Energy Storage Materials最新文献_第6页

Biphasic synergistic functional electrolyte enhances high-temperature performance of 4.85 V LiNi0.5Mn1.5O4||graphite pouch cells 双相协同功能电解质提高4.85V LiNi0.5Mn1.5O4||石墨袋电池的高温性能

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-31 DOI: 10.1016/j.ensm.2026.104950

Jinlong Sun, Shinuo Kang, Xiang Wu, Xiaobing Lou, Ming Shen, Bingwen Hu

Spinel-type LiNi_0.5Mn_1.5O₄ (LNMO) cathodes exhibit vulnerability to electrolyte decomposition, gas evolution, and instability at the electrode interface under conditions of high voltage and elevated temperature, which considerably restricts their practical applicability. In response to these challenges, the present study introduces a design strategy for high-voltage electrolytes, employing a biphasic synergistic functional electrolyte aimed at improving the high-temperature performance of LNMO||graphite pouch cells at 4.85 V. The lower layer of the electrolyte, characterized by a high-concentration saturated phase, facilitates the development of anion-rich solvation shells and solidification-induced cathode-electrolyte interphase (CEI) predominantly influenced by anion decomposition, thus promoting the stable formation of a LiF-rich CEI. Conversely, the upper layer of the electrolyte, which is a locally high-concentration phase diluted by TTE, presents a distinctive solvation shell with a high lowest unoccupied molecular orbital (LUMO) energy level, thereby enhancing the oxidative and reductive stability of the solvent and mitigating side reactions. After 140 cycles at 4.85 V and 45 °C, the cell maintained 92.17 % of its initial capacity, while total gas evolution was reduced by 78.57 % in comparison to conventional electrolyte systems.

尖晶石型LiNi0.5Mn1.5O4 （LNMO）阴极在高压和高温条件下易发生电解质分解、气体析出和电极界面不稳定，这极大地限制了其实际应用。为了应对这些挑战，本研究引入了一种高压电解质设计策略，采用双相协同功能电解质，旨在提高4.85 V下LNMO||石墨袋电池的高温性能。电解质下层以高浓度饱和相为特征，有利于富阴离子溶剂化壳的形成和主要受阴离子分解影响的固化诱导阴极-电解质间相（CEI）的形成，从而促进富lif CEI的稳定形成。相反，电解质的上层是被TTE稀释的局部高浓度相，呈现出独特的溶剂化壳层，具有较高的最低未占据分子轨道（LUMO）能级，从而增强了溶剂的氧化和还原稳定性，减轻了副反应。在4.85 V和45°C下循环140次后，电池保持了92.17%的初始容量，而与传统电解质系统相比，总气体释放量减少了78.57%。

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引用次数: 0

Electron-delocalized π-network enables low-reactive polyacrylonitrile-based solid-state electrolytes for lithium metal batteries 电子离域π网络制备低反应性聚丙烯腈基锂金属电池固态电解质

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-01 DOI: 10.1016/j.ensm.2026.104953

Jiayi Yang , Yangqian Zhang , Han Liu , Yaqi Liao , Chihon Leung , Rongfeng Chen , Ying Wei , Le Hu , Mengyuan Zhou , Gang Sun , Ziping Wu , Henghui Xu , Zhenbo Wang , Shaoming Huang , Yang Ren

As one of the most promising solid-state polymer electrolytes (SPEs), Polyacrylonitrile (PAN)-based SPEs suffer from unstable interfaces due to their highly reactivity with lithium metal anode. Here, the molecular chain of the PAN polymer is tailored through surface-basicity-guided reactions of Li₇La₃Zr_1.4Ta_0.6O₁₂ (LLZTO) and an electrostatic shielding effect of 1-Ethyl-3-methylimidazolium cation (EMIM⁺), effectively mitigating its reactivity with Li. The alkalinity of LLZTO catalyze PAN dehydrocyanation, transforming –CN groups to π-conjugated –C=N/–C=C– bonds, thus decreasing its inherent reactivity with the Li metal. Then, the positive EMIM⁺ with an electron-delocalized π-network electrostatically connect with polarized –C=N sites, shielding the direct contact of –CN groups with Li, further alleviating parasitic reactions. As a result, the Li//Li symmetric cells deliver high critical current density of 3.0 mA cm⁻² and maintain stable Li plating/stripping over 2000 h. The Li//LFP cell delivers a high capacity retention of 87.53 % after 1200 cycles at 2C, and the pouch battery presents excellent cycling and safety performance. This work provides a promising approach to enable the stable operation of solid-state lithium metal batteries via incorporating the electron-delocalized π-network.

