Pub Date : 2026-01-13DOI: 10.1016/j.ensm.2026.104901
Xiaoyi Wang , Yun Su , Hongyue Cui , Shiguang Zhang , Hang Su , Xiaohui Rong , Liquan Chen , Gaoping Cao , Yong-Sheng Hu
All-solid-state Na-ion batteries (ASSNIBs) are promising for enhanced safety and energy density, but hard carbon (HC) anodes suffer from limited Na+ transport and require high electrolyte content (>30 wt %) and pressure (>1 MPa) in inorganic systems. Herein, a polymer-HC composite anode (PEO@HC) with only 5 wt % polyethylene oxide (PEO) is developed, enabling high HC loading (90 wt %) and efficient Na+ conduction under low pressure (<0.2 MPa). Synchrotron nano-CT and Small-angle X-ray scattering (SAXS) revealed a uniform PEO coating on the HC surface, reducing defects and modifying pore structures for improved ion kinetics. In Na|PEO-ASPE-Na|PEO@HC half-cells, PEO@HC delivers a high initial Coulombic efficiency (86.3 %) and reversible capacity (295.5 mAh g-1 at 0.1C), comparable to liquid-electrolyte counterparts. The first reported pouch-type ASSNIB (PEO@HC|PEO-ASPE-Na|PEO@NVP) achieves 81 % capacity retention after 500 cycles at 0.1C. This polymer-based strategy overcomes interfacial challenges, paving the way for practical ASSNIBs in electric vehicles and stationary storage.
全固态钠离子电池（assnib）有望提高安全性和能量密度，但在无机系统中，硬碳（HC）阳极受Na+传输限制，需要高电解质含量（30 wt%）和高压力（1 MPa）。本文开发了一种仅含5 wt%聚乙烯氧化物（PEO）的聚合物-HC复合阳极（PEO@HC），在低压（<0.2 MPa）下实现了高HC负载（90 wt%）和高效的Na⁺传导。同步加速器纳米ct和小角度x射线散射（SAXS）显示，在HC表面有均匀的PEO涂层，减少了缺陷并改变了孔隙结构，从而改善了离子动力学。在Na|PEO-ASPE-Na|PEO@HC半电池中，PEO@HC提供了高初始库仑效率（86.3%）和可逆容量（295.5 mAh g-1, 0.1C），与液体电解质相当。首次报道的袋式ASSNIB （PEO@HC| peo - aspa - na |PEO@NVP）在0.1C下循环500次后容量保持率达到81%。这种基于聚合物的策略克服了界面挑战，为电动汽车和固定存储中实际的assnib铺平了道路。
{"title":"Hard carbon anodes for all-solid-state Na-ion batteries","authors":"Xiaoyi Wang , Yun Su , Hongyue Cui , Shiguang Zhang , Hang Su , Xiaohui Rong , Liquan Chen , Gaoping Cao , Yong-Sheng Hu","doi":"10.1016/j.ensm.2026.104901","DOIUrl":"10.1016/j.ensm.2026.104901","url":null,"abstract":"<div><div>All-solid-state Na-ion batteries (ASSNIBs) are promising for enhanced safety and energy density, but hard carbon (HC) anodes suffer from limited Na<sup>+</sup> transport and require high electrolyte content (>30 wt %) and pressure (>1 MPa) in inorganic systems. Herein, a polymer-HC composite anode (PEO@HC) with only 5 wt % polyethylene oxide (PEO) is developed, enabling high HC loading (90 wt %) and efficient Na<sup>+</sup> conduction under low pressure (<0.2 MPa). Synchrotron nano-CT and Small-angle X-ray scattering (SAXS) revealed a uniform PEO coating on the HC surface, reducing defects and modifying pore structures for improved ion kinetics. In Na|PEO-ASPE-Na|PEO@HC half-cells, PEO@HC delivers a high initial Coulombic efficiency (86.3 %) and reversible capacity (295.5 mAh g<sup>-1</sup> at 0.1C), comparable to liquid-electrolyte counterparts. The first reported pouch-type ASSNIB (PEO@HC|PEO-ASPE-Na|PEO@NVP) achieves 81 % capacity retention after 500 cycles at 0.1C. This polymer-based strategy overcomes interfacial challenges, paving the way for practical ASSNIBs in electric vehicles and stationary storage.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104901"},"PeriodicalIF":20.2,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955475","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 : 2026-01-13DOI: 10.1016/j.ensm.2026.104902
Kuiming Liu , Zhonghan Wu , Yue Li , Haoran Zhou , Meng Yao , Yiyang Peng , Chen Li , Xinhui Huang , Guoyu Ding , Zhichen Hou , Kang Liu , Ruyu Xi , Jiantao Guo , Meng Yu , Kai Zhang , Fangyi Cheng
Nickel-rich layered transition metal oxides are intriguing cathode materials for lithium-ion batteries because of high energy density, but they suffer from structural degradation at high voltages, caused by lattice distortion, cation migration/dissolution, and lattice oxygen loss. To address these degradation issues, herein we report a surface entropy-gradient strategy to construct a LiNi0.93Mn0.02Mg0.015Al0.015Co0.01Mo0.01O1.99F0.01 cathode featuring concentration gradients of Ni/Co/Mo/F/O elements at the primary particle surfaces. Comprehensive microscopic and spectroscopic characterizations, combined with theoretical calculations, reveal that this engineered gradient structure establishes a progressive strengthening mechanism driven by increasing configurational entropy from bulk to surface, thereby significantly enhancing structural stability and electrochemical reversibility. Specifically, the entropy-gradient configuration effectively mitigates the irreversible O3-to-O1 phase transition, promoting lithium-ion diffusion; simultaneously, it inhibits Ni migration and dissolution while suppressing excessive oxygen oxidation, thereby substantially improving the reversibility of both cationic and anionic redox reactions upon deep (de)lithiation. Under high cut-off voltage of 4.6 V, the formulated cathode retains 91.9% of its initial capacity (229.9 mAh g-1) after 100 cycles, outperforming the conventional high-nickel counterparts. This study highlights the entropy-gradient engineering as an innovative methodology to upgrade ultrahigh-nickel cathodes under high-voltage operation.
