Improved Battery Performance Research Articles

Electrospun Multiscale Structured Nanofibers for Lithium‐Based Batteries

Abstract Electrospun is a unique technique for the fabrication of multiscale structured nanofibers (MSNFs), which can be used as functional units for improving the performance of lithium‐based batteries. This review systematically examines how MSNFs, including core–shell, hollow porous, multichannel, wire‐in‐tube, tube‐in‐tube, and hierarchical nanofibers, effectively improve battery performance as components in lithium‐based batteries. The application of aforementioned MSNFs and their chemical modification contributes to the development of lithium‐based batteries with high energy density and enhanced safety when used as electrodes, separators, and electrolytes. Specifically, MSNFs are used to derive electrodes and electrolytes that improve electron/ion transfer rates, increase the utilization ratio of active materials, suppress dendrite growth, and mitigate volume expansion, enabling fast and stable electrochemical reactions at the electrodes. Additionally, MSNFs‐derived separators, which feature more ion transport channels, exceptional mechanical properties, and the capability to inhibit thermal runaway, are also discussed. Finally, the challenges and prospective pathways for electrospun technology in the application of lithium‐based batteries are reviewed.

Recycled graphite enabled superior performance for lithium ion batteries

Recycling graphite attracts growing attention since cumulative amount of spent Li-ion batteries and the shortage of graphite supply chain. Although various recycling methods have been reported, the recycled graphite cannot reach the strict commercial standards of purity, scalability, efficiency, and capacity, preventing it from battery manufacturing. Herein, the important roles of defects and functional groups on the graphite surface are deeply studied, and a closed-loop graphite recycling process with the surface recovery and modification for the graphite from the end-of-life batteries is demonstrated. The recovered graphite delivers a purity of over 99.9 % and an average initial coulombic efficiency of 91.5 %. Compared with commercial graphite in industrial standard battery testing parameters, full cells with recovered graphite possess enhanced rate reversibility, doubled cycle life, over 10 % higher capacity along with half anode material cost. These impressive results not only underscore the transformative potential of surface reconstruction and modification in graphite recycling, but also present economic feasibility and sustainable pathway for significantly improving battery performance and addressing global resource challenges via integration with the hydrometallurgical recycling process.

Influence of laminated porous cathode structure on the performance and mass transfer of Li[sbnd]O2 batteries

The porous cathode is a crucial component of LiO2 batteries, and its porous structure significantly impacts the battery's performance. In this study, a stacked porous cathode was fabricated via roller pressing. The influence of the cathode structure on the battery performance and mass transfer characteristics were examined using experimental and simulation methods. The structural characteristics, electrochemical properties, and overall battery performance of the stacked porous cathode were analyzed. Furthermore, the effects of the cathode structure on mass transfer within the cathode and battery performance were explored through numerical simulation. The results indicate that when the mass ratio of CNTs to ACET on the diaphragm side is 5:1, the cathode exhibits optimal structural parameters, with an average pore size of 24 nm and a maximum pore volume of 0.85564 cm3/g. Concurrently, the battery demonstrates an exceptionally high area specific capacity of 30.35 mAh/cm2. Integrating the simulation findings, it was observed that adjusting the structural parameters of the cathode enhances material transfer efficiency, thereby improving battery performance.

A biomacromolecular additive based on pullulan polysaccharide to enhance the life of lead-acid battery packs in DC systems

