Commercial Lithium-ion Batteries Research Articles

Imaging in-operando LiCoO2 nanocrystallites with Bragg coherent X-ray diffraction

Although the LiCoO2 (LCO) cathode material has been widely used in commercial lithium ion batteries (LIB) and shows high stability, LIB’s improvements have several challenges that still need to be overcome. In this paper, we have studied the in-operando structural properties of LCO within battery cells using Bragg Coherent X-ray Diffraction Imaging to identify ways to optimise the LCO batteries’ cycling. We have successfully reconstructed the X-ray scattering phase variation (a fingerprint of atomic displacement) within a ≈ (1.6 × 1.4 × 1.3) μm3 LCO nanocrystal across a charge/discharge cycle. Reconstructions indicate strained domains forming, expanding, and fragmenting near the surface of the nanocrystal during charging, with a determined maximum relative lattice displacements of 0.467 Å. While discharging, all domains replicate in reverse the effects observed from the charging states, but with a lower maximum relative lattice displacements of 0.226 Å. These findings show the inefficiency-increasing domain dynamics within LCO lattices during cycling.

Towards smart and secure batteries: Linking pressure and temperature profiles with electrochemical behavior through hybrid optical fiber sensors

A hybrid sensing configuration combining fiber Bragg grating (FBG) with a Fabry-Perot interferometer is proposed for highly sensitive detection of pressure and temperature inside a commercial lithium-ion battery (LiB). The battery is also instrumented externally with FBGs to monitor its surface temperature variations. The LiB is operated under several cycling tests at different C-rates and environmental temperatures. High pressure and temperature resolutions of ±0.4 mbar and ±0.5 °C, respectively, are attained for the developed hybrid sensor, along with a minimum response time of 1.7 s. When the LiB is subjected to higher environmental temperatures, reduced thermal variations and higher pressure variations are registered by the optical sensor. Overall, during the cycling tests, the external temperature sensors closely follows the internal sensors behavior. Incremental capacity analysis derivative curves were systematically applied throughout the battery cycling experiments to unveil relevant insights into the interplay between pressure and temperature variations and the LiB electrochemical behavior. It was found that the pressure fluctuations present a “breathing profile” directly linked with the volume electrode lithiation and delithiation processes.

On safety of swelled commercial lithium-ion batteries: A study on aging, swelling, and abuse tests

Lithium-ion battery technology has advanced significantly, making these power sources essential for portable electronic devices such as smartphones. In 2023, global smartphone shipments reached nearly 1.2 billion units, underscoring the widespread reliance on these batteries. However, as batteries age, they may swell and potentially pose explosion risks. To investigate the safety of swollen batteries, this study conducts accelerated aging and swelling tests on lithium-ion batteries from five leading brands, which together represent over half of the global smartphone market share. The research involves a series of comprehensive tests, including Accelerated Rate Calorimeters (ARC) test, mechanical, electrical, and thermal abuse tests in accordance with Chinese national standards, as well as gas composition and theoretical flammability analyses on both new and swollen batteries. The findings indicate that swollen batteries generally exhibit safer behavior under floating charging conditions, and both new and swollen batteries pass the abuse tests within the standard framework. This study suggests that the safety of swollen lithium-ion batteries cannot be categorically labeled as dangerous or safe and should be assessed within the context of specific environments.

Irreversible failure characteristics and microscopic mechanism of lithium-ion battery under high dynamic strong mechanical impacts

Lithium-ion battery is the most widely used battery currently, and its reliability and failure under various extreme working environments are therefore widely concerned. Among them, failures resulting from highly dynamic mechanical impacts are the most threatening and less covered by previous research. In this paper, with a specialized Machette hammer impact test system, the irreversible capacity loss of commercial cylindrical jelly-roll lithium-ion batteries under high dynamic mechanical impact was investigated, the influences of impact strength, impact number, and working temperature are also considered. Through microscopic characterization and finite element simulation, the failure mechanisms of anode, cathode, and separator are revealed, and their respective contributions to battery capacity loss are quantitatively analyzed. All these findings provide a theoretical basis for the redundancy design of batteries for missile electro-mechanical systems and other equipment which are subjected to high dynamic mechanical impact conditions.