{"title":"Tailoring surface entropy gradient towards 4.6 V ultrahigh-nickel cathodes with durable cationic and anionic redox","authors":"Kuiming Liu , Zhonghan Wu , Yue Li , Haoran Zhou , Meng Yao , Yiyang Peng , Chen Li , Xinhui Huang , Guoyu Ding , Zhichen Hou , Kang Liu , Ruyu Xi , Jiantao Guo , Meng Yu , Kai Zhang , Fangyi Cheng","doi":"10.1016/j.ensm.2026.104902","DOIUrl":"10.1016/j.ensm.2026.104902","url":null,"abstract":"<div><div>Nickel-rich layered transition metal oxides are intriguing cathode materials for lithium-ion batteries because of high energy density, but they suffer from structural degradation at high voltages, caused by lattice distortion, cation migration/dissolution, and lattice oxygen loss. To address these degradation issues, herein we report a surface entropy-gradient strategy to construct a LiNi<sub>0.93</sub>Mn<sub>0.02</sub>Mg<sub>0.015</sub>Al<sub>0.015</sub>Co<sub>0.01</sub>Mo<sub>0.01</sub>O<sub>1.99</sub>F<sub>0.01</sub> cathode featuring concentration gradients of Ni/Co/Mo/F/O elements at the primary particle surfaces. Comprehensive microscopic and spectroscopic characterizations, combined with theoretical calculations, reveal that this engineered gradient structure establishes a progressive strengthening mechanism driven by increasing configurational entropy from bulk to surface, thereby significantly enhancing structural stability and electrochemical reversibility. Specifically, the entropy-gradient configuration effectively mitigates the irreversible O3-to-O1 phase transition, promoting lithium-ion diffusion; simultaneously, it inhibits Ni migration and dissolution while suppressing excessive oxygen oxidation, thereby substantially improving the reversibility of both cationic and anionic redox reactions upon deep (de)lithiation. Under high cut-off voltage of 4.6 V, the formulated cathode retains 91.9% of its initial capacity (229.9 mAh g<sup>-1</sup>) after 100 cycles, outperforming the conventional high-nickel counterparts. This study highlights the entropy-gradient engineering as an innovative methodology to upgrade ultrahigh-nickel cathodes under high-voltage operation.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104902"},"PeriodicalIF":20.2,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145962226","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}
Sodium metal anodes (SMAs) present a compelling pathway toward next-generation high-energy-density batteries but face persistent challenges such as dendrite growth, low Coulombic efficiency, and safety concerns. These issues originate from the strong coupling between thermodynamic instability and kinetic limitations inherent to sodium metal. To address these fundamental coupling, this review establishes a unified framework linking “thermodynamic–kinetic coupling” as the failure origin to “structure–function optimization” as the solution core. We systematically dissect the synergistic interplay between thermodynamic and kinetic factors governing SMA failure, and highlight the pivotal role of advanced current collectors as a core mitigation strategy. Recent progress in 3D porous architectures, surface functionalization, and gradient engineering is comprehensively surveyed, demonstrating how these approaches synergistically regulate nucleation thermodynamics and ion transport kinetics. The discussion extends to anode‑free sodium metal batteries (AF-SMBs), where optimized current collectors are indispensable. By establishing a coherent framework linking thermodynamic-kinetic coupling to structural and functional optimization, this work lays a foundation for developing safe, durable, and high-performance sodium metal batteries.