Abstract With the rapid growth in demand for mobile power, lead-acid batteries still occupy a large market share due to their excellence in energy storage. However, their lifespan is affected by various factors, which limits the application efficiency and environmental friendliness. In this regard, this paper proposes a method to enhance the service life of lead-acid battery packs by applying biomacromolecule additives. A lead-acid battery pack modification method is investigated by introducing chitosan, a natural macromolecule with excellent electrical conductivity and biodegradation properties, into lead-acid batteries. So that the chitosan-modified material forms a stable and protective film on the surface of the battery electrode plate, thereby reducing the analysis of sulphate crystals on the electrode surface. The method of modification of lead-acid battery packs has been studied. Comparative analysis of the experimental data shows that the modified battery pack exhibits lower charge transfer impedance and better electrochemical stability than the traditional lead-acid battery during the cyclic charge/discharge test. Through the cycle charge/discharge test, the energy loss of the battery with biomolecules is 30% lower than that of the unmodified battery, and the number of charge/discharge cycles increases by 60%, which effectively prolongs the service life of the lead-acid battery. The progress of this paper not only has guiding significance for the performance improvement of traditional lead-acid batteries but also provides a significant theoretical and experimental basis for the development and application of environmental friendly battery materials.

A convection-enhanced flow field with height-changing ribs for redox flow batteries

Serpentine flow fields with flat ribs can effectively improve the performance of redox flow batteries. However, the marginal pressure difference between adjacent channels near the end side of ribs in conventional designs leads to weak convection in the regions, increasing the local concentration overpotential. This problem will be exacerbated in scaled-up redox flow battery stacks due to enlarged under-rib regions near the end side of ribs. In this work, two modified serpentine flow fields with height-changing ribs are proposed to adjust the electrode compression ratio at the under-rib region, thereby enhancing the convection in the electrode near the end side of ribs. Therefore, the active species are distributed more uniformly, resulting in an improved battery performance. Specifically, the uniformity of V2+, the energy efficiency and the system efficiency of the vanadium redox flow batteries with the ramp ribs are improved by 21 %, 2.7 %, and 2.7 % respectively compared with that of the conventional flat ribs, at the current density of 200 mA cm−2, the flow rate of 3.4 mL min−1 cm−2, and the active area of 117 cm2.

Graphene-Based Materials in Energy Storage and Conversion Devices

Global energy demand and environmental concerns have grown increasingly over the years. To solve these problems, advanced energy storage and conversion technologies are essential. This work explores the applications of graphene-based materials to enhance the performance of lithium-ion batteries, supercapacitors, and solar cells. In lithium-ion batteries, graphene significantly improves electrical conductivity, mechanical stability, and energy capacity, thereby improving battery performance. Likewise, in supercapacitors, graphene-based electrodes exhibit excellent specific capacitance and energy density, which are crucial for high-power applications. In solar cells, graphene improves photoelectric conversion efficiency and stability, especially in perovskite and ZnO/Si heterojunction solar cells. However, the high cost and complexity of producing graphene limit its widespread use. Future research should focus on developing cost-effective production methods, optimizing graphene properties through doping, exploring composite materials, and expanding graphene applications in sustainable energy and environmental fields. This work provides an overview of current progress and suggests directions for future research in this area.

Advanced Li-S Battery Configuration Featuring Sulfur-Coated Separator and Interwoven rGO/CNT Fabric Current Collector.

The development of lithium-sulfur batteries (LSBs) marks a crucial milestone in advancing energy storage solutions essential for sustainable energy transitions. With high theoretical specific capacity, cost-effectiveness, and reduced ecological footprint, LSBs promise to enhance electric vehicle ranges, extend portable electronics' operational times, and stabilize grids integrated with renewable energy. However, challenges like complex processing, electrode instability, and poor cycling stability hinder their commercialization. This study introduces a novel battery design that addresses these issues by coating sulfur directly onto the separator instead of the current collector, demonstrating that active sulfur can be effectively utilized without being incorporated into the electrode structure. Using an interwoven substrate made from carbon nanotube (CNT) fabric adorned with reduced graphene oxide (rGO), this setup enhances manufacturing scalability, supports optimal sulfur utilization, and improves battery performance. The rGO decoration provides multiple highly conductive polysulfide trapping sites, enhancing active material reutilization, while the flexibility and mechanical strength of CNT fabric contribute to electrode integrity. This combination boosts electrical conductivity and polysulfide-capturing capability, effectively managing migrating sulfur species during charge-discharge cycles and mitigating sulfur loss and polysulfide shuttling. The results demonstrate superior cycling stability and efficiency, highlighting the potential of this approach in advancing LSB technology.

