Pub Date : 2025-09-23DOI: 10.1007/s11581-025-06708-0
Kun Gao, Shu-Dan Li
Designing hybrid battery systems based on Li/Na coexisting silicate framework with synergized lithium’s high energy density with sodium’s economic advantages is still challenging. Herein, a series of Li2-xNaxFeSiO4 (where x = 0, 0.25, 0.5, and 1.0) cathode materials were constructed through vibratory ball milling-assisted solid-state synthesis. The optimized sample at the composition x = 0.25 showed a single-phase monoclinic P21-Li2FeSiO4 phase, with exceptional electrochemical performances. By contrast, higher sodium contents (x ≥ 0.5) resulted in dual-phase mixtures of Na2FeSiO4 and Li2FeSiO4, along with some undesirable impurities of Li5FeO4 and Na6Si2O7. The electrochemical characterization revealed that the introduction of sodium ions in the deintercalation reaction increased the interfacial charge transfer resistance (Rct) due to the Na+ barrier, but also significantly improved the Li+ diffusion coefficient (DLi⁺), suitable for enhancing ionic utilization efficiency for an optimized specific capacity. Overall, strategically incorporating sodium at lithium sites can effectively increase the storage capacity while reducing dependence on lithium resources for economical energy storage devices.
{"title":"Synthesis and performance of lithium/sodium iron-based silicate cathode prepared by a facile vibratory ball milling-assisted solid-phase method","authors":"Kun Gao, Shu-Dan Li","doi":"10.1007/s11581-025-06708-0","DOIUrl":"10.1007/s11581-025-06708-0","url":null,"abstract":"<div><p>Designing hybrid battery systems based on Li/Na coexisting silicate framework with synergized lithium’s high energy density with sodium’s economic advantages is still challenging. Herein, a series of Li<sub>2-<i>x</i></sub>Na<sub><i>x</i></sub>FeSiO<sub>4</sub> (where <i>x</i> = 0, 0.25, 0.5, and 1.0) cathode materials were constructed through vibratory ball milling-assisted solid-state synthesis. The optimized sample at the composition <i>x</i> = 0.25 showed a single-phase monoclinic P2<sub>1</sub>-Li<sub>2</sub>FeSiO<sub>4</sub> phase, with exceptional electrochemical performances. By contrast, higher sodium contents (<i>x</i> ≥ 0.5) resulted in dual-phase mixtures of Na<sub>2</sub>FeSiO<sub>4</sub> and Li<sub>2</sub>FeSiO<sub>4</sub>, along with some undesirable impurities of Li<sub>5</sub>FeO<sub>4</sub> and Na<sub>6</sub>Si<sub>2</sub>O<sub>7</sub>. The electrochemical characterization revealed that the introduction of sodium ions in the deintercalation reaction increased the interfacial charge transfer resistance (<i>R</i><sub>ct</sub>) due to the Na<sup>+</sup> barrier, but also significantly improved the Li<sup>+</sup> diffusion coefficient (<i>D</i><sub>Li⁺</sub>), suitable for enhancing ionic utilization efficiency for an optimized specific capacity. Overall, strategically incorporating sodium at lithium sites can effectively increase the storage capacity while reducing dependence on lithium resources for economical energy storage devices.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11555 - 11563"},"PeriodicalIF":2.6,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-22DOI: 10.1007/s11581-025-06680-9
Mingfang Kang, Fenglian Lu, Tong Liu, Song Li, Rui Tu, Sha Luo, Keliang Wang
To respond to the issue of weak conductivity and structural instability of MOF materials applied in the intrinsic characterization of lithium-ion batteries. In this paper, Ni-MOF and its complex with graphene (Ni-MOF/GR) have been successfully synthesized by one-step solvothermal method, which improved the electrochemical performance of Ni-MOF electrode. The morphology, structure, and composition of the electrode were also determined using SEM, XRD, FTIR, and XPS. Binding energy of Ni-MOF/GR is calculated to reach − 0.79 eV by density-functional theory (DFT). Graphene (GR) transfers charge 1.017 e to Ni-MOF. Simultaneous characterization by the four-probe method revealed that GR addition increased the conductivity by eight orders of magnitude (4.81 × 10−8–6.00 S/cm), which is consistent with the density of states (DOS) calculations. In comparison with the intrinsic Ni-MOF, cycling and rate properties of Ni-MOF/GR composite anode were substantially enhanced. When the charge/discharge test was conducted at 5 C rate, Ni-MOF/GR retained a discharge specific capacity up to 368.4 mAh g−1 despite 500 cycles, nearly two times more than Ni-MOF (only 185.1 mAh g−1). Additionally, the average specific capacity of Ni-MOF/GR material (958.01–500.66 mAh g−1) showed a higher recovery rate than that of pristine Ni-MOF (1106.7–297.38 mAh g−1) when charge/discharge tests were performed at different rates. In this work, it is shown that composite GR can improve the electronic conductivity and structural stability of materials, which is indispensable for enhancing the capacity, rate performance, and cycling stability of materials.
