Efficient Lithium-ion Batteries Research Articles

The Synergistic Effect of Cross-Linked and Electrostatic Self-Assembly Si/MXene Composites Anode for Highly Efficient Lithium-Ion Battery

Silicon is a promising anode material for high-performance lithium-ion batteries (LIBs), but its rapid capacity degradation has significantly hindered its large-scale application. In this study, we propose an in situ self-assembly polymerization method to fabricate a stable silicon-based anode by leveraging electrostatic self-assembly technology, in situ esterification, and amidation reactions. The incorporation of a cross-linked polymer, combined with the synergistic effects of electrostatic interactions between negatively charged MXene and positively charged silane-coupling-agent-modified silicon, offers a novel strategy for enhancing the electrochemical performance of LIBs. Notably, annealed electrodes with a 65 wt% nmSi-NH2/MXene ratio demonstrate outstanding electrochemical performance, achieving a capacity of 929.5 mAh g⁻¹ at a current density of 1 A g⁻¹ after 100 charge/discharge cycles. These findings suggest that the integration of cross-linked polymers and electrostatic self-assembly can significantly improve the intercalation and overall electrochemical performance of silicon anodes in lithium-ion batteries.

Towards Safer Li-Ion Batteries: A Study on Electrolyte Solvation and Dynamics with the Incorporation of Low Volatility Co-Solvents

Molecular dynamics (MD) simulations were employed to investigate how the content and type of co-solvents influence the solvation structure and transport properties of lithium ions (Li+) in electrolytes. Our focus was on lithium hexafluorophosphate (LiPF6) at a concentration of 1.0 M in a carbonate-based solvent composed of ethylene carbonate (EC) and dimethyl carbonate (DMC) with a 1:1 mixing ratio. Low-volatility co-solvents, including tetramethylene sulfone (TMS), dimethyl sulfoxide (DMSO), fluoroethylene carbonate (FEC), and succinonitrile (SN), were introduced into the electrolytic matrix at concentrations of 0, 10, 25, 50, 75, and 100 wt.%. Li+ dynamics were notably influenced by these factors. The highest Li+ transference number was observed at a 25 wt.% concentration for each co-solvent, particularly with 25 wt.% DMSO, resulting in the highest ionic conductivity (14.13 mS/cm) and Li+ transference number (0.47). In this system, the PF6 - anion refrains from joining the initial solvation shell of Li+. This is attributed to the higher donor number of DMSO compared to TMS, FEC, and SN, leading to a weakening of electrostatic interactions. These findings advance our comprehension of electrochemical principles in bulk electrolytes, providing insights for designing safer and more efficient lithium-ion batteries.

Multilayer Ti3C2Tx-loaded CoOHF composite structures for high-performance lithium-ion batteries

Research into new composites to enhance the performance of lithium-ion battery electrode materials has become a trendy area of study. Cobalt-based composites are particularly prominent due to their exceptional electrochemical performance and unique physicochemical properties. Additionally, Ti3C2Tx MXenes materials are anticipated to replace graphene and other carbonaceous materials since they possess an open structure and low lithium-ion diffusion barrier. In this work, we employed simple hydrothermal method to combine layered Ti3C2Tx with needle-shaped CoOHF. The resulting nanosheets showed an even dispersion of CoOHF in the surface, leading to a remarkable increase in specific capacity. Furthermore, Ti3C2Tx provided a higher number of lithium-ion active sites and improved the lithium-ion migration rate, while also ensuring the structure and stability of CoOHF. This composite material enables stable cycling for 1000 cycles at high current densities of 2 A g−1 and ultimately shows a large capacity of 802.4 mAh g−1 stably. Additionally, CoOHF/MXene composites display exceptional performance rate and cycling stability. This study highlights new feasible strategies for using multilayer Ti3C2Tx in lithium-ion batteries, along with metal hydroxyfluorides in new, highly efficient lithium-ion battery anode materials.

