High-performance Lithium-ion Batteries Research Articles

Enhanced High-Temperature Cycling Stability of Garnet-Based All Solid-State Lithium Battery Using a Multi-Functional Catholyte Buffer Layer

HighlightsThermally stable catholyte buffer layer was fabricated via incorporating a multi-functional flame-retardant triphenyl phosphate additive into poly(ethylene oxide).The optimized catholyte buffer layer enabled thermal and electrochemical stability at interface level, delivering comparable cycling stability of garnet-based all solid-state lithium battery, i.e., capacity retention of 98.5% after 100 cycles at 60 °C, and 89.6% after 50 cycles at 80 °C.Exceptional safety performances were demonstrated, i.e., safely cycling behavior at temperature up to 100 °C and spontaneous fire-extinguishing ability.

MOF-silsesquioxane synergistic modified hybrid porous membrane for high-performance and high-safety lithium battery

As an emerging alternative separator, electrospun PVDF-HFP (polyvinylidene fluoride-hexafluoropropylene) has been widely studied in lithium battery over the years. However, some shortcomings of PVDF-HFP have limited its further application, such as, poor thermal stability, mechanical and electrochemistry properties. In this work, the cage-like silsesquioxanes (CSQ) and metal–organic-framework (MOF) were chemically bound to PVDF-HFP, and a modified hybrid fibrous membrane with hierarchical pore was fabricated. These hybrid groups were successfully introduced into the backbone of PVDF-HFP, which was not only demonstrated by characterization of their chemical structures, and also demonstrated by morphologies and elemental mass spectrometry with the help of scanning electron microscopy/energy dispersive spectroscopy (SEM/EDS). Due to the incorporation of these hybrid groups, the membrane exhibited high thermal stabilities and good flame-retardant performance, and could also play an important role in regulating and improving the migration property of lithium ions and interface performance between electrolyte and electrodes during battery charging/discharging process.

Inert salt-assisted solvent-free synthesis of high-entropy oxide towards high-performance lithium-ion batteries

High-entropy oxide (HEO) is a promising anode material for lithium-ion battery (LIB) due to the synergistic effect of various metal species. Conventional HEO preparations typically involve a solid-state route or liquid-phase mixing followed by high-temperature calcination, leading to either a small surface area or environmental contamination. Herein, a novel, facile solvent-free preparation of HEOs is introduced, applying inert salt, NaCl, as an easily removable, eco-friendly and recyclable template. This approach realizes high-purity porous HEO (NPHEO) with specific surface area (28.1 m2 g−1) for high-performance lithium-ion batteries. With the enhanced electrochemical kinetics, the NPHEO anodes deliver a high reversible specific capacities of 1143.6 at 0.2 A/g. In addition, the NPHEO-based cells exhibit a desirable rate capability of 315.7 mAh/g at 5 A/g. At 1 A/g the cell delivers a good cyclability of 71.8 % capacity retention over 600 cycles, corresponding to an average coulombic efficiency of above 99.94 % per cycle. Ex-situ X-ray diffraction and in-situ electrochemical impedance spectroscopy experiments further probe the structural evolution and electrochemical behavior during lithiation/delithiation, confirming the structural stability and fast electrochemical kinetics of NPHEO. The proposed advanced synthesis approach offers a new platform for the preparation of HEOs with high quality.

In Situ Construction of a Polymer Coating Layer on the LiNi0.8Co0.1Mn0.1O2 Cathode for High-Performance Lithium-Ion Batteries.

Lithium-ion batteries (LIBs) are known for their high energy density but exhibit poor cyclic stability and safety risks due to side reactions between the electrode and electrolyte. To address these issues, a novel approach involving construction of a polymer coating layer (PCL) via in situ self-polymerization using 2,2,3,4,4,4-hexafluorobutyl methacrylate (HFBM) as an electrolyte additive on the cathode is proposed. The PCL endows the electrolyte with a high onset oxidation potential (4.78 V) and lithium-ion transference number (0.52). The uniform and robust in situ constructed PCL can effectively inhibit the severe irreversible side reactions and suppress harmful reactions, thus providing a protective barrier against degradation. The resulting Li||LiNi0.8Co0.1Mn0.1O2 batteries exhibit an improved discharge capacity retention of 80% at 1C over 100 cycles. These results demonstrate that the in situ self-polymerization strategy holds promising potential for enhancing LIB performance and long-term stability, especially when high-voltage cathode materials are used.

