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Insight Into Puncture-Induced Thermal Runaway in Lithium-Ion Batteries to Reduce Fire Risks in Electric Vehicle Collisions 研究锂离子电池刺痛性热失控以降低电动汽车碰撞中的火灾风险
Pub Date : 2025-08-03 DOI: 10.1002/bte2.20250036
Hong Zhao, Xiangkun Bo, Zhiguo Zhang, Li Wang, Walid A. Daoud, Xiangming He

Lithium-ion batteries (LIBs) power electric vehicles through exceptional energy density but pose critical safety risks when mechanically compromised, particularly through nail penetration-induced thermal runaway. This review synthesizes experimental and modeling studies to establish the thermal runaway initiation hierarchy: (1) State-of-charge (SOC) (doubles thermal runaway probability at over 60% SOC), (2) cathode chemistry (thermal runaway propagation of LiNi0.8Co0.1Mn0.1-based batteries is eightfold faster than that of LiFePO4-based batteries), (3) nail properties (the possibility of short-circuit current of steel-based batteries is 40% higher than that of copper-based batteries), and (4) penetration dynamics (depth's impact is more than that of separator thickness in triggering cascading failures). Thermal runaway mechanisms involve synergistic electrochemical–thermal–mechanical coupling, where localized heating (higher than 1 × 10⁴ K/s) initiates separator collapse (80°C–120°C) and electrolyte decomposition (200°C). Mitigation strategies focus on mechanically graded separators (SiO₂/polymer composites: increasing 180% in puncture resistance); shear-thickening adhesives reducing impact forces by 35%–60%; halogen-free electrolytes within a 2 s self-extinguishing time; and solid-state architectures showing 0% thermal runaway incidence in nail penetration tests. Critical gaps persist in standardizing penetration protocols (velocity: 0.1–80 mm/s variations across studies) and modeling micro-short circuits. Emerging solutions prioritize materials-by-design approaches combining sacrificial microstructures with embedded thermal sensors. This analysis provides a roadmap for developing intrinsically safe LIBs that maintain energy density while achieving automotive-grade mechanical robustness (ISO 6469-1 compliance), ultimately advancing collision-resilient electric vehicle battery systems.

锂离子电池(LIBs)通过超高的能量密度为电动汽车提供动力,但在机械损坏时,尤其是在钉子穿透引起热失控的情况下,会带来严重的安全风险。本文综合了实验和模型研究,建立了热失控起始层次:(1)荷电状态(SOC)(在SOC超过60%时热失控概率翻倍),(2)阴极化学(lini0.8 co0.1 mn0.1基电池的热失控传播速度比lifepo4基电池快8倍),(3)钉特性(钢基电池短路电流的可能性比铜基电池高40%),(4)穿透动力学(深度对触发级联失效的影响大于分离器厚度)。热失控机制涉及协同的电化学-热-机械耦合,其中局部加热(高于1 × 10⁴K/s)引发分离器坍塌(80°C - 120°C)和电解质分解(200°C)。缓解策略侧重于机械分级分离器(SiO₂/聚合物复合材料:抗穿刺性提高180%);剪切增稠胶粘剂可降低35%-60%的冲击力;无卤电解液在2s内自熄;在钉子穿透测试中,固态结构显示0%的热失控发生率。关键的差距仍然存在于标准化的渗透协议(速度:0.1-80毫米/秒的研究变化)和微短路建模。新兴的解决方案优先考虑将牺牲微结构与嵌入式热传感器相结合的材料设计方法。该分析为开发本质安全的锂电池提供了路线图,在保持能量密度的同时实现汽车级机械稳健性(符合ISO 6469-1标准),最终推进抗碰撞电动汽车电池系统。
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引用次数: 0
Integration of Oxide-Based All-Solid-State Batteries at 350°C by Infiltration of a Lithium-Rich Oxychloride Melt 在350°C下,通过渗透富锂氯化氧熔体集成氧化物基全固态电池
Pub Date : 2025-07-31 DOI: 10.1002/bte2.20250014
Junteng Du, Danna Yan, Seong Jin Choi, Joah Han, Yazhou Zhou, Yi Yang, Angel Burgos, Daeil Kim, Bo-Yun Jang, Ji Haeng Yu, Jae Chul Kim