{"title":"Failure mechanisms and current collector design for sodium metal anodes: From thermodynamic-kinetic coupling to structural-functional optimization","authors":"Saisai Qiu, Haolin Zhu, Qiang Wu, Shijie Cheng, Jia Xie","doi":"10.1016/j.ensm.2026.104898","DOIUrl":"10.1016/j.ensm.2026.104898","url":null,"abstract":"<div><div>Sodium metal anodes (SMAs) present a compelling pathway toward next-generation high-energy-density batteries but face persistent challenges such as dendrite growth, low Coulombic efficiency, and safety concerns. These issues originate from the strong coupling between thermodynamic instability and kinetic limitations inherent to sodium metal. To address these fundamental coupling, this review establishes a unified framework linking “thermodynamic–kinetic coupling” as the failure origin to “structure–function optimization” as the solution core. We systematically dissect the synergistic interplay between thermodynamic and kinetic factors governing SMA failure, and highlight the pivotal role of advanced current collectors as a core mitigation strategy. Recent progress in 3D porous architectures, surface functionalization, and gradient engineering is comprehensively surveyed, demonstrating how these approaches synergistically regulate nucleation thermodynamics and ion transport kinetics. The discussion extends to anode‑free sodium metal batteries (AF-SMBs), where optimized current collectors are indispensable. By establishing a coherent framework linking thermodynamic-kinetic coupling to structural and functional optimization, this work lays a foundation for developing safe, durable, and high-performance sodium metal batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104898"},"PeriodicalIF":20.2,"publicationDate":"2026-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145962228","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}
Aprotic lithium-oxygen (Li-O2) batteries represent a critical enabling technology in tomorrow’s portfolio of clean energy solutions due to their unparalleled theoretical energy density among existing battery chemistries. The solid–electrolyte interphase (SEI) formed on lithium metal anode (LMA) surfaces plays a crucial role in unlocking their energy capabilities. Over recent years, the oxygen crosstalk phenomenon at the LMA/electrolyte interface has emerged as a significant yet underexplored determinant of SEI stability and battery performance. In this contribution, three potential oxygen crosstalk effects on SEI formation pathways in the literature, are first recapitulated. Subsequently, a study paradigm is presented to achieve unified understandings of oxygen crosstalk and develop rational design strategies for stable LMA, which involves decoupling and probing complex oxygen crosstalk chemistries through well-designed model interfaces and in situ spectroscopies. Finally, future directions and perspectives are proposed, with a call to the wider research community to explore the significant effect of crosstalk chemistries beyond Li-O2 batteries and extend to emerging electrochemical devices.
{"title":"A Controversial Topic on Oxygen Crosstalk Effects in Aprotic Lithium-Oxygen Batteries","authors":"Zhiwei Zhao, Yantao Zhang, Limin Guo, Zhangquan Peng","doi":"10.1016/j.ensm.2026.104899","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104899","url":null,"abstract":"Aprotic lithium-oxygen (Li-O<ce:inf loc=\"post\">2</ce:inf>) batteries represent a critical enabling technology in tomorrow’s portfolio of clean energy solutions due to their unparalleled theoretical energy density among existing battery chemistries. The solid–electrolyte interphase (SEI) formed on lithium metal anode (LMA) surfaces plays a crucial role in unlocking their energy capabilities. Over recent years, the oxygen crosstalk phenomenon at the LMA/electrolyte interface has emerged as a significant yet underexplored determinant of SEI stability and battery performance. In this contribution, three potential oxygen crosstalk effects on SEI formation pathways in the literature, are first recapitulated. Subsequently, a study paradigm is presented to achieve unified understandings of oxygen crosstalk and develop rational design strategies for stable LMA, which involves decoupling and probing complex oxygen crosstalk chemistries through well-designed model interfaces and in situ spectroscopies. Finally, future directions and perspectives are proposed, with a call to the wider research community to explore the significant effect of crosstalk chemistries beyond Li-O<ce:inf loc=\"post\">2</ce:inf> batteries and extend to emerging electrochemical devices.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957113","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 : 2026-01-12DOI: 10.1016/j.ensm.2026.104895
Hongya Wang , Xiang Chen , Muya Cai , Shiyu Wang , Fengyin Zhou , Yongxin Wu , Danfeng Wang , Haochen Wang , Bingbing Wang , Fangzhao Pang , Junmin Peng , Weiguo Huang , Xiaowei Liu , Dihua Wang , Huayi Yin
Lead-acid batteries (LABs), due to their mature technology, high safety, low cost, and wide range of applications, remain one of the most popular secondary power sources today, particularly in electric bicycles and automotive starter-lighting-ignition systems. However, the ubiquity of LABs has precipitated a massive accumulation of end-of-life waste, resulting in an urgent imperative for robust recycling frameworks to mitigate resource depletion and environmental toxicity. This review presents a holistic analysis of the LAB ecosystem, bridging the gap between manufacturing advancements and closed-loop reclamation. We critically synthesize the evolution of LAB technology, detailing mainstream and emerging manufacturing paradigms, while comprehensively outlining failure mechanisms and repair strategies. Special emphasis is placed on state-of-the-art recycling methodologies, providing a granular evaluation of component-specific recovery (including paste, grids, separators, and electrolytes). Furthermore, we integrate a life cycle and economic assessment to rigorously quantify carbon footprints, environmental impacts, and economic viability. By reviewing the entire life cycle of LABs—from raw materials to waste—we aim to provide insights into the research directions and focal points at each stage, offering perspectives and guidance for the future of LAB research in both the scientific and industrial communities.