Enhancing the stability of Li2NiO2 cathode additive with polyborosiloxane coating for high-energy lithium-ion batteries

Li2NiO2 has garnered considerable interest as a Li-excess cathode additive for high-energy lithium-ion batteries (LIBs), attributed to its high irreversible capacity during the initial cycle and an operating voltage comparable with that of commercial cathode materials. However, its integration into practical applications is limited by its suboptimal cycling performance owing to moisture instability and gas evolution. To surmount these obstacles, we developed a hybrid surface coating strategy employing polyborosiloxane (PBS)—a structural derivative of polydimethylsiloxane (PDMS) synthesized with boric acid (H3BO3)—applied to a Li2NiO2 cathode additive. The bi-functional of the PBS layer enhances moisture resistance and ionic conductivity on the Li2NiO2 surface. A hydrophobic, elastic PDMS matrix offers conformal coverage, forestalling adverse moisture-induced side reactions. The introduction of H3BO3 into the PDMS matrix on the Li2NiO2 surface fosters the formation of Li–B–O bonds, thus augmenting the ionic conductivity of the coating. This innovative approach with the PBS layer significantly diminishes the interfacial resistance and improves the cycling performance of Li2NiO2 while preventing substantial structural degradation. In a full-cell configuration incorporating a PBS-coated Li2NiO2 cathode additive with a LiNi0.8Co0.1Mn0.1O2 cathode and a SiOx/Graphite anode, the enhanced energy density and sustained stable cycling performance exceed 300 cycles. This hybrid layer can aid in producing longer-lasting, more efficient LIBs that can fulfill the requirements for use in high-energy storage solutions.

Impact of dual nano-enhanced phase change materials on mitigating thermal runaway in lithium-ion battery cell

Thermal management remains a pivotal challenge in enhancing the safety and efficiency of lithium-ion batteries, especially under conditions prone to thermal runaway. This study investigates the performance of dual nano-enhanced phase change materials (NEPCM) in moderating extreme thermal events in battery cells. By integrating nanoparticles, specifically alumina and single-walled carbon nanotubes (SWCNT), into phase change materials (PCM), the study explores modifications in thermal behavior and phase change dynamics within a cylindrical battery enclosure. The research focuses on comparing the thermal performance of pure PCM and NEPCM, using two types of nanoparticles dispersed within the PCM matrix at various volume fractions. The findings indicate that NEPCM significantly improves heat transfer rates and accelerates the melting process. Specifically, NEPCM with 6 % SWCNT increases the melting temperature distribution by up to 15.27 % compared to pure PCM setups and enhances the liquid fraction by up to 66.54 % under similar conditions. The inclusion of SWCNT demonstrates a superior enhancement in thermal conductivity compared to alumina, leading to more effective heat absorption and dissipation. Liquid fraction analysis confirms that NEPCM configurations facilitate quicker and more uniform thermal behaviors, especially near the heat source. PCM1, positioned adjacent to the battery, exhibits an immediate increase in temperature and melting rate, significantly outperforming PCM2 in thermal regulation. This study underscores the potential of dual nano-enhanced PCM in improving the thermal management of lithium-ion batteries, particularly in scenarios at risk of thermal runaway. By optimizing the PCM formulation with nanoparticles, a robust solution is presented to control temperature spikes and improve battery safety and durability in challenging operational environments.

BC cone-shaped anodes for lithium-ion batteries

The efficiency of lithium-ion batteries (LIBs) depends upon anode materials possessing high capacity. In present study, we investigate boron carbide cone anode (BCC) for LIBs. The first-principles density functional theory (DFT) method is used to design anode materials based on BCC for application in LIBs. We found that the BCC shows negative Li adsorption energies. Our results also revealed the fast diffusions of Li ion on the BCC with the small energy barrier of 0.34 eV. The storage capacity of BCC system rank among the highest capacity of anodes for LIBs, with value of 785 mAh/g. The low average open-circuit voltage (OCV) value of BCC system indicates that this anode can handle a large operating voltage in LIBs.

The Enhancement of Recycling Processes Efficiency of Lithium Ion Batteries; A Review

The Enhancement of Recycling Processes Efficiency of Lithium Ion Batteries; A Review

Assessing performance in lithium-ion batteries recycling processes: A quantitative modeling perspective

In the shift toward sustainable energy solutions, the efficiency of lithium-ion battery (LIB) recycling within the supply chain is of paramount importance. This study evaluates the performance of LIB recycling processes by advancing a quantitative modeling approach. Through process simulations, a comprehensive assessment of pyrometallurgical and hydrometallurgical LIB recycling processes is presented by focusing on the key parameters that influence material recoveries and yields. Recycling efficiency indicators, accounting for the quantity and quality of recycled materials, are introduced and their dependence on the share of different battery chemistries and formats in the spent batteries feed is assessed via numerical simulations. A sensitivity analysis of process parameters identifies the unit operations mostly affecting the recycling performance, highlighting process criticalities. The model presented and its outcomes provide a valuable guide for stakeholders in the LIB industry, aiding informed decision-making to enhance sustainability and resource recovery in the ecosystem of electrochemical energy storage.