针对MOF材料在锂离子电池特性表征中存在的导电性弱、结构不稳定等问题。本文采用一步溶剂热法成功合成了Ni-MOF及其与石墨烯的配合物(Ni-MOF/GR),提高了Ni-MOF电极的电化学性能。采用SEM、XRD、FTIR和XPS等方法对电极的形貌、结构和组成进行了表征。利用密度泛函理论(DFT)计算出Ni-MOF/GR的结合能达到- 0.79 eV。石墨烯(GR)将1.017 e的电荷转移到Ni-MOF。通过四探针法的同时表征表明,GR的加入使电导率提高了8个数量级(4.81 × 10−8-6.00 S/cm),这与态密度(DOS)的计算结果一致。与Ni-MOF相比,Ni-MOF/GR复合阳极的循环性能和速率性能得到了显著提高。在5℃充放电条件下,经过500次循环,Ni-MOF/GR的放电比容量高达368.4 mAh g−1,几乎是Ni-MOF (185.1 mAh g−1)的两倍。在不同充放电速率下,Ni-MOF/GR材料的平均比容量(958.01 ~ 500.66 mAh g−1)的回收率高于原始Ni-MOF材料(1106.7 ~ 297.38 mAh g−1)。本研究表明,复合GR可以提高材料的电子导电性和结构稳定性,这对于提高材料的容量、速率性能和循环稳定性是必不可少的。
{"title":"Needle-shaped Ni-MOF/GR composite anode for superior lithium storage performance","authors":"Mingfang Kang, Fenglian Lu, Tong Liu, Song Li, Rui Tu, Sha Luo, Keliang Wang","doi":"10.1007/s11581-025-06680-9","DOIUrl":"10.1007/s11581-025-06680-9","url":null,"abstract":"<p>To respond to the issue of weak conductivity and structural instability of MOF materials applied in the intrinsic characterization of lithium-ion batteries. In this paper, Ni-MOF and its complex with graphene (Ni-MOF/GR) have been successfully synthesized by one-step solvothermal method, which improved the electrochemical performance of Ni-MOF electrode. The morphology, structure, and composition of the electrode were also determined using SEM, XRD, FTIR, and XPS. Binding energy of Ni-MOF/GR is calculated to reach − 0.79 eV by density-functional theory (DFT). Graphene (GR) transfers charge 1.017 e to Ni-MOF. Simultaneous characterization by the four-probe method revealed that GR addition increased the conductivity by eight orders of magnitude (4.81 × 10<sup>−8</sup>–6.00 S/cm), which is consistent with the density of states (DOS) calculations. In comparison with the intrinsic Ni-MOF, cycling and rate properties of Ni-MOF/GR composite anode were substantially enhanced. When the charge/discharge test was conducted at 5 C rate, Ni-MOF/GR retained a discharge specific capacity up to 368.4 mAh g<sup>−1</sup> despite 500 cycles, nearly two times more than Ni-MOF (only 185.1 mAh g<sup>−1</sup>). Additionally, the average specific capacity of Ni-MOF/GR material (958.01–500.66 mAh g<sup>−1</sup>) showed a higher recovery rate than that of pristine Ni-MOF (1106.7–297.38 mAh g<sup>−1</sup>) when charge/discharge tests were performed at different rates. In this work, it is shown that composite GR can improve the electronic conductivity and structural stability of materials, which is indispensable for enhancing the capacity, rate performance, and cycling stability of materials.</p>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11513 - 11524"},"PeriodicalIF":2.6,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561670","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
With high theoretical discharge specific capacity, excellent reversibility of electrochemical reaction, and suitable oxygen evolution overpotential, α-Ni(OH)2 is an auspicious cathode material for alkaline batteries, which supports the development of high-capacity nickel-based batteries. Nevertheless, α-Ni(OH)2 exhibits substandard structural stability and is susceptible to crystalline transformation, leading to capacity degradation, affecting the battery charge/discharge performance and cycle life. In this study, the TiO2-nickel hydroxide (TiO2-α-Ni(OH)2) is prepared by high-energy ball milling. Among them, TiO2 can be uniformly dispersed on the surface of α-Ni(OH)2, which can effectively prevent the collapse of the α-phase structure. Benefiting from the unique elemental doping technology, the TiO2-α-Ni(OH)2 composites as a nickel-metal hydride (Ni-MH) battery cathode can release a reversible specific capacity of 390 mAh g−1 at a 2 C rate for 200 cycles. A reversible specific capacity of 210 mAh g−1 is still released after 200 cycles at a 5 C rate. Consequently, TiO2-α-Ni(OH)2 is a promising candidate for high-power Ni-MH batteries.
