. (g) Cycling stabilities at 0.2 A g -1 of Si@C electrode samples. Reproduced with permission. [108] Copyright 2022, Elsevier. 4.3.2 Thickness Beyond the effects of carbon precursors and temperature on coating composition, precise regulation of carbon layer thickness critically governs the electrochemical performance of Si-C anodes. Gao et al. synthesized carbon coatings with controlled thicknesses via CVD by varying precursor deposition time, systematically investigating their influence on Li + ion diffusion kinetics and interfacial charge transfer. [108] As shown in Figure 12a, TEM analysis reveals pure Si nanoparticles with diameters of with reaction time, measuring 0.8, 1.0, 2.2, 6.1, and 9.7 nm, corresponding to 1-2, 2-3, 6-7, 15-16, and 29-30 graphene layers respectively. Thermogravimetric analysis (TGA) performed from room temperature to 1000 °C under oxygen quantified carbon content in Si@C composites: Si@C-1 (2.45 wt%), Si@C-2 (3.68 wt%), Si@C-3 (5.99 wt%), Si@C-4 (15.96 wt%), and Si@C-5 (35.66 wt%). The Si@C-2 electrode delivered 1759 mAh g -1 at 0.2 A g -1 after 500 cycles, demonstrating exceptional cyclability. This performance indicates that 2-3 carbon layers optimally balance electrical conductivity and mechanical strength, effectively buffering the volume expansion of Si during lithiation/delithiation. Unlike spherical morphologies, CVD-derived Si nanoparticles (typically dozens of nanometers to sub-nanometer scale) on high-surface-area substrates require distinct pore structure regulation. Recently, Yang et al. demonstrated a sieving-pore carbon design that overcomes mechano-kinetic limitations to enable stable, high-rate lithium cycling in Si anodes. [64] This sieving-pore architecture features an inner nanopore body with reserved voids to accommodate deformation in high-mass-content Si, and an outer sub-nanometer pore entrance that enables pre-desolvation while facilitating rapid intrapore ion transport during cycling. As shown in Figure. 13a, SCC materials were fabricated via a two-step CVD process: (1) thermal decomposition of SiH 4 at 450 °C on porous carbons (PCs) embeds a-Si along micropore walls, forming an open-pore Si/C electrode. (2) Subsequent pyrolysis of C 2 H 2 at 600 °C deposits sieving carbon that narrows pore entrances. Crucially, as C 2 H 2 pyrolysis is diffusion-controlled, rapid decomposition occurs preferentially at pore entrances rather than within pore bodies, enabling precise formation of sieving structures. The PC pore size distribution critically governs SiH 4 and C 2 H 2 pyrolysis behavior. By precisely controlling carbon deposition duration, sub-nanometer pore entrances were tuned. Figure 13b demonstrates pore characterization using molecular probes: N 2 (0.5 nm kinetic diameter at 77 K) and CO 2 (0.35 nm at 273 K). The specific area and pore volume under N 2 and CO 2 testing conditions are calculated using the Brunaure-Emmett-Teller (BET) mode. When the deposition time ranges from 20 to 80 minutes, both N 2 and CO 2 adsorption-desorption measurements show obvious adsorption, indicating that the pore entrance size is primarily above 0.5 nm, corresponding to an open-pore structure that is incapable of effectively sieving the electrolyte. When the deposition time exceeds 100 minutes, the N 2 measurement no longer shows significant adsorption, while the CO 2 measurement still exhibits noticeable adsorption, suggesting that the pore entrance size is primarily regulated between 0.35 and 0.5 nm, corresponding to a sieving-pore structure that effectively sieves the electrolyte. When the deposition time is extended to 200 minutes, neither N 2 nor CO 2 measurements show effective adsorption, indicating that the pore entrance size is primarily below 0.35 nm, which corresponds to the formation of a closed-pore structure. Systematic variation of C 2 H 2 deposition time revealed critical performance tradeoffs: smaller pore entrances marginally reduced capacity (1773 vs 1860 mAh g -1 ) due to non-active carbon, but significantly enhanced initial Coulombic efficiency (93.6% vs 87.2%) by limiting solvent ingress and side reactions. Excessive carbon coating degraded both metrics. The optimized 0.35-0.5 nm pore entrance size balances minimal capacity loss with maximized efficiency by promoting pre-desolvation and forming inorganic-rich SEI layers. This design enabled practical pouch cells achieving over 1,700 cycles with fast-charging capability. Figure 13. (a) Schematic of the synthetic procedure of SSC materials and the comparisons between the customized-micropore, undersized-pore, and oversized-pore PC supports for fabricating sieving pores. The PC support is illustrated as a grey pore, while the yellow and black irregular shapes represent the deposited Si layers and carbon layers, respectively. (b) CO 2 (273 K) and N 2 (77 K) adsorption-desorption isotherms of SC, SC samples with different C 2 H 2 deposition times, and SSC samples. (c-d) Pore size distributions derived from CO 2 and N 2 adsorption-desorption isotherms, based on DFT calculations, for SC, SC samples with different C 2 H 2 deposition time, and SSC samples. (e) The initial charge/discharge profiles of SC, SC samples with different C 2 H 2 deposition times, and SSC samples. (f) Electrochemical performance comparison of SC, SC samples with different C 2 H 2 deposition times, and SSC samples. Reproduced with permission. [64] Copyright 2025, Springer Nature. 