Battery Performance Research Articles

Indium Nanoparticle‐Decorated Graphite Felt Electrodes for Efficient and Long‐Cycle Zinc‐Bromine Flow Batteries

AbstractZinc‐bromine flow batteries (ZBFBs) offer the potential for large‐scale, low‐cost energy storage; however, zinc dendrite formation on the electrodes presents challenges such as short‐circuiting and diminished performance. Herein, an indium nanoparticle‐decorated graphite felt composite electrode for ZBFBs is proposed to mitigate zinc dendrite formation, improve performance, and prolong operational longevity. Using a facile in situ electrodeposition method, indium nanoparticles are uniformly and densely distributed on the carbon fiber surface, demonstrating exceptional efficacy in regulating zinc deposition. Thus, a higher prevalence of Zn (002) crystal planes and a smoother and more compact surface morphology are obtained, compared with those of thermally treated graphite felt. Furthermore, integration of the composite electrode into the negative side of a ZBFB yielded substantial improvements in cell performance, achieving an energy efficiency of 66.83% ± 0.45% at 120 mA cm−2, significantly surpassing the performance of batteries utilizing thermally treated graphite felt (52.64% ± 1.50%). Notably, the cycle life of the battery is extended by more than five‐fold with the composite electrode, underscoring the remarkable zinc deposition‐regulating capabilities of the indium nanoparticles.

Abnormal Gas Generation during First Discharge Process of Sodium Ion Battery.

In recent years, sodium-ion batteries (SIBs) have attracted a lot of attention and are considered an ideal alternative to lithium-ion batteries (LIBs). The hard carbon (HC) anode in SIBs presents a unique challenge for studying the formation process of the solid electrolyte interphase (SEI) during initial cycling, owing to its distinctive porous structure. This study employs a combination of ultrasonic scanning techniques and differential electrochemical mass spectrometry to conduct an in-depth analysis of the two-dimensional distribution and composition of gases during the formation process. The findings reveal distinct gas evolution behaviors in SIBs compared to LIBs during formation. Notably, significant gas evolution is observed during the discharge phase of the formation cycle in SIBs, with higher discharge rates leading to increased gas evolution rates. This phenomenon is likely attributed to the adsorption of CO2 gas by the abundant pores in HC, followed by desorption during discharge. Furthermore, the study demonstrates that the addition of 5A molecular sieves, which competitively adsorb gases, effectively reduces gas adsorption on the anode during formation, thereby significantly enhancing battery performance. This research elucidates the gas adsorption and desorption behavior at the battery interface, providing new insights into the SEI formation process in 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.

Tuning Na Occupation and Annealing Temperature on Na Diffusion Pathways in P2-Type NaxNi0.25Mn0.75O2 for Sodium-Ion Batteries by Ab Initio Calculations.

The NaxNi0.25Mn0.75O2 cathode material draws ongoing interest owing to its considerable specific capacity along with its elevated average operating voltage. However, its application is limited by weak rate performance and quick capacity fading. In this study, a series of NaxNi0.25Mn0.75O2 (x = 0.65, 0.70, 0.75, 0.80) cathode materials are prepared by the solid-phase method based on an orthogonal experiment. The optimum preparation process is investigated by optimizing factors such as Na content, calcination temperature, calcination time, and heating rate. The Nae/Naf ratio is adjusted, and the Na+ at different sites are rearranged to reduce the Na+/vacancy ordering by changing the Na content on the basis of process optimization. Owing to the fast migration kinetics of Nae sites, experimental results indicate that the P2-Na0.75Ni0.25Mn0.75O2 cathode material, which has Na+ occupying more thermodynamically stable Nae sites, demonstrates superior battery performance. High initial discharge specific capacity (157.2 mAh g-1) along with favorable cycle performance of the Na0.75Ni0.25Mn0.75O2 cathode material can be achieved by modifying the Nae site occupancy and optimizing the experimental conditions. Together with the microscopic control of Na+ occupancy, this novel orthogonal experiment design offers a fresh perspective and approach to a thorough comprehension of cathode materials for sodium-ion batteries.

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.

Organic-Inorganic Dual-Network Composite Separators for Lithium Metal Batteries.

