Siwar Ben Hadj Ali, Mohammed Alabdali, Virginie Viallet, Vincent Seznec, Alejandro A. Franco
In all-solid-state batteries (ASSBs), the mechanical stress generated during electrode (de)lithiation plays a critical role in determining the cell longevity because of the induced degradation mechanisms. This stress originates from local volume fluctuations in the active electrode materials, such as nickel-rich LiNixMnyCozO2, which are intrinsically coupled to spatial variations in lithium-ion concentration during electrochemical cycling. Herein, a novel ASSB model that considers electrochemistry and solid mechanics in a one-way coupled manner is presented. The model spatially resolves 3D-microstructure of an ASSB half-cell generated from wet manufacturing process simulations and is based on linear continuum mechanics. The coupling of electrochemistry and solid mechanics is incorporated via lithiation-dependent volumetric changes of the active material and the microstructural changes due to deformed geometries affecting the particles percolation paths. Furthermore, it is shown that the overall volume change of the half-cell is dependent on the C-rate and on the applied stack pressure. Finally, the findings demonstrate that solid-mechanical effects and their interplay with electrochemical phenomena significantly impact the evolution of interfacial surface area and the total pore volume. These factors are crucial for ensuring accurate computational predictions, underscoring the necessity of incorporating such interactions in battery modeling approaches.
{"title":"A New Three-Dimensional Microstructure-Resolved Model to Assess Mechanical Stress in Solid-State Battery Electrodes","authors":"Siwar Ben Hadj Ali, Mohammed Alabdali, Virginie Viallet, Vincent Seznec, Alejandro A. Franco","doi":"10.1002/batt.202500540","DOIUrl":"https://doi.org/10.1002/batt.202500540","url":null,"abstract":"<p>In all-solid-state batteries (ASSBs), the mechanical stress generated during electrode (de)lithiation plays a critical role in determining the cell longevity because of the induced degradation mechanisms. This stress originates from local volume fluctuations in the active electrode materials, such as nickel-rich LiNi<sub><i>x</i></sub>Mn<sub><i>y</i></sub>Co<sub>z</sub>O<sub>2</sub>, which are intrinsically coupled to spatial variations in lithium-ion concentration during electrochemical cycling. Herein, a novel ASSB model that considers electrochemistry and solid mechanics in a one-way coupled manner is presented. The model spatially resolves 3D-microstructure of an ASSB half-cell generated from wet manufacturing process simulations and is based on linear continuum mechanics. The coupling of electrochemistry and solid mechanics is incorporated via lithiation-dependent volumetric changes of the active material and the microstructural changes due to deformed geometries affecting the particles percolation paths. Furthermore, it is shown that the overall volume change of the half-cell is dependent on the C-rate and on the applied stack pressure. Finally, the findings demonstrate that solid-mechanical effects and their interplay with electrochemical phenomena significantly impact the evolution of interfacial surface area and the total pore volume. These factors are crucial for ensuring accurate computational predictions, underscoring the necessity of incorporating such interactions in battery modeling approaches.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500540","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146162477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Miguel Granados-Moreno, Rosalía Cid, Julia Maibach, Maria Arnaiz, Eider Goikolea, Jon Ajuria
Pre-lithiation is an essential step in lithium-ion capacitors (LICs) due to the lack of Li+ in both electrodes. The integration of dilithium squarate (Li2C4O4) into the positive electrode of LICs is considered one of the most promising pre-lithiation strategies. Therefore, the ability of Li2C4O4 decomposition products to modify the solid electrolyte interphase has been recently disclosed, although their impact on the positive electrode surface has not been studied yet. In this work, the improvement of the electrochemical performance when Li2C4O4 was included has been investigated by analyzing the surface of activated carbon-based electrodes with and without Li2C4O4 by scanning electron microscopy and X-ray photoelectron spectroscopy. The decomposition of Li2C4O4 leads to the formation of a surface layer on the positive electrode that remains unaltered regardless of the applied potential, as well as after an aging test. Thus, the improved electrochemical performance is attributed to the presence of a pseudocapacitive charge storage mechanism enabled by the surface layer. Lastly, the cells are modified to reveal the main components participating in the surface layer formation. These findings provide valuable insights into the impact, benefits, and limitations of Li2C4O4, which will accelerate the development of other suitable alternative sacrificial salts.
