Pub Date : 2026-01-27DOI: 10.1016/j.ensm.2026.104930
Seung-Bo Hong, Hyobin Lee, Young-Jun Lee, Choyeon Kim, Yong Min Lee, Un-Hyuck Kim, Dong-Won Kim
Sulfide-based all-solid-state lithium batteries (ASSLBs) have garnered considerable attention owing to their high energy density and enhanced safety. In such systems, composite cathodes are commonly fabricated via either a solvent-free dry process or a slurry-based wet process, typically employing polytetrafluoroethylene (PTFE) and acrylonitrile–butadiene rubber (NBR) as binders, respectively. However, a comprehensive understanding of how these binders influence electrochemical performance and degradation mechanisms remains limited. In this study, the effects of PTFE and NBR binders on interfacial degradation are systematically elucidated through electrochemical analyses, morphological characterizations, and digital-twin computational modeling. The results reveal that PTFE effectively mitigates interfacial deterioration by maintaining intimate contact and minimizing void formation, whereas NBR suffers from accelerated interfacial degradation and void growth during prolonged cycling. These findings highlight the critical role of binder-induced interfacial phenomena in determining cell performance and offer valuable insights for optimizing cathode fabrication strategies tailored to each processing route, while guiding the rational design of advanced binders for composite cathodes in ASSLBs.
{"title":"Unveiling Degradation Mechanisms of Sulfide-Based Composite Cathodes Supported by Digital-Twin Modeling: Dry Binder versus Wet Binder","authors":"Seung-Bo Hong, Hyobin Lee, Young-Jun Lee, Choyeon Kim, Yong Min Lee, Un-Hyuck Kim, Dong-Won Kim","doi":"10.1016/j.ensm.2026.104930","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104930","url":null,"abstract":"Sulfide-based all-solid-state lithium batteries (ASSLBs) have garnered considerable attention owing to their high energy density and enhanced safety. In such systems, composite cathodes are commonly fabricated via either a solvent-free dry process or a slurry-based wet process, typically employing polytetrafluoroethylene (PTFE) and acrylonitrile–butadiene rubber (NBR) as binders, respectively. However, a comprehensive understanding of how these binders influence electrochemical performance and degradation mechanisms remains limited. In this study, the effects of PTFE and NBR binders on interfacial degradation are systematically elucidated through electrochemical analyses, morphological characterizations, and digital-twin computational modeling. The results reveal that PTFE effectively mitigates interfacial deterioration by maintaining intimate contact and minimizing void formation, whereas NBR suffers from accelerated interfacial degradation and void growth during prolonged cycling. These findings highlight the critical role of binder-induced interfacial phenomena in determining cell performance and offer valuable insights for optimizing cathode fabrication strategies tailored to each processing route, while guiding the rational design of advanced binders for composite cathodes in ASSLBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"7 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146057137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-26DOI: 10.1016/j.ensm.2026.104926
Jianrong Lin , Wenxuan Hu , Jian Yang , Yonggang Hu , Siyuan Ma , Lixuan Pan , Fangmei Wen , Meifang Ding , Shijun Tang , Yiming Wei , Zhengliang Gong , Yong Yang
Lithium-ion batteries exhibit distinct degradation mechanisms under calendar and cycle aging, making it essential to establish correlations between key electrochemical performance metrics and evolution of underlying physicochemical properties. In this study, LiFePO4/graphite pouch cells are subjected to both cycle aging and calendar aging (at 100% State-of-Charge) at 65 °C. Throughout the aging processes, the capacity decay, impedance variation, and the evolution of solid electrolyte interphase (SEI) are quantitatively analyzed. The capacity fading follows a 0.5-power law relationship with time during cycle aging and a logarithmic trend during calendar aging. Both aging modes could be divided into two distinct stages based on SEI evolutions. In Stage Ⅰ, the growth of inorganic SEI components far exceeds that of its organic components, accompanied by a significant decrease in both capacity and impedance. The SEI even undergoes a drastic structural reconstruction during cycle aging. In Stage Ⅱ, the SEI composition stabilizes, and its thickness increases gradually, accompanied by a slower rate of capacity fade. Notably, in this stage, a strong linear correlation is observed between capacity loss and the reciprocal of SEI capacitance (1/CSEI) for both aging modes, which enables CSEI to serve as a key descriptor for evaluating battery health state.