Sustainable full-cell NCM||Graphite system with superior stability: The hybrid impact of sulfone-containing and flame-retardant additives on interface formation and cyclability

S-containing additives improve the performance, lifetime, and sustainability of lithium-ion batteries (LIBs) through the stabilization of electrode-electrolyte interfaces, modification of electrolyte properties, and facilitating the efficient resource utilization and rapid Li+ migration. Non-etheless, fire safety, extended shelf life, and capacity maintenance are critical concerns for commercial LIBs. Herein, a S-containing film-forming additive, including 4,4-diaminodiphenylsolfon (DADP) by incorporating flame retardancy of dimethyl methyl phosphonate (DMMP) was considered toward taking the barriers of above-mentioned challenges. Based on the calculation, the additives decompose sequentially to produce a distinct SEI via a narrower energy gap under both cathodic and anodic conditions. The NCM532||Graphite with DADP/DMMP showed the enhanced preservation and stability of structure, defined by XRD, Rietveld refinement pattern, SEM, and FT-IR. While the DMMP decreased the fire risk and lowered the capacity due to side reactions, the DADP improved the capacity loss, where the retention rate was 94.91%, 92.01%, 81.29%, and 76.22% within 100, 200, 300, and 400 cycles, respectively. The additive also maintained a capacity of 1123.115 mAhg−1 for 650 cycles, demonstrating excellent cyclability. Therefore, DADP/DMMP facilitate the formation of stable SEI layer, reduce fire risk, improve cycle stability, and offer an achievable path to develop the safe and long-lasting commercial batteries.

Accelerated commercial battery electrode-level degradation diagnosis via only 11-point charging segments

Accelerated and accurate degradation diagnosis is imperative for the management and reutilization of commercial lithium-ion batteries in the upcoming TWh era. This work proposes a framework combining both deep learning and physical modeling to extend traditional capacity degradation diagnosis to a rapid and accurate degradation diagnosis at the electrode level using only readily measurable charging current and voltage signals. Deep learning is used to rapidly and robustly predict polarization-free incremental capacity analysis (ICA) curves in minutes, which are traditionally obtained in a dozen hours, and the physical model is to quantitatively reveal the electrode-level degradation modes by decoupling them from the ICA curves. It is demonstrated that 11 points collected at any starting state-of-charge (SOC) in a minimum of 2.5 minutes are sufficient to predict reliable ICA curves with a mean root mean square error (RMSE) of 0.2774 Ah/V. Accordingly, batteries can be accurately elevated based on their degradation at both macro and electrode levels. Through transfer learning, such a method can also be adapted to different battery chemistries, emphasizing the enticing potential for rapid promotion of this work in battery degradation diagnosis.

Synchronously Stabilizing the Interphase of Cathode and Anode Enabling Lithium Metal Batteries via Multiple Electrolyte Additives

As the most promising high energy density technology, lithium metal batteries are associated with serious interfacial challenges because the electrolytes employed are unable to meet the requirements of both electrodes simultaneously, namely, the systems that work for Li metal are highly likely to be unsuitable for the cathode, and vice versa. In this study, we investigate the synergistic effects of lithium bis (oxalate) borate (LiBOB), fluoroethylene carbonate (FEC) and adiponitrile (ADN) to develop a formula that is compatible with both elements in the battery. The solid–electrolyte interphase (SEI) multi-layer generated from LiBOB and FEC successfully protects the electrolyte from the lithium and suppresses the decomposition of ADN on lithium, identified by the tiny amounts of isonitriles on the surface of the anode. Simultaneously, most of the ADN molecules remain and protect the cathode particles via the absorption layer of the nitrile groups, in the same way that this process works in commercial lithium-ion batteries. Benefiting from the stable interfacial films formed synchronously on the anode and cathode, the Li/LiNi0.8Co0.1Mn0.1O2 cells with an area capacity of ~3 mAh cm−2 operate stably beyond 250 cycles and target the accumulated capacity to levels as high as ~653.4 mAh cm−2. Our approach demonstrates that electrolyte engineering with known additives is a practical strategy for addressing the challenges of lithium batteries.

