Energy Storage Materials最新文献_第10页

Advancing all-solid polymer electrolytes for lithium batteries: From molecular design to device integration 推进锂电池的全固态聚合物电解质：从分子设计到设备集成

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2025-12-22 DOI: 10.1016/j.ensm.2025.104831

Muhammad Kashif Majeed , Rashid Iqbal , M. Zeeshan Ashfaq , Muhammad Akram , M. Umar Majeed , Adil Saleem

The growing demand for safe, high-energy-density lithium-ion batteries (LIBs) in electric vehicles and portable electronics has spurred intensive research into solid polymer electrolytes (SPEs) as promising alternatives to conventional liquid electrolytes. Liquid electrolytes, though widely used, suffer from issues such as leakage, flammability, and dendrite growth, which limit the long-term safety and reliability of LIBs. All-solid polymer electrolytes (ASPEs) address these challenges by combining intrinsic safety with excellent mechanical flexibility, scalable processability, and compatibility with lithium metal anodes (LMA). In this review, we systematically summarize the latest advances in ASPEs based on diverse polymer systems, including polyacrylonitrile (PAN), polyvinylidene fluoride (PVDF) and its copolymers, polyethylene oxide (PEO), polymethyl methacrylate (PMMA), polycarbonate (PC), polyethylene glycol (PEG), polyurethane (PU), polysulfone (PSU), polysiloxane-based electrolytes, polyphosphazenes, and poly(ionic liquids) (PILs). We highlight their structural features, electrochemical properties, and modification strategies aimed at enhancing ionic conductivity, lithium-ion (Li⁺) transference number (t_Li+), and interfacial stability. Particular emphasis is placed on hybrid and composite approaches, functional group engineering, and interfacial regulation techniques that balance ionic transport with mechanical and thermal robustness. Finally, we present a forward-looking perspective on future research opportunities, including the integration of self-healing functionalities, scalable synthesis methods, and advanced solid-state battery architectures. This comprehensive review aims to provide a roadmap for the rational design and application of ASPEs in next-generation lithium (Li) batteries.

电动汽车和便携式电子产品对安全、高能量密度锂离子电池（lib）的需求不断增长，促使人们对固体聚合物电解质（spe）进行了深入研究，将其作为传统液体电解质的有前途的替代品。液体电解质虽然被广泛使用，但存在泄漏、易燃性和枝晶生长等问题，这些问题限制了lib的长期安全性和可靠性。全固态聚合物电解质（ASPEs）通过将固有安全性与优异的机械灵活性、可扩展的可加工性以及与锂金属阳极（LMA）的兼容性相结合，解决了这些挑战。本文系统综述了基于聚丙烯腈（PAN）、聚偏氟乙烯（PVDF）及其共聚物、聚氧化物（PEO）、聚甲基丙烯酸甲酯（PMMA）、聚碳酸酯（PC）、聚乙二醇（PEG）、聚氨酯（PU）、聚砜（PSU）、聚硅氧烷基电解质、聚磷腈和聚离子液体（PILs）等不同聚合物体系的ASPEs的最新进展。我们重点介绍了它们的结构特征、电化学性能和旨在提高离子电导率、锂离子（Li+）转移数（tLi+）和界面稳定性的改性策略。特别强调的是混合和复合方法，官能团工程和界面调节技术，平衡离子传输与机械和热稳健性。最后，我们对未来的研究机会提出了前瞻性的观点，包括自我修复功能的集成、可扩展的合成方法和先进的固态电池架构。本文旨在为ASPEs在下一代锂电池中的合理设计和应用提供一个路线图。

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引用次数: 0

Anion substitution driven lattice-engineered tin-based quaternary chalcogenide for long-life and high-energy sodium-ion batteries 阴离子取代驱动的晶格工程锡基四元硫族化物用于长寿命高能钠离子电池

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-16 DOI: 10.1016/j.ensm.2026.104910

Ahmed Abdel-Aziz , Junwei Li , Mujtaba Aminu Muhammad , Puwu Liang , Baffa Haruna , Ahmed Zaki Alhakemy , Mukhammadjon Adilov , Rustam Ashurov , Khatam Ashurov , Da Chen , Xiang Hu , Zhenhai Wen