4.3.3 Method Beyond gas precursors and coating thickness, the deposition technique critically determines carbon layer quality. Fluidized bed chemical vapor deposition (FBCVD) offers distinct advantages over conventional CVD for fabricating Si-C anodes in LIBs, enabling uniform coatings, precise particle size control, and conformal deposition on complex geometries. This technique achieves high-quality carbon layers through enhanced mass/heat transfer in a reactor featuring bottom gas inlet and top outlet configurations. Optimal coating requires stable fluidization, primarily governed by minimum fluidization velocity. Particle size exerts the dominant influence on fluidization velocity, followed by particle density and bed diameter, thereby determining fluidization stability. As shown in Figure 14a, precisely measured pristine Si (PSi) powder was loaded onto the support plate of reactor. Process gases enter below the plate and exhaust through the overhead vent system. [109] The synthesis protocol comprised: (1) Ar gas introduction at room temperature; (2) temperature ramping to 800 °C at 5 °C min -1 ; (3) controlled introduction of 10% acetylene for 10, 30, or 50 min. Samples cooled naturally to room temperature were designated PSi@C10, PSi@C30, and PSi@C50. Figure 14b compares 100-cycle performance of PSi versus carbon-coated variants. While PSi delivers high initial capacity (2944.1 mAh g -1 ) and initial Coulombic efficiency (92.4%), it suffers rapid degradation (14.5% retention after 100 cycles). Conversely, PSi@C30 maintains 83.6% capacity retention. This performance enhancement stems from: (1) optimal carbon thickness achieved when gas diffusion and surface adsorption reach equilibrium; (2) conformal carbon encapsulation functioning as protective barrier; (3) selective pore-conformal deposition without overgrowth. Separately, PECVD recently produced onion-like carbon coatings on Si nanoparticles via CH 4 decomposition at 800 °C. [88] This composite delivers 802 mAh g -1 at 1 A g -1 and maintains 90.7% capacity retention after 500 cycles. When paired with a commercial NCM811 cathode in full-cell configuration, it achieves an energy density of 430 Wh kg -1 with exceptional cycling stability. Figure 14. (a) Schematic illustration of the FBCVD approach for PSi@C from a low-cost AlSi alloy powder. (b) The performance after 100 cycles at 0.5 A g -1 following 3 activation cycles. Reproduced with permission. [109] Copyright 2023, Elsevier. Despite significant efforts to utilize carbon films for addressing challenges in Si-C anodes, studies focused on theoretical or fundamental aspects remain limited. Future research should prioritize gaining deeper insights into how carbon film properties influence battery performance. Key parameters, such as film thickness, defect density, porosity, degree of graphitization, and grain size, significantly impact the electrochemical performance of Si-C anodes. However, the relationships between these parameters and performance are underexplored. This lack of comprehensive understanding hinders the full optimization of carbon films for Si-C anodes. A thorough elucidation of these correlations is essential to explore ideal carbon film structures and properties for battery applications. Industrial-scale CVD equipment for Si-C composites The performance of Si-C composite anode materials produced via next-generation CVD processes depends not only on the selection and optimization of raw materials but also critically on the deposition equipment itself. This novel Si-C composite is synthesized primarily from SiH 4 gas and porous carbon. Within its cost structure, SiH 4 gas accounts for up to 50% of the total, while the porous carbon precursor constitutes approximately 35%. The Si and C components in the composite exhibit a mass ratio of approximately 1:1. Producing one metric ton of the Si-C anode precursor requires over 0.6 ton of SiH 4 . Although SiH 4 currently commands a relatively high price, projections indicate it could potentially decrease to CNY 50,000 per ton or lower in the future, suggesting significant cost-reduction potential. Concurrently, porous carbon is currently priced around CNY 200,000 per ton, with projections indicating a