Energy Storage Materials最新文献

Additive-Induced Interfacial Chemistry: The Key to Next-Generation Lithium Metal Batteries 添加剂诱导界面化学：下一代锂金属电池的关键

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104650

Lei Sun, Gongxun Lu, Qingyue Han, Hongyan Li, Ouwei Sheng, Chengbin Jin

{"title":"Additive-Induced Interfacial Chemistry: The Key to Next-Generation Lithium Metal Batteries","authors":"Lei Sun, Gongxun Lu, Qingyue Han, Hongyan Li, Ouwei Sheng, Chengbin Jin","doi":"10.1016/j.ensm.2025.104650","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104650","url":null,"abstract":"The practical deployment of high-energy-density lithium metal batteries is critically hindered by their poor cycling stability, stemming from inherent electrode/electrolyte interfacial instability. Addressing this challenge requires strategic electrolyte design to stabilize electrode interfaces (that is, solid-electrolyte interphase) and suppress parasitic side reactions. Among the most promising approaches, electrolyte additives stand out by selectively modifying interfacial chemistry through in-situ chemical or electrochemical reactions, effectively prolonging battery lifespan without compromising energy density. This review transcends conventional classification by chemical composition or phase, proposing a mechanism-based framework that categorizes additives as decomposable, suspension, sustained-release, and electrode-adsorbing functional chemical regulators. By addressing practical challenges, it systematically elucidates how molecular structures and physicochemical properties govern interfacial reactions and electrochemical performance, particularly their interactions with bulk/interface chemistries. Furthermore, it offers forward-looking strategies emphasizing synergistic integration of interfacial engineering and data-driven approaches like artificial intelligence to predict molecular reactivity and interfacial efficiency. These insights deepen fundamental understanding of additive mechanisms, accelerating the design of next-generation additives through tailored liquid/interface chemistry for stable high-performance lithium metal batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"23 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216256","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

Dynamic interface engineering of softening metal-inorganic framework for dendrite-free zinc anodes 无枝晶锌阳极软化金属-无机骨架的动态界面工程

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104656

Yuqing Luo, Jiugang Hu, Jia Luo, Shan Cai, Lili He, Chengguo Wei, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji

{"title":"Dynamic interface engineering of softening metal-inorganic framework for dendrite-free zinc anodes","authors":"Yuqing Luo, Jiugang Hu, Jia Luo, Shan Cai, Lili He, Chengguo Wei, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji","doi":"10.1016/j.ensm.2025.104656","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104656","url":null,"abstract":"Rechargeable aqueous zinc-ion batteries (AZIBs) face significant challenges from zinc dendrites and side reactions, causing capacity decay and poor cycling stability. Herein, a dynamically softening zincophilic Zn(CN)2 metal-inorganic framework was in situ constructed on zinc foil (Zn(CN)2-Zn) via a vapor-phase etching strategy. In situ Raman monitoring revealed the dynamic interfacial transition from dense nonporous Pn3m phase to hexagonal P63/mmc phase (Lon-Zn(CN)2) during cycling. The resulting Lon-Zn(CN)2 framework features nanoconfined hexagonal linear channels that accelerate Zn2+ desolvation and enable uniform ion transport. In situ synchrotron radiation X-ray imaging and COMSOL simulations further confirmed that this structural transition homogenizes interfacial electric field and ensures excellent plating/stripping reversibility. Moreover, the high lattice matching between Lon-Zn(CN)2 (001) and Zn(002) planes promotes epitaxial zinc deposition while suppressing dendrite formation. Consequently, the Zn(CN)2-Zn electrode achieves stable cycling for over 3200 hours at 0.5 mA cm⁻² in symmetrical cells and superior rate performance with a capacity retention rate of 99.6% in full cells. This work demonstrates synergistic regulation of ion transport and crystallographic orientation via dynamic metal-inorganic framework engineering, providing a novel strategy for durable and dendrite-free AZIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"1 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216263","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

Advanced Ti-based multi-electron pair electro-active solid halide electrolyte for all-solid-state lithium batteries 全固态锂电池用新型钛基多电子对电活性固体卤化物电解质

