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Electrochemical Modeling and Degradation Analysis of Lithium-Ion Batteries in High Temperature Environments 高温环境下锂离子电池的电化学建模与降解分析
Pub Date : 2025-10-17 DOI: 10.1002/bte2.20250043
Fei Chen, Fan Yang, Haoran Chu, Jiatong Xu, Kaiyi Yang, Justice D. Akoto, Ali Haider, Xingrui Wang, Jie Yang, Xinhua Liu, Zhiming Feng, Rui Tan

Simulation models are of great importance in understanding the complexities of the internal electrochemical processes within batteries, aiding in design optimization and advancing energy storage technologies. One of the central challenges lies in predicting battery lifespan and elucidating side reactions under extreme operating conditions. This study aims to design an electrochemical model that considers multiple side reactions to predict the cycle life of lithium-ion batteries in high temperature environments. First, a basic simulation framework is established using a simplified electrochemical-mechanical coupling model. Subsequently, multiscale characterization of aged batteries is performed to identify five types of side reactions, encompassing phenomena such as solid electrolyte interphase (SEI) growth, cracking of negative electrode particles, electrolyte oxidation and decomposition/deposition of active materials. A comprehensive battery life prediction model is constructed by modeling these side reactions. Finally, the accuracy of the life prediction is validated using high temperature cycling data. The conclusions reveal that electrolyte decomposition and the loss of active material are the primary causes of battery degradation under high temperature conditions.

仿真模型对于理解电池内部电化学过程的复杂性,帮助设计优化和推进储能技术具有重要意义。其中一个核心挑战在于预测电池寿命和阐明极端操作条件下的副反应。本研究旨在设计一个考虑多种副反应的电化学模型来预测锂离子电池在高温环境下的循环寿命。首先,利用简化的电化学-力学耦合模型建立了基本的仿真框架。随后,对老化电池进行了多尺度表征,以确定五种类型的副反应,包括固体电解质间相(SEI)生长、负极颗粒开裂、电解质氧化和活性物质分解/沉积等现象。通过对这些副反应进行建模,建立了一个全面的电池寿命预测模型。最后,利用高温循环数据验证了寿命预测的准确性。结果表明,在高温条件下,电解液的分解和活性物质的损失是导致电池退化的主要原因。
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引用次数: 0
Investigation Into the Properties of γ-Valerolactone and γ-Butyrolactone Imide-Based Electrolytes for Lithium-Ion Batteries 锂离子电池用γ-戊内酯和γ-丁内酯亚胺基电解质性能研究
Pub Date : 2025-10-17 DOI: 10.1002/bte2.20250034
Khai Shin Teoh, Wanja Timm Schulze, Zihan Song, Alexander Croy, Juan Luis Gómez Urbano, Stefanie Gräfe, Andrea Balducci

This study presents a detailed comparative study of lactone-based electrolytes (γ-valerolactone, GVL and γ-butyrolactone, GBL) combined with lithium imide-based salts, namely lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) and lithium bis(fluoromethanesulfonyl)imide (LiFSI). Propylene carbonate is employed as a reference electrolyte solvent. The physicochemical properties of these electrolyte systems are determined experimentally and further calculated using our developed computational model. Besides, in-silico investigations are used to reveal valuable insights into the molecular interactions of the electrolyte components, such as self-diffusion coefficients and radial distribution functions. Furthermore, the suitability of lactone-based electrolytes for electrochemical applications is demonstrated by their promising rate capability and cycling stability over 200 cycles in graphite half-cells, especially with 1 M LiTFSI and 2 wt% vinylene carbonate, together with their favorable performance on lithium iron phosphate. An excellent capacity retention achieved in a full-cell configuration (> 80% after 200 cycles) further validates the potential of lactones as battery solvent alternatives, with GVL standing out due to its bio-based origin.

