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Keywords = lithium-ion transference number

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23 pages, 7464 KB  
Article
Thermal–Hydraulic Optimization of a Metal Foam Manifold Cold Plate for Energy Storage Battery Systems Using CFD and Machine Learning
by Xiang Li, Yilan Yin, Jun Ren, Hanshen Li and Benjun Xie
Batteries 2026, 12(8), 268; https://doi.org/10.3390/batteries12080268 - 23 Jul 2026
Viewed by 34
Abstract
This work presents a new Battery Thermal Management System (BTMS) concept utilizing a metal foam manifold cold plate (MFMCP), developed specifically to meet the rising thermal dissipation needs of lithium-ion batteries. By coupling a manifold flow design and high-conductivity metal foams (characterized via [...] Read more.
This work presents a new Battery Thermal Management System (BTMS) concept utilizing a metal foam manifold cold plate (MFMCP), developed specifically to meet the rising thermal dissipation needs of lithium-ion batteries. By coupling a manifold flow design and high-conductivity metal foams (characterized via SEM), the system significantly enhanced heat transfer and temperature uniformity. A Local Thermal Equilibrium (LTE) model evaluated thermal–hydraulic performance across varying Reynolds numbers (40–200), foam structures (PPI and porosity), and Al2O3 nanofluid concentrations. Results indicated that an optimal foam structure (95 PPI, porosity of 0.905) yielded a significant surface temperature reduction of 15 K. Although the Al2O3 nanofluid provided an additional cooling effect of 0.3 K, its pressure penalty lowered the performance evaluation criterion (PEC); the highest initial PEC of 2.57 was established when employing the pure base fluid without any functional additives. A Multi-Layer Perceptron (MLP) model was developed to expedite design validation, achieving high predictive accuracy as evidenced by an R2 of 0.983 and an MRE of 1.8%. Subsequent optimization via a genetic algorithm (GA) further increased the maximum PEC by 12% to 2.88. Equal pumping power system simulations indicated that the MFMCP design achieved a peak cell temperature of 304.35 K, outperforming traditional designs which peaked at 308.33 K. Furthermore, transient tests at 1C to 2C discharge rates confirmed consistent cooling improvements, demonstrating the MFMCP’s promising potential for dynamic operational conditions. Full article
(This article belongs to the Special Issue Thermal Management System for Lithium-Ion Batteries: 3rd Edition)
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15 pages, 4627 KB  
Article
Balanced Solvation and Ion Transport in a Salt-Regulated Ether Electrolyte for Fast-Charging Li-Ion Batteries
by Shenao Liu, Xinglin Jiang, Hao Li, Qi Sun and Haitao Zhang
J. Compos. Sci. 2026, 10(7), 365; https://doi.org/10.3390/jcs10070365 - 8 Jul 2026
Viewed by 411
Abstract
Fast-charging graphite-based lithium-ion batteries (LIBs) are limited by sluggish Li+ desolvation, interfacial charge transfer, and solid-state diffusion in graphite (Gr). Herein, a salt-concentration-regulated lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in 1,3-dioxolane (DOL) and fluoroethylene carbonate (FEC) electrolyte is developed to construct an anion-involved solvation structure [...] Read more.