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104651

Yibo Zhang, Shidong Li, Yihui Li, Li Yang, Jianyong Zhang, Yuyang Cai, Xin Tong, Xueya Zhang, Jingyuan Yu, Xin Pan, Jinxiao Liu, Shuai Huang, Aiqi Yi, Botao Wu, Ahmed Eissa Abdelmaoula, Salah Abdelghany Eleissawy Salman, Zhenzhen Dou, Lin Xu

{"title":"Advanced Ti-based multi-electron pair electro-active solid halide electrolyte for all-solid-state lithium batteries","authors":"Yibo Zhang, Shidong Li, Yihui Li, Li Yang, Jianyong Zhang, Yuyang Cai, Xin Tong, Xueya Zhang, Jingyuan Yu, Xin Pan, Jinxiao Liu, Shuai Huang, Aiqi Yi, Botao Wu, Ahmed Eissa Abdelmaoula, Salah Abdelghany Eleissawy Salman, Zhenzhen Dou, Lin Xu","doi":"10.1016/j.ensm.2025.104651","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104651","url":null,"abstract":"The development of high-energy-density all-solid-state lithium batteries (ASSLBs) hinges critically on the design of advanced composite cathode components. While significant progress has been made in optimizing solid electrolytes as separators, the advancement of catholytes—particularly those combining multi-electron pair redox activity, high ionic conductivity, and mechanical compressibility—remains underexplored. A key challenge in current composite cathodes is the non-negligible high loading of electro-inactive electrolytes, which drastically reduces the energy density of the ASSLBs. To address this limitation, we propose an alternative strategy to improve the energy density by using Li2.6Ti0.6Zr0.4Cl6 as an electro-active catholyte with multi-electron pair. This material exhibits exceptional ionic conductivity (1.39 mS cm–1 at 25°C) while simultaneously delivering a highly reversible specific capacity of approximately 90.62 mAh g–1. Aliovalent Ti substitution enhances ionic conductivity through a structural transition from high-symmetry to low-symmetry space groups, coupled with a crystallinity strengthening effect. Moreover, the composite cathode of Li2.6Ti0.6Zr0.4Cl6 and LiFePO4 reveals an impressive initial discharge capacity of 258.97 mAh g–1LFP. This work introduces a new type of functional electro-active catholyte, significantly enhancing the energy density and cost-effectiveness of ASSLBs, opening new avenues for the development of next-generation solid-state battery technologies.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"4 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216264","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

Operando characterisation of Na-Zn molten salt batteries using X-ray radiography: insights into performance degradation and cell failure 使用x射线摄影技术对Na-Zn熔盐电池的操作特性进行表征：对性能下降和电池失效的见解

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104654

Martins Sarma, Natalia Shevchenko, Norbert Weber, Tom Weier

{"title":"Operando characterisation of Na-Zn molten salt batteries using X-ray radiography: insights into performance degradation and cell failure","authors":"Martins Sarma, Natalia Shevchenko, Norbert Weber, Tom Weier","doi":"10.1016/j.ensm.2025.104654","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104654","url":null,"abstract":"The sodium-zinc system for grid-scale energy storage is a compelling solution due to its high cell voltage (1.8 V) and Earth abundance, resulting in minimal active material costs. Since the proposal of the cell concept, the research has been based on the assumption that separating the electrolyte into anolyte and catholyte using a porous medium to limit the molten salt mixing is essential for cell operation. This is deemed crucial in order to confine the produced ZnCl2 to the vicinity of the Zn pool and to reduce the probability of a direct contact between ZnCl2 and Na, which would result in self-discharge. However, the constructed cells have not demonstrated consistent performance over extended periods of more than a few weeks. Through in situ operation of the cells at an X-ray beamline, the underlying causes of battery failure have been identified, facilitating a conceptual overhaul of the cell design. It is demonstrated that the separator is not only unnecessary, but is the reason for cell failure. Its elimination enables a significant simplification of the design, while simultaneously ensuring stable cycling.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"28 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216258","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

Local Disordered Li2.7Zr0.3In0.7Cl6 for High Stable All Solid-state Batteries 高稳定全固态电池的局部无序Li2.7Zr0.3In0.7Cl6