本研究对内酯基电解质(γ-戊内酯,GVL和γ-丁内酯,GBL)与亚胺锂基盐,即双(三氟甲磺酰基)亚胺锂(LiTFSI)和双(氟甲磺酰基)亚胺锂(LiFSI)结合进行了详细的比较研究。采用碳酸丙烯酯作为基准电解质溶剂。这些电解质体系的物理化学性质是通过实验确定的,并使用我们开发的计算模型进一步计算。此外,硅研究还揭示了电解质组分的分子相互作用,如自扩散系数和径向分布函数。此外,内酯基电解质具有良好的电化学性能和在石墨半电池中超过200次循环的稳定性,特别是在1 M LiTFSI和2 wt%碳酸丙烯酯中,以及在磷酸铁锂上的良好性能,证明了内酯基电解质的适用性。在全电池配置中获得了出色的容量保持率(200次循环后达到80%),进一步验证了内酯作为电池溶剂替代品的潜力,其中GVL因其生物基起源而脱颖而出。
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引用次数: 0
Amorphous Sub-Stoichiometric Silicon Carbide (a-SiCx) Particles From the Gas Phase for Battery Applications 用于电池的非晶亚化学计量碳化硅(a-SiCx)气相颗粒
Pub Date : 2025-09-24 DOI: 10.1002/bte2.20250041
Moritz Loewenich, Jędrzej Kondek, Michael Ryan Hansen, Hartmut Wiggers

Capacity fading during cycling remains a significant challenge for silicon-based anode materials in Li-ion batteries. Amorphous, sub-stoichiometric silicon carbide (a-SiCx) nanoparticles have proven to be more stable than pure silicon, albeit with lower lithiation capacities. The incorporation of carbon during the nanoparticle synthesis is highly effective in the suppression of crystalline phases during both synthesis and cycling. In this study, a-SiCx materials with varying carbon concentrations (up to 22 wt.%) were produced via gas-phase synthesis in a hot-wall reactor. The primary objective is to understand the mechanism of carbon incorporation into the silicon particles, and secondly its impact on material properties and battery performance. Based on extensive materials science investigations and NMR analyses, we have determined that carbon is incorporated together with hydrogen, which further promotes amorphization. Furthermore, cycling analysis shows a strongly increased stability with 85% retention after 200 cycles for materials with more than 10 wt.% carbon, probably mainly due to a reduced buildup of internal resistances and reduced volume expansion. Furthermore, crystalline Si-Li-phases cannot be formed in this material during lithiation enabling deep lithiations, and Coulombic efficiency is increased. These results suggest that a-SiCx is a promising alternative to pure silicon as an anode material.

循环过程中的容量衰减是锂离子电池中硅基负极材料面临的一个重大挑战。非晶亚化学计量碳化硅(a-SiCx)纳米颗粒已被证明比纯硅更稳定,尽管其锂化能力较低。在纳米颗粒合成过程中,碳的掺入对合成和循环过程中晶体相的抑制都是非常有效的。在这项研究中,a-SiCx材料具有不同的碳浓度(高达22wt)。%)是在热壁反应器中气相合成的。主要目的是了解碳掺入硅颗粒的机理,其次是其对材料性能和电池性能的影响。基于广泛的材料科学研究和核磁共振分析,我们已经确定碳与氢结合在一起,这进一步促进了非晶化。此外,循环分析表明,超过10重量的材料在200次循环后,稳定性显著提高,保留率为85%。%的碳,可能主要是由于减少了内阻的积累和减少了体积膨胀。此外,在锂化过程中,该材料不能形成晶体si - li相,从而实现深度锂化,并提高了库仑效率。这些结果表明,a- sicx是一种很有希望替代纯硅作为阳极材料的材料。
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引用次数: 0
Cover Image, Volume 4, Issue 5, September 2025 封面图片,第四卷,第五期,2025年9月
Pub Date : 2025-09-07 DOI: 10.1002/bte2.12195

Front Cover: Aqueous rechargeable zinc-iodine batteries have emerged as a promising energy storage solution. In article number BTE.20250017, Fei Huang, Weihua Xu and Huibing He provide an in-depth summary and analysis of the current challenges and solutions facing these batteries. The core of their research focuses on the recent strategies for optimizing aqueous zinc-iodine batteries, including accelerating iodine conversion, promoting uniform zinc ion deposition, inhibiting multi-iodide shuttling, lowering energy barriers, electrostatic shielding, and bidentate coordination complexation. This review aims to provide insights and advance the real-world applications of aqueous zinc-iodine batteries.

