Silicon-based Anode Research Articles

Investigating the Impact of Si/C Supraparticles Size Distribution on the Lifetime of Li-Ion Battery Half-Cells

The development of high-performance anodes for lithium-ion batteries (LiBs) with robust cycling stability has become a prominent area of research. In our recent study (Amin et al. 2023), we demonstrated that adopting a hierarchical structuring strategy via spray drying can significantly improve the cycle life of silicon-based anode materials in contrast to their nanoparticle building blocks (4 wt.% of compounding carbon). This method enhances the structural stability of the anode, thereby improving cyclic performance and paving the way for the development of high-capacity LIBs.However, beyond phenomenological proof of principles, understanding the effect of supraparticles size distribution on electrochemical performance is of great significance for making Si-based active materials ready for the LiBs industry. Therefore, we systematically investigated the correlations between supraparticle median sizes/size distributions and other supraparticle properties such as their BET surface area, slurry rheology, coated layer quality, and the electrochemical Coulombic efficiency of half-cells. These findings revealed that supraparticles with large median sizes are stable against processing as compared to small size supraparticles as can be seen from atomic force microscopic (AFM) images of coated layers in Fig 1a. It is also discovered that large supraparticles enhance the 3rd cycle Coulombic efficiency (2 formation cycles) of Li-ion half cells at 0.5 C as shown in Fig.1b. However, there exists an optimal median size/size distribution above which the Coulombic efficiency and cycling stability of the supraparticles in half-cells starts to decrease.In short, supraparticles exhibit properties (e.g., high layer stability, low surface reactions) that outperform those of individual nanoparticles. Understanding the role of supraparticle sizes in generating anodes with a hierarchical structure demonstrates great promises towards tailored materials for enhanced LiB performance. This enables us to further unravel process-structure-property relationships and understand the physics behind the improved electrochemical performance of supraparticles. Publication bibliography Amin, Adil; Loewenich, Moritz; Kilian, Stefan O.; Wassmer, Theresa; Bade, Stefan; Lyubina, Julia et al. (2023): One-Step Non-Reactive Spray Drying Approach to Produce Silicon/Carbon Composite-Based Hierarchically Structured Supraparticles for Lithium-Ion Battery Anodes. In J. Electrochem. Soc. DOI: 10.1149/1945-7111/acb66b. Figure 1

Interphase Regulation by Multifunctional Additive Empowering High Energy Lithium-Ion Batteries with Enhanced Cycle Life and Thermal Safety.

High energy density lithium-ion batteries (LIBs) adopting high-nickel layered oxide cathodes and silicon-based composite anodes always suffer from unsatisfied cycle life and poor safety performance, especially at elevated temperatures. Electrode /electrolyte interphase regulation by functional additives is one of the most economic and efficacious strategies to overcome this shortcoming. Herein, cyano-groups (-CN) are introduced into lithium fluorinated phosphate to synthesize a novel multifunctional additive of lithium tetrafluoro (1,2-dihydroxyethane-1,1,2,2-tetracarbonitrile) phosphate (LiTFTCP), which endows high nickel LiNi0.8 Co0.1 Mn0.1 O2 /SiOx -graphite composite full cell with an ultrahigh cycle life and superior safety characteristics, by adding only 0.5 wt % LiTFTCP into a LiPF6 -carbonate baseline electrolyte. It is revealed that LiTFTCP additive effectively suppresses the HF generation and facilitates the formation of a robust and heat-resistant cyano-enriched CEI layer as well as a stable LiF-enriched SEI layer. The favorable SEI/CEI layers greatly lessen the electrode degradation, electrolyte consumption, thermal-induced gassing and total heat-releasing. This work illuminates the importance of additive molecular engineering and interphase regulation in simultaneously promoting the cycling and thermal safety of LIBs with high-nickel NCMxyz cathode and silicon-based composite anode.

MXene Clay (Ti2C)-Containing In Situ Polymerized Hollow Core-Shell Binder for Silicon-Based Anodes in Lithium-Ion Batteries.