α-Ni(OH)2具有较高的理论放电比容量、优异的电化学反应可逆性和适宜的析氧过电位,是碱性电池的理想正极材料,为大容量镍基电池的发展提供了支撑。但α-Ni(OH)2的结构稳定性不达标,易发生晶化,导致容量下降,影响电池的充放电性能和循环寿命。本研究采用高能球磨法制备了二氧化钛-氢氧化镍(TiO2-α-Ni(OH)2)。其中,TiO2能均匀分散在α-Ni(OH)2表面,能有效防止α-相结构的坍塌。得益于独特的元素掺杂技术,TiO2-α-Ni(OH)2复合材料作为镍氢(Ni-MH)电池正极,在2℃下循环200次,可释放390 mAh g−1的可逆比容量。以5℃的倍率放电200次后仍可释放210 mAh g−1的可逆比容量。因此,TiO2-α-Ni(OH)2是高功率镍氢电池的理想候选材料。
{"title":"Titanium-doped α-Ni(OH)2 as a cathode material for high-performance nickel-metal hydride batteries","authors":"Zhaomin Wang, Chaoyue Zhao, Xiaodong Niu, Yong Cheng, Limin Wang, Pai Huang","doi":"10.1007/s11581-025-06704-4","DOIUrl":"10.1007/s11581-025-06704-4","url":null,"abstract":"<div><p>With high theoretical discharge specific capacity, excellent reversibility of electrochemical reaction, and suitable oxygen evolution overpotential, <i>α</i>-Ni(OH)<sub>2</sub> is an auspicious cathode material for alkaline batteries, which supports the development of high-capacity nickel-based batteries. Nevertheless, <i>α</i>-Ni(OH)<sub>2</sub> exhibits substandard structural stability and is susceptible to crystalline transformation, leading to capacity degradation, affecting the battery charge/discharge performance and cycle life. In this study, the TiO<sub>2</sub>-nickel hydroxide (TiO<sub>2</sub>-<i>α</i>-Ni(OH)<sub>2</sub>) is prepared by high-energy ball milling. Among them, TiO<sub>2</sub> can be uniformly dispersed on the surface of <i>α</i>-Ni(OH)<sub>2</sub>, which can effectively prevent the collapse of the <i>α</i>-phase structure. Benefiting from the unique elemental doping technology, the TiO<sub>2</sub>-<i>α</i>-Ni(OH)<sub>2</sub> composites as a nickel-metal hydride (Ni-MH) battery cathode can release a reversible specific capacity of 390 mAh g<sup>−1</sup> at a 2 C rate for 200 cycles. A reversible specific capacity of 210 mAh g<sup>−1</sup> is still released after 200 cycles at a 5 C rate. Consequently, TiO<sub>2</sub>-<i>α</i>-Ni(OH)<sub>2</sub> is a promising candidate for high-power Ni-MH batteries.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11835 - 11841"},"PeriodicalIF":2.6,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561668","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-22DOI: 10.1007/s11581-025-06616-3
Ruoruo He, Junjie Jiang, Zhongzhu Qiu
Energy is an essential factor for human survival and development. With the development of new energy sources, the demand for energy storage devices has been increasing. In recent years, supercapacitors have gained more attention in the field of energy storage. Electrodes, as the core components in the energy storage process of supercapacitors, play a crucial role, and the design and preparation of electrode materials are key areas of research. Common electrode materials mainly involve carbon materials, conductive polymers, and transition metal oxides. Among them, cobalt-based nanomaterials are considered a highly promising pseudocapacitive electrode material due to their diverse valence states and excellent electrochemical performance. This article primarily reviews the research status of cobalt-based oxides, cobalt-based sulfides, cobalt-based hydroxides, cobalt-based inorganic salts, and cobalt-based phosphides as electrode materials for supercapacitors from the perspectives of synthesis methods, material morphology, and electrochemical performance. It summarizes the advantages and disadvantages of these materials, modification methods, and discusses the prospects and challenges of cobalt-based compounds and their composite materials in supercapacitor applications. Compared with previous reviews, this work integrates the most recent research findings from 2023 to 2025 and places particular emphasis on morphology control strategies (such as hollow, core–shell, and layered structures), composite design (such as integration with carbon materials or conductive polymers), and the correlation between structural features and electrochemical behavior. The goal is to provide up-to-date theoretical guidance and design strategies for the development of high-performance cobalt-based electrode materials.