The suboptimal ionic conductivity of commercial polyolefin separators exacerbates uncontrolled lithium dendrite formation, deteriorating lithium metal battery performance and posing safety hazards. To address this challenge, a novel organic-inorganic composite separator designed is prepared to enhance ion transport and effectively suppress dendrite growth. This separator features a thermally stable, highly porous poly(m-phenylene isophthalamide) (PMIA) electrospun membrane, coated with ultralong hydroxyapatite (HAP) nanowires that promote "ion flow redistribution." The synergistic effects of the nitrogen atoms in PMIA and the hydroxyl groups in HAP hinder anion transport while facilitating efficient Li+ conduction. Meanwhile, the optimized unilateral pore structure ensures uniform ion transport. These results show that the 19µm-thick HAP/PMIA composite separator achieves remarkable ionic conductivity (0.68mS cm-1) and a high lithium-ion transference number (0.51). Lithium symmetric cells using HAP/PMIA separators exhibit a lifespan exceeding 1000h with low polarization, significantly outperforming commercial polypropylene separators. Furthermore, this separator enables LiFePO4||Li cells to achieve an enhanced retention of 97.3% after 200 cycles at 1C and demonstrates impressive rate capability with a discharge capacity of 72.7mAh g-1 at 15C.

Equivalent Circuit Model for Electrochemical Impedance Spectroscopy of Commercial 18650 Lithium‐Ion Cell Under Over‐Discharge and Overcharge Conditions

AbstractThis study endeavors to assess the impedance responses exhibited by 18650 Graphite||LiCoO2 (C6||LCO) cells under conditions of over‐discharge and overcharge. The impedance measurements are conducted at a potential of 4.20 V, followed by subjecting the cells to over‐discharge and overcharge scenarios. It is observed that the impedance magnitude experiences augmentation in both instances. Upon reaching a potential of 2.70 V, the electrochemical attributes of the cells revert to their normal state post over‐discharge. However, the impedance characteristics persist even upon exceeding a potential of 4.70 V. These observations imply that overcharge induces enduring alterations in impedance behavior, while over‐discharge is a reversible phenomenon. To delve deeper into the underlying mechanisms, an equivalent circuit process model is constructed. This model elucidates that over‐discharge of Li‐ion batteries is reversible, indicating the potential for restoration of original impedance behavior upon recharge. Conversely, overcharge precipitates permanent alterations in impedance behavior, engendering irreversible changes in battery characteristics. In summation, this study underscores the criticality of meticulously managing the charging and discharging processes of Li‐ion batteries to avert irreversible impairment to impedance behavior, thereby safeguarding battery performance and longevity.

Abnormal Gas Generation during First Discharge Process of Sodium Ion Battery

AbstractIn recent years, sodium‐ion batteries (SIBs) have attracted a lot of attention and are considered an ideal alternative to lithium‐ion batteries (LIBs). The hard carbon (HC) anode in SIBs presents a unique challenge for studying the formation process of the solid electrolyte interphase (SEI) during initial cycling, owing to its distinctive porous structure. This study employs a combination of ultrasonic scanning techniques and differential electrochemical mass spectrometry to conduct an in‐depth analysis of the two‐dimensional distribution and composition of gases during the formation process. The findings reveal distinct gas evolution behaviors in SIBs compared to LIBs during formation. Notably, significant gas evolution is observed during the discharge phase of the formation cycle in SIBs, with higher discharge rates leading to increased gas evolution rates. This phenomenon is likely attributed to the adsorption of CO2 gas by the abundant pores in HC, followed by desorption during discharge. Furthermore, the study demonstrates that the addition of 5A molecular sieves, which competitively adsorb gases, effectively reduces gas adsorption on the anode during formation, thereby significantly enhancing battery performance. This research elucidates the gas adsorption and desorption behavior at the battery interface, providing new insights into the SEI formation process in SIBs.

Progress in aluminum-ion battery technology: innovations in cathode materials, electrolyte chemistry, and performance enhancement

The review explores recent advancements in aluminum-ion battery technology, focusing on innovations in cathode materials, electrolyte chemistry, and performance enhancement. Notable developments include new cathode materials like activated carbon and graphene composites, which improve surface area, conductivity, and overall battery performance. Advances in electrolyte formulations, particularly AlCl3-based ionic liquids, have optimized ion transport and stabilized electrochemical processes, extending cycle life and reliability. Studies on ion intercalation mechanisms using density functional theory and molecular dynamics have provided insights into electrode transformations during charge-discharge cycles, aiding in the design of cathode materials with higher ion storage capacities and improved cyclability. These advancements highlight AIBs' potential as a promising alternative for large-scale energy storage applications.