{"title":"Recycling of lead-acid batteries: A review","authors":"Hongya Wang , Xiang Chen , Muya Cai , Shiyu Wang , Fengyin Zhou , Yongxin Wu , Danfeng Wang , Haochen Wang , Bingbing Wang , Fangzhao Pang , Junmin Peng , Weiguo Huang , Xiaowei Liu , Dihua Wang , Huayi Yin","doi":"10.1016/j.ensm.2026.104895","DOIUrl":"10.1016/j.ensm.2026.104895","url":null,"abstract":"<div><div>Lead-acid batteries (LABs), due to their mature technology, high safety, low cost, and wide range of applications, remain one of the most popular secondary power sources today, particularly in electric bicycles and automotive starter-lighting-ignition systems. However, the ubiquity of LABs has precipitated a massive accumulation of end-of-life waste, resulting in an urgent imperative for robust recycling frameworks to mitigate resource depletion and environmental toxicity. This review presents a holistic analysis of the LAB ecosystem, bridging the gap between manufacturing advancements and closed-loop reclamation. We critically synthesize the evolution of LAB technology, detailing mainstream and emerging manufacturing paradigms, while comprehensively outlining failure mechanisms and repair strategies. Special emphasis is placed on state-of-the-art recycling methodologies, providing a granular evaluation of component-specific recovery (including paste, grids, separators, and electrolytes). Furthermore, we integrate a life cycle and economic assessment to rigorously quantify carbon footprints, environmental impacts, and economic viability. By reviewing the entire life cycle of LABs—from raw materials to waste—we aim to provide insights into the research directions and focal points at each stage, offering perspectives and guidance for the future of LAB research in both the scientific and industrial communities.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104895"},"PeriodicalIF":20.2,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957114","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}
In recent years, the evolution of Li-ion battery material components, cell architectures, and application scenarios has posed significant challenges for the rapid adaptation of battery management systems (BMS). Accurate health diagnostics and prognostics are fundamental to reliable battery operation. However, traditional approaches based on empirical equations, physical models, or handcrafted features often suffer from limited generalization, heavy data demands, and time-consuming development. Representation learning, a major advancement in deep learning, is emerging as a powerful tool to accelerate battery health modeling. Under novel chemistries and unseen operating conditions, it mitigates data scarcity through generative learning and enables rapid model adaptation via transfer learning, which was overlooked in earlier reviews. We systematically summarize representation learning architectures tailored for battery data, highlight their applications in data augmentation and cross-domain transfer, and further identify key challenges and future opportunities in data privacy, multimodal information integration, and model interpretability. Overall, representation learning establishes a solid foundation for the efficient development of next-generation intelligent BMS.
{"title":"Representation learning accelerates the development of models for Li-ion battery health diagnostics and prognostics","authors":"Quanquan Zhang, Mingyu Yang, Guanxi Sun, Yue Xiang, Shitong Wang, Junying Zhang, Shuangqi Li","doi":"10.1016/j.ensm.2026.104897","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104897","url":null,"abstract":"In recent years, the evolution of Li-ion battery material components, cell architectures, and application scenarios has posed significant challenges for the rapid adaptation of battery management systems (BMS). Accurate health diagnostics and prognostics are fundamental to reliable battery operation. However, traditional approaches based on empirical equations, physical models, or handcrafted features often suffer from limited generalization, heavy data demands, and time-consuming development. Representation learning, a major advancement in deep learning, is emerging as a powerful tool to accelerate battery health modeling. Under novel chemistries and unseen operating conditions, it mitigates data scarcity through generative learning and enables rapid model adaptation via transfer learning, which was overlooked in earlier reviews. We systematically summarize representation learning architectures tailored for battery data, highlight their applications in data augmentation and cross-domain transfer, and further identify key challenges and future opportunities in data privacy, multimodal information integration, and model interpretability. Overall, representation learning establishes a solid foundation for the efficient development of next-generation intelligent BMS.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"7 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957390","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}
In virtue of the wide electrochemical window and superior flame-retarded ability, phosphate electrolytes are widely employed as transport media in high-voltage lithium metal batteries. Unfortunately, the strong interaction of Li+-phosphates leads to inefficient Li+ transport. Furthermore, the uncontrollable electrode-electrolyte interphase originated from the labile interfacial species retards the stable cycling of lithium metal batteries during operation. Herein, in-built high dielectric dissociated reservoir and functional interfacial regulation additive were designed to boost the dissociation ability of Li+ and stabilize the bidirectional electrode-electrolyte interfaces. Benefitting from the strong desolvated kinetic of nanowires and excellent interfacial regulation function of lithium nitrate, the continuous Li+ transport pathway and homogeneous bidirectional electrode-electrolyte interfaces were constructed, preventing the lithium metal anode and high-nickel cathode from persistent reactive with phosphate electrolytes, revealed by theoretical calculation and ex-situ characterization. Attributed to the guided ion transfer pathway and oriented artificial solid electrolyte interface, the Li||Li symmetrical batteries exhibit excellent cycling stability of above 1000h at 2 mA cm−2 and 2 mAh cm−2. The Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) battery shows more than 90% capacity retention after 200 cycles at 1C. This strategy holds great promising for developing advanced electrolytes in other advanced electrochemical storage devices.