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104655

Peiyao Wang, Li Shen, Shuang Wu, Chenyao Ma, Xudong Chen, Shigang Lu, Yongyao Xia, Yufeng Zhao, Wuliang Feng

{"title":"Local Disordered Li2.7Zr0.3In0.7Cl6 for High Stable All Solid-state Batteries","authors":"Peiyao Wang, Li Shen, Shuang Wu, Chenyao Ma, Xudong Chen, Shigang Lu, Yongyao Xia, Yufeng Zhao, Wuliang Feng","doi":"10.1016/j.ensm.2025.104655","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104655","url":null,"abstract":"All solid-state batteries (ASSBs) enlighten the development of next secondary batteries with high energy density and safety, but still suffer from the obstacles of mechanical failure and sluggish ionic transportation. Herein, we present a quench induced local disordered Li2.7Zr0.3In0.7Cl6 (LZIC) halide solid electrolyte, which shows prominent compressibility and ionic conductivity. Mechanically, quench ‘freeze’ the high temperature state of LZIC, transforming LZIC from conventional high rigid crystalline state to softer local disordered glass-ceramics, thus significantly curtails the Young’s modulus from 53.5 GPa to 11.8 GPa. Ionic conductively, local disordering not only reduces the grain boundary resistance as the improved ionic conduction consecutiveness, but also promotes the bulk ionic transportation kinetics as the increased defects and enlarged lattice volume, which synergistically increased the ionic conductivity of LZIC from 1.07 mS/cm to 4.25 mS/cm. The co-promoted compressibility and ionic transportation of LZIC enabled a stable cycling of ASSBs at an ultra-low stack pressure of 3 MPa, thus providing new theoretical and technical approaches for the industrialization of ASSBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"164 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216257","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

Interface-driven phase stability enables co-sintered composite anodes for intrinsically safe all-solid-state-batteries 界面驱动的相稳定性使共烧结复合阳极具有本质安全的全固态电池

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-04 DOI: 10.1016/j.ensm.2025.104653

Pengpeng Dai, Shuyu Zhou, Junhong Liao, Yuxin Liu, Yudong Liu, Haoran Li, Zheng Yue, Guozhong Cao, Shixi Zhao

{"title":"Interface-driven phase stability enables co-sintered composite anodes for intrinsically safe all-solid-state-batteries","authors":"Pengpeng Dai, Shuyu Zhou, Junhong Liao, Yuxin Liu, Yudong Liu, Haoran Li, Zheng Yue, Guozhong Cao, Shixi Zhao","doi":"10.1016/j.ensm.2025.104653","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104653","url":null,"abstract":"The development of all-solid-state batteries (ASSBs) is hindered by interfacial instability between solid-electrolytes (SEs) and Li metal anodes. In this work, we propose a co-sintered composite anode strategy based on Li4Ti5O12 (LTO), a ‘zero-strain’ anode material, to address interfacial challenges in NASICON-type systems. Systematic investigations reveal that LTO undergoes progressive phase decomposition during co-sintering with Li1.3Al0.3Ti1.7(PO4)3 (LATP) due to the thermodynamic driving force from Li chemical potential difference and the high reactivity of phosphate groups. In contrast, LTO maintains structural integrity and chemical compatibility up to 900 °C when co-sintered with Li0.33La0.56TiO3 (LLTO). Additionally, thermodynamic instability between LATP and LLTO at high-temperatures is observed, indicating challenges in multi-electrolyte integration. Notably, the preferential Li loss from LLTO within the LTO+LLTO composite anode during co-sintering with LATP pellet exerts a protective effect for LTO, helping to maintain the structural integrity of LTO. Building upon these findings, an integrated (LTO+LLTO)|LATP bilayer structure is successfully fabricated via co-sintering at 600°C. This work offers critical insights into phase evolution and interfacial chemistry for coupling SEs with anode materials, guiding the rational design of co-sintering composite anodes and demonstrating a promising pathway toward intrinsically safe ASSBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"13 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216260","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

Selective Proton Acceleration Channel via Gradient Built-in Electric Field Strategy for High-performance Zinc-ion Batteries 基于梯度内建电场策略的高性能锌离子电池选择性质子加速通道

