Energy Storage Materials最新文献_第8页

Failure mechanisms and current collector design for sodium metal anodes: From thermodynamic-kinetic coupling to structural-functional optimization 金属钠阳极的失效机制和集流器设计：从热力学-动力学耦合到结构-功能优化

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-13 DOI: 10.1016/j.ensm.2026.104898

Saisai Qiu, Haolin Zhu, Qiang Wu, Shijie Cheng, Jia Xie

Sodium metal anodes (SMAs) present a compelling pathway toward next-generation high-energy-density batteries but face persistent challenges such as dendrite growth, low Coulombic efficiency, and safety concerns. These issues originate from the strong coupling between thermodynamic instability and kinetic limitations inherent to sodium metal. To address these fundamental coupling, this review establishes a unified framework linking “thermodynamic–kinetic coupling” as the failure origin to “structure–function optimization” as the solution core. We systematically dissect the synergistic interplay between thermodynamic and kinetic factors governing SMA failure, and highlight the pivotal role of advanced current collectors as a core mitigation strategy. Recent progress in 3D porous architectures, surface functionalization, and gradient engineering is comprehensively surveyed, demonstrating how these approaches synergistically regulate nucleation thermodynamics and ion transport kinetics. The discussion extends to anode‑free sodium metal batteries (AF-SMBs), where optimized current collectors are indispensable. By establishing a coherent framework linking thermodynamic-kinetic coupling to structural and functional optimization, this work lays a foundation for developing safe, durable, and high-performance sodium metal batteries.

金属钠阳极（sma）为下一代高能量密度电池的发展提供了一条引人注目的途径，但也面临着诸如枝晶生长、低库仑效率和安全问题等持续的挑战。这些问题源于金属钠固有的热力学不稳定性和动力学限制之间的强耦合。为了解决这些基本的耦合问题，本文建立了以“热力学-动力学耦合”为失效根源，以“结构-功能优化”为解决核心的统一框架。我们系统地剖析了控制SMA失效的热力学和动力学因素之间的协同相互作用，并强调了先进集流器作为核心缓解策略的关键作用。本文全面综述了三维多孔结构、表面功能化和梯度工程的最新进展，展示了这些方法如何协同调节成核热力学和离子传输动力学。讨论扩展到无阳极钠金属电池（af - smb），其中优化的集流器是必不可少的。通过建立一个将热力学-动力学耦合与结构和功能优化联系起来的连贯框架，本工作为开发安全、耐用和高性能的钠金属电池奠定了基础。

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引用次数: 0

A Controversial Topic on Oxygen Crosstalk Effects in Aprotic Lithium-Oxygen Batteries 非质子锂氧电池中氧串扰效应的争议话题

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-12 DOI: 10.1016/j.ensm.2026.104899

Zhiwei Zhao, Yantao Zhang, Limin Guo, Zhangquan Peng

Aprotic lithium-oxygen (Li-O2) batteries represent a critical enabling technology in tomorrow’s portfolio of clean energy solutions due to their unparalleled theoretical energy density among existing battery chemistries. The solid–electrolyte interphase (SEI) formed on lithium metal anode (LMA) surfaces plays a crucial role in unlocking their energy capabilities. Over recent years, the oxygen crosstalk phenomenon at the LMA/electrolyte interface has emerged as a significant yet underexplored determinant of SEI stability and battery performance. In this contribution, three potential oxygen crosstalk effects on SEI formation pathways in the literature, are first recapitulated. Subsequently, a study paradigm is presented to achieve unified understandings of oxygen crosstalk and develop rational design strategies for stable LMA, which involves decoupling and probing complex oxygen crosstalk chemistries through well-designed model interfaces and in situ spectroscopies. Finally, future directions and perspectives are proposed, with a call to the wider research community to explore the significant effect of crosstalk chemistries beyond Li-O2 batteries and extend to emerging electrochemical devices.

