High-performance Lithium-ion Battery Anodes Research Articles

Novel binary regulated silicon-carbon materials as high-performance anodes for lithium-ion batteries.

The massive volume dilation, unsteady solid electrolyte interphase, and weak conductivity about Si have failed to bring it to practical applications, although its potential capacity is up to 4200 mAh g-1. For solving these problems, novel binary regulated silicon-carbon materials (Si/BPC) were done by a sol-gel procedure combined with single carbonization. Analytical techniques were systematically utilized to examine the effects of element doping at several gradients on morphology, structure and electrochemical properties of composites, thus the optimal content was identified. Si/BPC preserves a discharge specific capacity of 1021.6 mAh g-1with a coulomb efficiency of 99.27% after 180 cycles at 1000 mA g-1, within the upgrade than single-doped and undoped. In rate test, it has a specific capacity of 1003.2 mAh g-1at a high current density of 5000 mA g-1, quickly back towards 2838.6 mAh g-1at 200 mA g-1. The inclusion of B and P elements is linked to the electrochemical characteristics. In the co-doped carbon layers, the synergistic impact of doping B and P accelerates the diffusion kinetics of lithium ions, boosts diffusion rate of Li+, offers low electrochemical impedance (45.75 Ω). This brings more defects to provide transport carriers and induces a substantial amount of electrochemically active sites, which fosters the storage of Li+, thus making silicon material electrochemically more active and potential.

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.

Layered Siloxene Microparticles: Unveiling Long-Term Stability and High Volumetric Capacity for Advanced Lithium-Ion Batteries

Two-dimensional (2D) Si π materials, a silicon counterpart of graphene, are particularly interesting because they exhibit intrinsic electrochemical and mechanical behavior combined with structural anisotropy. This work aims to improve the Li-storage performance of 2D siloxene (2DSi) microparticles by co-imidization with polymer binder. The proposed method combines 2DSi with poly(amic acid) to form a covalently bound poly(imide) (PI) layer upon thermal dehydration. Electrochemical evaluations reveal that the resulting 2DSi-PI electrode exhibits a unique electrochemical behavior toward Li+ based on intercalation, with additional reversible (de-)lithiation attributed to carbonyl oxygens of PI. Without suffering volume expansion, the 2DSi-PI electrodes display a highly stable capacity generation of 585 mAh g−1 at 250 mA g−1 with a capacity loss of 0.13 % per cycle at the 200th cycle. In addition, the full-cell of the 2DSi-PI electrode combined with the LiNi0.8Co0.1Mn0.1O2 cathode achieves an energy density of 426 Wh kg−1 at a power density of 1,155 W kg−1. Ex-situ and theoretical analyses of the (de-)lithiated 2DSi-PI electrodes demonstrate that the surface-bound PI suppresses solvent reduction, increases the amount of LiF in the SEI layer, and improves the binding affinity of 2DSi to LiF. As a result, the cycle stability of 2DSi-PI electrodes is significantly improved in comparison to 2DSi-polyvinylidene fluoride electrodes. Co-imidization with PI emerges as a promising strategy for advancing the electrochemical properties of 2DSi electrodes, offering insights for the design of high-performance lithium-ion battery anodes.

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.

Simple hydrothermal synthesis of HCNFs@CoNiO2 composite material for high-performance anode of lithium-ion batteries

In this study, a novel helical carbon nanofibers@CoNiO2 (HCNFs@CoNiO2) composite was first successfully synthesized by the simple hydrothermal method and utilized as anode materials of lithium-ion batteries (LIBs). CoNiO2 nanoparticles with a particle size of about 6 nm were distributed on the surface of HCNFs matrix. The HCNFs@CoNiO2 anode shows the excellent reversible specific capacity of 808.5 mAh/g after 100 cycles at 200 mA/g, which is about four and twenty times larger than that of HCNFs (193.5 mAh/g) and CoNiO2 (35.4 mAh/g), respectively. The electrochemical performance of HCNFs@CoNiO2 was improved due to the synergistic contribution of HCNFs and CoNiO2. In particular, HCNFs with the unique three-dimensional helical structure improve the conductivity and also provide a strong supporting network space during the volume expansion of CoNiO2 nanoparticles. The present study provides a useful reference for the development of the novel high-performance anode material for LIBs.

