Pub Date : 2026-03-25DOI: 10.1016/j.ensm.2026.105059
Zeba Khanam, Shu Jiang, Li Luo, Ting Ouyang, Yongchao Huang, Hao Yang, M.-Sadeeq Balogun, Xihong Lu
Achieving sodium-ion batteries (NIBs) with high areal capacity and high-rate capability remains a critical challenge, as it necessitates practically thick electrodes. Conventional current collectors, however, suffer from interfacial instability, uncontrolled electron leakage, and nonuniform Na+ flux, which impose severe diffusion limitations and ultimately restricts rate capability and long-term stability of thick electrodes. Herein, we introduce a three-dimensional (3D) molybdenum oxide/nitride (Mo–O/N) heteronanowire current collector interface for concurrently enabling high-rate and high-capacity anodes with long-term durability. The Mo–O/N interface electronically modulates the current collector (denoted MMN/C) and integrates it with the molybdenum sulfide (MoS2) active layer into a monolith framework (denoted MS@MMN/C). The theoretical and experimental analyses reveals that this Mo–O/N interface design suppresses interfacial electron tunnelling through lowering the Fermi level (Ef), regulating mass/charge transfer, homogenizing Na+ flux, and allow uniform electric field and stress distribution to accelerate Na+ transport kinetics. It not only provides abundant active sites for active layer deposition but also facilitates robust SEI formation, thereby enhancing structural integrity. Consequently, monolith MS@MMN/C anode deliver high areal capacity up to ≈ 8 mAh cm−2, remarkable rate capability and stable cycling (up to 500 cycles) at 5 mA cm−2 for NIB. The work establishes MMN/C current collector as a versatile and scalable platform for next-generation high-rate Na-batteries and beyond.
实现高面积容量和高倍率的钠离子电池（nib）仍然是一个关键的挑战，因为它需要实际的厚电极。然而，传统的集流器存在界面不稳定、不受控制的电子泄漏和不均匀的Na+通量等问题，这些问题造成了严重的扩散限制，最终限制了厚电极的速率能力和长期稳定性。本文介绍了一种三维（3D）氧化钼/氮化钼（Mo-O /N）杂线集流接口，可同时实现具有长期耐用性的高速率和高容量阳极。Mo-O /N接口通过电子方式调制电流收集器（表示MMN/C），并将其与硫化钼（MoS2）活性层集成为一个整体框架（表示MS@MMN/C）。理论和实验分析表明，这种Mo-O /N界面设计通过降低费米能级（Ef）、调节质量/电荷传递、均匀化Na+通量、使电场和应力分布均匀从而加速Na+输运动力学来抑制界面电子隧穿。它不仅为活性层沉积提供了丰富的活性位点，而且促进了坚固的SEI形成，从而提高了结构的完整性。因此，单片MS@MMN/C阳极提供高达≈8 mAh cm - 2的高面容量，卓越的速率能力和稳定的循环（高达500次循环），在5 mA cm - 2的NIB。这项工作将MMN/C电流收集器确立为下一代高倍率钠电池的通用和可扩展平台。
{"title":"Electron-Repellent 3D Heteronanowire Current Collector Interface for Na-ion Conductive High Areal Capacity Anodes","authors":"Zeba Khanam, Shu Jiang, Li Luo, Ting Ouyang, Yongchao Huang, Hao Yang, M.-Sadeeq Balogun, Xihong Lu","doi":"10.1016/j.ensm.2026.105059","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105059","url":null,"abstract":"Achieving sodium-ion batteries (NIBs) with high areal capacity and high-rate capability remains a critical challenge, as it necessitates practically thick electrodes. Conventional current collectors, however, suffer from interfacial instability, uncontrolled electron leakage, and nonuniform Na<sup>+</sup> flux, which impose severe diffusion limitations and ultimately restricts rate capability and long-term stability of thick electrodes. Herein, we introduce a three-dimensional (3D) molybdenum oxide/nitride (Mo–O/N) heteronanowire current collector interface for concurrently enabling high-rate and high-capacity anodes with long-term durability. The Mo–O/N interface electronically modulates the current collector (denoted MMN/C) and integrates it with the molybdenum sulfide (MoS<sub>2</sub>) active layer into a monolith framework (denoted MS@MMN/C). The theoretical and experimental analyses reveals that this Mo–O/N interface design suppresses interfacial electron tunnelling through lowering the Fermi level (<em>E</em><sub>f</sub>), regulating mass/charge transfer, homogenizing Na<sup>+</sup> flux, and allow uniform electric field and stress distribution to accelerate Na<sup>+</sup> transport kinetics. It not only provides abundant active sites for active layer deposition but also facilitates robust SEI formation, thereby enhancing structural integrity. Consequently, monolith MS@MMN/C anode deliver high areal capacity up to ≈ 8 mAh cm<sup>−2</sup>, remarkable rate capability and stable cycling (up to 500 cycles) at 5 mA cm<sup>−2</sup> for NIB. The work establishes MMN/C current collector as a versatile and scalable platform for next-generation high-rate Na-batteries and beyond.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"29 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507688","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}