Spatial‐Dependent Coupling of Electrochemistry, Mass Transport, and Stress in Silicon‐Graphite Composite Electrodes for Lithium‐Ion Batteries

AbstractThe commercialization of high‐capacity silicon materials in lithium‐ion batteries is hindered by significant volume changes. Composite anodes made from silicon and graphite, which increase battery capacity and maintain electrode structural stability, are receiving considerable attention. However, the spatial configuration of the active particles in the electrode is few investigated due to the complexity of experiments at the microscopic scale. Herein, this work focuses on electrochemical, mass transport, and stress coupling mechanisms by considering different spatial configurations of silicon and graphite. In situ electrochemical and stress measurements are first conducted to demonstrate the impact of the active material arrangement. Then, a 2D electrochemical‐mechanical model is developed considering the heterogeneity of electrochemical processes at the particle‐electrolyte interface. The results show that placing silicon in the upper active layer significantly reduces the ion transport resistance, while the graphite layer near the current collector provides a good conductive network for electron transport in the silicon layer, enhancing the performance of the composite electrode structure. By combining electrochemical and mechanical field models with experimental verification, this study deepens the understanding of composite electrode structure design, offering practical guidance for optimizing the spatial configuration of electrode materials to significantly improve battery performance.

Automated Robotic Cell Fabrication Technology for Stacked‐Type Lithium‐Oxygen Batteries

AbstractRechargeable lithium‐oxygen batteries (LOBs) are gaining interest as next‐generation energy storage devices due to their superior theoretical energy density. While recent years have seen successful operation of LOBs with high cell‐level energy density, the technology for cell fabrication is still in its infancy. This is because the cell fabrication procedure for LOBs is quite different from that of conventional lithium‐ion batteries. The study presents a fully automated sequential robotic experimental setup for the fabrication of stacked‐type LOB cells. This approach allows for high accuracy and high throughput fabrication of the cells. The developed system enables the fabrication of over 80 cells per day, which is 10 times higher than conventional human‐based experiments. In addition, the high alignment accuracy during the electrode stacking and electrolyte injection process results in improved battery performance and reproducibility. The effectiveness of the developed system was also confirmed by investigating a multi‐component electrolyte to maximize battery performance. We believe the methodology demonstrated in the present study is beneficial for accelerating the research and development of LOBs.

A deep learning approach to optimize remaining useful life prediction for Li-ion batteries

Accurately predicting the remaining useful life (RUL) of lithium-ion (Li-ion) batteries is vital for improving battery performance and safety in applications such as consumer electronics and electric vehicles. While the prediction of RUL for these batteries is a well-established field, the current research refines RUL prediction methodologies by leveraging deep learning techniques, advancing prediction accuracy. This study proposes AccuCell Prodigy, a deep learning model that integrates auto-encoders and long short-term memory (LSTM) layers to enhance RUL prediction accuracy and efficiency. The model’s name reflects its precision (“AccuCell”) and predictive strength (“Prodigy”). The proposed methodology involves preparing a dataset of battery operational features, split using an 80–20 ratio for training and testing. Leveraging 22 variations of current (critical parameter) across three Li-ion cells, AccuCell Prodigy significantly reduces prediction errors, achieving a mean square error of 0.1305%, mean absolute error of 2.484%, and root mean square error of 3.613%, with a high R-squared value of 0.9849. These results highlight its robustness and potential for advancing battery health management.