封面:水可充电锌-碘电池已经成为一种很有前途的能源存储解决方案。在BTE.20250017号文章中,黄飞、徐卫华、何惠兵对这些电池当前面临的挑战和解决方案进行了深入的总结和分析。他们的研究重点是优化水基锌碘电池的最新策略,包括加速碘转化、促进锌离子均匀沉积、抑制多碘离子穿梭、降低能量垒、静电屏蔽和双齿配位络合。本文综述的目的是提供见解和推进实际应用的水锌碘电池。
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引用次数: 0
Optimizing Hard Carbon Anodes for Sodium-Ion Batteries: Effects of Pre-Treatment and Post-Treatment Techniques 钠离子电池硬碳阳极的优化:前处理和后处理技术的影响
Pub Date : 2025-09-03 DOI: 10.1002/bte2.20250054
Muetaz Mohammed, Mohammad M. Hossain, Md Abdullah Al Bari

Hard carbon (HC), an amorphous carbon-based material, is a promising anode for sodium-ion batteries (SIBs) due to its sustainability and electrochemical performance. Direct carbonization offers a simple and energy-efficient synthesis route with relatively high initial coulombic efficiency (ICE), though often at the expense of capacity. To overcome this limitation, both pre-treatment and post-treatment strategies have been developed to enhance HC properties. pre-treatment methods modify structural characteristics during synthesis by increasing structural disorder, surface activity, and defect density. In contrast, post-treatment methods improve the electrochemical behavior of the final product, yet remain comparatively underexplored. These two approaches serve complementary functions and, when integrated, offer potential for optimizing performance. This review discusses the methodologies, benefits, limitations, and impact of various pre- and post-treatment strategies for HC anodes in SIBs. Advancing understanding in this area is essential for the development of high-performance and sustainable SIB technologies.

硬碳(HC)是一种非晶碳基材料,由于其可持续性和电化学性能,是一种很有前途的钠离子电池负极材料。直接碳化提供了一种简单、节能的合成途径,具有较高的初始库仑效率(ICE),但往往以牺牲产能为代价。为了克服这一限制,人们开发了预处理和后处理策略来提高HC的性能。预处理方法通过增加结构无序性、表面活性和缺陷密度来改变合成过程中的结构特征。相比之下,后处理方法改善了最终产品的电化学行为,但相对来说还没有得到充分的探索。这两种方法具有互补的功能,如果集成在一起,就有可能优化性能。这篇综述讨论了sib中HC阳极的各种前后处理策略的方法、益处、局限性和影响。推进对这一领域的理解对于开发高性能和可持续的SIB技术至关重要。
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引用次数: 0
Machine Learning Analysis of Hydrothermally Synthesized LiFePO4 for Lithium-Ion Battery 水热合成锂离子电池用LiFePO4的机器学习分析
Pub Date : 2025-08-31 DOI: 10.1002/bte2.20250021
Nita U. Kalugade, Digambar S. Sawant, Heena S. Mulla, Sandesh V. Gaikwad, Charudatta S. Pawar, Deepak P. Dubal, Gaurav M. Lohar

Rechargeable lithium-ion batteries (LIBs) have quickly become one of the most popular energy storage sources for electronic devices. The LIB cathode significantly affects the battery's energy density, safety, lifespan, and cost, and LIBs exhibit better chemical and thermal stability. Among various cathode materials, lithium iron phosphate (LiFePO4) has gained significant attention due to its excellent safety, low toxicity, cost-effectiveness, and structural stability, making it a preferred choice for commercial and high-performance battery applications. However, the electrochemical performance of LiFePO4 is strongly influenced by its morphology and nanostructure. This review provides a comprehensive analysis of hydrothermally synthesized LiFePO4 nanomaterials, focusing on their structural, morphological, and electrochemical properties. A detailed discussion of 1D, 2D, and 3D LiFePO4 nanostructures is presented, highlighting their impact on Li-ion transport, conductivity, and overall battery performance. Furthermore, the electronic structure of LiFePO4 is examined for its charge storage mechanisms. A novel aspect of this review is the application of machine learning techniques to analyze specific capacity variations under different hydrothermal synthesis conditions and electrochemical parameters, offering insights into performance optimization. Finally, the global challenges, prospects, and research opportunities for LiFePO4-based LIBs are discussed, providing a roadmap for further advancements in this field.