磷酸电解质由于具有较宽的电化学窗口和优异的阻燃性能，被广泛用作高压锂金属电池的输运介质。不幸的是，Li+-磷酸盐的强相互作用导致Li+输运效率低下。此外，不稳定的界面物质导致的电极-电解质界面相不可控，阻碍了锂金属电池在运行过程中的稳定循环。为此，设计了内置高介电离解储层和功能界面调节添加剂，以提高Li+的离解能力，稳定双向电极-电解质界面。理论计算和非原位表征表明，利用纳米线强大的脱溶动力学和硝酸锂优异的界面调节功能，构建了连续的Li+传输通道和均匀的双向电极-电解质界面，防止了锂金属阳极和高镍阴极与磷酸盐电解质的持续反应。锂||锂对称电池在2ma cm - 2和2mah cm - 2下具有1000h以上的循环稳定性，这主要归功于离子转移路径和定向人造固体电解质界面。Li||LiNi0.8Co0.1Mn0.1O2 （NCM811）电池在1C下循环200次后容量保持率超过90%。该策略对开发先进电解质用于其他先进的电化学存储装置具有很大的前景。
{"title":"Ameliorating the Ionic Transport Behavior in Nonflammable Phosphate towards High-Energy and Safe Lithium Metal Batteries","authors":"Ya-Fang Wang, Yuan Liu, Xiang-Dan Zhang, Xiong-Wei Wu, Yi-Lei Zhang, Hai-Yan Hu, Qiang Ma, Zhen-Ling Wang, Yao Xiao","doi":"10.1016/j.ensm.2026.104896","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104896","url":null,"abstract":"In virtue of the wide electrochemical window and superior flame-retarded ability, phosphate electrolytes are widely employed as transport media in high-voltage lithium metal batteries. Unfortunately, the strong interaction of Li<ce:sup loc=\"post\">+</ce:sup>-phosphates leads to inefficient Li<ce:sup loc=\"post\">+</ce:sup> transport. Furthermore, the uncontrollable electrode-electrolyte interphase originated from the labile interfacial species retards the stable cycling of lithium metal batteries during operation. Herein, in-built high dielectric dissociated reservoir and functional interfacial regulation additive were designed to boost the dissociation ability of Li<ce:sup loc=\"post\">+</ce:sup> and stabilize the bidirectional electrode-electrolyte interfaces. Benefitting from the strong desolvated kinetic of nanowires and excellent interfacial regulation function of lithium nitrate, the continuous Li<ce:sup loc=\"post\">+</ce:sup> transport pathway and homogeneous bidirectional electrode-electrolyte interfaces were constructed, preventing the lithium metal anode and high-nickel cathode from persistent reactive with phosphate electrolytes, revealed by theoretical calculation and ex-situ characterization. Attributed to the guided ion transfer pathway and oriented artificial solid electrolyte interface, the Li||Li symmetrical batteries exhibit excellent cycling stability of above 1000h at 2 mA cm<ce:sup loc=\"post\">−2</ce:sup> and 2 mAh cm<ce:sup loc=\"post\">−2</ce:sup>. The Li||LiNi<ce:inf loc=\"post\">0.8</ce:inf>Co<ce:inf loc=\"post\">0.1</ce:inf>Mn<ce:inf loc=\"post\">0.1</ce:inf>O<ce:inf loc=\"post\">2</ce:inf> (NCM811) battery shows more than 90% capacity retention after 200 cycles at 1C. This strategy holds great promising for developing advanced electrolytes in other advanced electrochemical storage devices.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"26 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145957392","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 : 2026-01-12DOI: 10.1016/j.ensm.2026.104900
Xueying Su , Shunyao Li , Zhenxin Chen , Hengrui Guo , Zihao Liu , Yutong Wang , Duo Chen , Zaijun Cheng , Tiefeng Liu , Hao Luo
The concurrent improvement of interfacial stability and Zn2+ transport kinetics across a broad temperature window continues to challenge aqueous zinc-ion batteries (AZIBs). Herein, a trifunctional polycationic interfacial layer (PDDA-TFSI, PTF) is introduced to broaden the advantages of the Zn(ClO4)2 electrolyte beyond its unique low-temperature tolerance. Specifically, while the hydrophobic architecture (TFSI−) of PTF locally disrupts the hydrogen-bond network of free water molecules, its uniformly distributed cationic sites (N+−R4) guarantee the efficient anchoring of corrosive ClO4−, fundamentally mitigating the strong oxidative propensity under high water activity particularly at ambient temperatures. Zn2+ desolvation and migration are facilitated by decoupling bulk and interfacial processes, with consequent improvement in transport kinetics and enhancement of the rate capability. The PTF@Zn electrode exhibits stable Zn plating/stripping for over 7000 h at 0.5 mA cm−2 and −30 °C. The PTF@Zn||AC@I2 full cell exhibits a low-capacity decay rate of merely ∼0.006% per cycle over 3000 cycles at 2.0 A g−1 over a wide temperature range from –30 °C to 25 °C. Notably, the pouch cell delivers 800 mAh capacity while retaining 92.3% after 100 cycles at –30 °C. This approach customizes a route to stabilize zinc anodes for wide-temperature operation, offering valuable insights into advanced AZIBs.