非质子锂氧（Li-O2）电池由于其在现有电池化学成分中具有无与伦比的理论能量密度，因此代表了未来清洁能源解决方案组合中的关键使能技术。在锂金属阳极（LMA）表面形成的固体-电解质界面（SEI）在释放其能量能力方面起着至关重要的作用。近年来，LMA/电解质界面上的氧串扰现象已成为影响SEI稳定性和电池性能的重要因素，但尚未得到充分研究。在这一贡献中，首先概述了文献中三种潜在的氧串扰对SEI形成途径的影响。随后，提出了一种研究范式，以实现对氧串扰的统一理解，并制定稳定LMA的合理设计策略，其中包括通过精心设计的模型界面和原位光谱进行解耦和探测复杂的氧串扰化学。最后，提出了未来的方向和观点，呼吁更广泛的研究界探索Li-O2电池之外的串声化学的重要影响，并扩展到新兴的电化学装置。

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引用次数: 0

Recycling of lead-acid batteries: A review 铅酸蓄电池回收利用研究进展

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-12 DOI: 10.1016/j.ensm.2026.104895

Hongya Wang , Xiang Chen , Muya Cai , Shiyu Wang , Fengyin Zhou , Yongxin Wu , Danfeng Wang , Haochen Wang , Bingbing Wang , Fangzhao Pang , Junmin Peng , Weiguo Huang , Xiaowei Liu , Dihua Wang , Huayi Yin

Lead-acid batteries (LABs), due to their mature technology, high safety, low cost, and wide range of applications, remain one of the most popular secondary power sources today, particularly in electric bicycles and automotive starter-lighting-ignition systems. However, the ubiquity of LABs has precipitated a massive accumulation of end-of-life waste, resulting in an urgent imperative for robust recycling frameworks to mitigate resource depletion and environmental toxicity. This review presents a holistic analysis of the LAB ecosystem, bridging the gap between manufacturing advancements and closed-loop reclamation. We critically synthesize the evolution of LAB technology, detailing mainstream and emerging manufacturing paradigms, while comprehensively outlining failure mechanisms and repair strategies. Special emphasis is placed on state-of-the-art recycling methodologies, providing a granular evaluation of component-specific recovery (including paste, grids, separators, and electrolytes). Furthermore, we integrate a life cycle and economic assessment to rigorously quantify carbon footprints, environmental impacts, and economic viability. By reviewing the entire life cycle of LABs—from raw materials to waste—we aim to provide insights into the research directions and focal points at each stage, offering perspectives and guidance for the future of LAB research in both the scientific and industrial communities.

铅酸电池由于其成熟的技术、高安全性、低成本和广泛的应用，仍然是当今最受欢迎的二次电源之一，特别是在电动自行车和汽车起动-照明-点火系统中。然而，无处不在的实验室导致了大量报废废物的积累，导致迫切需要强有力的回收框架来减轻资源枯竭和环境毒性。本文对LAB生态系统进行了全面分析，弥合了制造业进步和闭环回收之间的差距。我们批判性地综合了LAB技术的发展，详细介绍了主流和新兴的制造范式，同时全面概述了故障机制和修复策略。特别强调的是最先进的回收方法，提供特定组件回收的颗粒评估（包括粘贴，网格，分离器和电解质）。此外，我们整合了生命周期和经济评估，严格量化碳足迹、环境影响和经济可行性。通过回顾实验室从原材料到废物的整个生命周期，我们旨在提供每个阶段的研究方向和重点的见解，为未来科学和工业界的实验室研究提供观点和指导。

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引用次数: 0

Representation learning accelerates the development of models for Li-ion battery health diagnostics and prognostics 表征学习加速了锂离子电池健康诊断和预测模型的发展

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-12 DOI: 10.1016/j.ensm.2026.104897

Quanquan Zhang, Mingyu Yang, Guanxi Sun, Yue Xiang, Shitong Wang, Junying Zhang, Shuangqi Li