Silicon, an attractive anode material, suffers fast capacity fading due to the electrical isolation from massive volumetric expansion upon cycling. However, it holds a high theoretical capacity and low operation voltage in its practical application. In this study, a new water-based binder, MXene clay/hollow core-shell acrylate composite, was synthesized through an in situ emulsion polymerization technique to alleviate the fast capacity fading of the silicon anode efficiently. The efficient introduction of conductive MXene clay and the hollow core-shell structure, favorable to electron and ion transport in silicon-based electrodes, gives a novel conceptual design of the binder material. Such a strategy could alleviate electrical isolation after cycling and promises better electrochemical performance of the high-capacity anodes. The effect of the MXene introduction and hollow core-shell on the binder performance is thoroughly investigated using various characterization tools by comparison with no MXene-containing, core-shell acrylate, and commercial styrene-butadiene latex binders. Consequently, the silicon-based electrode containing the MXene clay/hollow core-shell acrylate binder exhibits a high capacity retention of 1351 mAh g-1 at 0.5C after 100 cycles and good rate capability of over 1100 mAh g-1 at 5C.

Dual-functional trisiloxane as binder additive for high volume expansion Li-ion battery electrodes

Silicon-based anodes for lithium-ion batteries have the inherent advantage of higher capacity. However, the inherent expansion of Si within the anodes during cycling, causing low battery life, has limited its application. Various approaches are being investigated to mitigate the adverse effects, ranging from the patterned deposition of Si, blending silicon materials with graphite active materials, and using modified polymeric binders. Inspired by the super spreading capabilities of siloxane compounds and with an aim to optimize the graphite-SiO composite electrode, this work focuses on tweaking the binder formulation with a trisiloxane-based additive which enables uniform dispersion of active material within the electrode and enhances the wetting of the electrolyte within the electrode. In this work, graphite with 15 wt% silicon monoxide was used as an electrode with trisiloxane-modified binder showing much improved electrochemical performance with better mechanical integrity compared to the benchmark electrode. The cell with modified binder exhibited remarkable cycling stability up to 400 cycles at 0.2 C-rate. A detailed study on the role of the trisiloxane additives on the physicochemical properties of electrode materials has also been elucidated. The prospects of employing these additives for similar high-volume expansion electrodes are also discussed.

Insights into mechanics and electrochemistry evolution of SiO/graphite anode by a composite electrode model

Silicon-based materials are crucial for high-capacity anodes, but their volume expansion in batteries due to the presence of silicon requires further analysis and research. Silicon monoxide/Graphite (SiO/C) is a composite material that combines the volume expansion of silicon oxide material with the practical application of carbon material. Therefore, understanding its behavior during actual use is important, particularly in full batteries and in pairs with high-capacity LiNi0.8Co0.15Al0.05O2 (NCA) cathode. There are fewer studies on this topic, which highlights the need for research. Thus, in this work, SiO/C composite negative electrodes are prepared with different compaction densities (CDs) of 1.38, 1.52, and 1.62 g cm−3. Pouch cells are assembled with NCA positive electrode to investigate the changes in battery thickness and internal resistance under different CDs and state of charge (SOC), as well as the Coulombic efficiency and cyclic performance of batteries are also examined. Additionally, the capacity-voltage curves, expansion curves under different CDs and SOC, particle stress change, and lithium concentration distribution under different CDs are comprehensively simulated. Thus, the evolution of lithium concentration distribution and electrodes volumetric strain during charge and discharge are directly presented. The established model through matching experimental data provides a research basis for predicting the performance of SiO/C negative electrodes, especially its electrochemical and mechanical performance evolution in high‑nickel full batteries. This study has important implications for the development of high-performance silicon-based anodes in practical applications.

High-Safety Lithium-Ion Batteries with Silicon-Based Anodes Enabled by Electrolyte Design.

High-energy-density lithium-ion batteries (LIBs) with high safety have long been pursued for extending the cruise range of electric vehicles. Owing to the high gravimetric capacity, silicon is a promising alternative to the convention graphite anode for high-energy LIBs. However, it suffers from intrinsic poor interfacial stability with liquid electrolytes, inevitably increasing the risk of thermal runaway and posing serious safety challenges. In this review, we will focus on mitigating thermal runaway of silicon anodes-based LIBs from the perspective of electrolyte design. First, the thermal runaway mechanism of LIBs is briefly introduced, while the specific thermal failure reactions associated with silicon anodes and electrolytes are discussed in detail. We then summarize the safety countermeasures (e. g., thermally stable solid electrolyte interphase, nonflammable electrolytes, highly stable lithium salts, mitigating electrode crosstalk, and solid-state electrolytes) enabled by customized electrolyte design to address these triggers of thermal runaway. Finally, the remaining unanswered questions regarding the thermal runaway mechanism are presented, and future directions to achieve intrinsically safe electrolytes for silicon-based anodes are prospected. This review is expected to provide insightful knowledge for improving the safety of LIBs with silicon-based anodes.