Fast-charging graphite-based lithium-ion batteries (LIBs) are limited by sluggish Li+ desolvation, interfacial charge transfer, and solid-state diffusion in graphite (Gr). Herein, a salt-concentration-regulated lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) in 1,3-dioxolane (DOL) and fluoroethylene carbonate (FEC) electrolyte is developed to construct an anion-involved solvation structure for fast-charging graphite-based LIBs. At an appropriate LiTFSI concentration, TFSI is incorporated into the primary Li+ solvation sheath, forming a contact-ion-pair (CIP)-dominated solvation structure. The optimized electrolyte exhibits a Li+ transference number of 0.76 and an exchange current density of 0.28 mA cm−2, indicating accelerated Li+ transport and interfacial charge transfer. Furthermore, a more uniform interfacial Li+ flux distribution is obtained, contributing to suppressed localized Li growth. As a result, Gr||Li half cells deliver 168 mAh g−1 at 10 C (1 C = 370 mAh g−1). LFP||Gr full cells with an LiFePO4 (LFP) areal capacity of 4 mAh cm−2 deliver 115 mAh g−1 at 2 C and retain 69% capacity after 200 cycles. This work highlights moderate salt-concentration regulation in DOL/FEC electrolytes as an effective strategy for fast graphite lithiation without relying on fluorinated ether solvents or localized high-concentration formulations. Full article
(This article belongs to the Special Issue Composite Materials for Energy Management, Storage or Transportation)
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17 pages, 12997 KB  
Article
Effect of Pore Structure Parameters on Thermal Insulation Performance of Porous Ceramics Fabricated by Material Jetting
by Qintao Shen, Peng Wang, Chunan Song, Chao Ding, Yapeng Ning, Viboon Saetang, Mengji Shen, Yaxuan Wei, Jiying Wang, Renquan Ji, Xin Yang and Huan Qi
Materials 2026, 19(12), 2667; https://doi.org/10.3390/ma19122667 - 21 Jun 2026
Cited by 5 | Viewed by 353
Abstract
Porous ceramics have shown great application potential in aerospace, electronics, and lithium-ion battery thermal management due to their low density, high specific strength, and excellent thermal insulation. Material Jetting (MJ), a high-precision 3D printing technology, enables the fabrication of porous ceramics with tailored [...] Read more.
Porous ceramics have shown great application potential in aerospace, electronics, and lithium-ion battery thermal management due to their low density, high specific strength, and excellent thermal insulation. Material Jetting (MJ), a high-precision 3D printing technology, enables the fabrication of porous ceramics with tailored pore structures, but the synergistic effects of pore structure parameters (configuration, porosity, and number of periods) on their thermal insulation performance remain insufficiently explored. This study systematically investigates the thermal insulation behavior of zirconia porous ceramics fabricated by MJ through experimental tests and numerical simulations. Three typical lattice configurations (Octet, Schwarz, and Gyroid) were selected, and samples with varying porosities (40%, 50%, 60%) and numbers of periods (1, 2, 3) were prepared. The results indicate that the Octet configuration (60% porosity, 3 periods) exhibits the optimal thermal insulation performance, with a minimum cold-end temperature of 58.5 °C (experiment) and 59.21 °C (simulation), attributed to its strut-based structure that forms a more tortuous heat conduction path. For the Gyroid configuration, thermal insulation performance improves with increasing porosity (reducing solid conduction dominance under non-forced convection) and decreases with decreasing number of periods (due to inhomogeneous pore distribution extending heat transfer paths). Notably, the trend of porosity affecting thermal insulation is opposite to that of compressive performance. Numerical simulation results are consistent with experimental data in both values and trends, verifying the reliability of the model. This work clarifies the key factors regulating the thermal insulation of MJ-fabricated porous ceramics and provides practical structural design guidelines for applications such as lithium-ion battery thermal runaway management. Full article
(This article belongs to the Section Advanced and Functional Ceramics and Glasses)
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18 pages, 3402 KB  
Article
Gel Polymer Electrolyte Membranes via Slit-Coating Technology for High-Energy Lithium Batteries
by Pengzhen Chen, Xinghua Liang, Te Zheng, Lei Zhang, Jiajia Dong, Yangying Ou, Lingxiao Lan and Jianghua Wei
Gels 2026, 12(6), 534; https://doi.org/10.3390/gels12060534 - 14 Jun 2026
Viewed by 449
Abstract
Liquid electrolytes in conventional lithium-ion batteries pose safety risks associated with flammability, leakage, and explosion, whereas solid polymer electrolytes are generally limited by insufficient ionic conductivity at ambient temperature, restricting the development of high-energy lithium batteries. To address these issues, flexible poly (vinylidene [...] Read more.