Tin-based chalcogenides hold great promise as high-energy anodes for sodium-ion batteries (SIBs) due to their rich redox chemistry, yet their performance is hindered by sluggish ion transport and structural degradation. Herein, we present sophisticated multinary SnSSeTe/C core-shell nanostructures, wherein the concurrent incorporation of Se and Te not only establishes robust interfacial C-Se-Te-Sn bonds but also induces precise lattice-level substitution within SnS, thereby unlocking unprecedented structural and electronic tunability, along with structural resilience, significantly facilitating the reverse alloy conversion mechanism. Comprehensive kinetic analyses and in situ characterization reveal that anion substitution generates abundant lattice vacancies, which not only enhance Na-ion adsorption but also open fast-diffusion channels for accelerated transport kinetics. Density functional theory calculations further confirm that selenium/tellurium-rich coordination weakens polar C-S-Sn bonding and lowers redox energy barriers, thus markedly accelerating reaction dynamics. Consequently, the SnSSeTe/C anode delivers ultrahigh initial Coulombic efficiency of 91.71%, excellent rate capability, and long-term cycling stability with a reversible capacity of 395 mAh g^-1 over 2000 cycles at a high current density of 5 A g^-1. Moreover, a full SIB assembled with a Na₃V₂(PO₄)₃/C cathode achieves an impressive energy density of 258 Whkg^-1. This work underscores the disruptive potential of multinary structural engineering in guiding rational electrode design toward high-performance SIBs for sustainable energy.

锡基硫族化合物由于其丰富的氧化还原化学性质，作为钠离子电池（sib）的高能阳极具有很大的前景，但其性能受到离子传输缓慢和结构降解的阻碍。在此，我们提出了复杂的多SnSSeTe/C核壳纳米结构，其中Se和Te的同时结合不仅建立了坚固的界面C-Se-Te- sn键，而且还在SnS内部诱导了精确的晶格级取代，从而解锁了前所未有的结构和电子可调性，以及结构弹性，显著促进了合金的反向转化机制。综合动力学分析和原位表征表明，阴离子取代产生了丰富的晶格空位，这不仅增强了钠离子的吸附，而且为加速运输动力学打开了快速扩散通道。密度泛函理论计算进一步证实，富硒/富碲配位弱化极性C-S-Sn键，降低氧化还原能垒，从而显著加快反应动力学。因此，SnSSeTe/C阳极具有高达91.71%的超高初始库仑效率，出色的倍率能力和长期循环稳定性，在5 a g-1的高电流密度下，在2000次循环中可逆容量为395 mAh g-1。此外，用Na3V₂（PO₄）₃/C阴极组装的完整SIB达到了258 Whkg-1的能量密度。这项工作强调了多结构工程在指导合理电极设计以实现可持续能源高性能sib方面的颠覆性潜力。

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引用次数: 0

Ammonium fluoride plasma-triggered interface reconstruction of LLZTO for advanced solid-state batteries 先进固态电池用氟化铵等离子体触发LLZTO界面重构

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-16 DOI: 10.1016/j.ensm.2026.104996

Jiawen Chen , Tianqi Yang , Chunxiang Xian , Long Wang , Haijun Yang , Yang Wang , Chen Li , Fengxiang Chen , Guoxiang Pan , Jianbo Wu , Tengfei Zhang , Jiayuan Xiang , Yongqi Zhang , Ming Song , Lingjie Zhang , Yang Xia , Wenkui Zhang , Qi Liu , Xinhui Xia