Dual immobilization of porous Si by graphene supported anatase TiO2/carbon for high-performance and safe lithium storage

Smart surface coatings have been proven to be an effective strategy to significantly enhance the electronic conductivity and cycling stability of silicon-based anode materials. However, the single/conventional coatings face critical challenges, including low initial Coulomb efficiency (ICE), poor cyclability, and kinetics failure, etc. Hence, we proposed a dual immobilization strategy to synthesize graphene supported anatase TiO2/carbon-coated porous silicon composite (denoted as PSi@TiO2@C/Graphene) using industrial-grade ferrosilicon as lithium storage raw materials through the simple etching, combined with sol–gel and hydrothermal coating processes. In this work, the dual immobilization from the “confinement effect” of the inner TiO2 shell and the “synergistic effect” of the outer carbon shell, improves the kinetics of the electrochemical reaction and ensures the integrity of the electrode material structure during lithiation. Furthermore, the introduction of the graphene substrate offers ample space for dispersing and anchoring the Si-based granules, which in turn provides a stable 3D conductive network between the particles. As a result, the PSi@TiO2@C/Graphene electrode delivers high reversible capacity of 1605.4 mAh g−1 with 93.65% retention at 0.5 A g−1 after 100 cycles (vs. 4th discharge), high initial Coulomb efficiency (82.30%), and superior cyclability of 1159.9 mAh g−1 after 250 cycles. The above results suggest that the particle structure has great potential for applications in Si-based anode and may provide some inspiration for the design of other energy storage materials.

CNTs and rGO synergistically enhance the cycling stability of yolk-shell silicon anodes for efficient lithium storage

Si-based anode materials have received a lot of attention from researchers due to their ultra-high theoretical specific capacity. However, poor conductivity and volume expansion during cycling have seriously hindered their further commercialization. To address the problems of Si-based materials, the multidimensional carbon materials constructed from Zeolitic imidazolate framework (ZIF) derived carbon and carbon nanotubes (CNTs) followed by the addition of reduced graphene oxide (rGO) are employed to encapsulate silicon nanoparticles (Si@C-ZIF@CNTs@rGO) to prepare a composite anode with a yolk-shell structure, which are prepared by mechanical stirring, electrostatic self-assembly and two-step calcination. The heat-treated ZIF materials not only form a unique yolk-shell structure that can effectively inhibit the volume expansion of silicon nanoparticles, but also derive rigid carbon shells and carbon nanotubes to improve the electrical conductivity of the anode materials, while rGO introduced by electrostatic self-assembly provides a large number of transport paths for electrons and ions. In a full battery test composed of LiFePO4 cathode, the composite cathode material loses only 2.4 % of its specific capacity after 100 cycles at 0.5 C current density. This work provides new ideas for multidimensional carbon structures to improve the lithium storage performance of silicon-based anodes.

Crystal Engineering of Silica Anode Achieving Intrinsic Zero-Strain.

Si-based anodes have large intrinsic volume expansion, which hinders their practicality and commercialization. To address this challenge, the design principle of intrinsic zero-strain anodes (① large intracrystalline cavities and ② strong bonds) is proposed, and silica with large intracrystalline cavities (SLIC) established by strong Si─O bonds ([SiO4 ] coordinate structures) is obtained and acts as an anode, achieving the intrinsic zero-strain feature first in silicon-based anodes. The phase structure of SLIC is maintained and the [SiO4 ] coordinate structure merely shows slight disorder during cycling. The feature stems from lithiation taking place by the solid-solution insertion reaction rather than the conventional conversion/alloying addition reactions, because the solid-solution insertion reaction for the SLIC has the lowest change in the Gibbs free energy. The SLIC anode demonstrates excellent cycling stability and high initial Coulombic efficiency (≈85%). Moreover, owing to the low working voltage (≈0.28V) and relatively high specific capacity, the SLIC anode presents the highest gravimetric energy density among reported zero-/quasi-zero-strain anodes and high volumetric energy density (around twice as much as graphite). The universality of the designing principle is also validated. This work provides design guidelines for zero-strain anodes in next-generation batteries.