We highlight the lowest-temperature manufacturing of oxide-based all-solid-state batteries in this study. A lithium-rich oxychloride melt was employed to integrate Li6.25Ga0.25La3Zr2O12 (Ga-LLZO) solid electrolyte particles and LiCoO2 cathode-active particles at 350°C. As observed by X-ray diffraction, scanning electron microscopy, and microcomputed tomography, the infiltration and subsequent solidification of the melt can promote interparticle contact without chemical crosstalk in the cathode and across the cathode–solid electrolyte interface. The melt-infiltrated all-solid cathode exhibits respectable capacity, 83 mA h g−1 at 90°C. Due to mechanical degradation of the interfaces, the cathode failed to maintain good cycle stability. Given that the minute amount of liquid electrolyte addition leads to substantial improvement of achievable capacity (106 mA h g−1 at RT) and capacity retention, ensuring electric wiring in the cathode is key to achieving desirable electrochemical properties of the all-solid cells produced by the melt-infiltration process. Identified cathode optimization to better leverage this melt-infiltration approach includes, but is not limited to, engineering particle size distribution of Ga-LLZO and LiCoO2 and configurations of the cathode components. While our proposed method is yet to be perfected, we have established a practical foundation to integrate oxide-based all-solid-state batteries.

在这项研究中,我们强调了最低温度下氧化物基全固态电池的制造。采用富锂氯化氧熔体在350℃下对Li6.25Ga0.25La3Zr2O12 (Ga-LLZO)固体电解质颗粒和LiCoO2阴极活性颗粒进行了整合。通过x射线衍射、扫描电子显微镜和微计算机断层扫描观察到,熔体的渗透和随后的凝固可以促进阴极和阴极-固体电解质界面的颗粒间接触,而不会产生化学串扰。熔融渗透的全固态阴极在90°C时表现出可观的83 mA h g−1容量。由于界面的机械退化,阴极不能保持良好的循环稳定性。考虑到微量的液体电解质添加导致可实现容量(RT下106 mA h g−1)和容量保持的大幅提高,确保阴极中的电线是实现熔融渗透工艺生产的全固体电池理想电化学性能的关键。为了更好地利用这种熔融渗透方法,确定的阴极优化包括但不限于Ga-LLZO和LiCoO2的工程粒度分布以及阴极组件的配置。虽然我们提出的方法还有待完善,但我们已经为集成氧化物基全固态电池奠定了实践基础。
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引用次数: 0
Enhanced Structural Transformation Enabled by Low-Crystalline Vanadium Oxides in Aqueous Zinc-Ion Batteries 低晶钒氧化物促进锌离子电池结构转变
Pub Date : 2025-07-13 DOI: 10.1002/bte2.20250016
Hyeonjun Lee, Hyungjin Lee, Sangki Lee, Hyojun Lim, Seung-Tae Hong, Hyung Do Kim, Munseok S. Chae

Aqueous batteries are gaining attention owing to their high safety and cost-effectiveness. Among these, Zn-based aqueous batteries excel because of Zn's low redox potential (−0.76 V vs. SHE), its abundance, and eco-friendliness. However, despite their advantages, challenges, such as low energy density and limited cycle life limit their usage. This study addresses these issues by employing low-crystalline V2O4.86 as a cathode material, enhanced with oxygen vacancies created by controlled annealing time. The structure of low-crystalline V2O4.86 facilitates rapid structural transformation into the highly active phase Zn3+x(OH)2V2O7·2(H2O). Electrochemical tests revealed a 22% capacity improvement for low-crystalline V2O4.86 (360 mAh g−1) over high-crystalline V2O5 (295 mAh g−1) at 0.8 A g−1, attributed to the presence of active oxygen vacancies. Comprehensive structural analysis, spectroscopy, and diffusion path/barrier studies elucidate the underlying mechanisms for the first time, highlighting the potential of oxygen-engineered V2O5. These findings indicate that electrodes engineered with oxygen vacancies offer promising insights in advancing cathode materials for high-performance secondary battery technologies.