可充电锂离子电池(lib)已迅速成为电子设备中最受欢迎的能量存储来源之一。锂离子电池阴极显著影响电池的能量密度、安全性、寿命和成本,并且锂离子电池具有更好的化学和热稳定性。在各种正极材料中,磷酸铁锂(LiFePO4)因其优异的安全性、低毒性、成本效益和结构稳定性而备受关注,成为商业和高性能电池应用的首选。然而,LiFePO4的电化学性能受到其形貌和纳米结构的强烈影响。本文综述了水热合成的LiFePO4纳米材料的结构、形态和电化学性能。详细讨论了1D、2D和3D LiFePO4纳米结构,强调了它们对锂离子传输、电导率和整体电池性能的影响。进一步研究了LiFePO4的电子结构及其电荷存储机制。本综述的一个新颖方面是应用机器学习技术来分析不同水热合成条件和电化学参数下的比容量变化,为性能优化提供见解。最后,讨论了基于lifepo4的锂离子电池的全球挑战、前景和研究机会,为该领域的进一步发展提供了路线图。
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引用次数: 0
Bismuth Vanadate as a Multifunctional Material for Advanced Energy Storage Systems 钒酸铋作为先进储能系统的多功能材料
Pub Date : 2025-08-31 DOI: 10.1002/bte2.20250028
Deepak Rajaram Patil, Shrikant Sadavar, Abhishek Amar Kulkarni, Kiyoung Lee, Deepak Dubal

The increasing reliance on renewable energy sources, electric vehicles, and portable electronics has intensified the demand for advanced energy storage systems that are both efficient and sustainable. Among the critical components of these systems, electrode materials play a pivotal role in determining performance. In this context, bismuth vanadate (BVO) has emerged as a highly promising material, thanks to its distinctive structural and electrochemical properties. BVO offers immense potential across various energy storage technologies, including lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), zinc-ion batteries (ZIBs) and supercapacitors. Its unique characteristics, such as efficient ion intercalation and robust battery-like behavior, position it as an ideal candidate for next-generation devices. Recent advances in morphological optimization have further enhanced the specific capacitance and cycling stability of BVO-based materials, paving the way for significant progress in energy storage technology. Furthermore, innovative approaches, such as leveraging BVO's photocatalytic capabilities in ZIBs, offer a cost-effective and environmentally friendly route to energy storage. This review highlights the transformative potential of BVO as an electrode material, emphasizing its role in addressing the pressing need for energy storage technologies that support clean and renewable energy initiatives. Through detailed exploration, it underscores the adaptability and promise of BVO in shaping the future of sustainable energy solutions.

对可再生能源、电动汽车和便携式电子产品的日益依赖,加剧了对高效和可持续的先进能源存储系统的需求。在这些系统的关键部件中,电极材料在决定性能方面起着关键作用。在这种情况下,钒酸铋(BVO)由于其独特的结构和电化学性能而成为一种非常有前途的材料。BVO在包括锂离子电池(LIBs)、钠离子电池(SIBs)、锌离子电池(zbs)和超级电容器在内的各种能源存储技术中具有巨大的潜力。其独特的特性,如高效的离子嵌入和坚固的电池样行为,使其成为下一代设备的理想候选者。最近在形态优化方面的进展进一步提高了bvo基材料的比电容和循环稳定性,为储能技术的重大进展铺平了道路。此外,创新的方法,如利用BVO在zib中的光催化能力,为能源存储提供了一种具有成本效益和环境友好的途径。这篇综述强调了BVO作为一种电极材料的变革潜力,强调了它在解决支持清洁和可再生能源倡议的储能技术的迫切需求方面的作用。通过详细的探索,它强调了BVO在塑造未来可持续能源解决方案方面的适应性和前景。
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引用次数: 0
A Solid–Liquid Hybrid Electrolyte With Weak-Solvated Solvent to Reduce Li+ Transfer Barrier at Electrode and Solid Electrolyte Interphase 一种具有弱溶剂溶剂的固液杂化电解质降低电极和固体电解质界面Li+转移势垒
Pub Date : 2025-08-27 DOI: 10.1002/bte2.20250029
Xiaojuan Zhang, Dongni Zhao, Yin Quan, Hui Wang, Junwei Zhang, Jinlong Sun, Yu Zhu, Liping Mao, Ningshuang Zhang, Shiyou Li

