Anode Material For Lithium-ion Batteries Research Articles

3D porous structure Fe3O4@SnO2/MXene composites with enhanced electrochemical performance for lithium ion battery anode

The low theoretical capacity of the commercial graphite electrodes used in lithium-ion batteries (LIBs) necessitates the development of novel anode materials with higher rate performance, reversible specific capacities, long cycle lives, and low costs. In this work, three-dimensional porous structure Fe3O4 nanosphere with extremely thin SnO2 coatings are prepared by a method of getting twice the result with half the effort. And it was uniformly dispersed in an MXene flexible conductive matrix to fabricate a 3D porous heterogeneous Fe3O4@SnO2/MXene composite to act as an anode material for LIBs. The 3D porous heterojunction structure integrates the advantages of Fe3O4@SnO2 and MXene, achieving rapid electron and ion transport at the interface and the effective release of structural stress. The introduction of MXene markedly enhances the conductibility of the materials, limits the expansion of Fe3O4 during the Li+ insertion/removal process, and inhibits its aggregation. The Fe3O4@SnO2/MXene anode exhibits excellent electrochemical performance (1609 mAh g−1 over 200 cycles at 100 mA g−1 and 626.1 mAh g−1 over 900 cycles at 1000 mA g−1). These findings demonstrate that the Fe3O4@SnO2/MXene composite is a promising anode material for LIBs.

Improved cycle stability and high-rate capability of LiNbO3-coated Li3VO4 as anode material for lithium-ion battery

Lithium vanadate (Li3VO4) has garnered considerable attention as an alternative negative electrode material for non-aqueous lithium-ion batteries due to its high capacity, energy efficiency, and stable discharge voltage. Nonetheless, the Li3VO4 material displays a low rate capability, attributed mainly to its poor intrinsic electronic conductivity. Here, we report the synthesis of lithium niobate LiNbO3-coated Li3VO4 (LVO@LNO) using a one-pot sol-gel method. The resulting LVO@LNO demonstrates a high reversible capacity of approximately 530 mAh/g, which is more than double that of free Li3VO4. To explore the effect of the LNO coating process on the morphological and structural properties, Raman, XRD, operando XRD, XPS, SEM and HTEM analyses were conducted. To explain the enhancement of electronic conductivity in our modified material after a LiNbO3 coating, we conducted an Ex-Situ electrochemical impedance (EIS) and Density Functional Theory (DFT) computational study. Additionally, we designed a full cell utilizing a 1 wt% LNO-coated LVO anode and NMC-811 cathode. The cell yielded an output voltage of approximately 2.8 V with a high initial specific capacity of 350 mAh/g versus to the anode, at 1C with a capacity retention of 85 % after 100 cycles.

First-principles prediction of one-dimensional conductive metallic organic polymers as ultrahigh energy density anode for lithium-ion batteries.

Metal-Organic Polymers (MOPs) have attracted growing attention for lithium-ion battery (LIB) applications due to their merits in orderly ionic transportation and robust structure stability in electrochemical reactions. However, they suffer from poor electronic conductivity. In this work, we apply first-principles density functional theory to explore the potential of three one-dimensional (1D) electrically conductive C6H2S4TM (TM = Fe, Co, and Ni) MOPs with the π-d conjugated coordination as anode materials for Li+ ions storage. Our theoretical results reveal that these 1D MOPs possess a superior theoretical capacity of over 748 mA h g-1. In particular, the 1D C6H2S4Ni MOP shows an exceptional theoretical specific capacity of 1110 mA h g-1 based on the three-electron transferring reaction, which significantly outperforms the traditional graphite-based anode material in LIBs. Moreover, the resonant charge transfer between Ni metal and ligand within the 1D C6H2S4Ni MOP reduces the diffusion energy barrier of the Li atoms when they migrate on the surface of the MOP. The ultrahigh theoretical specific capacity of the C6H2S4Ni MOP predicts that it can be a promising anode material for LIBs.

Imidazole-Intercalated Cobalt Hydroxide Enabling the Li+ Desolvation/Diffusion Reaction and Flame Retardant Catalytic Dynamics for Lithium Ion Batteries.