Liquid electrolytes in conventional lithium-ion batteries pose safety risks associated with flammability, leakage, and explosion, whereas solid polymer electrolytes are generally limited by insufficient ionic conductivity at ambient temperature, restricting the development of high-energy lithium batteries. To address these issues, flexible poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based gel polymer electrolyte membranes (GPEs) were prepared via a slit-coating process combined with UV curing. NASICON-type lithium aluminum titanium phosphate (Li1.3Al0.3Ti1.7P3O12, LATP) and garnet-type tantalum-doped lithium lanthanum zirconate (Li6.4La3Zr1.4Ta0.6O12, LLZTO) were introduced as inorganic ceramic fillers to improve the ion-transport and interfacial properties of the GPE. Among the investigated samples, the PVDF-HFP-based GPE containing 10 wt% LLZTO exhibited the best overall performance, with an ionic conductivity of 3.40 × 10−4 S·cm−1 at ambient temperature and a Li+ transference number of 0.77. Cyclic voltammetry results showed that the LLZTO-modified electrolyte membrane exhibited sharper and more symmetric redox peaks, higher peak current response, and better curve overlap during repeated cycles, indicating improved electrochemical reversibility and interfacial stability. In addition, LLZTO incorporation enhanced the mechanical strength, broadened the electrochemical stability window, and improved the flame-retardant behavior of the membrane. The LiFePO4/GPE/Li cell assembled with the optimized membrane delivered an initial discharge capacity of 160 mAh·g−1 at 0.1 C and maintained 80 mAh·g−1 at 1 C, demonstrating good rate capability. Moreover, a capacity retention of 96% was maintained after 100 cycles at 0.1 C, confirming excellent cycling stability. Therefore, this work provides an effective strategy for the structural optimization and scalable preparation of high-performance gel polymer electrolyte membranes for lithium battery applications. Full article
(This article belongs to the Special Issue Gel Materials for Advanced Energy Systems and Flexible Devices)
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34 pages, 32644 KB  
Article
Predictive Active Cell Balancing for Li-Ion Batteries Using GRU-Based Voltage Estimation
by Mirela Olteanu and Dorin Petreuș
Electronics 2026, 15(10), 1985; https://doi.org/10.3390/electronics15101985 - 7 May 2026
Viewed by 533
Abstract
One of the most important functions of a battery management system (BMS) is cell balancing. The limitations of active balancing systems arise from reactive control strategies that rely exclusively on instantaneous measurements of cell voltage or state of charge (SOC). Such strategies do [...] Read more.
One of the most important functions of a battery management system (BMS) is cell balancing. The limitations of active balancing systems arise from reactive control strategies that rely exclusively on instantaneous measurements of cell voltage or state of charge (SOC). Such strategies do not account for short-term voltage dynamics, which can lead to unnecessary energy transfers. This paper proposes a predictive cell balancing strategy based on cell voltage estimation, intended for active balancing systems, particularly those employing flyback converters. The proposed predictive model uses historical voltage and current measurements, as well as operating temperature information, to estimate the short-term evolution of the cell voltage. The model is trained using experimental datasets obtained from NCR18650B lithium-ion cells (Panasonic, Osaka, Japan) subjected to multiple current profiles and temperature conditions. The proposed strategy is implemented on the DC2100B-C module (Linear Technology, Milpitas, CA, USA), which employs the LTC3300-1 integrated circuit (Linear Technology, Milpitas, CA, USA), and is experimentally validated on a battery pack consisting of 12 NCR18650B cells connected in series. The experimental results demonstrate that the use of short-term voltage prediction improves the balancing process by reducing the voltage equalization time and the number of balancing command reconfigurations. Full article
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37 pages, 8194 KB  
Article
Multi-Objective Optimization on Enhanced Heat Transfer and Pumping Power of Cooling Plate-Based Indirect Cooling System for 6S2P Lithium-Ion Battery Module
by Jin-Hyeok Park, Tai Duc Le and Moo-Yeon Lee
Energies 2026, 19(9), 2218; https://doi.org/10.3390/en19092218 - 3 May 2026
Cited by 1 | Viewed by 834
Abstract
This study proposes a multi-objective optimization framework for a cooling plate-based indirect liquid cooling system applied to a 6S2P lithium-ion battery module during 3C fast charging. A three-dimensional computational fluid dynamics (CFD) model coupled with the multi-scale multi-domain (MSMD)–Newman–Tiedemann–Gu–Kim (NTGK) battery heat generation [...] Read more.