The interface problem caused by the contact between electrode and solid electrolyte (SE) is the main factor hindering the development of solid-state batteries. And adding liquid electrolyte (LE) at the interface to form a solid–liquid hybrid electrolyte is the common strategy. The ion transport kinetics at the SE/LE interface include an active role for the (de)solvation of ions, and the energy barrier for Li+ transport between the liquid and solid phases is closely related to the solvation capacity of the solvent. Herein, the influence of the solvation structure of the electrolyte itself on the interface is investigated. Compared to dimethyl carbonate (DMC), the lower Li+ binding energy of tetrahydrofuran (THF) is more easily desolvated at the solid–liquid interface, allowing the formation of abundant aggregates and the generation of inorganic-rich interfacial phases, leading to interfacial compatibility. Using the combination of polyvinylidene fluoride (PVDF)-based SPE and THF-based LE, the cycle performance and rate performance of LiFePO4(LFP) |SPE|Li batteries are improved. The Li/Li symmetric cell can achieve stable cycling over 1000 h at a current density of 0.05 mA cm−2, and LFP/Li half-cell retains 93% of its initial capacity after 100 cycles at 0.5 C. This study can provide inspiration for the design of solid–LE interface.

由于电极与固体电解质接触而产生的界面问题是阻碍固态电池发展的主要因素。在界面处加入液体电解质(LE)形成固液混合电解质是常用的策略。离子在SE/LE界面的输运动力学包括离子的(脱)溶剂化的积极作用,并且Li+在液相和固相之间输运的能垒与溶剂的溶剂化能力密切相关。本文研究了电解质本身的溶剂化结构对界面的影响。与碳酸二甲酯(DMC)相比,四氢呋喃(THF)的Li+结合能较低,更容易在固液界面处脱溶,从而形成丰富的团聚体,生成富无机界面相,实现界面相容性。采用聚偏氟乙烯(PVDF)基SPE和thf基LE相结合的方法,提高了LiFePO4(LFP) |SPE|锂电池的循环性能和倍率性能。Li/Li对称电池在0.05 mA cm−2电流密度下可稳定循环1000 h以上,LFP/Li半电池在0.5 C下循环100次后仍能保持93%的初始容量。本研究可为固体le接口的设计提供启示。
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引用次数: 0
Impact of Conductive Agents in Sulfide Electrolyte Coating on Cathode Active Materials for Composite Electrodes in All-Solid-State Batteries 硫化电解质涂层中导电剂对全固态电池复合电极正极活性材料的影响
Pub Date : 2025-08-26 DOI: 10.1002/bte2.20250027
Dongyoung Kim, Jongjun Lee, Seungyeop Choi, Myunggeun Song, Hyobin Lee, Yong Min Lee

All-solid-state batteries (ASSBs) with sulfide-based solid electrolytes (SEs) are promising next-generation lithium-ion batteries owing to their high energy density and safety. The composite electrode is crucial in electrochemical performance, and SE coating on the cathode active material (CAM) is an effective strategy for improving the composite electrode structure. However, despite the importance of conducting agents (CAs) in composite electrodes, their impact on the SE coating process has not been thoroughly investigated. Here, the effect of CA incorporation during the SE coating process on the morphology of the coating layer, composite electrode structure, and resulting electrochemical performance of ASSBs were examined. When the SE coating excluded CA (SE@CAM), a dense SE layer was formed on the CAM surface. By contrast, incorporating carbon black (Super P) during SE coating (SE–SP@CAM) resulted in a Super P-rich SE coating layer, reducing the active surface area and electrical conductivity of electrode and resulting in poor electrochemical performance. Meanwhile, incorporating vapor-grown carbon fibers (VGCF, 1D CA) during the SE coating process (SE–VGCF@CAM) resulted in the formation of VGCF-embedded SE coating layer. This enlarged the active surface area and facilitated electron conduction, yielding an electrochemical performance higher than that of SE–SP@CAM and comparable to that of SE@CAM. This study revealed the impact of CA incorporation during the SE coating process on the morphology of the coating layer and composite electrode structure. Furthermore, it emphasizes the importance of the mixing protocol and CA selection in electrode fabrication, offering valuable insights into developing high-performance ASSBs.