界面稳定性和Zn2+在宽温度窗内传输动力学的同时提高，继续挑战着水性锌离子电池（azib）。本文引入了一种三功能聚阳离子界面层（pda - tfsi， PTF），以扩大Zn(ClO4)2电解质在其独特的低温耐受性之外的优势。具体来说，虽然PTF的疏水结构（TFSI−）局部破坏了自由水分子的氢键网络，但其均匀分布的阳离子位点（N+−R4）保证了腐蚀性ClO4−的有效锚定，从根本上减轻了高水活度（特别是在环境温度下）下的强氧化倾向。解耦体和界面过程促进了Zn2+的脱溶和迁移，从而改善了输运动力学和提高了速率能力。PTF@Zn电极在0.5 mA cm - 2和- 30 °C下表现出稳定的镀锌/剥离超过7000小时。在-30°C至25°C的宽温度范围内，在2.0 a g - 1下，PTF@Zn||AC@I2全电池在3000次循环中显示出低容量衰减率，每周期仅为~ 0.006%。值得注意的是，袋式电池在-30°C下循环100次后，可提供800毫安时的容量，同时保持92.3%的容量。这种方法定制了一种稳定锌阳极的途径，用于宽温度操作，为先进的azib提供了有价值的见解。
{"title":"Steering Zn(ClO4)2 electrolyte: Trifunctional polycationic artificial interphase for Wide-Temperature Ah-level Zn-I2 pouch cells","authors":"Xueying Su , Shunyao Li , Zhenxin Chen , Hengrui Guo , Zihao Liu , Yutong Wang , Duo Chen , Zaijun Cheng , Tiefeng Liu , Hao Luo","doi":"10.1016/j.ensm.2026.104900","DOIUrl":"10.1016/j.ensm.2026.104900","url":null,"abstract":"<div><div>The concurrent improvement of interfacial stability and Zn<sup>2+</sup> transport kinetics across a broad temperature window continues to challenge aqueous zinc-ion batteries (AZIBs). Herein, a trifunctional polycationic interfacial layer (PDDA-TFSI, PTF) is introduced to broaden the advantages of the Zn(ClO<sub>4</sub>)<sub>2</sub> electrolyte beyond its unique low-temperature tolerance. Specifically, while the hydrophobic architecture (TFSI<sup>−</sup>) of PTF locally disrupts the hydrogen-bond network of free water molecules, its uniformly distributed cationic sites (N<sup>+</sup>−R<sub>4</sub>) guarantee the efficient anchoring of corrosive ClO<sub>4</sub><sup>−</sup>, fundamentally mitigating the strong oxidative propensity under high water activity particularly at ambient temperatures. Zn<sup>2+</sup> desolvation and migration are facilitated by decoupling bulk and interfacial processes, with consequent improvement in transport kinetics and enhancement of the rate capability. The PTF@Zn electrode exhibits stable Zn plating/stripping for over 7000 h at 0.5 mA cm<sup>−2</sup> and −30 °C. The PTF@Zn||AC@I<sub>2</sub> full cell exhibits a low-capacity decay rate of merely ∼0.006% per cycle over 3000 cycles at 2.0 A g<sup>−1</sup> over a wide temperature range from –30 °C to 25 °C. Notably, the pouch cell delivers 800 mAh capacity while retaining 92.3% after 100 cycles at –30 °C. This approach customizes a route to stabilize zinc anodes for wide-temperature operation, offering valuable insights into advanced AZIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104900"},"PeriodicalIF":20.2,"publicationDate":"2026-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955476","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}
The sluggish Na+ diffusion within hard carbon (HC) anodes remains the key bottleneck restricting the low-temperature operation of sodium-ion batteries (SIBs). While previous studies have mainly optimized closed-pore structures, the critical role of interdomain interconnectivity in governing ion transport has been largely overlooked. Here, we develop a pillar-supporting strategy to unfold carbon layers and construct interstitial topological diffusion networks, enabling efficient bulk Na⁺ transport under low temperatures. The reconstructed hard carbon (P-HC) exhibits a loosely packed architecture with enlarged carbon layers (∼4-5 nm) and closed pores (∼9 Å), compared to conventional HC (∼1-2 nm layers, 5.7 Å pores). Modeling further reveals that the interstitial spacing of P-HC (1.66 nm) is nearly twice that of HC (0.83 nm), providing open topological pathways that effectively facilitate Na+ diffusion. Consequently, P-HC delivers a reversible capacity of 403.5 mAh g-1 with an initial Coulombic efficiency of 93% at 25 °C and maintains 268.5 mAh g-1 at -20 °C, far exceeding HC (47 mAh g-1). This work introduces the concept of interstitial topology beyond conventional closed-pore models, offering fresh insights into designing advanced carbon anodes for SIBs operating in extreme environments.
