High-performance Lithium-ion Batteries Research Articles

Poly(Acrylic Acid)-Based Polymer Binders for High-Performance Lithium-Ion Batteries: From Structure to Properties.

Poly(acrylic acid) (PAA) and its derivatives have emerged as promising candidates for enhancing the electrochemical performance of lithium-ion batteries (LIBs) as binder materials. Recent research has focused on evaluating their ability to improve adhesion with silicon (Si) particles and facilitate ion transport while maintaining electrode integrity. Various strategies, including mixing modifications and copolymerization methods, are highlighted and the structural and physicochemical properties of these binders are examined. Additionally, the interaction mechanisms between PAA-based binders and active materials and their impact on key electrochemical properties such as initial Coulombic efficiency (ICE) and cycle stability are discussed. The findings underscore the efficacy of tailored PAA-based binders in enhancing the electrochemical properties of LIBs, offering insights into the design principles and practical implications for advanced battery materials. These advancements hold promise for developing high-performance lithium batteries capable of meeting future energy storage demands.

Triazine-Based Large-Sized Single-Crystalline Two-Dimensional Covalent Organic Framework for High-Performance Lithium-Ion Batteries.

A large-sized single crystalline 2D COFs with excellent crystallinity and stability was prepared through the traditional thermal solvent method. The electrochemical performance can be significantly enhanced using a straightforward hybrid approach that involves in situ growth of the 2D COFs on multi-walled carbon nanotubes (MWCNTs). Both the advantages of COFs and CNTs are mutually enhanced. The single-crystalline feature of the obtained COFs improves the structural integrity and brings excellent chemical and electrochemical stabilities for lithium-ion battery applications. The resultant COF-CNT core-shell hybrids greatly improved the conductivity and demonstrated excellent lithium-ion storage performance with a high capacity of 228 mAh g-1 (0.2 A g-1).

Electric Field and Nanocontact Effects in Metal-Organic Framework/Li6.4La3Zr1.4Ta0.6O12 Ionic Conductors for Fast Interfacial Lithium-Ion Transport Kinetics.

The slow ion transport kinetics inside or between the nanofillers in composite polymer electrolytes (CPEs) lead to the formation of lithium dendrites for solid-state lithium batteries. To address the critical issues, CPEs (U@UNL) composed of a UIO-66@UIO-66-NH2 (U@UN) core-shell heterostructure and Li6.4La3Zr1.4Ta0.6O12 (LLZTO) filler is designed. Due to the different band structures of the U@UN heterostructure, a built-in electric field is constructed to promote the transfer kinetics of carriers. Besides, the introduction of LLZTO facilitates the formation of a close nanometer contact interface between U@UN and LLZTO, reducing interface impedance and accelerating the lithium-ion transfer rate. As a benefit from the built-in electric field and the nanometer contact interface, U@UNL exhibits a wide electrochemical window of 5.17 V, a large lithium-ion transference number of 0.76, and a high ionic conductivity of 3.50 × 10-3 S cm-1. Consequently, the U@UNL electrolyte possesses excellent interfacial stability against Li metal after 1200 h at 0.1 mA cm-2 and shows a high specific capacity of 160.2 and 152.6 mAh g-1 at 0.5 and 1 C, respectively. This work proposes a complete strategy for building high-performance solid-state lithium batteries by a built-in electric field and nanometer contact interface between U@UN and LLZTO.

Effect of Various Carbon Coating Techniques on the Electrochemical Performance of Li4Ti5O12 Synthesized by Sol-Gel Method

This study aimed to prepare spinel carbon-coated Li4Ti5O12 (LTO/C) via sol-gel reaction and applied as a high-performance lithium-ion battery anode. The LTO powder was coated using various carbon sources, super P (SP), sugar and PVDF-assisted SP. The crystal structure, morphology, conductivity and electrochemical performance of the samples were examined using X-ray diffraction (XRD), Field Emission scanning electron microscopy (FESEM), Fourier Transform Infrared (FTIR) spectroscopy, Electrochemical Impedance Spectroscopy (EIS) and Cyclic Voltammetry/Charge-discharge (CV/CD), respectively. The XRD analysis results showed that the samples contain highly crystalline spinel LTO as the main phase and rutile as impurity. The FESEM image showed that SP covers the entire LTO surface more homogenous than sugar. However, sugar carbon makes roughness on the LTO surface. FTIR spectra showed that the coating using sugar and PVDF still contain hydrocarbon element. Electrochemical performance evaluations showed that SP carbon-coated-LTO possesses higher lithium diffusion and specific capacity than pure LTO, while sugar-coated-LTO shows the lowest specific capacity. Moreover, the SP carbon-coated-LTO sample high-rate capability has improved during full cell evaluation, delivering a discharge capacity of 249, 231, 211, 194, 58, and 23 mAhg-1 at the charge or discharge current density of 0.05, 0.1, 0.5, 1, 5, and 10 C, respectively.

