Energy Storage Materials最新文献

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Heteroatom-tuned Bi pz-orbital hybridization of single-atom catalysts for high-power density vanadium flow batteries 高功率密度钒液流电池单原子杂原子调谐Bi - pz轨道杂化
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-20 DOI: 10.1016/j.ensm.2025.104472
Fei Xing , Shuo Wang , Qiang Fu , Tao Liu , Xianfeng Li
{"title":"Heteroatom-tuned Bi pz-orbital hybridization of single-atom catalysts for high-power density vanadium flow batteries","authors":"Fei Xing ,&nbsp;Shuo Wang ,&nbsp;Qiang Fu ,&nbsp;Tao Liu ,&nbsp;Xianfeng Li","doi":"10.1016/j.ensm.2025.104472","DOIUrl":"10.1016/j.ensm.2025.104472","url":null,"abstract":"<div><div>Highly active single-atom electrocatalysts can effectively enhance the power density of vanadium flow batteries by forming hybrid orbitals between metal atoms and heteroatoms. However, the mechanism through which hybrid orbitals boost the activity of vanadium ions remains unclear. Herein, we report the Bi single atoms electrocatalysts (XBi, <em>X</em> = <em>N</em>, P, S, B) with different heteroatoms coordination, while catalytic activity towards [V(H<sub>2</sub>O)<sub>6</sub>]<sup>3+</sup>/[V(H<sub>2</sub>O)<sub>6</sub>]<sup>2+</sup>is proved to be NBi&gt;PBi&gt;SBi&gt;BBi. The results demonstrated that PBi, SBi, and BBi display the electron cloud distributions of Bi atoms near the fermi level towards the planar direction (p<sub>x</sub>, p<sub>y</sub>), while NBi exhibits an axial orbital (p<sub>z</sub>) distribution and a more pronounced Bi-N p-orbital hybridization due to the high electronegativity of N, thereby promoting vanadium ion dehydration. In consequence, a VFB single cell equipped with NBi decorated graphite felt (GF) electrode demonstrates the most superior battery performance among all fabricated electrodes, achieving a 7 % increase in energy efficiency at a current density of 240 mA cm<sup>−2</sup> compared to the BBi-loaded counterpart. The hybrid orbital engineering strategy establishes a design paradigm for single-atom electrocatalysts in high-power density VFBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104472"},"PeriodicalIF":18.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144664565","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}
引用次数: 0
Unveiling the role of base layer in the fluorinated cathode interface for robust single-crystal Na-layered oxide 揭示基层在稳健性单晶钠层氧化物氟化阴极界面中的作用
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-20 DOI: 10.1016/j.ensm.2025.104474
Huiru Wang , Shihao Li , Fangyan Liu , Yi Zhang , Wei Zhou , Ziyue Qiu , Rui Jin , Yuhang Zhang , Zhian Zhang
{"title":"Unveiling the role of base layer in the fluorinated cathode interface for robust single-crystal Na-layered oxide","authors":"Huiru Wang ,&nbsp;Shihao Li ,&nbsp;Fangyan Liu ,&nbsp;Yi Zhang ,&nbsp;Wei Zhou ,&nbsp;Ziyue Qiu ,&nbsp;Rui Jin ,&nbsp;Yuhang Zhang ,&nbsp;Zhian Zhang","doi":"10.1016/j.ensm.2025.104474","DOIUrl":"10.1016/j.ensm.2025.104474","url":null,"abstract":"<div><div>Fluorinated interface engineering has emerged as a viable strategy for designing high-performance layered oxide cathodes and sodium-ion batteries (SIBs). Nevertheless, the rational approaches for the interface fluorination of oxide cathodes remain controversial. In particular, the influence exerted by various surfaces of Na-layered oxides as the base layer on the fluorinated interface remains an unresolved issue. Herein, the cathode surface fluorination engineering (CSFE) is proposed to modulate the state of the base layer and the fluorinated electrolyte additive engineering (FEAE) is adopted to synergistically construct fluorinated cathode interface on the single-crystal NaNi<sub>1/3</sub>Fe<sub>1/3</sub>Mn<sub>1/3</sub>O<sub>2</sub> (NFM). CSFE converts the surface Na<sub>2</sub>CO<sub>3</sub> layer into a NaF layer in-situ with partial F surface doping, which gives rise to a NaF-rich cathode-electrolyte interface (CEI) with enhanced stability during cycling even in the fluorine-free carbonate-based electrolyte and makes surface fluorinated oxide (NFM@F) possess higher coulombic efficiency and better cycling stability than the oxide with Na<sub>2</sub>CO<sub>3</sub> base layer. While in the electrolyte with fluorinated additive, a NaF-rich CEI that is thinner, more uniform and denser can be formed on the NaF base layer of NFM@F (NFM@F-FE) than on the Na<sub>2</sub>CO<sub>3</sub> based layer, thereby significantly reducing side reactions, shielding the layered structure, mitigating structural change during charge-discharge, and manifesting exceptional structure stability. Consequently, NFM@F-FE exhibits a remarkable capacity retention of up to 94.26 % even after 200 cycles at 1 C.