Energy Storage Materials最新文献_第3页

Oxysulfide Solid Electrolytes: The Impact of Oxygen in Sulfides 硫化氧固体电解质：氧在硫化物中的影响

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-08 DOI: 10.1016/j.ensm.2025.104669

Woojung Lee, Yuna Kim, Jiyun Han, In Young Kim

{"title":"Oxysulfide Solid Electrolytes: The Impact of Oxygen in Sulfides","authors":"Woojung Lee, Yuna Kim, Jiyun Han, In Young Kim","doi":"10.1016/j.ensm.2025.104669","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104669","url":null,"abstract":"Sulfide solid electrolytes have gained significant attention because they are crucial to the development of high-performance all-solid-state batteries (ASSBs). However, their practical application is hindered by chemical instability and incompatible interfaces with electrodes, highlighting the need for advanced technological solutions. Oxygen doping into sulfide solid electrolytes has emerged as a promising approach for balancing high ionic conductivity and robust stability. However, the underlying chemistry of oxysulfide solid electrolytes remains insufficiently understood. This review discusses the challenges faced by sulfide solid electrolytes and highlights the advantages of oxysulfide counterparts in addressing these limitations. It covers synthesis and characterization methods for oxysulfide solid electrolytes, categorized by their crystallinity and parent sulfide structures. This review also examines the fundamental mechanisms by which oxygen doping enhances ionic conductivities, lowers activation energies for lithium migration, and improves chemical and electrochemical stabilities. In addition, this review summarizes the battery performance of state-of-the-art oxysulfide solid electrolytes. Finally, future research directions are proposed to advance the viability and safety of next-generation ASSBs that incorporate oxysulfide solid electrolytes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"24 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247661","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

Defect-promoted domain-free dipole growth and optimized energy storage performance in weakly polar dielectrics 弱极性电介质中缺陷促进的无畴偶极子生长和优化的储能性能

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-08 DOI: 10.1016/j.ensm.2025.104666

Lei Cao, Lang Zhang, Ying Yuan, Yao Hu, Kaixin Song

{"title":"Defect-promoted domain-free dipole growth and optimized energy storage performance in weakly polar dielectrics","authors":"Lei Cao, Lang Zhang, Ying Yuan, Yao Hu, Kaixin Song","doi":"10.1016/j.ensm.2025.104666","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104666","url":null,"abstract":"The progress of modern electronic devices puts forward higher requirements for the energy storage performance of capacitors. In order to further improve the energy storage density of existing advanced weakly polar dielectrics, we propose an innovative strategy for polarization optimization through the construction of a domain-free polarization configuration achieved by developing substantially grown non-aggregated dipolar entities with sub-nanometer scale and additional polarity sources. This is achieved based on the induction of donor/acceptor-free intrinsic cation vacancy-oxygen vacancy complexes, which regulate the cation-oxygen bonding structures, promote the highly disordered polar displacement distortion of Ti atoms in the oxygen cage, and significantly enhance the local electric field. In addition, this method avoids generating additional impurity energy levels and increases the band gap. The polarization and insulation of the optimized system exhibits a significant enhancement compared to the defect-free system, resulting in a recoverable energy density of 10.74 J/cm3, while maintaining a high efficiency of 94.1% and excellent high-temperature stability. Contrary to conventional paradigms that associate defects with deteriorated polarization response and thermal degradation, our findings establish a novel defect-utilization methodology, paving the way for advancing energy storage capabilities in broader weakly polar dielectrics.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"11 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241230","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

Bilayer Artificial Interface Engineering Enables Dendrite-Free and Low-Temperature Stable Lithium Metal Batteries 双层人工界面工程实现无枝晶低温稳定锂金属电池

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-08 DOI: 10.1016/j.ensm.2025.104664