水溶液电池因其高安全性和高性价比而备受关注。其中,锌基水电池的优势在于锌的低氧化还原电位(- 0.76 V vs. SHE)、丰富度和生态友好性。然而,尽管它们具有优势,但能量密度低和循环寿命有限等挑战限制了它们的使用。本研究通过采用低晶V2O4.86作为正极材料,通过控制退火时间产生氧空位来增强正极材料,从而解决了这些问题。低晶V2O4.86的结构有利于快速转变为高活性相Zn3+x(OH)2V2O7·2(H2O)。电化学测试表明,在0.8 a g−1时,低晶V2O4.86 (360 mAh g−1)的容量比高晶V2O5 (295 mAh g−1)的容量提高了22%,这是由于活性氧空位的存在。全面的结构分析、光谱学和扩散路径/势垒研究首次阐明了潜在的机制,突出了氧工程V2O5的潜力。这些发现表明,利用氧空位设计的电极为高性能二次电池技术的正极材料的发展提供了有希望的见解。
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引用次数: 0
Modulation of a NiFe-Layered Double Hydroxide Electrode Using Zn Doping and Selective Etching Process for High-Performance Oxygen Evolution Reaction 用Zn掺杂和选择性蚀刻工艺调制nife层状双氢氧化物电极用于高性能析氧反应
Pub Date : 2025-07-08 DOI: 10.1002/bte2.70012
Yeonsu Park, Suok Lee, Eunwoo Park, Yong-Hwan Mo, Juwon Lee, Jong Bae Park, Bong Kyun Kang, Younghyun Cho, Gyeong Hee Ryu, Sang-Beom Han, John Hong, Young-Woo Lee

In the generation of green hydrogen and oxygen from water, transition metal–based electrode materials have been considered high-performance water-splitting catalysts. In water splitting, the oxygen evolution reaction (OER) is the rate-determining step. To overcome the high overpotential and slow kinetics of OER, the development of effective catalysts to improve electrolysis efficiency is essential. Nickel–iron-layered double hydroxides (NiFe-LDHs) have been recognized for their superior electrochemical performance under alkaline OER conditions and have emerged as promising catalysts owing to their unique structure that enhances electrolyte infiltration and exposes more active sites. However, the unique modulation of the crystalline structure of NiFe-LDHs can further improve OER performance. Accordingly, this study introduces an innovative synthesis approach based on Zn doping and selective Zn etching to increase the ECSA and induce favorable transition-metal oxidation states in NiFe-LDHs, thereby improving OER efficiency. After 6 h of Zn etching (Ni2.9Zn0.1Fe-6h), the optimized Ni2.9Zn0.1Fe LDH sample demonstrated remarkable electrochemical performance and stability, requiring small overpotentials of 192 and 260 mV at current densities of 10 and 100 mA cm−2, respectively. Moreover, the Ni2.9Zn0.1Fe-6h electrode could maintain its original overpotential (260 mV) at a current density of 100 mA cm−2 for 250 h. The proposed Zn doping and subsequent partial Zn etching can practically be applied to numerous high-performance transition metal–based electrochemical catalysts.

在从水中生成绿色氢和氧的过程中,过渡金属基电极材料被认为是高性能的水分解催化剂。在水裂解过程中,析氧反应(OER)是决定速率的步骤。为了克服OER的高过电位和慢动力学,开发有效的催化剂来提高电解效率是必不可少的。镍铁层状双氢氧化物(NiFe-LDHs)在碱性OER条件下具有优异的电化学性能,并且由于其独特的结构可以增强电解质的渗透并暴露更多的活性位点而成为有前途的催化剂。然而,NiFe-LDHs晶体结构的独特调制可以进一步提高OER性能。因此,本研究引入了一种基于Zn掺杂和选择性Zn蚀刻的创新合成方法,以增加nfe - ldhs的ECSA并诱导有利的过渡金属氧化态,从而提高OER效率。经过6h的Zn刻蚀(Ni2.9Zn0.1Fe-6h),优化后的Ni2.9Zn0.1Fe LDH样品在10和100 mA cm−2电流密度下的过电位分别为192和260 mV,表现出了良好的电化学性能和稳定性。此外,Ni2.9Zn0.1Fe-6h电极在100 mA cm−2的电流密度下可以维持250 h的原始过电位(260 mV)。提出的锌掺杂和随后的部分锌蚀刻可以实际应用于许多高性能过渡金属基电化学催化剂。
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引用次数: 0
Probing the Compositional and Structural Effects on the Electrochemical Performance of Na(Mn-Fe-Ni)O2 Cathodes in Sodium-Ion Batteries 钠离子电池中Na(Mn-Fe-Ni)O2阴极的组成和结构对电化学性能的影响
Pub Date : 2025-07-08 DOI: 10.1002/bte2.70018
Samriddhi Saxena, Hari Narayanan Vasavan, Neha Dagar, Karthik Chinnathambi, Velaga Srihari, Asish Kumar Das, Pratiksha Gami, Sonia Deswal, Pradeep Kumar, Himanshu Kumar Poswal, Sunil Kumar