{"title":"Research progress on cobalt-based compounds as electrode materials for supercapacitors","authors":"Ruoruo He, Junjie Jiang, Zhongzhu Qiu","doi":"10.1007/s11581-025-06616-3","DOIUrl":"10.1007/s11581-025-06616-3","url":null,"abstract":"<div><p>Energy is an essential factor for human survival and development. With the development of new energy sources, the demand for energy storage devices has been increasing. In recent years, supercapacitors have gained more attention in the field of energy storage. Electrodes, as the core components in the energy storage process of supercapacitors, play a crucial role, and the design and preparation of electrode materials are key areas of research. Common electrode materials mainly involve carbon materials, conductive polymers, and transition metal oxides. Among them, cobalt-based nanomaterials are considered a highly promising pseudocapacitive electrode material due to their diverse valence states and excellent electrochemical performance. This article primarily reviews the research status of cobalt-based oxides, cobalt-based sulfides, cobalt-based hydroxides, cobalt-based inorganic salts, and cobalt-based phosphides as electrode materials for supercapacitors from the perspectives of synthesis methods, material morphology, and electrochemical performance. It summarizes the advantages and disadvantages of these materials, modification methods, and discusses the prospects and challenges of cobalt-based compounds and their composite materials in supercapacitor applications. Compared with previous reviews, this work integrates the most recent research findings from 2023 to 2025 and places particular emphasis on morphology control strategies (such as hollow, core–shell, and layered structures), composite design (such as integration with carbon materials or conductive polymers), and the correlation between structural features and electrochemical behavior. The goal is to provide up-to-date theoretical guidance and design strategies for the development of high-performance cobalt-based electrode materials.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11371 - 11408"},"PeriodicalIF":2.6,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561669","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-20DOI: 10.1007/s11581-025-06701-7
Baochang Liu, Jianxin Wang, Bo Wang, Chongqing Kang
Rechargeable aqueous zinc-ion batteries (RAZIBs) have emerged as promising candidates for large-scale energy storage systems, owing to their low cost, high safety, and environmental benignity. However, their practical application is hindered by intrinsic limitations of cathode materials, including sluggish Zn2+ diffusion kinetics, poor electrical conductivity, and structural degradation during cycling. Herein, we report a facile hydrothermal strategy to synthesize Ag-doped MnO2 cathode with uniform urchin-like nanostructures surrounded by nanowires as high-performance cathodes for RAZIBs. The optimal 5 wt% Ag doping yields denser nanowire arrays, namely 5Ag/MnO2, increases accessible active sites, and introduces lattice defects while preserving the tetragonal MnO2 crystal structure (I4/m). The electrochemical characterization demonstrated that 5Ag/MnO2 exhibited significantly enhanced kinetics, including lower charge-transfer resistance, reduced polarization, and higher Zn2+ diffusion coefficient. Consequently, the 5Ag/MnO2 cathode delivered a high initial discharge capacity of 153.4 mAh g−1 at 1 A g−1 and superior long-term cycling stability (the discharge specific capacity remained at 135.5 mAh g−1 and 88.3% capacity retention after 500 cycles). Mechanism studies via ex situ XRD, XPS, and CV reveal a reversible Zn2+/H+ storage mechanism involving phase transformation between MnO2 and ZnMn2O4, with mixed capacitive and intercalation behavior. The enhanced performance is attributed to Ag doping facilitating rapid ion diffusion, improving electronic conductivity, and stabilizing the hierarchical structure. This work provides a viable strategy for designing high-performance MnO2-based cathodes for advanced zinc-ion batteries, advancing the practical application of RAZIBs.
可充电水锌离子电池(razib)由于其低成本、高安全性和环境友好性而成为大规模储能系统的有希望的候选者。然而,它们的实际应用受到阴极材料固有局限性的阻碍,包括缓慢的Zn2+扩散动力学,差的导电性和循环过程中的结构降解。在此,我们报告了一种简单的水热策略来合成具有均匀海胆状纳米结构的ag掺杂MnO2阴极,并被纳米线包围,作为RAZIBs的高性能阴极。最佳的5wt % Ag掺杂产生了更密集的纳米线阵列,即5Ag/MnO2,增加了可访问的活性位点,并引入了晶格缺陷,同时保留了MnO2的四边形晶体结构(I4/m)。电化学表征表明,5Ag/MnO2表现出明显增强的动力学,包括更低的电荷转移电阻、更低的极化和更高的Zn2+扩散系数。因此,5Ag/MnO2阴极在1 a g−1下具有153.4 mAh g−1的高初始放电容量和优异的长期循环稳定性(放电比容量保持在135.5 mAh g−1,500次循环后容量保持率为88.3%)。通过非原位XRD、XPS和CV对Zn2+/H+的机理进行了研究,揭示了一种可逆的Zn2+/H+储存机制,涉及MnO2和ZnMn2O4之间的相变,具有混合电容性和插层性行为。Ag的掺杂促进了离子的快速扩散,提高了电子导电性,并稳定了层状结构。本研究为高性能锌离子电池mno2基阴极的设计提供了可行的策略,促进了RAZIBs的实际应用。
{"title":"Sea urchin-like hierarchical structured Ag-doped MnO2 cathode material for stable aqueous zinc-ion batteries","authors":"Baochang Liu, Jianxin Wang, Bo Wang, Chongqing Kang","doi":"10.1007/s11581-025-06701-7","DOIUrl":"10.1007/s11581-025-06701-7","url":null,"abstract":"<div><p>Rechargeable aqueous zinc-ion batteries (RAZIBs) have emerged as promising candidates for large-scale energy storage systems, owing to their low cost, high safety, and environmental benignity. However, their practical application is hindered by intrinsic limitations of cathode materials, including sluggish Zn<sup>2+</sup> diffusion kinetics, poor electrical conductivity, and structural degradation during cycling. Herein, we report a facile hydrothermal strategy to synthesize Ag-doped MnO<sub>2</sub> cathode with uniform urchin-like nanostructures surrounded by nanowires as high-performance cathodes for RAZIBs. The optimal 5 wt% Ag doping yields denser nanowire