A Novel Structured Si‐Based Composite with 2D Structured Graphite for High‐Performance Lithium‐Ion Batteries

AbstractSilicon is a promising alternative to graphite anodes for achieving high‐energy‐density in lithium‐ion batteries (LIBs) because of its high theoretical capacity (3579 mAh g−1). However, silicon anode must be developed to address its disadvantages, such as volume expansion and low electronic conductivity. Therefore, the use of silicon as composed with graphite and carbon anode materials is investigated, which requires properties such as a spherical morphology for high density and encapsulation of silicon particles in the composite. Herein, a graphite@silicon@carbon (Gr@Si@C) micro‐sized spherical anode composite is synthesized by mechanofusion process. This composite comprises an outer surface, middle layer, and core pore, which are formed by the capillary force arising from 2D structured graphite and pitch properties. This structure effectively addresses the intrinsic issues associated with Si. Gr@Si@C exhibits a high capacity of 1622 mAh g−1 and capacity retention of 72.2% after 100 cycles, with a high areal capacity 4.2 mAh cm−2. When Gr@Si@C is blended with commercial graphite, the composite exhibits high capacity retention and average Coulombic efficiency after cycling. The Gr@Si@C blended electrode exhibits a high energy density of 820 Wh L−1 with ≈16% metallic Si in the electrode (40 wt.% composite), enabling the realization of practical commercial LIBs.

Deep learning from three-dimensional lithium-ion battery multiphysics model part I: Data development

Fast growing demands for electric vehicles require better longevity, safety and reliability for next-generation high-energy battery technologies. A data-centered battery management system is thus desired to interpret complex battery data and make decisions for properly managing multi-physics battery dynamics. Nowadays, Battery informatics are emerging as promising solutions by leveraging advanced machine learning tools to deliver accurate prediction of battery performance, health and safety, but is hurdled by a scarcity of data. To mitigate this issue, this study presents one of the first studies for data development through both experimental studies and three-dimensional (3-D) multi-physics modeling to underpin a deep learning framework with in-depth examination for battery performance and thermal risk prediction. Specifically, Part I focused on the development of the battery model which was thoroughly validated and analyzed to guarantee the model accuracy by two steps: firstly, we validated the multi-physics model against two commercial Lithium-ion batteries, i.e., Panasonic NCR18650B and 18650BD; Then, the coupling between thermal and electrochemical battery behaviors were analyzed deeply to demonstrate insights obtained from the model, such as voltage evolution and maximum local temperature (hot spot). The developed model proves to be capable of providing insightful and reliable data for the training of convolutional neural network and long short-term memory (CNN-LSTM) in part II.

Roll-to-roll fabrication and characterization of ultra-thin ceramic-coated separator for high-energy-density lithium-ion batteries

Ceramic-coated separators (CCSs) used in lithium-ion batteries (LIBs) play an important role in ensuring the safety of LIBs. However, conventional CCSs fabricated by coating the slurry consisting of ceramic particles and binder have limitations due to the micrometer-thick ceramic coating layer (CCL), compromising the energy density and power capabilities of LIBs. To address this relationship, ultra-thin CCSs fabricated by the sputtering process have attracted attention due to their high thermal stability even with nanometer-thick CCL. Nevertheless, batch-type sputtering machines cannot provide roll-based CCSs for commercial LIBs. Herein, we demonstrate the continuous fabrication of ultra-thin CCS rolls with a pilot-scale direct current (DC) roll-to-roll sputtering process. The ionic conductance and thermal stability are compared with the slurry-based CCS by controlling the coating thickness through the line speed. In addition, the electrochemical performance of the pouch cell (LiNi0.6Co0.2Mn0.2O2/graphite, 550 mAh) is evaluated to confirm the applicability of the roll-to-roll sputtered ultra-thin, binder-free CCS (R2R-UB-CCS) to LIBs. Owing to the nanometer-thick CCL, the pouch cell with the R2R-UB-CCS shows higher power capabilities than the bare polyethylene (PE) separator and slurry-based CCS. Thus, the roll-to-roll sputtering process for large-scale, high-speed mass production of ultra-thin CCS has the potential for high safety and high-energy-density LIBs.

Sustainable Fabrication of Graphene Oxide Cathodes from Graphite of Failed Commercial Li-Ion Batteries for High-Performance Aqueous Zn-Ion Batteries.