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104474"},"PeriodicalIF":18.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144664563","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}
引用次数: 0
Interplay of interfacial and structural cracking degradation modes for the high-voltage LiCoO2 cathode at particle’s level 颗粒级高电压LiCoO2阴极界面与结构裂纹退化模式的相互作用
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-20 DOI: 10.1016/j.ensm.2025.104473
Xuerui Yang , Ying Lin , Shijun Tang , Yuqi Zhou , Xuan Huang , Wen Song , Wen Yang , Yong Yang
{"title":"Interplay of interfacial and structural cracking degradation modes for the high-voltage LiCoO2 cathode at particle’s level","authors":"Xuerui Yang ,&nbsp;Ying Lin ,&nbsp;Shijun Tang ,&nbsp;Yuqi Zhou ,&nbsp;Xuan Huang ,&nbsp;Wen Song ,&nbsp;Wen Yang ,&nbsp;Yong Yang","doi":"10.1016/j.ensm.2025.104473","DOIUrl":"10.1016/j.ensm.2025.104473","url":null,"abstract":"<div><div>Elevating the cut-off voltage is a promising strategy to enhance the energy density of LiCoO<sub>2</sub> (LCO), as demonstrated by a ∼22 % increase in discharge capacity at 4.6 V compared to 4.5 V. However, severe structural degradation and interfacial instability above 4.5 V hinder its practical application, with limited research focusing on decoupling these mechanisms to mitigate performance decay. Herein, LCO samples with distinct particle sizes are systematically investigated by using electrochemical techniques and numerical modeling to elucidate complex failure modes. Larger-sized LCO particles exhibit structural cracking and fracture, particularly at high current density, due to prolonged Li<sup>+</sup> diffusion pathways, inhomogeneous lithium distribution, and stress accumulation. Conversely, smaller-sized LCO particles suffer from intensified interfacial side reactions attributed to their higher surface area, especially at low current density. These results highlight that LCO degradation arises from the interplay of size- and rate-dependent mechanisms rather than a single dominant factor. To address this complexity, we develop a multivariate nonlinear equation to fully decouple different degradation mechanisms and successfully determine the optimal mass mixing ratios of larger- and smaller-sized LCO particles under various current density conditions to maximize cycling stability. This work provides valuable mechanistic insights into degradation pathways and effectively bridges the gap between empirical optimization and a deeper understanding of LCO degradation.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104473"},"PeriodicalIF":18.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144664561","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}
引用次数: 0
Advancing sodium-ion batteries toward commercialization: A review on phosphate and sulfate-based polyanionic cathodes 推进钠离子电池商业化:磷酸盐和硫酸盐基多阴离子阴极研究进展
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-19 DOI: 10.1016/j.ensm.2025.104468
Hao Ge, Fan Kong, Shikang Jiang, Heru Huang, DaiJun He, Xin Huang, Xiaowei Mu, Hui Xia
{"title":"Advancing sodium-ion batteries toward commercialization: A review on phosphate and sulfate-based polyanionic cathodes","authors":"Hao Ge,&nbsp;Fan Kong,&nbsp;Shikang Jiang,&nbsp;Heru Huang,&nbsp;DaiJun He,&nbsp;Xin Huang,&nbsp;Xiaowei Mu,&nbsp;Hui Xia","doi":"10.1016/j.ensm.2025.104468","DOIUrl":"10.1016/j.ensm.2025.104468","url":null,"abstract":"<div><div>Sodium-ion batteries (SIBs) are considered as a promising supplement to lithium-ion batteries for large-scale energy storage applications due to the abundance and cost-effectiveness of sodium resources. Among various cathode materials, polyanionic compounds, particularly phosphate and sulfate-based ones, have garnered significant attention for their good structural stability, high redox