{"title":"Quantifying aging kinetics in LiFePO4/graphite pouch cells: Cycle aging vs calendar aging via a novel impedance descriptor","authors":"Jianrong Lin , Wenxuan Hu , Jian Yang , Yonggang Hu , Siyuan Ma , Lixuan Pan , Fangmei Wen , Meifang Ding , Shijun Tang , Yiming Wei , Zhengliang Gong , Yong Yang","doi":"10.1016/j.ensm.2026.104926","DOIUrl":"10.1016/j.ensm.2026.104926","url":null,"abstract":"<div><div>Lithium-ion batteries exhibit distinct degradation mechanisms under calendar and cycle aging, making it essential to establish correlations between key electrochemical performance metrics and evolution of underlying physicochemical properties. In this study, LiFePO<sub>4</sub>/graphite pouch cells are subjected to both cycle aging and calendar aging (at 100% State-of-Charge) at 65 °C. Throughout the aging processes, the capacity decay, impedance variation, and the evolution of solid electrolyte interphase (SEI) are quantitatively analyzed. The capacity fading follows a 0.5-power law relationship with time during cycle aging and a logarithmic trend during calendar aging. Both aging modes could be divided into two distinct stages based on SEI evolutions. In Stage Ⅰ, the growth of inorganic SEI components far exceeds that of its organic components, accompanied by a significant decrease in both capacity and impedance. The SEI even undergoes a drastic structural reconstruction during cycle aging. In Stage Ⅱ, the SEI composition stabilizes, and its thickness increases gradually, accompanied by a slower rate of capacity fade. Notably, in this stage, a strong linear correlation is observed between capacity loss and the reciprocal of SEI capacitance (1/C<sub>SEI</sub>) for both aging modes, which enables C<sub>SEI</sub> to serve as a key descriptor for evaluating battery health state.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104926"},"PeriodicalIF":20.2,"publicationDate":"2026-01-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146047996","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-25DOI: 10.1016/j.ensm.2026.104927
Ye Li, Qinyang Zhao, Yi Xing, Hanlin Wang, Yuanlin Yan, Bosen Li, Qinfen Gu, Haitao Hu, Limin Zhou, Mingzhe Chen
Electrolytes strongly influence battery energy density, safety, and cycle life through their solvation structures and interfacial behaviors. Traditional experimental methods are limited in resolving atomic-scale solvation evolution and dynamic interfaces. Density functional theory (DFT), molecular dynamics, and their advanced variants (e.g., Ab Initio Molecular Dynamics and Machine-Learning Molecular Dynamics) are advancing electrolyte research tools by precisely decoding ion-solvent interactions, coordination configurations, and electronic structures. This review systematically outlines the DFT framework and its key applications: elucidating solvation energies, coordination preferences, and concentration-dependent solvation structure regulation; and revealing interfacial mechanisms, redox stability, and ion transport kinetics. Furthermore, it highlights machine learning-accelerated advances in high-throughput electrolyte screening, property prediction, and multiscale modeling. Tight integration of computational theory with experimental validation provides atomic-level guidance for rational design of stable, highly conductive electrolytes, thereby accelerating the development of next-generation battery materials.
