Anode Material For Lithium-ion Batteries Research Articles

One-pot synthesis of interconnected carbon-coated silicon nanosheets from clay minerals for high-performance lithium-ion battery anodes

The silicon nanosheet/carbon composite emerges as a promising anode material for the next-generation commercial lithium-ion batteries. However, complex, costly, and energy-intensive synthesis procedures impede its practical application. Herein, the carbon-coated silicon nanosheets (Si/C) have been successfully synthesized via a one-pot strategy, involving a modified magnesiothermic reduction of talc followed by a reaction with CO2. The distinct chemical composition and layered nanostructure of talc enable the retention of Si nanosheets during exothermic reactions without additional templates or heat absorbents. The method shows significant potential for the scalable production of Si/C owing to the abundant silicon source, sustainable carbon source, and straightforward protocol. The resulting Si/C displays a hierarchical porous structure, with both macropores and mesopores, and an interconnected network of carbon-coated Si nanosheets. These structural characteristics facilitate rapid Li+ diffusion and enable the material to accommodate the lithiation-induced mechanical strains. As a result, the Si/C electrode exhibits outstanding electrochemical performance, including a remarkable rate capability (with a specific capacity of 1220 mAh g−1 at 10.0 A g−1) and a high initial Coulombic efficiency of 88%. The work opens a new avenue for the development of Si/C composites from natural clay minerals through an economical and scalable strategy, which would contribute to the practical application of advanced Si-based anodes in lithium-ion batteries.

Double-layered SnO2@NC hollow spheres as anode materials for high-performance lithium-ion batteries

Double-layered SnO2@NC hollow spheres as anode materials for high-performance lithium-ion batteries

Influence of defects on enhancing lithium diffusivity in crystalline silicon anodes for fast charging lithium-ion batteries

The energy storage sector requires high capacity, long cycling life batteries. Silicon (Si) arises as a pivotal anode material for next-generation lithium-ion batteries owing to its exceptional capacity. However, challenges arise from lithium interactions, causing volumetric expansion and structural concerns like cracking. Si anodes also exhibit diverse phenomena during lithiation, influenced by crystal orientations. A thorough comprehension of the (de)lithiation process is essential to address challenges, despite existing gaps in knowledge, with strategic design and complementary materials, offering potential solutions by enhancing ion mobility and minimizing diffusion barriers. Here we have developed and applied first-principles simulations to offer fundamental insights into atomic interactions, providing a realistic atomistic representation of lithiation processes. Our simulations systematically incorporate Li+ into Si and Si- nitrogen vacancies (NV) orientations, and evaluation between Si and Si-NV (110) indicates a more favorable behavior in ionic diffusion for Si-NV(110), with a range of 2.55 × 10−3 to 1.64 × 10−2 (cm2/s) and a 15 % decrease in volume expansion. Our results explain the ternary Si–Li–N electrode materials and the identification of optimal site disorders to maximize the rate of Li+ diffusion in crystalline Si anodes.

In situ Preparation of SiOx/Carbon Nanotube Composite Films with Excellent Mechanical and Electrochemical Properties as an Anode Material for Lithium‐Ion Batteries

Silicon monoxide (SiOx) has become one of the most promising anode materials for next‐generation lithium‐ion batteries (LIBs) due to its high theoretical capacity. However, the inherent low electrical conductivity and large volume change during lithiation/delithiation processes hinder its practical applications. Here, a novel and facile strategy is designed to prepare SiOx/carbon nanotube (CNT) composite films in one step by using a method involving floating catalytic chemical vapor deposition (FCCVD). That is, SiOx particles and CNTs form at high temperature and winded directly on a drum to give rise to a film in an open air environment. The composite film is made up of a 3D CNT network with SiOx particles uniformly embedded. The as‐prepared composite film not only has a tensile strength of 78 MPa and elongation at break of 52%, but also exhibits a high specific capacity of 966.4 mA h g−1 after 120 cycles at the current density of 0.1 A g−1 and a good rate capacity of 448.7 mA h g−1 at the current density of 2 A g−1 when used as an anode material for LIBs. The results from the in‐situ preparation and resultant composite suggest a new route for developing high‐performance anode materials for LIBs.