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-03 DOI: 10.1016/j.ensm.2025.104647

Hongfeng Jia, Yanxin Li, Bingqiu Liu, Lingyu Zhang, Lu Li, Haozhi Wang, Chungang Wang

{"title":"Selective Proton Acceleration Channel via Gradient Built-in Electric Field Strategy for High-performance Zinc-ion Batteries","authors":"Hongfeng Jia, Yanxin Li, Bingqiu Liu, Lingyu Zhang, Lu Li, Haozhi Wang, Chungang Wang","doi":"10.1016/j.ensm.2025.104647","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104647","url":null,"abstract":"In the emerging energy storage mechanism of Zn2+ and proton (H+) co-embedding in aqueous zinc ion batteries (ZIBs), H+ with minimal molar mass and fast (un)coordination kinetics significantly alleviate the structural strain to boost the cycling stability. Yet, existing storage mechanisms make the high percentage of proton storage limited. Here, an entropy-modulated gradient built-in electric field strategy is employed to construct selective proton transport channels and provide proton immobilization sites to enhance proton storage. Through experimental and theoretical analyses of materials with different entropy values, the unique charge characteristics of high-entropy materials resulting in the gradient built-in electric fields inside the materials to form a continuous ion transport pathway are demonstrated. Compared with Zn2+, H+ with high charge-to-mass ratio and low transport energy barrier enable more continuous and rapid ion transport in the accelerated channel to selectively modulate the H+ transport kinetics. Additionally, the multiple active centers of the gradient built-in electric field serve as immobilizers for proton embedding, which markedly enhances the binding capacity of protons in the material. These findings provide insight into the essential function of the entropy-regulated gradient built-in electric field mechanism for proton-selective storage, and provide a new reference for developing high-performance ZIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"75 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209387","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

Heteroatoms doped holey graphene enhanced carbon frameworks with chemical pre-lithiation affording reversible lithium plating/stripping in anode-free lithium metal batteries 杂原子掺杂多孔石墨烯增强碳框架与化学预锂化提供可逆的锂电镀/剥离无阳极锂金属电池

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-03 DOI: 10.1016/j.ensm.2025.104648

Mingliang Bai, Min Zhong, Xuchang Tang, Wenzhuo Shen, Jiali Zhang, Shouwu Guo

{"title":"Heteroatoms doped holey graphene enhanced carbon frameworks with chemical pre-lithiation affording reversible lithium plating/stripping in anode-free lithium metal batteries","authors":"Mingliang Bai, Min Zhong, Xuchang Tang, Wenzhuo Shen, Jiali Zhang, Shouwu Guo","doi":"10.1016/j.ensm.2025.104648","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104648","url":null,"abstract":"The host electrode plays a pivotal role in facilitating the lithium plating and stripping in anode-free lithium metal batteries (AF-LMBs). In the work, we design and fabricate a series of hierarchical carbon frameworks composed of cellulose-derived carbon fibers, holey graphene doped with heteroatoms (B, N, F), and lithium salts, to address the challenges of low coulombic efficiency, poor lithium plating and stripping, and rapid capacity fading of AF-LMBs. The holey graphene provides abundant lithium nucleation sites, leading to uniform plating/stripping, and lower Fermi level of the host electrode, thereby helping to suppress side reactions. The pre-lithiation improves the initial coulombic efficiency to >100 % by offsetting irreversible first-cycle consumption. In parallel, heteroatom doping tends to promote a beneficial, inorganically enriched SEI, thereby reinforcing interfacial stability during lithium plating/stripping. The AF-LMBs assembled with the as-prepared hierarchical carbon frameworks as host electrodes, and NCM811 as cathodes deliver exceptional cycling stability, retaining ∼72 % and ∼67 % of capacity after 100 cycles at 1.93//1.93 mA cm⁻² and 1.93//3.86 mA cm⁻² with carbonate-based electrolyte.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"327 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216265","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

Green and Economically Viable Dry-Electrode Manufacturing for High-Energy-Density Lithium Batteries 绿色和经济可行的高能量密度锂电池干电极制造

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-03 DOI: 10.1016/j.ensm.2025.104649