In recent years, the evolution of Li-ion battery material components, cell architectures, and application scenarios has posed significant challenges for the rapid adaptation of battery management systems (BMS). Accurate health diagnostics and prognostics are fundamental to reliable battery operation. However, traditional approaches based on empirical equations, physical models, or handcrafted features often suffer from limited generalization, heavy data demands, and time-consuming development. Representation learning, a major advancement in deep learning, is emerging as a powerful tool to accelerate battery health modeling. Under novel chemistries and unseen operating conditions, it mitigates data scarcity through generative learning and enables rapid model adaptation via transfer learning, which was overlooked in earlier reviews. We systematically summarize representation learning architectures tailored for battery data, highlight their applications in data augmentation and cross-domain transfer, and further identify key challenges and future opportunities in data privacy, multimodal information integration, and model interpretability. Overall, representation learning establishes a solid foundation for the efficient development of next-generation intelligent BMS.

近年来，锂离子电池材料成分、电池结构和应用场景的发展对电池管理系统（BMS）的快速适应提出了重大挑战。准确的健康诊断和预测是电池可靠运行的基础。然而，基于经验方程、物理模型或手工特征的传统方法往往泛化有限、数据需求大、开发耗时长。表征学习是深度学习的一个重大进展，它正在成为加速电池健康建模的强大工具。在新的化学物质和不可见的操作条件下，它通过生成式学习减轻了数据稀缺性，并通过迁移学习实现了快速模型适应，这在早期的评论中被忽视了。我们系统地总结了为电池数据量身定制的表征学习架构，重点介绍了它们在数据增强和跨域传输中的应用，并进一步确定了数据隐私、多模态信息集成和模型可解释性方面的关键挑战和未来机遇。总体而言，表征学习为下一代智能BMS的高效开发奠定了坚实的基础。

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引用次数: 0

Ameliorating the Ionic Transport Behavior in Nonflammable Phosphate towards High-Energy and Safe Lithium Metal Batteries 改善不可燃磷酸盐对高能安全锂金属电池的离子传输行为

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-12 DOI: 10.1016/j.ensm.2026.104896

Ya-Fang Wang, Yuan Liu, Xiang-Dan Zhang, Xiong-Wei Wu, Yi-Lei Zhang, Hai-Yan Hu, Qiang Ma, Zhen-Ling Wang, Yao Xiao

In virtue of the wide electrochemical window and superior flame-retarded ability, phosphate electrolytes are widely employed as transport media in high-voltage lithium metal batteries. Unfortunately, the strong interaction of Li+-phosphates leads to inefficient Li+ transport. Furthermore, the uncontrollable electrode-electrolyte interphase originated from the labile interfacial species retards the stable cycling of lithium metal batteries during operation. Herein, in-built high dielectric dissociated reservoir and functional interfacial regulation additive were designed to boost the dissociation ability of Li+ and stabilize the bidirectional electrode-electrolyte interfaces. Benefitting from the strong desolvated kinetic of nanowires and excellent interfacial regulation function of lithium nitrate, the continuous Li+ transport pathway and homogeneous bidirectional electrode-electrolyte interfaces were constructed, preventing the lithium metal anode and high-nickel cathode from persistent reactive with phosphate electrolytes, revealed by theoretical calculation and ex-situ characterization. Attributed to the guided ion transfer pathway and oriented artificial solid electrolyte interface, the Li||Li symmetrical batteries exhibit excellent cycling stability of above 1000h at 2 mA cm−2 and 2 mAh cm−2. The Li||LiNi0.8Co0.1Mn0.1O2 (NCM811) battery shows more than 90% capacity retention after 200 cycles at 1C. This strategy holds great promising for developing advanced electrolytes in other advanced electrochemical storage devices.

