High-capacity Batteries Research Articles

Phthalocyanine-based solid-state electrolyte for high-capacity and long-life lithium-ion batteries

Phthalocyanine-based solid-state electrolyte for high-capacity and long-life lithium-ion batteries

Achieving High Stability and Capacity in Micron-Sized Conversion-Type Iron Fluoride Li-Metal Batteries.

Iron fluoride, a conversion-type cathode material with high energy density and low-cost iron, holds promise for Li-ion batteries but faces challenges in synthesis, conductivity, and cycling stability. This study addresses these issues by synthesizing micron-sized iron-fluoride using a simple solid-state synthesis. Despite a large particle size, a high capacity of 571mAhg-1 is achieved, which is attributed to the unique surface and internal pores within the iron-fluoride particles, which provided a large surface area. This is the first study to demonstrate the feasibility of using large iron fluoride particles to enhance the energy density of the electrode and achieve an iron fluoride full cell with high capacity. Also, the cause of the capacity fading is investigated. Electrode delamination from the current collector, which is the main cause of capacity fading in early cycles, is resolved using a carbon-coated aluminum (C/Al) current collector. Moreover,iron (Fe) dissolution and the deposition of dissolved Fe on the Li metal also contributed significantly to the degradation. Localized high-concentration electrolytes (LHCEs)suppress iron dissolution and Li dendrite growth, resulting in long-cycle stability for 300 cycles. This study provides insights into the further development of conversion-type metal fluorides across various compositions.

Biomass-derived hard carbon material for high-capacity sodium-ion battery anode through structure regulation

Economical and environmentally friendly hard carbon materials are attractive options for high-performance sodium-ion battery anode materials. Biomass-derived hard carbon materials have good economic benefits and environmentally friendliness as anode materials for sodium-ion batteries. In this work, we propose a new hard carbon material prepared from agricultural waste olive shells through a simple and environmentally friendly process. The effects of high-temperature treatments and pre-carbonization strategies on the pore structure and graphitization degree of the hard carbon materials were investigated. Combined with electrochemical performance tests, the influence of structural changes on the sodium storage properties of the olive shell-derived hard carbon was revealed. Under the optimized conditions of carbonization temperature and pre-carbonization strategy, the OSHC-Air electrode exhibits excellent sodium storage capacity with 87 % capacity remaining after 1000 cycles at 1000 mA g−1. The assembled PB//OSHC-Air sodium-ion full cell exhibits a high capacity of 216 mAh g−1. Our research provides a potential candidate for commercial anode materials for high-capacity sodium-ion batteries.

Free-standing medium-entropy porous needle-like FeCoCuNi phosphide nanowires-formed flower clusters/carbon fiber anode with high capacity and long durability for sodium-ion batteries

The drastic volume expansion and slow sodium-ion kinetics hinder the practical application of phosphides with high specific capacity and low discharge voltage in sodium-ion batteries (SIBs). Herein, we introduced entropy configuration into nanostructures and prepared a novel free-standing, three-dimensional, porous needle-like medium-entropy Fe, Co, Cu, Ni phosphide (ME-FCCNP) nanowires-formed flower clusters/carbon fiber cloth (CFC) anode (ME-FCCNP@CFC) for SIBs. The distorted lattices caused by medium-entropy configuration provide abundant sites for sodium-ion reactions and improve the electron transfer rate. The medium-entropy effects improve the mechanical stability, while the three-dimensional networks and porous needle-like nanowires provide sufficient space for the volume expansion. These combined properties enable the ME-FCCNP@CFC electrode to exhibit a high-rate capability of 170.8 mAh g−1 at 5.0 A g−1 and deliver a specific capacity of 325.8 mAh g−1 after 2000 cycles at 2.0 A g−1, far surpassing most of reported transition-metal phosphides. Moreover, the Na3V2(PO4)3 || ME-FCCNP@CFC full cell showcases a high-energy density of 256.8 Wh kg−1 and a long cycling life (267.8 mAh g−1 at 2.0 A g−1 with a capacity retention of 83.2 % after 1000 cycles). These results provide significantly promising implications for the anode design of SIBs by employing self-supporting and medium-entropy structures.