Derivation of porous cellulose propionate using hydrated hydroxyl groups and hydraulic pressure

This study aimed to enhance the thermal stability of microporous separators by introducing cellulose propionate (CP) as an innovative polymer matrix material, supplemented with glycerin as an additive. CP/glycerin composite membranes were created using hydraulic pressure techniques to reinforce essential separator properties. SEM analysis unveiled interconnected pores crucial for efficient ion transport, initiating water flux measurements at 5 bar. These measurements showcased improved mechanical strength, resulting in a porosity of 74.1 %. FT-IR spectroscopy illustrated CP-glycerin interactions, inducing plasticization and facilitating pore formation. Thermal Gravimetric Analysis (TGA) demonstrated superior thermal stability in CP/glycerin composite membranes compared to cellulose acetate (CA). Differential Scanning Calorimetry (DSC) revealed a slight reduction in thermal stability within a specific temperature range due to glycerin-induced plasticization effects. Nonetheless, the melting temperature (Tm) of CP/glycerin membranes increased to 188.4 °C, indicating heightened stability at elevated temperatures. Despite pressure-induced pore formation, CP/glycerin membranes exhibited enhanced thermal stability, suggesting reinforced molecular interactions. Overall, this study introduces a novel CP/glycerin composite membrane featuring improved thermal stability, enhanced strength, and controlled pore structures essential for efficient lithium-ion battery applications.

Layered CoS@NC in situ loaded onto Ti3C2Tx MXene as an efficient lithium-ion battery anode.

Due to its large capacity and relatively high conductivity, cobalt sulfide has been considered an excellent electrode material for lithium-ion batteries, but its extreme volume change during charging and discharging and lower conductivity than graphite limits its development. In this work, composite nanosheets of MXene and N-doped carbon-confined cobalt sulfide nanosheets (CoS@NC/MXene) were synthesized by growing the Co metal-organic framework of ZIF-67 onto MXene sheets, followed by sulfidation treatment. Different from normal ZIF-67 generally prepared in methanol, this work fabricates ZIF-67 in aqueous solution, which induces ZIF-67 to undergo some degree of hydrolysis and form more dispersed Co layered hydroxides mounted onto MXene. Also, the MXene incorporation imparts better water stability to ZIF-67(Co) and helps maintain its morphology during the sulfidation. CoS@NC/MXene has a conductive network supported by MXene and enhanced by NC, as well as a 3D hierarchical porous structure offered by the rational combination of its components. These favorable characteristics allow CoS@NC/MXene to deliver a capacity of 691 mA h g-1 at 200 mA g-1 in the 100th cycle and retain the specific capacity of 382 mA h g-1 at a higher current density of 8000 mA g-1.

Non-aqueous direct leaching using a reusable nickel-selective amic-acid extractant for efficient lithium-ion battery recycling

The demand for lithium-ion secondary batteries (LiBs) is rapidly increasing in pursuit of the Sustainable Development Goals. In particular, the recycling of nickel-based cathodes is attracting attention owing to the...

Reduced graphene oxide-encaged submicron-silicon anode interfacially stabilized by Al2O3 nanoparticles for efficient lithium-ion batteries.