potential decrease to the CNY 80,000-100,000 per ton range. Besides, core parameters of the deposition equipment, such as temperature field uniformity, gas flow distribution characteristics, and pressure control precision, directly impact the deposition uniformity, reproducibility, and process safety of the material. Furthermore, the single-run deposition capacity and continuous production capability of the equipment are key metrics determining its industrial feasibility. These factors directly influence production costs and large-scale manufacturing efficiency, thereby governing the commercialization progress of the technology. The rotary kiln is a stationary bed calcination equipment that ensures uniform heating of materials through tilting and rotation. During the preparation of CVD-derived Si-C anode materials, porous carbon substrate material is loaded into the rotary kiln. An inert gas is introduced, and the temperature is raised to approximately 500 °C. SiH 4 gas is then fed in for vapor deposition to form a Si layer. Subsequently, heating continues, and a carbon source is introduced for secondary deposition to form a carbon layer, thereby synthesizing the Si-C composite material. As a widely adopted calcination unit in various industries, rotary kilns offer mature technology, stable operation, reliable safety, high single-unit capacity, straightforward production scale-up, and good fuel adaptability. However, when utilized as deposition equipment, rotary kilns are prone to non-uniform deposition, low SiH 4 utilization efficiency, and poor batch-to-batch consistency, ultimately resulting in inferior performance of the final Si-C composite material. Consequently, resolving the uniformity issue during the deposition process within rotary kilns requires further optimization. Equipment currently used for the industrial production of CVD Si-C anodes is primarily dominated by fluidized beds and rotary kilns. Fluidized bed equipment is a process unit that fluidizes solid particles using a gas or liquid stream. [110] As illustrated in Figure 15, during the preparation of Si-C anodes via CVD, the flow velocity and temperature of the fluid are adjusted to ensure uniform distribution of Si particles within the bed. This facilitates the deposition of nano-Si onto/into the porous carbon and enables carbon coating of the Si particles. Fluidized beds are regarded as the future direction for industry development due to their superior deposition uniformity, high SiH 4 utilization efficiency, and the capability to control Si particle morphology and size, thereby ensuring the homogeneity and stability of the Si-C composite material. However, the adsorption and cracking of SiH 4 require high-pressure and high-temperature conditions. Consequently, fluidized bed equipment necessitates excellent sealing integrity and high-pressure capability to achieve gaseous coating of fine particles. This results in high operational complexity, significant safety risks, and substantial challenges for scale-up. Currently, most manufacturers utilize fluidized bed reactors with capacities around 20 kg per batch for producing CVD Si-C anodes, resulting in relatively low output. While equipment suppliers have developed fluidized bed units exceeding 100 kg per batch, the validation of these systems, optimization and refinement of the associated processes, and their deployment for mass production will require considerable time. Figure 15. Schematic representation of the plasma combined with a fluidized bed reactor. Reproduced with permission. [110] Copyright 2025, Elsevier. Summary and perspectives This review provides a systematic summarization of recent research progress in the preparation of Si-C composite anode materials via CVD technique. Firstly, it focuses on the influence mechanisms of different carbon matrices, including graphite, CNTs, and porous carbon, on SiH 4 deposition kinetics. Secondly, the characteristics of various Si source materials and their impact on the deposition process are analyzed in detail. Particular emphasis is placed on elucidating the deposition kinetics mechanism of SiH 4 on carbon matrix surfaces, including temperature and atmosphere. Thirdly, the growth of carbon films via CVD is influenced by various processing parameters, such as gaseous precursors, temperature, time, and processing methods. Finally, the current technological status and development trends of industrial-scale production equipment for CVD-fabricated Si-C anode materials. In recent years, the third-generation Si-based anode technology route, which utilizes CVD deposition of SiH 4 onto porous carbon, has progressively advanced towards large-scale production and commercial applications, gaining substantial favor among numerous new energy enterprises. Notwithstanding significant advancements in the performance of CVD Si-C anodes achieved through collaborative academia-industry efforts, several persistent challenges and limitations remain. Based on the current research landscape, the following critical directions warrant focused attention to accelerate technological development (Figure 16): Figure 16. Illustrates of possible and feasible methods for modulating the CVD-fabricated Si-C anodes. 