This study proposes a multi-objective optimization framework for a cooling plate-based indirect liquid cooling system applied to a 6S2P lithium-ion battery module during 3C fast charging. A three-dimensional computational fluid dynamics (CFD) model coupled with the multi-scale multi-domain (MSMD)–Newman–Tiedemann–Gu–Kim (NTGK) battery heat generation model was developed to investigate the system thermal–hydraulic behavior. The numerical model was experimentally validated through single-cell charging tests, with temperature deviations below 5%, confirming its reliability. A systematic parametric analysis was conducted to evaluate the effects of coolant channel number, channel width, channel spacing, and coolant mass flow rate on maximum temperature (Tmax), temperature difference (ΔT), and pressure drop (ΔP). The results indicated that increasing the coolant flow rate significantly enhanced thermal performance but caused a substantial increase in hydraulic losses, whereas geometric parameters had comparatively smaller effects. To improve optimization efficiency, 30 design samples were generated using Latin hypercube sampling and used to train ANN surrogate models, which demonstrated high predictive accuracy with test R2 values of 0.9931, 0.9960, and 0.9842 for Tmax, ΔT, and pumping power (Ppump), respectively. Subsequently, NSGA-II combined with TOPSIS identified the optimal design with a channel width of 6.22 mm, channel spacing of 4.84 mm, and coolant flow rate of 2.55 LPM. Under these conditions, the optimized system achieved a Tmax of 30.47 °C, a ΔT of 4.50 °C, and a Ppump of 0.05879 W. The relative deviations between ANN predictions and CFD results were all below 1%, demonstrating the robustness of the proposed optimization framework. These findings provide an effective design methodology for enhancing heat transfer while minimizing pumping power in advanced battery thermal management systems. Full article
(This article belongs to the Special Issue Recent Advances in Heat Transfer and Fluid Flow)
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12 pages, 2298 KB  
Article
Interfacial In Situ Polymerization of DOL for High-Performance Solid-State Lithium Metal Batteries
by Jintian Wu, Zixuan Fang and Lifen Wang
Energies 2026, 19(9), 2158; https://doi.org/10.3390/en19092158 - 29 Apr 2026
Viewed by 684
Abstract
Limited ionic conductivity and unstable interfaces, primarily caused by poor solid–solid contact, pose significant challenges to the stable cycling of solid-state batteries. In this study, an interfacial in situ polymerization strategy is proposed to construct a poly(1,3-dioxolane) (PDOL) gel electrolyte layer between a [...] Read more.
Limited ionic conductivity and unstable interfaces, primarily caused by poor solid–solid contact, pose significant challenges to the stable cycling of solid-state batteries. In this study, an interfacial in situ polymerization strategy is proposed to construct a poly(1,3-dioxolane) (PDOL) gel electrolyte layer between a poly(vinylidene fluoride) (PVDF)-based solid polymer electrolyte and the electrodes. This approach aims to address interfacial compatibility issues in solid-state lithium metal batteries. By precisely tuning the composition of the gel precursor and employing characterization techniques such as FTIR and NMR, the efficient ring-opening polymerization of 1,3-dioxolane (DOL) was confirmed, achieving a high conversion rate of 90%. The precursor was drop-cast onto the PVDF-based electrolyte/electrode interfaces before cell assembly. Electrochemical evaluations revealed that the in situ formed solidified interlayer significantly enhanced interfacial compatibility and ion transport, yielding a high Li+ transference number (0.341), an exceptional critical current density (1.4 mA cm−2), and remarkable cycling stability exceeding 1600 h in Li||Li symmetric cells. Furthermore, full cells incorporating LiFePO4 cathodes demonstrated excellent rate capability and long-term cyclability, retaining 98.7% of their capacity after 1000 cycles. These results collectively underscore the effectiveness of this in situ solidification strategy in optimizing the interface structure and improving the overall performance of PVDF-based solid-state batteries. Full article
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19 pages, 14779 KB  
Article
Numerical Investigation on the Thermal Management Performance of the PCM and Fin Network Structure for Lithium-Ion Batteries
by Yiyao Chu, Shian Li, Ruiyang Zhang and Qiuwan Shen
J. Mar. Sci. Eng. 2026, 14(9), 776; https://doi.org/10.3390/jmse14090776 - 23 Apr 2026
Viewed by 675
Abstract
With the accelerated transformation of green shipping and the advancement of ship electrification, lithium-ion batteries have become the core solution for ship propulsion due to their advantages of high energy density and zero emission. Efficient thermal management serves as a key technical support [...] Read more.
