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Evaluating the feasibility and air stability of high-entropy doping in garnet electrolytes 评价石榴石电解质中高熵掺杂的可行性和空气稳定性
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-10 DOI: 10.1016/j.ensm.2025.104603
Jiameng Yu , Tianyi Gao , Ruixin Hao , Yuanyuan Cui , Luyao Wang , Yihang Yang , Yuyao Zhang , Wenbo Zhai , Fenwei Cui , Ziran Xu , Xiangchen Hu , Ning Xue , Yi Yu , Fei Song , Hui Zhang , Zhi Liu , Wei Liu
{"title":"Evaluating the feasibility and air stability of high-entropy doping in garnet electrolytes","authors":"Jiameng Yu ,&nbsp;Tianyi Gao ,&nbsp;Ruixin Hao ,&nbsp;Yuanyuan Cui ,&nbsp;Luyao Wang ,&nbsp;Yihang Yang ,&nbsp;Yuyao Zhang ,&nbsp;Wenbo Zhai ,&nbsp;Fenwei Cui ,&nbsp;Ziran Xu ,&nbsp;Xiangchen Hu ,&nbsp;Ning Xue ,&nbsp;Yi Yu ,&nbsp;Fei Song ,&nbsp;Hui Zhang ,&nbsp;Zhi Liu ,&nbsp;Wei Liu","doi":"10.1016/j.ensm.2025.104603","DOIUrl":"10.1016/j.ensm.2025.104603","url":null,"abstract":"<div><div>High-entropy electrolytes have attracted extensive attention for their potential to overcome the limits of traditional materials. However, confirming the accurate synthesis of a single-phase high-entropy electrolyte remains a challenge. Herein, we develop a quinary garnet electrolyte of cubic phase with high resistance to air corrosion. By employing a straightforward method that analyzes the variations of diffraction peak intensity, we can evaluate the feasibility of high-entropy doping, the degree of cubic phase, and the extent of H<sup>+</sup>/Li<sup>+</sup> exchange. Meanwhile, ambient pressure X-ray photoelectron spectroscopy is utilized to investigate the degradation of garnet electrolyte by H<sub>2</sub>O, with the failure mechanism further elucidated by nuclear magnetic resonance analysis. On this basis, the high-entropy garnet electrolyte demonstrated increased cubic phase content and better air stability, compared with traditional counterpart. Consequently, a higher current critical density is achieved, facilitating the integration of commercial cathodes with high area capacities into the quasi-solid-state batteries. Our findings provide an effective method for synthesizing and evaluating high entropy electrolytes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104603"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026043","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
Stabilizing electrolytic Zn||MnO2 batteries under lean electrolyte conditions via synergistic anode and electrolyte engineering 通过协同阳极和电解质工程在贫电解质条件下稳定电解Zn||MnO2电池
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-10 DOI: 10.1016/j.ensm.2025.104601
Wenli Xin , Yaheng Geng , Hui Zhang , Lei Zhang , Yu Han , Zichao Yan , Fangyi Cheng , Zhiqiang Zhu
{"title":"Stabilizing electrolytic Zn||MnO2 batteries under lean electrolyte conditions via synergistic anode and electrolyte engineering","authors":"Wenli Xin ,&nbsp;Yaheng Geng ,&nbsp;Hui Zhang ,&nbsp;Lei Zhang ,&nbsp;Yu Han ,&nbsp;Zichao Yan ,&nbsp;Fangyi Cheng ,&nbsp;Zhiqiang Zhu","doi":"10.1016/j.ensm.2025.104601","DOIUrl":"10.1016/j.ensm.2025.104601","url":null,"abstract":"<div><div>Electrolytic Zn||MnO<sub>2</sub> batteries utilizing acidic electrolytes are promising for large-scale energy storage owing to their high energy/power densities. However, they encounter challenges such as hydrogen evolution corrosion on Zn anodes and excessive electrolyte-to-cathode capacity ratios (E/C ratio &gt; 0.05 mL mAh<sup>−1</sup>). Here, we introduce a synergistic approach combining a zeolitic imidazolate frameworks (ZIFs)-coated Zn anode and acetic acid (HOAc)-modified electrolyte to stabilize electrolytic Zn||MnO<sub>2</sub> batteries under lean electrolyte conditions. Specifically, HOAc substitutes partial imidazole ligands within the ZIFs coating, forming a dense, acid-resistant amorphous ZIFs (aZIFs) layer that effectively mitigates Zn anode corrosion. Simultaneously, the