Silicon-carbon composites have been recognized as some of the most promising anode candidates for advancing new-generation lithium-ion batteries (LIBs). The development of high-efficiency silicon/graphene anodes through a simple and cost-effective preparation route is significant. Herein, by using micron silicon as raw material, we designed a mesoporous composite of silicon/alumina/reduced graphene oxide (Si/Al2O3/RGO) via a two-step ball milling combined annealing process. Commercial Al2O3 nanoparticles are introduced as an interlayer due to the toughening effect, while RGO nanosheets serve as a conductive and elastic coating to protect active submicron silicon particles during lithium alloying/dealloying reactions. Owing to the rational porous structure and dual protection strategy, the core/shell structured Si/Al2O3/RGO composite is efficient for Li+ storage and demonstrates improved electrical conductivity, accelerated charge transfer and electrolyte diffusion, and especially high structural stability upon charge/discharge cycling. As a consequence, Si/Al2O3/RGO yields a high discharge capacity of 852 mA h g-1 under a current density of 500 mA g-1 even after 200 cycles, exhibiting a high capacity retention of ∼85%. Besides, Si/Al2O3/RGO achieves excellent cycling reversibility and superb high-rate capability with a stable specific capacity of 405 mA h g-1 at 3000 mA g-1. Results demonstrate that the Al2O3 interlayer is synergistic with the indispensable RGO nanosheet shells, affording more buffer space for silicon cores to alleviate the mechanical expansion and thus stabilizing active silicon species during charge/discharge cycles. This work provides an alternative low-cost approach to achieving high-capacity silicon/carbon composites for high-performance LIBs.

Li-Ion Battery Immersed Heat Pipe Cooling Technology for Electric Vehicles

Lithium-ion batteries, crucial in powering Battery Electric Vehicles (BEVs), face critical challenges in maintaining safety and efficiency. The quest for an effective Battery Thermal Management System (BTMS) arises from critical concerns over the safety and efficiency of lithium-ion batteries, particularly in Battery Electric Vehicles (BEVs). This study introduces a pioneering BTMS solution merging a two-phase immersion cooling system with heat pipes. Notably, the integration of NovecTM 649 as the dielectric fluid substantially mitigates thermal runaway-induced fire risks without requiring an additional power source. Comprehensive 1-D modeling, validated against AMESim (Advanced Modeling Environment for Simulation of Engineering Systems) simulations and experiments, investigates diverse design variable impacts on thermal resistance and evaporator temperature. At 10 W, 15 W, and 20 W heat inputs, the BTMS consistently maintained lithium-ion battery temperatures within the optimal range (approximately 27–34 °C). Optimized porosity (60%) and filling ratios (30–40%) minimized thermal resistance to 0.3848–0.4549 °C/W. This innovative system not only enhances safety but also improves energy efficiency by reducing weight, affirming its potential to revolutionize lithium-ion battery performance and address critical challenges in the field.

Construction of liquid metal nanoparticles-decorated on nitrogen-doped Ti3C2Tx MXene with flower-like structure for efficient lithium-ion batteries

Two-dimensional (2D) transition metal carbides, nitride compounds, or carbon-nitride compounds (MXenes), has attracted great attention as very popular energy storage materials, since their obvious characteristics compared with other energy storage materials, such as outstanding electrical conductivity, 2D lamellar structure, and abundant surface functional groups. These merits are further boosted by the construction of three-dimensional (3D) structures. Herein, we present a facile strategy of spontaneous converting 2D titanium carbide (Ti3C2Tx) MXene nanoflakes into 3D conductive frameworks of Ti3C2Tx /PANI (TP) composites, which is achieved by conducting oxidation-free polymerization of aniline on the surface of Ti3C2Tx MXene nanosheet, and then introducing liquid metal nanoparticles (LMNPs) with high theoretical capacity into the TP framework to build a 3D hydrangea macrophylla like Ti3C2Tx/PANI/LMNPs (TPL) composite. The TPL composites integrated the unique high-capacity speciality of LMNPs and the conductivity of the MXene framework. Lithium-ion batteries (LIBs) based on TPL electrodes exhibit higher specific capacity of 906.9 mAh g−1 at 0.1 A g−1, capacity retaining ratio of 96.44 % as well as a long cyclic stability (467.0 mAh g−1 after 1500 cycles at 5 A g−1).