{"title":"Interface Engineering via Li2C4O4 Prelithiation: Boosting Activated Carbon Electrode Performance in Lithium-Ion Capacitors","authors":"Miguel Granados-Moreno, Rosalía Cid, Julia Maibach, Maria Arnaiz, Eider Goikolea, Jon Ajuria","doi":"10.1002/batt.202500495","DOIUrl":"https://doi.org/10.1002/batt.202500495","url":null,"abstract":"<p>Pre-lithiation is an essential step in lithium-ion capacitors (LICs) due to the lack of Li<sup>+</sup> in both electrodes. The integration of dilithium squarate (Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub>) into the positive electrode of LICs is considered one of the most promising pre-lithiation strategies. Therefore, the ability of Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub> decomposition products to modify the solid electrolyte interphase has been recently disclosed, although their impact on the positive electrode surface has not been studied yet. In this work, the improvement of the electrochemical performance when Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub> was included has been investigated by analyzing the surface of activated carbon-based electrodes with and without Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub> by scanning electron microscopy and X-ray photoelectron spectroscopy. The decomposition of Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub> leads to the formation of a surface layer on the positive electrode that remains unaltered regardless of the applied potential, as well as after an aging test. Thus, the improved electrochemical performance is attributed to the presence of a pseudocapacitive charge storage mechanism enabled by the surface layer. Lastly, the cells are modified to reveal the main components participating in the surface layer formation. These findings provide valuable insights into the impact, benefits, and limitations of Li<sub>2</sub>C<sub>4</sub>O<sub>4</sub>, which will accelerate the development of other suitable alternative sacrificial salts.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135785","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hydrogen-bonded organic frameworks (HOFs) have been increasingly applied in industrial fields owing to their low weight and high pore volume. In particular, HOFs incorporating redox-active units have emerged as promising electrode materials for energy storage devices alongside other porous organic polymers. This study explores the application of HOFs incorporating tetrathiafulvalene (TTF) derivatives that are well-known as molecular conductors with multielectron redox properties for rechargeable batteries. Specifically, the battery performance of HOFs-based TTF-tetrabenzoate (H4TTFTB) as a cathode active material in lithium-ion (LIBs) and sodium-ion batteries (SIBs) is evaluated. H4TTFTB-based HOFs demonstrate enhanced cycling stability, with a particularly large enhancement achieved in SIB systems, due to the inherent structural stability of HOFs. Additionally, driven by the synergistic redox activity of TTF and bipyridine units, TTF-hybrid-HOFs combining H4TTFTB with redox-active bipyridine units exhibit improved battery capacities. These findings underscore the potential of H4TTFTB-based HOFs, which combine excellent redox activity and mechanical stability, as promising candidates for high-performance energy storage devices, highlighting the advantages of integrating rigid heterocyclic compounds with redox-active functionalities into HOF structures for future battery applications.
{"title":"Design and Application of Hydrogen-Bonded Organic Frameworks with Tetrathiafulvalene-Tetrabenzoate for Cathode Active Materials in Lithium- and Sodium-Ion Batteries","authors":"Katsuhiro Wakamatsu, Soichiro Furuno, Hosei Oshima, Naoki Kobayashi, Tomohiro Miyaji, Takeshi Shimizu, Heng Wang, Hirofumi Yoshikawa","doi":"10.1002/batt.202500524","DOIUrl":"https://doi.org/10.1002/batt.202500524","url":null,"abstract":"<p>Hydrogen-bonded organic frameworks (HOFs) have been increasingly applied in industrial fields owing to their low weight and high pore volume. In particular, HOFs incorporating redox-active units have emerged as promising electrode materials for energy storage devices alongside other porous organic polymers. This study explores the application of HOFs incorporating tetrathiafulvalene (TTF) derivatives that are well-known as molecular conductors with multielectron redox properties for rechargeable batteries. Specifically, the battery performance of HOFs-based TTF-tetrabenzoate (H<sub>4</sub>TTFTB) as a