1. Carbon substrate. Given the adoption of porous carbon as the matrix material in novel CVD Si-C composites, an in-depth investigation into the structure-performance relationships between the structural characteristics of porous carbon and its deposition behavior holds significant scientific merit. Specifically, key structural parameters of porous carbon, including pore size distribution, pore volume, and specific surface area, exert a decisive influence on mass transport kinetics, nucleation mechanisms, and deposition uniformity during SiH 4 deposition. These parameters not only govern the diffusion and adsorption behavior of precursors but also dictate the morphological characteristics and distribution uniformity of the Si deposited. Consequently, systematic mechanistic studies spanning from the molecular to the microscale are essential to establish quantitative relationships between porous carbon structural parameters and deposition behavior. Research indicates that porous carbon matrices featuring high specific surface area, large pore volume, and abundant micropores indeed facilitate uniform Si deposition within the pores. This is primarily attributed to their provision of increased active sites and enhanced diffusion pathways. However, it is noteworthy that parameters such as specific surface area and pore volume should not be pursued solely for maximization. Excessive porosity may compromise the structural integrity of the carbon skeleton, specifically manifested as reduced mechanical strength and diminished bulk modulus. These structural defects directly impact the cycling stability and rate capability. Therefore, practical material design necessitates seeking an optimal balance point between pore structure optimization and mechanical property retention. Furthermore, developing low-cost, high-performance porous carbon precursor material systems represents a key current research focus. Particular emphasis lies on the conversion of low-cost precursors, such as biomass-based and pitch-based materials, into porous carbon with suitable pore structures via controlled carbonization-activation protocols. This conversion process requires precise regulation of critical factors including pyrolysis temperature, activator type, and processing parameters. In practical applications, researchers must establish a multi-dimensional evaluation framework when selecting carbon matrices. This involves a holistic consideration of the interplay between raw material cost, structural parameters and electrochemical performance, aiming to achieve the optimal balance between material performance and economic viability. 2. Si Deposition. In the preparation of novel CVD Si-C composites, the Si deposition process is equally critical as carbon matrix selection. Although the fundamental mechanisms of SiH 4 deposition were systematically studied as early as the 20th century, numerous unresolved questions persist regarding the deposition mechanism of SiH 4 within the complex pore structures of porous carbon matrices. Specifically, under given temperature-pressure conditions, the diffusion kinetics of SiH 4 pyrolysis products within porous carbon, their adsorption behavior, and the interaction mechanisms with pore walls remain incompletely elucidated. Key unresolved research challenges include: (1) How the surface chemical composition, defect structure, and functional group characteristics of porous carbon influence SiH 4 diffusion and deposition behavior. (2) How to achieve selective deposition of Si within the pores while preventing excessive surface deposition. Resolving these fundamental scientific questions is essential for optimizing the microstructure and enhancing the electrochemical performance of Si-C composites. Moreover, given the extreme air sensitivity and inherent safety risks, establishing a robust safety management system for its storage and handling is a critical prerequisite for large-scale production. This necessitates implementing comprehensive safety measures at multiple levels, including precise pressure control and continuous leak monitoring devices. Only by constructing such a comprehensive safety assurance framework can the industrial implementation of the SiH 4 CVD process be reliably achieved. 