The need for revamping spent graphite (SG) from battery waste of commercial lithium-ion batteries and employing it as a source for the synthesis of graphene oxide (GO) is focused. Thus, this work emphasizes the study of GO sheets, synthesized via modified Hummer's method from spent graphite (SG-GO) as cathodes for an aqueous zinc ion battery (AZIB) system, for the first time in literature. For comparison, graphene oxide is also synthesized using commercial graphite powder, its structural and morphological properties are analyzed with SG-GO. The coin cell AZIB device is fabricated for both the GOs and the electrochemical performances revealed that SG-GO portrayed an enhanced charge capacity of 270 mAh g-1 at 0.1 A g-1 in 3m ZnSO4 in comparison to GO which delivered ≈198 mAh g-1 at the same current density of 0.1 A g-1. The long-run cycling analysis of SG-GO elucidated the capacity retention of 77.3% at 1 A g-1 even after 1000 cycles. Moreover, the performance of SG-GO is inspected in different electrolyte systems and the suitable electrolyte underwent concentration variation studies to figure out the capability of the system in storing Zn2+ ions which is found to be more in 3M ZnSO4 electrolyte.

A Review of Carbon Anode Materials for Sodium-Ion Batteries: Key Materials, Sodium-Storage Mechanisms, Applications, and Large-Scale Design Principles.

Sodium-ion batteries (SIBs) have been proposed as a potential substitute for commercial lithium-ion batteries due to their excellent storage performance and cost-effectiveness. However, due to the substantial radius of sodium ions, there is an urgent need to develop anode materials with exemplary electrochemical characteristics, thereby enabling the fabrication of sodium-ion batteries with high energy density and rapid dynamics. Carbon materials are highly valued in the energy-storage field due to their diverse structures, low cost, and high reliability. This review comprehensively summarizes the typical structure; energy-storage mechanisms; and current development status of various carbon-based anode materials for SIBs, such as hard carbon, soft carbon, graphite, graphene, carbon nanotubes (CNTs), and porous carbon materials. This review also provides an overview of the current status and future development of related companies for sodium-ion batteries. Furthermore, it offers a summary and outlook on the challenges and opportunities associated with the design principles and large-scale production of carbon materials with high-energy-density requirements. This review offers an avenue for exploring outstanding improvement strategies for carbon materials, which can provide guidance for future application and research.

The high-rate cycling stability of the LiFe0.6Mn0.4PO4/C cathode material is enhanced through in-situ Nb-doping

LiFe0.6Mn0.4PO4/C, due to its low cost and safety advantages, is gradually becoming a safe and reliable commercial lithium battery storage material. However, its lower capacity at high rates and poor cycle performance limit its further industrial application. To address this, this work used a one-step solvothermal method to prepare Li(Fe0.6Mn0.4)1‑xNbxPO4 (x = 0, 0.01, 0.02, 0.03) cathode materials to improve electrochemical performance. Characterization of the samples indicates that Nb doping promoted the growth of the material's [001] crystal orientation, thus enhancing the lithium ion diffusion rate, effectively reducing electrode polarization and charge transfer resistance, which helps to explain its excellent rate performance. More importantly, Nb doping increases the M-O bond energy, making the LMFP/C metal-oxygen framework more stable, and enhancing the stability of the crystal structure of lithium ions intercalating and deintercalating during cycling. The electrochemical test results further indicate that the LFMP/CNb0.02 cathode exhibits excellent electrochemical performance. It has remarkable capacities of 156.9 mAh·g‑1 at 0.2 C and 135.9 mAh·g‑1 at 1 C, particularly showing an initial discharge specific capacity of 121.4 mAh·g‑1 at a high rate of 5 C. After 500 cycles, it still maintains a capacity of 114.3 mAh·g‑1, with a capacity retention rate of 94.15 %, significantly outperforming the original LMFP/C (initial discharge specific capacity of 109.8 mAh·g‑1) which only retains 61.47 % of its capacity after 300 cycles.

Development of Solid-State Lithium-Ion Batteries (LIBs) to Increase Ionic Conductivity through Interactions between Solid Electrolytes and Anode and Cathode Electrodes

Although in general ions are not able to migrate in the solid-state position due to rigid skeletal structure, in some solid electrolytes with a low energy barrier and high ionic conductivities, these ion transition can occur. In this work, we considered several solid electrolytes including lithium phosphorus oxy-nitride (LIPON), a lithium super-ionic conductor (SILICON), and thio-LISICON. For the fabrication and characterization of the solid electrolyte’s fabrication, we used a single-step ball milling (SSBM) procedure. Through this research on all-solid-state rechargeable lithium-ion batteries, our target is to discuss solving several problems in solid LIBs that have recently escalated due to raised concerns relating to safety hazards such as solvent leakage and the flammability of the liquid electrolytes used for commercial LIBs. Through this research, we tested the conductivity amounts of various substrates containing amorphous glass, SSBM, and glass-ceramic samples. Obviously, the SSBM glass-ceramics increased the conductivity, and we also found that the values for conductivity attained by SSBM were higher than those values for glass-ceramics. Using an SSBM technique, silicon nanoparticles were used as an anode material and it was found that the charge and discharge curves in the battery cell cycled between 0.009 and 1.45 V versus Li+/Li at a current density of 210 mA g−1 at room temperature. Since high resistance causes degradation between the cathode material (LiCoO2) and the solid electrolyte, we added GeS2 and SiS2 to the Li2S-P2S5 system to obtain higher conductivities and better stability of the electrode–electrolyte interface.