cathode active material in lithium-ion (LIBs) and sodium-ion batteries (SIBs) is evaluated. H<sub>4</sub>TTFTB-based HOFs demonstrate enhanced cycling stability, with a particularly large enhancement achieved in SIB systems, due to the inherent structural stability of HOFs. Additionally, driven by the synergistic redox activity of TTF and bipyridine units, TTF-hybrid-HOFs combining H<sub>4</sub>TTFTB with redox-active bipyridine units exhibit improved battery capacities. These findings underscore the potential of H<sub>4</sub>TTFTB-based HOFs, which combine excellent redox activity and mechanical stability, as promising candidates for high-performance energy storage devices, highlighting the advantages of integrating rigid heterocyclic compounds with redox-active functionalities into HOF structures for future battery applications.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 12","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145754521","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The work proposes a novel and fast method to synthesize Ti3C2Tx MXene with enhanced redox activity and improved structural, optical, and electronic properties by incorporating NaOH in the late etching stage. The technique eliminates the need for postetching delamination while maintaining the properties of delaminated MXene. Optimizing the concentration of NaOH leads to the removal of the unetched MAX phase from MXene in the mild in situ HF etching technique. The obtained ultrapure MXene is used as the negative electrode in an asymmetric supercapacitor device configuration. The MXene//RuO2 asymmetric device showed superior electrochemical performance with a specific capacitance of 73.3 F g−1, energy density of 23 Wh kg−1, and power density of 796 W kg−1, with potential extendable up to 1.5 volts. The device retained more than 90% of its performance at the end of 2000 cycles. The all-solid-state asymmetric supercapacitor device fabricated using PVA/H2SO4 gel polymer as the electrolyte, and Na-MX and RuO2 as the electrodes gave a specific capacitance of 845 mF g−1, energy density of 470 mWh kg−1, and power density of 5000 mW kg−1 at a current density of 5 mA g−1 with an extendable voltage window up to 2 V, more than twice the window obtained using symmetric supercapacitor with MXene as electrode.
本研究提出了一种新颖、快速的方法,通过在蚀刻后期加入NaOH来合成具有增强氧化还原活性和改善结构、光学和电子性能的Ti3C2Tx MXene。该技术消除了拉伸后分层的需要,同时保持了分层MXene的特性。优化NaOH浓度可以去除MXene中未蚀刻的MAX相。所得的超纯MXene用作非对称超级电容器器件配置中的负极。MXene//RuO2非对称器件具有优异的电化学性能,比电容为73.3 F g−1,能量密度为23 Wh kg−1,功率密度为796 W kg−1,电位扩展最高可达1.5伏。该设备在2000次循环结束时仍保持了90%以上的性能。以PVA/H2SO4凝胶聚合物为电解液,Na-MX和RuO2为电极制备的全固态非对称超级电容器器件在电流密度为5 mA g - 1时的比电容为845 mF g - 1,能量密度为470 mWh kg - 1,功率密度为5000 mW kg - 1,可扩展电压窗口为2 V,是以MXene为电极的对称超级电容器的两倍多。
{"title":"Flexible Asymmetric Supercapacitors using Mildly Etched Ti3C2Tx MXene for Powering Wearable Devices","authors":"Anamika Ashok, Varsha Vijayan, Shalu Mariam George, Aleena Tomy, Asha Arackal Sukumaran, Oleksii Klymov, Vicente Muñoz-Sanjose, Mahesh Eledath Changarath, Juan F. Sánchez Royo","doi":"10.1002/batt.202500389","DOIUrl":"https://doi.org/10.1002/batt.202500389","url":null,"abstract":"<p>The work proposes a novel and fast method to synthesize Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> MXene with enhanced redox activity and improved structural, optical, and electronic properties by incorporating NaOH in the late etching stage. The technique eliminates the need for postetching delamination while maintaining the properties of delaminated MXene. Optimizing the concentration of NaOH leads to the removal of the unetched MAX phase from MXene in the mild in situ HF etching technique. The obtained ultrapure MXene is used as the negative electrode in an asymmetric supercapacitor device configuration. The MXene//RuO<sub>2</sub> asymmetric device showed superior electrochemical performance with a specific capacitance of 73.3 F g<sup>−</sup><sup>1</sup>, energy density of 23 Wh kg<sup>−</sup><sup>1</sup>, and power density of 796 W kg<sup>−1</sup>, with potential extendable up to 1.5 volts. The device retained more than 90% of its performance at the end of 2000 cycles. The all-solid-state asymmetric supercapacitor device fabricated using PVA/H<sub>2</sub>SO<sub>4</sub> gel polymer as the electrolyte, and Na-MX and RuO<sub>2</sub> as the electrodes gave a specific capacitance of 845 mF g<sup>−1</sup>, energy density of 470 mWh kg<sup>−1</sup>, and power density of 5000 mW kg<sup>−1</sup> at a current density of 5 mA g<sup>−1</sup> with an extendable voltage window up to 2 V, more than twice the window obtained using symmetric supercapacitor with MXene as electrode.