磷酸电解质由于具有较宽的电化学窗口和优异的阻燃性能，被广泛用作高压锂金属电池的输运介质。不幸的是，Li+-磷酸盐的强相互作用导致Li+输运效率低下。此外，不稳定的界面物质导致的电极-电解质界面相不可控，阻碍了锂金属电池在运行过程中的稳定循环。为此，设计了内置高介电离解储层和功能界面调节添加剂，以提高Li+的离解能力，稳定双向电极-电解质界面。理论计算和非原位表征表明，利用纳米线强大的脱溶动力学和硝酸锂优异的界面调节功能，构建了连续的Li+传输通道和均匀的双向电极-电解质界面，防止了锂金属阳极和高镍阴极与磷酸盐电解质的持续反应。锂||锂对称电池在2ma cm - 2和2mah cm - 2下具有1000h以上的循环稳定性，这主要归功于离子转移路径和定向人造固体电解质界面。Li||LiNi0.8Co0.1Mn0.1O2 （NCM811）电池在1C下循环200次后容量保持率超过90%。该策略对开发先进电解质用于其他先进的电化学存储装置具有很大的前景。

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引用次数: 0

Steering Zn(ClO4)2 electrolyte: Trifunctional polycationic artificial interphase for Wide-Temperature Ah-level Zn-I2 pouch cells 转向Zn(ClO4)2电解质：宽温度ah级Zn- i2袋状电池的三功能多阳离子人工界面

IF 20.2 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-12 DOI: 10.1016/j.ensm.2026.104900

Xueying Su , Shunyao Li , Zhenxin Chen , Hengrui Guo , Zihao Liu , Yutong Wang , Duo Chen , Zaijun Cheng , Tiefeng Liu , Hao Luo

The concurrent improvement of interfacial stability and Zn²⁺ transport kinetics across a broad temperature window continues to challenge aqueous zinc-ion batteries (AZIBs). Herein, a trifunctional polycationic interfacial layer (PDDA-TFSI, PTF) is introduced to broaden the advantages of the Zn(ClO₄)₂ electrolyte beyond its unique low-temperature tolerance. Specifically, while the hydrophobic architecture (TFSI⁻) of PTF locally disrupts the hydrogen-bond network of free water molecules, its uniformly distributed cationic sites (N⁺−R₄) guarantee the efficient anchoring of corrosive ClO₄⁻, fundamentally mitigating the strong oxidative propensity under high water activity particularly at ambient temperatures. Zn²⁺ desolvation and migration are facilitated by decoupling bulk and interfacial processes, with consequent improvement in transport kinetics and enhancement of the rate capability. The PTF@Zn electrode exhibits stable Zn plating/stripping for over 7000 h at 0.5 mA cm⁻² and −30 °C. The PTF@Zn||AC@I₂ full cell exhibits a low-capacity decay rate of merely ∼0.006% per cycle over 3000 cycles at 2.0 A g⁻¹ over a wide temperature range from –30 °C to 25 °C. Notably, the pouch cell delivers 800 mAh capacity while retaining 92.3% after 100 cycles at –30 °C. This approach customizes a route to stabilize zinc anodes for wide-temperature operation, offering valuable insights into advanced AZIBs.

界面稳定性和Zn2+在宽温度窗内传输动力学的同时提高，继续挑战着水性锌离子电池（azib）。本文引入了一种三功能聚阳离子界面层（pda - tfsi， PTF），以扩大Zn(ClO4)2电解质在其独特的低温耐受性之外的优势。具体来说，虽然PTF的疏水结构（TFSI−）局部破坏了自由水分子的氢键网络，但其均匀分布的阳离子位点（N+−R4）保证了腐蚀性ClO4−的有效锚定，从根本上减轻了高水活度（特别是在环境温度下）下的强氧化倾向。解耦体和界面过程促进了Zn2+的脱溶和迁移，从而改善了输运动力学和提高了速率能力。PTF@Zn电极在0.5 mA cm - 2和- 30 °C下表现出稳定的镀锌/剥离超过7000小时。在-30°C至25°C的宽温度范围内，在2.0 a g - 1下，PTF@Zn||AC@I2全电池在3000次循环中显示出低容量衰减率，每周期仅为~ 0.006%。值得注意的是，袋式电池在-30°C下循环100次后，可提供800毫安时的容量，同时保持92.3%的容量。这种方法定制了一种稳定锌阳极的途径，用于宽温度操作，为先进的azib提供了有价值的见解。

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引用次数: 0

Unfolding Carbon Layers to Engineer Interstitial Topological Space for Hard Carbon Anodes in Low-Temperature Sodium-Ion Batteries 展开碳层以设计低温钠离子电池硬碳阳极的间隙拓扑空间