Yahui Li, Kai Yang, Zengjie Fan, Chong Xu, Zhemin Li, Hui Dou, Xiaogang Zhang

{"title":"Bilayer Artificial Interface Engineering Enables Dendrite-Free and Low-Temperature Stable Lithium Metal Batteries","authors":"Yahui Li, Kai Yang, Zengjie Fan, Chong Xu, Zhemin Li, Hui Dou, Xiaogang Zhang","doi":"10.1016/j.ensm.2025.104664","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104664","url":null,"abstract":"Rational design of lithium (Li) metal anodes is critical for achieving uniform Li deposition and long-term cycling stability. Here, we report a sequential atomic layer deposition of lithiophilic ZnO and Li2O coatings on 3D carbon paper to construct a vertically graded bilayer artificial interface. The underlying ZnO-derived LiZn/Li2O domains act as mixed ionic/electronic conductors and provide stable nucleation sites for Li deposition. The high-resistance Li2O top layer suppresses electron tunneling and increases the nucleation size. This synergistic design directs bottom-up Li growth, fully exploiting the internal voids of the 3D scaffold, suppressing dendrite formation. As a result, the Li@CP/Z6L1||LCO cell achieves 83.1% capacity retention after 200 cycles at −20 °C (∼4000 h), while the Li@CP/Z6L1||LFP cell maintains 96.4% capacity after 500 cycles, with only 0.0072% capacity loss per cycle. This work demonstrates a rational bilayer interface design that leverages vertical conductivity gradients and interfacial chemistry to achieve high-performance, durable, and low-temperature-tolerant lithium metal anodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247655","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

Elimination of volatile components in cellulose enabling ultrahigh initial Coulombic efficiency in sodium-ion batteries 消除纤维素中的挥发性成分，使钠离子电池具有超高的初始库仑效率

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-08 DOI: 10.1016/j.ensm.2025.104667

Yanzhao Huang, Jiahua Zhao, Pandeng Zhao, Qinghang Chen, Chuangchuang Li, Lingling Zhang, Lin Li, Shu-Lei Chou, Xingqiao Wu

{"title":"Elimination of volatile components in cellulose enabling ultrahigh initial Coulombic efficiency in sodium-ion batteries","authors":"Yanzhao Huang, Jiahua Zhao, Pandeng Zhao, Qinghang Chen, Chuangchuang Li, Lingling Zhang, Lin Li, Shu-Lei Chou, Xingqiao Wu","doi":"10.1016/j.ensm.2025.104667","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104667","url":null,"abstract":"Hard carbon has emerged as a promising anode material for sodium-ion batteries (SIBs) due to its low working potential and cost-effectiveness. However, its commercialization is hindered by suboptimal initial Coulombic efficiency (ICE) and practical reversible capacity. To address these limitations, we propose a vacuum-modulated pre-carbonization strategy to optimize the adsorption-intercalation sodium storage behavior for hard carbon with ultrahigh ICE. This strategy effectively utilizes volatile components during the pyrolysis process, constructs hierarchical open-pore networks with interconnected channels on the surfaces of the carbon matrix, and then produces hard carbon materials with closed-pore and a moderate degree of graphitization through high-temperature carbonization. Furthermore, the surface oxygen-containing functional groups are also optimized in this process. As a result, the optimized hard carbon anode (CS-2C-0.06P) achieves enhanced ICE in the slope (2.0-0.1 V) and capacity in the plateau (0.1-0.0 V) regions, with the plateau capacity exhibiting nearly fully reversible characteristics. The resulting anode achieves an ICE exceeding 95% with a high reversible capacity of 331.54 mAh g-1, surpassing those of most previously reported biomass‐derived hard carbons. This work establishes a novel paradigm for designing advanced carbonaceous materials through synergistic optimization of adsorption-intercalation-filling storage behavior, providing critical insights for developing high-energy-density SIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"204 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145247657","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

Layered P2/P3-intergrowth cathode materials with biphasic interlocking towards stable potassium (de)intercalation 具有两相互锁的层状P2/ p3互生长阴极材料，可实现稳定的钾（de）嵌入

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-05 DOI: 10.1016/j.ensm.2025.104659

Yongwei Tang, Xu Zhu, Chen Cheng, Lingfei Zhao, Qinfen Gu, Haojie Dong, Mengting Liu, Wenjie Tang, Guang-Xu Wei, Yi-Hu Feng, Liang Zhang, Bing Xiao, Peng-Fei Wang