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 12","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145754529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The surging demand for electric vehicles and energy storage technologies drives an unprecedented accumulation of spent batteries, which leads to severe environmental burdens and critical resource wastage. Traditional recycling technologies rely on high-temperature calcination or acid/base leaching, and the final products in the form of alloys or salts can only be used as precursors. In contrast, advanced direct recycling regenerates spent cathode and anode into materials that can be directly used in battery production, simplifying the recycling process and improving economic benefits, which is expected to become a shortcut for lithium-ion battery recycling in the future. This review analyzes the state-of-the-art direct recycling methods based on the failure mechanisms for anodes and cathodes, divides them into solid-state recycling, hydrothermal repair, and others according to different recycling conditions, and summarizes separately the advancements and limitations of each method, to guide the scale-up and sustainability of recycling. Furthermore, this review systematically introduces artificial intelligence (AI) assisted direct recycling strategies, emphasizing the role of AI in optimizing the pretreatment and recycling processes. Finally, the practical challenges and future opportunities for direct recycling are discussed, providing important reference for further development.
{"title":"Sustainable Direct Recycling of Spent Lithium-Ion Batteries: Closed-Loop Regeneration and AI-Optimized Systems Toward Next-Generation Battery Circular Economy","authors":"Tianran Liang, Yi Chen, Jing Xu, Yang Jin","doi":"10.1002/batt.202500536","DOIUrl":"https://doi.org/10.1002/batt.202500536","url":null,"abstract":"<p>The surging demand for electric vehicles and energy storage technologies drives an unprecedented accumulation of spent batteries, which leads to severe environmental burdens and critical resource wastage. Traditional recycling technologies rely on high-temperature calcination or acid/base leaching, and the final products in the form of alloys or salts can only be used as precursors. In contrast, advanced direct recycling regenerates spent cathode and anode into materials that can be directly used in battery production, simplifying the recycling process and improving economic benefits, which is expected to become a shortcut for lithium-ion battery recycling in the future. This review analyzes the state-of-the-art direct recycling methods based on the failure mechanisms for anodes and cathodes, divides them into solid-state recycling, hydrothermal repair, and others according to different recycling conditions, and summarizes separately the advancements and limitations of each method, to guide the scale-up and sustainability of recycling. Furthermore, this review systematically introduces artificial intelligence (AI) assisted direct recycling strategies, emphasizing the role of AI in optimizing the pretreatment and recycling processes. Finally, the practical challenges and future opportunities for direct recycling are discussed, providing important reference for further development.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135920","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
To address the dual challenges of fragile structures prone to damage and packaging systems susceptible to leakage in thermal management of electronic devices for traditional phase change materials, this study proposes an organic-porous synergistic packaging strategy. A porous TiO2 skeleton is in situ constructed via a one-pot one-step method to synchronously encapsulate paraffin wax and thermoplastic elastomer styrene ethylene butylene styrene (SEBS). The innovation lies in utilizing solvent evaporation-induced phase separation and sol–gel reaction to enable the porous TiO2 (specific surface area 316.307 m2 g–1) and SEBS to form a rigid-flexible synergistic structure, achieving low leakage rate and stability in 2000 thermal cycles. In battery thermal management, the battery temperature is controlled within a safe range at 1–3C rates, extending the safe operation duration of the battery by more than 10 times. It provides a referable option for efficient thermal management of wearable electronic devices and flexible devices.