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-11 DOI: 10.1016/j.ensm.2026.104894

Ru Wang, Yaxin Chen, Zhipeng Cao, Liluo Shi, Nannan Guo, Xia Qiu, Yirong Wang, Luxiang Wang, Quanchao Zhuang, Zhicheng Ju

The sluggish Na⁺ diffusion within hard carbon (HC) anodes remains the key bottleneck restricting the low-temperature operation of sodium-ion batteries (SIBs). While previous studies have mainly optimized closed-pore structures, the critical role of interdomain interconnectivity in governing ion transport has been largely overlooked. Here, we develop a pillar-supporting strategy to unfold carbon layers and construct interstitial topological diffusion networks, enabling efficient bulk Na⁺ transport under low temperatures. The reconstructed hard carbon (P-HC) exhibits a loosely packed architecture with enlarged carbon layers (∼4-5 nm) and closed pores (∼9 Å), compared to conventional HC (∼1-2 nm layers, 5.7 Å pores). Modeling further reveals that the interstitial spacing of P-HC (1.66 nm) is nearly twice that of HC (0.83 nm), providing open topological pathways that effectively facilitate Na⁺ diffusion. Consequently, P-HC delivers a reversible capacity of 403.5 mAh g^-1 with an initial Coulombic efficiency of 93% at 25 °C and maintains 268.5 mAh g^-1 at -20 °C, far exceeding HC (47 mAh g^-1). This work introduces the concept of interstitial topology beyond conventional closed-pore models, offering fresh insights into designing advanced carbon anodes for SIBs operating in extreme environments.

硬碳（HC）阳极内Na+扩散缓慢仍然是制约钠离子电池低温运行的关键瓶颈。虽然以往的研究主要是优化闭孔结构，但在很大程度上忽视了域间互连在控制离子输运中的关键作用。在这里，我们开发了一种支柱支撑策略来展开碳层并构建间隙拓扑扩散网络，使Na⁺在低温下高效传输。与传统的硬碳（1-2纳米层，5.7 Å孔）相比，重建的硬碳（P-HC）具有松散的结构，具有扩大的碳层（~ 4-5 nm）和封闭的孔隙（~ 9 Å）。模型进一步表明，P-HC的间隙（1.66 nm）几乎是HC （0.83 nm）的两倍，提供了开放的拓扑通路，有效促进Na+扩散。因此，P-HC在25°C时提供403.5 mAh g-1的可逆容量，初始库仑效率为93%，在-20°C时保持268.5 mAh g-1，远远超过HC （47 mAh g-1）。这项工作在传统的闭孔模型之外引入了间隙拓扑的概念，为在极端环境中工作的sib设计先进的碳阳极提供了新的见解。

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引用次数: 0

Thermodynamically Tuned Element Diffusion Enables Ultrafast Kinetics and Structural Reversibility in Grain-Refined LiMn0.8Fe0.2PO4 Cathodes for High-Energy-Density Batteries 热动力学调谐元素扩散实现高能量密度电池晶粒细化LiMn0.8Fe0.2PO4阴极的超快动力学和结构可逆性

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-10 DOI: 10.1016/j.ensm.2026.104893

Yuanpeng Cao, Wenhui Tu, Jingjing He, Jianguo Duan, Runlin Li, Xinyu Zhang, Chenyi Huang, Liqi Li, Yingjie Zhang, Yuanbing Wang, Peng Dong, Xianshu Wang, Ding Wang