arrays, namely 5Ag/MnO<sub>2</sub>, increases accessible active sites, and introduces lattice defects while preserving the tetragonal MnO<sub>2</sub> crystal structure (<i>I</i>4<i>/m</i>). The electrochemical characterization demonstrated that 5Ag/MnO<sub>2</sub> exhibited significantly enhanced kinetics, including lower charge-transfer resistance, reduced polarization, and higher Zn<sup>2+</sup> diffusion coefficient. Consequently, the 5Ag/MnO<sub>2</sub> cathode delivered a high initial discharge capacity of 153.4 mAh g<sup>−1</sup> at 1 A g<sup>−1</sup> and superior long-term cycling stability (the discharge specific capacity remained at 135.5 mAh g<sup>−1</sup> and 88.3% capacity retention after 500 cycles). Mechanism studies via ex situ XRD, XPS, and CV reveal a reversible Zn<sup>2+</sup>/H<sup>+</sup> storage mechanism involving phase transformation between MnO<sub>2</sub> and ZnMn<sub>2</sub>O<sub>4</sub>, with mixed capacitive and intercalation behavior. The enhanced performance is attributed to Ag doping facilitating rapid ion diffusion, improving electronic conductivity, and stabilizing the hierarchical structure. This work provides a viable strategy for designing high-performance MnO<sub>2</sub>-based cathodes for advanced zinc-ion batteries, advancing the practical application of RAZIBs.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11797 - 11810"},"PeriodicalIF":2.6,"publicationDate":"2025-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The prediction of the remaining useful life (RUL) of lithium-ion batteries (LIBs) is essential for effective battery management systems (BMS), safety assurance, and timely maintenance, particularly in ensuring the reliable operation of electric vehicles (EVs). This study aims to develop an accurate prediction model using Optuna for hyper-tuning with the Kolmogorov Arnold Network (KAN) to assess battery health and estimate its lifespan. KAN, an advanced neural network, introduces a novel approach to machine learning by replacing traditional linear weights with univariate functions parameterised by splines. This enables the model to flexibly capture complex activation patterns, significantly enhancing its predictive capabilities. In this study, we propose Opt-KAN-XAI as an effective method to accurately estimate the RUL in energy storage devices. To further enhance interpretability, we integrate explainable artificial intelligence (XAI) techniques using Shapley additive explanations (SHAP) values. This analysis examines the influence of key features, such as temperature, cycle index, voltage, and current, on RUL predictions, highlighting the substantial impact of temperature on discharge capacity. The findings of this research underscore the potential of machine learning models in LIBs management within the XAI framework, demonstrating their strategic role in optimising energy storage systems. To validate the Opt-KAN-XAI method, we conducted experiments on the NASA and CALCE datasets and compared the results with other existing approaches. The experimental results confirm the model’s high accuracy and robustness, achieving a minimum test loss, root mean square error (RMSE) and a minimum mean absolute error (MAE), demonstrating its effectiveness in the precise estimation of RUL.
锂离子电池(lib)剩余使用寿命(RUL)的预测对于有效的电池管理系统(BMS)、安全保障和及时维护至关重要,特别是对于确保电动汽车(ev)的可靠运行。本研究旨在利用Optuna与Kolmogorov Arnold Network (KAN)进行超调谐,开发一个准确的预测模型,以评估电池健康状况并估计其寿命。KAN是一种先进的神经网络,它通过用样条参数化的单变量函数取代传统的线性权重,引入了一种新的机器学习方法。这使得模型能够灵活地捕获复杂的激活模式,显著增强其预测能力。在本研究中,我们提出Opt-KAN-XAI作为一种有效的方法来准确估计储能装置中的RUL。为了进一步提高可解释性,我们使用Shapley加性解释(SHAP)值整合可解释人工智能(XAI)技术。该分析考察了关键特征(如温度、循环指数、电压和电流)对RUL预测的影响,强调了温度对放电容量的重大影响。这项研究的结果强调了机器学习模型在XAI框架内lib管理中的潜力,展示了它们在优化储能系统方面的战略作用。为了验证Opt-KAN-XAI方法,我们在NASA和CALCE数据集上进行了实验,并将结果与其他现有方法进行了比较。实验结果证实了该模型具有较高的精度和鲁棒性,实现了最小的测试损失、最小的均方根误差(RMSE)和最小的平均绝对误差(MAE),证明了该模型在RUL精确估计中的有效性。
{"title":"Explainable artificial intelligence driven estimation of remaining useful life for lithium-ion battery","authors":"Rahul Kumar Kamboj, Mukesh Singh, Ashima Singh, Anju Bala","doi":"10.1007/s11581-025-06707-1","DOIUrl":"10.1007/s11581-025-06707-1","url":null,"abstract":"<div><p>The prediction of the remaining useful life (RUL) of lithium-ion batteries (LIBs) is essential for effective battery management systems (BMS), safety assurance, and timely maintenance, particularly in ensuring the reliable operation of electric vehicles (EVs). This study aims to develop an accurate prediction model using Optuna for hyper-tuning with the Kolmogorov Arnold Network (KAN) to assess battery health and estimate its lifespan. KAN, an advanced neural network, introduces a novel approach to machine learning by replacing traditional linear weights with univariate functions parameterised by splines. This enables the model to flexibly capture complex activation patterns, significantly enhancing its predictive capabilities. In this study, we propose Opt-KAN-XAI as an effective method to accurately estimate the RUL in energy storage devices. To further enhance interpretability, we integrate explainable artificial intelligence (XAI) techniques using Shapley additive explanations (SHAP) values. This analysis examines the influence of key features, such as temperature, cycle index, voltage, and current, on RUL predictions, highlighting the substantial impact of temperature on discharge capacity. The findings of this research underscore the potential of machine learning models in LIBs management within the XAI framework, demonstrating their strategic role in optimising energy storage systems. To validate the Opt-KAN-XAI method, we conducted experiments on the NASA and CALCE datasets and compared the results with other existing approaches. The experimental results confirm the model’s high accuracy and robustness, achieving a minimum test loss, root mean square error (RMSE) and a minimum mean absolute error (MAE), demonstrating its effectiveness in the precise estimation of RUL.