Boron-doped polyhedral graphite catalyzed by h-BN via structural induction for lithium storage

Artificial graphite is extensively used in power lithium-ion batteries for its exceptional stability and high-rate performance. However, the commercial high-temperature graphitization process is conducted at temperatures up to 3000 °C to enhance the degree of graphitization, resulting in significant electricity consumption and lengthy production cycles. This study aimed to lower graphitization temperatures and shorten times by using h-BN as a catalyst. Employing anthracite coal as the precursor and catalyzing with BN at 2800 °C for just 2 h, we achieved a remarkable graphitization degree of 93.3 %, compared to 83.5 % without BN. This indicates BN's effectiveness in accelerating graphite phase formation. Interestingly, the resultant graphite exhibited polyhedral morphology and incorporated boron doping. As edges increased, lithium-ion diffusion pathways and boron doping enhanced stability within the graphite layers, imparting high rate capability and robust cycle performance. The material delivered reversible specific capacities of 369.6 and 226 mA h g−1 at current densities of 0.1 and 3C, and maintained capacity retentions of 95 % and 92 % after 500 cycles at 0.5C and 1C. These results substantiate the potential for large-scale production of artificial graphite from anthracite coal using BN catalysis and underscore its promise as a superior anode material for lithium-ion batteries.

High content pyridine nitrogen-doped carbon nanosheets derived from ZIF-L as anode materials of lithium-ion batteries with excellent capacity and rate performance

The precise control of nitrogen doping types in carbon materials is crucial for optimizing energy storage devices. In this study, we synthesize nitrogen-doped carbon nanosheets (NCS) using ZIF-L as a precursor. Comparatively, the two-dimensional crystal structure of ZIF-L provides several advantages over ZIF-8 as a precursor in terms of nitrogen doping efficiency, achieving a higher doping level (14.56 %) and an increased ratio of pyridinic nitrogen (53.60 %). Consequently, NCS display a greater capacity for pseudocapacitive lithium storage. Furthermore, by adjusting the carbonization temperature, we precisely tailor the graphite-nitrogen doping level of NCS within the range of 16.80–31.22 %. Remarkably, when employed as an anode material in lithium-ion batteries, NCS-800 demonstrates exceptional cycling stability, with a capacity retention of 1078 mAh g−1 after 500 cycles at a current density of 0.5 A g−1, as well as excellent rate capability (735 mAh g−1 at 5 A g−1). This study not only compares the impact of precursor crystal structure modifications on nitrogen doping and lithium storage performance but also introduces a novel synthesis methodology for highly nitrogen-doped carbon materials, offering new avenues for future research in this field.

Biochar-Derived Anode Materials for Lithium-Ion Batteries: A Review

Highly portable nanoelectronics and large-scale electronics rely on lithium-ion batteries (LIBs) as the most reliable energy storage technology. This method is thought to be both environmentally friendly and cost-effective. We provide a study of a low-cost, abundant, and renewable supply of carbon-based biomass with potential uses in LIBs. Renewable feedstocks have received significant attention in recent decades as promising tools for efficient and alternative anode materials for LIBs. Researchers can synthesise carbon-rich biochar through the pyrolytic process of biomass. Depending on the synthetic process, precise surface chemistry, and textural qualities such as specific surface area and porosity, this material can be customised to favour application-specific properties with a preferred application. In this research, we look at the performance of biochar in LIBs, its properties, and the biomass supply, and we discuss the prospects for these biomass-derived materials in energy storage devices.

Facile fabrication of mesoporous SnO2@N-rGO nanocomposites by electrostatic self-assembly as anode for high performance lithium-ion batteries

Tin dioxide (SnO2) have been considered to be a promising anode material for high performance lithium-ion batteries (LIBs) due to its high lithium storage capacity of as high as 1494 mAh g−1, which has been impeded greatly due to its large volumetric expansion and low conductivity. Thus, the simple but effective approach for the fabrication of SnO2-based material is ever-urgent. To this end, the mesoporous SnO2@N-rGO nanocomposites were designed and fabricated by a simple and scalable electrostatic self-assembly method and investigated electrochemically as anode for LIBs. The results show that the as-obtained mesoporous SnO2@N-rGO nanocomposites exhibit an excellent cycling stability and outstanding rate capability after an initial activation due to the formation of SEI layer on the surface, which are mainly ascribed to the synergistic effect of nano-SnO2, high conductive N-doped rGO matrix network and rich mesopores. Therefore, this work offers an ingenious strategy to design and fabricate the SnO2-based anode material for high performance lithium-ion batteries.