{"title":"Multiscale Simulation for Electrolyte Design: From Microstructure-Property Decoding to Macroscopic Performance Prediction","authors":"Ye Li, Qinyang Zhao, Yi Xing, Hanlin Wang, Yuanlin Yan, Bosen Li, Qinfen Gu, Haitao Hu, Limin Zhou, Mingzhe Chen","doi":"10.1016/j.ensm.2026.104927","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104927","url":null,"abstract":"Electrolytes strongly influence battery energy density, safety, and cycle life through their solvation structures and interfacial behaviors. Traditional experimental methods are limited in resolving atomic-scale solvation evolution and dynamic interfaces. Density functional theory (DFT), molecular dynamics, and their advanced variants (e.g., Ab Initio Molecular Dynamics and Machine-Learning Molecular Dynamics) are advancing electrolyte research tools by precisely decoding ion-solvent interactions, coordination configurations, and electronic structures. This review systematically outlines the DFT framework and its key applications: elucidating solvation energies, coordination preferences, and concentration-dependent solvation structure regulation; and revealing interfacial mechanisms, redox stability, and ion transport kinetics. Furthermore, it highlights machine learning-accelerated advances in high-throughput electrolyte screening, property prediction, and multiscale modeling. Tight integration of computational theory with experimental validation provides atomic-level guidance for rational design of stable, highly conductive electrolytes, thereby accelerating the development of next-generation battery materials.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"53 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146047997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-25DOI: 10.1016/j.ensm.2026.104925
Emma J. Hopkins , Qiushi Miao , Haichen Lin , Ke Zhou , Jaejun Lee , John Holoubek , Ping Liu
Operating Li-S batteries at low temperatures necessitates the initial stripping of the lithium anode. In this paper, we demonstrate that stripping lithium metal at low temperatures leads to the formation of faceted lithium crystals which regulate subsequent deposition as an extrusion-based process. At 25°C, subsequent growth features polycrystalline lithium structures growing from the bottom of the pits. At -20°C, the extruded lithium needles form a nanoporous structure after cycling, while the pores formed at 25°C are much larger. By shrinking the length scale of the cycled morphology at -20°C, the compressibility of the cycled interface decreases and the response to applied pressure is reduced. In contrast, at 25°C, the larger length scale of the cycled morphology creates a minimum of ideal pressure. Low temperature stripping thus fundamentally changes the growth mode and the optimal pressure needed to extend the cycle life of lithium metal anodes.
{"title":"Effects of stripping at low temperature on the subsequent growth of lithium metal","authors":"Emma J. Hopkins , Qiushi Miao , Haichen Lin , Ke Zhou , Jaejun Lee , John Holoubek , Ping Liu","doi":"10.1016/j.ensm.2026.104925","DOIUrl":"10.1016/j.ensm.2026.104925","url":null,"abstract":"<div><div>Operating Li-S batteries at low temperatures necessitates the initial stripping of the lithium anode. In this paper, we demonstrate that stripping lithium metal at low temperatures leads to the formation of faceted lithium crystals which regulate subsequent deposition as an extrusion-based process. At 25°C, subsequent growth features polycrystalline lithium structures growing from the bottom of the pits. At -20°C, the extruded lithium needles form a nanoporous structure after cycling, while the pores formed at 25°C are much larger. By shrinking the length scale of the cycled morphology at -20°C, the compressibility of the cycled interface decreases and the response to applied pressure is reduced. In contrast, at 25°C, the larger length scale of the cycled morphology creates a minimum of ideal pressure. Low temperature stripping thus fundamentally changes the growth mode and the optimal pressure needed to extend the cycle life of lithium metal anodes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104925"},"PeriodicalIF":20.2,"publicationDate":"2026-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146047998","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-24DOI: 10.1016/j.ensm.2026.104923
Lulu Liu, Lei Chen, Xianghui Liu, Xiaoen Wang, Zhongwei Chen
Conventional solid polymer electrolytes (SPEs) face critical challenges such as low Li+ conductivity, excessive anion mobility and interfacial instability, which hinder their applications in high-energy lithium (Li) metal batteries. Herein, we develop a multi-mechanism synergistic strategy by incorporating a polymer–metal–organic framework (PolyMOF) into a poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF) matrix to construct a composite solid-state electrolyte (PolyMOF@PVHF). Within this design, polymer ligands in PolyMOF induce electron redistribution via p‑π conjugation, forming strong anion–π⁺ interactions that selectively immobilizes TFSI⁻ and suppresses anion migration. Concurrently, surface hydrogen-bonding motifs trap residual solvent molecules while the nanoconfinement effect promotes Li⁺ desolvation, enabling rapid ion transport through ultralow-barrier channels. The synergistic mechanism collectively inhibits side reactions and facilitate uniform Li+ deposition at the solid electrolyte interphase (SEI) interface. As a result, the PolyMOF@PVHF electrolyte achieves a high ionic conductivity of 1.23 × 10-3 S cm-1 and a Li⁺ transference number of 0.75 at room temperature (RT). The electrolyte also exhibits exceptional interfacial stability, enabling reversible Li plating/stripping over 1900 h and long-term cycling in Li metal batteries (1500 cycles at 2C with 99.9% capacity retention for LFP; 200 cycles with 93.5% retention for NCM811). Moreover, the assembled NCM811|Li pouch cell shows outstanding safety and mechanical robustness under bending, folding and cutting. This work provides a viable strategy to overcome Li⁺ transport and interfacial issues in SPEs, paving the way for high-performance solid-state Li metal batteries.