Lithium-ion batteries have found extensive applications due to their high energy density and low self-discharge rates, spanning from compact consumer electronics to large-scale energy storage facilities. Despite their widespread use, challenges such as inherent capacity degradation and the potential for thermal runaway hinder sustainable development. In this study, we introduce a unique approach to synthesize anode materials for lithium-ion batteries, specifically imidazole-intercalated cobalt hydroxide. This innovative material significantly enhances the Li+ desolvation/diffusion reaction and flame-retardant dynamics through complexing and catalytic synergetic effects. The lithium-ion batteries incorporating these materials demonstrate exceptional performance, boasting an impressive capacity retention of 997.91 mAh g-1 after 500 cycles. This achievement can be attributed to the optimization of the solid electrolyte interphase (SEI) interface engineering, effectively mitigating anode degradation and minimizing electrolyte consumption. Experimental and theoretical calculations validate these improvements. Importantly, imidazole intercalated Co(OH)2 (MI- Co(OH)2) exhibits a remarkable catalytic effect on electrolyte carbonization and the conversion of CO to CO2. This dual action suppresses smoke and reduces toxicity significantly. The presented work introduces a novel approach to realizing high-performance and safe lithium-ion batteries, addressing key challenges in the pursuit of sustainable energy solutions.

Triblock Polymer/Acetylene Black Dual‐Assisted Preparation of Ge/C Nanocomposites with Superior Lithium Storage Performance

Anode materials based on IV main group elements like Si, Ge, and Sn show great potential for lithium‐ion batteries (LIBs) due to their high specific capacity and low working potential. However, issues such as volume expansion and lattice pulverization hinder their practical usage. To address these issues for Ge, a novel F127 triblock polymer/acetylene black dual‐assisted strategy is proposed to achieve uniform dispersion of polycrystalline Ge, enabling the preparation of Ge@C nanocomposites via hydrogen reduction. The introduced F127 triblock polymer and acetylene black serves a dual purpose to enhance electrical conductivity and prevent Ge nanoparticles from agglomeration. When tested as anode material for LIBs, the Ge@C nanocomposites exhibit exceptional electrochemical performances, demonstrating a sustained specific discharge capacity of 780 mA h g‐1 at 0.2 A g‐1 after 100 cycles. Moreover, the capacity remains at 767 mA h g‐1 even after 300 cycles at a higher current density of 0.5 A g‐1. These enhanced lithium storage performances are attributed to the combined effects of well‐dispersed tiny Ge nanoparticles, uniform carbon coating, and an abundance of defects. These factors effectively mitigate the volume expansion and lattice pulverization of Ge nanoparticles and concurrently enhance their conductivity, leading to improved overall performance in LIBs.

Facile Synthesis and Li-Electroactivity of Cobalt Oxide Based on Resources Recovered from Waste Lithium-Ion Batteries

In this study, cobalt oxide (Co3O4) powder was prepared by simple precipitation and heat-treatment process of cobalt sulfate that is recovered from waste lithium-ion batteries (LIBs), and the effect of heat-treatment on surface properties of as-synthesized Co(OH)2 powder was systematically investigated. With different heat-treatment conditions, a phase of Co(OH)2 is transformed into CoOOH and Co3O4. The result showed that the porous and large BET surface area (ca. 116 m2/g) of Co3O4 powder was prepared at 200°C for 12 h. In addition, the lithium electroactivity of Co3O4 powder was investigated. When evaluated as an anode material for LIB, it exhibited good electrochemical performance with a specific capacity of about 500 mAh g–1 at a current density of C/5 after 50 cycles, which indicates better than those of commercial graphite anode material.

Interface Engineering of MOF-Derived Co3O4@CNT and CoS2@CNT Anodes with Long Cycle Life and High-Rate Properties in Lithium/Sodium-Ion Batteries.