Bi-Continuous Si/C Anode Materials Derived from Silica Aerogels for Lithium-Ion Batteries

Poor cycling performance caused by massive volume expansion of silicon (Si) has always hindered the widespread application of silicon-based anode materials. Herein, bi-continuous silicon/carbon (Si/C) anode materials are prepared via magnesiothermic reduction of silica aerogels followed by pitch impregnation and carbonization. To fabricate the expected bi-continuous structure, mesoporous silica aerogel is selected as the raw material for magnesiothermic reduction. It is successfully reduced to mesoporous Si under the protection of NaCl. The as-obtained mesoporous Si is then injected with molten pitch via vacuuming, and the pitch is subsequently converted into carbon at a high temperature. The innovative point of this strategy is the construction of a bi-continuous structure, which features both Si and carbon with a cross-linked structure, which provides an area to accommodate the colossal volume change of Si. The pitch-derived carbon facilitates fast lithium ion transfer, thereby increasing the conductivity of the Si/C anode. It can also diminish direct contact between Si and the electrolyte, minimizing side reactions between them. The obtained bi-continuous Si/C anodes exhibit excellent electrochemical performance with a high initial discharge capacity of 1481.7 mAh g−1 at a current density of 300 mA g−1 and retaining as 813.5 mAh g−1 after 200 cycles and an improved initial Coulombic efficiency of 82%. The as-prepared bi-continuous Si/C anode may have great potential applications in high-performance lithium-ion batteries.

Advancements in anode and cathode nanomaterials for high-performance Li-ion batteries

Commercially, lithium-ion batteries are the most popular batteries for electric devices, while energy density and stability have become more important for electric vehicles. Therefore, there is an increased interest in producing advanced lithium-ion batteries with a greater range of electric storage capability and improved electron transfer efficiency. Over the past few years, nanotechnology has been widely applied to enhance the physical properties of materials through the application of surface treatments or the modification of nanostructures. The significant development potential of nanotechnic applications for lithium-ion batteries is the reason for this discussion. There have been several advancements in graphene, carbon nanotubes, silicon-based and other metal-based anodes, lithium cobalt oxide, lithium iron phosphate, and nickel-based cathodes, their fabrication processes and understanding of mechanisms, as well as trends for further improvement of those previously discovered. These advancements have led to the development of batteries with greater capacity and greater performance, better stability, quicker charging times, and a longer cycle life.

Ongoing advancement in examining si-based anode materials for lithium ion batteries

There is a developing interest in Lithium-ion batteries (LIBs) with more prominent energy thickness, and further developed cycling soundness has become progressively critical because of the rising fame of electric vehicles and convenient gadgets; efficient energy storage and utilization are vital for meeting these demands. Silicon-based materials offer a promising solution with a high hypothetical explicit limit, low lithium inclusion potential, predominance, and eco-agreeableness. Silicon has emerged as a formidable contender in advanced energy storage technology. Silicon-based materials are perceived as a highly promising option for the anode material in the up-and-coming age of LIBs. Despite the potential benefits of silicon-based anode materials, some limitations currently restrict their commercial use. Its significant volume changes during Li insertion/extraction resulting poor cycling performance and rapid electrochemical decay. This article summarizes current research on this issue. It analyzes silicon anode materials from two perspectives: different dimensional silicon nanostructures (zero-, one-, two-, and three-dimensional) and silicon-based composite materials. Like Carbon/Silicon composite materials. This article provides a comprehensive understanding of silicon anode materials' research status and a vital reference for optimizing their cycling abilities and improving their commercial value and serviceable range.

Boosting the Cell Performance of the SiO/Cu and SiO/PPy Anodes via In-Situ Reduction/Oxidation Coating Strategies.

Silicon monoxide (SiO) has attracted great attention due to its high theoretical specific capacity as an alternative material for conventional graphite anode, but its poor electrical conductivity and irreversible side reactions at the SiO/electrolyte interface seriously reduce its cycling stability. Here, to overcome the drawbacks, the dicharged SiO anode coated with Cu coating layer is elaborately designed by in-situ reduction method. Compared with the pristine SiO anode of lithium-ion battery (293 mAh g-1 at 0.5 A g-1 after 200 cycles), the obtained SiO/Cu composite presents superior cycling stability (1206 mAh g-1 at 0.5 A g-1 after 200 cycles). The tight combination of Cu particles and SiO significantly improves the conductivity of the composite, effectively inhibits the side-reaction between the active material and electrolyte. In addition, polypyrrole-coated SiO composites are further prepared by in-situ oxidation method, which delivers a high reversible specific capacity of 1311 mAh g-1 at 0.5 A g-1 after 200 cycles. The in-situ coating strategies in this work provide a new pathway for the development and practical application of high-performance silicon-based anode.