Ta-doped garnet Li_7-xLa₃Zr_2-xTa_xO₁₂ (LLZTO) solid electrolytes are emerging as a premier oxide electrolyte, however, its practical application is hindered by surface Li₂CO₃ inert layers and poor electrode compatibility. Herein, we report a novel and efficient solid-source ammonium fluoride plasma method to modify the surface of LLZTO to address its interfacial challenges. The synergistic modification via NH₄F plasma achieves one-step conversion of Li₂CO₃ into beneficial LiF/Li₃N composite interphase layer on LLZTO in several minutes. The formation mechanism of dual-phase LiF/Li₃N layer is due to coupling reactions between Li₂CO₃ and F⁻ and N^x− radicals from NH₄F plasma. This synergistic design not only eliminates the Li₂CO₃ inert layer, but also simultaneously optimizes interfacial wettability, minimizes impedance, and reinforces mechanical integrity, supported by theoretical calculations. The plasma modification also activates LLZTO lattices with increased room-temperature ionic conductivity from 6 × 10⁻⁴ to 7.6 × 10⁻⁴ S cm⁻¹. Consequently, symmetric cells assembled with the modified LLZTO exhibit stable cycling life for 4000 h at 0.4 mA cm⁻² and 0.4 mAh cm⁻². Furthermore, full cells paired with LFP and NCM cathodes demonstrate enhanced rate performance and cycling stability. The developed plasma approach resolves the interfacial bottlenecks of LLZTO, offering mechanistic insights for oxide electrolyte optimization for advanced solid-state batteries.

掺ta石榴石Li7-xLa3Zr2-xTaxO12 （LLZTO）固体电解质正在成为一种首选的氧化物电解质，但其实际应用受到表面Li2CO3惰性层和电极相容性差的阻碍。在此，我们报告了一种新颖高效的固体源氟化铵等离子体方法来修饰LLZTO表面以解决其界面挑战。通过NH4F等离子体的协同修饰，在几分钟内实现了Li2CO3在LLZTO上一步转化为有益的LiF/Li3N复合间相层。双相LiF/Li3N层的形成机制是Li2CO3与NH4F等离子体中的F -和Nx -自由基的耦合反应。这种协同设计不仅消除了Li2CO3惰性层，而且同时优化了界面润湿性，最小化了阻抗，增强了机械完整性，理论计算支持。等离子体修饰还激活了LLZTO晶格，室温离子电导率从6 × 10−4提高到7.6 × 10−4 S cm−1。因此，用改性LLZTO组装的对称电池在0.4 mA cm - 2和0.4 mAh cm - 2下具有4000小时的稳定循环寿命。此外，与LFP和NCM阴极配对的全电池表现出更高的倍率性能和循环稳定性。开发的等离子体方法解决了LLZTO的界面瓶颈，为先进固态电池的氧化物电解质优化提供了机制见解。

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引用次数: 0

Hybrid experts-decoupled and physics-informed neural network for lithium-ion battery degradation modeling and prognosis 用于锂离子电池退化建模和预测的混合专家解耦和物理信息神经网络

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-22 DOI: 10.1016/j.ensm.2026.105002

Jialiu Zeng , Zhiming Yang , Haitao Zhu , Yifu Chen , Tianlun Huang , Penghui Tan , Xinyu Zhou , Mengyuan Zhou , Yun Zhang , Huamin Zhou

Accurate estimation of the State of Health (SOH) for lithium-ion batteries is crucial for extending service life and mitigating safety risks. However, the prevailing data-driven approaches for SOH estimation regard the internal degradation mechanisms as a black box, resulting in significant challenges such as high data requirements for complex physical models, limited model transferability, and poor electrochemical interpretability. To address these challenges with precision and comprehensiveness, we propose a hybrid experts-decoupled and physics-informed neural network (HyED-PINN), which decouples the degradation behavior and different physical fields. The HyED-PINN leverages expert models for different physical fields to extract electrochemical quantities, and employs physics-informed loss functions to train and recouple the related quantities for accurate SOH estimation. Notably, the sufficient transferability of HyED-PINN is validated by the combination of diverse datasets (electrode types, charge/discharge protocols, and operating conditions). The proposed model achieves high prediction accuracy, with the lowest RMSE reaching 0.54% on the CALCE dataset and remaining below 1.6% across all evaluated datasets. Compared with conventional neural networks, the HyED-PINN exhibits superior performance in small-sample scenarios, enhanced transfer learning capability, and importantly improved electrochemical interpretability. Overall, this study highlights the promise of physics-informed machine learning for accurate SOH estimation and extends its applicability to real-time risk detection of physical fields during battery operation.