potentials, and favorable Na<sup><sup>+</sup></sup>x002B diffusion channels. However, challenges such as low electronic conductivity, limited capacity, and complex synthesis procedures hinder their widespread application. This review starts with the key characteristics of polyanionic materials, followed by a thorough summary of recent advancements in phosphate and sulfate-based cathodes, emphasizing their crystal structures, electrochemical properties, and sodium storage mechanisms. Then, the preparation methods and advanced modification strategies, including surface coating, particle size engineering, morphology and interface design, and element doping, are reviewed in detail. By systematically comparing phosphates and sulfates, this review integrates their commercialization progress and application scenarios from an industry-oriented perspective. This highlights the importance of industry-academia collaboration in accelerating the transition of polyanionic cathode materials from laboratory research to practical applications. Finally, future research directions and innovative approaches are proposed to overcome existing challenges, paving the way for the practical deployment of these materials in next-generation sustainable energy storage systems.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104468"},"PeriodicalIF":18.9,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144664597","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}
引用次数: 0
Advancing NASICON solid-state electrolytes for lithium metal batteries: interfacial challenges, engineering strategies, and future directions 推进NASICON固态电解质用于锂金属电池:界面挑战,工程策略和未来方向
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-19 DOI: 10.1016/j.ensm.2025.104471
Jiangwei Shen, Can Cui, Jie Zhao, Haiqin Lin, Yudong Zhang, Weiji Dai, Cuijiao Zhao, Saifang Huang
{"title":"Advancing NASICON solid-state electrolytes for lithium metal batteries: interfacial challenges, engineering strategies, and future directions","authors":"Jiangwei Shen,&nbsp;Can Cui,&nbsp;Jie Zhao,&nbsp;Haiqin Lin,&nbsp;Yudong Zhang,&nbsp;Weiji Dai,&nbsp;Cuijiao Zhao,&nbsp;Saifang Huang","doi":"10.1016/j.ensm.2025.104471","DOIUrl":"10.1016/j.ensm.2025.104471","url":null,"abstract":"<div><div>Solid-state lithium metal batteries (SSLMBs) have emerged as a highly promising next-generation energy storage technology due to their superior safety and high energy-density. Among all solid-state electrolytes, sodium superionic conductor (NASICON) electrolytes are particularly noteworthy, offering high ionic conductivity, excellent air stability, and wide electrochemical window, making them one of the most extensively studied and technologically viable options. However, critical interfacial challenges persist between NASICON electrolytes and lithium metal anodes, including poor physical contact, insufficient chemical/electrochemical stability, and detrimental side reactions, all of which significantly hinder battery performance. These interfacial phenomena involve multifaceted complexities, such as intrinsic material properties, dynamic side reactions, and spatiotemporal evolution-processes, which are inherently difficult to observe using conventional characterization techniques. Here, this review systematically analyzes the interfacial issues between NASICON electrolytes and Li anodes, evaluating existing modification strategies (e.g., inorganic coatings, organic/polymer coatings, composite coatings, and anode protection mechanisms) and highlighting advanced characterization techniques which provide deeper insights into the dynamic interactions occurring at the interface, facilitating the rational design and optimization of solid-state batteries. Advanced characterization techniques are discussed for interfacial analysis. By leveraging advanced interfacial engineering strategies and characterization techniques, researchers can accelerate the development of safer, more efficient, and longer-lasting solid-state lithium batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104471"},"PeriodicalIF":18.9,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144664564","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}
引用次数: 0