A Review of Electrospun Carbon-Based Nanofibers Materials used in Lithium-Sulfur Batteries.

Commercial lithium-ion batteries are gradually approaching their theoretical specific energy, which cannot meet the fast-growing energy storage demands. Lithium-sulfur (Li-S) batteries are anticipated to supersede lithium-ion batteries as the next-generation energy storage system owing to their high atheoretical specific capacity (1675 mAh g-1) and energy density (2600 Wh kg-1). Nonetheless, Li-S batteries encounter several challenges, including the inadequate conductivity of sulfur and lithium sulfide, sulfur's volume expansion, and the shuttle effect of lithium polysulfides, all of which significantly impact the practical utilization of Li-S batteries. Electrospun carbon-based nanofibers can simultaneously resolve these issues with their economical preparation, distinctive nanostructure, and exceptional flexibility. This review presents the most recent research findings on electrospun carbon-based nanofibers materials serving as sulfur hosts and interlayer components in Li-S batteries. We analyzed the impact of the material's structural design on the performance of Li-S batteries and the relative underlying mechanism. Finally, the current challenges and issues faced by carbon-based nanofibers composites in the application of Li-S batteries are summarized, and the future development trajectory are outlined.

Unveiling the Interplay Between Silicon and Graphite in Composite Anodes for Lithium-Ion Batteries.

Si provides an effective approach to achieving high-energy batteries owing to its high energy density and abundance. However, the poor stability of Si requires buffering with graphite particles when used as anodes. Currently, commercial lithium-ion batteries with Si/graphite composite anodes can provide a high energy density and are expected to replace traditional graphite-based batteries. The different lithium storage properties of Si and graphite lead to different degrees of lithiation and chemical environments for this composite anode, which significantly affects the performance of batteries. Herein, the interplay between Si and graphite in mechanically mixed Si/graphite composite anodes is emphasized, which alters the lithiation sequence of the active materials and thus the cycling performance of the battery. Furthermore, performance optimization can be achieved by changing the intrinsic properties of the active materials and external operating conditions, which are summarized and explained in detail. The investigation of the interplay based on Si/graphite composite anodes lays the foundation for developing long-life and high-energy batteries. The abovementioned experimental methods provide logical guidance for future research on composite electrodes with multiple active materials.

Effects of liquid-phase carbon combining surfactant coatings on the performance of LiMn0.2Fe0.8PO4 cathode materials

Efforts to reduce the particle size of LiFexMn1-xPO4 materials and apply conductive carbon coatings have yielded substantial benefits in terms of obtaining lithium-ion batteries (LIBs) with enhanced electrochemical performance. However, LiFexMn1-xPO4 materials with small particle sizes and uniform carbon layers cannot be obtained by the conventional high-temperature solid-phase method, which is the most convenient and applicable method for the industrial-scale preparation of the cathode materials used in commercial LIBs. The present work addresses this issue by applying the cationic surfactant cetyltrimethylammonium bromide (CTAB) in conjunction with LiMn0.2Fe0.8PO4 (LMFP) particles, and obtaining a carbon layer by replacing the conventional in-situ solid-phase carbon coating process with a secondary liquid-phase coating process using sucrose as the carbon source. The CTAB surfactant is observed to be uniformly adsorbed on the surface of LMFP particles, and maintains small LMFP particle sizes by operating as a dispersant preventing their agglomeration. Additionally, the carbon network formed by CTAB pyrolysis acts as an intermediate medium ensuring that the conductive carbon layer is uniformly and firmly adhered to the LMFP particle surfaces at a high preparation temperature of 680°C. This composite carbon layer is demonstrated to enhance lithium-ion transport, while concurrently acting as a barrier interfering with manganese diffusion within the electrolyte during charge-discharge cycling. As a result, the optimal LMFP-based cathode material achieves reversible specific capacities of 160 mAh g−1 and 120 mAh g−1 at charge-discharge rates of 0.1 C and 5 C, respectively, and the capacity retention is 88 % after 500 cycles at 1 C. Hence, the results verify that the proposed surfactant-mediated liquid-phase carbon coating process is an effective method for enhancing the overall electrochemical performance of LMFP-based cathode materials.