Fe2O3 nanoparticles encapsulated in the inner walls of integrated 3D carbon tube grid as high-performance anode for lithium-ion batteries

Ferric oxide (Fe2O3) holds huge potential as a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical capacity and low cost, however, its battery performance is still limited by the intrinsic poor conductivity and huge volume variation during lithiation and de-lithiation processes. Herein, we developed a self-standing 3D interconnected vertical and lateral carbon tube (3D-CT) grid with Fe2O3 nanoparticles (NPs) encapsulated in the wall of CT (denoted as 3D-CT@Fe2O3-NPs@C), as structurally-integrated anode without any inactive components. The 3D-interconnected vertical and lateral CTs with open channels not only provide plenty of attachment sites for the Fe2O3 NPs and accommodate the strain generated by the volume variation of Fe2O3, but also facilitate the fast ions and electrons transfer. Therefore, the self-supported 3D-CT@Fe2O3-NPs@C electrode delivers superior cycling and high-rate performance with a high stable specific capacity of 896.2 mAh g−1 at the current density of 1.0 A g−1 after 700 cycles. Even at the high current density of 4.0 A g−1, a reversible capacity of 488.1 mAh g−1 can be reached based on the mass of the electrode. This study provides a facile and efficient strategy to improve the electrochemical performance of LIBs through the design of structurally-integrated grid electrode.

Conductive copper ion-reinforced sodium alginate aerogel based free-standing Si anode for Li-ion storage

Biomass materials with great advantages of wide accessibility, low cost and environmental benignity have favorable application prospects as Si anodes for lithium-ion batteries (LIBs). In order to alleviate the volume effect and improve the conductance of Si, we fabricated a conductive copper ion-reinforced sodium alginate (SA) aerogel based free-standing Si anode (Si@CNTs/Alg-Cu-II) containing silicon nanoparticles, sodium alginate aerogel, carbon nanotubes and Cu nanoparticles, via a simple, low-cost and sustainable process (under 1 × 10−1 Pa, 1 °C/min to 200 °C holding for 1 h). In the irregular lamellar porous aerogel, silicon particles with good dispersion are bound by macromolecular chains of SA via dynamic hydrogen bonds and subsequently restrained in the porous aerogel to release volume stress. The in situ generated Cu particles and well-dispersed carbon nanotubes (CNTs) construct the conductive network around Si particles to improve the electrical conductivity of the electrode. This unique structure delivers a capacity of 835.6 mAh/g after 100 cycles at 0.1 A/g based on the total mass of Si@CNTs/Alg-Cu-II composite (Si content of 25.62%). Moreover, it also shows outstanding stability under high current density (a capacity retention of 84.1% after 100 cycles at 0.5 A/g). The sustainable preparation method and excellent electrochemical performance of Si@CNTs/Alg-Cu-II provide a new strategy to develop high-performance free-standing Si-based anodes for LIBs.

Mechanically robust and conductive Ti5Te4/P@C composite materials as promising lithium-ion battery anodes

An urgent need has emerged to develop lithium-ion battery anodes that exhibit high reversible capacity and rate performance surpassing carbonaceous materials. Si-based composites have been investigated extensively. However, in this study, we explored another potential alloy anode consisting of Te and phosphorus without Si. Herein, we present a novel composite material, Ti5Te4/P@C, as an anode for lithium-ion batteries (LIBs). Tellurium, which exhibits good electrical conductivity and high volumetric capacity, and red phosphorus, which exhibits high theoretical capacity, were selected as potential anode materials. To overcome the common drawbacks of the two materials, including the vigorous expansion of volume, electrochemically inactive materials, such as titanium and carbon, were introduced as matrix buffers. Te, Ti, red phosphorus, and C were synthesized using a three-step high energy ball milling (HEBM) technique, that is, stepwise synthesis of (1) Ti and Te, (2) red phosphorus, and (3) carbon. The developed Ti5Te4/P@C composites revealed that the introduction of red P led to the generation of additional pure Te in the Ti5Te4/P@C composites, which was owing to the different binding interactions between Ti, Te, and red P, as confirmed by DFT calculations. Among the developed Ti5Te4/P@C anodes, Ti5Te4/P(30 wt%)@C exhibited outstanding cyclability and high rate performance (440 mAh g−1 at 300 mA g−1 after 500 cycles). To confirm the electrochemical responses and Li+ ion diffusion mechanisms, CV and GITT analyses were performed. Based on the electrochemical characteristics, the superior electrochemical performance of the Ti5Te4/P@C anodes can be ascribed to the well-defined composite structure, including the high electrical conductivity of Te, high theoretical capacity of red P, and effective buffering agents of Ti as a mechanical supporter and conductive C, which enable a pseudocapacitive response, providing better reversibility. Therefore, the Ti5Te4/P@C composite materials are viable anodes for high-performance LIBs.