Modification and Functionalization of Separators for High Performance Lithium–Sulfur Batteries

Lithium–sulfur batteries (LSB) have been recognized as a prominent potential next-generation energy storage system, owing to their substantial theoretical specific capacity (1675 mAh g−1) and high energy density (2600 Wh kg−1). In addition, sulfur’s abundance, low cost, and environmental friendliness make commercializing LSB feasible. However, challenges such as poor cycling stability and reduced capacity, stemming from the formation and diffusion of lithium polysulfides (LiPSs), hinder LSB’s practical application. Introducing functional separators represents an effective strategy to surmount these obstacles and enhance the electrochemical performance of LSBs. Here, we have conducted a comprehensive review of recent advancements in functional separators for LSBs about various (i) carbon and metal compound materials, (ii) polymer materials, and (iii) novel separators in recent years. The detailed preparation process, morphology and performance characterization, and advantages and disadvantages are summarized, aiming to fundamentally understand the mechanisms of improving battery performance. Additionally, the development potential and future prospects of advanced separators are also discussed.

Visualizing and Understanding the Ionic Liquid-Mediated Polybromide Electrochemistry for Aqueous Zinc-Bromine Redox Batteries.

Aqueous zinc-bromine redox systems possess multiple merits for scalable energy storage. Applying bromine complexing agents shows effectiveness in alleviating the key challenge of ubiquitous crossover of reactive liquid bromine species, while the underlying microscopic mechanism requires a deep understanding to engineer better complexing electrochemistry. Herein, taking a series of quaternary ammonium ionic liquids (methyl4NBr, ethyl4NBr, propyl4NBr, and butyl4NBr) as a redox mediator model, operando optical monitoring was used to visualize the dynamic electrochemical behaviors, unveiling the ionic liquid-mediated polybromide electrochemistry with a distinct chain length effect. A longer chain length possesses a stronger electrostatic interaction in the complexing product to effectively capture Br2. Operando results reveal the liquid nature of the reversibly electrogenerated polybromide microdroplets in the butyl4NBr-added redox system, which promoted the Br3-/Br- conversion kinetics and alleviated the self-discharge for improved battery performance. This work provides direct evidence and new insights into complexing electrochemistry for advancing Zn-Br2 batteries.

Nb1.60Ti0.32W0.08O5−δ as negative electrode active material for durable and fast-charging all-solid-state Li-ion batteries

Li-based all-solid-state batteries (ASSBs) are considered feasible candidates for the development of the next generation of high-energy rechargeable batteries. However, ASSBs are detrimentally affected by a limited rate capability and inadequate performance at high currents. To circumvent these issues, here we propose the use of Nb1.60Ti0.32W0.08O5-δ (NTWO) as negative electrode active material. NTWO is capable of overcoming the limitation of lithium metal as the negative electrode, offering fast-charging capabilities and cycle stability. Physicochemical and electrochemical characterizations of NTWO in combination with the Li6PS5Cl (LPSCl) solid-state electrolyte demonstrate that the formation of LiWS2 at the electrode|electrolyte interphase is the main responsible for the improved battery performance. Indeed, when an NTWO-based negative electrode and LPSCl are coupled with a LiNbO3-coated LiNi0.8Mn0.1Co0.1O2-based positive electrode, the lab-scale cell is capable of maintaining 80% of discharge capacity retention after 5000 cycles at 45 mA cm−2 at 60 °C and 60 MPa.

Operando Fabricated Quasi-Solid-State Electrolyte Hinders Polysulfide Shuttles in an Advanced Li-S Battery

Lithium-sulfur (Li-S) batteries are a promising option for energy storage due to their theoretical high energy density and the use of abundant, low-cost sulfur cathodes. Nevertheless, several obstacles remain, including the dissolution of lithium polysulfides (LiPS) into the electrolyte and a restricted operational temperature range. This manuscript presents a promising approach to addressing these challenges. The manuscript describes a straightforward and scalable in situ thermal polymerization method for synthesizing a quasi-solid-state electrolyte (QSE) by gelling pentaerythritol tetraacrylate (PETEA), azobisisobutyronitrile (AIBN), and a dual salt lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium nitrate (LiNO3)-based liquid electrolyte. The resulting freestanding quasi-solid-state electrolyte (QSE) effectively inhibits the polysulfide shuttle effect across a wider temperature range of −25 °C to 45 °C. The electrolyte’s ability to prevent LiPS migration and cluster formation has been corroborated by scanning electron microscopy (SEM) and Raman spectroscopy analyses. The optimized QSE composition appears to act as a physical barrier, thereby significantly improving battery performance. Notably, the capacity retention has been demonstrated to reach 95% after 100 cycles at a 2C rate. Furthermore, the simple and scalable synthesis process paves the way for the potential commercialization of this technology.