Olivine-structured LiMn_1–xFe_xPO₄ phosphates have emerged as one of the most promising cathodes for Lithium-ion batteries owing to their high energy density, low cost, and non-toxicity. However, the intrinsic electronic/ionic insulating properties and the Jahn-Teller effect limit their rate performance and reversibility. Here, we propose grain-refining and fast-ion-conductive epitaxial layer regulation via a thermodynamics-sanctified multi-cationic interaction strategy to booming Li-storage kinetics and reversibility of LiMn_0.8Fe_0.2PO₄ cathodes. Both computational and experimental results demonstrate that the thermodynamically driven enrichment of V and Ti on the surfaces of V-Ti-Mg co-modified LiMn_0.8Fe_0.2PO₄ (LMFP-VTM) promotes the particle refinement and the formation of quasi-amorphous epitaxial layers. Particle nanometrization assisted with coherent multi-ion quasi-disordered epitaxial layers facilitate the Li⁺ transport kinetics strikingly, as well as mitigate Jahn-Teller effect-driven pernicious structural degradation. The optimized LMFP-VTM cathode achieves 151.6 mAh g^-1 initial capacity at 0.1 C and retains 93.5 mAh g^-1 at 15 C. It exhibits exceptional cyclability with 95.4 and 82.5% capacity retentions after 1000 cycles (1 C) and 3000 cycles (5 C), respectively. The findings in this work expanded the perspective on the structural engineering of high energy density olivine-structured cathode materials with ultrafast kinetics.

橄榄石结构的LiMn1-xFexPO4磷酸盐由于其高能量密度、低成本和无毒性而成为锂离子电池最有前途的阴极之一。然而，固有的电子/离子绝缘性能和扬-泰勒效应限制了它们的速率性能和可逆性。在这里，我们提出了晶粒细化和快速离子导电外延层调节，通过一个热力学的多阳离子相互作用策略，以提高锂存储动力学和LiMn0.8Fe0.2PO4阴极的可逆性。计算和实验结果表明，V-Ti- mg共改性LiMn0.8Fe0.2PO4 （LMFP-VTM）表面V和Ti的热驱动富集促进了颗粒细化和准非晶外延层的形成。粒子纳米化辅助的相干多离子准无序外延层显著地促进了Li+的输运动力学，并减轻了Jahn-Teller效应驱动的有害结构降解。优化后的LMFP-VTM阴极在0.1℃时达到151.6 mAh g-1的初始容量，在15℃时保持93.5 mAh g-1，在1000次循环（1℃）和3000次循环（5℃）后分别保持95.4和82.5%的容量。本工作的发现拓展了高能量密度橄榄石结构超快动力学正极材料结构工程的研究前景。

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引用次数: 0

Large Battery Model for Multi-State Co-estimation and Intelligent Recommendation using Mixed Data Sources 基于混合数据源的多状态联合估计和智能推荐的大电池模型

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-10 DOI: 10.1016/j.ensm.2026.104892

Zhen Zhang, Yunlong Shang, Xiangjun Li, Zeyu Cheng

Accurate, efficient, and robust multi-state co-estimation can empower more advanced battery management systems, essential for enhancing the intelligence and safety of lithium-ion batteries. Recently, the paradigm driven by artificial intelligence and big data is envisioned as a promising solution; however, it falls short due to entrenched constraints arising from redundant isolated training, complex feature engineering, and data diversity. Here, we propose a highly generalized and automatic feature mining technology to construct a multi-modal input architecture that integrates both data and text information, without stringent prerequisites. Thereafter, we develop and validate a large battery model that fundamentally achieves reliable pooled training using mixed data sources for multi-state co-estimation. Furthermore, to transform the proposed framework into a complete “perception + decision-making” system, this work designs a generative recommender to offer drivers/users comprehensive suggestions and guidance. Nearly 260,000 cycling samples from 433 cells in ten large-scale datasets support this work. The validation results indicate that over 90% of the samples exhibit absolute errors below 1.8% (with over 98% below 2.6%), underscoring the superiority, generalizability, and reliability of the proposed framework. Various ablation experiments further corroborate that the large battery model can precisely identify data sources and decompose multi-task learning, thereby sustaining excellent performance. This work highlights the potential of multi-modal architectures, pooled training, and larger models in domain-specific multi-task learning.