Metal sulfide-decorated lamellar porous carbon framework hybrids for fast lithium storage with high volumetric capacity

Porous carbon nanosheets have shown great potential in electrochemical energy storage devices, yet their intrinsic limited volumetric capacity and energy density remain a great concern. Herein, lamellar porous carbon framework hybrids (LPCFHs) have been facilely developed by thermal-induced bulk self-assembly of block copolymers with precisely controllable molecular structure, followed by stepwise chemical crosslinking and morphology-persistent carbonization processes. The as-obtained LPCFHs consist of densely covalent connected alternate layers (porous carbon nanosheets and porous carbon spacers) and homogenously dispersed metal sulfide nanoparticles. The ordered compact stacking structure of carbon nanosheets endows LPCFHs with a high tap density and fast electron transfer both in lateral and vertical dimension, while the porous carbon spacers enable fast channels for ion transfer. Moreover, the metal sulfide nanoparticles strongly interacted with carbon nanosheets are homogenously distributed in LPCFHs, resulting in sufficient active sites. As a result, when used as anode materials in lithium-ion batteries (LIBs), tin sulfide-decorated LPCFHs (LPCFHs-SnS) deliver a volumetric capacity of up to 1285 mAh cm−3; meanwhile, high-rate capability (488 mAh g−1 at 5 A g−1) and excellent cycling stability (capacity retention of 88.3 % after 500 cycles at 1 A g−1) are also achieved, demonstrating great potential for practical application in LIBs.

Dual regulation of particle size and surface structure of SrVO3 for high volumetric capacity

Perovskite SrVO3 stands out as a promising anode material for lithium-ion batteries due to its inherent redox activity, excellent electrical conductivity, and structural adaptability. Despite these advantages, challenges persist, such as in achieving high tap density and volumetric specific capacity. In this study, we overcome these challenges by finely regulating particle size and constructing a tailored surface structure for SrVO3. The implementation of ball milling during the synthesis process proves to be a simple yet highly efficient method for simultaneously tailoring particle size and in-situ creating an amorphous layer on SrVO3 particles. The reduction in particle size not only facilitates enhanced electron and ion transport but also significantly improves the tap density of SrVO3, increasing it from 2.61 to 3.15 g cm−3. The in-situ construction of an amorphous layer introduces a multitude of defects and high valence V5+. These defects serve as active sites for lithium ions, while the V5+ species contribute to increased electron transfer, collectively resulting in a high gravimetric specific capacity. The engineered SrVO3 anode delivers an impressive volumetric capacity of 1134 mAh cm−3 at 0.1 A g−1, surpassing both pristine SrVO3 (733 mAh cm−3) and commercial graphite anode (∼460 mAh cm−3).

Advanced Micro/Nanostructure Silicon-Based Anode Materials for High-Energy Lithium-Ion Batteries: From Liquid- to Solid-State Batteries

Advanced Micro/Nanostructure Silicon-Based Anode Materials for High-Energy Lithium-Ion Batteries: From Liquid- to Solid-State Batteries

Mechanistic analysis of Co2VO4/X (X = Ni, C) heterostructures as anode materials of lithium-ion batteries

Mechanistic analysis of Co2VO4/X (X = Ni, C) heterostructures as anode materials of lithium-ion batteries

Synthesis and Characterization of MnIn2S4/Single-Walled Carbon Nanotube Composites as an Anode Material for Lithium-Ion Batteries.

In this study, we synthesized a transition metal sulfide (TMS) with a spinel structure, i.e., MnIn2S4 (MIS), using a two-step hydrothermal and sintering process. In the context of lithium-ion battery (LIB) applications, ternary TMSs are being considered as interesting options for anode materials. This consideration arises from their notable attributes, including high theoretical capacity, excellent cycle stability, and cost-effectiveness. However, dramatic volume changes result in the electrochemical performance being severely limited, so we introduced single-walled carbon nanotubes (SWCNTs) and prepared an MIS/SWCNT composite to enhance the structural stability and electronic conductivity. The synthesized MIS/SWCNT composite exhibits better cycle performance than bare MIS. Undergoing 100 cycles, MIS only yields a reversible capacity of 117 mAh/g at 0.1 A/g. However, the MIS/SWCNT composite exhibits a reversible capacity as high as 536 mAh/g after 100 cycles. Moreover, the MIS/SWCNT composite shows a better rate capability. The current density increases with cycling, and the SWCNT composite exhibits high reversible capacities of 232 and 102 mAh/g at 2 A/g and 5 A/g, respectively. Under the same conditions, pristine MIS can only deliver reversible capacities of 21 and 4 mAh/g. The results indicate that MIS/SWCNT composites are promising anode materials for LIBs.