This study systematically investigates an Mn-Fe-Ni pseudo-ternary system for Na(Mn-Fe-Ni)O2 cathodes, focusing on the effects of varying transition metal fractions on structural and electrochemical properties. X-ray diffraction reveals that increasing Mn content induces biphasic behavior. A higher Ni content reduces the c parameter, while higher Mn and Fe concentrations expand the lattice. Average particle size increases with an increase in Mn content and Fe/Ni ratio. NaMn0.500Fe0.125Ni0.375O2 delivers a high specific capacity of ~149 mAh g⁻¹ in the 2.0–4.0 V range. Galvanostatic charge-discharge and dQ/dV versus V curves suggest that a Ni/Fe ratio > 1 enhances specific capacity and lowers voltage polarization in the materials. NaMn0.500Fe0.250Ni0.250O2 demonstrated the best rate performance, exhibiting 85.7% capacity at 1C and 69.7% at 3C, compared to 0.1C, while biphasic NaMn0.625Fe0.125Ni0.250O2 (MFN-512) excelled in cyclic stability, retaining 93% of capacity after 100 cycles. The performance of MFN-512 in a full cell configuration was studied with hard carbon as the anode, resulting in a specific capacity of ~92 mAh g−1 and a nominal voltage of ~2.9 V at a 0.1C rate, demonstrating its potential in practical applications. Transmission electron microscopy confirmed the biphasic nature of MFN-512, with columnar growth of P2 and O3 phases. Electrochemical impedance spectroscopy revealed that better-performing samples have lower charge transfer resistance. Operando Synchrotron XRD reveals reversible phase transformations in MFN-512, driven by its optimized transition metal ratios and phase fraction. This work outlines a systematic approach to optimizing low-cost, high-performance Mn-Fe-Ni layered oxides.

本研究系统地研究了Na(Mn-Fe-Ni)O2阴极的Mn-Fe-Ni伪三元体系,重点研究了不同过渡金属组分对结构和电化学性能的影响。x射线衍射表明,Mn含量的增加诱导了双相行为。较高的Ni含量降低了c参数,而较高的Mn和Fe浓度则扩大了晶格。平均粒径随Mn含量和Fe/Ni比的增加而增大。在2.0-4.0 V范围内,namn0.500 fe0.125 ni0.3750 o2的比容量高达~149 mAh g⁻¹。恒流充放电和dQ/dV / V曲线表明,当Ni/Fe比为1时,材料的比容量增大,电压极化降低。NaMn0.500Fe0.250Ni0.250O2表现出最好的倍率性能,在1C和3C下的倍率分别为85.7%和69.7%,而双相NaMn0.625Fe0.125Ni0.250O2 (MFN-512)在循环稳定性方面表现优异,循环100次后仍保持93%的倍率。以硬碳为阳极,研究了MFN-512在全电池结构下的性能,在0.1C倍率下的比容量为~92 mAh g−1,标称电压为~2.9 V,证明了其实际应用潜力。透射电镜证实了MFN-512的双相性质,P2和O3相呈柱状生长。电化学阻抗谱分析表明,性能较好的样品具有较低的电荷转移电阻。Operando同步加速器XRD显示,在优化的过渡金属比和相分数的驱动下,MFN-512发生了可逆的相变。本研究概述了一种优化低成本、高性能Mn-Fe-Ni层状氧化物的系统方法。
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引用次数: 0
Cover Image, Volume 4, Issue 4, July 2025 封面图片,第四卷,第四期,2025年7月
Pub Date : 2025-07-08 DOI: 10.1002/bte2.12193

Front Cover: Solid-state electrolytes are essential for developing safe and efficient lithium metal batteries. In article number BTE.70007, Xinhao Yang and co-workers investigate the effect of AlF3 incorporation on lithium borate glass electrolytes, revealing a counterintuitive performance deterioration. While fluoride additives are widely used to enhance interfacial stability, their incorporation into the glass matrix was found to reduce ionic conductivity and lead to early short-circuiting under moderate current densities. In contrast, fluoride-free lithium borate glasses exhibited excellent thermal stability, wide electrochemical windows, and maintained stable operation for 500 hours under current densities ranging from 0.04 to 1 mA cm-2. This work provides critical insights into the complex interplay between fluoride content, glass chemistry, and electrochemical performance, offering new guidelines for interfacial design in solid-state batteries.