HOAc-modified electrolyte acts as a proton reservoir for the MnO<sub>2</sub> cathode, enabling reversible MnO<sub>2</sub>/Mn<sup>2+</sup> redox chemistry. This dual modification allows the ZIFs@Zn||MnO<sub>2</sub> coin cell to retain 80.4 % capacity after 1000 cycles at 5.0 A g<sup>–1</sup> and the pouch cell to achieve an output voltage exceeding 1.5 V at 0.5 A g<sup>−1</sup> with a E/C ratio of 0.018 mL mAh<sup>−1</sup>. Our work provides a feasible approach to develop practical electrolytic Zn||MnO<sub>2</sub> batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104601"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145025765","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
Covalent organic framework-engineered separators enabling selective sodium ion transport for sodium metal anode storage 共价有机框架-工程分离器实现选择性钠离子传输的钠金属阳极存储
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-10 DOI: 10.1016/j.ensm.2025.104599
Shusheng Tao , Xiquan Ke , Dongxiao Li , Zheng Luo , Huimin Lian , Shengrui Gao , Shaozhen Huang , Wentao Deng , Hongshuai Hou , Guipeng Yu , Guoqiang Zou , Xiaobo Ji
{"title":"Covalent organic framework-engineered separators enabling selective sodium ion transport for sodium metal anode storage","authors":"Shusheng Tao ,&nbsp;Xiquan Ke ,&nbsp;Dongxiao Li ,&nbsp;Zheng Luo ,&nbsp;Huimin Lian ,&nbsp;Shengrui Gao ,&nbsp;Shaozhen Huang ,&nbsp;Wentao Deng ,&nbsp;Hongshuai Hou ,&nbsp;Guipeng Yu ,&nbsp;Guoqiang Zou ,&nbsp;Xiaobo Ji","doi":"10.1016/j.ensm.2025.104599","DOIUrl":"10.1016/j.ensm.2025.104599","url":null,"abstract":"<div><div>Sodium metal energy storage devices with high power/energy densities offer scalability without requiring complex presodiation. However, the sluggish migration of Na<sup>+</sup> and the uncontrollable growth of sodium dendrites have hindered their commercial adoption. Herein, we construct functionalized separators using quinoline carboxylic acid covalent organic frameworks (QL-COFs) to achieve selective Na<sup>+</sup> transport and uniform deposition. Molecular dynamics simulations and theoretical calculations confirm that QL-COFs with uniform pore structures restrict PF<sub>6</sub><sup>-</sup> ion migration while providing highly selective transport channels for Na<sup>+</sup>, doubling the Na<sup>+</sup> transference number to 0.89 (<em>vs.</em> 0.43 for polyethylene separators), surpassing values reported for state-of-the-art functionalized separators and solid-state electrolytes. <em>In-situ</em> XRD directly visualizes the reversible Na<sup>+</sup> deposition/stripping behavior on Cu foil, corroborated by the stable Coulombic efficiency of Na-Cu cells over 800 h, jointly demonstrating that the uniform pore architecture of QL-COFs guides homogeneous Na<sup>+</sup> electrodeposition. The modified separator enables symmetric cells to achieve 1300-h cycling stability and empowers a sodium metal capacitor to deliver 203.33 Wh kg<sup>-1</sup> at an ultrahigh power density of 24,000 W kg<sup>-1</sup>, surpassing the performance metrics of previously reported devices. This work first elucidates the mechanism of QL-COF-modified separators in accelerating Na<sup>+</sup> migration, expands the application boundaries of COF materials, and proposes a new paradigm for constructing scalable sodium metal capacitors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104599"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026045","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
The modulation of adsorption balance effect for promoting selenium cathode redox reaction kinetics in aqueous zinc-selenium battery 调节吸附平衡效应促进锌硒水电池中硒阴极氧化还原反应动力学
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-10 DOI: 10.1016/j.ensm.2025.104604
Huiting Xu , Shiyuan Fan , Huibin Liu , Peng Guo , Nanxing Ji , Chunli Li , Honghai Wang , Wenchao Peng , Xiaobin Fan , Jiapeng Liu