准确、高效、稳健的多状态联合估计可以为更先进的电池管理系统提供支持，这对于提高锂离子电池的智能和安全性至关重要。最近，人工智能和大数据驱动的范式被认为是一个很有前途的解决方案；然而，由于冗余的孤立训练、复杂的特征工程和数据多样性所产生的根深蒂固的限制，它的能力不足。在这里，我们提出了一种高度一般化和自动化的特征挖掘技术来构建一个集成数据和文本信息的多模态输入架构，而不需要严格的先决条件。此后，我们开发并验证了一个大型电池模型，该模型使用混合数据源进行多状态共估计，从根本上实现了可靠的池化训练。此外，为了将提出的框架转化为一个完整的“感知 + 决策”系统，本工作设计了一个生成式推荐器，为驾驶员/用户提供全面的建议和指导。来自10个大型数据集的433个细胞的近26万个循环样本支持这项工作。验证结果表明，超过90%的样本的绝对误差低于1.8%（超过98%的样本低于2.6%），强调了所提出框架的优越性、通用性和可靠性。各种烧蚀实验进一步证实了大电池模型能够精确识别数据源并分解多任务学习，从而保持优异的性能。这项工作强调了在特定领域的多任务学习中，多模式架构、集合训练和更大模型的潜力。

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引用次数: 0

Monitoring Gas Evolution during Ageing of Industrial Supercapacitors Studied by in situ GC-MS 用原位气相色谱-质谱法监测工业超级电容器老化过程中的气体演化

IF 20.4 1区材料科学 Q1 CHEMISTRY, PHYSICAL

Energy Storage Materials

Pub Date : 2026-01-10 DOI: 10.1016/j.ensm.2026.104888

Mihkel Kaarel Raidal, Rebecka Kost, Taron Makaryan, Andrea Balducci

Understanding gas evolution during the ageing of electrical double layer capacitors (EDLCs) is critical for improving long-term performance and safety. However, direct gas analysis in industrial-scale cells has been hindered by their sealed design, complex internal structure, and small gas volumes. This study aimed to develop and validate a novel in situ gas chromatography–mass spectrometry (GC–MS) method capable of analysing gas evolution in intact, industrial-format supercapacitor cells under realistic ageing conditions. A custom stainless-steel jig with a detachable gas extraction piece was designed to enable controlled, on-demand sampling from cylindrical EDLCs undergoing an accelerated floating ageing protocol at 3.0 V and 65°C. The system was evaluated for mechanical stability and non-intrusiveness through electrochemical performance metrics and internal pressure monitoring, while extracted gases were analysed qualitatively by GC–MS. The integrated sampling hardware maintained normal ageing behaviour, with capacitance fading, coulombic efficiency, and logarithmic pressure growth comparable to unmodified cells. The developed in situ GC–MS technique bridges the gap between model-cell studies and real supercapacitor devices, enabling direct correlation of molecular-level gas formation with macroscopic ageing behaviour. This reliable approach provides a versatile platform for investigating alternative electrolytes, electrode materials, and ageing conditions, paving the way for deeper mechanistic understanding of supercapacitor degradation.

了解双电层电容器（edlc）老化过程中的气体演化对于提高其长期性能和安全性至关重要。然而，由于密封设计、复杂的内部结构和较小的气体体积，工业规模电池的直接气体分析一直受到阻碍。本研究旨在开发和验证一种新的原位气相色谱-质谱（GC-MS）方法，该方法能够在实际老化条件下分析完整的工业超级电容器电池中的气体演化。定制的不锈钢夹具带有可拆卸的气体提取件，可以在3.0 V和65°C的加速浮动老化协议下对圆柱形edlc进行受控的按需采样。通过电化学性能指标和内部压力监测评估了该系统的机械稳定性和非侵入性，同时通过GC-MS对提取的气体进行了定性分析。集成的采样硬件保持了正常的老化行为，电容衰减、库仑效率和对数压力增长与未修改的电池相当。开发的原位GC-MS技术弥合了模型细胞研究和真实超级电容器设备之间的差距，使分子水平的气体形成与宏观老化行为直接相关。这种可靠的方法为研究替代电解质、电极材料和老化条件提供了一个通用的平台，为深入了解超级电容器退化的机理铺平了道路。

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