{"title":"Layered P2/P3-intergrowth cathode materials with biphasic interlocking towards stable potassium (de)intercalation","authors":"Yongwei Tang, Xu Zhu, Chen Cheng, Lingfei Zhao, Qinfen Gu, Haojie Dong, Mengting Liu, Wenjie Tang, Guang-Xu Wei, Yi-Hu Feng, Liang Zhang, Bing Xiao, Peng-Fei Wang","doi":"10.1016/j.ensm.2025.104659","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104659","url":null,"abstract":"Potassium layered oxide cathodes usually deliver diverse prismatic-coordinated structural chemistry, enabling to explore thermodynamic-stable P2/P3 biphasic structures to tailor the electrochemical properties for potassium-ion batteries (PIBs). However, their intrinsic thermodynamic phase preference and complex electrochemical reaction mechanism in terms of phase evolution, charge compensation and stress response remain unclear. With this perspective, a P2/P3 biphasic cathode material-KxLi0.03Mg0.03Ti0.07Ni0.1Mn0.77O2 with a specific phase proportion (P2: P3 = 35.2%: 64.8%) is designed under the guidance of first principles calculation. Benefiting from the interfacial interlocking effect at the phase boundary, the sliding of TM layers is well inhibited. Moreover, the different orientation of P2 and P3 crystalline domain serves to mitigate long range Jahn-Teller ordering of MnO6 octahedron, lattice mismatch and mechanical stress. Consequently, the P2/P3 biphasic cathode exhibits a high capacity of 110.8 mA h g−1 at 0.2 C and good cycling stability of 82.0% after 150 cycles at 1 C. This work provides insightful guidelines to develop stable biphasic cathode materials through thermodynamic phase modulation for high-performance PIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"17 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145229294","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

Operando characterisation of Na-Zn molten salt batteries using X-ray radiography: insights into performance degradation and cell failure 使用x射线摄影技术对Na-Zn熔盐电池的操作特性进行表征：对性能下降和电池失效的见解

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104654

Martins Sarma, Natalia Shevchenko, Norbert Weber, Tom Weier

{"title":"Operando characterisation of Na-Zn molten salt batteries using X-ray radiography: insights into performance degradation and cell failure","authors":"Martins Sarma, Natalia Shevchenko, Norbert Weber, Tom Weier","doi":"10.1016/j.ensm.2025.104654","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104654","url":null,"abstract":"The sodium-zinc system for grid-scale energy storage is a compelling solution due to its high cell voltage (1.8 V) and Earth abundance, resulting in minimal active material costs. Since the proposal of the cell concept, the research has been based on the assumption that separating the electrolyte into anolyte and catholyte using a porous medium to limit the molten salt mixing is essential for cell operation. This is deemed crucial in order to confine the produced ZnCl2 to the vicinity of the Zn pool and to reduce the probability of a direct contact between ZnCl2 and Na, which would result in self-discharge. However, the constructed cells have not demonstrated consistent performance over extended periods of more than a few weeks. Through in situ operation of the cells at an X-ray beamline, the underlying causes of battery failure have been identified, facilitating a conceptual overhaul of the cell design. It is demonstrated that the separator is not only unnecessary, but is the reason for cell failure. Its elimination enables a significant simplification of the design, while simultaneously ensuring stable cycling.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"28 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216258","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

Interface-driven phase stability enables co-sintered composite anodes for intrinsically safe all-solid-state-batteries 界面驱动的相稳定性使共烧结复合阳极具有本质安全的全固态电池

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104653

Pengpeng Dai, Shuyu Zhou, Junhong Liao, Yuxin Liu, Yudong Liu, Haoran Li, Zheng Yue, Guozhong Cao, Shixi Zhao