3D binder-free nanoarchitecture design of porous silicon/graphene fibers for ultrastable lithium storage

Enhancing the stability and fast-charging capability of battery electrodes is of paramount importance in the field of battery technology. Silicon (Si), renowned for its high specific capacity, has emerged as a promising candidate for anodes. However, the limited structural stability and electron/ion conductivity of silicon-based anodes have raised significant concerns, including fractures and the continuous formation of unstable solid-electrolyte interphase (SEI) layers, leading to rapid capacity decay. In this study, we introduce a comprehensive approach to fabricating a binder-free and free-standing anode electrode paper using a combination technique of employing electrospinning, magnetron sputtering, and chemical vapor deposition (CVD) techniques. This developed paper electrode incorporates a 3D interconnected network of nitrogen-doped vertical graphene nanosheets (VGs) that connect porous carbon fibers (PCFs) with uniformly distributed Si nanoparticles (VGs@Si@PCFs). The as-fabricated VGs@Si@PCFs paper effectively addresses the mechanical and chemical stability issues commonly associated with Si anodes. The VGs@Si@PCFs anode demonstrates a remarkable reversible capacity of 2205 mAh g-1 at 0.1 A g-1 and exhibits exceptional cycling performance with 83.5% capacity retention at 1.0 A g-1 after 3000 cycles. This design leverages the nanoporous carbon fibers and nitrogen-doped vertical graphene nanosheets as flexible and conductive supports, enhancing the robustness and flexibility of the electrode. Additionally, mechanical modeling reveals that the overall Mises strain in the porous VGs@Si@PCFs structure is significantly lower compared to nonporous cases, potentially minimizing low-cycle fatigue. Our free-standing Si/C composite anode introduces a new class of low-strain Si-based materials, showcasing significantly improved stabilities and fast-charging capabilities.

The comparison of different deposition methods to prepare thin film of silicon-based anodes and their performances in Li-ion batteries

The comparison of different deposition methods to prepare thin film of silicon-based anodes and their performances in Li-ion batteries

The effect of Ti-based surface layer on AlSi thin film as a high-performance anode for the lithium-ion battery

Significant volume changes during cycling and the instability of the solid electrolyte interphase (SEI) are the main challenges that limit the practical application of silicon-based anodes. TiN and TiO2 were selected as surface layers and deposited on the HCl-etched AlSi (AlSi’) thin films by atomic layer deposition (ALD) to enhance the electrochemical performance of the anode. The surface layers with excellent mechanical strength can effectively suppress the volume expansion of the AlSi thin film and maintain excellent electrical contact between the film and the substrate during cycling. The effects of TiN and TiO2 surface layers on the composition and growth of the SEI layer on the AlSi’ film anode have been discussed in detail. The TiO2 surface layer was found to inhibit the continuous growth of the SEI layer and promote the formation of a mechanically robust and stable SEI layer. The AlSi’/TiO2(8 nm) anode shows a high initial discharge capacity of 2802 mA h g-1 with an initial coulomb efficiency (ICE) of 88% at 0.8 A g-1, and it maintains a capacity retention rate of 83% after 500 cycles. Moreover, the AlSi’/TiO2(8 nm) anode exhibits outstanding rate performance, as it sustains a capacity of 1710 mA h g-1 after 500 cycles at 5 A g-1, and maintains a capacity above 1032 mA h g-1 even at 30 A g-1.

Unlocking the potential of silicon anodes in lithium-ion batteries: A claw-inspired binder with synergistic interface bonding

Binders play a crucial role in enhancing the cycling stability of silicon anodes in next-generation Li-ion batteries. However, traditional linear polymer binders have difficulty withstanding the volume expansion of silicon during cycling. Herein, inspired by the fact that animals’ claws can grasp objects firmly, a claw-like taurine-grafted-poly (acrylic acid) binder (Tau-g-PAA) is designed to improve the electrochemical performance of silicon anodes. The synergistic effects of different polar groups (sulfo and carboxyl) in Tau-g-PAA facilitate the formation of multidimensional interactions with silicon nanoparticles and the diffusion of Li ions, thereby greatly improving the stability and rate performance of silicon anodes, which aligns with results from density functional theory (DFT) simulations. As expected, a Tau-g-PAA/Si electrode exhibits excellent cycling performance with a high specific capacity of 1003 ​mA ​h ​g−1 ​at 1 ​C (1 ​C ​= ​4200 ​mA ​h ​g−1) after 300 cycles, and a high rate performance. The design strategy of using polar small molecule-grafted polymers to create claw-like structures could inspire the development of better binders for silicon-based anodes.