{"title":"The modulation of adsorption balance effect for promoting selenium cathode redox reaction kinetics in aqueous zinc-selenium battery","authors":"Huiting Xu ,&nbsp;Shiyuan Fan ,&nbsp;Huibin Liu ,&nbsp;Peng Guo ,&nbsp;Nanxing Ji ,&nbsp;Chunli Li ,&nbsp;Honghai Wang ,&nbsp;Wenchao Peng ,&nbsp;Xiaobin Fan ,&nbsp;Jiapeng Liu","doi":"10.1016/j.ensm.2025.104604","DOIUrl":"10.1016/j.ensm.2025.104604","url":null,"abstract":"<div><div>Aqueous zinc-selenium (Zn-Se) battery shows promising applications because of its inherent safety and high theoretical capacity. However, the slow redox reaction kinetics of Se cathode limit its development. The strategy of designing functional catalytic host materials with suitable adsorption ability is essential to promote Se redox reaction kinetics. We construct a catalytic host material consisting of axially oxygen-coordinated Cu single atoms and neighboring Cu atomic clusters (Cu-N<sub>4</sub>O/Cu<sub>ACs</sub>) to probe its modulation mechanism of suitable adsorption ability on Se redox reaction. The Cu-N<sub>4</sub>O/Cu<sub>ACs</sub> enable the aqueous Zn-Se battery to exhibit a specific capacity of 643 mAh g<sup>–1</sup> at 0.2 A g<sup>–1</sup> and fast Se redox reaction kinetics. Experimental characterization and density functional theory confirm the “adsorption balance effect” of Cu-N<sub>4</sub>O/Cu<sub>ACs</sub>. The neighboring Cu<sub>ACs</sub> can enhance the adsorption ability for Se species. The axially coordinated O atoms can promote electron delocalization and downshift d-band center, weakening the excess adsorption ability brought by Cu<sub>ACs</sub> and lowering the energy barrier of redox reaction. The adsorption balance effect between clusters of Cu<sub>ACs</sub> and axial O atom causes Cu-N<sub>4</sub>O/Cu<sub>ACs</sub> to exhibit excellent catalytic effect. This work gives new insights for the optimization of the catalytic behavior between the adsorption ability of SACs and redox reaction kinetics in aqueous Zn-Se battery.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104604"},"PeriodicalIF":20.2,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145043675","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
Constructing stable high-energy polymer-based all-solid-state lithium battery at room temperature through breaking multi-electron transfer barriers 突破多电子转移势垒构建室温稳定高能聚合物全固态锂电池
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-09 DOI: 10.1016/j.ensm.2025.104595
Tenghui Wang, Butian Chen, Taiguang Li, Chong Liu, Xiangfeng Liu
{"title":"Constructing stable high-energy polymer-based all-solid-state lithium battery at room temperature through breaking multi-electron transfer barriers","authors":"Tenghui Wang,&nbsp;Butian Chen,&nbsp;Taiguang Li,&nbsp;Chong Liu,&nbsp;Xiangfeng Liu","doi":"10.1016/j.ensm.2025.104595","DOIUrl":"10.1016/j.ensm.2025.104595","url":null,"abstract":"<div><div>Matching polymer-inorganic composite electrolytes (PICEs) with ultrahigh-nickel cathode (LiNi<sub>x</sub>Co<sub>y</sub>Mn<sub>1−x−y</sub>O<sub>2</sub>, <em>x</em> ≥ 0.9) ​​is highly anticipated for​ high-energy-density all-solid-state lithium batteries (ASSLBs). However, at room temperature (RT), PICEs confront some critical bottlenecks i.e. sluggish interfacial/intrinsic Li<sup>+</sup> transport kinetics, unstable interface to ultrahigh-nickel cathode and Li metal, and poor cycling stability, which severely hinders their practical applications. Herein, we successfully construct stable high-energy-density ASSLBs based on poly (ethylene oxide)-based PICEs and LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub> cathode via breaking multi-electron transfer barriers-induced interfacial self-reconfigurations. Multi-functional electrocatalytic activity additive [(CH<sub>3</sub>CN)<sub>4</sub>Cu(I)]BF<sub>4</sub> preferentially break the reaction energy barriers of four/six electrons and even direct eight-electrons transfer kinetics in