Energy Storage Materials最新文献_第8页

Decoupling the areal-volumetric-kinetic trilemma in high-mass-loading supercapacitors via a 3D topological electrode design 通过三维拓扑电极设计解耦高质量负载超级电容器的面积-体积-动力学三难困境

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.2026.105004

Zhilin Wu , Chensheng Wang , Wenbin Kang , Xiyuan Zhong , Haojie Zuo , Haitao Hu , Yingze Song

The advancement of modern electronic and energy systems requires supercapacitors that simultaneously exhibit rapid kinetics, high areal and volumetric performance. Achieving this combination is critical for applications with stringent spatial and volumetric constraints and necessitates the design of electrodes with high mass loading in a compact, densified structure. However, the fundamental areal-volumetric-kinetic trilemma, has historically made these goals mutually exclusive due to restricted electrolyte transport within tortuous electrode architectures. In this work, a multiscale topological electrode design is presented to decouple this trilemma. The strategy utilizes additive manufacturing to architect macroscopically ordered electrolyte pathways, which are synergistically integrated with a conformal overlay of a mixed ionic-electronic conductor to enhance microscopic electrolyte connectivity, enabling an exceptional combination of areal (6.8 F/cm²) and volumetric (79.7 F/cm³) capacitance at a 121.1 mg/cm² loading density, without compromised kinetic capability. The underlying mechanism for overcoming this trade-off is further explored, highlighting the critical role of the topological design in reducing electrochemical polarization and significantly enhancing ionic diffusivity within a compact transport environment. These findings unlock a new design paradigm that targets the mitigation of key transport limitations and lays the groundwork for compact, fast-charging energy storage devices with significantly enhanced energy densities.

现代电子和能源系统的进步需要超级电容器同时表现出快速动力学，高面积和体积性能。实现这种组合对于具有严格空间和体积限制的应用至关重要，并且需要在紧凑，致密的结构中设计具有高质量负载的电极。然而，由于扭曲的电极结构限制了电解质的传输，基本的面积-体积-动力学三难困境历来使这些目标相互排斥。在这项工作中，提出了一种多尺度拓扑电极设计来解耦这种三难困境。该策略利用增材制造来构建宏观有序的电解质路径，这些路径与混合离子-电子导体的保形覆盖层协同集成，以增强微观电解质的连通性，从而在121.1 mg/cm2的负载密度下实现面积（6.8 F/cm2）和体积（79.7 F/cm3）电容的卓越组合，而不影响动力学能力。进一步探讨了克服这种权衡的潜在机制，强调了拓扑设计在减少电化学极化和显著提高紧凑传输环境中离子扩散率方面的关键作用。这些发现开启了一种新的设计范式，旨在缓解关键的传输限制，并为显著提高能量密度的紧凑、快速充电储能设备奠定了基础。

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引用次数: 0

Cyclodextrin stabilized thick iodine cathodes with dry-processability for high-performing pouch Zn-Ion batteries 用于高性能袋式锌离子电池的具有干加工性能的环糊精稳定厚碘阴极

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.2026.105005

Yongxin Su , Siwen Deng , Dongcheng Zhou , Shurui Lin , Liping Shu , Xiumei Li , Qimin Guo , Wei Liu , Shaohong Shi , Fangchao Cheng