{"title":"Synthesis of Flexible Phase Change Materials with In Situ Formed Porous TiO2 for Highly Efficient Battery Thermal Management","authors":"Guangyuan Liang, Runyang Wang, Qiang Zhou, Jiahuan He, Yuanzheng Liu, Jiateng Zhao, Changhui Liu","doi":"10.1002/batt.202500460","DOIUrl":"https://doi.org/10.1002/batt.202500460","url":null,"abstract":"<p>To address the dual challenges of fragile structures prone to damage and packaging systems susceptible to leakage in thermal management of electronic devices for traditional phase change materials, this study proposes an organic-porous synergistic packaging strategy. A porous TiO<sub>2</sub> skeleton is in situ constructed via a one-pot one-step method to synchronously encapsulate paraffin wax and thermoplastic elastomer styrene ethylene butylene styrene (SEBS). The innovation lies in utilizing solvent evaporation-induced phase separation and sol–gel reaction to enable the porous TiO<sub>2</sub> (specific surface area 316.307 m<sup>2 </sup>g<sup>–1</sup>) and SEBS to form a rigid-flexible synergistic structure, achieving low leakage rate and stability in 2000 thermal cycles. In battery thermal management, the battery temperature is controlled within a safe range at 1–3C rates, extending the safe operation duration of the battery by more than 10 times. It provides a referable option for efficient thermal management of wearable electronic devices and flexible devices.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146136872","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Lithium–oxygen (Li–O2) batteries have attracted substantial interest due to their high theoretical specific energy and environmental benignity. However, their practical electrochemical performance remains hampered by sluggish cathode reaction kinetics, unstable solid electrolyte interphase (SEI) at electrode/electrolyte interfaces, and lithium dendrite growth. Addressing these system-wide challenges necessitates the development of novel functional materials as a pivotal strategy. Among explored materials, high-entropy alloys (HEAs) demonstrate significant advantages through finely tunable composition and electronic structure, enabling synergistic functionality that offers new pathways for enhancing the comprehensive performance of Li–O2 batteries. This review outlines the fundamental reaction mechanisms and core challenges of Li–O2 batteries, and then systematically examines recent advances in HEA applications across three critical domains: cathode catalyst design, electrolyte optimization, and anode protection. Finally, perspectives on future research directions for HEAs in Li–O2 batteries are offered.
{"title":"High-Entropy Alloys for Cathode, Electrolyte, and Anode Applications in Lithium–O2 Batteries","authors":"Xin Xu, Wanzhen Li, Wentao Wang, Ningxuan Zhu, Chuan Tan, Xiangwen Gao, Yuhui Chen","doi":"10.1002/batt.202500567","DOIUrl":"https://doi.org/10.1002/batt.202500567","url":null,"abstract":"<p>Lithium–oxygen (Li–O<sub>2</sub>) batteries have attracted substantial interest due to their high theoretical specific energy and environmental benignity. However, their practical electrochemical performance remains hampered by sluggish cathode reaction kinetics, unstable solid electrolyte interphase (SEI) at electrode/electrolyte interfaces, and lithium dendrite growth. Addressing these system-wide challenges necessitates the development of novel functional materials as a pivotal strategy. Among explored materials, high-entropy alloys (HEAs) demonstrate significant advantages through finely tunable composition and electronic structure, enabling synergistic functionality that offers new pathways for enhancing the comprehensive performance of Li–O<sub>2</sub> batteries. This review outlines the fundamental reaction mechanisms and core challenges of Li–O<sub>2</sub> batteries, and then systematically examines recent advances in HEA applications across three critical domains: cathode catalyst design, electrolyte optimization, and anode protection. Finally, perspectives on future research directions for HEAs in Li–O<sub>2</sub> batteries are offered.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146136772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Katharina Lilith Quade, Elias Hempen, Hanna van den Berg, Dominik Jöst, Franziska Berger, Florian Ringbeck, Dirk Uwe Sauer
Despite the abundance of battery state estimation algorithms in the BMS literature, their applicability to emerging cell chemistries remains uncertain, as evaluating their performance across diverse use cases is complex, resource-intensive, and time-consuming. In this work, we introduce an evaluation framework designed to assess the performance of diagnostic algorithms across various applications and external conditions. Our framework relies on simulations of different operational scenarios grouped into categories and evaluates algorithm performance using statistical metrics that represent accuracy, bias, and precision. While our framework can be used for various state estimators and applications, we demonstrate its functionality by benchmarking three common and real-time capable State of Charge (SOC) algorithms across three cell types, including a sodium-ion battery. Within our case study, we show that the tested model-based algorithms offer excellent transferability for the specific sodium-ion battery considering different operation conditions. Additionally, we demonstrate that the characteristic OCV(SOC) relationship of the sodium-ion cell allows for the use of lower-quality and more affordable sensors, as the cell is less sensitive to measurement inaccuracies. Overall, our open-source framework supports the systematic assessment of diagnostic algorithm transferability and provides a foundation for informed decision-making when selecting algorithms for a specific application and cell type.