Highly hygroscopic needle-punched carbon fiber felt with high evaporative cooling efficiency and fire resistance for safe operation of ultrahigh-rate lithium-ion batteries

The effective thermal management of lithium-ion batteries is the key to ensuring their fast charging-discharging, safe and efficient operation. Herein, inspired by transpiration-driven water transport in plants, we report a highly hygroscopic needle-punched carbon fiber felt (HS/CFF) with high evaporative cooling efficiency and fire resistance for the safe operation of lithium-ion batteries working at ultrahigh-rate conditions. The three-dimensional fiber skeleton structure constructed by needle punching in the carbon fiber felt enables effective water transport and storage in HS/CFF, without any water leakage. At an ultra-high discharge rate of 10 C, HS/CFF can reduce the maximum temperature of commercial lithium-ion batteries by 18 °C, and can keep the battery temperature below 60 °C. During 500 cycles of charge-discharge, HS/CFF maintains stable evaporative heat dissipation performance, which helps to improve the safety of lithium-ion batteries and extend their service life. Moreover, HS/CFF remains non-combustible even under exposure to a flame (600-700 °C) for 10 min, and the HS/CFF can be reused after the burning test, with the original excellent heat dissipation effect unchanged. This flexible, fire-resistant cooling material offers a promising avenue for low-energy intelligent thermal management of lithium-ion batteries and other heat-generating electronic devices.

Surface engineering of TiSiO4 nano-coating for high-voltage nickel-rich ternary cathodes: An approach to improve cyclic performance

In recent years, layered ternary transition metal oxides with a high nickel content have gained substantial attention as a potential positive electrode material for lithium-ion batteries. However, its poor rate capability, cyclability, and capacity retention at high working voltages limit its use in commercial lithium-ion batteries. To overcome these challenges, we synthesize a cost-effective wet-chemical deposition of novel TiSiO4 nano-coatings over the surface of LiNi0.83Mn0.06Co0.11O2 (NMC-83). X-ray diffraction and electron microscopy confirm the presence of a coating and verify that the deposition process did not alter the crystallinity and morphology of the NMC-83 particles. In addition, during cycling, it completely protects NMC-83 with enhancements in hexagonal phase transitions between H2 and H3, resulting in excellent cycling stability at upper cut-off voltages. Likewise, when the amount of coated material is equal to 1 wt%, it provides faster ion kinetics and a stable electrode-electrolyte interface. The 1 wt% TiSiO4 coating provides 35 % retention after 250 cycles at a 0.5C rate, while the pristine NMC-83 shows only 13.7 %. From postmortem analysis, the 1 wt% TiSiO4-coated NMC-83 cathode maintains its stable polycrystalline nature compared with pristine NMC-83. Thus, this novel TiSiO4 nanocoating has significant implications for developing high-performance rechargeable batteries for energy applications.

Si/Graphite@C Composite Fabricated by Electrostatic Self-Assembly and Following Thermal Treatment as an Anode Material for Lithium-Ion Battery.

Commercial graphite anode has advantages such as low potential platform, high electronic conductivity, and abundant reserves. However, its theoretical capacity is only 372 mA h g-1. High-energy lithium-ion batteries have been a research hotspot. The Si anode has an extremely high specific capacity, but its application is hindered by defects such as large volume changes, poor electronic conductivity, and a small lithium-ion diffusion coefficient. Here, the Si/thermally reduced graphite oxide@carbon (Si/RGtO@C) composite was fabricated by electrostatic self-assembly followed by thermal treatment. The RGtO synergistic carbon coating layer can effectively compensate for the low electronic conductivity and buffer the volume expansion effect of the Si nanoparticles during charge/discharge cycles. The Si/RGtO@C anode demonstrated a significantly increased capacity compared to the RGtO. After 300 cycles, Si/RGtO@C kept a discharged capacity of 367.6 mA h g-1 at a high current density of 1.0 A g-1. The Si/RGtO@C anode shows an application potential for commercial high-energy lithium-ion batteries.