With the accelerated transformation of green shipping and the advancement of ship electrification, lithium-ion batteries have become the core solution for ship propulsion due to their advantages of high energy density and zero emission. Efficient thermal management serves as a key technical support to ensure the safe and stable operation of batteries, extend their service life, and mitigate the risk of thermal runaway. Lithium-ion batteries accumulate heat during discharge, and pure phase change material (PCM) cooling systems are limited by low thermal conductivity, leading to excessive battery temperature rise and poor temperature uniformity. To address this problem, RT42 (a paraffin-based PCM with a melting temperature range of 311.15–316.15 K) was selected as the PCM in this study. The battery thermal management system (BTMS) coupling RT42 with a three-dimensional fin network structure was designed. Numerical simulations were conducted via ANSYS Fluent, and the enthalpy-porosity method was adopted to simulate the PCM phase change process. The effects of fin distribution, spacing and layer number on BTMS performance were systematically investigated and compared. Results show that the heat transfer process in the PCM can be significantly improved due to the three-dimensional fin network, and the battery maximum temperature can be reduced by 7.53 K compared with the pure PCM system. This study provides theoretical support for the design and optimization of high-efficiency BTMS. Full article
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16 pages, 2074 KB  
Article
A Polymer Electrolyte with Rigid–Flexible Coupled Architecture for High-Voltage Lithium-Metal Batteries
by Haoru Xie, Zhengyin Yao, Zhen Liu, Ruiyong Chen and Peng Zhang
Polymers 2026, 18(8), 987; https://doi.org/10.3390/polym18080987 - 18 Apr 2026
Viewed by 571
Abstract
A polymer electrolyte is developed by integrating a poly(methyl methacrylate) (PMMA)/eutectic electrolyte (EE) phase into a porous polyethylene (PE) scaffold via a solution-casting strategy. In this rigid–flexible coupled architecture, the PMMA matrix serves as a solid host that coordinates with Li+ through [...] Read more.
A polymer electrolyte is developed by integrating a poly(methyl methacrylate) (PMMA)/eutectic electrolyte (EE) phase into a porous polyethylene (PE) scaffold via a solution-casting strategy. In this rigid–flexible coupled architecture, the PMMA matrix serves as a solid host that coordinates with Li+ through its polar carbonyl groups, thereby promoting lithium salt dissociation and establishing a stable ion transport network. The incorporated EE, composed of ethylene carbonate and LiTFSI, effectively reduces the glassy rigidity of PMMA and provides continuous pathways for fast ionic conduction. Meanwhile, the porous PE scaffold reinforces mechanical strength and resists lithium dendrite penetration, enabling a thin electrolyte membrane with excellent flexibility. The resulting electrolyte achieves an ionic conductivity of 1.59 × 10−4 S cm−1 at 30 °C, a lithium-ion transference number of 0.45, and an electrochemical stability window up to 4.75 V. In Li||LiFePO4 cells, it delivers stable cycling at 3 C for 1000 cycles with 76.8% capacity retention and a Coulombic efficiency exceeding 99.9%. The monomer-free design eliminates residual reactive species that commonly compromise interfacial stability, offering a reliable pathway toward high-voltage solid-state lithium-metal batteries. Full article
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19 pages, 7761 KB  
Article
A Microchannel Liquid Cold Plate for Cooling Prismatic Lithium-Ion Batteries with High Discharging Rate: Full Numerical Model and Thermal Flows
by Chuang Liu, Deng-Wei Yang, Cheng-Peng Ma, Shang-Xian Zhao, Yu-Xuan Zhou and Fu-Yun Zhao
World Electr. Veh. J. 2026, 17(4), 196; https://doi.org/10.3390/wevj17040196 - 8 Apr 2026
Viewed by 1001
Abstract
The thermal safety and longevity of lithium-ion batteries are critically constrained by excessive temperature rise and spatial thermal non-uniformity, particularly during high-rate discharges. Most existing numerical investigations rely on simplified heat generation models that fail to capture the spatiotemporal heterogeneity of electrochemical heat [...] Read more.