Microstructured pebble stone like Ni-NiO composite as anode of high-performance lithium-ion batteries

Ni-NiO electrodes were synthesized via thermal oxidation of pure nickel powder and evaluated as anode of lithium-ion batteries (LIBs). The composite synthesized at 600˚C, 800˚C, and 1000˚C exhibited nanochips, crushed gravel stone, and pebble stone-like morphology, respectively. The nanochips- and crushed gravel stone featured-like electrodes exhibited erratic behavior, and specific capacity faded rapidly from 754.49 mAh g-1 and 101.12 mAh g-1 to 464.04 mAh g-1 and 9.55 mAh g-1, respectively over 10th cycle at a current rate of 1C as the electrode experiences internal short circuit. The pebble stone-like Ni-NiO electrode exhibited improved and stable cyclic performance with 1st discharge capacity of 365.17 mAh g-1 and reduced to 67.42 mAh g-1 even after 40th cycle at 1C current rate. The improved electrochemical performance of composite Ni-NiO with a pebble stone-like feature can be attributed to the mechanical stability of the electrode, which can buffer volume expansion, and the presence of more nanoparticles on the electrode surface allows more interaction with Li+.

High-performance solid-state Li-ion batteries enabled by homogeneous, large-area ferroelectric PVDF-TrFE solid polymer electrolytes via horizontal centrifugal casting method

Solid polymer electrolytes (SPEs) have emerged as promising alternatives for enhancing the safety features of lithium-ion batteries (LIBs) while remaining compatible with established LIB manufacturing processes. However, a persistent challenge has been the relatively limited yield achieved via traditional fabrication techniques such as solution casting and doctor blade methods. In this study, we present a novel strategy to produce extensive and uniform films of solid polymer electrolytes using a ferroelectric polyvinylidene fluoride-trifluoroethylene (PVDF-TrFE) polymer. This approach employs horizontal centrifugal casting (HCC), a technique hitherto unutilized for SPE production. The substantial centrifugal forces generated during the HCC process yield SPE films characterized by uniform thickness across the surface and elevated ionic conductivity at ambient temperature. Compared to conventional solution casting techniques, the Li//Li cell featuring the SPE derived from HCC manifests stable electrochemical performance and increased cycle endurance. Additionally, a full cell incorporating a Li iron phosphate cathode displays consistent electrochemical behavior at room temperature. Notably, a 3 × 4 cm2 pouch cell maintains its performance attributes even under mechanical stress conditions such as folding and punching. These findings underscore the potential effectiveness of employing the HCC method in the development of high-performance SPE-based LIB systems.

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.

LiMn2O4 – MXene nanocomposite cathode for high-performance lithium-ion batteries

Lithium-ion batteries still face many significant challenges for practical applications, including low discharge capacity, cyclic efficiency, initial coulombic efficiency, areal performance, volumetric capacity, and high materials cost. LiMn2O4 (LMO) characterized by its spinel structure, is a highly appealing cathode material attributed to its remarkable energy density, cost-effectiveness, and minimal environmental impact. However, LMO experiences capacity fading while shifting between the C rates. The 2D material MXene with its very high electrical conductivity functions as a conductive matrix, allowing for volume expansion and contraction during Li+ intercalation while retaining structural and electrical connections. In this work, the LiMn2O4-MXene (LMO-MX) nanocomposite was synthesized by a cost-effective microwave-assisted chemical coprecipitation and examined. Structural characterization confirmed the effective synthesis of LMO-MX nanocomposite. Electrochemical characterizations demonstrate that LMO-MX nanocomposites exhibit outstanding electrochemical performance, with an initial specific discharge capacity of roughly 111 mAhg-1 at 0.1 C, and capacity retention of 95.2% after 100 cycles in contrast to the pristine LMO which gave an initial specific discharge capacity of 97 mAhg-1 and cyclability of 89.3%. The incorporation of MXenes enhances the electrochemical characteristics of LMO cathode material and implies that MXene-based nanocomposites might be useful as cathodes in high-performance lithium-ion batteries.