硬碳（HC）阳极内Na+扩散缓慢仍然是制约钠离子电池低温运行的关键瓶颈。虽然以往的研究主要是优化闭孔结构，但在很大程度上忽视了域间互连在控制离子输运中的关键作用。在这里，我们开发了一种支柱支撑策略来展开碳层并构建间隙拓扑扩散网络，使Na⁺在低温下高效传输。与传统的硬碳（1-2纳米层，5.7 Å孔）相比，重建的硬碳（P-HC）具有松散的结构，具有扩大的碳层（~ 4-5 nm）和封闭的孔隙（~ 9 Å）。模型进一步表明，P-HC的间隙（1.66 nm）几乎是HC （0.83 nm）的两倍，提供了开放的拓扑通路，有效促进Na+扩散。因此，P-HC在25°C时提供403.5 mAh g-1的可逆容量，初始库仑效率为93%，在-20°C时保持268.5 mAh g-1，远远超过HC （47 mAh g-1）。这项工作在传统的闭孔模型之外引入了间隙拓扑的概念，为在极端环境中工作的sib设计先进的碳阳极提供了新的见解。
{"title":"Unfolding Carbon Layers to Engineer Interstitial Topological Space for Hard Carbon Anodes in Low-Temperature Sodium-Ion Batteries","authors":"Ru Wang, Yaxin Chen, Zhipeng Cao, Liluo Shi, Nannan Guo, Xia Qiu, Yirong Wang, Luxiang Wang, Quanchao Zhuang, Zhicheng Ju","doi":"10.1016/j.ensm.2026.104894","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104894","url":null,"abstract":"The sluggish Na<sup>+</sup> diffusion within hard carbon (HC) anodes remains the key bottleneck restricting the low-temperature operation of sodium-ion batteries (SIBs). While previous studies have mainly optimized closed-pore structures, the critical role of interdomain interconnectivity in governing ion transport has been largely overlooked. Here, we develop a pillar-supporting strategy to unfold carbon layers and construct interstitial topological diffusion networks, enabling efficient bulk Na⁺ transport under low temperatures. The reconstructed hard carbon (P-HC) exhibits a loosely packed architecture with enlarged carbon layers (∼4-5 nm) and closed pores (∼9 Å), compared to conventional HC (∼1-2 nm layers, 5.7 Å pores). Modeling further reveals that the interstitial spacing of P-HC (1.66 nm) is nearly twice that of HC (0.83 nm), providing open topological pathways that effectively facilitate Na<sup>+</sup> diffusion. Consequently, P-HC delivers a reversible capacity of 403.5 mAh g<sup>-1</sup> with an initial Coulombic efficiency of 93% at 25 °C and maintains 268.5 mAh g<sup>-1</sup> at -20 °C, far exceeding HC (47 mAh g<sup>-1</sup>). This work introduces the concept of interstitial topology beyond conventional closed-pore models, offering fresh insights into designing advanced carbon anodes for SIBs operating in extreme environments.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"268 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145949856","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}
Olivine-structured LiMn1–xFexPO4 phosphates have emerged as one of the most promising cathodes for Lithium-ion batteries owing to their high energy density, low cost, and non-toxicity. However, the intrinsic electronic/ionic insulating properties and the Jahn-Teller effect limit their rate performance and reversibility. Here, we propose grain-refining and fast-ion-conductive epitaxial layer regulation via a thermodynamics-sanctified multi-cationic interaction strategy to booming Li-storage kinetics and reversibility of LiMn0.8Fe0.2PO4 cathodes. Both computational and experimental results demonstrate that the thermodynamically driven enrichment of V and Ti on the surfaces of V-Ti-Mg co-modified LiMn0.8Fe0.2PO4 (LMFP-VTM) promotes the particle refinement and the formation of quasi-amorphous epitaxial layers. Particle nanometrization assisted with coherent multi-ion quasi-disordered epitaxial layers facilitate the Li+ transport kinetics strikingly, as well as mitigate Jahn-Teller effect-driven pernicious structural degradation. The optimized LMFP-VTM cathode achieves 151.6 mAh g-1 initial capacity at 0.1 C and retains 93.5 mAh g-1 at 15 C. It exhibits exceptional cyclability with 95.4 and 82.5% capacity retentions after 1000 cycles (1 C) and 3000 cycles (5 C), respectively. The findings in this work expanded the perspective on the structural engineering of high energy density olivine-structured cathode materials with ultrafast kinetics.