Metal-organic framework materials can be converted into carbon-based nanoporous materials by pyrolysis, which have a wide range of applications in energy storage. Here, we design special interface engineering to combine the carbon skeleton and nitrogen-doped carbon nanotubes (CNTs) with the transition metal compounds (TMCs) well, which mitigates the bulk effect of the TMCs and improves the conductivity of the electrodes. Zeolitic imidazolate framework-67 is used as a precursor to form a carbon skeleton and a large number of nitrogen-doped CNTs by pyrolysis followed by the in situ formation of Co3O4 and CoS2, and finally, Co3O4@CNTs and CoS2@CNTs are synthesized. The obtained anode electrodes exhibit a long cycle life and high-rate properties. In lithium-ion batteries (LIBs), Co3O4@CNTs have a high capacity of 581 mAh g-1 at a high current of 5 A g-1, and their reversible capacity is still 1037.6 mAh g-1 after 200 cycles at 1 A g-1. In sodium-ion batteries (SIBs), CoS2@CNTs have a capacity of 859.9 mAh g-1 at 0.1 A g-1 and can be retained at 801.2 mAh g-1 after 50 cycles. The unique interface engineering and excellent electrochemical properties make them ideal anode materials for high-rate, long-life LIBs and SIBs.

Silver-Decorated MoO3 as an Anode Material in Lithium-Ion Batteries

Silver-Decorated MoO₃ as an Anode Material in Lithium-Ion Batteries

Innovative design of silicon-core mesoporous carbon composite for high performance anode material in advanced lithium-ion batteries

Silicon is widely recognized as an exceptionally auspicious anode material for lithium−ion batteries due to its remarkable specific capacity, suitable operational potential, and ecologically innocuous characteristics. This study presents a novel silicon@void@FC (fibrous carbon) composite anode material for lithium-ion batteries. Utilizing a one-step synthesis approach, the resulting hollow core–shell structure, combined with a mesoporous carbon shell, demonstrates exceptional electrochemical performance. The Si@Void@FC electrode exhibits remarkable cycle stability and rate performance, maintaining structural integrity over 500 cycles without observable degradation. The outer carbon shell acts as a protective layer and accommodates silicon volume expansion during cycling, preventing excessive contact with the electrolyte. The rich mesoporous structure facilitates efficient lithium-ion diffusion, enhancing lithiation and delithiation processes. The simplified one-step synthesis method further streamlines the preparation process, eliminating the need for complete silica template formation. This innovative Si@Void@FC composite material holds promise for advancing lithium-ion battery technology, addressing challenges associated with silicon-based anode materials, and offering insights into the design and synthesis of high-performance energy storage materials.

Atomic-Level Insights into Defect-Driven Nitrogen Doping of Reduced Graphene Oxide

Nitrogen-doped graphene has been increasingly utilized in a variety of energy-related applications, serving as a catalyst or support material for fuel cells, and as an anode material for lithium-ion batteries, among others. The thermal reduction of graphene oxide (GO) in nitrogenous sources to incorporate nitrogen, producing nitrogen-doped reduced graphene oxide (NRGO), is the most favored method. Controlling atomic configurations of nitrogen-doped sites is the key factor for tailoring the physico-chemical properties of NRGO, but major challenges remain in identifying detailed atomic arrangements at nitrogen binding sites on highly defective and chemically functionalized GO surfaces. In this paper, we present atomistic-scale modeling of the nitrogen doping process of GO with different types of vacancy defects. Molecular dynamics simulations using a reactive force field indicate that the edge carbon atoms on defect sites are the dominant initiation location for nitrogen doping. Further, first-principles calculations using density functional theory present energetically favorable chemical transition pathways for nitrogen doping. The significance of this work lies in providing important chemical insights for the effective control of the desired properties of NRGO by suggesting a detailed mechanism of the nitrogen doping process of GO.

Li3PO4-Enriched SEI on Graphite Anode Boosts Li+ De-Solvation Enabling Fast-Charging and Low-Temperature Lithium-Ion Batteries.