Interface Engineering via Manipulating Solvation Chemistry for Liquid Lithium-Ion Batteries Operated≥100 °C.

High-performance and temperature-resistant lithium-ion batteries (LIBs), which are able to operate at elevated temperatures (i.e., >60 °C) are highly demanded in various fields, especially in military or aerospace exploration. However, their applications were largely impeded by the poor electrochemical performance and unsatisfying safety issues, which were induced by the severe side reactions between electrolytes and electrodes at high temperatures. Herein, with the synergetic effects of solvation chemistry and functional additive in the elaborately designed weakly solvating electrolyte, a unique robust organic/inorganic hetero-interphase, composed of gradient F, B-rich inorganic components and homogeneously distributed Si-rich organic components, was successfully constructed on both cathodes and anodes, which would effectively inhibit the constant decomposition of electrolytes and dissolution of transition metal ions, thus highly enhancing the high-temperature electrochemical performance. As a result, both cathodes and anodes, without compromising their low-temperature performance, can operate at temperatures ≥100 °C, with excellent capacity retentions of 96.1 % after 500 cycles and 93.5 % after ≥200 cycles, respectively, at 80 °C. Ah-level LiCoO2||graphite full cells with a cut-off voltage of 4.3 V also exhibited superior temperature-resistance with a capacity retention of 89.9 % at temperature as high as 120 °C. Moreover, the fully charged pouch cells exhibited highly enhanced safety, demonstrating their potentials in practical applications at ultrahigh temperatures.

Facile One-Pot Synthesis of Fe3O4 Nanoparticles Composited with Reduced Graphene Oxide as Fast-Chargeable Anode Material for Lithium-Ion Batteries.

To address the rapidly growing demand for high performance of lithium-ion batteries (LIBs), the development of high-capacity anode materials should focus on the practical perspective of a facile synthetic process. In this work, iron oxide nanoparticles (Fe3O4 NPs) in situ grown on the surface of reduced graphene oxide (rGO), denoted as Fe3O4 NPs@rGO, were prepared through a facile one-pot synthesis under the wet-colloidal conditions. The synthesized Fe3O4 NPs showed that uniform Fe3O4 NPs, with a size of around 9 nm, were distributed on the rGO surfaces. When applied as an anode material for LIBs, the Fe3O4 NPs@rGO anode revealed a high reversible capacity of 1191 mAh g-1 at 1.0 A g-1 after 200 cycles. It also exhibited excellent rate performance, achieving 608 mAh g-1 at a current density of 5.0 A g-1 over 500 cycles, with improved electronic and ionic conductivities due to the rGO template. This suggested that practically available anode materials can be developed through our one-pot synthesis by in situ growing the Fe3O4 NPs.

DNA: Novel Crystallization Regulator for Solid Polymer Electrolytes in High-Performance Lithium-Ion Batteries.

In this work, we designed a novel polyvinylidene fluoride (PVDF)@DNA solid polymer electrolyte, wherein DNA, as a plasticizer-like additive, reduced the crystallinity of the solid polymer electrolyte and improved its ionic conductivity. At the same time, due to its Lewis acid effect, DNA promotes the dissociation of lithium salts when interacting with lithium salt anions and can also fix the anions, creating more free lithium ions in the electrolyte and thus improving its ionic conductivity. However, owing to hydrogen bonding between DNA and PVDF, excess DNA occupies the lone pairs of electrons of the fluorine atoms on the PVDF molecular chains, affecting the conduction of lithium ions and the conductivity of the solid electrolyte. Hence, in this study, we investigated the effects of adding different DNA amounts to solid polymer electrolytes. The results show that 1% DNA addition resulted in the best improvement in the electrochemical performance of the electrolyte, demonstrating a high ionic conductivity of 3.74 × 10-5 S/cm (25 °C). The initial capacity reached 120 mAh/g; moreover, after 500 cycles, the all-solid-state batteries exhibited a capacity retention of approximately 71%, showing an outstanding cycling performance.