{"title":"Benchmarking the Transferability of Real-Time State of Charge Algorithms to Sodium-Ion Cells Using an Open-Source Diagnostics Framework","authors":"Katharina Lilith Quade, Elias Hempen, Hanna van den Berg, Dominik Jöst, Franziska Berger, Florian Ringbeck, Dirk Uwe Sauer","doi":"10.1002/batt.202500456","DOIUrl":"https://doi.org/10.1002/batt.202500456","url":null,"abstract":"<p>Despite the abundance of battery state estimation algorithms in the BMS literature, their applicability to emerging cell chemistries remains uncertain, as evaluating their performance across diverse use cases is complex, resource-intensive, and time-consuming. In this work, we introduce an evaluation framework designed to assess the performance of diagnostic algorithms across various applications and external conditions. Our framework relies on simulations of different operational scenarios grouped into categories and evaluates algorithm performance using statistical metrics that represent accuracy, bias, and precision. While our framework can be used for various state estimators and applications, we demonstrate its functionality by benchmarking three common and real-time capable State of Charge (SOC) algorithms across three cell types, including a sodium-ion battery. Within our case study, we show that the tested model-based algorithms offer excellent transferability for the specific sodium-ion battery considering different operation conditions. Additionally, we demonstrate that the characteristic OCV(SOC) relationship of the sodium-ion cell allows for the use of lower-quality and more affordable sensors, as the cell is less sensitive to measurement inaccuracies. Overall, our open-source framework supports the systematic assessment of diagnostic algorithm transferability and provides a foundation for informed decision-making when selecting algorithms for a specific application and cell type.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500456","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146139978","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Urban Košir, Alen Vizintin, Elena Tchernychova, Gregor Kapun, Matteo Gastaldi, Alia Jouhara, Margaud Lecuyer, Claudio Gerbaldi, Miran Gaberšček, Robert Dominko, Sara Drvarič Talian
The push to use metallic lithium-based batteries motivates a shift toward the use of solid polymer electrolytes. To improve the ionic conductivity values of such electrolytes, liquid additives (plasticizers) are usually added. However, the improvement in conductivity comes at the expense of a deterioration of the anode–electrolyte interface, resulting in poorer electrochemical cell performance. In this study, the use of a polymer coating consisting of polyethylene oxide, LiTFSI, and LiNO3 is proposed. The coating shows improved electrochemical performance and stability, delayed cell failure and a more uniform distribution of Li deposits. These improvements are attributed to the increased stability of the solid electrolyte interphase, which is confirmed by using a combination of electrochemical impedance spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. In contrast, it is found that the interphase in uncoated Li electrodes is likely affected by continuous reactions with the plasticizer, further confirming the need to use such protective coatings to achieve long-term operation in practical solid-state Li metal batteries.