{"title":"Interface-driven phase stability enables co-sintered composite anodes for intrinsically safe all-solid-state-batteries","authors":"Pengpeng Dai, Shuyu Zhou, Junhong Liao, Yuxin Liu, Yudong Liu, Haoran Li, Zheng Yue, Guozhong Cao, Shixi Zhao","doi":"10.1016/j.ensm.2025.104653","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104653","url":null,"abstract":"The development of all-solid-state batteries (ASSBs) is hindered by interfacial instability between solid-electrolytes (SEs) and Li metal anodes. In this work, we propose a co-sintered composite anode strategy based on Li4Ti5O12 (LTO), a ‘zero-strain’ anode material, to address interfacial challenges in NASICON-type systems. Systematic investigations reveal that LTO undergoes progressive phase decomposition during co-sintering with Li1.3Al0.3Ti1.7(PO4)3 (LATP) due to the thermodynamic driving force from Li chemical potential difference and the high reactivity of phosphate groups. In contrast, LTO maintains structural integrity and chemical compatibility up to 900 °C when co-sintered with Li0.33La0.56TiO3 (LLTO). Additionally, thermodynamic instability between LATP and LLTO at high-temperatures is observed, indicating challenges in multi-electrolyte integration. Notably, the preferential Li loss from LLTO within the LTO+LLTO composite anode during co-sintering with LATP pellet exerts a protective effect for LTO, helping to maintain the structural integrity of LTO. Building upon these findings, an integrated (LTO+LLTO)|LATP bilayer structure is successfully fabricated via co-sintering at 600°C. This work offers critical insights into phase evolution and interfacial chemistry for coupling SEs with anode materials, guiding the rational design of co-sintering composite anodes and demonstrating a promising pathway toward intrinsically safe ASSBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"13 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216260","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

Heteroatoms doped holey graphene enhanced carbon frameworks with chemical pre-lithiation affording reversible lithium plating/stripping in anode-free lithium metal batteries 杂原子掺杂多孔石墨烯增强碳框架与化学预锂化提供可逆的锂电镀/剥离无阳极锂金属电池

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-03 DOI: 10.1016/j.ensm.2025.104648

Mingliang Bai, Min Zhong, Xuchang Tang, Wenzhuo Shen, Jiali Zhang, Shouwu Guo

{"title":"Heteroatoms doped holey graphene enhanced carbon frameworks with chemical pre-lithiation affording reversible lithium plating/stripping in anode-free lithium metal batteries","authors":"Mingliang Bai, Min Zhong, Xuchang Tang, Wenzhuo Shen, Jiali Zhang, Shouwu Guo","doi":"10.1016/j.ensm.2025.104648","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104648","url":null,"abstract":"The host electrode plays a pivotal role in facilitating the lithium plating and stripping in anode-free lithium metal batteries (AF-LMBs). In the work, we design and fabricate a series of hierarchical carbon frameworks composed of cellulose-derived carbon fibers, holey graphene doped with heteroatoms (B, N, F), and lithium salts, to address the challenges of low coulombic efficiency, poor lithium plating and stripping, and rapid capacity fading of AF-LMBs. The holey graphene provides abundant lithium nucleation sites, leading to uniform plating/stripping, and lower Fermi level of the host electrode, thereby helping to suppress side reactions. The pre-lithiation improves the initial coulombic efficiency to >100 % by offsetting irreversible first-cycle consumption. In parallel, heteroatom doping tends to promote a beneficial, inorganically enriched SEI, thereby reinforcing interfacial stability during lithium plating/stripping. The AF-LMBs assembled with the as-prepared hierarchical carbon frameworks as host electrodes, and NCM811 as cathodes deliver exceptional cycling stability, retaining ∼72 % and ∼67 % of capacity after 100 cycles at 1.93//1.93 mA cm⁻² and 1.93//3.86 mA cm⁻² with carbonate-based electrolyte.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"327 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216265","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

Green and Economically Viable Dry-Electrode Manufacturing for High-Energy-Density Lithium Batteries 绿色和经济可行的高能量密度锂电池干电极制造

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-03 DOI: 10.1016/j.ensm.2025.104649