The shuttle effect of iodine cathodes in the aqueous zinc-iodine (Zn-I₂) batteries (AZIBs) induces the loss of active iodine and triggers Zn corrosion, greatly deteriorating the cell lifespan. In this study, we report a biofriendly, facile and highly effective cathode additive (β-cyclodextrin, β-CD) to inhibit shuttle effect. As 10 % β-CD incorporation is added into the electrode, the iodine loss is greatly mitigated by forming the β-CD/I inclusion. Besides, the wettability of electrode is significantly enhanced after incorporating β-CD, thereby enabling to fully contribute the inherent electrochemical capacity of thick electrodes. In addition. the β-CD/I inclusion practiced in electrochemical reaction and contributed capacity. Owing to these, the 91.8 % capacity retention after 1000 cycles at 1 C, and 95.4 % retention after 8000 cycles at 5 C are achieved under 186 mAh·g^-1 and 1.16 mAh·cm^-2, respectively. More impressively, the dry-processing pouch cell (0.3 Ah) with large-areal thick electrodes (40 cm², 500 μm) realizes a high area capacity (3.75 mAh·cm^-2) and capacity retention (92.8 % after 120 cycles), demonstrating its promising potential for the large-scale production of cells. Overall, this facile strategy not only presents a biocompatible stabilizer for the thick I₂ cathode, but also develops a novel approach for fabricating the advanced aqueous Zn-I₂ batteries for extended lifespan and sustainability.

锌-碘（Zn- i2）水电池中碘阴极的穿梭效应导致活性碘的损失和锌的腐蚀，大大降低了电池寿命。在这项研究中，我们报道了一种生物友好的、简单的、高效的阴极添加剂（β-环糊精，β-CD）来抑制穿梭效应。在电极中加入10%的β-CD，通过形成β-CD/I包合物，大大减轻了碘的损失。此外，加入β-CD后，电极的润湿性显著增强，从而能够充分发挥厚电极固有的电化学容量。此外。β-CD/I包合物在电化学反应中发挥作用，对容量有贡献。因此，在186 mAh·g-1和1.16 mAh·cm-2条件下，在1℃下1000次循环后的容量保持率为91.8%，在5℃下8000次循环后容量保持率为95.4%。更令人印象深刻的是，具有大面积厚电极（40 cm2, 500 μm）的干处理袋状电池（0.3 Ah）实现了高面积容量（3.75 mAh·cm-2）和120次循环后的容量保持率（92.8%），显示了其大规模生产电池的潜力。总的来说，这种简单的策略不仅为厚I2阴极提供了一种生物相容性稳定剂，而且为制造先进的水性锌-I2电池提供了一种新的方法，从而延长了电池的使用寿命和可持续性。

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引用次数: 0

Interlayer architecture and performance code: Structural mechanism and modification decoding of manganese base layer oxides in potassium-ion batteries 层间结构与性能代码：钾离子电池中锰基氧化物的结构机理与修饰解码

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-26 DOI: 10.1016/j.ensm.2026.105012

Xinran Li , Longjiao Chang , Shaohua Luo , Yongbing Li , Zenglei Hou , Jie Zou , Ruohao Ruan , Fan Guo , Longqan Cui , Mingyang Song

Potassium-ion batteries exhibit high environmental friendliness and low cost, positioning them as one of the most promising energy storage materials following lithium-ion and sodium-ion batteries. Among these, manganese layered oxides (MLO) stand out due to their high theoretical specific capacity and excellent tunability. However, numerous challenges persist in their structural and electrochemical properties. For researchers, a thorough understanding of the structure and critical issues of manganese layered oxides is pivotal for further advancement. This paper provides a detailed exposition of the structure of manganese-based layered oxides, conducting an in-depth analysis of their critical challenges. It classifies and thoroughly examines commonly used doping elements from the perspective of modification mechanisms, while also elaborating on morphology control and surface coating techniques. This review offers detailed exposition and synthesis of underlying mechanisms, providing valuable insights for ongoing modification efforts. Building upon recent research achievements, it concludes with an outlook on the future applications of manganese-based layered oxides in potassium-ion batteries.

