High-performance Lithium-ion Batteries Research Articles

Fluorine-Doping Carbon-Modified Si/SiOx to Effectively Achieve High-Performance Anode.

To address the significant challenges encountered by silicon-based anodes in high-performance lithium-ion batteries (LIBs), including poor cycling stability, low initial coulombic efficiency (ICE), and insufficient interface compatibility, this work innovatively prepares high-performance Si/SiOx@F-C composites via in situ coating fluorine-doping carbon layer on Si/SiOx surface through high-temperature pyrolysis. The Si/SiOx@F-C electrodes exhibit superior LIB performance with a high ICE of 79%, exceeding the 71% and 43% demonstrated by Si/SiOx@C and Si/SiOx, respectively. These electrodes also show excellent rate performance, maintaining a capacity of 603 mAhg-1 even under a high current density of 5000 mAg-1. Notably, the Si/SiOx@F-C electrode sustains a high reversible capacity of 829 mAh g-1 at 1000mA g-1 over 1400 cycles, and 588 mAhg-1 at 3000 mAg-1 even over 2400 cycles, capacity retention of up to 82.12%. Comprehensive characterization and analysis of the fluorine-doped carbon layer reveal its role in enhancing electrical conductivity and preventing structural degradation of the material. The abundant fluorine in the coating layer significantly increases the LiF concentration in the solid electrolyte interface (SEI) film, improving interfacial compatibility and overall lithium storage performance. This method is both straightforward and effective, providing a promising blueprint for the broader application of Si-based anodes in advanced lithium batteries.

N, P co-Doped Hard Carbon Anodes for High-Performance Lithium-Ion Batteries with Enhanced Capacity Retention and Cycle Stability.

Compared to the traditional graphite anode, heteroatom-doped polymer carbon materials have high capacity retention due to their high porosity and porous structure. Therefore, they have great potential for application in lithium-ion battery (LIB) anodes. In this work,an N, P co-doped precursor polymer material (MBPp), synthesized via a one-pot method using bisphenol-A (C-source), melamine (N-source), and 9,10-Dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (P-source). The resulting N, P-co-doped hard carbon materials (MBPs) were prepared at various pyrolysis temperatures, yielding microporous, mesoporous, and macroporous structures. MBP materials demonstrated excellent electrochemical performance as LIB anodes. Notably, MBP-900 achieved a reversible capacity of 262 mAh g-1 at 1000 mA g-1 (in 0.005-2.0 V voltage range) with a capacity retention rate of 97.2% after 1000 cycles. These findings highlight the significance of MBP materials, which possess numerous defects, large layer gaps, and excellent cycle stability, in advancing the development of polymer anode materials for LIBs.

Robust, High-Temperature-Resistant Polyimide Separators with Vertically Aligned Uniform Nanochannels for High-Performance Lithium-Ion Batteries.

Separator is an essential component of lithium-ion batteries (LIBs), playing a pivotal role in battery safety and electrochemical performance. However, conventional polyolefin separators suffer from poor thermal stability and nonuniform pore structures, hindering their effectiveness in preventing thermal shrinkage and inhibiting lithium (Li) dendrites. Herein, we present a robust, high-temperature-resistant polyimide (PI) separator with vertically aligned uniform nanochannels, fabricated via ion track-etching technology. The resultant PI track-etched membranes (PITEMs) effectively homogenize Li-ion distribution, demonstrating enhanced ionic conductivity (0.57 mS cm-1) and a high Li+ transfer number (0.61). PITEMs significantly prolong the cycle life of Li/Li cells to 1200 h at 3 mA cm-2. For Li/LiFePO4 cells, this approach enables a specific capacity of 143 mAh g-1 and retains 83.88% capacity after 300 cycles at room temperature. At 80 °C, the capacity retention remains at 85.92% after 200 cycles. Additionally, graphite/LiFePO4 pouch cells with PITEMs display enhanced cycling stability, retaining 73.25% capacity after 1000 cycles at room temperature and 78.41% after 100 cycles at 80 °C. Finally, PITEMs-based pouch cells can operate at 150 °C. This separator not only addresses the limitations of traditional separators, but also holds promise for mass production via roll-to-roll methods. We expect this work to offer insights into designing and manufacturing of functional separators for high-safety LIBs.

Dual active sites of N-rich triptycene-based 2D conductive metal–organic framework with 3D extended structures in high-performance lithium-ion batteries

Two-dimensional conductive metal–organic frameworks (2D c-MOFs) have attracted much attention in energy storage due to their special conjugated structures and electronic properties. However, the insufficient exposure of the active site due to layer stacking and the non-redox-active ligand molecules are detrimental to the specific capacity. In this study, a nitrogen-rich triptycene-based 2D c-MOF (M−TH5) with vertical extension was synthesized for the first time as an anode material. The triptycene-based ligand structure confers a 3D extension of the MOF alleviating the stacking problem and allowing full exposure of its active site. Furthermore, M−TH5 has a dual redox center (TH5 and MO4 units containing N sites), which can provide additional lithium storage sites. Expectedly, Mn-TH5 compared to Co-TH5 exhibits higher initial capacity (486.3 mAh·g−1 at 100 mA·g−1) and excellent long-term cycling stability (capacity retention of 91.9 % at 500 mA·g−1 after 400 cycles). Experimentally and computationally, the flower-like morphology and the nitrogen-rich system with three-dimensional (3D) expansion have more exposed active sites to facilitate Li+/e- transport. This finding provides new opportunities to improve anode material properties by integrating multiple active centers into 2D c-MOF

How dispersed LLZTO enhances ionic conductivity in LiFePO4 composite cathodes for solid-state batteries

To improve the ionic conductivity of the LiFePO4 cathode for high-performance solid-state lithium-ion batteries, we incorporated the chemically stable and ion-conductive Li6.75La3Zr1.75Ta0.25O12 (LLZTO) into the cathode. We discovered that the impact of this incorporation on enhancing conductivity was influenced by how well the LLZTO particles were dispersed. A solid-state battery constructed with the LiFePO4 cathode without any LLZTO incorporated exhibited an initial capacity of 146 mAh g−1 at 0.2C, with a retention of 26 % after 100 cycles of charge-discharge. When the cathode was incorporated with LLZTO particles in their original agglomerated state, the initial capacity remained similar to the pristine one, but the retention decreased to <20 %. However, when LLZTO was well-dispersed during incorporation, the initial capacity increased to 160 mAh g−1, and retention improved to over 95 %. The difference in the effectiveness of incorporating dispersed and agglomerated LLZTO on the electrochemical performance has been clarified to be mainly related to the polarization of Li+ during transport in the cathodes. This was elucidated by numerical simulations based on finite element analysis, which revealed that incorporating LLZTO agglomerates leads to a deficiency of Li+ transport in specific regions within the LiFePO4 cathode and non-uniform Li+ transport through LLZTO, resulting in reduced overall cathode conductivity and battery performance.

In situ construction of an electron-withdrawing polymer coating layer on NCM811 interface for high-performance lithium-ion batteries

In situ construction of an electron-withdrawing polymer coating layer on NCM811 interface for high-performance lithium-ion batteries

Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Ammonium-driven modulation of 1T-MoS2 structure and composite with graphene: A pathway to high-performance lithium-ion battery anodes

Ammonium-driven modulation of 1T-MoS2 structure and composite with graphene: A pathway to high-performance lithium-ion battery anodes

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.