Analytical computation of stress intensity factor for active material particles of lithium ion batteries

The stress intensity factor is a widely used parameter in linear elastic fracture mechanics to assess the stress field near the crack tip, and it is usually defined as the product between the remote stress, the square root of the crack length, and a geometric factor depending on the geometry of the test specimen, the size and location of the crack. However, this well-established expression cannot be used in case of non-constant stress distribution on crack surfaces, typically resulting from diffusive field. This work presents an analytical procedure to compute the stress intensity factor due to any kind of stress distribution that can be expressed as a polynomial. Firstly, the non-constant stress distribution is expressed as a polynomial. Then, the stress intensity factor is computed according to the principle of superposition of effects, as the sum of the stress components of each single polynomial grade and the corresponding geometric factors. The geometric factors for sphere with central and superficial cracks are determined using a finite element model, and closed-form expressions for these geometric factors are provided as functions of a normalized geometric parameter. These functions can be used in case of any stress loading and spherical geometry. The analytical procedure is specifically applied to assess the stress intensity factor caused by stress resulting from lithium diffusion in active material particles of lithium ions batteries electrodes. The results are compared with those obtained using a multiphysics finite element fracture model, showing good agreement and demonstrating the accuracy of the proposed analytical procedure. Then, the procedure presented in this work enables avoiding expensive multiphysics simulations and can be used to develop fast, accurate, and computationally efficient lithium ion batteries degradation models for the online estimation of the capacity decay with charge/discharge cycles.

Fast charging of lithium-ion battery using multistage charging and optimization with Grey relational analysis

Slow charging of batteries is one of the main challenges for the deployment of battery electric vehicles (BEVs) into market. There are multiple concerns with fast charging of lithium-ion batteries, such as rapid rise of surface temperature, accelerated aging, dendrite formation and lower charging efficiency. In order to achieve fast charging without compromising the aging of lithium-ion battery, one of the possible solutions is multistage constant current (MCC) charging. In this study, the charging levels of 5S-CC (five stage- constant current) charging (a type of MCC charging) has been optimized by using a new efficient approach Grey relational analysis (GRA) with Taguchi Design of experiment. It is also the part of the study to investigate CC-CV (Constant current-Constant voltage) charging and provide a comparative analysis with 5S-CC charging for creating an efficient lithium-ion battery charging technique for battery-powered vehicles. Panasonic NCR 18650PF lithium-ion batteries with LiNiCoAlO2 as the cathode and graphite as the anode having nominal capacity of 2750mAh were used in this study. The optimized 5S-CC charging takes 48.11 min compared to 73.48 min for CC-CV_0.05C charging, and the maximum temperature in CC-CV charging is 41.02 °C while in 5S-CC charging is 40.08 °C. The 5S-CC charging, generates significantly lower amount of surface heat up to 93.66 J while CC-CV_0.05C charging, generates 100.11 J, which may address the existing issue of rapid charging while extending battery life.

Effective coating of Si@NiO nanoflowers with nitrogen-doped wheat protein-derived biochar for efficient lithium-ion and lithium-sulfur batteries anode materials

As the most promising anode material for ultra-high specific capacity lithium-ion batteries, Si has been hindered from widespread use by large volume effects and limited electrical conductivity during cycling. In this study, NiO nanoflowers were coated onto the exterior of Si NPs by hydrothermal method. Si@NiO was then mixed and annealed with natural biomass gel extracted from moldy wheat to produce Si@NiO@Biochar ternary composites, which were prepared. Si NPs are the source of high specific capacity of anode materials. The carbon layer minimizes the electrode bulk effect and enhances cycling stability, while the NiO flowers expand the lithium-ion transport channel and reduce Si NPs bulk effect. Furthermore, the N element from wheat protein in the carbon layer enhances the electrical conductivity of the material. After 100 cycles at 0.1 A g−1 and 1000 cycles at 1 A g−1, the capacity of the electrode rose to 952.12 mAh g−1 and 1098.05 mAh g−1, respectively. The Si@NiO@Biochar material showed remarkable electrochemical stability at various current densities and the thickness grew by just 27.97% after 500 cycles. It can also be utilized in lithium-sulfur batteries because of its microporous structure and capacity to transport sulfur. The reversible capacity was 388.21 mAh g−1 after 70 cycles at 1 C. Biomass carbon from biomass gels coated on Si@NiO reduces biomass energy waste. This research is a significant step for commercializing Si anode materials and providing an eco-friendly new method for storing energy.