Li+ de-solvation at solid-electrolyte interphase (SEI)-electrolyte interface stands as a pivotal step that imposes limitations on the fast-charging capability and low-temperature performance of lithium-ion batteries (LIBs). Unraveling the contributions of key constituents in the SEI that facilitate Li+ de-solvation and deciphering their mechanisms, as a design principle for the interfacial structure of anode materials, is still a challenge. Herein, we conducted a systematic exploration of the influence exerted by various inorganic components (Li2CO3, LiF, Li3PO4) found in the SEI on their role in promoting the Li+ de-solvation. The findings highlight that Li3PO4-enriched SEI effectively reduces the de-solvation energy due to its ability to attenuate the Li+-solvent interaction, thereby expediting the de-solvation process. Building on this, we engineer Li3PO4 interphase on graphite (LPO-Gr) anode via a simple solid-phase coating, facilitating the Li+ de-solvation and building an inorganic-rich SEI, resulting in accelerated Li+ transport crossing the electrode interfaces and interphases. Full cells using the LPO-Gr anode can replenish its 80 % capacity in 6.5 minutes, while still retaining 70 % of the room temperature capacity even at -20 °C. Our strategy establishes connection between the de-solvation characteristics of the SEI components and the interfacial structure design of anode materials for high performance LIBs.

Li3PO4‐Enriched SEI on Graphite Anode Boosts Li+ De‐Solvation Enabling Fast‐Charging and Low‐Temperature Lithium‐Ion Batteries

AbstractLi+ de‐solvation at solid‐electrolyte interphase (SEI)‐electrolyte interface stands as a pivotal step that imposes limitations on the fast‐charging capability and low‐temperature performance of lithium‐ion batteries (LIBs). Unraveling the contributions of key constituents in the SEI that facilitate Li+ de‐solvation and deciphering their mechanisms, as a design principle for the interfacial structure of anode materials, is still a challenge. Herein, we conducted a systematic exploration of the influence exerted by various inorganic components (Li2CO3, LiF, Li3PO4) found in the SEI on their role in promoting the Li+ de‐solvation. The findings highlight that Li3PO4‐enriched SEI effectively reduces the de‐solvation energy due to its ability to attenuate the Li+‐solvent interaction, thereby expediting the de‐solvation process. Building on this, we engineer Li3PO4 interphase on graphite (LPO−Gr) anode via a simple solid‐phase coating, facilitating the Li+ de‐solvation and building an inorganic‐rich SEI, resulting in accelerated Li+ transport crossing the electrode interfaces and interphases. Full cells using the LPO−Gr anode can replenish its 80 % capacity in 6.5 minutes, while still retaining 70 % of the room temperature capacity even at −20 °C. Our strategy establishes connection between the de‐solvation characteristics of the SEI components and the interfacial structure design of anode materials for high performance LIBs.

Reutilization of Silicon-Cutting Waste via Constructing Multilayer Si@SiO2@C Composites as Anode Materials for Li-Ion Batteries.

The rapid development of the photovoltaic industry has also brought some economic losses and environmental problems due to the waste generated during silicon ingot cutting. This study introduces an effective and facile method to reutilize silicon-cutting waste by constructing a multilayer Si@SiO2@C composite for Li-ion batteries via two-step annealing. The double-layer structure of the resultant composite alleviates the severe volume changes of silicon effectively, and the surrounding slightly graphitic carbon, known for its high conductivity and mechanical strength, tightly envelops the silicon nanoflakes, facilitates ion and electron transport and maintains electrode structural integrity throughout repeated charge/discharge cycles. With an optimization of the carbon content, the initial coulombic efficiency (ICE) was improved from 53% to 84%. The refined Si@SiO2@C anode exhibits outstanding cycling stability (711.4 mAh g-1 after 500 cycles) and rate performance (973.5 mAh g-1 at 2 C). This research presents a direct and cost-efficient strategy for transforming photovoltaic silicon-cutting waste into high-energy-density lithium-ion battery (LIB) anode materials.