Earth-abundant, low-cost raw micro-silicon enabled by mechanically strengthened binder for high-capacity and long-life battery electrode

Nano-structured silicon materials with high capacity, are currently being gradually commercialized and composited with graphite in high-energy batteries, although their fabrication cost is rather high. However, the low-cost micro-silicon materials are always criticized and discarded in batteries due to the severe particle-to-electrode crack and huge volume change. Herein, inspired by the human ligament, a cross-linked binder with greatly enhanced mechanical properties is designed and fabricated to stabilize micro-silicon anodes. This biomimetic polymer can not only act as flexible “fibrils” in ligament, to adapt the high-volume change of silicon anode; but also act as “proteoglycan” in ligament to firmly hold these flexible fibrils and proactively constrain stress concentration of silicon anode. The combination of “soft to hard” hierarchical structure would endow binders with excellent elasticity and toughness. The pure micro-Si (5∼10 μm) electrodes with PSB binder exhibit high initial coulombic efficiency (ICE) of 93.3 % and favorable reversible capacity of ∼1500 mAh g−1 at 4000 mA g−1 after 600 cycles. Furthermore, the PSB binder also enables the μSi/GR//NCM811 full cell with 91.4 % capacity retention over 200 cycles. This functional PSB binders provide inspiration for constructing μSi anodes with high-ICE, high reversible capacity, and long-cycling life.

Cooling Performance of a Nano Phase Change Material Emulsions-Based Liquid Cooling Battery Thermal Management System for High-Capacity Square Lithium-Ion Batteries

This study investigated the application of nanophase change material emulsions (NPCMEs) for thermal management in high-capacity ternary lithium-ion batteries. We formulated an NPCME of n-octadecane (n-OD) and n-eicosane (n-E) with a mass fraction of 10%, whose phase change temperatures are 25.5 °C and 32.5 °C, respectively, with specific heat capacities 2.1 and 2.4 times greater than water. Experiments were conducted to evaluate the thermal control performance and latent heat utilization efficiency of these NPCMEs. The NPCMEs with an n-OD mass fraction of 10% (NPCME-n-OD), particularly reduced the battery pack’s maximum temperature and temperature difference to 41.6 °C and 3.72 °C under a 2 C discharge rate, lower than the water-cooled group by 1.3 °C and 0.3 °C. This suggests that nano emulsions with phase change temperatures close to ambient temperatures exhibit superior cooling performance. Increased flow rates from 50 mL/min to 75 mL/min significantly lowered temperatures, resulting in temperature reductions of 2.73 °C for the NPCME-n-OD group and 3.37 °C for the NPCME-n-E group. However, the latent heat utilization efficiency of the nano emulsions decreased, leading to increased system energy consumption. Also, it was found that the inlet temperature of the NPCMEs was very important for good thermal management. The right inlet temperatures make it easier to use phase change latent heat, while excessively high temperatures may make thermal management less effective.

Capacity recovery by transient voltage pulse in silicon-anode batteries.

In the quest for high-capacity battery electrodes, addressing capacity loss attributed to isolated active materials remains a challenge. We developed an approach to substantially recover the isolated active materials in silicon electrodes and used a voltage pulse to reconnect the isolated lithium-silicon (LixSi) particles back to the conductive network. Using a 5-second pulse, we achieved >30% of capacity recovery in both Li-Si and Si-lithium iron phosphate (Si-LFP) batteries. The recovered capacity sustains and replicates through multiple pulses, providing a constant capacity advantage. We validated the recovery mechanism as the movement of the neutral isolated LixSi particles under a localized nonuniform electric field, a phenomenon known as dielectrophoresis.