采用硫化物基固体电解质(SEs)的全固态电池(assb)因其高能量密度和安全性而成为下一代锂离子电池。复合电极的电化学性能至关重要,在阴极活性材料(CAM)上涂SE是改善复合电极结构的有效策略。然而,尽管导电剂(CAs)在复合电极中的重要性,但它们对SE涂层过程的影响尚未得到深入研究。本文考察了SE涂层过程中CA掺入对涂层形貌、复合电极结构和assb电化学性能的影响。当SE涂层排除CA (SE@CAM)后,在CAM表面形成致密的SE层。而在SE涂层过程中加入炭黑(Super P) (SE - SP@CAM)导致SE涂层Super P富集,降低了电极的活性表面积和电导率,导致电化学性能变差。同时,在SE涂层过程中加入气相生长碳纤维(VGCF, 1D CA) (SE - VGCF@CAM),形成嵌入VGCF的SE涂层。这扩大了活性表面积,促进了电子传导,产生了比SE - SP@CAM更高的电化学性能,与SE@CAM相当。本研究揭示了在SE涂层过程中CA掺入对涂层形貌和复合电极结构的影响。此外,它强调了混合协议和CA选择在电极制造中的重要性,为开发高性能assb提供了有价值的见解。
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引用次数: 0
An Amino Acid-Modified Bifunctional Separator for Shuttle Control and Li Metal Stabilization in Li-S Batteries 用于Li- s电池穿梭控制和锂金属稳定的氨基酸修饰双功能分离器
Pub Date : 2025-08-12 DOI: 10.1002/bte2.20250025
Justin Zhong, Lulu Ren, Ying Guo, Jin Liu, Wei-Hong Zhong

Lithium–sulfur batteries offer high theoretical energy density, affordability, and environmental friendliness, but lack commercial viability due to performance issues stemming from Li dendrite growth and the shuttle effect. In this study, we apply a positively charged amino acid in a surface coating for commercial polypropylene separators, endowing it with shuttle-inhibiting and anode-stabilizing functions. The amino acid-modified separator (A-PC@PP) features a nanocomposite interlayer of L-Arginine (Arg), polyacrylic acid (PAA), and carbon nanofibers (CNFs) to trap and convert polysulfides. Meanwhile, Arg and PAA functional groups introduced throughout the separator homogenize the flux of Li+, suppressing the growth of dendrites on the Li metal anode. Arising from these favorable functions, Li-S cells equipped with A-PC@PP separators show excellent rate capability (> 530 mAh/g at an ultrahigh current density of 5 A/g) and improved cycling stability (with a low decay rate of 0.068% per cycle for 500 cycles at 0.5 A/g). This study showcases the viability of a promising and abundant amino acid in addressing the critical issues of Li-S batteries.

锂硫电池具有较高的理论能量密度、可负担性和环境友好性,但由于锂枝晶生长和穿梭效应引起的性能问题,缺乏商业可行性。在这项研究中,我们将带正电的氨基酸应用于商用聚丙烯分离器的表面涂层中,赋予其抑制穿梭和稳定阳极的功能。氨基酸修饰的分离器(A-PC@PP)具有l -精氨酸(Arg),聚丙烯酸(PAA)和纳米碳纤维(CNFs)的纳米复合中间层,用于捕获和转化多硫化物。同时,在整个分离器中引入的Arg和PAA官能团使Li+的通量均匀,抑制了Li金属阳极上枝晶的生长。由于这些有利的功能,配备A-PC@PP分离器的Li-S电池表现出优异的倍率能力(在5 A/g的超高电流密度下>; 530 mAh/g)和改善的循环稳定性(在0.5 A/g下循环500次,每循环衰减率低至0.068%)。这项研究展示了一个有前途的和丰富的氨基酸在解决锂电池的关键问题的可行性。
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引用次数: 0
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Battery Energy
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