钾离子电池具有高环境友好性和低成本的特点，是继锂离子电池和钠离子电池之后最有前途的储能材料之一。其中，锰层状氧化物（MLO）因其较高的理论比容量和优异的可调性而脱颖而出。然而，它们的结构和电化学性能仍然存在许多挑战。对于研究人员来说，深入了解锰层状氧化物的结构和关键问题是进一步发展的关键。本文详细介绍了锰基层状氧化物的结构，并对其关键挑战进行了深入分析。从改性机理的角度对常用掺杂元素进行了分类和深入的研究，同时对形貌控制和表面涂层技术进行了阐述。这篇综述提供了对潜在机制的详细阐述和综合，为正在进行的修改工作提供了有价值的见解。结合近年来的研究成果，对锰基层状氧化物在钾离子电池中的应用前景进行了展望。

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引用次数: 0

Interpretable enhanced-ECFP-guided deep learning for rational electrolyte design and Coulombic efficiency prediction in lithium metal batteries 可解释的增强ecfp引导深度学习用于锂金属电池的合理电解质设计和库仑效率预测

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-07 DOI: 10.1016/j.ensm.2026.104972

Doo Bong Lee , Jinwoo Park , Eunji Kim , Woong Kim

Rational electrolyte design is essential for enhancing the Coulombic efficiency (CE) and interfacial stability of lithium metal batteries. However, current molecular representations limited in their description of molecular connectivity and lacking substructure frequency information constrain the development of accurate and interpretable AI models. This paper introduces an interpretable AI framework to predict CE using an enhanced extended-connectivity fingerprint representation that integrates molecular type, substructure frequency, and concentration weighting. A dataset of 168 CE values from Li–Cu half–cells was used to train a deep neural network, which outperformed conventional methods in predictive accuracy. SHapley Additive exPlanations analysis identified fluorine-containing and cyclic ether motifs as key structural features for high CE. Accordingly, a fluorine-rich, cyclic-ether-based electrolyte (1 M lithium bis(fluorosulfonyl)imide in methyltetrahydrofuran and 1,1,2,2-tetrafluoroethyl 2,2,3,3-tetrafluoropropyl ether (1:3 v/v)) achieved a CE of 99.72% in Li–Cu cells and excellent cycling stability in lithium–lithium iron phosphate full cells. This framework can facilitate AI-based molecular design for electrochemical energy storage and conversion.

合理的电解液设计对于提高锂金属电池的库仑效率和界面稳定性至关重要。然而，目前的分子表征在描述分子连通性和缺乏子结构频率信息方面受到限制，限制了准确和可解释的人工智能模型的发展。本文介绍了一个可解释的AI框架，使用增强的扩展连接指纹表示来预测CE，该指纹表示集成了分子类型、子结构频率和浓度权重。使用来自锂铜半电池的168个CE值数据集来训练深度神经网络，该网络在预测精度上优于传统方法。SHapley加性解释分析确定含氟和环醚基序是高CE的关键结构特征。因此，一种富含氟的环醚电解质（1 M双（氟磺酰基）锂亚胺甲基四氢呋喃和1,1,2,2,2 -四氟乙基2,2,3,3-四氟丙基醚（1:3 v/v））在Li-Cu电池中的CE为99.72%，在锂-磷酸铁锂电池中具有优异的循环稳定性。该框架可以促进基于人工智能的电化学能量存储和转换分子设计。

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引用次数: 0

Smoothing S8 redox conversions in lean ester electrolytes by nucleophilic shielding and polar ZnS electrovalent mediation: Toward near-practical S cathodes 通过亲核屏蔽和极性ZnS电介质平滑贫酯电解质中的S8氧化还原转化：接近实用的S阴极

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-02 DOI: 10.1016/j.ensm.2026.104958

Zhihao Yan , Chunyan Ye , Jianhui Zhu , Lu Zhang , Junxiang Wang , Maowen Xu , Jian Jiang