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11711 - 11728"},"PeriodicalIF":2.6,"publicationDate":"2025-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561736","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Accurate estimation of the State of Health (SOH) of lithium-ion batteries enables battery management systems to effectively monitor battery status, thereby preventing the occurrence of battery safety accidents. To address the challenges of difficult acquisition of complete charge–discharge data and low estimation accuracy under actual operating conditions, this study proposes an SOH estimation method based on time–frequency analysis and charging voltage segments. Health-related features are extracted within the voltage interval with the highest frequency in the charging data, and Discrete Wavelet Transform (DWT) is utilised to perform time–frequency decomposition on the input features. Each decomposed component is transmitted to the Temporal Convolutional Network (TCN) and Bidirectional Long Short-Term Memory (BiLSTM) branches respectively. Concurrently, the Transformer is used to capture global information, and finally, the SOH estimation value is output through the fully connected layer. Relatively accurate estimation of battery SOH can be achieved using only charging voltage data with a length of 0.1 V. Validation and analysis on the CACLE dataset demonstrate that the mean absolute error is within 1%. Generalisation verification is completed on the Oxford dataset, indicating that the proposed model exhibits excellent generalisation performance.
{"title":"A method for estimating the SOH of lithium batteries based on DWT-fused neural network and charging voltage segments","authors":"Hai Tian, Jing Peng, Wei Duan, Wenjie Zhu, Haixin Yu, Luping Dong","doi":"10.1007/s11581-025-06683-6","DOIUrl":"10.1007/s11581-025-06683-6","url":null,"abstract":"<div><p>Accurate estimation of the State of Health (SOH) of lithium-ion batteries enables battery management systems to effectively monitor battery status, thereby preventing the occurrence of battery safety accidents. To address the challenges of difficult acquisition of complete charge–discharge data and low estimation accuracy under actual operating conditions, this study proposes an SOH estimation method based on time–frequency analysis and charging voltage segments. Health-related features are extracted within the voltage interval with the highest frequency in the charging data, and Discrete Wavelet Transform (DWT) is utilised to perform time–frequency decomposition on the input features. Each decomposed component is transmitted to the Temporal Convolutional Network (TCN) and Bidirectional Long Short-Term Memory (BiLSTM) branches respectively. Concurrently, the Transformer is used to capture global information, and finally, the SOH estimation value is output through the fully connected layer. Relatively accurate estimation of battery SOH can be achieved using only charging voltage data with a length of 0.1 V. Validation and analysis on the CACLE dataset demonstrate that the mean absolute error is within 1%. Generalisation verification is completed on the Oxford dataset, indicating that the proposed model exhibits excellent generalisation performance.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11729 - 11745"},"PeriodicalIF":2.6,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-09-19DOI: 10.1007/s11581-025-06697-0
T. Nesavi, L. Balu, R. Ezhil Pavai
The CuO/SnO2 nanocomposites (NCs) were synthesized using a simple hydrothermal process to produce high-performance photocatalytic and electrochemical applications. X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), field emission scanning electron microscopy with energy-dispersive X-ray spectroscopy (FESEM-EDX), high-resolution transmission electron microscopy with selected area electron diffraction (HRTEM-SAED), UV–visible diffuse reflectance spectroscopy (UV-DRS), and X-ray photoelectron spectroscopy (XPS) investigations were used to characterize the properties of the prepared NCs. The XRD patterns ensured tetragonal and combined (monoclinic/tetragonal) phases for SnO2 and CuO/SnO2 composites, respectively. The estimated crystallite sizes were in the nanometer range and decreased from 29 to 21 nm with increasing CuO content. FTIR spectra were used to identify the metal oxide peaks that corresponded to SnO2 and CuO. The FESEM image for 1CS7 NC shows spherically agglomerated particles, whereas for 2CS7 and 3CS7, NCs exhibit a few rod structures along with spherical-shaped particles. The HRTEM images revealed the spherical morphology for optimized 1CS7 NCs. The oxidation states of synthesized CuO/SnO2 composites were confirmed using XPS investigations. Utilizing Kubelka–Munk method, the band gap values were determined for 1CS7, 2CS7, and 3CS7 NCs that rise from 2.66, 3.33, and 3.50 eV, respectively. The photocatalytic behavior of CuO/SnO2 NCs was studied by degrading methyl violet (MV) dye under solar irradiation for 70 min. The 1CS7 NC had higher degradation efficiency (91%) than other synthesized NCs. Furthermore, at a current density of 0.5 Ag−1, the 1CS7 electrode exhibited a specific capacitance of 770 Fg−1, and this electrode shows enhanced cyclic stability, maintaining 93.4% up to 2000 cycles. This investigation reveals that the 1CS7 composite is the outstanding material for photocatalytic and supercapacitor applications.