聚丙烯腈（PAN）基固态聚合物电解质是最有前途的固态聚合物电解质之一，但由于其与锂金属阳极的高反应性，导致其界面不稳定。在这里，PAN聚合物的分子链是通过Li7La3Zr1.4Ta0.6O12 （LLZTO）的表面碱度引导反应和1-乙基-3-甲基咪唑阳离子（EMIM +）的静电屏蔽效应来定制的，有效地减轻了它与Li的反应性。LLZTO的碱度催化PAN脱氢氰化，将- cn基团转化为π共轭的- C=N/ - C=C -键，从而降低了其与Li金属的固有反应活性。然后，带电子离域π网络的EMIM +与极化的c =N位静电连接，屏蔽了-CN基团与Li的直接接触，进一步缓解了寄生反应。结果表明，Li//Li对称电池可提供3.0 mA cm−2的临界电流密度，并在2000 h内保持稳定的镀/剥离锂。Li//LFP电池在2C下1200次循环后的容量保持率高达87.53%，袋状电池具有良好的循环和安全性能。本研究为引入电子离域π网络实现固态锂金属电池的稳定运行提供了一种有前景的方法。

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引用次数: 0

Roadmaps for dendrite suppression in next generation lithium-ion batteries: Toward sustainable energy solutions 下一代锂离子电池枝晶抑制路线图：迈向可持续能源解决方案

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-23 DOI: 10.1016/j.ensm.2026.105000

Yi Li , Sachin Poudel , Sweta Kumari , Erfan Azqadan , Anil Kunwar , Nele Moelans

Dendrite formation remains one of the most pressing challenges in advancing the performance and safety of rechargeable lithium-ion batteries (LiBs). These needle-like structures not only compromise battery capacity but also pose significant safety risks, such as short circuits and thermal runaway. This review explores recent advancements in battery design aimed at overcoming these issues. Key strategies include electrolyte engineering, which focuses on developing stable solid electrolyte interfaces (SEIs) to suppress dendrite growth by optimizing coordination forces and stabilizing nucleation sites. Advanced computational techniques, such as multiscale computational design and battery informatics, provide predictive insights into dendrite suppression. The density functional theory (DFT) studies reveal dendrite formation energies typically ranging from 1.2345–6.7890 eV. Furthermore, optical nucleation site mapping has emerged as a powerful tool for visualizing lithium deposition dynamics, offering new perspectives on dendrite prevention. By addressing challenges in stability criteria and maximizing specific energy densities beyond 300 Wh/kg, this review emphasizes the integration of experimental, computational, and informatics-driven approaches to enable the design of safer, dendrite-free LiBs.

枝晶的形成仍然是提高可充电锂离子电池（LiBs）性能和安全性的最紧迫挑战之一。这些针状结构不仅会损害电池容量，还会带来重大的安全风险，如短路和热失控。这篇综述探讨了旨在克服这些问题的电池设计的最新进展。关键策略包括电解质工程，其重点是开发稳定的固体电解质界面（SEIs），通过优化配位力和稳定成核位点来抑制枝晶的生长。先进的计算技术，如多尺度计算设计和电池信息学，为树突抑制提供了预测性见解。密度泛函理论（DFT）研究表明，枝晶形成能通常在1.2345-6.7890 eV之间。此外，光学成核位置测绘已经成为可视化锂沉积动力学的有力工具，为枝晶预防提供了新的视角。通过解决稳定性标准方面的挑战，并最大限度地提高比能量密度超过300 Wh/kg，本综述强调了实验、计算和信息学驱动方法的集成，以实现更安全、无枝晶的lib的设计。