Practical sulfur (S) cathode usage is still in a dilemma owing to their low-areal-capacity and polysulfide-shuttle challenges in ether electrolytes. Though using ester-compatible small-molecule S_x can bypass these kinetic issues, their low S content limits high-energy charge-storage utilizations. To overcome above constraints, we propose to make lean-ester-electrolyte-compatible S₈-rich Zn_0.06S@S_x (total usable S content >64 wt%) microsphere cathodes featured by high tap/compaction densities and gradient core-shell configurations. The outer nucleophilic shielding layers can protect S₈ components from ester solvent penetrations, help to stabilize cathode interfaces and offer capacity contributions/prompt solid-state Li⁺ paths for inner thionic reactions. Systematic in-situ detections affirm the dispersed polar ZnS nano domains (∼4 nm) in cores can expedite adjacent S₈ redox conversions by chemical coordination and electrovalent mediations (Zn⁺²→Zn^+1.01). Such cathodes own a very impressive S utilization ratio of ∼89.3%, with exceptional discharge capacity (893 mAh g^-1; based on all usable Zn_0.06S@S_x cathode mass) and rate/cyclic behaviors. Packed pouch cells with remarkable cathode areal loading (∼14.4 mg cm^-2) and lean electrolyte conditions (∼2 μL mg_s^-1) exhibit salient energy densities of ∼883.3 W h L^-1/398.6 Wh kg^-1, holding great promise as high-energy power sources for robotic industries.

由于硫阴极在乙醚电解质中的低面积容量和多硫化物穿梭挑战，实际硫阴极的使用仍然处于两难境地。虽然使用酯兼容的小分子Sx可以绕过这些动力学问题，但它们的低S含量限制了高能电荷存储的利用。为了克服上述限制，我们建议制造具有高轻敲/压实密度和梯度核壳结构的贫酯-电解质兼容的富含s8的Zn0.06S@Sx（总可用S含量>；64 wt%）微球阴极。外亲核屏蔽层可以保护S8组分免受酯溶剂的渗透，有助于稳定阴极界面，并为内硫离子反应提供容量贡献/提示固态Li+路径。系统的原位检测证实，岩心中分散的极性ZnS纳米畴（~ 4 nm）可以通过化学配位和电位介质（Zn+2→Zn+1.01）加速相邻的S8氧化还原转化。这种阴极具有非常令人印象深刻的S利用率~ 89.3%，具有出色的放电容量（893 mAh g-1；基于所有可用的Zn0.06S@Sx阴极质量）和速率/循环行为。具有显著阴极面积负载（~ 14.4 mg cm-2）和稀薄电解质条件（~ 2 μL mg -1）的包装袋电池具有显著的能量密度（~ 883.3 Wh L-1/398.6 Wh kg-1），有望成为机器人工业的高能电源。

{"title":"Smoothing S8 redox conversions in lean ester electrolytes by nucleophilic shielding and polar ZnS electrovalent mediation: Toward near-practical S cathodes","authors":"Zhihao Yan , Chunyan Ye , Jianhui Zhu , Lu Zhang , Junxiang Wang , Maowen Xu , Jian Jiang","doi":"10.1016/j.ensm.2026.104958","DOIUrl":"10.1016/j.ensm.2026.104958","url":null,"abstract":"<div><div>Practical sulfur (S) cathode usage is still in a dilemma owing to their low-areal-capacity and polysulfide-shuttle challenges in ether electrolytes. Though using ester-compatible small-molecule S<sub>x</sub> can bypass these kinetic issues, their low S content limits high-energy charge-storage utilizations. To overcome above constraints, we propose to make lean-ester-electrolyte-compatible S<sub>8</sub>-rich Zn<sub>0.06</sub>S@S<sub>x</sub> (total usable S content >64 wt%) microsphere cathodes featured by high tap/compaction densities and gradient core-shell configurations. The outer nucleophilic shielding layers can protect S<sub>8</sub> components from ester solvent penetrations, help to stabilize cathode interfaces and offer capacity contributions/prompt solid-state Li<sup>+</sup> paths for inner thionic reactions. Systematic <em>in-situ</em> detections affirm the dispersed polar ZnS nano domains (∼4 nm) in cores can expedite adjacent S<sub>8</sub> redox conversions by chemical coordination and electrovalent mediations (Zn<sup>+2</sup>→Zn<sup>+1.01</sup>). Such cathodes own a very impressive S utilization ratio of ∼89.3%, with exceptional discharge capacity (893 mAh g<sup>-1</sup>; based on all usable Zn<sub>0.06</sub>S@S<sub>x</sub> cathode mass) and rate/cyclic behaviors. Packed pouch cells with remarkable cathode areal loading (∼14.4 mg cm<sup>-2</sup>) and lean electrolyte conditions (∼2 μL mg<sub>s</sub><sup>-1</sup>) exhibit salient energy densities of ∼883.3 W h L<sup>-1</sup>/398.6 Wh kg<sup>-1</sup>, holding great promise as high-energy power sources for robotic industries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104958"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146110646","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