Optimization of electrode thickness of lithium-ion batteries for maximizing energy density

AbstractThe demand for high capacity and high energy density lithium-ion batteries (LIBs) has drastically increased nowadays. One way of meeting that rising demand is to design LIBs with thicker electrodes. Increasing electrode thickness can enhance the energy density of LIBs at the cell level by reducing the ratio of inactive materials in the cell. However, after a certain value of electrode thickness, the rate of energy density increase becomes slower. On the other hand, the impact of associated limitations becomes stronger, reducing the practical applicability of LIBs with thicker electrodes. Hence, an optimum value of thickness is of utmost importance for the practicability of thicker electrode design. In this paper, both the cathode thickness and the anode thickness of an NCM LIB cell were optimized by applying response surface methodology (RSM) with a Box-Behnken design (BBD) to maximize the energy density. Moreover, the influence of electrode porosity, together with the interaction of porosity with cathode and anode thickness, was incorporated into the optimization. A full factorial design of 3-level, 3-factor was used to generate 15 simulation conditions in accordance with the design of experiment (DoE) achieved through BBD. Then, those conditions were used to achieve 15 responses by simulating a reduced-order electrochemical model. Finally, the statistical technique analysis of variance (ANOVA) was used to analyze and validate the results of RSM. The results show that the RSM-BBD optimization method, coupled with ANOVA, has successfully optimized the thicknesses of both positive and negative electrodes for maximum energy density, despite the nonlinearity of the electrochemical system. The findings suggest an optimized cathode thickness of 401.56 µm and anode thickness of 186.36 µm for a maximum energy density of 292.22 of an NCM LIB cell, while electrode porosity is preferred to be 0.2.

Sulfur-doped enhanced ZnMn2O4 spinel for high-capacity zinc-ion batteries: Facilitating charge transfer

ZnMn2O4 spinel is considered a promising cathode material for zinc-ion batteries due to its superior Zn2+ storage capability. However, the widespread utilization of ZnMn2O4 spinel as a high-capacity cathode material is impeded by its insufficient electrical conductivity. To tackle this limitation, we have employed a sulfur doping approach by substituting sulfur for oxygen atoms within the ZnMn2O4 lattice structure. After theoretical calculation, the charge exchange between metal Zn/Mn and surrounding coordinated atoms is enhanced after sulfur doping. The sulfur-doped ZnMn2O4 spinel effectively enhances the electrical conductivity, improving its electrochemical discharge capacity. Furthermore, the results reveals that a doping level of 20 % provided the greatest enhancement in capacitance, achieving a specific capacity of 220.1 mAh/g. This work improves the disadvantages of ZnMn2O4 at the atomic level and can provide ideas for the optimization and modification of spinel cathode materials.

Remaining useful life prediction of high-capacity lithium-ion batteries based on incremental capacity analysis and Gaussian kernel function optimization

Remaining useful life (RUL) is a key indicator for assessing the health status of lithium (Li)-ion batteries, and realizing accurate and reliable RUL prediction is crucial for the proper operation of battery systems. As high-capacity Li batteries have more complex chemical properties, most of the current RUL prediction methods rely mainly on a priori knowledge to make judgments. As a result, prediction accuracy is not high. In this study, we developed a health indicator-capacity (HI-C) dual Gaussian process regression (GPR) model based on incremental capacity analysis (ICA) and optimized its kernel function to achieve accurate RUL prediction for 280 Ah high-capacity Li batteries. Validation against the United States National Aeronautics and Space Administration’s four battery test datasets showed that the use of the HI-C dual GPR model resulted in a mean absolute percentage error and root mean square error of less than 0.02 and 0.04, respectively, for the four battery-rated capacity predictions. Additionally, this model achieved an absolute error of less than five battery failure turns. Compared with a single model, the HI-C dual GPR model not only had high accuracy but also solved the problem that the HI was not measurable in the actual battery operation, which made it more suitable for RUL prediction of Li batteries.

High-capacity and fast-charging Al battery based on Cu/KB cathode

Rechargeable aluminum-ion batteries (RABs) are promising for energy storage due to their high theoretical energy density, but face challenges in cathode materials that match aluminum's capacity and stability. We propose copper (Cu) as an inexpensive and easily synthesized cathode material for RABs, using KetjenBlack (KB) as a carbon framework to enhance cycling stability by reducing structural damage. Key findings include: (1) Specific capacities of 793.5 mAhg-1 (charge) and 414.5 mAhg-1 (discharge) at 2 Ag-1 current density; (2) Good rate performance with a capacity maintained around 200 mAhg-1 at 12 Ag-1; (3) After 300 cycles at 2 Ag-1, discharge capacity stabilized at 225.1 mAhg-1. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD) were used to analyze electrode changes and understand the Cu/KB||Al battery's energy storage mechanism. This study introduces a novel electrode material and proposes a carbon framework for enhancing RAB performance.