Boron-doped three-dimensional porous carbon framework/carbon shell encapsulated silicon composites for high-performance lithium-ion battery anodes

Deleterious volumetric expansion and poor electrical conductivity seriously hinder the application of Si-based anode materials in lithium-ion batteries (LIBs). Herein, boron-doped three-dimensional (3D) porous carbon framework/carbon shell encapsulated silicon (B-3DCF/Si@C) hybrid composites are successfully prepared by two coating and thermal treatment processes. The presence of 3D porous carbon skeleton and carbon shell effectively improves the mechanical properties of the B-3DCF/Si@C electrode during the cycling process, ensures the stability of the electrical contacts of the silicon particles and stabilizes the solid electrolyte interface (SEI) layer, thus enhancing the electronic conductivity and ion migration efficiency of the anode. The developed B-3DCF/Si@C anode has a high reversible capacity, excellent cycling stability and outstanding rate performance. A reversible capacity of 1288.5 mAh/g is maintained after 600 cycles at a current density of 400 mA g−1. The improved electrochemical performance is demonstrated in a full cell using a LiFePO4-based cathode. This study presents a novel approach that not only mitigates the large volume expansion effects in LIB anode materials, but also provides a reference model for the preparation of porous composites with various functionalities.

Scalable Synthesis of a Si/C Composite Derived from Photovoltaic Silicon Kerf Waste toward Anodes for High-Performance Lithium-Ion Batteries

Scalable Synthesis of a Si/C Composite Derived from Photovoltaic Silicon Kerf Waste toward Anodes for High-Performance Lithium-Ion Batteries

Constructing a buffer macroporous architecture on silicon/carbon anode for high-performance lithium-ion battery

Constructing a buffer macroporous architecture on silicon/carbon anode for high-performance lithium-ion battery

A Study of Porous Activated Carbon Anodes for High-Performance Lithium-Ion Batteries

This research paper explores the intricate realm of porous activated carbon anodes for high-performance lithium-ion batteries, responding to the escalating demand for advanced energy storage systems. The study begins by delving into various synthesis methods, including physical and chemical activation, and hybrid approaches, aiming to optimize porosity and surface chemistry. Detailed investigations into structural characteristics encompass surface area, pore distribution, morphology, and surface chemistry. Advanced microscopy techniques and characterization tools provide insights into the complex interplay between structural features and electrochemical performance. Moving beyond the laboratory, the paper explores potential applications of porous activated carbon anodes. In electric vehicles, these anodes demonstrate promise in enhancing energy and power density, critical factors for the widespread adoption of electric transportation. For portable electronic devices, the lightweight nature and improved safety profile make them an attractive choice. Additionally, the study assesses the feasibility of integrating porous activated carbon anodes in grid-scale energy storage, contributing to the stability and reliability of renewable energy integration. Environmental considerations are addressed, evaluating the sustainability and recyclability of porous activated carbon anodes. The paper concludes by summarizing key findings, emphasizing the significance of porous activated carbon in advancing lithium-ion battery technology, and proposing future research directions to overcome current challenges. The extensive array of references underscores the interdisciplinary nature of the research, incorporating a diverse range of sources to provide a comprehensive overview of the field.

Constructing a Stable Conductive Network for High-Performance Silicon-Based Anode in Lithium-Ion Batteries.

The application of carbon nanotubes to silicon nanoparticles has been used to improve the electrical conductivity of silicon-carbon anodes and prevent agglomeration of silicon nanoparticles during cycling. In this study, the composites are synthesized through an uncomplicated technique that involves the ultrasonication mixing of pyrene derivatives and carbon nanotubes and the formation of complexes with silicon nanoparticles in ultrasonic dispersion and magnetic stirring and then treated under vacuum. When the prepared composites are applied as lithium-ion battery anodes, the Si@(POH-AOCNTs) electrode displays a high reversible capacity of 3254.7 mAh g-1 at a current density of 0.1 A g-1. Furthermore, it exhibits excellent cycling stability with a specific capacity of 1195.8 mAh g-1 after 500 cycles at 1.0 A g-1. The superior electrochemical performance may be attributed to a large π-conjugated electron system of pyrene derivatives, which prompts the formation of a homogeneous CNTs conductive network and ensures the effective electron transfer, while the interaction between hydroxyl functional groups of hydroxypyrene and binder synergizes with CNTs network to further enhance the cycling stability of the composite.