Estimation of state of charge for polymer solid-state batteries: Ensemble learning models and temperature impact study

In addition to the research and development of solid electrolytes to improve battery performance, an efficient battery management system (BMS) is a must to ensure safe use and extend battery life, and state of charge (SOC) estimation is critical in the BMS. This paper presents a novel temperature-influenced method for estimating the SOC of polymer-based solid-state batteries in real-time, using machine learning to capture the relationship between SOC and battery characteristics at different temperatures. The results show that accurate SOC estimation results can be achieved at different temperatures, with an average root mean square error of 1.42 %. Furthermore, the method uses Shapley Additive explanation (SHAP) to reduce the degree of black box nature of the model and analyzes the electrochemical processes inside the battery at different temperatures through relaxation time distribution. Accurate estimates of SOC and guidelines for appropriate operating temperatures can serve as a basis for BMS decision-making and improve the lifetime of polymer-based solid-state batteries.

Biological small molecule interface-modification fostering resilient interfacial chemistry for silicon-based anodes

Silicon-based materials, particularly at the microscale, are prone to rapid capacity fade due to substantial volume fluctuations during the charge-discharge cycles, significantly impeding their commercial viability. Constructing a stable solid electrolyte interface (SEI) is an effective means to improve the performances of silicon-based anodes. Here small biomolecules, tryptophan (Trp) and phytic acid (PA), are introduced as interface modifiers to optimize the interfacial chemistry of micron-silicon anodes. By engaging in the SEI formation process, these small biomolecules effectively regulate the chemical composition and mechanical properties of the formed SEI, fostering a more cohesive and durable interface. The simultaneous addition of PA and Trp has been observed to yield a synergistic effect, creating a tightly bonded and resilient SEI that confers markedly improved battery performances upon the co-modified micron silicon anodes. Density functional theory calculations reveal charge interactions between these small biomolecules and silicon particles, facilitating effective adsorption onto the silicon surface. Simultaneous adsorption of Trp and PA on silicon surface can significantly enhance adsorption strength, providing a compelling explanation for the observed synergistic effect of Trp and PA co-modification.

Imaging the microstructure of lithium and sodium metal in anode-free solid-state batteries using electron backscatter diffraction.

'Anode-free' or, more fittingly, metal reservoir-free cells could drastically improve current solid-state battery technology by achieving higher energy density, improving safety and simplifying manufacturing. Various strategies have been reported so far to control the morphology of electrodeposited alkali metal films to be homogeneous and dense, but until now, the microstructure of electrodeposited alkali metal is unknown, and a suitable characterization route is yet to be identified. Here we establish a reproducible protocol for characterizing the size and orientation of metal grains in differently processed lithium and sodium samples by a combination of focused ion beam and electron backscatter diffraction. Electrodeposited films at Cu|Li6.5Ta0.5La3Zr1.5O12, steel|Li6PS5Cl and Al|Na3.4Zr2Si2.4P0.6O12 interfaces were characterized. The analyses show large grain sizes (>100 µm) within these films and a preferential orientation of grain boundaries. Furthermore, metal growth and dissolution were investigated using in situ electron backscatter diffraction, showing a dynamic grain coarsening during electrodeposition and pore formation within grains during dissolution. Our methodology and results deepen the research field for the improvement of solid-state battery performance through a characterization of the alkali metal microstructure.