准确估计锂离子电池的健康状态（SOH）对于延长使用寿命和降低安全风险至关重要。然而，目前流行的数据驱动SOH估算方法将内部降解机制视为一个黑匣子，这导致了对复杂物理模型的高数据要求、模型可移植性有限以及电化学可解释性差等重大挑战。为了精确和全面地解决这些挑战，我们提出了一种混合专家解耦和物理信息神经网络（HyED-PINN），它将退化行为和不同的物理场解耦。HyED-PINN利用不同物理领域的专家模型来提取电化学量，并使用物理信息损失函数来训练和重新耦合相关量，以准确估计SOH。值得注意的是，HyED-PINN的充分可转移性通过不同数据集（电极类型、充放电协议和操作条件）的组合得到验证。该模型具有较高的预测精度，CALCE数据集的RMSE最低达到0.54%，所有评估数据集的RMSE均低于1.6%。与传统神经网络相比，HyED-PINN在小样本场景下表现出优越的性能，增强了迁移学习能力，并显著提高了电化学可解释性。总的来说，这项研究强调了物理信息机器学习在精确SOH估计方面的前景，并将其应用于电池运行期间物理场的实时风险检测。

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引用次数: 0

An Ion–dipole interaction regulation of desolvation kinetics and interfacial stability for stable and fast-charging sodium-ion batteries 离子-偶极相互作用对稳定和快速充电钠离子电池脱溶动力学和界面稳定性的影响

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.2026.104943

Dong-Sheng Bai (白东升) , Shuai-Wei Wu (吴帅伟) , Na Wu (吴娜) , An-Min Liu (刘安敏) , Yang Yan (颜洋)

Sodium-ion batteries are promising candidates for grid-scale energy storage application. Nevertheless, hard carbon anodes suffer from compromised Na⁺ desolvation kinetics and inferior interfacial stability in conventional carbonate-based electrolytes. Herein, we propose an ion-pulling strategy via incorporating the ionic liquid N-methyl-N-propylpyrrolidinium bis(trifluoromethanesulfonyl)imide (Pyr₁₃TFSI) as an additive into the ester-based electrolyte. The Pyr₁₃⁺ cation competitively interacts with carbonate solvents through ion-dipole interactions, which effectively weakens Na⁺-solvent coordination and reduces the desolvation energy at the electrode-electrolyte interface. Meantime, the ion-dipole interactions suppress the diffusion of solvent molecular, thereby reducing the distribution of organic solvents at the interface and promoting the formation of a uniform and inorganic-rich solid electrolyte interface (SEI). As a result, HC anodes exhibit a high initial coulombic efficiency (81.37%), superior rate capability (252.7 mAh g^-1), and remarkable cycling stability. When paired with Na₃V₂(PO₄)₃ cathode, the full cells deliver a specific capacity of 65.1 mA h g^-1 at 20C and retain 80% of their initial capacity after 1216 cycles. This work demonstrates that regulating the bulk electrolyte properties by ionic additive can synergistically enhance interfacial kinetics and stability simultaneously, providing a viable strategy for high-performance SIBs .

钠离子电池是电网规模储能应用的有前途的候选者。然而，在传统的碳酸基电解质中，硬碳阳极受到Na+脱溶动力学和界面稳定性的影响。在此，我们提出了一种离子液体- n-甲基- n-丙基吡啶二（三氟甲烷磺酰基）亚胺（Pyr13TFSI）作为添加剂加入到酯基电解质中的离子拉动策略。Pyr13+阳离子通过离子偶极相互作用与碳酸盐溶剂竞争性相互作用，有效地减弱了Na+与溶剂的配位，降低了电极-电解质界面处的脱溶能。同时，离子偶极相互作用抑制了溶剂分子的扩散，从而减少了有机溶剂在界面处的分布，促进了均匀且富无机的固体电解质界面（SEI）的形成。结果表明，HC阳极具有较高的初始库仑效率（81.37%）、优良的倍率性能（252.7 mAh g-1）和显著的循环稳定性。当与Na3V2(PO4)3阴极配对时，完整的电池在20C下提供65.1 mA h -1的比容量，并在1216次循环后保持其初始容量的80%。本研究表明，通过离子添加剂调节本体电解质性能可以协同提高界面动力学和稳定性，为高性能sib提供了可行的策略。