Bioinspired aerogel-confined phase change materials for high-performance thermal rectification and device cooling 用于高性能热整流和器件冷却的生物气凝胶约束相变材料

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-03 DOI: 10.1016/j.ensm.2026.104961

Zubair Ashraf , Akbar Bashir , Ali Usman , Mulin Qin , Atif Nazir , Haiwei Han , Kaihang Jia , Sadia Noreen , Waseem Aftab , Zhenghui Shen , Ruqiang Zou

Efficient thermal regulation is essential for advanced electronic and energy systems, yet conventional phase-change materials (PCMs) often suffer from leakage, limited thermal rectification, and inadequate long-term cycling stability. Here, we report a bioinspired and scalable strategy for constructing hierarchically asymmetric aerogels integrating isotropic graphene oxide (GO) and anisotropic vertically aligned reduced graphene oxide (v-rGO) networks, followed by in situ paraffin wax (PW) confinement to form GOX@PW and v-rGOX@PW composites. The synergistic coupling between structural anisotropy and the phase-dependent thermal behavior of PW yields leakage-free composites with high latent-heat retention (∼96–98%) after 300 cycles and pronounced anisotropic thermal conductivity, reaching 1.65 W m^-1 K^-1 in the through-plane direction. An asymmetric GOX@PW/v-rGOX@PW bilayer device exhibits a thermal rectification ratio of up to ∼2.6 under a small temperature bias of ∼13 °C, demonstrating effective direction-dependent heat transport. The aerogel-confined hierarchical architecture enables stable, reversible phase transitions, efficient heat routing, and diode-like one-way thermal regulation. When implemented as thermal interface layers for CPU and GPU cooling, v-rGOX@PW significantly suppresses peak operating temperatures, demonstrating strong device-level applicability. Overall, this work establishes a multifunctional platform integrating structurally confined PCMs with anisotropic aerogel architectures, offering a general design pathway for next-generation thermal management, anisotropic heat control, and energy-efficient electronics.

高效的热调节对于先进的电子和能源系统至关重要，然而传统的相变材料（pcm）经常存在泄漏、有限的热整流和长期循环稳定性不足的问题。在这里，我们报告了一种生物启发和可扩展的策略，用于构建层次不对称气凝胶，整合各向同性氧化石墨烯（GO）和各向异性垂直排列还原氧化石墨烯（v-rGO）网络，然后原位石蜡（PW）约束形成GOX@PW和v-rGOX@PW复合材料。PW的结构各向异性和相相关热行为之间的协同耦合产生了无泄漏复合材料，在300次循环后具有高的潜热保留率（~ 96-98%）和显著的各向异性导热系数，在透平面方向达到1.65 W m-1 K-1。不对称GOX@PW/v-rGOX@PW双层器件在~ 13°C的小温度偏置下显示出高达~ 2.6的热整流比，证明了有效的方向相关热传输。气凝胶约束的分层结构实现了稳定、可逆的相变、高效的热路由和类似二极管的单向热调节。当作为CPU和GPU冷却的热接口层实现时，v-rGOX@PW显着抑制峰值工作温度，显示出强大的设备级适用性。总的来说，这项工作建立了一个多功能平台，将结构受限的pcm与各向异性气凝胶结构集成在一起，为下一代热管理、各向异性热控制和节能电子产品提供了通用的设计途径。