The thermal safety and longevity of lithium-ion batteries are critically constrained by excessive temperature rise and spatial thermal non-uniformity, particularly during high-rate discharges. Most existing numerical investigations rely on simplified heat generation models that fail to capture the spatiotemporal heterogeneity of electrochemical heat sources, leading to compromised predictive accuracy. To address this deficiency, this study develops a comprehensive three-dimensional electrochemical–thermal coupled framework, integrating the Newman pseudo-two-dimensional (P2D) electrochemical model with conjugate heat transfer and laminar flow dynamics. The predictive robustness of this framework is rigorously validated against experimental data across multiple discharge rates (3 C and 5 C). The validated model is then deployed to evaluate a water-cooled microchannel cold plate designed for prismatic LiMn2O4/graphite cells under a demanding 5 C discharge. A systematic parametric investigation is conducted to quantify the effects of ambient temperature (293–343 K), microchannel number (2–6), and coolant inlet velocity (0.1–0.6 m/s) on the maximum battery temperature (Tmax) and temperature difference (ΔT). Results demonstrate that the proposed system exhibits exceptional environmental robustness: over a 50 K ambient temperature span, Tmax increases by merely 2.0 K, remaining safely below the 323 K industry limit. Densifying the channel count from 2 to 6 further reduces Tmax by 1.55 K and narrows ΔT to 4.25 K, successfully satisfying the strict 5 K temperature uniformity standard. Furthermore, the thermal benefit of elevating inlet velocity exhibits a pronounced diminishing-return trend governed by the asymptotic reduction in bulk coolant temperature rise, dictating a critical trade-off against the quadratically escalating pumping power. Ultimately, these findings provide robust theoretical guidelines for the rational design of safe and energy-efficient battery thermal management systems. Full article
(This article belongs to the Section Storage Systems)
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24 pages, 4666 KB  
Article
Numerical Study on Heat Transfer Characteristics of Microchannel with Ferrofluid Under Influence of Magnetic Intensity
by Seong-Guk Hwang, Tai Duc Le and Moo-Yeon Lee
Micromachines 2026, 17(3), 383; https://doi.org/10.3390/mi17030383 - 21 Mar 2026
Cited by 1 | Viewed by 613
Abstract
Effective thermal management is critical for high-power lithium-ion batteries to mitigate excessive heat generation and ensure operational reliability. Failure to maintain a uniform temperature distribution can lead to accelerated capacity fading and severe safety risks, such as thermal runaway. In this study, a [...] Read more.
Effective thermal management is critical for high-power lithium-ion batteries to mitigate excessive heat generation and ensure operational reliability. Failure to maintain a uniform temperature distribution can lead to accelerated capacity fading and severe safety risks, such as thermal runaway. In this study, a ferrofluid-based magnetohydrodynamic (MHD) microchannel cooling system was numerically investigated to elucidate the influence of magnetic intensity, magnet geometry, and electrical boundary conditions on flow behavior and heat transfer performance for battery cooling applications. A fully coupled multiphysics model incorporating electromagnetic, fluid flow, and heat transfer phenomena was developed and validated against experimental and numerical data from the literature. The results show that increasing the applied voltage enhances current density and Lorentz force almost linearly, leading to significant flow acceleration and improved convective heat transfer. Electrical insulation effectively suppresses current leakage into the channel walls, increasing the average current density by up to 222% and the Lorentz force by more than 300%. Compared with a cylindrical magnet, a rectangular magnet provides a more uniform magnetic field distribution and stronger near-wall Lorentz forcing, resulting in superior cooling performance. Under a 4C discharge condition, the insulated rectangular magnet reduces the maximum battery temperature by approximately 30% and increases the average Nusselt number by up to 103% relative to the non-insulated case. The findings reveal the critical roles of magnetic-field-controlled flow symmetry and near-wall forcing in MHD-driven microchannels, and provide practical design guidelines for battery cooling systems with no moving mechanical parts and active electromagnetic flow control. Full article
(This article belongs to the Special Issue Complex Fluid Flows in Microfluidics)
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17 pages, 4143 KB  
Article
Simultaneous Optimization of Bulk Ion Transport and Interfacial Stability in Gel Polymer Electrolytes via a Multifunctional Triazole Additive
by Jie Zhao, Yubo Cheng, Maoyi Yi, Chunman Zheng and Qingpeng Guo
Batteries 2026, 12(3), 101; https://doi.org/10.3390/batteries12030101 - 16 Mar 2026
Viewed by 708
Abstract
Gel polymer electrolytes (GPEs) typically suffer from sluggish kinetics and interfacial instability at elevated temperatures and high voltages. Herein, 3-(trifluoromethyl)-1H-1,2,4-triazole (TTA) is employed to construct an ultrathin (~25 μm), robust, and homogeneous GPE. TTA acts as a molecular bridge, significantly improving compatibility between [...] Read more.