Areal capacity balance to maximize the lifetime of layered oxide/hard carbon sodium-ion batteries

Optimizing the areal capacity balance between the negative and positive electrodes is crucial for enhancing the performance of sodium-ion batteries (SIBs). This study investigates NaNi1/3Fe1/3Mn1/3O₂ || hard carbon full cells with varying N/P ratios, employing three-electrode measurements to evaluate cycling performance and identify failure mechanisms in situ. A novel full cell design principle is proposed to determine the threshold N/P ratio for sodium plating. Electrochemical tests demonstrate that an N/P ratio slightly above the threshold value, particularly around 0.9, provides the best cycling performance within 1.5–4.1 V. The cycling degradation mechanism with different N/P ratios was also elucidated. It is due to either the PE or NE exceeding its critical window, leading to active material loss on the positive side and loss of sodium inventory on the negative side. The research further emphasizes that reasonably adjusting the working voltage window can significantly extend the battery's lifetime by suppressing degradation processes. The optimized cell, with an N/P ratio of 0.9 and operating within a 1.0–4.0 V window, demonstrates an 81 % capacity retention over 500 cycles. These findings provide a practical framework for designing high-performance SIBs that balance energy density and longevity.

Unraveling the contribution of nucleation to the intercalation energy barrier for phase-transforming Li-ion battery materials

Phase-transforming intercalation compounds, such as LiFePO4 (LFP) and Li4Ti5O12 (LTO), are widely utilized in Li-ion batteries, particularly for applications requiring high power and operation at low temperatures. However, the impact of phase transformation kinetics on energy density losses under extreme conditions has been largely unexplored. Specifically, the role of nucleation, the initial stage of phase transformation, in contributing to battery performance losses has not been previously investigated. In this study, we not only quantified the significance of material-level factors, such as interfacial charge transfer, in the low-temperature and high-rate performance of LFP and LTO materials, but also provided the first estimates of the apparent activation energies of nucleation. Our findings revealed that nucleation, particularly in the case of LFP, contributes significantly to overpotential, highlighting its pivotal role among material-level factors. Furthermore, our analysis allowed us to differentiate between material-level and particle-level limitations for the LTO/LFP cell, emphasizing the paramount importance of controlling the porosity of secondary particles to ensure high tolerance towards high-rate/low-temperature discharge.

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.

Recyclability study for the next generation of cobalt-free lithium-ion battery systems with C-LNMO, Si/C- LRLO and TiNbO-LNMO active materials via hydrometallurgical route

The scarcity and uncertain supply of cobalt poses significant challenges for the lithium-ion battery industry. To address this issue, alternative chemistries excluding cobalt have been developed. Despite solving supply issues, these developments raise concerns about recyclability and their impact on current recycling trends.This study presents a recycling strategy and evaluates its performance for next-generation cobalt-free lithium-ion batteries. It focuses on three prototypes that use innovative cathode materials (titanium niobium oxide, carbon, and silicon/carbon) and electrolyte systems (ionic liquid and gelified). The proposed recycling process includes pyrolysis, mechanical separation, neutral and acid leaching, cementation, and neutralisation for selective metal separation.The results indicate that gelified electrolytes exhibit greater thermal stability than their liquid counterparts, indicating an effect on the degradation temperature and gas emissions, which are crucial for metal recovery. This study highlights the reduced toxicity of ionic liquid electrolytes and emphasises the need for strict pyrolysis gas handling due to hazardous emissions. High recovery rates (65–90 %) were achieved for nickel, manganese, lithium, and anode components.With potential for process optimisation to improve the quality of products, this study shows that cobalt-free battery systems can be integrated into existing recycling frameworks with adjustments, supporting progress towards sustainable battery practices.

A novel insight into the enhanced electrochemical performance of Mg-air battery in mixed aqueous and organic electrolytes

A new strategy of utilizing mixtures of ethanol and complexing agents on Mg-air battery is investigated systematically. The presence of ethanol promotes formation of a dense inner layer with a high portion of oxide in the discharge film, leading to significantly enhanced utilization efficiency. The highest utilization efficiency of Mg anode has been increased from 53.6 % to 85.7 % and the discharge potential is decreased 300 mV, when discharges in mixed electrolyte. The adsorption/deposition of S-like species on metal surface is evidenced in ethanol and 5-sulfosalicylate acid containing solution, resulting in inhibition of the hydroxide-rich outer layer growth.