传统的固体聚合物电解质（spe）面临着Li+电导率低、阴离子迁移率过高和界面不稳定等严峻挑战，阻碍了它们在高能锂（Li）金属电池中的应用。在此，我们开发了一种多机制协同策略，通过将聚合物-金属-有机框架（PolyMOF）结合到聚偏氟乙烯-共六氟丙烯（PVHF）基体中来构建复合固态电解质（PolyMOF@PVHF）。在这个设计中，PolyMOF中的聚合物配体通过p -π偶联诱导电子重新分布，形成强阴离子-π +相互作用，选择性地固定TFSI⁻并抑制阴离子迁移。同时，表面的氢键基序捕获了残留的溶剂分子，而纳米约束效应促进了Li +的脱溶，使离子能够通过超低势垒通道快速传输。协同机制共同抑制副反应，促进Li+在固体电解质界面（SEI）均匀沉积。结果，PolyMOF@PVHF电解质在室温（RT）下获得了1.23 × 10-3 S cm-1的高离子电导率和0.75的迁移数。该电解质还表现出优异的界面稳定性，能够在1900小时内实现可逆的锂电镀/剥离，并在锂金属电池中长期循环（LFP在2C下循环1500次，容量保持率为99.9%；NCM811循环200次，容量保持率为93.5%）。此外，组装的NCM811|锂袋电池在弯曲，折叠和切割下具有出色的安全性和机械坚固性。这项工作为克服spe中Li⁺的传输和界面问题提供了一种可行的策略，为高性能固态锂金属电池的发展铺平了道路。
{"title":"Immobilizing Anions via Electron‑deficient π Desgin: A PolyMOF-Based Composite Electrolyte for Stable Solid-State Lithium Metal Batteries","authors":"Lulu Liu, Lei Chen, Xianghui Liu, Xiaoen Wang, Zhongwei Chen","doi":"10.1016/j.ensm.2026.104923","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104923","url":null,"abstract":"Conventional solid polymer electrolytes (SPEs) face critical challenges such as low Li<ce:sup loc=\"post\">+</ce:sup> conductivity, excessive anion mobility and interfacial instability, which hinder their applications in high-energy lithium (Li) metal batteries. Herein, we develop a multi-mechanism synergistic strategy by incorporating a polymer–metal–organic framework (PolyMOF) into a poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF) matrix to construct a composite solid-state electrolyte (PolyMOF@PVHF). Within this design, polymer ligands in PolyMOF induce electron redistribution via p‑π conjugation, forming strong anion–π⁺ interactions that selectively immobilizes TFSI⁻ and suppresses anion migration. Concurrently, surface hydrogen-bonding motifs trap residual solvent molecules while the nanoconfinement effect promotes Li⁺ desolvation, enabling rapid ion transport through ultralow-barrier channels. The synergistic mechanism collectively inhibits side reactions and facilitate uniform Li<ce:sup loc=\"post\">+</ce:sup> deposition at the solid electrolyte interphase (SEI) interface. As a result, the PolyMOF@PVHF electrolyte achieves a high ionic conductivity of 1.23 × 10-3 S cm<ce:sup loc=\"post\">-1</ce:sup> and a Li⁺ transference number of 0.75 at room temperature (RT). The electrolyte also exhibits exceptional interfacial stability, enabling reversible Li plating/stripping over 1900 h and long-term cycling in Li metal batteries (1500 cycles at 2C with 99.9% capacity retention for LFP; 200 cycles with 93.5% retention for NCM811). Moreover, the assembled NCM811|Li pouch cell shows outstanding safety and mechanical robustness under bending, folding and cutting. This work provides a viable strategy to overcome Li⁺ transport and interfacial issues in SPEs, paving the way for high-performance solid-state Li metal batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"41 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146048000","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-24DOI: 10.1016/j.ensm.2026.104921
Amit Chanda , Abdulrahman Alfadhli , Vijay A. Sethuraman , Daniel P. Abraham , Siva P.V. Nadimpalli