Gel polymer electrolytes (GPEs) typically suffer from sluggish kinetics and interfacial instability at elevated temperatures and high voltages. Herein, 3-(trifluoromethyl)-1H-1,2,4-triazole (TTA) is employed to construct an ultrathin (~25 μm), robust, and homogeneous GPE. TTA acts as a molecular bridge, significantly improving compatibility between the PVDF-HFP (Poly(vinylidene fluoride-co-hexafluoropropylene)) matrix and LLZTO (Li6.4La3Zr1.4Ta0.6O12) fillers to create continuous ion-conducting pathways. Consequently, the TTA-GPEs exhibits high ionic conductivity (0.267 mS cm−1 at room temperature), low activation energy (0.181 eV), and an increased lithium-ion transference number (0.425). Advanced surface analysis reveals that TTA preferentially reacts to form a dense, gradient hierarchical interphase (solid electrolyte interphase/cathode electrolyte interphase, SEI/CEI) enriched with inorganic species (LiF, Li3N, and Li2S) on the inner side. This architecture suppresses parasitic reactions and lithium dendrite growth. Accordingly, NCM811(LiNi0.8Co0.1Mn0.1O2)//Li batteries with TTA-GPEs demonstrate stable cycling at 80 °C and 1C, retaining 57.68% capacity after 125 cycles—significantly outperforming benchmarks. This study offers a molecular engineering strategy to simultaneously optimize bulk transport and interfacial stability for high-energy-density solid-state batteries. Full article
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17 pages, 5259 KB  
Article
Harnessing the Dual-Charge Characteristics of Halloysite Nanotubes for High-Performance Composite Polymer Electrolytes in Lithium-Ion Batteries
by Yunxiang Li, Xuehui Li, Ke Wang, Peilin Chen, Xiaowei Li, Guocheng Lv and Libing Liao
Minerals 2026, 16(3), 307; https://doi.org/10.3390/min16030307 - 14 Mar 2026
Cited by 1 | Viewed by 540
Abstract
Naturally occurring halloysite nanotubes (HNTs), a clay mineral characterized by a unique dual-charge architecture, offer a promising strategy for enhancing the performance of composite polymer electrolyte (CPE). In this work, HNTs are introduced as a low-cost, functional filler to simultaneously address two key [...] Read more.
Naturally occurring halloysite nanotubes (HNTs), a clay mineral characterized by a unique dual-charge architecture, offer a promising strategy for enhancing the performance of composite polymer electrolyte (CPE). In this work, HNTs are introduced as a low-cost, functional filler to simultaneously address two key limitations of poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP)-based CPE: low ionic conductivity and inadequate lithium-ion transference number. The negatively charged outer surface of HNTs facilitates Li+ transport, while the positively charged inner lumen confines anions such as TFSI. Controlled acid etching (6 M HCl, 12 h) further optimizes this structure by removing surface impurities and enlarging the lumen, thereby enhancing both charge-directed ion transport pathways. The resulting HNT-modified CPE achieves a high ionic conductivity of 6.1 × 10−4 S⋅cm−1 and a Li+ transference number of 0.73. When assembled into Li||CPE||LiFePO4 cells, the electrolyte enables stable cycling over 300 cycles at 0.2C, retains 119.2 mAh/g at 2C, and delivers 85.7 mAh/g even at 5C, demonstrating excellent cycling stability and rate capability. This study reveals the potential of mineral-derived nanomaterials, with their inherent structural and physicochemical properties, to serve as key functional components in high-performance batteries. Full article
(This article belongs to the Special Issue Clay Minerals for Environmental Remediation and Sustainable Energy)
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17 pages, 2548 KB  
Article
High-Performance Solid Polymer Electrolyte Constructed from Long-Chain Regulated Random Copolymers and Porous PI Composites
by Qian Zhang, Mingyang Cao, Chenxia Tang, Yuqing Zhou and Xiaoli Peng
Polymers 2026, 18(6), 685; https://doi.org/10.3390/polym18060685 - 11 Mar 2026
Viewed by 829
Abstract
Solid polymer electrolytes (SPEs) hold great potential in high-safety energy storage but face two key bottlenecks: low room-temperature ionic conductivity and insufficient mechanical strength. This study proposes a synergistic optimization strategy of “long-carbon-chain regulation of polymer microstructure combined with porous polyimide (PI) support”. [...] Read more.