前盖:固态电解质对于开发安全高效的锂金属电池至关重要。在编号BTE.70007的文章中,杨鑫浩及其同事研究了AlF3掺入对硼酸锂玻璃电解质的影响,揭示了一种违反直觉的性能下降。虽然氟化物添加剂被广泛用于增强界面稳定性,但它们掺入玻璃基体会降低离子电导率,并在中等电流密度下导致早期短路。相比之下,无氟硼酸锂玻璃表现出优异的热稳定性,宽电化学窗口,并在0.04至1 mA cm-2的电流密度下保持500小时的稳定运行。这项工作为氟化物含量、玻璃化学和电化学性能之间复杂的相互作用提供了重要的见解,为固态电池的界面设计提供了新的指导方针。
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引用次数: 0
High-Capacity Economically Viable Catholyte for Alkaline Aqueous Redox Flow Battery 用于碱性水氧化还原液流电池的高容量经济可行阴极液
Pub Date : 2025-07-08 DOI: 10.1002/bte2.70014
Zahid M. Bhat, Mohammad Furquan, Muhammad A. Z. G. Sial, Umair Alam, Iqbal A. Al Hamid, Atif S. Alzahrani, Mohammad Qamar

Alkaline aqueous organic redox flow batteries (AORFB) show great potential as viable options for storing energy in commercial power grids. While there has been notable advancement in the development of anolytes, there has been a lack of focus on the catholyte component. In this study, we present a novel all-alkaline AORFB that utilizes a highly soluble catholyte based on manganese (Mn). The formulated combination of catholyte, MnO4/NaOH, has remarkably high solubility, approximately 3.9 M, and possesses a theoretical capacity of 105 Ah L–1. This capacity is the greatest among all reported catholytes thus far. Half-cell experiments indicate that there is a high level of reversibility and stability, with minimal capacity degradation over time. In addition to three-electrode configuration, the efficacy of MnO4/NaOH is evaluated in full-cell redox flow systems utilizing alizarin as anolyte. The AORFB shows an open circuit voltage of approximately 1.3 V, which is nearly 250 mV higher than the state-of-the-art ferrocyanide-based AORFBs. This resulted in an energy and power output that is approximately 20% higher. In addition, the system exhibits consistent performance with minimal decrease in capacity (0.1% per day) while achieving approximately 85% energy efficiency and 100% coulombic efficiency. The impact of the cutoff potential and plausible degradation mechanisms of the catholyte are also discussed. The findings of this electrolyte formulation offer fresh impetus for developing high-capacity all-alkaline AORFBs.

碱性水有机氧化还原液流电池(AORFB)作为商业电网中储能的可行选择显示出巨大的潜力。虽然阳极电解质的发展取得了显著的进步,但对阴极电解质成分的关注一直不足。在这项研究中,我们提出了一种新型的全碱性orfb,它利用基于锰(Mn)的高可溶性阴极电解质。所制备的阴极电解质MnO4 - /NaOH具有很高的溶解度,约为3.9 M,理论容量为105 Ah L-1。这种能力是迄今为止所有报道的天主教中最大的。半电池实验表明,有高水平的可逆性和稳定性,与最小的容量退化随着时间的推移。除了三电极结构外,MnO4 - /NaOH在以茜素为阳极液的全电池氧化还原流系统中的效率也得到了评估。orfb的开路电压约为1.3 V,比目前最先进的基于氰化铁的orfb高出近250 mV。这导致能量和功率输出大约高出20%。此外,该系统表现出稳定的性能,容量下降最小(每天0.1%),同时实现约85%的能源效率和100%的库仑效率。还讨论了截止电位的影响和阴极液的可能降解机制。该电解质配方的发现为开发高容量全碱性主动脉动脉输送膜提供了新的动力。
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引用次数: 0
New Trends in SERS Substrates With Micro- and Nanostructures: Materials, Substrates, Preparation, and Applications 微纳米结构SERS衬底的新趋势:材料、衬底、制备和应用
Pub Date : 2025-07-08 DOI: 10.1002/bte2.70023
Xiaoyu Tian, Bo Zhang, Lei Song, Jingwei Bao, Junsheng Yang, Liangbo Sun, Houchang Pei, Chunpeng Song