Metal‐N Coordination in Lithium‐Sulfur Batteries: Inhibiting Catalyst Passivation

Lithium‐sulfur (Li‐S) batteries exhibit great potential as the next‐generation energy storage techniques. Application of catalyst is widely adopted to accelerate the redox kinetics of polysulfide conversion reactions and improve battery performance. Although significant attention has been devoted to seeking new catalysts, the problem of catalyst passivation remains underexplored. Herein, we find that metal‐N coordination has a previously overlooked role in preventing the catalyst passivation. In the case of nickel, the Ni catalyst reacts with S8 to produce NiSx compounds on the surface, leading to catalyst passivation and slow the kinetics of LiPSs conversion. In contrast, when Ni is coordinated with N (typically Ni‐N4), S8 remains stable on the surface. The Ni‐N4 exhibits excellent resistance to passivation and rapid kinetics of LiPSs conversion. Consequently, the sulfur cathode with Ni‐N4 exhibits a high rate capability of 604.11 mAh g‐1 at 3 C and maintains a low capacity decay rate of 0.046% per cycle over 1000 cycles at 2 C. Furthermore, preventing S passivation in M‐N coordination applies not only to Ni‐N4 but also to various coordination numbers and transition metals. This study reveals a new aspect of metal‐N coordination in inhibiting catalyst passivation, improving our understanding of catalysts in Li‐S batteries.

Metal-N Coordination in Lithium-Sulfur Batteries: Inhibiting Catalyst Passivation.

Lithium-sulfur (Li-S) batteries exhibit great potential as the next-generation energy storage techniques. Application of catalyst is widely adopted to accelerate the redox kinetics of polysulfide conversion reactions and improve battery performance. Although significant attention has been devoted to seeking new catalysts, the problem of catalyst passivation remains underexplored. Herein, we find that metal-N coordination has a previously overlooked role in preventing the catalyst passivation. In the case of nickel, the Ni catalyst reacts with S8 to produce NiSx compounds on the surface, leading to catalyst passivation and slow the kinetics of LiPSs conversion. In contrast, when Ni is coordinated with N (typically Ni-N4), S8 remains stable on the surface. The Ni-N4 exhibits excellent resistance to passivation and rapid kinetics of LiPSs conversion. Consequently, the sulfur cathode with Ni-N4 exhibits a high rate capability of 604.11 mAh g-1 at 3 C and maintains a low capacity decay rate of 0.046 % per cycle over 1000 cycles at 2 C. Furthermore, preventing S passivation in M-N coordination applies not only to Ni-N4 but also to various coordination numbers and transition metals. This study reveals a new aspect of metal-N coordination in inhibiting catalyst passivation, improving our understanding of catalysts in Li-S batteries.

MoC nanoparticles decorated carbon nanofibers loaded with Li2S as high-performance lithium sulfur battery cathodes

Lithium sulfur (Li-S) batteries have broad development potential in the field of electrochemical energy storage due to their high theoretical specific capacity, low cost, and environmentally friendly. However, the notorious shuttle effect of lithium polysulfides (LiPSs) during cycling process severely limits the performance improvement of Li-S batteries. In this work, carbon nanofibers (CNFs) decorated by MoC nanoparticles have been successfully established through electrospin combined with carbothermal reduction method. The effect of calcination temperature and MoC loading amount on the catalytic activity on LiPSs, as well as the electrochemical performance have been first investigated in detail. Based on the visualized adsorption and LiPSs conversion kinetics testing, the CNFs@MoC composites with 37 wt% MoC loading (CNFs@MoC-37 %) are confirmed to be the optimized sample. By using liquid-phase impregnation to load Li2S onto the CNFs@MoC-37 % composites to act as cathode, the assembled cells can achieve a reversible capacity of 941 mAh g−1 and 751 mAh g−1 at the current density of 0.1C and 1C respectively. The reversible capacity can still maintain at 550 mAh g−1 at 1C after 500 cycles, corresponding to the capacity decay rate of 0.054 % per cycle.