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引用次数: 0

Regenerate large-scale retired second-life battery datasets via recovered capacity labels-based deep learning 通过基于回收容量标签的深度学习，再生大规模退役二次电池数据集

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.2026.104947

Yuchen Xu , Tianxiang Zeng , Weiwen Peng , Jinpeng Tian , Xiaojian Yi , Qizhi Xu , Shun-Peng Zhu

Accurate diagnosis of the health degradation of retired batteries is crucial for ensuring their safe and reliable reuse. While machine learning offers promising solutions, training models to overcome the high heterogeneity of retired batteries requires massive degradation data, leading to high testing costs and substantial energy waste. Here, we reveal the potential to recover large-scale and high-quality second-life battery datasets from field data to assist in diagnosing the health of retired batteries. By seamlessly fusing deep learning and domain knowledge, we enabled the accurate recovery of capacity labels for operating data without regular fully charging or discharging calibrations. To validate the proposed method, we develop a large-scale degradation test on 96 realistic retired batteries, performing over 50,000 charge/discharge cycles to simulate different stationary energy storage scenarios with 24 charge-discharge intervals. With only 3 capacity measurements available over the second-life, the proposed method accurately recovers the capacity labels with a root mean square error below 30 mAh. Furthermore, the health diagnostic model trained on regenerated dataset is comparable to the model trained on real data, with an almost negligible error of less than 5 mAh. More importantly, we expect to save at least 98% of test time, electricity and energy consumption to generate datasets cost-effectively. This study highlights the potential of field data to bridge the critical data gap in diagnosing the health degradation of retired batteries.

准确诊断退役电池的健康退化对于确保电池安全可靠地重复使用至关重要。虽然机器学习提供了有前途的解决方案，但训练模型来克服退役电池的高度异质性需要大量的退化数据，从而导致高测试成本和大量的能源浪费。在这里，我们揭示了从现场数据中恢复大规模和高质量二次寿命电池数据集的潜力，以帮助诊断退役电池的健康状况。通过无缝融合深度学习和领域知识，我们能够准确地恢复运行数据的容量标签，而无需定期进行完全充电或放电校准。为了验证所提出的方法，我们对96个实际退役电池进行了大规模的退化测试，进行了超过50,000次充放电循环，以模拟不同的固定储能方案，具有24个充放电间隔。由于在第二寿命期间只有3次可用的容量测量，所提出的方法可以准确地恢复容量标签，均方根误差低于30 mAh。此外，在再生数据集上训练的健康诊断模型与在真实数据上训练的模型相当，误差小于5毫安，几乎可以忽略不计。更重要的是，我们希望节省至少98%的测试时间，电力和能源消耗，以经济有效地生成数据集。这项研究强调了现场数据在诊断退役电池健康退化方面弥合关键数据差距的潜力。

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引用次数: 0

ACS structure (Anode/Current collector/Separator) for zinc-ion batteries 锌离子电池ACS结构（阳极/集流/分离器）

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.2026.104935

Hongfei Lu , Di Zhang , Zhiyi Du , Xinyao Yuan , Yuhang Song , Zili Zhang , Nawei Lyu , Xin Jiang , Yang Jin