An advanced solid electrolyte interphase (SEI) is considered an effective strategy to regulate lithium (Li) deposition for promoting high-energy Li metal batteries. However, SEIs still fracture due to uneven Li+ flux and external stress accumulation leading to dendrite growth. Considering that the cracking is difficult to avoid and irreversible, the SEI with a homogeneous microcrack network structure is pre-constructed on Li metal via internal stress release inspired by the crackle glaze effect (cracks are not always bad for Li deposition). Herein, an artificial SEI composed of Li3N and Li-Al alloy is fabricated by magnetron sputtering AlN onto Li metal, which confers high ionic conductivity and lithiophilic compound at the microscale. Whereafter, at the mesoscale, a controllable annealing strategy is introduced to form numerous and homogeneous microcracks, which induces the improved uniformity of Li+ flux and appropriate stress release. Benefiting from this artificial SEI with cross-scale structural design, the corresponding Li||Li symmetric battery can cycle for 2000 h with low polarization at 3 mA cm-2, and the lifespan of full battery also exhibits a fourfold enhancement.
先进的固体电解质界面相（SEI）被认为是调控锂沉积的有效策略，可以促进高能锂金属电池的发展。然而，由于Li+通量不均匀和外部应力积累导致枝晶生长，SEIs仍然会断裂。考虑到裂纹的不可避免性和不可逆性，利用裂纹釉效应激发的内应力释放，在Li金属上预构建具有均匀微裂纹网络结构的SEI（裂纹并不总是不利于Li沉积）。本文通过磁控溅射制备了一种由Li3N和Li- al合金组成的人工SEI，该SEI具有高离子电导率和微尺度的亲锂化合物。然后，在中尺度，引入可控退火策略，形成大量均匀的微裂纹，提高了Li+通量的均匀性和适当的应力释放。得益于这种具有跨尺度结构设计的人工SEI，相应的Li||Li对称电池可以在3 mA cm-2的低极化下循环2000 h，并且电池的寿命也有4倍的提高。
{"title":"The Double-Edged Effect of Cracks in SEI for Li Metal Batteries","authors":"Yumin Liu, Xueyang Li, Guanwu Li, Yuan Yuan, Wei Zhang, Xinyan Zhou, Xuepeng Li, Hao Guo, Qing Liang, Xing Ou, Kan Zhang, Dong Wang, Weitao Zheng","doi":"10.1016/j.ensm.2026.105061","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105061","url":null,"abstract":"An advanced solid electrolyte interphase (SEI) is considered an effective strategy to regulate lithium (Li) deposition for promoting high-energy Li metal batteries. However, SEIs still fracture due to uneven Li<sup>+</sup> flux and external stress accumulation leading to dendrite growth. Considering that the cracking is difficult to avoid and irreversible, the SEI with a homogeneous microcrack network structure is pre-constructed on Li metal via internal stress release inspired by the crackle glaze effect (cracks are not always bad for Li deposition). Herein, an artificial SEI composed of Li<sub>3</sub>N and Li-Al alloy is fabricated by magnetron sputtering AlN onto Li metal, which confers high ionic conductivity and lithiophilic compound at the microscale. Whereafter, at the mesoscale, a controllable annealing strategy is introduced to form numerous and homogeneous microcracks, which induces the improved uniformity of Li<sup>+</sup> flux and appropriate stress release. Benefiting from this artificial SEI with cross-scale structural design, the corresponding Li||Li symmetric battery can cycle for 2000 h with low polarization at 3 mA cm<sup>-2</sup>, and the lifespan of full battery also exhibits a fourfold enhancement.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"14 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507686","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}
Pub Date : 2026-03-25DOI: 10.1016/j.ensm.2026.105060
Minjeong Gong, Yoonjung Choi, Han Mo Yang, Sang Bok Ma, Dong-Hwa Seo
Rapid, accurate diagnosis of the State of Health (SoH) is essential for the second-life applications of spent lithium-ion batteries. However, most diagnostic methods require pre-set conditions (such as voltage or state of charge), leading to time-consuming measurements. Here, we report a machine-learning-based SoH prediction process typically completed within 130 seconds without pre-settings. The process comprises two sequential steps: diagnostic protocol classification, which uses voltage data from a 10-second 1 C-rate discharge, and SoH regression, which predicts SoH from voltage responses collected under the selected diagnostic protocol. The models, trained on data from 18650 cells (LiNixCoyAlzO2/graphite) cycled under diverse conditions, demonstrated superior performance: the classification accuracy achieved 0.999, and the Mean Absolute Error (MAE) of the SoH regression yielded 0.85%. This process was successfully extended to 21700 cells without model retraining through feature engineering, achieving a 69.1% reduction in MAE by rescaling features using the cell capacity-to-external volume ratio. This pre-setting-free and rapid SoH diagnostic strategy offers a generalized, energy-efficient route for evaluating spent battery.