Solid polymer electrolytes (SPEs) hold great potential in high-safety energy storage but face two key bottlenecks: low room-temperature ionic conductivity and insufficient mechanical strength. This study proposes a synergistic optimization strategy of “long-carbon-chain regulation of polymer microstructure combined with porous polyimide (PI) support”. A linear random copolyester, poly(1,3-propylene-co-1,4-butylene succinate-co-sebacate) (PBPSS), was synthesized via melt polycondensation using 1,3-propanediol, 1,4-butanediol, succinic acid, and sebacic acid as monomers. Subsequently, the PBPSS-75 composite electrolyte was prepared with this copolyester as the matrix and porous PI as support. Results show that long-carbon-chain sebacic acid effectively regulates polymer segment flexibility and free volume, synergistically enhancing ionic conductivity and interfacial mechanical stability with lithium metal. Experimental data indicate that PBPSS-75 composite electrolyte exhibits an ionic conductivity of up to 4.25 × 10−5 S cm−1 (30 °C), a lithium-ion transference number of 0.81, and an electrochemical stability window of 4.48 V (vs. Li/Li+). In LiFePO4//Li batteries, it maintains nearly 100% capacity retention after 300 cycles at 0.5 C, and achieves stable cycling for over 800 h in lithium symmetric cells. This study confirms that the combined strategy effectively addresses the conductivity-mechanical property trade-off of SPEs, providing theoretical guidance and technical reference for high-performance solid-state battery material design. Full article
(This article belongs to the Special Issue Self-Healing Polymers for Advanced Battery Applications)
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15 pages, 3276 KB  
Article
The Application of Polyrotaxane Cellulose Composite Materials in Quasi-Solid Electrolytes
by Tianyi Wang, Wenzhuo Chen, Yichen Liu, Kailiang Ren, Jin Liang and Jie Kong
Bioengineering 2026, 13(3), 292; https://doi.org/10.3390/bioengineering13030292 - 28 Feb 2026
Viewed by 871
Abstract
Due to its affordability, widespread availability, non-toxicity, biodegradability, and renewability, cellulose is considered a crucial material for addressing the depletion of petroleum resources. In this study, a rotaxane-based supramolecular polymer derived from thermoplastic polyurethane (TPU) was synthesized and combined with cellulose to create [...] Read more.
Due to its affordability, widespread availability, non-toxicity, biodegradability, and renewability, cellulose is considered a crucial material for addressing the depletion of petroleum resources. In this study, a rotaxane-based supramolecular polymer derived from thermoplastic polyurethane (TPU) was synthesized and combined with cellulose to create a TPU–cellulose composite (TPU-C). This composite was employed as a separator for acrylate-based quasi-solid polymer electrolytes (QPEs). The polymer electrolyte demonstrated a high ionic conductivity of 0.16 mS cm−1 at room temperature, a lithium-ion transference number of 0.63, and an electrochemical stability window extending up to 4.7 V. When paired with a LiFePO4 (LFP) cathode, the coin cell retained 88.8% of its capacity after 100 cycles at 1 C. A cell assembled with Li and a high-voltage NCM622 cathode maintained a capacity of 65.8% after 100 cycles at 0.3 C. Additionally, the excellent electrochemical performance was analyzed through density functional theory (DFT) calculations to identify the underlying reasons for its outstanding behavior. This study offers new insights into expanding the application potential of cellulose-based composite materials. Full article
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