Porous Si/Ca-Si-O nanocomposite lithium storage materials by calciothermic reduction of Si with CaH2

Silicon monoxide (SiO)-based anode materials are one of the most intensively investigated class of materials for use as high-capacity anodes in lithium-ion batteries. However, their low initial Coulombic efficiency (ICE), resulting from the irreversible electrochemical reaction of the amorphous SiO2 (a-SiO2) phase in the SiO, restricts the wide-spread adoption of SiO-based anode materials in lithium-ion batteries. Pre-emptive formation of an irreversible phase that converts a-SiO2 to a non-reactive state with lithium prior to cell assembly has received much attention for enhancing ICE. However, this process has the drawback of not ensuring long-term cycle performance. Herein, the pre-emptive formation of irreversible phase combined with the high-energy mechanical milling (HEMM) process is proposed to simultaneously improve both the ICE and long-term cycle performance. The resulting porous Si/Ca-Si-O nanocomposite electrode exhibits an impressive ICE of 86.4 % and maintains 55 % of its capacity over 200 cycles. The key factor in the significant ICE improvement is the irreversible Ca-Si-O phase, which is formed by the calciothermic reduction of Si with CaH2. In addition, the microstructural changes induced by the HEMM process effectively mitigate the volume expansion of Si during cycling, resulting in improved long-term cycle stability.

Enhancing the Lithium Storage Performance of the Nb2O5 Anode via Synergistic Engineering of Phase and Cu Doping.

Nb2O5 has been viewed as a promising anode material for lithium-ion batteries by virtue of its appropriate redox potential and high theoretical capacity. However, it suffers from poor electric conductivity and low ion diffusivity. Herein, we demonstrate the controllable fabrication of Cu-doped Nb2O5 with orthorhombic (T-Nb2O5) and monoclinic (H-Nb2O5) phases through annealing the solvothermally presynthesized Nb2O5 precursor under different temperatures in air, and the Cu doping amount can be readily controlled by the concentration of the precursor solution, whose effect on the lithium storage behaviors of the Cu-doped Nb2O5 is thoroughly investigated. H-Nb2O5 shows obvious redox peaks (Nb5+/Nb4+ and Nb4+/Nb3+) with much higher capacity and better cycling stability than those for the widely investigated T-Nb2O5. When introducing appropriate Cu doping, the optimized H-Cu0.1-Nb2O5 electrode shows greatly enhanced conductivity and lower diffusion barrier as revealed by the theoretical calculations and electrochemical characterizations, delivering a high reversible capacity of 203.6 mAh g-1 and a high capacity retention of 140.8 mAh g-1 after 5000 cycles at 1 A g-1, with a high initial Coulombic efficiency of 91% and a high rate capacity of 144.2 mAh g-1 at 4 A g-1. As a demonstration for full-cell application, the H-Cu0.1-Nb2O5||LiFePO4 cell displays good cycling performance, exhibiting a reversible capacity of 135 mAh g-1 after 200 cycles at 0.2 A g-1. More importantly, this work offers a new synthesis protocol of the monoclinic Nb2O5 phase with high capacity retention and improved reaction kinetics.

Silicon-tin thin-film anodes for low and high power-density lithium-ion batteries

Silicon (Si) is a promising replacement material for graphite, the commonly utilized anode material in lithium-ion batteries (LIBs). Si has a theoretical specific capacity up to 11 times higher than that of graphite. However, pure Si has two main issues: high electronic resistivity and significant volume change during charge/discharge cycling. To overcome these issues, Si was alloyed with high-conductivity materials. In this contribution, physical vapor deposition was utilized to produce binderless silicon-tin anodes for LIBs. Tin is a lithium-active alloying material that has high electrical conductivity and high specific capacity (i.e., up to three times that of graphite). Electronic resistivity, residual film stress, X-ray photoelectron spectroscopy, Raman spectroscopy, and cyclic voltammetry measurements were performed to thoroughly analyze the deposited Si-Sn films and help understand their charge/discharge cycling performance at low and high C-rates. At a low C-rate of 0.5 C, the alloyed films did not show any improvement compared to pure Si. However, the alloyed films showed better performance compared to pure Si when tested at a high C-rate of 10 C. Si-Sn films with (40 – 50 wt.% Sn) were able to retain a specific capacity of around 680 mAh g−1 after 1000 cycles.

Bio-synthesized TiO2 nanoparticles and the aqueous binder-based anode derived thereof for lithium-ion cells.