In Operando Health Monitoring for Lithium-Ion Batteries in Electric Propulsion Using Deep Learning

Battery management systems (BMSs) play a vital role in understanding battery performance under extreme conditions such as high C-rate testing, where rapid charge or discharge is applied to batteries. This study presents a novel BMS tailored for continuous monitoring, transmission, and storage of essential parameters such as voltage, current, and temperature in an NCA 18650 4S lithium-ion battery (LIB) pack during high C-rate testing. By incorporating deep learning, our BMS monitors external battery parameters and predicts LIB’s health in terms of discharge capacity. Two experiments were conducted: a static experiment to validate the functionality of BMS, and an in operando experiment on an electrically propelled vehicle to assess real-world performance under high C-rate abuse testing with vibration. It was found that the external surface temperatures peaked at 55 °C during in operando flight, which was higher than that during static testing. During testing, the deep learning capacity estimation algorithm detected a mean capacity deviation of 0.04 Ah, showing an accurate state of health (SOH) by predicting the capacity of the battery. Our BMS demonstrated effective data collection and predictive capabilities, mirroring real-world conditions during abuse testing.

Entropy-Stabilized Multication Fluorides as a Conversion-Type Cathode for Li-Ion Batteries-Impact of Element Selection.

Metal fluorides (e.g., FeF2 and FeF3) have received attention as conversion-type cathode materials for Li-ion batteries due to their higher theoretical capacity compared to that of common intercalation materials. However, their practical use has been hindered by low round-trip efficiency, voltage hysteresis, and capacity fading. Cation substitution has been proposed to address these challenges, and recent advancements in battery performance involve the introduction of entropy stabilization in an attempt to facilitate reversible conversion reactions by increasing configurational entropy. Building on this concept, high entropy fluorides with five cations were synthesized by using a simple mechanochemical route. In order to examine the impact of element selection, Co0.2Cu0.2Ni0.2Zn0.2Fe0.2F2 (HEF-Fe) was compared with Co0.2Cu0.2Ni0.2Zn0.2Mg0.2F2 (HEF-Mg), replacing electrochemically inactive Mg with Fe as an active participant in the conversion reaction. Combining electrochemical measurements with first-principles calculations, high-resolution electron microscopy, and synchrotron X-ray analysis, HEFs' battery performances and conversion reaction mechanisms were investigated in detail. The results highlighted that replacement of Mg with Fe was beneficial, with enhanced capacity, rate capability, and surface stability. In addition, it was found that HEF-Fe showed similar cycle stability without an electrochemically inactive element. These findings provide valuable insights for the design of high entropy multielement fluorides for improved Li-ion battery performance.

Exploring Mo2B MBene as a high-capacity anode material for multi-valent metal-ion batteries: Insights from first-principles calculations

A novel class of 2-dimensional (2D) materials, known as MBenes, has recently been proposed as a promising candidate for electrode applications in metal-ion batteries due to their high conductivity and rich chemistry. In this study, we present a computational investigation into the potential of Mo2B MBene as an anode material for Na-, Mg-, and Al-ion batteries. Using density functional theory (DFT) calculations, we examine the structural, electronic, and electrochemical properties of both H- and T-type configurations of Mo2B. Our findings reveal that Mo2B exhibits metallic behavior and excellent metal adsorption characteristics, with Al exhibiting the strongest binding affinity, followed by Mg and Na. This strong binding, especially with Al, although results in higher diffusion barriers, it enhances layer adsorption leading to increased theoretical capacity. The calculated maximum capacities are significant, with Al (1323 mAh g−1) showing the highest capacity, followed by Mg (923 mAh g−1) and Na (216 mAh g−1). Additionally, the open-circuit voltage (OCV) for all metals ranges between 0.1 and 1.0 V, suggesting the suitability of Mo2B MBene as an anode material that minimizes dendrite formation risks. These results indicate the potential of Mo2B for high-performance multi-valence ion batteries, with particular promise for Al-ion batteries due to their superior capacity. Furthermore, we propose that strain engineering could optimize Mo2B for enhanced performance in Na-ion batteries. Overall, this study suggests Mo2B MBene as a highly promising anode material for next-generation metal-ion batteries, offering significant advantages in terms of capacity, voltage, and safety. Our findings provide insights that could be used for further experimental design of Mo2B-based anodes for energy storage technologies.