Surface-enhanced Raman scattering (SERS) is a frontier technology for high-sensitivity analysis of molecules and chemical substances, and a useful tool in the sensing field relying on fingerprint recognition ability, high sensitivity, multiple detection, biocompatibility, and so forth. SERS substrates have been well concerned attributed to their ability to enhance Raman signals, which makes them useful in various applications, including sensing and detection. At the same time, flexible SERS substrates enable sample loads to meet requirements and, therefore, have high sensitivity for Raman detection, but the detection capacity is still limited. In this paper, the basic principle and method of SERS were reviewed, and some new trends of micro- and nanostructured SERS substrates were reviewed from the aspects of material, matrix type, preparation, and application.

表面增强拉曼散射(Surface-enhanced Raman scattering, SERS)是分子和化学物质高灵敏度分析的前沿技术,凭借指纹识别能力、高灵敏度、多重检测、生物相容性等优点,是传感领域的重要工具。SERS衬底由于其增强拉曼信号的能力而受到广泛关注,这使得它们在包括传感和检测在内的各种应用中都很有用。同时,柔性SERS衬底使样品负载满足要求,因此对拉曼检测具有很高的灵敏度,但检测能力仍然有限。本文综述了SERS的基本原理和方法,并从材料、基体类型、制备和应用等方面综述了微纳米结构SERS基板的一些新动向。
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引用次数: 0
Uncovering the Potential of Layered InOCI as Anode Material in Lithium, Magnesium, and Aluminum Ion Batteries: First-Principles Investigations 揭示层状二氧化钛作为锂、镁、铝离子电池负极材料的潜力:第一性原理研究
Pub Date : 2025-07-08 DOI: 10.1002/bte2.70013
Sawaira Tasawar, Abdul Majid, Sheraz Ahmad, Mohammad Alkhedher, Sajjad Haider, Kamran Alam

This study reports the utilization of indium oxychloride (InOCl) as a promising electrode material for rechargeable lithium-ion battery (LIB), magnesium ion battery (MIB), and aluminum ion battery (AIB). The anodic properties of InOCl are carefully investigated using density functional theory (DFT) and ab initio molecular dynamics (AIMD) calculations to explore structural, electronic, transport, and electrochemical characteristics. The results reveal that InOCl stores more metal ions than the commercially used anode materials. The values of the charge capacity are found as 3604, 4700, 2820 mAhg−1 for LIBs, MIBs and AIBs,respectively which shows that InOCl could be a capable anode material. The open circuit voltage of the host material is given as 2.05 V for Li, 1.7 V for Mg and 0.95 V for Al, respectively. The volume expansion is calculated as 9.12%, 3.6% and 15.5% for LIBs, MIBs and AIBs, respectively which points to resilience of the host against swelling during charge/discharge cycles. The electrochemical performance of the host is studied on the basis of diffusion kinetics and transition barrier faced by Li-ions, Mg-ions and Al-ions. The minimum energy barrier is calculated as 0.20, 0.80, and 0.44 eV whereas the values of diffusion coefficient are calculated as 1.14 × 10−9, 1.1 × 10–11, and 0.88 × 10−9 m2/s for LIBs, MIBs and AIBs, respectively. Furthermore, the respective values of ionic conductivity are calculated as 10.32 × 10−2, 1.1 × 10−2, and for 8.50 × 10−3 S/m.