Structurally-constrained wrinkled NiO nanomembranes for high-performance lithium and sodium storage

In light of its exceptional capacity and safety features, nickel oxide (NiO) has emerged as a highly promising electrode material for advanced lithium-ion batteries (LIBs) and sodium-ion batteries (SIBs), which operate through conversion mechanisms, meeting the growing demand for high-efficiency rechargeable batteries. To address the capacity degradation challenges associated with NiO anodes, we present an innovative approach involving the fabrication of wrinkled NiO nanomembranes through magnetron sputtering deposition followed by thermal treatment. This distinctive three-dimensional, ultra-thin architecture integrates nanostructural and microstructural features that effectively reduce ionic diffusion distances and mitigate dimensional fluctuations during cycling, thereby markedly enhancing the electrochemical performance and reliability. Specifically, for lithium storage, these wrinkled NiO nanomembranes achieve an impressive reversible specific capacity of 773 mA h g−1 at 100 mA g−1, with excellent rate capability of 468 mA h g−1 at 5000 mA g−1 and long-term cycling performance, maintaining 523 mA h g−1 at 500 mA g−1 even after 1000 cycles. Likewise, for sodium storage, they exhibit a substantial reversible capacity of 288 mA h g−1 at 50 mA g−1 and retain 202 mA h g−1 at 200 mA g−1 after 100 cycles. These findings underscore the promising application of wrinkled NiO nanomembranes as robust anodic materials for high-performance LIBs and SIBs.

Facile Synthesis of flexible free-standing electrode for high energy density batteries by using PTMSP as binder

As a crucial component of the electrode, the binder greatly impacts battery performance. Herein, we report a novel binder, poly[1-(trimethylsilyl)-1-propyne] (PTMSP), which enables the construction of flexible free-standing electrodes for high performance lithium-ion batteries. The free-standing electrodes based on the PTMSP binder demonstrate remarkable cycling performance in various electrode materials, including LFP, S, and LTO, demonstrating significant potential for market application.

A Trimeric-Imidazole Ring-Containing Naphthoquinone Compound with Hydrogen Bonds for High-Performance Lithium-Ion Batteries

A Trimeric-Imidazole Ring-Containing Naphthoquinone Compound with Hydrogen Bonds for High-Performance Lithium-Ion Batteries

Utilizing copper waste to develop silicon-carbon anode materi als for lithium-ion batteries

This study dedicated to a novel method for synthesizing silicon-carbon (Si/C) and silicon dioxide-carbon (SiO2/C) nanocomposite anodes for lithium-ion batteries, utilizing industrial copper slags from the Almalyk Mining and Metallurgical Complex as a cost-effective source of SiO2. The synthesized nanocomposites address key challenges in lithium-ion battery anodes, including the volumetric expansion of silicon and its low conductivity, by leveraging the high lithiation capacity of silicon combined with the structural stability and conductivity of carbon. Amorphous SiO3 was extracted from copper slags via ammonium fluoride (NH4F) treatment and subsequently reduced to metallurgical-grade silicon through carbothermal reduction. The resulting SiO2/C and Si/C composites were thoroughly characterized using SEM, XRD, and electrochemical analyses, demonstrating improved electrochemical performance, favorable particle size distribution, and stability. This approach not only reduces material costs but also promotes environmental sustainability by repurposing industrial waste, offering promising candidates for high-performance lithium-ion battery anodes.

Fully sp2 Carbon-Conjugated Covalent Organic Frameworks with Multiple Active Sites for Advanced Lithium-Ion Battery Cathodes.

Covalent organic frameworks (COFs) hold great promise for rechargeable batteries. However, the synthesis of COFs with abundant active sites, excellent stability, and increased conductivity remains a challenge. Here, chemically stable fully sp2 carbon-conjugated COFs (sp2c-COFs) with multiple active sites are designed by the polymerization of benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-tricarbaldehyde) (BTT) and s-indacene-1,3,5,7(2H,6H)-tetrone (ICTO) (denoted as BTT-ICTO). The morphology and structure of the COF are precisely regulated from "butterfly-shaped" to "cable-like" through an in situ controllable growth strategy, significantly promoting the exposure and utilization of active sites. When the unique "cable-like" BTT-ICTO@CNT is employed as lithium-ion batteries (LIBs) cathode, it exhibits exceptional capacity (396 mAh g-1 at 0.1 A g-1 with 97.9 % active sites utilization rate), superb rate capacity (227 mAh g-1 at 5.0 A g-1), and excellent cycling performance (184 mAh g-1 over 8000 cycles at 2.0 A g-1 with 0.00365 % decay rate per cycle). The lithium storage mechanism of BTT-ICTO is exhaustively revealed by in situ Fourier transform infrared, in situ Raman, and density functional theory calculations. This work provides in-depth insights into fully sp2c-COFs with multiple active sites for high-performance LIBs.