Performance study of GaN-based betavoltaic nuclear batteries with 3D interfaces

This study presents a design of a 3D interface simulation model featuring an inverted pyramid structure. Our objective is to forecast the performance of GaN-based betavoltaic nuclear batteries with the PN junction 3D interface structures comparing a practical machining process. Initially, we computed the electron-hole pairs (EHPs) generation rate in GaN materials irradiated by both 63Ni and 147Pm sources using Geant4. Furthermore, we employed COMSOL Multiphysics, a finite element analysis software, to simulate the EHPs transport phenomena within the battery and investigate the influence of structural parameters on the output performance. Despite maintaining thicknesses of the P- and N-regions and consistent doping concentrations (Hp-GaN, Hn-GaN, Na, and Nd) as constants, the simulation results revealed notable disparities in the short-circuit current density (Jsc), open-circuit voltage (Voc), and maximum output power density (Pmax) among batteries irradiated with various radioactive sources. Subsequently, we investigated the output performance of the nuclear battery by altering parameters such as the number of inverted pyramid structures, junction depth, and type of radioactive source. Our investigation revealed that selecting 63Ni as the radioactive source, with Na at 1017 cm−3, Nd at 1014 cm−3, a junction depth of 0.1 μm, and inverted pyramid structures of 25, resulted in the following battery performance parameters: a short-circuit current density (Jsc) of 0.648 μA/cm2, an open-circuit voltage (Voc) of 2.3481 V, and a maximum output power density (Pmax) of 1.2949 μW/cm2. Substituting the radioactive source with 147Pm, the average short-circuit current density, Jsc, increased to 56.865 μA/cm2, and the maximum output power density, Pmax, increased to 94.975 μW/cm2, It's a significant enhancement in output performance.

Impact of Laser Ablation Strategies on Electrochemical Performances of 3D Batteries Containing Aqueous Acid Processed Li(Ni0.6Mn0.2Co0.2)O2 Cathodes with High Mass Loading

Lithium-ion batteries are currently one of the most important energy storage devices for various applications. However, it remains a great challenge to achieve both high energy density and high-power density while reducing the production costs. Cells with three-dimensional electrodes realized by laser ablation are proven to have enhanced electrochemical performance compared to those with conventional two-dimensional electrodes, especially at fast charging/discharging. Nevertheless, laser structuring of electrodes is still limited in terms of achievable processing speed, and the upscaling of the laser structuring process is of great importance to gain a high technology readiness level. In the presented research, the impact of different laser structuring strategies on the electro-chemical performance was investigated on aqueous processed Li(Ni0.6Mn0.2Co0.2)O2 cathodes with acid addition during the slurry mixing process. Rate capability analyses of cells with laser structured aqueous processed electrodes exhibited enhanced performance with capacity increases of up to 60 mAh/g at high current density, while a 65% decrease in ionic resistance was observed for cells with laser structured electrodes. In addition, pouch cells with laser structured acid-added electrodes maintained 29–38% higher cell capacity after 500 cycles and their end-of-life was extended by a factor of about 4 in contrast to the reference cells with two-dimensional electrodes containing common organic solvent processed polyvinylidene fluoride binder.

Enhanced carbon host with N-reinforced S-sites to catalyze rapid iodine conversion kinetics for Zn-I2 battery

Aqueous zinc-iodine (Zn-I2) battery is a promising energy storage system in the establishment of a low-carbon, clean society, but they are limited by unsatisfied reversible capacity and poor cycle life. Ultimately, this is due to the poor iodine conversion kinetics and the shuttle effect of the intermediate polyiodide. Herein, a N-reinforced S-site carbon host (labeled as NS-YP80F) is designed to resolve these issues. DFT calculation shows that the electrochemical activity of the NS-YP80F with abundant S-site can be further enhanced by introducing N-atom at the original S-site. The synergistic effect of N-reinforced S-site carbon host cannot only enhance the adsorption of polyiodide to avoid the shuttle effect, but also induce the smooth conversion of iodine through enhanced catalytic mechanism. Consequently, the Zn-I2 battery with NS-YP80F@I2 cathode shows high reversible capacity (127 mAh g−1 at 1C) and stable cycling lifespan (15,000 cycles) with a high current density of 50 C. This strategy achieved a breakthrough in the electrochemical activity of the heteroatom doping carbon hosts, and provided a simple and effective solution for optimizing the performance of Zn-I2 battery.