本文报道了氧化氯化铟(InOCl)作为可充电锂离子电池(LIB)、镁离子电池(MIB)和铝离子电池(AIB)极材的应用前景。利用密度泛函理论(DFT)和从头算分子动力学(AIMD)计算仔细研究了InOCl的阳极性能,以探索其结构、电子、输运和电化学特性。结果表明,与工业上使用的阳极材料相比,InOCl能储存更多的金属离子。锂离子电池、锂离子电池和锂离子电池的电荷容量分别为3604、4700、2820 mAhg−1,表明inol是一种性能良好的阳极材料。基体材料的开路电压分别为:Li为2.05 V, Mg为1.7 V, Al为0.95 V。计算得出,LIBs、MIBs和AIBs的体积膨胀率分别为9.12%、3.6%和15.5%,这表明宿主在充放电周期中具有抗膨胀的弹性。基于li -离子、mg -离子和al -离子的扩散动力学和过渡势垒,研究了寄主的电化学性能。LIBs、MIBs和AIBs的最小能垒分别为0.20、0.80和0.44 eV,而扩散系数分别为1.14 × 10 - 9、1.1 × 10 - 11和0.88 × 10 - 9 m2/s。此外,离子电导率分别为10.32 × 10−2、1.1 × 10−2和8.50 × 10−3 S/m。
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引用次数: 0
In Situ Coating Li3PO4 on Li6.5La3Zr1.5Ta0.5O12 Achieving Lithium Dendrites Inhibition and High Chemical Stability 在Li6.5La3Zr1.5Ta0.5O12上原位涂覆Li3PO4,实现了锂枝晶抑制和高化学稳定性
Pub Date : 2025-07-08 DOI: 10.1002/bte2.70009
Jun Ma, Ruilin He, Yidong Jiang, Ludan Zhang, Hongli Xu, Hongbo Zeng, Chaoyang Wang, Xiaoxiong Xu, Yonghong Deng, Jun Wang, Shang-Sen Chi

Solid-state electrolyte (SSE) is a potential way to solve the safety problems of lithium metal batteries (LMBs), and Li6.5La3Zr1.5Ta0.5O12 (LLZTO) is one of the most extensive research SSEs due to its good air stability and wide electrochemical window. However, the residual alkali on LLZTO surface limits its application with polyvinylidene difluoride (PVDF)-contained binders, and the uncontrollable lithium dendrites growing between the grain boundaries of LLZTO particles would lead to rapid capacity fading and potential short circuit risk. Herein, by in situ coating Li3PO4 (LPO) on LLZTO particles (LLZTO@LPO) evenly, the residual alkali on the LLZTO surface is neutralized and the pH value is reduced to 8.84. The modified LLZTO can be mixed with PVDF solution and shows good fluidity without a cross-linking reaction, making the subsequent ceramic coating on the separator feasible. The LLZTO@LPO coating polyethylene (PE) separator can achieve 1400 h (115% increase) stable cycling under 1 mA cm−2 current density in the Li∥Li symmetrical cell and 80% capacity retention after 260 cycles (NCM622-Li coin cell with 3 mAh cm−2 loading). Furthermore, the LLZTO SSE pellets were prepared with the LLZTO@LPO and assembled in coin cell. The critical current density (CCD) result increases from 0.7 to 1.6 mA cm−2 owing to that the LPO coating effectively inhibits the lithium dendrites formation through LLZTO grain boundaries. This work provides a strategy for fabricating the coating layer on LLZTO to improve the stability of LMBs.

固态电解质(SSE)是解决锂金属电池(lmb)安全问题的潜在途径,而Li6.5La3Zr1.5Ta0.5O12 (LLZTO)因其良好的空气稳定性和较宽的电化学窗口而成为研究最广泛的固态电解质之一。然而,LLZTO表面残留的碱限制了其与含聚偏氟乙烯(PVDF)粘合剂的应用,并且LLZTO颗粒晶界之间不可控的锂枝晶生长会导致容量快速衰减和潜在的短路风险。本文通过在LLZTO颗粒(LLZTO@LPO)上均匀地原位涂覆Li3PO4 (LPO),使LLZTO表面的残碱得到中和,pH值降至8.84。改性后的LLZTO可与PVDF溶液混合,且流动性好,不发生交联反应,使后续在分离器上涂覆陶瓷成为可能。LLZTO@LPO涂层聚乙烯(PE)隔膜在1 mA cm−2电流密度下可在Li∥Li对称电池中稳定循环1400 h(增加115%),260次循环后(NCM622-Li硬币电池,3 mAh cm−2负载)容量保持率为80%。在此基础上,用LLZTO@LPO制备了LLZTO SSE微球,并在硬币池中组装。LPO涂层通过LLZTO晶界有效抑制了锂枝晶的形成,使得临界电流密度(CCD)从0.7 mA cm−2提高到1.6 mA cm−2。本工作为在LLZTO上制备涂层以提高lmb的稳定性提供了一种策略。
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Battery Energy
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