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引用次数: 0

Toward breakthroughs in wide-temperature aqueous sodium-ion batteries: Challenges, advances and prospects 宽温水钠离子电池的突破：挑战、进展与展望

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-28 DOI: 10.1016/j.ensm.2026.105014

Yaqi Hou , Fanchen Gu , Dongmei Dai , Bao Li , Shuming Zheng , Bao Wang , Shiming Yang , Jian Qi

In the face of an escalating global energy crisis, the demand for sustainable and cost-effective energy storage solutions has significantly propelled sodium-ion batteries (SIBs) to the forefront of research, particularly due to the abundance and affordability of sodium. Among various SIB technologies, aqueous sodium-ion batteries (ASIBs) have garnered considerable attention for their superior safety, eco-friendliness, and potential for wide-temperature-range applications. However, the reliability under extreme conditions is limited by electrolyte instability and interfacial degradation. This review provides a comprehensive synthesis of the latest advancements in ASIBs over the past five years, focusing on breakthrough achievements in enhancing wide-temperature performance for key components, including electrolytes, electrodes, separators, binders, and current collectors. It also explores persistent challenges encountered during operation in extreme environments. A key innovation presented in this review is the integration of machine learning (ML) techniques into SIB research. This approach offers new perspectives and potential references for future ML-driven advancements, enabling accelerated material discovery and performance optimization. Furthermore, the review summarizes the current status and future trajectories of hydroxide-based sodium-ion batteries, providing researchers with valuable insights and directions for further exploration in this dynamic field. Overall, this review underscores the transformative potential of ASIBs in large-scale energy storage, while also identifying key areas for future research and development.

面对不断升级的全球能源危机，对可持续和具有成本效益的能源存储解决方案的需求极大地推动了钠离子电池（sib）的研究前沿，特别是由于钠的丰富和可负担性。在各种SIB技术中，水钠离子电池（asib）因其优越的安全性、环保性和宽温度范围的应用潜力而受到广泛关注。然而，在极端条件下的可靠性受到电解质不稳定性和界面降解的限制。本文综述了近五年来asib的最新进展，重点介绍了在提高关键部件（包括电解质、电极、分离器、粘结剂和集流器）的宽温性能方面取得的突破性进展。它还探讨了在极端环境下作业时遇到的持续挑战。本综述中提出的一个关键创新是将机器学习（ML）技术集成到SIB研究中。这种方法为未来机器学习驱动的进步提供了新的视角和潜在的参考，加速了材料的发现和性能优化。综述了氢氧化物钠离子电池的研究现状和发展趋势，为研究人员在这一动态领域的进一步探索提供了有价值的见解和方向。总的来说，这篇综述强调了asib在大规模储能方面的变革潜力，同时也确定了未来研究和开发的关键领域。

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引用次数: 0

Unveiling degradation mechanisms of sulfide-based composite cathodes supported by digital-twin modeling: Dry binder versus wet binder 揭示由数字孪生模型支持的硫化物基复合阴极的降解机制：干粘合剂与湿粘合剂

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-27 DOI: 10.1016/j.ensm.2026.104930

Seung-Bo Hong , Hyobin Lee , Young-Jun Lee , Choyeon Kim , Yong Min Lee , Un-Hyuck Kim , Dong-Won Kim

Sulfide-based all-solid-state lithium batteries (ASSLBs) have garnered considerable attention owing to their high energy density and enhanced safety. In such systems, composite cathodes are commonly fabricated via either a solvent-free dry process or a slurry-based wet process, typically employing polytetrafluoroethylene (PTFE) and acrylonitrile–butadiene rubber (NBR) as binders, respectively. However, a comprehensive understanding of how these binders influence electrochemical performance and degradation mechanisms remains limited. In this study, the effects of PTFE and NBR binders on interfacial degradation are systematically elucidated through electrochemical analyses, morphological characterizations, and digital-twin computational modeling. The results reveal that PTFE effectively mitigates interfacial deterioration by maintaining intimate contact and minimizing void formation, whereas NBR suffers from accelerated interfacial degradation and void growth during prolonged cycling. These findings highlight the critical role of binder-induced interfacial phenomena in determining cell performance and offer valuable insights for optimizing cathode fabrication strategies tailored to each processing route, while guiding the rational design of advanced binders for composite cathodes in ASSLBs.