Metal plating remains a critical challenge in rechargeable batteries, directly impacting cell lifetime and safety. Understanding the underlying mechanism of plating and its early detection is essential for the safe operation of batteries. In this work, real-time stress evolution was monitored during electrochemical cycling in a range of working electrodes differing in material (graphite, hard carbon, and Ge), geometry (composite vs. solid binder-less thin film), chemistry (Li-ion and Na-ion), and electrochemical reaction mechanism (intercalation and alloying). Three half-cell systems, Na–hard carbon (Na–HC), Li–graphite (Li–Gr), and Na–germanium (Na–Ge), were studied using the substrate-curvature method to quantify in-situ stress evolution during plating. In all systems, a distinct stress reversal coincided with the onset of plating, representing a universal mechanical signature of the process. The stress response revealed that (i) a two-stage plating mechanism exists and (ii) ions from both the electrolyte and host matrix contribute to initial metal deposition, a phenomenon not captured by existing models. This coupling between stress and electrochemical response provides a powerful diagnostic tool for detecting plating onset and offers new mechanistic insight into ion transport during metal deposition. These findings establish a framework for developing more accurate models of plating and improving the reliability and safety of rechargeable batteries.
{"title":"Revealing the stress signature and ion origin of metal plating in rechargeable batteries","authors":"Amit Chanda , Abdulrahman Alfadhli , Vijay A. Sethuraman , Daniel P. Abraham , Siva P.V. Nadimpalli","doi":"10.1016/j.ensm.2026.104921","DOIUrl":"10.1016/j.ensm.2026.104921","url":null,"abstract":"<div><div>Metal plating remains a critical challenge in rechargeable batteries, directly impacting cell lifetime and safety. Understanding the underlying mechanism of plating and its early detection is essential for the safe operation of batteries. In this work, real-time stress evolution was monitored during electrochemical cycling in a range of working electrodes differing in material (graphite, hard carbon, and Ge), geometry (composite vs. solid binder-less thin film), chemistry (Li-ion and Na-ion), and electrochemical reaction mechanism (intercalation and alloying). Three half-cell systems, Na–hard carbon (Na–HC), Li–graphite (Li–Gr), and Na–germanium (Na–Ge), were studied using the substrate-curvature method to quantify in-situ stress evolution during plating. In all systems, a distinct stress reversal coincided with the onset of plating, representing a universal mechanical signature of the process. The stress response revealed that (i) a two-stage plating mechanism exists and (ii) ions from both the electrolyte and host matrix contribute to initial metal deposition, a phenomenon not captured by existing models. This coupling between stress and electrochemical response provides a powerful diagnostic tool for detecting plating onset and offers new mechanistic insight into ion transport during metal deposition. These findings establish a framework for developing more accurate models of plating and improving the reliability and safety of rechargeable batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104921"},"PeriodicalIF":20.2,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146034211","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-24DOI: 10.1016/j.ensm.2026.104924
Ziliang Feng , Xiaohua Guo , Bao Zhang , Yongkang Liu , Enfeng Zhang , Peng Luo , Quanyi Zhang , Peng Dong , Wei-Li Song , Yingjie Zhang , Yannan Zhang