Exploring the Mechanisms of LiNiO2 Cathode Degradation by the Electrolyte Interfacial Deprotonation Reaction.

Nickel-rich layered oxides stand as ideal cathode candidates for high specific capacity and energy density next-generation lithium-ion batteries. However, increasing the Ni content significantly exacerbates structural degradation under high operating voltage, which greatly restricts large-scale commercialization. While strategies are being developed to improve cathode material stability, little is known about the effects of electrolyte-electrode interaction on the structural changes of cathode materials. Here, using LiNiO2 in contact with electrolytes with different proton-generating levels as model systems, we present a holistic picture of proton-induced structural degradation of LiNiO2. Through ab initio molecular dynamics calculations based on density functional theory, we investigated the mechanisms of electrolyte deprotonation, protonation-induced Ni dissolution, and cathode degradation and the impacts of dissolved Ni on the Li metal anode surfaces. We show that the proton-transfer reaction from electrolytes to cathode surfaces leads to dissolution of Ni cations in the form of NiOOHx, which stimulates cation mixing and oxygen loss in the lattice accelerating its layered-spinel-rock-salt phase transition. Migration of dissolved Ni2+ ions to the anode side causes their reduction into the metallic state and surface deposition. This work reveals that interactions between the electrolyte and cathode that result in protonation can be a dominant factor for the structural stability of Ni-rich cathodes. Considering this factor in electrolyte design should be of benefit for the development of future batteries.

Electrifying the bus network with trolleybus: Analyzing the in motion charging technology

Currently, electric buses are becoming more and more popular, and their number in operation is increasing. The range of electric buses is also increasing and solutions that seem to be working almost without fixed infrastructure are being promised. However, this requires the use of high-capacity batteries, which increases the weight and price of the vehicle and causes high costs of battery replacement during operation. Moreover, if we take into account the growing demand for batteries, limited raw material resources, and the environmental impact of the battery production process, the optimization of battery capacity in vehicles may turn out to be a key issue. In this light, trolleybus becomes a sustainable and economically efficient bus electrification technology, if considered in an international scope and a medium- to long-term approach. The article provides a comprehensive study of challenges and potential solutions related to electric buses, which covers the theoretical analysis, technical aspects and practical applications, thus making a valuable resource for readers interested in sustainable urban transport systems. It presents the trolleybus technology, especially with modern solutions, as a sustainable and economically efficient tool for bus electrification. The article shows that the In Motion Charging (IMC) system reduces the need for high-capacity batteries under 100 kWh, which allows to extend their service life up to 15 years and, consequently, to reduce the number of buses needed for operation. The research was based on real measurement data from the transport system in Gdynia (Poland).

Unraveling the enhanced sodium-storage mechanism in a strongly bonded 2D honeycomb borophene/boron phosphide heterostructure

The growing modern demand for battery capacity is driving the development of high-capacity metal-ion battery anodes for future energy storage. Two-dimensional (2D) material-based heterostructures have shown advantages as alternative anodes due to their enhanced adsorption capacity. The lightweight nature of honeycomb borophene (HB) is beneficial for serving as a high-capacity anode but is constrained by structural instability arising from electron deficiency. In this study, using first-principles calculations, we propose a HB/boron phosphide (BP) heterostructure as an anode for both lithium-ion batteries and sodium-ion batteries (SIBs). The heterostructure engineering not only stabilizes the HB structure but also leads to a bonding heterostructure instead of common van der Walls type. The HB/BP demonstrates robust structural stability and reversibility when multiple ions are stored. In addition, the HB/BP offers stable storage sites and low diffusion barriers for lithium (0.31 eV) and sodium (0.28 eV), indicating rapid charging–discharging performance. Notably, the predicted maximum sodium storage capacity reaches 2402 mAh/g, surpassing that of the constituent monolayers and most 2D heterostructures. The underlying mechanism for high storage capacity is elucidated through detailed charge image model analysis, offering atomistic-scale insights for constructing high-capacity anodes. All results suggest that the presented HB/BP is a promising anode candidate for SIBs and opens an avenue for stabilizing HB in energy storage.