3. Carbon films. Despite extensive research on carbon films for mitigating challenges in Si-C anodes, fundamental investigations into their underlying mechanisms remain insufficient. Future studies should focus on elucidating the structure-property-performance relationships of carbon films in Si-C systems. Critical parameters, including film thickness, defect density, porosity, graphitization degree, grain size, and dopant species, exert profound yet incompletely understood influences on electrochemical performance. The absence of systematic studies impedes the rational design of carbon films for optimized Si-C anode architectures. A comprehensive understanding of these correlations is imperative for determining the optimal structural characteristics of carbon films in Si-C applications. Moreover, precise control over carbon film microstructures via CVD, achieved through careful optimization of deposition time, temperature, and precursor gases, requires deeper exploration. Establishing clear processing-structure-property relationships is vital for engineering carbon films with tailored morphologies and functionalities. Future research should aim to establish clear correlations between carbon film properties and Si-C anode performance, while exploring synthetic parameters to achieve optimized carbon film designs. This will pave the way for developing more effective and powerful solutions for next-generation Si-C anode technologies. Beyond the CVD-derived Si-C composite anodes, various other factors critically determine the comprehensive properties of the materials. High-voltage fast-charging technology in high-energy-density LIBs has emerged as a pivotal solution to dramatically reduce charging times while simultaneously addressing range anxiety, establishing fast-charging as an indispensable trajectory for next-generation LIB development. Nevertheless, Si-based anodes have yet to achieve commercial adoption in fast-charging LIBs due to the intrinsically low electrical conductivity and Li + diffusion coefficient exacerbate insufficient diffusion efficiency. Recently, Choi et al. identified the state-of-charge (SOC) range of 30 to 70% is most suitable for the long-term cycling of Si anode. [111] This study underscores the critical importance of balancing volume expansion and reaction kinetics across different lithiation stages of active materials. The coordinated optimization of these enabling components proves critical for further enhancing the stability and efficiency of Si-based fast-charging LIBs. Besides, the established SEI model requires interfacial layers that simultaneously suppress parasitic reactions while enabling unhindered Li + transport. These layers form through inevitable reactions between highly reactive electrodes and strongly electrophilic electrolyte components, exacerbated by trace water and HF impurities, particularly when LiPF 6 is used as the primary lithium salt. Crucially, intrinsic surface reactions between Li-Si alloys and electrophilic alkyl carbonate solvents/salt anions often generate non-ideal passivation films. Consequently, incorporating functional additives into standard electrolyte formulations becomes imperative. Boron-based additives, by virtue of their Lewis acid nature, function as anion receptors that strongly coordinate with PF 6 - anions, thereby enhancing the dissociation of LiPF 6 . Fluorinated co-solvents offer advantages including flame-retardant capability, low viscosity, favorable low-temperature conductivity, and superior electrochemical performance, albeit at higher cost. Nitrogen-containing additives provide overcharge protection. When cost is the primary consideration, sulfur-containing additives like commercially available propylene sulfite present a more suitable option for large-scale applications. While pursuing extended cycle life for secondary lithium batteries, safety remains paramount, phosphorus-containing additives emerge as a preferred choice due to their exceptional flame retardancy and low cost, though their inherently high viscosity warrants consideration. Future research directions for liquid electrolytes encompass: (a) development of functional electrolyte additives; (b) design of flame-retardant electrolyte systems; (c) novel electrolyte formulations addressing fast-charging protection and operation across wide temperature ranges. Simultaneously, solid-state electrolytes represent a strategic direction for safer, higher-energy-density batteries. [112] Achieving commercial viability requires increased Si anode mass loading, making the study of interface evolution and nanoscale mechanical behavior in solid-state configurations an essential prerequisite for industrialization. Moreover, for Si-based composite systems, research must evolve beyond conventional coating approaches to prioritize the design of self-healing binders. These advanced binders incorporate dynamic covalent bonds or hydrogen-bonding networks to create adaptive frameworks that accommodate volumetric