{"title":"Hydrothermal synthesis of heterostructured CuO/SnO₂ nanocomposites for photocatalytic degradation and supercapacitor applications","authors":"T. Nesavi, L. Balu, R. Ezhil Pavai","doi":"10.1007/s11581-025-06697-0","DOIUrl":"10.1007/s11581-025-06697-0","url":null,"abstract":"<div><p>The CuO/SnO<sub>2</sub> nanocomposites (NCs) were synthesized using a simple hydrothermal process to produce high-performance photocatalytic and electrochemical applications. X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), field emission scanning electron microscopy with energy-dispersive X-ray spectroscopy (FESEM-EDX), high-resolution transmission electron microscopy with selected area electron diffraction (HRTEM-SAED), UV–visible diffuse reflectance spectroscopy (UV-DRS), and X-ray photoelectron spectroscopy (XPS) investigations were used to characterize the properties of the prepared NCs. The XRD patterns ensured tetragonal and combined (monoclinic/tetragonal) phases for SnO<sub>2</sub> and CuO/SnO<sub>2</sub> composites, respectively. The estimated crystallite sizes were in the nanometer range and decreased from 29 to 21 nm with increasing CuO content. FTIR spectra were used to identify the metal oxide peaks that corresponded to SnO<sub>2</sub> and CuO. The FESEM image for 1CS7 NC shows spherically agglomerated particles, whereas for 2CS7 and 3CS7, NCs exhibit a few rod structures along with spherical-shaped particles. The HRTEM images revealed the spherical morphology for optimized 1CS7 NCs. The oxidation states of synthesized CuO/SnO<sub>2</sub> composites were confirmed using XPS investigations. Utilizing Kubelka–Munk method, the band gap values were determined for 1CS7, 2CS7, and 3CS7 NCs that rise from 2.66, 3.33, and 3.50 eV, respectively. The photocatalytic behavior of CuO/SnO<sub>2</sub> NCs was studied by degrading methyl violet (MV) dye under solar irradiation for 70 min. The 1CS7 NC had higher degradation efficiency (91%) than other synthesized NCs. Furthermore, at a current density of 0.5 Ag<sup>−1</sup>, the 1CS7 electrode exhibited a specific capacitance of 770 Fg<sup>−1</sup>, and this electrode shows enhanced cyclic stability, maintaining 93.4% up to 2000 cycles. This investigation reveals that the 1CS7 composite is the outstanding material for photocatalytic and supercapacitor applications.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"12027 - 12044"},"PeriodicalIF":2.6,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Accurate prediction of the State of Health (SOH) is essential for the safety and reliability of lithium-ion batteries. Traditional single-model architectures encounter challenges related to noise resistance and prediction accuracy when processing complex battery aging patterns. This paper proposes a DSwin-Transformer architecture that integrates relaxation voltage analysis with deep learning techniques. The method combines a denoising autoencoder (DAE) for feature dimensionality reduction with a hierarchical window attention mechanism to capture local degradation details and global aging dependencies. In this framework, the relaxation voltage is selected as the primary aging feature. Additionally, representative auxiliary aging features are identified from variables such as constant current charging time and voltage area using Pearson correlation analysis, mutual information, and SHAP values. Experimental validation across the CALCE and Tongji datasets demonstrates performance with mean absolute errors below 0.95%, showing improvements over Convolutional Neural Networks (CNN)-Gated Recurrent Units, CNN-Long Short-Term Memory, and CNN-Transformer baseline methods across various battery cells and training volumes. Ablation studies reveal the contribution of the DAE module, with the root mean square error (RMSE) improving from 0.179 to 0.0084 on the CALCE dataset for complex degradation patterns. The model maintains accuracy during both capacity decay and recovery periods while requiring a footprint of 15.6 MB. The results indicate that combining relaxation voltage features with adapted computer vision architectures provides a practical approach for predicting battery SOH.