硫化物基全固态锂电池（ASSLBs）因其高能量密度和增强的安全性而受到广泛关注。在这种系统中，复合阴极通常通过无溶剂干法或基于浆料的湿法制造，通常分别采用聚四氟乙烯（PTFE）和丙烯腈-丁二烯橡胶（NBR）作为粘合剂。然而，对这些粘合剂如何影响电化学性能和降解机制的全面理解仍然有限。在这项研究中，通过电化学分析、形态表征和数字孪生计算模型系统地阐明了聚四氟乙烯和丁腈橡胶粘合剂对界面降解的影响。结果表明，PTFE通过保持紧密接触和减少空隙形成，有效地缓解了界面退化，而NBR在长时间循环过程中界面降解和空隙生长加速。这些发现强调了粘合剂诱导的界面现象在决定电池性能方面的关键作用，并为优化阴极制造策略提供了有价值的见解，同时指导了ASSLBs复合阴极先进粘合剂的合理设计。

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引用次数: 0

Vacancy-induced Li+ Conduction of Li3–xAl1–xTixF6 fluoride solid electrolyte for 5 V all-solid-state batteries 5v全固态电池中Li3-xAl1-xTixF6氟化固体电解质的空位诱导Li+导电

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-28 DOI: 10.1016/j.ensm.2026.104938

Changhoon Kim , Jae-Seung Kim , Juhyoun Park , Jun Pyo Son , Jaehan Park , Seokjae Hong , Youngsu Lee , Kyu-Young Park , Hyungsub Kim , Dong-Hwa Seo , Yoon Seok Jung

Despite their exceptional oxidative stability, fluoride-based solid electrolytes suffer from low ionic conductivities, impeding the further development of high-voltage all-solid-state batteries (ASSBs). Here, we report a monoclinic Li₃_–_xAl₁_–_xTi_xF₆, achieving a Li⁺ conductivity reaching 1.5 × 10^–5 S cm^–1 at 30 °C for x = 0.5, which is 1000-fold higher than Li₃AlF₆. X-ray and neutron powder diffraction analyses reveal that Ti⁴⁺ substitution induces anisotropic lattice expansion and increased monoclinic distortion. Bond valence energy landscape calculations, radial distribution function analysis, and ab-initio molecular dynamics simulations show that Ti⁴⁺ substitution diversifies Li⁺ migration pathways, expands transport channels, and flattens the potential energy landscape. The optimized composition offers outstanding stability up to 5.0 V (vs. Li/Li⁺) and retains 81.4% capacity over 600 cycles with 5 V-class LiNi_0.5Mn_1.5O₄ cathodes cycled between 3.0–5.0 V. These results highlight that compositional tuning and lattice engineering unlock the potential of fluoride-based electrolytes for high-voltage ASSBs.

尽管氟基固体电解质具有优异的氧化稳定性，但其离子电导率较低，阻碍了高压全固态电池（assb）的进一步发展。在这里，我们报道了单斜Li3-xAl1-xTixF6，在30°C下，x = 0.5时，Li+电导率达到1.5 × 10-5 S cm-1，比Li3AlF6高1000倍。x射线和中子粉末衍射分析表明，Ti4+取代引起各向异性晶格膨胀和单斜畸变增加。键价能格局计算、径向分布函数分析和ab-initio分子动力学模拟表明，Ti4+取代使Li+迁移途径多样化，扩展了运输通道，并使势能格局平坦化。优化后的组合物在5.0 V （vs. Li/Li+）下具有出色的稳定性，并且在5个V级LiNi0.5Mn1.5O4阴极在3.0-5.0 V之间循环时，在600次循环中保持81.4%的容量。这些结果表明，成分调整和晶格工程释放了氟基电解质用于高压assb的潜力。

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引用次数: 0

Hydrogen bond network induced interfacial dipoles enhance built-in electric fields and ion transport in vanadium oxide heterostructures 氢键网络诱导界面偶极子增强氧化钒异质结构内建电场和离子输运