Transient freezing strategy of metastable lithium titanate for high performance lithium-ion battery anodes under high pressure

Lithium-ion batteries (LIBs) with a solid-solution or single-phase intercalation mechanism are considered to be excellent candidates for fast charging and addressing range anxiety, as they have few kinetic energy barriers apart from ion diffusion. In this regard, we capture metastable lithium titanate using High-Pressure High-Temperature (HPHT) synthesis technique under thermodynamic control in only 30 min. Compared with most conventional synthesis methods in the field, the preparation time is only 1.6–3.6% of them. Interestingly, stable and controllable structural defects can be induced under high pressure. Additionally, the HPHT-induced “fracture” structure significantly improves the kinetics of electrolyte storage and exhibits a remarkable pseudocapacitance of up to 89.1%. After 1000 cycles at 10 C, it still retains a reversible capacity of 165 mAh g−1 with a capacity retention rate of 97%. The capture of metastable phase by HPHT technology provides a new perspective and approach for material optimization and design.

Synergistic Performance Boosts of Dopamine-Derived Carbon Shell Over Bi-metallic Sulfide: A Promising Advancement for High-Performance Lithium-Ion Battery Anodes.

A CoMoS composite is synthesized to combine the benefits of cobalt and molybdenum sulfides as an anodic material for advanced lithium-ion batteries (LIBs). The synthesis is accomplished using a simple two-step hydrothermal method and the resulting CoMoS nanocomposites are subsequently encapsulated in a carbonized polydopamine shell. The synthesis procedure exploited the self-polymerization ability of dopamine to create nitrogen-doped carbon-coated cobalt molybdenum sulfide, denoted as CoMoS@NC. Notably, the de-lithiation capacity of CoMoS and CoMoS@NC is 420 and 709 mAh g⁻1, respectively, even after 100 lithiation/de-lithiation cycles at a current density of 200mA g⁻1. Furthermore, excellent capacity retention ability is observed for CoMoS@NC as it withstood 600 consecutive lithiation/de-lithiation cycles with 94% capacity retention. Moreover, a LIB full-cell assembly incorporating the CoMoS@NC anode and an NMC-532 cathode is subjected to comprehensive electrochemical and practical tests to evaluate the performance of the anode. In addition, the density functional theory showcases the increased lithium adsorption for CoMoS@NC, supporting the experimental findings. Hence, the use of dopamine as a nitrogen-doped carbon shell enhanced the performance of the CoMoS nanocomposites in experimental and theoretical tests, positioning the material as a strong candidate for LIB anode.

Surface modification of electrospun nitrogen-doped Ge@C fiber with highly porous NiCo2O4 layer as high-performance lithium-ion battery anode

Elemental germanium (Ge) is considered a high-capacity anode material for lithium-ion batteries (LIBs). However, it suffers from severe capacity degradation and inherent material instability owing to inevitable volumetric changes during the alloying/dealloying reactions with lithium. In this study, we report a hierarchical architecture comprising Ge nanoparticles in electrospun carbon fibers (Ge@C) coated with an in situ grown NiCo2O4 (NCO) layer to enhance the structural stability and electrochemical reversibility of Ge. The Ge@C@NCO fibers possess unique features, including well-dispersed Ge in nitrogen-doped porous carbon network that serves as a conductive volumetric buffer. This configuration allows for effective volume accommodation and improved electronic conductivity. Moreover, the porous NCO contributed to enhanced reversible capacity and rapid ionic transfer during electrochemical reactions. As a result, the Ge@C@NCO anode exhibited an ultrahigh specific capacity of 981.7 mAh g−1 and excellent capacity retention over 200 cycles under a current density of 1 A g−1, indicating superior lithium storage properties compared to pure Ge. Additionally, it retained approximately 80 % of initial capacity after 300 cycles even at 5 A g−1, demonstrating fast charging capability. The outstanding performance of this hierarchical structure presents a new path for designing alloying-based anodes for high-energy-density LIBs.