Kun Cao, Jingqin Ji, Yanlan Zhao, Kaiyan Wang, Lixi Zeng, Li Wang, Xiangming He

{"title":"Green and Economically Viable Dry-Electrode Manufacturing for High-Energy-Density Lithium Batteries","authors":"Kun Cao, Jingqin Ji, Yanlan Zhao, Kaiyan Wang, Lixi Zeng, Li Wang, Xiangming He","doi":"10.1016/j.ensm.2025.104649","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104649","url":null,"abstract":"The global transition to electrification is driving the demand for lithium-ion batteries (LIBs) with higher energy density, lower cost, and reduced environmental footprint. Conventional slurry-based electrode manufacturing, which relies on toxic solvents and energy-intensive drying processes, poses significant economic and environmental challenges. Solvent-free dry electrode technology has emerged as a transformative alternative to overcome these limitations. This review provides a comprehensive and critical analysis of the dry process from three pivotal perspectives: economic advantages, environmental benefits, and performance superiority, conducting a multidimensional comparative analysis with slurry-process electrode manufacturing. The scientific principles behind these advantages are elucidated through microstructural and electrochemical characterization. Meanwhile, comparative life cycle assessment (LCA) data are employed to demonstrate the significant advantages of dry electrodes in terms of energy consumption and carbon emissions. Regarding application potential, leveraging Tesla's successful industrial application case, we explore the broad prospects of dry electrodes in LIBs, solid-state batteries, and other domains. Finally, in the context of the rapidly advancing dry electrode technology, we highlight the severe challenges that remain before truly achieving industrial-scale application. This work offers a holistic theoretical foundation and practical guidance for adopting dry electrode technology as a core strategy for sustainable battery manufacturing.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"37 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216123","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

Tailored Modulation of Jahn-Teller Distortion via Electron-Lattice Coupling to Enhance the Cycling Stability of Polyanionic Cathodes for Advance Sodium-Ion Batteries 通过电子-晶格耦合调制jhn - teller畸变以提高先进钠离子电池的聚阴离子阴极的循环稳定性

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-02 DOI: 10.1016/j.ensm.2025.104645

Jiajia An, Hanlin Wang, Lingfei Zhao, Qiang Wang, Binkai Yu, Ye Li, Wenxi Zhao, Jinqiao Hu, Jiarun Geng, Limin Zhou, He Zhu, Hui Xia, Qinfen Gu, Ruohan Yu, Mei Yang, Guoxiu Wang, Mingzhe Chen

{"title":"Tailored Modulation of Jahn-Teller Distortion via Electron-Lattice Coupling to Enhance the Cycling Stability of Polyanionic Cathodes for Advance Sodium-Ion Batteries","authors":"Jiajia An, Hanlin Wang, Lingfei Zhao, Qiang Wang, Binkai Yu, Ye Li, Wenxi Zhao, Jinqiao Hu, Jiarun Geng, Limin Zhou, He Zhu, Hui Xia, Qinfen Gu, Ruohan Yu, Mei Yang, Guoxiu Wang, Mingzhe Chen","doi":"10.1016/j.ensm.2025.104645","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104645","url":null,"abstract":"Manganese-based polyanionic compounds are one of the most promising cathode materials for sodium-ion batteries due to cost-effectiveness, high-voltage capability, and environmental friendliness. Nevertheless, the strong Jahn-Teller distortion (JTD) in high-spin Mn3+ state induces localized stress concentration and irreversible structural collapse, while the low-JTD state causes elevated lattice rigidity via enhanced Mn–O bond covalency, leading to inferior electrochemical stability. Herein, we propose an electron-lattice coupling modulation strategy by constructing a Ti4+-mediated Mn-O-Ti superexchange interactions within the polyanionic NaMnPO4 framework to enable electronic state reconfiguration and dynamic lattice response for controllable JTD regulation. We show that the strong orbital hybridization between Ti4+ d0 and O 2p enhances the covalency of Mn–O bonds and broadens the Mn3+ eg orbitals into Mn(eg)-O(2p) hybridized bands, thus reducing the intrinsic electron degeneracy of the Mn3+ eg orbitals. Furthermore, the flexible TiO6 octahedra facilitate homogeneous reversible microstrains through elastic deformation and enable effective lattice stress dissipation. The NaMn0.80Ti0.20PO4 exhibits an optimal JTD magnitude of σ2 = 0.009 and a 91.03% improvement in strain homogeneity compared to the pristine sample. These enhancements contribute to a high-capacity retention of 96.75% after 500 cycles at 2 C. (vs. 77.85% for NaMnPO4). This work establishes a universal paradigm to modulate the JTD in high-spin transition-metal cathodes, opening new avenues for high-stability cathode design.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"98 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209388","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