Understanding the capacity increase mechanism in MoO2/C anodes for Lithium-Ion batteries

A facile and eco-friendly hydrothermal method, which does not employ surfactants, is used to synthesize MoO2/C as an anode material for lithium-ion batteries. Our approach overcomes kinetic barrier associated with the conversion reaction. The morphological analysis reveals that primary particles of MoO2/C are individual crystals forming secondary nanoparticles, which aggregate into tertiary micron-sized particles. This unique morphology plays a crucial role in enhancing the kinetics of lithium storage. It facilitates a gradual conversion reaction during the cycling process, even at ambient temperatures. The gradual nature of the conversion reaction of MoO2 upon cycling is clearly evidenced from the observed morphologies. These findings are thoroughly supported by thorough electrochemical investigations and analyses, which combined demonstrate the structural and electrochemical properties of the produced MoO2/C.

Exploring lithium storage performance of two-dimensional Sb2Si2Te6-derived composites with carbon coating through polyacrylonitrile pyrolysis

Two-dimensional materials have emerged as potential electrodes for lithium-ion storage, attributed to their adjustable band gap, abundant active sites, and efficient ion/electron transport properties. In this study, we synthesized Sb2Si2Te6 with layered structures via mechanical alloying and subsequent annealing, investigating its suitability as an anode material for lithium-ion batteries. We employed polyacrylonitrile (PAN) pyrolysis to encapsulate Sb2Si2Te6 in an amorphous carbon layer, resulting in the decomposition of Sb2Si2Te6 into Sb2Te3, Si and Te (denoted as Sb-Si-Te@C composite). This composite electrode exhibited excellent cycling stability, maintaining 505.6 mAh g−1 after 200 cycles (92.2% capacity retention), and enhanced rate performance compared to uncoated Sb2Si2Te6, which showed only 98.7 mAh g−1 after 200 cycles (33.1% capacity retention). Furthermore, the electrode expansion rate was significantly curtailed to 80.6% for Sb-Si-Te@C, compared to 174.3% for Sb2Si2Te6 after 100 cycles. This reduction indicates that the amorphous carbon layer enhances electron transfer during charging and discharging, effectively mitigating the electrode volume changes associated with cycling. These results underscore the potential of two-dimensional Sb2Si2Te6-derived composites as a promising anode material in lithium-ion batteries.

MXene as Promising Anode Material for High-Performance Lithium-Ion Batteries: A Comprehensive Review.

Broad adoption has already been started of MXene materials in various energy storage technologies, such as super-capacitors and batteries, due to the increasing versatility of the preparation methods, as well as the ongoing discovery of new members. The essential requirements for an excellent anode material for lithium-ion batteries (LIBs) are high safety, minimal volume expansion during the lithiation/de-lithiation process, high cyclic stability, and high Li+ storage capability. However, most of the anode materials for LIBs, such as graphite, SnO2, Si, Al, and Li4Ti5O12, have at least one issue. Hence, creating novel anode materials continues to be difficult. To date, a few MXenes have been investigated experimentally as anodes of LIBs due to their distinct active voltage windows, large power capabilities, and longer cyclic life. The objective of this review paper is to provide an overview of the synthesis and characterization characteristics of the MXenes as anode materials of LIBs, including their discharge/charge capacity, rate performance, and cycle ability. In addition, a summary of the potential outlook for developments of these materials as anodes is provided.

Compact homogeneous Si/SiC/C in-situ nanocomposite microspheres as anode materials for lithium-ion batteries

Compact homogeneous Si/SiC/C in-situ nanocomposite microspheres are synthesized by a procedure consisted of sol-gel, air calcination and magnesiothermic reduction processes. The components of Si, C, and SiC are all generated in situ and have the advantages of high dispersion and uniform distribution at the nanoscale level, which can maximize the conductivity and structural stability of nanocomposite microspheres when used as the anode materials for lithium-ion batteries. A series of samples with different compositions and morphologies are obtained by controlling the temperature in the air calcination step. Electrochemical tests reveal that the sample with the best comprehensive performance delivers an initial coulombic efficiency of 79.1 %, a reversible specific capacity of 1513 mAh g−1, and a capacity retention of 87.8 % after 200 cycles. The significantly enhanced electrochemical performance relative to the pure Si sample composed of irregular nanoparticles confirms that the method of synthesizing compact homogeneous materials through in-situ means is highly effective and promising for the fabrication of high-performance electrode materials.