Dynamic interface regulation in solid-state lithium-metal batteries by in situ polymerized highly elastic ultrathin layers 原位聚合高弹性超薄层在固态锂金属电池中的动态界面调节
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-19 DOI: 10.1016/j.ensm.2025.104469
Kaiming Wang , Jingjin Xu , Ming Xu , Fei Shen , Liang Zhang , Zhiyi Zhou , Aaron Jue Kang Tieu , Haowen Wu , Xiaogang Han , Stefan Adams
{"title":"Dynamic interface regulation in solid-state lithium-metal batteries by in situ polymerized highly elastic ultrathin layers","authors":"Kaiming Wang ,&nbsp;Jingjin Xu ,&nbsp;Ming Xu ,&nbsp;Fei Shen ,&nbsp;Liang Zhang ,&nbsp;Zhiyi Zhou ,&nbsp;Aaron Jue Kang Tieu ,&nbsp;Haowen Wu ,&nbsp;Xiaogang Han ,&nbsp;Stefan Adams","doi":"10.1016/j.ensm.2025.104469","DOIUrl":"10.1016/j.ensm.2025.104469","url":null,"abstract":"<div><div>Poly(vinylidene fluoride) (PVDF)-based solid-stated electrolytes (SSEs) hold great promise for high-energy-density solid-state lithium metal batteries (SSLMBs) due to their relatively high ionic conductivity and excellent flexibility. However, their practical performance is hindered by instability at the Li/PVDF interface, where the porous PVDF induces uneven ion deposition and residual N,N-dimethylformamide (DMF) solvent triggers severe side reactions with Li. Here, we demonstrate that a highly elastic layer, introduced via in situ polymerization of 1,3-dioxolane (P-DOL) containing thermoplastic polyurethane (TPU), effectively stabilizes and dynamically regulates the Li/PVDF interface. The incorporation of TPU enhances the elastic modulus of the cured layer, enabling local stress redistribution and dynamic retention of intimate interfacial contact at the Li/PVDF interface during cycling, which in turn promotes dense and flat Li deposition morphology to prolong the cycle life. Moreover, the interlayer prevents side reactions between DMF residues and Li anode, preserving an electrochemically stable contact. Consequently, the Li|PVDF|LiNi<sub>0.8</sub>Co<sub>0.</sub><sub><sub>1</sub></sub>Mn<sub>0.1</sub>O<sub>2</sub> cell with TPU/P-DOL interlayer delivers a capacity of 136 mA h <em>g</em><sup>−1</sup> over 800 cycles at 1 C. Our findings demonstrate a scalable interfacial engineering strategy that addresses the key bottleneck of PVDF-based SSEs and significantly advances the performance of SSLMBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104469"},"PeriodicalIF":18.9,"publicationDate":"2025-07-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144664593","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}
引用次数: 0
Recycling-regenerating salt enables the economic viability of aqueous high-concentration electrolytes 盐的回收再生使高浓度水电解质具有经济可行性
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-18 DOI: 10.1016/j.ensm.2025.104465
Jiuzhou Lu , Hefei Fan , Dexin Dan , Anxing Zhou , Kaiyuan Zheng , Yang Yang , Yong-Sheng Hu , Liquan Chen , Liumin Suo
{"title":"Recycling-regenerating salt enables the economic viability of aqueous high-concentration electrolytes","authors":"Jiuzhou Lu ,&nbsp;Hefei Fan ,&nbsp;Dexin Dan ,&nbsp;Anxing Zhou ,&nbsp;Kaiyuan Zheng ,&nbsp;Yang Yang ,&nbsp;Yong-Sheng Hu ,&nbsp;Liquan Chen ,&nbsp;Liumin Suo","doi":"10.1016/j.ensm.2025.104465","DOIUrl":"10.1016/j.ensm.2025.104465","url":null,"abstract":"<div><div>The aqueous high-salt-concentrated electrolytes expand the electrochemical stability window (ESW), providing aqueous batteries with high output voltage and energy density. However, the increased salt concentration also raises costs, negatively affecting the economic feasibility for electric energy storage. Herein, we demonstrate that the aqueous highly concentrated lithium trifluoromethyl sulfonamide (LiTFSI) electrolytes are easy to recycle through salt extraction methods. Furthermore, to circumvent energy-intensive dehydration processes induced by LiTFSI hygroscopicity, we propose a direct regeneration protocol based on concentration-density correlation. The recycled/regenerated electrolytes maintain similar physical and chemical properties comparable to pristine electrolytes, exhibiting a wide ESW of 3 V. Pouch cells (0.5 Ah) assembled with the recycled and regenerated electrolyte exhibit equivalent performance to the pristine electrolyte, maintaining a capacity of over 87 % after 300 cycles. Techno-economic analysis indicates that recycling salt