{"title":"Polymer Coating for Li-Metal Anode in Polyethylene Oxide-Based Electrolyte Batteries","authors":"Urban Košir, Alen Vizintin, Elena Tchernychova, Gregor Kapun, Matteo Gastaldi, Alia Jouhara, Margaud Lecuyer, Claudio Gerbaldi, Miran Gaberšček, Robert Dominko, Sara Drvarič Talian","doi":"10.1002/batt.202500402","DOIUrl":"https://doi.org/10.1002/batt.202500402","url":null,"abstract":"<p>The push to use metallic lithium-based batteries motivates a shift toward the use of solid polymer electrolytes. To improve the ionic conductivity values of such electrolytes, liquid additives (plasticizers) are usually added. However, the improvement in conductivity comes at the expense of a deterioration of the anode–electrolyte interface, resulting in poorer electrochemical cell performance. In this study, the use of a polymer coating consisting of polyethylene oxide, LiTFSI, and LiNO<sub>3</sub> is proposed. The coating shows improved electrochemical performance and stability, delayed cell failure and a more uniform distribution of Li deposits. These improvements are attributed to the increased stability of the solid electrolyte interphase, which is confirmed by using a combination of electrochemical impedance spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. In contrast, it is found that the interphase in uncoated Li electrodes is likely affected by continuous reactions with the plasticizer, further confirming the need to use such protective coatings to achieve long-term operation in practical solid-state Li metal batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500402","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Polysulfides formed in Li–S batteries pose various characteristics. For example, Li2S is solid while Li2S4 is liquid. Li2S is insoluble in battery electrolytes while Li2S4 is soluble. All of them are negative charge bearing molecules. Lithium polysulfides are Lewis acids. Herein, a binder with multiple interaction motifs is presented to confine the polysulfides in the cathode. The base of the binder is sodium salt of carboxy methyl cellulose (CMC). β-cyclodextrin (CD) that comprises 21 hydroxyl groups is used because they hydrogen bond with the carboxylate moieties of CMC to impart mechanical strength to the binder to accommodate volume change during the sulfur to polysulfide conversion. Indeed, it is found that the binder with CD shows improved mechanical properties compared to CMC. The cavity of the CD is used to prepare an inclusion complex with ferrocene methanol. Due to the presence of Fe2+, the batteries comprising the inclusion complex show improved electrocatalytic properties. The Li–S batteries deliver a specific capacity of 780 mA h g−1 (1 C) at a high sulfur loading of 4.7 mg cm−2 and lean electrolyte (E/S of 5 μL mg−1).
锂硫电池中形成的多硫化物具有多种特性。例如,Li2S是固体,而Li2S4是液体。Li2S不溶于电池电解质,而Li2S4可溶。它们都是带负电荷的分子。锂多硫化物是路易斯酸。本文提出了一种具有多个相互作用基序的粘结剂来限制阴极中的多硫化物。粘结剂的基材为羧甲基纤维素钠盐。采用由21个羟基组成的β-环糊精(CD),是因为它们与CMC的羧酸基团形成氢键,赋予粘合剂机械强度,以适应硫到多硫转化过程中的体积变化。结果表明,与CMC相比,含CD的粘结剂具有更好的力学性能。CD的空腔用于制备二茂铁甲醇包合物。由于Fe2+的存在,包含包合物的电池表现出更好的电催化性能。在4.7 mg cm−2的高硫负载和5 μL mg−1的稀薄电解质(E/S)下,Li-S电池的比容量为780 mA h g−1 (1c)。
{"title":"Multitype Interaction Between a Redox-Active Inclusion Complex, Polymer, and Polysulfides that Boosts the Performance of Lithium–Sulfur Batteries","authors":"Marimuthu Senthilkumaran, Bharathkumar H. Javaregowda, Tejas Rajput, Kadhiravan Shanmuganathan, Prakashbabu Rajendran, Debmalya Roy, Kothandam Krishnamoorthy","doi":"10.1002/batt.202500485","DOIUrl":"https://doi.org/10.1002/batt.202500485","url":null,"abstract":"<p>Polysulfides formed in Li–S batteries pose various characteristics. For example, Li<sub>2</sub>S is solid while Li<sub>2</sub>S<sub>4</sub> is liquid. Li<sub>2</sub>S is insoluble in battery electrolytes while Li<sub>2</sub>S<sub>4</sub> is soluble. All of them are negative charge bearing molecules. Lithium polysulfides are Lewis acids. Herein, a binder with multiple interaction motifs is presented to confine the polysulfides in the cathode. The base of the binder is sodium salt of carboxy methyl cellulose (CMC). <i>β</i>-cyclodextrin (CD) that comprises 21 hydroxyl groups is used because they hydrogen bond with the carboxylate moieties of CMC to impart mechanical strength to the binder to accommodate volume change during the sulfur to polysulfide conversion. Indeed, it is found that the binder with CD shows improved mechanical properties compared to CMC. The cavity of the CD is used to prepare an inclusion complex with ferrocene methanol. Due to the presence of Fe<sup>2+</sup>, the batteries comprising the inclusion complex show improved electrocatalytic properties. The Li–S batteries deliver a specific capacity of 780 mA h g<sup>−1</sup> (1 C) at a high sulfur loading of 4.7 mg cm<sup>−2</sup> and lean electrolyte (E/S of 5 μL mg<sup>−1</sup>).</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"9 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146136486","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}