fluctuations during cycling. The self-healing capability enabled by robust supramolecular interactions constitutes a fundamental requirement for achieving long-term cyclability in Si anodes. While individual supramolecular anchoring points exhibit limited binding strength, branched polymeric architectures overcome this limitation through two synergistic mechanisms: (a) optimized stress distribution: branched chains dissipate external forces across multiple anchoring points; (b) enhanced chain cohesion: cooperative intrachain interactions between branched chains significantly amplify overall adhesion strength. Furthermore, to study the Si expansion and the evolution of the SEI, advanced in-situ characterization techniques, such as TEM, XRD, and Raman spectroscopy are essential. [113] Additionally, molecular dynamics simulations can clarify the mechanisms behind SEI formation, while DFT calculations can provide information on the reaction dynamics at the Si-electrolyte interface. Finite element analysis should also be applied to optimize stress distribution in the electrode structure, thereby improving mechanical stability and electrochemical performance. This comprehensive strategy, integrating material engineering, interfacial modifications, and multiscale computational modeling, will advance the development of resilient Si-based anodes for next-generation energy storage systems. In conclusion, CVD-derived Si-C anodes represent a next-generation high-energy-density LIBs technology, exhibiting outstanding electrochemical performance and promising application potential. However, to accelerate their industrialization, key challenges must be addressed: (a) long-term cycling stability, (b) high-rate charge/discharge capability, and (c) operational resilience across extreme temperatures (-30 to 60 °C). Considering the double-edged effects of Si-C material modifications: no single modification strategy can comprehensively address all key performance issues. While certain approaches, such as electrolyte additives and porous carbon materials, effectively enhance cycling stability, they may adversely affect storage performance. Therefore, combining different modification strategies can achieve a better trade-off between cycle life and calendar life, thereby optimizing overall performance. Advanced in-situ monitoring and characterization techniques, particularly non-destructive testing methods, are critically needed to elucidate the structural evolution and failure mechanisms within these internal architectures. By advancing fundamental research, particularly in elucidating degradation mechanisms under harsh conditions and developing tailored mitigation strategies, this technology is nearing commercial viability. With academia and industry working synergistically, CVD-fabricated Si-C anodes are poised to drive transformative advancements in next-generation LIBs. Acknowledgements M. F. and J. L. contributed equally to this work. This work was supported by the National Natural Science Foundation of China (No. 22209055), the China Postdoctoral Science Foundation (No. 2022M721330), the Foshan Postdoctoral Science Foundation (No. X221081MS210). Innovation Team of Universities of Guangdong Province (No. 2022KCXTD030). The “Targeted Technology Innovation Initiative” Project at the Foshan National Institute of Innovation (No. JBGS2024002). Received: (will be filled in by the editorial staff) Revised: (will be filled in by the editorial staff) Published online: (will be filled in by the editorial staff) Yong Chen is currently a professor at Hainan University and Foshan University, China. He received his PhD from the Institute of Metal Research, Chinese Academy of Sciences, China, in 2006. As the first author and corresponding author, he has published over 150 research papers in peer-reviewed journals, 3 edited books, and more than 30 China granted invention patents. 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Keywords chemical vapor deposition coulombic efficiency lithium-ion battery silicon anode volume expansion Authors Affiliations Meng Fan Foshan University View all articles by this author Jiajun Lin Foshan University View all articles by this author Zhenxing Wang 0009-0004-6008-3183 Foshan University View all articles by this author Xianyou Luo Foshan University View all articles by this author Feng Yu Foshan University View all articles by this author Yong Chen 0000-0002-0419-7504 [email protected] Foshan University View all articles by this author Metrics & Citations Metrics Article Usage 297 views 159 downloads .FvxKWukQNSOunydq8rnd { width: 100px; } Citations Download citation Meng Fan, Jiajun Lin, Zhenxing Wang, et al. Advances and perspectives of CVD-fabricated nano-scale Si-C anodes. Authorea . 14 October 2025. 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