Preparation of core-shell Si/C/graphene composite for high-performance lithium-ion battery anodes

One of the important objectives for the development of enhanced lithium-ion batteries is developing high-performance silicon-based anodes with durable operational capability. Herein, a three-dimensional graphene-decorated core-shell Si/C composite is fabricated by the in-situ polymerization of organic pyrrole molecule and pyrolysis process, in which the melamine formaldehyde resin is subtly used as three-dimensional porous framework to offer abundant loading area for the uniform dispersion of active silicon nanoparticles. Meanwhile, the core-shell structure deriving from polypyrrole in the composite can effectively buffer the volume change of silicon ingredient and avoid the direct contact with the electrolyte during the cycling process, leading to the improved structural stability and electrochemical performance. The outermost layer of graphene nanosheets is designed to enhance the electrical conductivity of the electrode. As a result, the synthesized Si/C/graphene composite exhibits a high capacity and excellent cycling performance. This work reveals that combining a three-dimensional carbon substrate with a core-shell structure might be a promising solution for anode materials with obvious volume transformation.

Monofluorinated Phosphate with Unique P-F Bond for Nonflammable and Long-Life Lithium-Ion Batteries.

Lithium-ion batteries (LIBs) with conventional carbonate-based electrolytes suffer from safety concerns in large-scale applications. Phosphates feature high flame retardancy but are incompatible with graphite anode due to their inability to form a passivated solid electrolyte interphase (SEI). Herein, we report a monofluorinated co-solvent, diethyl fluoridophosphate (DEFP), featuring a unique P-F bond that allows a trade-off between safety and electrochemical performance in LIBs. The P-F bond in DEFP weakens ion-dipole interactions with Li+ ions, lowering the desolvation barrier, and simultaneously reduces the lowest unoccupied molecular orbital (LUMO) of DEFP, promoting the formation of a robust and inorganic-rich SEI. Additionally, DEFP exhibits improved thermal stability due to both robust SEI and the inherent flame-retardant properties of the P-F bond. Consequently, the optimized DEFP-based electrolyte exhibits improved cyclability and rate capacity in LiNi0.8Co0.1Mn0.1O2 || graphite full cells compared with triethyl phosphate-based electrolytes and commercial carbonate electrolytes. Even at a low E/C ratio of 3.45 g Ah-1, the 1.16 Ah NCM811||Gr pouch cells achieve a high capacity retention of 94.2% after 200 cycles. This work provides a promising approach to decouple phosphate safety and graphite compatibility, paving the way for safer and high-performance lithium-ion batteries.

High-entropy chemistry enhanced pyrochlore (Y0.2La0.2Ce0.2Nd0.2Ca0.2)2Sn2O7 for high-performance lithium-ion battery anode

High-entropy chemistry enhanced pyrochlore (Y0.2La0.2Ce0.2Nd0.2Ca0.2)2Sn2O7 for high-performance lithium-ion battery anode

Tuning architectural synergy reactivity of nano-tin oxide on high storage reversible capacity retention of ammonium vanadate nanobelt array cathode for lithium-ion battery

Enabling ambient cycling stability of vanadium-based materials is of fundamental importance in the advancement of next generation electrodes for high-performance lithium-ion batteries. Although, extending these host layered nano-architectures illustrate the effective electrochemical activity by regulating the gallery space for fast Li+ storage, the reported structural integrity in terms of the cycling stability for vanadium-based cathodes is highly challenging. In present study, a series of NH4V4O10-SnO2 (NHV-SnO2) nanocomposite consisting of diverse contents of SnO2 (x: 5.0, 15.0 and 30.0 wt%) were synthesized through a three-step program based on sonochemical-calcination-hydrothermal treatment and employed as an advanced energetic material for lithium-ion battery cathodes. For the first time, understanding the impact of SnO2 loading on electrochemical reactions of NHV-based electrodes was regarded as an effective engineering strategy to optimize structural modulation and cell lifetime without distinct capacity fading. Notably, combination of NHV and SnO2 in optimum proportions not only enhances the specific surface area, but also expand buffer the volume change for lithium-ion intercalation/extraction. By this design, the assembled battery containing 15.0 wt% SnO2 illustrated stable capacities of 301.77 mAh g−1 (30 mA g−1) and 232.05 mAh g−1 (240 mA g−1) with capacity retention values as high as 97.94 % and 97.03 % for 50 cycles, respectively. Of note, the results described here could show a vital guidance toward designing better composite-based cathode material for energy storage devices.