NO<sub>3</sub><sup>−</sup> reduction chemistry, and subsequently accelerates the bond cleavage kinetics of multi-anions. The <em>in-situ</em> formed Li<sub>2</sub>O-Li<sub>3</sub>N-LiF-rich superlithiophilic gradient interphase enables the fast Li<sup>+</sup> transport kinetics (<em>t<sub>Li</sub><sup>+</sup></em> = 0.73, σ= 5.5 × 10<sup>−4</sup> S cm<sup>−1</sup>) at RT and a long-term cycling stability. The assembled LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub>-based ASSLBs exhibit a super-high specific capacity (228.8 mAh g<sup>−1</sup>@0.1C) and a high energy density (811.7 Wh kg<sub>cathode</sub><sup>−1</sup>@0.2C), an ultrahigh cycling stability (95.1 %@500 [email protected]) and a high-rate performance (89.2 % retention @400 cycles@1C with zero voltage decay). This work fundamentally addresses the critical issues in PICEs-based ASSLBs and should accelerate the development and practical applications of high-energy-density ASSLBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104595"},"PeriodicalIF":20.2,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017685","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
Synergizing self-expandable ion channels and electrokinetic phenomena in supramolecular anodes enables extremely fast-charging lithium-ion batteries 协同自膨胀离子通道和超分子阳极中的电动现象使极快充电的锂离子电池成为可能
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-09 DOI: 10.1016/j.ensm.2025.104593
Wenjing Zhang, Huang Xiao, Xin Cheng, Cong Tian, Jian Gao, Zhongqiang Wang, Yunfeng Zheng, Fang Li, Guoxing Li
{"title":"Synergizing self-expandable ion channels and electrokinetic phenomena in supramolecular anodes enables extremely fast-charging lithium-ion batteries","authors":"Wenjing Zhang,&nbsp;Huang Xiao,&nbsp;Xin Cheng,&nbsp;Cong Tian,&nbsp;Jian Gao,&nbsp;Zhongqiang Wang,&nbsp;Yunfeng Zheng,&nbsp;Fang Li,&nbsp;Guoxing Li","doi":"10.1016/j.ensm.2025.104593","DOIUrl":"10.1016/j.ensm.2025.104593","url":null,"abstract":"<div><div>The sluggish lithium (Li)-ion transport kinetics in anodes limit fast-charging performance of Li-ion batteries. Here, we develop a self-assembled tetralithium carboxylated porphyrin (SA-TCPP-Li) supramolecular anode with efficient Li-ion diffusion for high-performance fast-charging Li-ion batteries. Conjugated functional groups and self-assembled framework endow SA-TCPP-Li with ordered, fast and self-expandable transport channels as well as promoted electrokinetic phenomena, significantly improving Li-ion transport kinetics. Largely delocalized π electrons and ordered Li carboxylate groups promote anion decomposition to form LiF-rich solid-electrolyte interphase. Consequently, SA-TCPP-Li anodes exhibit exceptional fast-charging capability with a high capacity of 350 mA h g⁻¹ (72% of the capacity at 0.5 A g<sup>−1</sup> delivered in 2 minutes) and an ultra-long lifespan over 30,000 cycles at 10 A g⁻¹. Full cells paired with LiFePO<sub>4</sub> cathodes demonstrate remarkable fast-charging performance with negligible capacity decay over 2550 cycles at an extremely high rate of 6 C (1 C = 170 mA g<sup>−1</sup>).</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104593"},"PeriodicalIF":20.2,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145017684","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
Comprehensive review of thermal management strategies for lithium-ion batteries: from heat generation mechanism to advanced cooling solutions 锂离子电池热管理策略综述:从热产生机制到先进的冷却解决方案
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-09 DOI: 10.1016/j.ensm.2025.104597
Kai Du , Guopeng Chen , Yuheng Zhang , Shuo Li , Benqi Shi , Tianze Zhang , Junhao Liu , Fengxiang Chen , Shangzhen Xie , Zhiguang Guo