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引用次数: 0

Boosting polysulfide redox via cobalt spin-state manipulation in lithium-sulfur batteries 锂硫电池中钴自旋态操纵促进多硫化物氧化还原

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.2026.104954

Chunze Zhou , Lei Chen , Weifeng Shen , Xiaoliang Zhang , Xiaojie Lu , Meltem Yanilmaz , Yong Liu

The commercialization of lithium-sulfur batteries (LSBs) has been significantly hindered by rapid performance degradation during long-term cycling, which originates from lithium polysulfides (LiPSs) shuttling and uncontrolled lithium dendrite growth. In this work, guided by ligand field theory and molecular orbital principles, we modulate the spin state of spinel-type oxides via boron doping, leading to the formation of nanoflower-structured catalysts with an intermediate spin (IS, t_2g⁵e_g¹) configuration. Boron doping effectively regulates the spin state of Co³⁺, resulting in the generation of numerous unpaired electrons distributed across different 3d orbitals. This electronic reconstruction causes an upshift in energy levels and creates more active electronic states, which collectively enhance LiPSs adsorption, facilitate charge transfer, and improve redox kinetics. Employing the modified separator enables outstanding rate performance, with the cell delivering 1255.2 and 960 mAh g⁻¹ at 0.2 and 2 C, respectively. The electrode maintains exceptional capacity retention with suppressed polysulfide loss under high sulfur loading, confirming the functional separator's efficacy. This work proposes a doping-based strategy for electronic spin-state modulation in LSBs catalysts, offering a promising direction for next-generation energy storage systems.

锂硫电池（LSBs）在长期循环过程中，由于多硫化物锂（LiPSs）的穿梭和不受控制的锂枝晶生长而导致的性能快速下降，严重阻碍了锂硫电池（LSBs）的商业化。在配体场理论和分子轨道原理的指导下，我们通过硼掺杂来调节尖晶石型氧化物的自旋态，从而形成具有中间自旋（IS, t2g5eg1）构型的纳米花结构催化剂。硼掺杂有效地调节了Co3+的自旋状态，从而产生了分布在不同三维轨道上的大量不成对电子。这种电子重构导致能级的上升，并产生更活跃的电子态，这共同增强了LiPSs的吸附，促进了电荷转移，并改善了氧化还原动力学。采用改进的分离器可以实现出色的倍率性能，电池在0.2℃和2℃下分别提供1255.2和960 mAh g - 1。在高硫负载下，电极保持了特殊的容量保持，抑制了多硫损失，证实了功能性分离器的功效。本研究提出了一种基于掺杂的lsb催化剂的电子自旋态调制策略，为下一代储能系统提供了一个有希望的方向。

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引用次数: 0

Exfoliated coal-derived hard carbon enabling the trade-off between plateau capacity and Fast Na+ kinetics for sodium-ion batteries 剥离煤衍生硬碳实现了钠离子电池平台容量和快速Na+动力学之间的权衡

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.2026.104974

Gaoxu Han , Shengle Hao , Yuxin Shi , Wei Lv , Ruitao Lv , Wanci Shen , Feiyu Kang , Deping Xu , Zheng-Hong Huang

Coal is an attractive precursor for hard carbon anodes in sodium-ion batteries. However, these carbons often face the challenge of achieving high capacity and fast Na⁺ kinetics simultaneously. Herein, we propose an oxidized-coal precursor-derived hard carbon that exhibits a sheet-like structure and a tunable interlayer spacing, which addresses the aforementioned problem. A H₂O₂/H₂SO₄ chemical oxidation-exfoliation produces an oxidized-coal precursor with nanosheet morphology enriched in -COOH/-OH.