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.

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

Glycerol solvothermal synthesis of high-performance lithium-ion battery cathode materials with surface oxygen vacancies

Glycerol solvothermal synthesis of high-performance lithium-ion battery cathode materials with surface oxygen vacancies

Doping Strategy in Developing Ni-Rich Cathodes for High-Performance Lithium-Ion Batteries

Doping Strategy in Developing Ni-Rich Cathodes for High-Performance Lithium-Ion Batteries

Al- and Nb-Comodified Ni-Rich NCM Cathode for High-Performance Lithium-Ion Batteries

Al- and Nb-Comodified Ni-Rich NCM Cathode for High-Performance Lithium-Ion Batteries

MOF-Derived Bimetallic Selenide CoNiSe2 Nanododecahedrons Encapsulated in Porous Carbon Matrix as Advanced Anodes for Lithium-Ion Batteries.

Transition metal selenides have received considerable attention as promising candidates for lithium-ion battery (LIB) anode materials due to their high theoretical capacity and safety characteristics. However, their commercial viability is hampered by insufficient conductivity and volumetric fluctuations during cycling. To address these issues, we have utilized bimetallic metal-organic frameworks to fabricate CoNiSe2/C nanodecahedral composites with a high specific surface area, abundant pore structures, and a surface-coated layer of the carbon-based matrix. The optimized material, CoNiSe2/C-700, exhibited impressive Li+ storage performance with an initial discharge specific capacity of 2125.5 mA h g-1 at 0.1 A g-1 and a Coulombic efficiency of 98% over cycles. Even after 1000 cycles at 1.0 A g-1, a reversible discharge specific capacity of 549.9 mA h g-1 was achieved. The research highlights the synergistic effect of bimetallic selenides, well-defined nanodecahedral structures, stable carbon networks, and the formation of smaller particles during initial cycling, all of which contribute to improved electronic performance, reduced volume change, increased Li+ storage active sites, and shorter Li+ diffusion paths. In addition, the pseudocapacitance behavior contributes significantly to the high energy storage of Li+. These features facilitate rapid charge transfer and help maintain a stable solid-electrolyte interphase layer, which ultimately leads to an excellent electrochemical performance. This work provides a viable approach for fabricating bimetallic selenides as anode materials for high-performance LIBs through architectural engineering and compositional tailoring.

Si@Fe3O4/AC composite with interconnected carbon nano-ribbons network for high-performance lithium-ion battery anodes

Si-based anode materials have a relatively high theoretical specific capacity and low operating voltage, greatly enhancing the energy density of rechargeable lithium-ion batteries (LIBs). However, their practical application is seriously hindered by the instability of active particles and anode electrodes caused by the huge swelling during cycling. How to maintain the stability of the charge transfer network and interface structure of Si particles is full of challenges. To address this issue, we have developed a novel Si@Fe3O4/AC/CNR anode by in-situ growing one-dimensional high elastic carbon nano-ribbons to wrap Si nanoparticles. This special structure can construct fast channels of electron transport and lithium ion diffusion, and stabilize the surface structure of Si nanoparticles during cycling. With these promising architectural features, the Si@Fe3O4/AC/CNR composite possesses a high specific capacity of 1279.4 mAh/g at 0.5 A/g, and a superior cycling life with 80 % capacity retention after 700 cycles. Even at a high current density of 20.0 A/g, the composite still delivers a capacity of 621.2 mAh/g. The facile synthetic approach and high performance of Si@Fe3O4/AC/CNR anodes provide practical insight into advanced anode materials with large volume expansion for high-energy-density LIBs.

High-Performance Lithium-Ion Batteries with High Stability Derived from Titanium-Oxide- and Sulfur-Loaded Carbon Spherogels.