{"title":"Comprehensive review of thermal management strategies for lithium-ion batteries: from heat generation mechanism to advanced cooling solutions","authors":"Kai Du ,&nbsp;Guopeng Chen ,&nbsp;Yuheng Zhang ,&nbsp;Shuo Li ,&nbsp;Benqi Shi ,&nbsp;Tianze Zhang ,&nbsp;Junhao Liu ,&nbsp;Fengxiang Chen ,&nbsp;Shangzhen Xie ,&nbsp;Zhiguang Guo","doi":"10.1016/j.ensm.2025.104597","DOIUrl":"10.1016/j.ensm.2025.104597","url":null,"abstract":"<div><div>Lithium-ion batteries (LIBs) are pivotal in decarbonizing transportation due to their high energy density and efficiency. However, their long-term performance and safety critically depend on effective thermal management, as excessive heat accumulation can precipitate catastrophic failures like thermal runaway. This review systematically analyzes LIB thermal dynamics, beginning with the fundamental operational principles and heat generation mechanisms, followed by an in-depth examination of thermal runaway triggers. We then present a dual-pathway approach to thermal management: Internal strategies focus on material-level modifications to reduce heat generation and enhance thermal conduction, while external strategies evaluate four advanced cooling techniques, including liquid cooling, phase change materials, thermoelectric coolers, and heat pipes, with detailed discusSiOns on their heat transfer physics, efficiency, and implementation challenges. Furthermore, concerning the issue of thermal runaway propagation, the article presents reasonable countermeasures. To enable the prediction of battery behavior, the article introduces the Battery Management System (BMS) and two prediction methods (model-based and AI-based methods) in its final part, and also provides thermal management solutions for battery systems other than lithium-ion batteries, with sodium-ion batteries as an example. By integrating theoretical insights with practical applications, this review not only synthesizes the state-of-the-art in LIB thermal management but also provides actionable guidelines for researchers and engineers to optimize battery safety and durability in next-generation energy storage systems.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104597"},"PeriodicalIF":20.2,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145018098","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
Deep-learning based prediction of chemo-mechanics and damage in battery active materials 基于深度学习的电池活性材料化学力学和损伤预测
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-08 DOI: 10.1016/j.ensm.2025.104581
Zehou Wang , Ying Zhao , Zheng Zhong , Bai-Xiang Xu
{"title":"Deep-learning based prediction of chemo-mechanics and damage in battery active materials","authors":"Zehou Wang ,&nbsp;Ying Zhao ,&nbsp;Zheng Zhong ,&nbsp;Bai-Xiang Xu","doi":"10.1016/j.ensm.2025.104581","DOIUrl":"10.1016/j.ensm.2025.104581","url":null,"abstract":"<div><div>Layer-structured cathode active materials of Li-ion batteries such as <figure><img></figure> (NMC) provide benefits including high specific capacity and energy density. However, NMC materials (secondary particles) consist of randomly oriented grains (primary particles), which features anisotropic lattice chemical strain inside each grain and weak intergranular bonding. During <figure><img></figure> insertion into and extraction from the active material, high stresses arise at the interfaces between primary particles and particle disconnection occurs. Therefore, material microstructure characteristics such as grain orientation and morphology play a critical role in determining cycling performance of the active material. However, resolving particle microstructures with different characteristics remains challenging due to high computational costs and limited statistical generalizability. In this work, ConvLSTM is employed to predict the dynamic evolution of critical physical fields — including <figure><img></figure> concentration, stresses and damage — inside secondary particles with diverse microstructures. First, the microstructure of active particles are generated with a certain number of primary particles, whose sizes and orientations can strictly