Carbon-Coated Tin-Titanate derived SnO2/TiO2 nanowires as High-Performance anode for Lithium-Ion batteries

Tin dioxide (SnO2) is a promising alternative material to graphite anode, but the large volume change induced electrode pulverization issue has limited its application in lithium-ion batteries (LIBs). In contrast, titanium dioxide (TiO2) anode shows high structure stability upon lithium insertion/extraction, but with low specific capacity. To overcome their inherent disadvantages, combination of SnO2 with TiO2 and highly conductive carbon material is an effective way. Herein, we report a facile fabrication method of carbon-coated SnO2/TiO2 nanowires (SnO2/TiO2@C) using tin titanate nanowires as precursor, which are prepared by reacting SnCl2·2H2O with layered sodium titanate (Na2Ti3O7) nanowires in the aqueous solution though the ion exchange between Sn2+ and Na+. After annealing under argon atmosphere, the hydrothermally carbon-coated tin-titanate nanowires decompose, forming a unique hybrid structure, where ultrafine SnO2 nanoparticles are uniformly embedded within the TiO2 substrate with carbon coating. Consequently, the SnO2/TiO2@C nanowires demonstrate excellent lithium storage capacity with high pseudocapacitance contribution, excellent reversible capacity, and long-term cycling stability (673.7/510.5 mAh/g at 0.5/1.0 A/g after 250/800 cycles), owing to the unique hybrid structure, as the well-dispersion of ultra-small SnO2 within TiO2 nanowire substrate with simultaneous carbon coating efficiently suppresses the volume changes of SnO2, provides abundant reactive sites for lithium storage, and enhances the electrical conductivity with shortened ion transport distance.

Green method of encapsulating SnO2 in the matrix of corn stalk-derived carbon used for high-performance lithium-ion battery anode material

Green method of encapsulating SnO2 in the matrix of corn stalk-derived carbon used for high-performance lithium-ion battery anode material

Cobalt Oxide-Decorated on Carbon Derived from Onion Skin Biomass for Li-Ion Storage Application

Onion waste, particularly onion skin, is a widely generated waste material, and harnessing its potential for energy storage aligns with sustainable development goals. Despite the high specific surface area exhibited by biocarbon derived from onion skin, its Li-ion storage performance is not desirable. In this study, biocarbon derived from purple onion skin serves as the substrate for accommodating cobalt oxide (Co3O4) through a hydrothermal method, employing Co(NO3)2·6H2O at various concentrations, and with and without prior activation using KOH treatment. The resulting samples undergo comprehensive analyses, including phase, morphological, surface, and electrochemical characterizations. The Co3O4 decoration on activated carbon derived from onion skin, synthesized using Co(NO3)2·6H2O at a concentration of 1 M, reveals a porous structure with a surface area of 702 m2/g, featuring predominant pore sizes of less than 5 nm. Significantly, the Li-ion storage performance of this sample surpasses that of alternative samples, demonstrating a remarkable reversible capacity of 451 mAh/g even after 500 cycles at an elevated current density of 2000 mAh/g. The charge transfer resistance of the sample (110.3 Ω) is found to be substantially lower than that of the sample prepared using carbonized onion skin biomass without activation. This research introduces an innovative approach leveraging onion skin waste as a template for Co3O4 decoration, thereby fabricating high-performance anodes for lithium-ion batteries.

Engineering ultra-small tin phosphide encapsulated in 3D phosphorous-doped porous carbon nanosheets as high-performance anodes for lithium-ion batteries

Transition-metal phosphides (TMPs) with high theoretical specific capacity and appropriate reaction potential have been recognized as prospective anode materials for lithium-ion batteries (LIBs). However, the practical application is still hindered by the inferior rate capability and worse cycling stability, which is mainly arising from large volume variations and inferior electric conductivities of TMPs. Herein, ultra-small Sn4P3 particles are fully embedded into three-dimensionally interconnected P-doped porous carbon nanosheets (Sn4P3/P-C@CNs), which is fabricated by a feasible and environmentally friendly synthesis strategy with phytic acid as phosphorus source. The ultra-small Sn4P3 particles and the conductive P-doped 3D carbon backbone is advantage to alleviate the volume changes of Sn4P3 nanoparticles, reduce side reaction with electrolyte and promote the transfer of ions/electrons, leading to a significant improvement in electrochemical performance. Consequently, the Sn4P3/P-C@CNs composite electrode delivers a high reversible capacity of 770 mA h g−1 at 0.1 A/g upon 100 cycles, and exhibits 717 mA h g−1 at 1 A/g after 1000 loops. The lithium storage mechanism is investigated by density functional theory calculations. This research could offer a sensible and facile design strategy for TMPs-based electrode materials and make it hopeful for the applications in next-generation high-energy–density LIBs.