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-05 DOI: 10.1016/j.ensm.2026.104969

Shuai Zhang , Zixuan Gao , Dongdong Zhang , Kittima Lolupiman , Wanwisa Limphirat , Xiang Wu , Jiaqian Qin , Jin Cao

Vanadium-based oxides are among the most promising cathodes for aqueous zinc-ion batteries (AZIBs), yet their practical deployment is hindered by severe vanadium dissolution and inefficient interfacial charge/ion transport. Herein, l-tartaric acid (L-TA) is made to self-assemble on a preconstructed V₂O₅/V₃O₇·H₂O (V₂V₃) heterointerface, forming a hydrogen bond interfacial layer (HB-V₂V₃). The hydrogen-bond network reinforces interfacial cohesion and induces oriented dipoles, which cooperate with the heterojunction’s built-in electric field to enhance electronic coupling and accelerate Zn²⁺ transport. Meanwhile, the strengthened V-O interactions and regulated interfacial hydration environment effectively suppress vanadium dissolution and preserve lattice integrity. Functioning as a noninvasive and compliant molecular “sheath”, it regulates the local chemical environment while preserving the host lattice. As a result, HB-V₂V₃ delivers a reversible capacity of 464.53 mAh g^-1 at 0.1 A g^-1 within 0.2–1.6 V and exhibits outstanding durability, retaining 95.5% after 500 cycles at 2.0 A g^-1 and 93.1% after 2200 cycles at 5.0 A g^-1. It also maintains approximately 81% of its capacity after 300 cycles at 1 A g^-1 in a pouch-cell configuration. These results establish hydrogen-bond-driven interfacial modulation as an effective and broadly applicable route to stabilize vanadium cathodes and enhance the performance of AZIBs.

钒基氧化物是水溶液锌离子电池（AZIBs）最有前途的阴极之一，但其实际部署受到严重的钒溶解和低效的界面电荷/离子传输的阻碍。本文利用l -酒石酸（L-TA）在预先构建的V2O5/V3O7·H2O （V2V3）异质界面上自组装，形成氢键界面层（HB-V2V3）。氢键网络增强了界面内聚力并诱导了取向偶极子，偶极子与异质结的内置电场协同作用，增强了电子耦合，加速了Zn2+的输运。同时，V-O相互作用的增强和界面水化环境的调节有效地抑制了钒的溶解，保持了晶格的完整性。它作为一种非侵入性和柔顺的分子“鞘”，在保持宿主晶格的同时调节局部化学环境。因此，HB-V2V3在0.2-1.6 V范围内，在0.1 a g-1下提供464.53 mAh g-1的可逆容量，并具有出色的耐用性，在2.0 a g-1下循环500次后保持95.5%，在5.0 a g-1下循环2200次后保持93.1%。在袋式电池配置中，在1 A g-1的电压下循环300次后，它还能保持约81%的容量。这些结果表明，氢键驱动的界面调制是稳定钒阴极和提高AZIBs性能的有效且广泛适用的途径。

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引用次数: 0

A barium lanthanum oxynitride hydride for fast H− conduction 一种用于快速H -传导的氮化氧化镧钡

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-30 DOI: 10.1016/j.ensm.2026.104941

Shukun Liu , Hong Wen , Weijin Zhang , Jungu Xu , Jirong Cui , Shangshang Wang , Ren Zou , Hetong Chen , Weiwei Wang , Tao Gan , Peng Jiang , Xiaohua Ju , Hujun Cao , Ping Chen