follow given statistical distributions with binning method, even with limited particle numbers. Second, images carrying essential characteristics of microstructure evolution are incorporated into the model. A hybrid loss combining Mean Squared Error (MSE) and Structural Similarity Index (SSIM) is employed, along with a scheduled sampling training strategy, to enhance prediction accuracy. The model’s out-of-sample predictive performance has also been evaluated. Additionally, a microcrack density-based damage model is also used to assess microstructure damage evolution. This work reveals that the proposed approach achieves highly accurate predictions, providing valuable insights into microstructure behavior.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104581"},"PeriodicalIF":20.2,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145018099","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
Reversible Mn3+/Mn2+ redox chemistry for high-rate aqueous manganese-ion batteries 高倍率锰离子电池的可逆Mn3+/Mn2+氧化还原化学
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-08 DOI: 10.1016/j.ensm.2025.104598
Wenfang Yuan , Lejuan Cai , Lisha Lu , Qian Chen , Mengxiang Han , Zihua Li , Fan Zhang , Yingying Lan , Jian Shang , Bocheng Qiu , Wenlong Wang
{"title":"Reversible Mn3+/Mn2+ redox chemistry for high-rate aqueous manganese-ion batteries","authors":"Wenfang Yuan ,&nbsp;Lejuan Cai ,&nbsp;Lisha Lu ,&nbsp;Qian Chen ,&nbsp;Mengxiang Han ,&nbsp;Zihua Li ,&nbsp;Fan Zhang ,&nbsp;Yingying Lan ,&nbsp;Jian Shang ,&nbsp;Bocheng Qiu ,&nbsp;Wenlong Wang","doi":"10.1016/j.ensm.2025.104598","DOIUrl":"10.1016/j.ensm.2025.104598","url":null,"abstract":"<div><div>The Mn<sup>3+</sup>/Mn<sup>2+</sup> redox couple is a promising candidate for high-rate energy storage scenarios owing to its high theoretical voltage and rapid redox kinetics. However, critical challenges such as Mn<sup>3+</sup> disproportionation and shuttle effects in aqueous electrolytes significantly limit practical implementation. Herein, we propose a synergistic strategy integrating coordination optimization and interfacial confinement to achieve highly reversible Mn<sup>3+</sup>/Mn<sup>2+</sup> redox chemistry in a mild aqueous electrolyte. Ethylenediaminetetraacetic coordinating anions are utilized to reshape the first solvation shell of Mn<sup>2+</sup>, stabilizing hydrated Mn<sup>3+</sup> intermediates and enabling a single-electron-dominated redox pathway. A sucrose-derived molecular adsorption layer is engineered on the cathode surface through electrostatic polarity interactions, effectively suppressing Mn<sup>3+</sup> migration into the bulk electrolyte. The well-designed Mn<sup>3+</sup>/Mn<sup>2+</sup> cathode delivers an areal capacity of 0.36 mAh cm<sup>−2</sup> at 4 mA cm<sup>−2</sup> with 81 % capacity retention over 3000 cycles. As proof of concept, a high-rate aqueous Mn-ion battery is assembled by pairing the Mn<sup>3+</sup>/Mn<sup>2+</sup> cathode with a polyimide anode, achieving a specific capacity of 104 mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup>, exceptional rate capability, and 73.2 % capacity retention after 1000 cycles. This work unveils the directional regulation of manganese redox chemistry by a solvation-interfacial coupling mechanism, offering a design blueprint for next-generation grid-scale energy storage technologies.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104598"},"PeriodicalIF":20.2,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009324","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
Mitigating the fast-charging limitations of graphite anodes via g-C3N4 surface engineering 通过g-C3N4表面工程减轻石墨阳极的快速充电限制
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-09-07 DOI: 10.1016/j.ensm.2025.104596
Joo Hyeong Suh , Hong Rim Shin , Taehee Kim , Dong Ki Kim , Ki Jae Kim , Jong-Won Lee , Min-Sik Park
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