Aqueous zinc-ion batteries (AZIBs) are promising for energy storage due to their safety and resource abundance. However, thin zinc anodes that are highly efficient, easy to apply on a large scale and have few dendrites remain a challenge. This study introduces a novel anode/current collector/separator (ACS) structure, replacing traditional configurations. The novel ACS design employs a microporous copper (Mp-Cu) foil to physically separate the zinc foil and separator. The skeleton of the Mp-Cu foil ensures the conductive pathway, while its micropores facilitate ion transport. This innovative structure delivers several key advantages: 1) uniform distribution of zinc ions and initial stripping, 2) in-situ Cu@Zn alloying to promote uniform zinc deposition, 3) physical separation of reserve zinc and active zinc, and 4) enhanced zinc utilization on Mp-Cu foil. Therefore, Zn||Zn cell lifespan increased from 124 h (CAS) to over 1100 h (ACS) at 49.6 % zinc utilization (4 mAh cm^-2). The ACS-structured zinc-iodine coin cell achieved over 4000 h and 60,000 cycles (vs. 2116 cycles for CAS). The cycle lifetime of a double-layer ACS-structured zinc-iodine pouch cell was more than 1200 cycles with 89.8 % capacity retention. At low current density, the ACS-structured 2.79 Ah zinc-iodine pouch cell cycled 200 times with a capacity retention of 82.65 % and practical energy density of 29.7 Wh kg^-1 (based on all battery components). The operational mechanism of this novel structure helps us to gain a deeper understanding of ion mobility and metal stripping/deposition behavior in the cell. The novel ACS structure facilitates large-scale applications of high-performance metal anodes that do not require electroplating, effectively facilitating the development of advanced AZIBs.

水锌离子电池（azib）由于其安全性和资源丰富而在储能方面具有广阔的应用前景。然而，高效、易于大规模应用且枝晶较少的薄锌阳极仍然是一个挑战。本研究提出一种新的阳极/集流/分离器（ACS）结构，取代传统结构。新型ACS设计采用微孔铜箔（Mp-Cu）将锌箔和分离器进行物理分离。Mp-Cu箔的骨架保证了导电通道，而其微孔促进了离子的传输。这种创新的结构具有以下几个关键优势：1)锌离子均匀分布和初始剥离；2)原位Cu@Zn合金化促进均匀的锌沉积；3)储备锌和活性锌的物理分离；4)提高Mp-Cu箔上锌的利用率。因此，当锌利用率为49.6% （4 mAh cm-2）时，锌电池寿命从124 h （CAS）增加到1100 h （ACS）以上。acs结构的锌碘硬币电池实现了超过4000小时和60,000次循环（而CAS为2116次循环）。双层acs结构锌碘袋电池的循环寿命超过1200次，容量保留率为89.8%。在低电流密度下，acs结构的2.79 Ah锌碘袋电池循环200次，容量保持率为82.65%，实际能量密度为29.7 Wh kg-1（基于所有电池组件）。这种新型结构的运作机制有助于我们更深入地了解离子迁移和金属在电池中的剥离/沉积行为。新型的ACS结构促进了不需要电镀的高性能金属阳极的大规模应用，有效地促进了先进azib的发展。

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引用次数: 0

Immobilizing anions via electron‑deficient π desgin: A PolyMOF-based composite electrolyte for stable solid-state lithium metal batteries 通过缺电子π设计固定化阴离子：用于稳定固态锂金属电池的多晶硅基复合电解质

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-24 DOI: 10.1016/j.ensm.2026.104923

Lulu Liu, Lei Chen, Xianghui Liu, Xiaoen Wang, Zhongwei Chen

Conventional solid polymer electrolytes (SPEs) face critical challenges such as low Li⁺ conductivity, excessive anion mobility and interfacial instability, which hinder their applications in high-energy lithium (Li) metal batteries. Herein, we develop a multi-mechanism synergistic strategy by incorporating a polymer–metal–organic framework (PolyMOF) into a poly(vinylidene fluoride-co-hexafluoropropylene) (PVHF) matrix to construct a composite solid-state electrolyte (PolyMOF@PVHF). Within this design, polymer ligands in PolyMOF induce electron redistribution via p‑π conjugation, forming strong anion–π⁺ interactions that selectively immobilizes TFSI⁻ and suppresses anion migration. Concurrently, surface hydrogen-bonding motifs trap residual solvent molecules while the nanoconfinement effect promotes Li⁺ desolvation, enabling rapid ion transport through ultralow-barrier channels. The synergistic mechanism collectively inhibits side reactions and facilitate uniform Li⁺ deposition at the solid electrolyte interphase (SEI) interface. As a result, the PolyMOF@PVHF electrolyte achieves a high ionic conductivity of 1.23 × 10-3 S cm^-1 and a Li⁺ transference number of 0.75 at room temperature (RT). The electrolyte also exhibits exceptional interfacial stability, enabling reversible Li plating/stripping over 1900 h and long-term cycling in Li metal batteries (1500 cycles at 2C with 99.9 % capacity retention for LFP; 200 cycles with 93.5 % retention for NCM811). Moreover, the assembled NCM811|Li pouch cell shows outstanding safety and mechanical robustness under bending, folding and cutting. This work provides a viable strategy to overcome Li⁺ transport and interfacial issues in SPEs, paving the way for high-performance solid-state Li metal batteries.