橄榄石结构的LiMn1-xFexPO4磷酸盐由于其高能量密度、低成本和无毒性而成为锂离子电池最有前途的阴极之一。然而，固有的电子/离子绝缘性能和扬-泰勒效应限制了它们的速率性能和可逆性。在这里，我们提出了晶粒细化和快速离子导电外延层调节，通过一个热力学的多阳离子相互作用策略，以提高锂存储动力学和LiMn0.8Fe0.2PO4阴极的可逆性。计算和实验结果表明，V-Ti- mg共改性LiMn0.8Fe0.2PO4 （LMFP-VTM）表面V和Ti的热驱动富集促进了颗粒细化和准非晶外延层的形成。粒子纳米化辅助的相干多离子准无序外延层显著地促进了Li+的输运动力学，并减轻了Jahn-Teller效应驱动的有害结构降解。优化后的LMFP-VTM阴极在0.1℃时达到151.6 mAh g-1的初始容量，在15℃时保持93.5 mAh g-1，在1000次循环（1℃）和3000次循环（5℃）后分别保持95.4和82.5%的容量。本工作的发现拓展了高能量密度橄榄石结构超快动力学正极材料结构工程的研究前景。
{"title":"Thermodynamically Tuned Element Diffusion Enables Ultrafast Kinetics and Structural Reversibility in Grain-Refined LiMn0.8Fe0.2PO4 Cathodes for High-Energy-Density Batteries","authors":"Yuanpeng Cao, Wenhui Tu, Jingjing He, Jianguo Duan, Runlin Li, Xinyu Zhang, Chenyi Huang, Liqi Li, Yingjie Zhang, Yuanbing Wang, Peng Dong, Xianshu Wang, Ding Wang","doi":"10.1016/j.ensm.2026.104893","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104893","url":null,"abstract":"Olivine-structured LiMn<sub>1–x</sub>Fe<sub>x</sub>PO<sub>4</sub> phosphates have emerged as one of the most promising cathodes for Lithium-ion batteries owing to their high energy density, low cost, and non-toxicity. However, the intrinsic electronic/ionic insulating properties and the Jahn-Teller effect limit their rate performance and reversibility. Here, we propose grain-refining and fast-ion-conductive epitaxial layer regulation via a thermodynamics-sanctified multi-cationic interaction strategy to booming Li-storage kinetics and reversibility of LiMn<sub>0.8</sub>Fe<sub>0.2</sub>PO<sub>4</sub> cathodes. Both computational and experimental results demonstrate that the thermodynamically driven enrichment of V and Ti on the surfaces of V-Ti-Mg co-modified LiMn<sub>0.8</sub>Fe<sub>0.2</sub>PO<sub>4</sub> (LMFP-VTM) promotes the particle refinement and the formation of quasi-amorphous epitaxial layers. Particle nanometrization assisted with coherent multi-ion quasi-disordered epitaxial layers facilitate the Li<sup>+</sup> transport kinetics strikingly, as well as mitigate Jahn-Teller effect-driven pernicious structural degradation. The optimized LMFP-VTM cathode achieves 151.6 mAh g<sup>-1</sup> initial capacity at 0.1 C and retains 93.5 mAh g<sup>-1</sup> at 15 C. It exhibits exceptional cyclability with 95.4 and 82.5% capacity retentions after 1000 cycles (1 C) and 3000 cycles (5 C), respectively. The findings in this work expanded the perspective on the structural engineering of high energy density olivine-structured cathode materials with ultrafast kinetics.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"7 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145949871","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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