Kun Cao, Jingqin Ji, Yanlan Zhao, Kaiyan Wang, Lixi Zeng, Li Wang, Xiangming He

{"title":"Green and Economically Viable Dry-Electrode Manufacturing for High-Energy-Density Lithium Batteries","authors":"Kun Cao, Jingqin Ji, Yanlan Zhao, Kaiyan Wang, Lixi Zeng, Li Wang, Xiangming He","doi":"10.1016/j.ensm.2025.104649","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104649","url":null,"abstract":"The global transition to electrification is driving the demand for lithium-ion batteries (LIBs) with higher energy density, lower cost, and reduced environmental footprint. Conventional slurry-based electrode manufacturing, which relies on toxic solvents and energy-intensive drying processes, poses significant economic and environmental challenges. Solvent-free dry electrode technology has emerged as a transformative alternative to overcome these limitations. This review provides a comprehensive and critical analysis of the dry process from three pivotal perspectives: economic advantages, environmental benefits, and performance superiority, conducting a multidimensional comparative analysis with slurry-process electrode manufacturing. The scientific principles behind these advantages are elucidated through microstructural and electrochemical characterization. Meanwhile, comparative life cycle assessment (LCA) data are employed to demonstrate the significant advantages of dry electrodes in terms of energy consumption and carbon emissions. Regarding application potential, leveraging Tesla's successful industrial application case, we explore the broad prospects of dry electrodes in LIBs, solid-state batteries, and other domains. Finally, in the context of the rapidly advancing dry electrode technology, we highlight the severe challenges that remain before truly achieving industrial-scale application. This work offers a holistic theoretical foundation and practical guidance for adopting dry electrode technology as a core strategy for sustainable battery manufacturing.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"37 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145216123","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

Highly Selective and Near-Complete Electrochemical Recovery of Cobalt and Nickel from Spent Batteries through Mutifunctional Deep Eutectic Solvent 利用多功能深共晶溶剂从废电池中高选择性、近完全电化学回收钴和镍

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-10-02 DOI: 10.1016/j.ensm.2025.104646

Seongmin Choi, Kenta Motobayashi, Kwiyong Kim

{"title":"Highly Selective and Near-Complete Electrochemical Recovery of Cobalt and Nickel from Spent Batteries through Mutifunctional Deep Eutectic Solvent","authors":"Seongmin Choi, Kenta Motobayashi, Kwiyong Kim","doi":"10.1016/j.ensm.2025.104646","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104646","url":null,"abstract":"Electrochemical recovery presents a sustainable route for battery recycling, yet it is hindered by a trade-off between achieving purity and yield. This challenge arises because, as the target metal depletes during electrodeposition, mass transport limitations reduce its availability, thereby shifting the electrochemical environment in favor of co-deposition of competing metal – particularly during prolonged deposition intended for near-complete recovery. Here, we report a strategy that leverages a multifunctional deep eutectic solvent (DES), ethaline, where ethylene glycol preferentially coordinates with nickel while chloride stabilizes cobalt as tetrachlorocobaltate complexes. Even at elevated temperatures, where nickel undergoes a partial thermochromic transition to chloride coordination, the system maintains a broadened Ni–Co separation window of ∼0.3 V at 85°C. By fine-tuning the applied potential and utilizing the intrinsic chlorine redox activity of the DES, self-purification was achieved during electrodeposition, yielding a Ni/Co separation factor >3,000 and >97% nickel recovery in a single-step electrodeposition from a synthetic Ni/Co mixture. Building upon this binary separation, we developed a sequential strategy to recover nickel, cobalt, and manganese from real battery leachates. Applied to real NMC leachates, our process enabled the sequential recovery of nickel, cobalt, and manganese with purities of 99.1%/96.3% (NMC111) and 99.2%/98.8% (NMC811) for nickel and cobalt, respectively, all with >95% recovery. For NMC111, >97% nickel purity and >93% cobalt purity were retained over repeated reuse of the DES, enabling minimal wastewater discharge, with Cl2-assisted refining enhancing purity to >99.9%. A technoeconomic analysis validated the economic feasibility and revealed further potential through thermal optimization.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"39 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145209391","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