Hydride ion (H⁻) is expected to promote innovation in hydrogen energy storage and conversion because of its unique characteristics of low mass and high redox potential. However, fast ion conduction, critical for advancing electrochemical technologies, remains a challenge for H⁻ conductors. Mixed-anion hydrides exhibit tunability in both structure and functionality, positioning them as promising systems for H⁻ conduction. However, their development is hindered by harsh synthesis conditions. Herein, we develop an approach that incorporates oxygen treatment under mild conditions of 0.4 MPa and 450 °C, thereby enabling the efficient synthesis of a novel mixed-anion oxynitride hydride (Ba₃La₂O_4.4N_0.81H_0.77) from its precursory nitride hydride. Experimental and simulative results indicate that Ba₃La₂O_4.4N_0.81H_0.77 crystallizes in the Pnma space group and that H⁻ migration is vacancy-mediated. Consequently, Ba₃La₂O_4.4N_0.81H_0.77 achieves an H⁻ conductivity more than two orders of magnitude higher than its precursor, with an optimum conductivity of 2.52 × 10⁻² S cm^–1 at 420 °C. Using Ba₃La₂O_4.4N_0.81H_0.77 as electrolyte, a primary hydride ion battery operating in a mid-temperature range is demonstrated. This finding underscores the promise of these materials in H⁻-based energy storage applications such as hydride ion batteries and electrochemical cells.

氢化物离子（H−）具有低质量和高氧化还原电位的特点，有望推动氢储能和转化技术的创新。然而，对于推进电化学技术至关重要的快速离子传导仍然是氢导体面临的挑战。混合阴离子氢化物在结构和功能上都表现出可调性，使它们成为有前途的H -传导系统。然而，它们的发展受到苛刻的合成条件的阻碍。在此，我们开发了一种在0.4 MPa和450°C的温和条件下进行氧处理的方法，从而可以从其前体氮化物中高效合成新型混合阴离子氮化氧氢化物（Ba3La2O4.4N0.81H0.77）。实验和模拟结果表明，Ba3La2O4.4N0.81H0.77在Pnma空间群中结晶，H−迁移是由空位介导的。因此，Ba3La2O4.4N0.81H0.77的H -电导率比前驱体高出两个数量级以上，在420℃时的最佳电导率为2.52 × 10−2 S cm-1。以Ba3La2O4.4N0.81H0.77为电解液，制备了在中温范围内工作的一次氢化物离子电池。这一发现强调了这些材料在氢基储能应用中的前景，如氢化物离子电池和电化学电池。

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引用次数: 0

Entropy-stabilized engineering enables stable high-voltage phosphate cathode materials for sodium-ion batteries 熵稳定工程为钠离子电池提供稳定的高压磷酸盐正极材料

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-04 DOI: 10.1016/j.ensm.2026.104964

Xiaohao Liu , Xiaoyue Zhang , Longhai Zhang , Xin Tan , Li Li , Weibo Hua , Chaofeng Zhang , Shulei Chou

High-voltage phosphate cathodes are a kind of promising electrode materials for constructing high-energy density sodium-ion batteries (SIBs). However, as a typical representative, Na₄Co₃(PO₄)₂P₂O₇ (NCPP), which commonly suffers from inevitably complicated structural evolution and sluggish kinetics resulting in generally unsatisfactory rate and cycling performance, which severely hinders its practical applications as ultra high-voltage cathode materials. Herein, Na₄Co₂Fe(PO₄)₂P₂O₇ (NCFPP) is designed to optimize the Co²⁺/Co³⁺ redox reaction, enabling a highly reversible single-phase transformation mechanism that displays enhanced rate capability and cycling stability. Furthermore, an entropy-regulation strategy is proposed to further strengthen the structural stability by suppressing undesirable topotactic phase transition. As a result, the designed medium-entropy cathode, Na_3.7Co_1.5Fe_0.75(MgAlCuZn)_0.2(PO₄)₂P₂O₇ (ME-NCFPP), delivers remarkably ultra-long cycling stability (80.3% capacity retention after 10,000 cycles at 10 C) and excellent two-year storage performance, far surpassing the NCFPP electrode. Additionally, the ME-NCFPP||hard carbon (HC) full cell displays excellent cycling stability. The underlying sodium-storage mechanism of the ME-NCFPP electrode is systematically unraveled through theoretical calculations combined with advanced characterization techniques, including in situ X-ray diffraction and synchrotron-based X-ray absorption spectroscopy. This work highlights the critical role of entropy engineering in suppressing multi-phase transitions, paving the way for constructing highly stable high-voltage cathodes for SIBs.