Titanium dioxide nanoparticles (TiO2-NPs) are a promising anode material for Lithium-ion batteries (LIBs) due to their good rate capability, low cost, non-toxicity, excellent structural stability, extended cycle life, and low volumetric change (∼4%) during the Li+insertion/de-insertion process. In the present paper, anatase TiO2-NPs with an average particle size of ~ 12nm were synthesized via a green synthesis route using Beta vulgaris (Beetroot) extract, and the synthesized TiO2-NPs were evaluated as anode material in LIBs. Furthermore, we employed an aqueous binder (1:1 mixture of carboxy methyl cellulose and styrene butadiene) for electrode processing, making the process cost-effective and environmentally friendly. The results revealed that the Li/TiO2 half-cells delivered an initial discharge capacity of 209.7 mAh g-1 and exhibited superior rate capability (149 mAh g-1 at 20 C) and cycling performances. Even at the 5C rate, the material retained a capacity of 82.2% at the end of 100 cycles. The synthesis route of TiO2-NPs and the aqueous binder-based electrode processing described in the present work are facile, green, and low-cost and are thus practically beneficial for producing low-cost and high-performance anodes for advanced LIBs.

Exploring Lead Zirconate Titanate, the Potential Advancement as an Anode for Li-Ion Batteries.

Graphite, widely adopted as an anode for lithium-ion batteries (LIBs), faces challenges such as an unsustainable supply chain and sluggish rate capabilities. This emphasizes the urgent need to explore alternative anode materials for LIBs, aiming to resolve these challenges and drive the advancement of more efficient and sustainable battery technologies. The present research investigates the potential of lead zirconate titanate (PZT: PbZr0.53Ti0.47O3) as an anode material for LIBs. Bulk PZT materials were synthesized by using a solid-state reaction, and the electrochemical performance as an anode was examined. A high initial discharge capacity of approximately 686 mAh/g was attained, maintaining a stable capacity of around 161 mAh/g after 200 cycles with diffusion-controlled intercalation as the primary charge storage mechanism in a PZT anode. These findings suggest that PZT exhibits a promising electrochemical performance, positioning it as a potential alternative anode material for LIBs.

MXene-reinforced Sb@C nanocomposites with synergizing spatial confinement architecture enabled ultra-stable and fast lithium ion storage

Antimony (Sb) is recognized as a potential anode material for lithium-ion batteries due to its high theoretical capacity and adequate working potential. However, its application is hindered by the significant volume expansion during lithiation and low intrinsic conductivity, leading to considerable capacity fading and reduced rate capability. Herein, a unique MXene-reinforced Sb@C (MSC) nanocomposite is constructed via in-situ growing Sb-MOF over the conductive MXene substrate, followed by annealing. MXene substrate and MOF-derived carbon layer coupling effectively creates a continuous and conductive framework, encapsulating Sb nanoparticles. This unique architecture mitigates volume expansion, prevents particle aggregation, and enhances interfacial charge transfer, significantly improving the lithium storage performance of the MSC nanocomposite over its Sb@C (SC) counterpart. The MSC nanocomposite achieves a high capacity of 625 mAh g−1 at 100 mA g−1, superior rate capability of 305 mAh g−1 at 10 A g−1, as well as excellent cycling stability with a capacity retention of 84.4 % over 2000 continuous cycles. Additionally, a lithium-ion full batteries with MSC anode and LiFePO4 cathode demonstrates a capacity of 168.9 mAh g−1 at 100 mA g−1 and a maximum energy density of 381.2 Wh kg−1 based on the cathode mass, illustrating its promising potential for constructing high-performance lithium ion batteries.

Thermodynamic stability and ionic conductivity in lithium–germanium binary system

Lithium–germanium binary compounds are promising anode materials for secondary lithium-ion batteries due to their high capacity, low operating voltage, and high electronic conductivity of lithiated Ge. For their successful application in batteries, it is essential to know the temperature stability of different Li–Ge phases and the variation of their ionic conductivity depending on the operating temperatures of the batteries. This work aims to comprehensively study the thermodynamic stability and ionic conductivity in Li–Ge binary compounds using a combination of first-principle computations and machine-learning interatomic potentials. We calculated convex hulls of the Li–Ge system at various temperatures and a temperature–composition phase diagram was obtained, delineating stability fields of each phase. Our calculations show that at temperatures higher than 590 K, LiGe undergoes a I41/a–P4/mmm transition, which leads to a change in the ionic conductivity. We show that all stable and metastable Li–Ge compounds have high ionic conductivity, but LiGe and Li7Ge12 have the lowest lithium diffusion. Trajectories of diffusion and Ge arrangements depend on lithium concentration. Based on advanced theoretical approaches, this study provides insights for the development of Li–Ge materials in lithium-ion and lithium-metal battery applications.