High-nickel layered cathode materials undergo structural degradation caused by enlarged internal stress arising from Li+/Ni2+ cation mixing and lattice oxygen release, which accelerates capacity decay and raises safety concerns. To mitigate this stress, a rational design of LiNi0.8Co0.1Mn0.1O2 (NCM811) was developed through precise strain engineering by Mo6+ and Sb3+ co-doping. Compared with pristine NCM811, the incorporation of Sb3+ significantly reduced the lattice distortion, thereby enabling stable and reversible Li+ de/intercalation and suppressing the migration from Ni2+ to Li+ sites. Meanwhile, Mo6+ doping established stronger Mo–O coordination in the bulk and formed electrochemically stable Li2MoO4 at the interfaces, which decreased the bulk stress by reducing oxygen release and simultaneously enhanced resistance to electrolyte corrosion. Thus, this strain-engineering strategy produced robust NCM811 lattice and interface structures, favorable for the construction of stable particles and thinner, more homogeneous cathode-electrolyte interfaces. The assembled pouch full cell (∼0.8 Ah) achieved a markedly improved capacity retention ∼93 % after 1000 cycles at 1 C (capacity retention ∼69 % after 500 cycles in the pouch cell assembled with pristine NCM811), compared with the state-of-the-art values typically below 85 %. This strategy provides an effective route for developing stable Ni-rich cathodes for long-term lithium-ion batteries.
{"title":"Strain engineering of particles and interfaces for long-life stable LiNi0.8Co0.1Mn0.1O2 cathodes","authors":"Ziliang Feng , Xiaohua Guo , Bao Zhang , Yongkang Liu , Enfeng Zhang , Peng Luo , Quanyi Zhang , Peng Dong , Wei-Li Song , Yingjie Zhang , Yannan Zhang","doi":"10.1016/j.ensm.2026.104924","DOIUrl":"10.1016/j.ensm.2026.104924","url":null,"abstract":"<div><div>High-nickel layered cathode materials undergo structural degradation caused by enlarged internal stress arising from Li<sup>+</sup>/Ni<sup>2+</sup> cation mixing and lattice oxygen release, which accelerates capacity decay and raises safety concerns. To mitigate this stress, a rational design of LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) was developed through precise strain engineering by Mo<sup>6+</sup> and Sb<sup>3+</sup> co-doping. Compared with pristine NCM811, the incorporation of Sb<sup>3+</sup> significantly reduced the lattice distortion, thereby enabling stable and reversible Li<sup>+</sup> de/intercalation and suppressing the migration from Ni<sup>2+</sup> to Li<sup>+</sup> sites. Meanwhile, Mo<sup>6+</sup> doping established stronger Mo–O coordination in the bulk and formed electrochemically stable Li<sub>2</sub>MoO<sub>4</sub> at the interfaces, which decreased the bulk stress by reducing oxygen release and simultaneously enhanced resistance to electrolyte corrosion. Thus, this strain-engineering strategy produced robust NCM811 lattice and interface structures, favorable for the construction of stable particles and thinner, more homogeneous cathode-electrolyte interfaces. The assembled pouch full cell (∼0.8 Ah) achieved a markedly improved capacity retention ∼93 % after 1000 cycles at 1 C (capacity retention ∼69 % after 500 cycles in the pouch cell assembled with pristine NCM811), compared with the state-of-the-art values typically below 85 %. This strategy provides an effective route for developing stable Ni-rich cathodes for long-term lithium-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104924"},"PeriodicalIF":20.2,"publicationDate":"2026-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146047999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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