reduces costs by 69.3 % and regeneration electrolyte by 71.2 %, both of which require wastewater treatment amounting to merely 5.6 % of salt production. Remarkably, regeneration achieves substantial reductions in energy consumption (93.9 %) and CO<sub>2</sub> emissions (94.8 %) by eliminating energy-intensive drying processes, surpassing salt recycling's 85.4 % and 87.9 % reductions. Our work aims to provide a cost-effective and sustainable solution for using high-concentration electrolytes, enabling the practical implementation of aqueous lithium-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104465"},"PeriodicalIF":18.9,"publicationDate":"2025-07-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652594","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}
引用次数: 0
Enabling anion-anchoring and anti-degradation cellulose separators for sodium metal batteries 用于钠金属电池的阴离子锚定和抗降解纤维素分离器
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-17 DOI: 10.1016/j.ensm.2025.104463
Ying Zhang , Shanchen Yang , Shan Liu , Zichan Yuan , Jie Deng , Ningxin Chen , Yiju Li , Chaoji Chen , Zhaohui Wang
{"title":"Enabling anion-anchoring and anti-degradation cellulose separators for sodium metal batteries","authors":"Ying Zhang ,&nbsp;Shanchen Yang ,&nbsp;Shan Liu ,&nbsp;Zichan Yuan ,&nbsp;Jie Deng ,&nbsp;Ningxin Chen ,&nbsp;Yiju Li ,&nbsp;Chaoji Chen ,&nbsp;Zhaohui Wang","doi":"10.1016/j.ensm.2025.104463","DOIUrl":"10.1016/j.ensm.2025.104463","url":null,"abstract":"<div><div>Renewable cellulose biopolymers have emerged as sustainable and efficient separator materials for sodium metal batteries, owing to their capacity to regulate ion transport and sodium deposition. In this study, we engineer nanocellulose separators by introducing a Zr-O complex coating layer, which negates the intrinsically strong hydrogen bond interactions in conventional nanocellulose, endowing the separator with anti-degradation and anion-anchoring properties. The Zr-O complex not only preserves the nanofibrous network and improves the electrochemical stability of nanocellulose but also expands and stabilizes ion transport channels. More importantly, this Zr-O complex coating transforms the predominantly Na<sup>+</sup> ions adsorption on carboxyl groups into preferentially ClO<sub>4</sub><sup>-</sup> anions immobilization, leading to a high Na<sup>+</sup> transference number of 0.76. Meanwhile, both experimental and calculation results demonstrate that the intrinsic ferroelectric properties of the Zr-O complex promote the reduction of ClO<sub>4</sub><sup>-</sup> anions, and facilitate the formation of a NaCl/NaF-enriched solid electrolyte interphase. These enhancements significantly improved cycle stability, with the Na||Na cells operating over 1100 h at 0.25 mA cm<sup>-2</sup>/0.25 mAh cm<sup>-2</sup>, about 2.6 times longer than traditional cellulose separators. This research offers new insights into the development of sustainable, and high-performance rechargeable sodium metal batteries through the innovative engineering of natural biopolymers.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104463"},"PeriodicalIF":18.9,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652596","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}
引用次数: 0
Synergistic ionic-molecular coordination engineering in weakly solvating ether electrolytes for stable high-voltage lithium metal batteries 稳定高压锂金属电池弱溶剂化醚电解质的离子-分子协同工程
IF 18.9 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-17 DOI: 10.1016/j.ensm.2025.104467
Suyun Liu , Zhiwei Ni , Zhengran Wang , Junjie Liu , Huizi Zhang , Chen Yang , Yuan Li , Shenglin Xiong , Baojuan Xi , Xiaohang Lin , Jinkui Feng