传统的固体聚合物电解质（spe）面临着Li+电导率低、阴离子迁移率过高和界面不稳定等严峻挑战，阻碍了它们在高能锂（Li）金属电池中的应用。在此，我们开发了一种多机制协同策略，通过将聚合物-金属-有机框架（PolyMOF）结合到聚偏氟乙烯-共六氟丙烯（PVHF）基体中来构建复合固态电解质（PolyMOF@PVHF）。在这个设计中，PolyMOF中的聚合物配体通过p -π偶联诱导电子重新分布，形成强阴离子-π +相互作用，选择性地固定TFSI⁻并抑制阴离子迁移。同时，表面的氢键基序捕获了残留的溶剂分子，而纳米约束效应促进了Li +的脱溶，使离子能够通过超低势垒通道快速传输。协同机制共同抑制副反应，促进Li+在固体电解质界面（SEI）均匀沉积。结果，PolyMOF@PVHF电解质在室温（RT）下获得了1.23 × 10-3 S cm-1的高离子电导率和0.75的迁移数。该电解质还表现出优异的界面稳定性，能够在1900小时内实现可逆的锂电镀/剥离，并在锂金属电池中长期循环（LFP在2C下循环1500次，容量保持率为99.9%；NCM811循环200次，容量保持率为93.5%）。此外，组装的NCM811|锂袋电池在弯曲，折叠和切割下具有出色的安全性和机械坚固性。这项工作为克服spe中Li⁺的传输和界面问题提供了一种可行的策略，为高性能固态锂金属电池的发展铺平了道路。

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引用次数: 0

Multicomponent alloy–engineered interfaces for magnetic regulation of sodium deposition in anode-free sodium metal batteries 无阳极钠金属电池中钠沉积磁调节的多组分合金工程界面

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-01-19 DOI: 10.1016/j.ensm.2026.104915

Zewei Hu , Haiying Lu , Liyang Liu , Yunqi Gao , Yuju Qi , Xin Wang , Jiayao Wang , Peng Xie , Chao Han , Weijie Li

Anode-free sodium metal batteries (AFSMBs) hold great promise for high-energy sodium storage but are plagued by unstable interfaces and dendritic sodium growth arising from uneven plating and stripping. Here, we introduce a magnetic–electric dual-field interfacial regulation strategy by engineering a FeCoNiCuSn multicomponent alloy (MA) integrated with a carbon nanotube (CNT) scaffold on commercial aluminum foil (MA@CNT). The interconnected CNT framework provides a three-dimensional conductive network that accommodates volume changes and firmly anchors MA nanoparticles. The Sn component ensures homogeneous Na nucleation, while Cu, Fe, Co, and Ni form multicomponent alloys with Sn to mitigate volume expansion during cycling. More importantly, the magnetic elements (Fe, Co, Ni) create localized magnetic fields that direct Na⁺ flux through Lorentz-force-driven migration, leading to uniform deposition and effective suppression of dendritic growth–an interfacial regulation mechanism unexplored in AFSMBs. Benefiting from these synergistic effects, MA@CNT||Na asymmetric cells deliver stable cycling for over 600 cycles at 1 mA cm^–², and the MA@CNT||Na₃V₂(PO₄)₃ full cells exhibit excellent rate capability and long-term stability. This study establishes magnetic-interface engineering as a powerful strategy to achieve dendrite-free sodium deposition, offering a new paradigm for the design of stable, high-performance anode-free sodium metal batteries.