Facile one-pot synthesis of Bi2S3 nanorod @ N, S co-doped carbon composite for high performance lithium ion batteries

Bismuth sulfide is favoured in lithium ion batteries due to its high specific capacity of 625 mAh/g. However, the Bi2S3 anode faces severe volume expansion problems during the lithium intercalation process, resulting in continuous electrode fragmentation and rapid degradation of lithium storage performance. In this study, Bi2S3 nanorod@N, S co-doped carbon composite prepared by a simple sintering method was used as the anode material for lithium ion batteries. 1D Bi2S3 nanorods with a length of 1 μm and a diameter of 50 nm were loaded in situ on 2D N, S co-doped carbon nanosheets. This unique structure can not only alleviate the volume change of bismuth sulfide, but also effectively shorten the diffusion distance of lithium ions, thereby improving the cycling stability and rate capability at the same time. The discharge capacity of Bi2S3@N, SC remained at 583.4 mAh g –1 after 400 cycles at 0.5 A g–1. Even at a high current density of 2 A/g, the discharge capacity of Bi2S3@N, SC still reached 374.3 mAh g –1. This simple method also can be extended to the preparation of other metal sulfide composites.

Porous silicon/carbon composites as anodes for high-performance lithium-ion batteries

Silicon anodes are promising for use in lithium-ion batteries. However, their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects. This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile (PAN) for a nitrogen-doped carbon coating, which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation. We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode. After treatment at 400 -, the PAN coating retains a high nitrogen content of 11.35%, confirming the presence of C―N and C―O bonds that improve the ionic-electronic transport properties. This treatment not only results in a more intact carbon layer structure, but also introduces carbon defects, and produces a material that has remarkable stable cycling even at high rates. When cycled at 4 A g−1, the anode had a specific capacity of 857.6 mAh g−1 even after 200 cycles, demonstrating great potential for high-capacity energy storage applications.

Nitrogen‑sulfur doped graphene-loaded SiO2/Co9S8 composites as anode materials for improved lithium storage

Heteroatom-doped graphene lamellae can effectively modulate the physical and chemical surface activities of Co9S8 materials. The addition of a second dopant atom, such as nitrogen (N) can further improve the composite properties. Herein, novel nitrogen‑sulfur double-doped graphene-loaded SiO2/Co9S8 composites (SiO2/Co9S8@NSG) were prepared by a one-step solvothermal method using polyethylene glycol as the carbon source and cobalt chloride hexahydrate as the cobalt source to yield a Deep Eutectic Solvents (DESs) system. The precursor was then obtained by adding tetraethyl silicate as the silicon source, thiourea as the sulfur source, and urea as the nitrogen source. The uniform distribution of Co9S8 in the N/S-doped graphene matrix formed graphene-coated SiO2 particles SiO2/Co9S8@NSG with high specific surface area, superior ionic conductivity, and elevated theoretical specific capacity. The N/S co-doped graphene matrix not only improved the electrical conductivity and hindered the adhesion of the particles, but also buffered the volume of the Co9S8 change and enhanced the electrochemical performance. The testing of SiO2/Co9S8@NSG composite as an anode for lithium-ion batteries (LIBs) revealed an impressive specific capacity with reversible capacity of 850 mA h/g after 900 cycles at a current density of 0.5 A/g and multiplicative capacity of 730 mA h/g at a current density of 0.1 A/g, confirming excellent cycling stability and a Coulombic efficiency close to 100 %. Overall, the proposed doping strategy looks promising for the development of high-performance LIBs.

Core–shell Fe2O3@MnO2 nanoring composites as anode materials for high-performance lithium-ion batteries

Core–shell Fe2O3@MnO2 nanoring composites as anode materials for high-performance lithium-ion batteries