{"title":"Synergistic ionic-molecular coordination engineering in weakly solvating ether electrolytes for stable high-voltage lithium metal batteries","authors":"Suyun Liu ,&nbsp;Zhiwei Ni ,&nbsp;Zhengran Wang ,&nbsp;Junjie Liu ,&nbsp;Huizi Zhang ,&nbsp;Chen Yang ,&nbsp;Yuan Li ,&nbsp;Shenglin Xiong ,&nbsp;Baojuan Xi ,&nbsp;Xiaohang Lin ,&nbsp;Jinkui Feng","doi":"10.1016/j.ensm.2025.104467","DOIUrl":"10.1016/j.ensm.2025.104467","url":null,"abstract":"<div><div>Lithium metal batteries (LMBs) face critical challenges such as uncontrolled Li dendrite growth, unstable interfaces, and irreversible inactive Li formation. This study proposes an ionic-molecule synergistic electrolyte engineering strategy utilizing a weakly solvating electrolyte (WSE) with dual additives—lithium nitrate (LiNO₃) and tris(pentafluorophenyl)borane (TPFPB). The molecular interactions between TPFPB and NO₃⁻ allow LiNO₃ to be effectively dissolved in DOX. Meanwhile, TPFPB coordinates with FSI⁻ anions to facilitate salt dissociation. These processes optimise the solvation structure towards contact ion pairs (CIPs) and aggregates (AGGs). Density functional theory (DFT) calculations and molecular dynamics (MD) simulations confirm that the solvation structure has been effectively optimized through the introduction of synergistic additives, which promotes the formation of inorganic-rich interfacial layers to protect both the anode and the cathode. Consequently, Li||LiFePO₄ cells maintain 98.14 % capacity retention over 480 cycles at 1 C. Moreover, a full battery assembled with high-loading LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cathode (1.82 mAh cm⁻²) coupled with ultrathin Li anode (50 μm) retains 88.0 % capacity after 250 cycles under high-voltage operation (4.4 V). This work elucidates an ionic-molecular coordination paradigm for WSE design, providing insights into next-generation electrolyte engineering in practical high-energy-density lithium metal batteries. Furthermore, the proposed strategy holds broader implications for the development of other metal-based battery systems, including but not limited to Na, K, Mg, and Zn multivalent ion systems.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104467"},"PeriodicalIF":18.9,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652592","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}
引用次数: 0
Dual-Interface Engineering via Boron Pre-anchoring and Electronegative Synergy for Coupled Ion Transport and Self-stabilizing Interphases in Lithium Metal Batteries 基于硼预锚定和电负协同的锂金属电池离子输运和自稳定界面双界面工程
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-17 DOI: 10.1016/j.ensm.2025.104466
Jiongjing Lu, Qiujiang Dong, Kang Liao, Minjie Yao, Hao Guo, Qianqiu Tian, Hui Hu, He Huang, Wanyao Li, Zhaoyong Sun, Qiang Chen, Xiaopeng Han, Wenbin Hu
{"title":"Dual-Interface Engineering via Boron Pre-anchoring and Electronegative Synergy for Coupled Ion Transport and Self-stabilizing Interphases in Lithium Metal Batteries","authors":"Jiongjing Lu, Qiujiang Dong, Kang Liao, Minjie Yao, Hao Guo, Qianqiu Tian, Hui Hu, He Huang, Wanyao Li, Zhaoyong Sun, Qiang Chen, Xiaopeng Han, Wenbin Hu","doi":"10.1016/j.ensm.2025.104466","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104466","url":null,"abstract":"Lithium metal anodes hold immense promise for next-generation high-energy-density batteries due to their outstanding theoretical capacity and low electrochemical potential. Despite these advantages, their practical implementation remains restricted by the unstable solid electrolyte interphase (SEI) and the uncontrollable lithium dendrite growth, which compromise cycling stability and safety. In this work, we propose a dual-interface engineering approach involving boron pre-anchoring in lithium anodes and coordination with electronegative components. This design establishes coupled mechanisms for ion transport optimization and self-stabilizing interphase formation through a hierarchical interface architecture. Theoretical simulations reveal that pre-embedded boron atoms lower the adsorption energy for lithium-ion diffusion while directing homogeneous metal deposition. Consequently, symmetric cells deliver stable Li plating/stripping behavior for over 2500 hours at 0.5 mA cm<sup>-2</sup>. Full cells paired with LiCoO<sub>2</sub> retain 92% capacity after 200 cycles, while Li-B||NCM811 pouch cells (6.5Ah) exhibit a high energy density of 526 Wh kg⁻¹ and maintain 95% capacity retention after 60 cycles. The interfacial design principles provide a blueprint for synchronizing ion transport kinetics and chemical stability in high-performance lithium metal batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"109 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144652593","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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