-OH groups. These functional groups induce premature crosslinking of organic macromolecules, constructing a turbostratic carbon framework that suppresses ordered layer growth and expands the interlayer spacing. As the carbonization temperature further increases, polycondensation and structural reorganization are enhanced, driving more compact stacking of carbon layers. This enables a controllable decrease in interlayer spacing accompanied by the evolution of closed pores. The result small microcrystallite size with expanded interlayer spacing reduces Na⁺ intercalation/diffusion resistance. The optimized sample exhibits a capacity of 327 mAh g^-1, including a high plateau capacity of 191 mAh g^-1. Note that the capacity of 214 mAh g^-1 at an ultra-high current density of 10 A g^-1 is retained, much higher than the previous reports. This work provides a new insight into the preparation of high-power, high-energy coal-based hard carbon for advanced sodium ion batteries.

煤是钠离子电池硬碳阳极的有吸引力的前体材料。然而，这些碳经常面临同时实现高容量和快速Na⁺动力学的挑战。在此，我们提出了一种氧化煤前驱体衍生的硬碳，它具有片状结构和可调节的层间距，解决了上述问题。H2O2/H2SO4化学氧化-剥落反应生成了富含-COOH/-OH基团的纳米片状氧化煤前驱体。这些官能团诱导有机大分子的过早交联，构建了一个抑制有序层生长和扩大层间距的涡轮层碳框架。随着炭化温度的进一步升高，缩聚和结构重组增强，促使碳层的堆积更加致密。这使得层间间距的可控减小伴随着封闭孔隙的演化。微晶尺寸小，层间距扩大，降低了Na⁺的插渗/扩散阻力。优化后的样品显示出327 mAh g-1的容量，其中包括191 mAh g-1的高平台容量。请注意，在10 A g-1的超高电流密度下，保留了214 mAh g-1的容量，远高于之前的报道。本研究为先进钠离子电池用高功率、高能量煤基硬碳的制备提供了新的思路。

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引用次数: 0

Fluorinated fluid cooling to address thermal safety issues in lithium-ion batteries with radicals capturing and boiling heat transfer 氟化流体冷却，以解决锂离子电池的热安全问题，自由基捕获和沸腾传热

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.2026.104980

Xinyu Liu , Yang Li , Zhining Zhang , Zihao Zhao , Zhifu Zhou , Wei-Tao Wu , Lei Wei , Chengzhi Hu , Linsong Gao , Yubai Li , Yongchen Song

Thermal runaway (TR) is a severe challenge to the widespread commercial adoption of high energy-density lithium-ion batteries (LIBs). Nonetheless, the current strategies lack responsiveness for both extreme heat dissipation and explosion suppression. Here, a thermal safety protection strategy based on liquid immersion cooling (LIC) is proposed. The peak temperature of overcharge-induced TR is decreased below 300 °C through boiling heat exchange of FS49, rapidly (3 min) stabilizing the LIB temperature around 49 °C. Simultaneously, critical radicals are captured by FS49 in the combustion chain reaction, reducing emissions of combustible toxic gases by approximately 62.65%. This effectively prevents LIB explosions and secondary re-ignition disasters. Surprisingly, when applied as 1 mm interlayers between cells for a pack with four LIBs, the FS49 not only suppresses the TR propagation but also maintains the adjacent LIB temperature at 53.89 °C. Additionally, it is further demonstrated that the thermal safety of a large-scale 36-cell LIB pack through finite volume method simulations. This strategy can represent a critical step forward in enhancing the safety performance of electric vehicles and grid-scale energy storage systems.