Sulfur/reduced graphite oxide and dual-anion solid polymer‒electrolyte integrated structure for high-loading practical all-solid-state lithium–sulfur batteries

The demand for high-capacity batteries with long cycle life and safety has been increasing owing to the expanding mid-to-large battery market. Li–S batteries are suitable energy-storage devices because of their reversibility, high theoretical capacity, and inexpensive construction materials. However, their performance is limited by various factors, including the shuttle effect and dendrite growth at the anode. Here, an integrated electrode for use in all-solid-state (ASS) Li–S batteries was formed via hot pressing. In detail, S particles dispersed in a functionalized reduced graphite oxide (rGO) cathode with a binder-less polymer electrolyte (PE) and a dual-anion ionic liquid-containing cross-linked poly(ethylene oxide)–Li bis(fluoromethanesulfonyl)imide–N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl) imide-based solid polymer electrolyte (SPE, PEO–LiFSI0.1(Pyr14TFSI)0.4) were hot-pressed into an integrated electrode, which serves as both the cathode and electrolyte. The resulting S/rGO-based solid-state Li–S batteries exhibited more stable performance than Li–S batteries using liquid electrolytes did, indicating that the dual-anion SPE layer effectively suppressed dendritic Li formation and the shuttle effect with high ionic conductivity. At 0.1 C, the battery discharge capacities were 957 and 576 mAh g−1 in the first cycle and after 100 cycles, respectively. At 1 C, the reversible capacity was 590 and 417 mAh g−1 in the first cycle and after 100 cycles, respectively (capacity retention = 71%). Therefore, the proposed S/rGO/PE//LiFSI0.1(Pyr14TFSI)0.4-integrated electrodes are beneficial for ASS Li–S batteries.

A high-capacity and stable dual-ion battery based on an ultra-large lattice-spacing amorphous carbon anode

Compared with traditional lithium-ion batteries (LIBs), dual-ion batteries (DIBs) offer advantages such as high operating voltage, good safety performance, and low cost. However, DIBs often suffer from challenges such as low specific capacity and poor cycling performance in practical applications. Here, a layered nitrogen-doped carbon anode has been prepared using a one-step pyrolysis method with excellent Li+ storage sites. The large lattice spacing of 0.55 nm provides more space for the storage and migration of active ions. Concurrently, the utilization of concentrated electrolyte facilitated the electrochemical window and the restrained solvation of ions, which helps to boost ion transport and improve the stability of the electrolyte and the operating voltage of DIBs. The assembled DIBs exhibit a high specific discharge capacity of 179.27 mA h g−1, within a 2.5–4.8 V voltage range, and excellent cycling stability of 3500 cycles without degradation. Specifically, the structural evolution of the electrodes during charging and discharging and the working mechanism of the DIBs are also explored. The DIBs system designed in this paper provides a facile and scalable approach to promote the development of DIBs with low-cost and high-performance.

Enhancing Unmanned Aerial Vehicle Security: A Zero-Knowledge Proof Approach with Zero-Knowledge Succinct Non-Interactive Arguments of Knowledge for Authentication and Location Proof.

UAVs are increasingly being used in various domains, from personal and commercial applications to military operations. Ensuring the security and trustworthiness of UAV communications is crucial, and blockchain technology has been explored as a solution. However, privacy remains a challenge, especially in public blockchains. In this work, we propose a novel approach utilizing zero-knowledge proof techniques, specifically zk-SNARKs, which are non-interactive cryptographic proofs. This approach allows UAVs to prove their authenticity or location without disclosing sensitive information. We generated zk-SNARK proofs using the Zokrates tool on a Raspberry Pi, simulating a drone environment, and analyzed power consumption and CPU utilization. The results are promising, especially in the case of larger drones with higher battery capacities. Ethereum was chosen as the public blockchain platform, with smart contracts developed in Solidity and tested on the Sepolia testnet using Remix IDE. This novel proposed approach paves the way for a new path of research in the UAV area.