This study presents a novel approach to developing high-performance lithium-ion battery electrodes by loading titania-carbon hybrid spherogels with sulfur. The resulting hybrid materials combine high charge storage capacity, electrical conductivity, and core-shell morphology, enabling the development of next-generation battery electrodes. We obtained homogeneous carbon spheres caging crystalline titania particles and sulfur using a template-assisted sol-gel route and carefully treated the titania-loaded carbon spherogels with hydrogen sulfide. The carbon shells maintain their microporous hollow sphere morphology, allowing for efficient sulfur deposition while protecting the titania crystals. By adjusting the sulfur impregnation of the carbon sphere and varying the titania loading, we achieved excellent lithium storage properties by successfully cycling encapsulated sulfur in the sphere while benefiting from the lithiation of titania particles. Without adding a conductive component, the optimized material provided after 150 cycles at a specific current of 250 mA g-1 a specific capacity of 825 mAh g-1 with a Coulombic efficiency of 98%.

Cellulose-derived carbon aerogel from rice straw for high-performance lithium-ion battery anodes

Cellulose-derived carbon aerogel from rice straw for high-performance lithium-ion battery anodes

Residual alkali-evoked cross-linked polymer layer for anti-air-sensitivity LiNi0.89Co0.06Mn0.05O2 cathode

High-energy density lithium-ion batteries (LIBs) with layered high-nickel oxide cathodes (LiNixCoyMn1−x−yO2, x ≥ 0.8) show great promise in consumer electronics and vehicular applications. However, LiNixCoyMn1−x−yO2 faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air. To address this issue, we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface. Through the neutralization of polyacrylic acid (PAA) with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane (KH550), a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi0.89Co0.06Mn0.05O2 (NCM) cathode. Our characterization and measurements demonstrate its effectiveness. The NCM material exhibits impressive cycling performance, retaining 88.4% of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g−1 at 10 C. Importantly, this layer on the NCM efficiently suppresses unfavorable phase transitions, severe electrolyte degradation, and CO2 gas evolution, while maintaining commendable resistance to air exposure. This surface modification strategy shows widespread potential for creating air-stable LiNixCoyMn1−x−yO2 cathodes, thereby advancing high-performance LIBs.

Carbon-coated Ni2P nanoparticles coated on CNTs synthesized by an in-situ solid-state method for high-performance hybrid supercapacitors and lithium-ion batteries

The pursuit of electrode materials with excellent performance in both supercapacitors and lithium-ion batteries holds the potential to streamline the construction of hybrid electrochemical energy storage systems and contribute to cost reduction. In this paper, we introduce a novel nanocomposite—carbon-coated Ni2P nanoparticles coated on CNTs (CNTs@(Ni2P@C))—via an in-situ one-step solid-state method. This design not only prevents the aggregation of Ni2P nanoparticles with a size of 5–8 nm but also mitigates its volume change during charging and discharging cycles. Simultaneously, it establishes a rapid electron transfer pathway between CNTs and Ni2P nanoparticles, enhancing the electron transport kinetics within the synthesized nanocomposite. The synthesized CNTs@(Ni2P@C) nanocomposite exhibits high performance in both SCs and LIBs. An ultra-high specific capacity of 378.5 mAh g−1 (2725.2 F g−1) at 1 A g−1 and a good rate capacity (189.3 mAh g−1 at 20 A g−1) are achieved when used in supercapacitors. The hybrid supercapacitor device assembled using the synthesized nanocomposite exhibits a high specific capacity of 84.3 mAh g−1 at 1 A g−1 and excellent capacity retention of 92 % after 10,000 cycles. A high energy density of 67.47 Wh kg−1 can be delivered at a power density of 0.84 kW kg−1. When used in LIBs, the synthesized nanocomposite exhibits a reliable reversible specific capacity of 329 mAh g−1 at 0.1 A g−1 after 100 cycles and a high capacity retention of 90 % after 5000 cycles at 2.0 A g−1. The proposed in-situ solid-state method and the synthesized CNTs@(Ni2P@C) nanocomposite will strongly promote the development of difunctional electrode materials for supercapacitors and lithium-ion batteries.