热失控（TR）是高能量密度锂离子电池（LIBs）广泛商业化应用的一个严峻挑战。然而，目前的策略缺乏对极端散热和爆炸抑制的响应性。本文提出了一种基于液浸冷却（LIC）的热安全保护策略。通过FS49的沸腾换热，过充诱导TR的峰值温度降至300℃以下，快速（3 min）将LIB温度稳定在49℃左右。同时，FS49在燃烧链式反应中捕获临界自由基，使可燃有毒气体的排放量减少约62.65%。这有效地防止了LIB爆炸和二次再点火灾难。令人惊讶的是，当FS49作为1毫米的中间层应用于具有四个LIB的电池组时，它不仅抑制了TR的传播，而且还将相邻LIB的温度保持在53.89°C。此外，通过有限体积法模拟，进一步验证了大型36芯LIB电池组的热安全性。这一战略是提高电动汽车和电网规模储能系统安全性能的关键一步。

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引用次数: 0

Model-informed design of microcrack-tolerant cathodes for fast-charging lithium-ion batteries 基于模型的快充锂离子电池微裂纹阴极设计

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-03-01 Epub Date: 2026-02-12 DOI: 10.1016/j.ensm.2026.104985

Woojae Lee , Siwon Kim , Soo Young Yang , Dong Ki Kim , Min-Sik Park , Jong-Won Lee

Boosting the fast-charging capability of lithium-ion batteries (LIBs) is essential for the widespread adoption of electric vehicles. However, nickel-rich layered oxides—the leading cathode materials for high-energy LIBs—suffer from microcracking during fast-charge cycling, resulting in severe capacity fading. Here, we propose an advanced design strategy for mechanically robust bimodal Ni-rich layered oxide cathodes guided by three-dimensional (3D) electrochemo-mechanical modeling. The 3D models, constructed with realistic particle morphologies and electrode microstructures, resolve the evolution of reaction heterogeneity and mechanical stress in the cathodes upon fast charging. Combined with experimental validation, we reveal that the dominant degradation pathway is microcracking of large cathode particles (diameter ∼12 µm) near the separator driven by coupled electrode- and particle-level reaction heterogeneity—namely, sluggish electrolyte-phase ionic transport in densely packed electrodes and diffusion limitation within large particles. To address these issues, we develop a bilayer cathode architecture featuring a ∼10 µm-thick top layer of small single-crystalline particles (∼3 µm). Due to their uniform small size and mechanical robustness, the single-crystalline particles enable fast, homogeneous reactions in the current-concentrated region near the separator and simultaneously act as a mechanical buffer that suppresses localized stress in the underlying large particles. As a result, the bilayer cathode effectively suppresses microcrack formation and subsequent parasitic reactions, delivering a high capacity retention of 76.2% after 300 cycles at 3C, compared with 62.4% for a conventional cathode. This work establishes a practical electrode design principle for enabling durable, high-energy, fast-charging LIBs.

提高锂离子电池（LIBs）的快速充电能力对于电动汽车的广泛采用至关重要。然而，富镍层状氧化物——高能锂离子电池的主要正极材料——在快速充电循环过程中会发生微裂纹，导致严重的容量衰减。在这里，我们提出了一种先进的设计策略，在三维（3D）电化学-力学建模的指导下，机械坚固的双峰富镍层状氧化物阴极。三维模型构建了真实的粒子形态和电极微观结构，解决了快速充电时阴极反应非均质性和机械应力的演变。结合实验验证，我们发现主要的降解途径是由电极和颗粒级反应非均质耦合驱动的分离器附近大阴极颗粒（直径~ 12µm）的微开裂，即密集排列的电极中缓慢的电解质相离子传输和大颗粒内的扩散限制。为了解决这些问题，我们开发了一种双层阴极结构，其特征是有一个约10微米厚的小单晶颗粒（约3微米）顶层。由于其均匀的小尺寸和机械稳健性，单晶颗粒可以在分离器附近的电流集中区域进行快速，均匀的反应，同时作为机械缓冲，抑制底层大颗粒的局部应力。因此，双层阴极有效地抑制了微裂纹的形成和随后的寄生反应，在3C下循环300次后，其容量保持率高达76.2%，而传统阴极的容量保持率为62.4%。这项工作建立了一个实用的电极设计原则，使耐用，高能量，快速充电的lib。

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