无阳极金属钠电池（AFSMBs）在高能钠存储方面具有很大的前景，但由于镀层和剥离不均匀而导致界面不稳定和枝状钠生长而受到困扰。本文介绍了一种磁电双场界面调节策略，通过将FeCoNiCuSn多组分合金（MA）与碳纳米管（CNT）支架集成在商用铝箔上（MA@CNT）。相互连接的碳纳米管框架提供了一个三维导电网络，可以适应体积变化并牢固地锚定MA纳米颗粒。Sn成分确保了均匀的Na形核，而Cu、Fe、Co和Ni与Sn形成多组分合金，以减轻循环过程中的体积膨胀。更重要的是，磁性元素（Fe, Co, Ni）产生了局部磁场，引导Na⁺的通量通过洛伦兹力驱动的迁移，导致均匀沉积并有效抑制枝晶生长——这是afsmb中尚未探索的界面调节机制。受益于这些协同效应，MA@CNT||Na不对称电池在1 mA cm-2下提供超过600次的稳定循环，MA@CNT||Na₃V₂（PO₄）₃全电池表现出优异的速率能力和长期稳定性。本研究确立了磁界面工程作为实现无枝晶钠沉积的有力策略，为设计稳定、高性能的无阳极金属钠电池提供了新的范例。

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引用次数: 0

Unraveling A lattice lithium supplementation-interfacial catalysis tandem effect for enabling durable lithium-ion full cells 揭示晶格锂补充-界面催化串联效应，使持久的锂离子充满电池

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-09 DOI: 10.1016/j.ensm.2026.104973

Yuetong Chen , Guomin Li , Xiaodan Yang , Yanyi Wang , Liang Tian , Hongwei Mi , Ning Zhao , Dingtao Ma , Peixin Zhang

Prelithiation has been widely recognized as an effective strategy to compensate for active lithium loss and enhance the energy density of lithium-ion batteries. This work unlocks a green and efficient La-doped pre-lithiation additive La-Li₂NiO₂. As revealed, such cathode prelithiation material exhibits dual functionality, it can effectively compensate LiFePO₄ for irreversible lattice lithium loss during cycling, and upon completion of the first cycle, it will transform into catalytically active La-LiNiO₂. Interestingly, this transformed material enables reducing the dissociation energy barrier of LiPF₆ while concurrently catalyzing the decomposition of LiPF₆ leading to the formation of a thin, uniform, and LiF-rich cathode/electrolyte interphase (CEI). Compared with the pristine Li‖LiFePO₄ half-cell, benefiting from the tandem effect of lithium supplementation and interface optimization, the Li‖LiFePO₄ with 5 % La-Li₂NiO₂ prelithiation additive exhibits superior rate performance, achieving a specific capacity of 95.2 mAh g^-1 at 10 C rate. Beyond that, the Graphite‖LiFePO₄ with 5 % La-LNO full cells exhibit an 86.0 % capacity retention rate after 1000 cycles even at 5 C condition. This work highlights a new design paradigm for cathode prelithiation additives that integrate efficient lithium compensation and interface regulation, it can deepen the understanding of constructing practical full cells including but not limited to lithium-ion batteries.

预锂化是一种补偿活性锂离子损失和提高锂离子电池能量密度的有效策略，已被广泛认可。本研究揭示了一种绿色高效的la掺杂预锂化添加剂La-Li2NiO2。结果表明，这种阴极预锂化材料具有双重功能，它可以有效补偿LiFePO4在循环过程中不可逆晶格锂的损失，并且在第一次循环完成后，它将转化为具有催化活性的La-LiNiO2。有趣的是，这种转化后的材料能够降低LiPF6的解离能垒，同时催化LiPF6的分解，从而形成薄、均匀、富liff的阴极/电解质界面（CEI）。与原始Li‖LiFePO4半电池相比，受益于锂补充和界面优化的串联效应，添加5% La-Li2NiO2预锂化添加剂的Li‖LiFePO4表现出更好的倍率性能，在10℃倍率下达到95.2 mAh g-1的比容量。除此之外，含有5%添加剂的石墨‖LiFePO4在5℃条件下，即使在1000次循环后也表现出86.0%的容量保持率。这项工作强调了阴极预锂化添加剂的一种新的设计范式，它集成了有效的锂补偿和界面调节，它可以加深对构建实用的全电池的理解，包括但不限于锂离子电池。

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引用次数: 0