高压磷酸盐阴极是一种很有前途的构建高能量密度钠离子电池的电极材料。然而，Na4Co3(PO4)2P2O7 （NCPP）作为其中的典型代表，由于其结构演变不可避免的复杂和动力学缓慢，导致其速率和循环性能普遍不理想，严重阻碍了其作为超高压正极材料的实际应用。本文设计了Na4Co2Fe(PO4)2P2O7 (NCFPP)，优化了Co2+/Co3+氧化还原反应，实现了高可逆的单相转化机制，提高了速率能力和循环稳定性。此外，提出了一种熵调节策略，通过抑制不理想的拓扑相变来进一步增强结构稳定性。结果表明，所设计的中熵阴极Na3.7Co1.5Fe0.75(MgAlCuZn)0.2(PO4)2P2O7 （ME-NCFPP）具有显著的超长循环稳定性（10℃下10,000次循环后容量保持率为80.3%）和优异的两年存储性能，远远超过NCFPP电极。此外，ME-NCFPP||硬碳（HC）全电池表现出优异的循环稳定性。通过理论计算结合先进的表征技术，包括原位x射线衍射和基于同步加速器的x射线吸收光谱，系统地揭示了ME-NCFPP电极的潜在钠储存机制。这项工作强调了熵工程在抑制多相转变方面的关键作用，为构建高稳定的sib高压阴极铺平了道路。

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引用次数: 0

Stablizing the oxygen redox and crystal structure of O3-type layered oxides for sodium-ion batteries under Harsh conditions 恶劣条件下稳定钠离子电池用o3型层状氧化物的氧氧化还原和晶体结构

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-11 DOI: 10.1016/j.ensm.2026.104982

Zhuomin Liu , Yunhai Zhang , Yonghuang Ye , Hongwei Liu , Pengcheng Mao , Haizu Jin , Aiyang Li , Yougen Tang , Haiyan Wang , Dan Sun

O3-NaNi_1/3Fe_1/3Mn_1/3O₂ (NFM) layered oxides have shown promise as cost-effective cathode materials for sodium-ion batteries (SIBs). However, under harsh operational conditions such as high-voltage cycling (>4.2 V), elevated temperature, and humid environments, the practical application of NFM cathode is hindered by significant performance degradation caused by irreversible oxygen oxidation, detrimental phase transitions, and moisture-induced surface degradation. To address these issues, we propose a one-step Gd-doping strategy to address these challenges synergistically. The unique electronic configuration of Gd³⁺ can effectively regulate charge distribution, enhance oxygen redox reversibility and suppress irreversible oxygen release. Simultaneously, its appropriate ionic radius helps to reduce interlayer spacing and mitigate phase transition strain to stabilize the layered structure. The optimized Gd-doped NFM cathode delivers a high capacity of 180.47 mAh/g at 0.1 C (1 C = 150 mA/g), outstanding rate capability (130.10 mAh/g at 5 C), and exceptional cycling stability (87.5% retention after 200 cycles at 5 C). More importantly, it demonstrates remarkable resilience under high-temperature and humid conditions, offering a practical design strategy for high-performance SIBs operable under realistic harsh environments.

O3-NaNi1/3Fe1/3Mn1/3O2 （NFM）层状氧化物作为钠离子电池（sib）的极具成本效益的正极材料具有广阔的前景。然而，在高压循环（>4.2 V）、高温和潮湿环境等恶劣操作条件下，不可逆的氧氧化、有害的相变和水分引起的表面降解会导致性能显著下降，从而阻碍了NFM阴极的实际应用。为了解决这些问题，我们提出了一个一步式的兴奋剂策略来协同解决这些挑战。Gd3+独特的电子构型能有效调节电荷分布，增强氧的氧化还原可逆性，抑制不可逆氧释放。同时，适当的离子半径有助于减小层间距，减轻相变应变，稳定层状结构。优化后的gd掺杂NFM阴极在0.1 C （1 C = 150 mA/g）下提供180.47 mAh/g的高容量，出色的倍率能力（5 C时130.10 mAh/g），以及出色的循环稳定性（5 C下200次循环后保持87.5%）。更重要的是，它在高温和潮湿条件下表现出卓越的弹性，为在现实恶劣环境下可操作的高性能sib提供了实用的设计策略。

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