Printable and Free-Standing Silicon-Based Anode for Current Collector-Free Lithium-Ion Batteries.

The evolution of Li-ion rechargeable batteries has driven a demand for systems exceeding the energy density and shape diversity of conventional lithium-ion batteries. Silicon (Si)-based materials, suitable for high-energy-density applications, have been restricted in practical use due to their inherent structural instability and poor conductivities upon electrochemical cycling. Here, we propose a fully printable and free-standing anode, composed of hollow SiOx/C (H-SiOx/C) composite material and an MXene conductive binder, exhibiting high specific capacity, structural reliability, and superior ionic conductivity without any current collector. The hollow structure of H-SiOx/C accommodates volume changes during cycling, while the MXene binder forms a three-dimensional interconnected conducting structure for maintaining the structural integrity of electrodes without a current collector. Furthermore, the printability and free-standing nature of the H-SiOx/C/MXene anode are validated in both coin-type full cell and heart-shaped pouch cell configurations through a straightforward stencil printing technique. This work establishes a foundation for advanced Si-based anodes, enhancing performance and design flexibility and potentially contributing to practical printable battery systems.

ZIFs derived multilayer carbon and CNT skeleton networks and graphene to encapsulate silicon nanoparticles for efficient lithium storage

The severe volume expansion and low electron mobility of silicon-based anode materials during cycling limit their further practical applications, and the use of a multilayer carbon skeleton network and graphene to encapsulate silicon nanoparticles is an effective strategy to cope with the volume expansion of silicon-alloyed anodes and to improve their electron transport. In this work, a carbon skeleton derived from dual ZIF materials was designed and the controlled growth of carbon nanotubes was achieved by changing the capping order of the ZIF materials, which effectively slowed down the capacity degradation of the battery during the cycling process. At a current density of 1 A g−1, the specific capacity of Si@D-C-ZIF@CNTs@rGO was maintained at 1498.3 mAh g−1 after 500 cycles, and the capacity was maintained at 96 % after 200 cycles of assembling Si@D-C-ZIF@CNTs@rGO as the anode into a full cell. The design of silicon-based anode materials with multi‑carbon skeletons is given a fresh concept by this work.

Nitrogen-rich carbon/SiO2 nanotubes composites prepared by self-assembly as high-performance anode lithium-ion battery

Silicon dioxide (SiO2) has huge reserves and relatively high theoretical specific capacity (1965 mAh g−1) on the earth, so it is recognized by many researchers as one of the anode materials for the next generation lithium-ion battery (LIBs). However, compared with commercial graphite materials, silicon-based anode materials are severely limited in wide application because of their poor conductivity, low lithium-ion (Li+) diffusivity and huge volume effect, which lead to obvious capacity attenuation and poor rate performance. Herein, we developed a simple method to prepare silica nanotubes (SNTs) by sol-gel method with Cetrimonium Bromide-Disodium edetate dihydrate (CTAB-EDTA) template. SNTs were modified by 3-aminopropyltriethoxysilane (APTES) to form SNTs with amino groups (SNTs-NH2). The SiO2 tubes were coated with N−doped carbon layer by self-assembly of amino carboxyl groups of tartaric acid, melamine and SNTs-NH2. The unique hollow tubular structure can maintain the stability of the structure and interface to a certain extent during the lithium/de-lithium process, thus improving the cycle stability of the electrode. In addition, N-doped carbon layer can not only improve the electron migration rate, but also contribute to the storage and transfer of Li+. Compared with the original SNTs, N−doped carbon-coated SNTs (NC@SNTs) has a reversible capacity of 972 mAh g−1 after 100 cycles at a current density of 0.1 A g−1, a cycle stability capacity of 634 mAh g−1 after 500 cycles at a current density of 1 A g−1. Therefore, the unique template and self-assembly process can prepare anode composites with excellent properties. It is of great significance to the large-scale production and commercial application of silicon−based anode LIBs in the future.