Novel hybrid BTMS by considering safety and driving cycle under extreme fast charge/discharge rates

A battery thermal management system integrating phase change material and mini-channels, with a focus on safety and economic considerations, is proposed to enhance thermal performance across various working conditions, safety scenarios, and realistic driving cycles while minimizing energy consumption. A battery thermal model and PCM simulation model were developed and validated using experimental data. Numerical analyses were conducted to compare the combination of PCM and liquid cooling (hybrid cooling) with fully liquid cooling under different charge/discharge rates and realistic driving cycles, evaluating their safety characteristics, power consumption, and thermal efficiency. The results demonstrated that the hybrid cooling approach can effectively maintain both the maximum temperature and the temperature difference within a desirable range, even when the inlet velocity is reduced from 0.12 to 0.05 m/s compared to liquid cooling. Additionally, the hybrid BTMS provides better working conditions for the battery pack, requiring only 4 × 10−5 W of pumping power compared to 16 × 10−5 W in the liquid cooling system. This underscores the capability of the designed BTMS to cool high-capacity battery packs with significantly lower fluid flow rates. Furthermore, the performance of the proposed cooling system was examined in the event of liquid channel failure, with results showing that the hybrid BTMS can successfully maintain the battery's maximum temperature within an allowable range during fast charge/discharge processes. Lastly, evaluations under realistic driving conditions revealed the superiority of hybrid cooling in reducing peak temperatures and minimizing battery temperature variation.

Advanced 3D-Printed Potassium Ammonium Vanadate/rGO Aerogel Cathodes for Durable and High-Capacity Potassium-Ion Batteries.

A 3D-printed oxygen-vacancy-rich potassium ammonium vanadate/reduced graphene oxide (KNVOv/rGO) microlattice aerogel is designed for the cathode in high-performance K-ion batteries (KIBs). The 3D-printed KNVOv/rGO electrode with periodic submillimeter microchannels and interconnected printed filaments is composed of highly dispersed KNVOv nanobelts, wrinkled graphene nanoflakes, and abundant micropores. The well-defined 3D porous microlattice structure of the rGO backbone not only provides the interconnected conductive 3D network and the required mechanical robustness but also facilitates the penetration of the liquid electrolyte into inner active sites, consequently ensuring a stable electrochemical environment for K-ion intercalation/deintercalation within the KNVOv nanobelts. The 3D-printed KNVOv/rGO microlattice aerogel electrode has a high discharge capacity of 109.3 mAh g-1 with a capacity retention rate of 92.6% after 200 cycles at 50mA g-1 and maintains a discharge capacity of 75.8 mAh g-1 after 2000 cycles at 500mA g-1. The flexible pouch-type KIB battery consisting of the 3D-printed KNVOv/rGO has good mechanical durability and retains a high specific capacity under different forms of deformation such as bending and folding. The results provide valuable insights into the integration of advanced 3D-printed electrode materials into K-ion batteries and the design of flexible and wearable energy storage devices.

Optimization of multi-vehicle charging and discharging efficiency under time constraints based on reinforcement learning

In the Vehicle-to-Grid (V2G) scenario, a multitude of coordinated electric vehicles (EVs) equipped with high-capacity batteries actively participate in power grid dispatching as energy carriers, aiming to achieve a tripartite objective encompassing peak load reduction and valley filling, enhanced utilization of renewable energy sources, and added benefits for electric vehicle owners. To address the existing limitations in the charging–discharging decision-making process for electric vehicles based on V2G, such as the lack of consideration for charging pile constraints, EV profitability, EV transportation timeliness, and high costs associated with central servers, we proposed a reinforcement learning-based Multi-vehicle Joint Routing and Charging–Discharging Decision algorithm (MJRCDD). Firstly, the Markov decision process (MDP) was established to describe the problem, and the route selection and charging–discharging behavior of the vehicle were innovatively integrated in the vehicle action space. Secondly, the multi-vehicle joint route planning and charging–discharging decision problem was solved by multi-agent reinforcement learning. Finally, the effectiveness of MJRCDD was verified by simulation and comparison experiments based on PeMS.