Strong metal oxide-support interaction in MoO2/N-doped MCNTs heterostructure for boosting lithium storage performance

The low-rate capability and fast capacity decaying of the molybdenum dioxide anode material have been a bottleneck for lithium-ion batteries (LIBs) due to low carrier transport, drastic volume expansion and inferior reversibility. Furthermore, the lithium-storage mechanism is still controversial at present. Herein, we fabricate a new kind of MoO2 nanoparticles with nitrogen-doped multiwalled carbon nanotubes (MoO2/N-MCNTs) as anode for LIBs. The strong chemical bonding (MoOC) endows MoO2/N-MCNTs a strong metal oxide–support interaction (SMSI), rendering electron/ion transfer and facilitate significant Li+ intercalation pseudocapacitance, which is evidenced by both theoretical computation and detailed experiments. Thus, the MoO2/N-MCNTs exhibits high-rate performance (523.7 mAh/g at 3000 mA g−1) and long durability (507.8 mAh/g at 1000 mA g−1 after 500 cycles). Furthermore, pouch-type full cell composed of MoO2/N-MCNTs anodes and commercial LiNi0.6Co0.2Mn0.2O2 (NCM622) cathodes demonstrate impressive rate performance and cyclic life, which displays an unparalleled energy density of 553.0 Wh kg−1. Ex-situ X-ray absorption spectroscopy (XAS) indicates the enhanced lithium-storage mechanism is originated from a partially irreversible phase transition from Li0.98MoO2 to Li2MoO4 via delithiation. This work not only provides fresh insights into the enhanced lithium-storage mechanism but also proposes new design principles toward efficient LIBs.

Architecting versatile NiFe2O4 coating for enhancing structural stability and rate capability of layered Ni-rich cathodes

Nickel-rich layered oxides are considered one of the most promising cathode materials for efficient lithium-ion batteries due to their high energy density and reasonable cost. However, at high cut-off voltage, the interfacial instability and structural degradation lead to severe capacity attenuation and poor thermal stability, which greatly hinder their large-scale applications. Herein, a multifunctional antispinel NiFe2O4 coated LiNi0.6Co0.2Mn0.2O2 (NCM@NFO) material is in-situ induced by co-precipitation and subsequent sintering, boosting the cycling stability of Ni-rich materials. Coupling in-depth characterizations (in-situ X-ray diffraction, etc.) with density functional theory calculations, the versatility of the NFO coating has been revealed. Including suppressing the transition metal dissolution, preventing the unwanted phase transition, inhibiting the oxygen vacancy generation, and stabilizing the crystal structure of the NCM by forming an M-O-N bonding network. More importantly, attributing to the high ion/electron conductivity of the NFO layer, the Li+ transport kinetics between NCM@NFO particles have been facilitated. Benefitting from the collaborative effect of the protective NFO coating, the optimized 2 wt% NFO@NCM (NCM@NFO-2) sample achieves higher capacity retention (81.25 vs 67.88% after 200 cycles) at high voltages (2.75 ∼ 4.5 V@0.5C) and more excellent rate capabilities (109.86 vs 49.52 mAh·g−1 at 10C), as well as impressive capacity retention of 81.72% after 100 cycles (at 60 °C@1C). Constructing a versatile bimetallic oxide protective layer at the secondary particle surface of layered oxides provides an effective strategy for Ni-rich cathodes towards high-energy, long-duration, and safe lithium ion batteries.

A novel lithium-ion battery capacity prediction framework based on SVMD-AO-DELM

Accurate and efficient lithium-ion battery capacity prediction plays an important role in improving performance and ensuring safe operation. In this study, a novel lithium-ion battery capacity prediction model combining successive variational mode decomposition (SVMD) and aquila optimized deep extreme learning machine (AO-DELM) is proposed. Firstly, SVMD is used to divide capacity signal and it improves short-term trend prediction, especially for capacity growth that occurs during the degradation process. Secondly, the DELM network outperforms other networks in efficiently extracting time-dependent features, and it is more accurate than other standard ELM-based methods. The AO algorithm is used to find the parameters of the DELM training process for the problem of sensitivity to initial weights. Finally, experiments are conducted to validate the predictive performance of the proposed model based on NASA and CALCE lithium-ion batteries sequences. The MAE (0.0066Ah, 0.0044Ah), RMSE (0.0113Ah, 0.0078Ah), MAPE (0.44%, 0.82%) are effectively reduced, and the R2 (98.94%, 99.87%) is better than the prediction performance of other hybrid models.