{"title":"A DSwin-transformer-based SOH prediction method for lithium-ion batteries using relaxation voltages","authors":"Simin Yang, Xiaojun Tan, Jiagen Li, Yuqian Fan, Ziyu Zhao, Binbin Chen, Quanxue Guan","doi":"10.1007/s11581-025-06679-2","DOIUrl":"10.1007/s11581-025-06679-2","url":null,"abstract":"<div><p>Accurate prediction of the State of Health (SOH) is essential for the safety and reliability of lithium-ion batteries. Traditional single-model architectures encounter challenges related to noise resistance and prediction accuracy when processing complex battery aging patterns. This paper proposes a DSwin-Transformer architecture that integrates relaxation voltage analysis with deep learning techniques. The method combines a denoising autoencoder (DAE) for feature dimensionality reduction with a hierarchical window attention mechanism to capture local degradation details and global aging dependencies. In this framework, the relaxation voltage is selected as the primary aging feature. Additionally, representative auxiliary aging features are identified from variables such as constant current charging time and voltage area using Pearson correlation analysis, mutual information, and SHAP values. Experimental validation across the CALCE and Tongji datasets demonstrates performance with mean absolute errors below 0.95%, showing improvements over Convolutional Neural Networks (CNN)-Gated Recurrent Units, CNN-Long Short-Term Memory, and CNN-Transformer baseline methods across various battery cells and training volumes. Ablation studies reveal the contribution of the DAE module, with the root mean square error (RMSE) improving from 0.179 to 0.0084 on the CALCE dataset for complex degradation patterns. The model maintains accuracy during both capacity decay and recovery periods while requiring a footprint of 15.6 MB. The results indicate that combining relaxation voltage features with adapted computer vision architectures provides a practical approach for predicting battery SOH.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11767 - 11782"},"PeriodicalIF":2.6,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561478","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The extensive application of the electrolyte for solid oxide fuel cells (SOFCs) at intermediate temperatures (IT) is limited mainly owing to low conductivity. The effects of the Yb2O3 content on the phase stability, microstructure and ionic conductivity of the Yb2O3 and Sc2O3 co-doped ZrO2 (YbScSZ) ceramic electrolyte synthesized by the sol–gel-hydrothermal and calcination methods were investigated through X-ray diffraction (XRD), scanning electron microscopy (SEM), and electrochemical impedance spectroscopy (EIS) in this paper. The results show that the 3Yb2O3–8Sc2O3–89ZrO2 (mol%, 3Yb8ScSZ) exhibits a density of 5.80 g cm−3, an activation energy of 0.578 eV, and an ionic conductivity of 1.02 × 10−1 S cm−1 at 800 ℃. It is attributed to the good phase stability and high density of the cubic Yb2O3 and Sc2O3 co-doped ZrO2, and the low activation energy. Certain Yb3+ replacements for Sc3+ can increase the grain size and uniformity without reducing the oxygen vacancy density, which is beneficial for enhancing ionic conduction.
固体氧化物燃料电池(sofc)电解质在中温条件下的广泛应用主要受到其电导率低的限制。通过x射线衍射(XRD)、扫描电镜(SEM)和电化学阻抗谱(EIS)研究了Yb2O3含量对溶胶-凝胶-水热法和煅烧法合成的Yb2O3与Sc2O3共掺杂ZrO2 (YbScSZ)陶瓷电解质的相稳定性、微观结构和离子电导率的影响。结果表明,3Yb2O3-8Sc2O3-89ZrO2 (mol%, 3Yb8ScSZ)在800℃时的密度为5.80 g cm−3,活化能为0.578 eV,离子电导率为1.02 × 10−1 S cm−1。这是由于Yb2O3和Sc2O3共掺杂ZrO2具有良好的相稳定性和高密度,活化能低。在不降低氧空位密度的情况下,一定量的Yb3+取代Sc3+可以增加晶粒尺寸和均匀性,有利于提高离子电导率。
{"title":"The effect of Yb2O3 content on the phase stability, microstructure, and conductivity of YbScSZ electrolyte at intermediate temperatures","authors":"Weiqi Li, Jintao Ma, Fanjun Tang, Huan He, Tianquan Liang","doi":"10.1007/s11581-025-06691-6","DOIUrl":"10.1007/s11581-025-06691-6","url":null,"abstract":"<div><p>The extensive application of the electrolyte for solid oxide fuel cells (SOFCs) at intermediate temperatures (IT) is limited mainly owing to low conductivity. The effects of the Yb<sub>2</sub>O<sub>3</sub> content on the phase stability, microstructure and ionic conductivity of the Yb<sub>2</sub>O<sub>3</sub> and Sc<sub>2</sub>O<sub>3</sub> co-doped ZrO<sub>2</sub> (YbScSZ) ceramic electrolyte synthesized by the sol–gel-hydrothermal and calcination methods were investigated through X-ray diffraction (XRD), scanning electron microscopy (SEM), and electrochemical impedance spectroscopy (EIS) in this paper. The results show that the 3Yb<sub>2</sub>O<sub>3</sub>–8Sc<sub>2</sub>O<sub>3</sub>–89ZrO<sub>2</sub> (mol%, 3Yb8ScSZ) exhibits a density of 5.80 g cm<sup>−3</sup>, an activation energy of 0.578 eV, and an ionic conductivity of 1.02 × 10<sup>−1</sup> S cm<sup>−1</sup> at 800 ℃. It is attributed to the good phase stability and high density of the cubic Yb<sub>2</sub>O<sub>3</sub> and Sc<sub>2</sub>O<sub>3</sub> co-doped ZrO<sub>2</sub>, and the low activation energy. Certain Yb<sup>3+</sup> replacements for Sc<sup>3+</sup> can increase the grain size and uniformity without reducing the oxygen vacancy density, which is beneficial for enhancing ionic conduction.</p></div>","PeriodicalId":599,"journal":{"name":"Ionics","volume":"31 11","pages":"11867 - 11877"},"PeriodicalIF":2.6,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145561455","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}