Blackberry Seeds-Derived Carbon as Stable Anodes for Lithium-Ion Batteries.

The suitability of biocarbons derived from blackberry seeds as anode materials in lithium-ion batteries has been assessed for the first time. Blackberry seeds have antibacterial, anticancer, antidysentery, antidiabetic, antidiarrheal, and potent antioxidant properties and are generally used for herbal medical purposes. Carbon is extracted from blackberries using a straightforward carbonization technique and activated with KOH at temperatures 700, 800, and 900 °C. The physical characterization demonstrates that activated blackberry seeds-derived carbon at 900 °C (ABBSC-900 °C) have well-ordered graphene sheets with high defects compared to the ABBSC-700 °C and ABBSC-800 °C. It is discovered that an ABBSC-900 °C is mesoporous, with a notable Brunauer-Emmett-Teller surface area of 65 m2 g-1. ABBSC-900 has good electrochemical characteristics, as studied under 100 and 1000 mA g-1 discharge conditions when used as a lithium intercalating anode. Delivered against a 500 mA g-1 current density, a steady reversible capacity of 482 mA h g-1 has been achieved even after 200 cycles. It is thought that disordered mesoporous carbon with a large surface area account for the improved electrochemical characteristics of the ABBSC-900 anode compared to the other ABBSC-700 and ABBSC-800 carbons. The research shows how to use a waste product, ABBSC, as the most desired anode for energy storage applications.

Ladderlike polysilsesquioxanes derived dual-carbon-buffer-shell structural silicon as stable anode materials for lithium-ion batteries

Silicon-carbon (Si/C) composite materials have been proven to be one of the most promising anode materials for the next generation of lithium-ion batteries (LIBs) due to their high theoretical capacity. However, the substantial volume changes during alloying/dealloying processes have posed significant challenges to the working lifespan of Si-based anodes. In this study, we designed a dual-carbon-layer-structured Si composite anode material (DCS-Si). Using ladderlike polysilsesquioxanes as a precursor, we employed a zinc thermal reaction to internally reduce the Si–O–Si framework to Si0. Simultaneously, the phenyl groups directly connected to Si atoms served as a carbon source for the internally dense coating layer. The obtained product underwent further coating controllable pyrolysis reactions to form an external carbon coating layer. As anode for LIBs, DCS-Si delivered a reversible specific capacity exceeding 1000 mAh g−1. Even after 1350 cycles at a current density of 0.3 A g−1, the specific capacity remained above 500 mAh g−1. Moreover, even under a high current density of 3 A g−1, after nearly 1000 cycles, the capacity retention rate still exceeded 70%. Further testing of the full cell also indicated that DCS-Si is a highly promising high-energy-density anode, with potential applications in future commercial lithium-ion batteries.

Enhanced electrochemical performance of N, F co-doped and etched needle coke-based lithium-ion battery anode materials by NF3 plasma treatment

NF3 plasma treatments were used to improve the electrochemical properties of needle coke-based lithium-ion battery (LIB) anode materials. The effects of the NF3 plasma treatments on the chemical, structural, and morphological properties of the needle cokes were evaluated with various analyses, and simultaneous heteroatom doping coupled with surface etching was identified. With these effects, N and F functional groups and micropores were generated on the surfaces of the needle cokes. The NF3 plasma-modified needle cokes were analyzed with LIB performance tests, and considerable enhancements were observed in the discharge capacities, rate capabilities and cycling stabilities. The resulting nitrogen functional groups and micropores improved the lithium storage capacities and rates by providing lithium-ion adsorption sites. The fluorine functional groups enhanced the cycling stability by forming LiF-based SEI layers. These effects of the NF3 plasma treatment on the electrochemical properties were proven with analytical techniques, and mechanisms for the overall process were suggested based on the results. The NF3 plasma-treated needle cokes are promising materials for fast charging LIB anodes with high stabilities and competitive discharge capacities.