{"title":"Fast and direct diagnosis of states of health of spent batteries","authors":"Minjeong Gong, Yoonjung Choi, Han Mo Yang, Sang Bok Ma, Dong-Hwa Seo","doi":"10.1016/j.ensm.2026.105060","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105060","url":null,"abstract":"Rapid, accurate diagnosis of the State of Health (SoH) is essential for the second-life applications of spent lithium-ion batteries. However, most diagnostic methods require pre-set conditions (such as voltage or state of charge), leading to time-consuming measurements. Here, we report a machine-learning-based SoH prediction process typically completed within 130 seconds without pre-settings. The process comprises two sequential steps: diagnostic protocol classification, which uses voltage data from a 10-second 1 C-rate discharge, and SoH regression, which predicts SoH from voltage responses collected under the selected diagnostic protocol. The models, trained on data from 18650 cells (LiNi<sub>x</sub>Co<sub>y</sub>Al<sub>z</sub>O<sub>2</sub>/graphite) cycled under diverse conditions, demonstrated superior performance: the classification accuracy achieved 0.999, and the Mean Absolute Error (MAE) of the SoH regression yielded 0.85%. This process was successfully extended to 21700 cells without model retraining through feature engineering, achieving a 69.1% reduction in MAE by rescaling features using the cell capacity-to-external volume ratio. This pre-setting-free and rapid SoH diagnostic strategy offers a generalized, energy-efficient route for evaluating spent battery.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"44 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147507687","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}
{"title":"Distributed Force Field Heterogeneity for Early Sensing and Hierarchical Warning of Battery Thermal Runaway","authors":"Xianyi Jia, Jiangong Zhu, Donghai Chen, Chao Yu, Jixiang Cai, Linyue Xin, Xiaoyang Wang, Hong Ye, Wentao Xu, Haifeng Dai, Xuezhe Wei","doi":"10.1016/j.ensm.2026.105053","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105053","url":null,"abstract":"","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"17 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147496595","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}
Pub Date : 2026-03-22DOI: 10.1016/j.ensm.2026.105051
Saima Batool, Muhammad Idrees, Xingyu Chen, Kaishuai Yang, Li Jialin, Yang Zehao, Junguo Xu
The strategic engineering of heterostructured cathodes can significantly enhance lithium-ion storage kinetics and structural stability. Here, we report a 3D-printed V₂O₅-Ti₃C₂Tx-Au (3DP-VTA) cathode, in which an in-situ TiO₂ interface forms via synergistic interactions between V₂O₅, Ti₃C₂Tx, and Au nanoparticles. The TiO₂ interface introduces abundant oxygen vacancies that act as Li⁺ adsorption sites. Density functional theory (DFT) calculations confirm the presence of localized mid-gap states with reduced Li⁺ adsorption energy (Eₐd = -0.54 eV) and high orbital hybridization, which enhancing the electronic properties. Au NPs further contribute to interfacial redox dynamics, catalysis, and conductivity, forming Au-Ti intermetallics that act as conductive bridges, reduce interfacial resistance, and reinforce mechanical stability. Compared to pristine V₂O₅ (∼20% capacity), the 2D-VTA configuration doubles performance (∼40%), while 3D printing with Au synergy boosts it five-fold (∼100%) in half-cells. Full-cell assemblies retain ∼68% capacity, over three times higher than V₂O₅, demonstrating the efficacy of architectural and interfacial optimization. Electrochemical kinetics reveal predominantly surface-controlled behavior, with b-values of 0.96/0.84 (anodic/cathodic) and capacitive contributions increasing from 72.6% to 86.1% at 0.2-1.2 mV s⁻¹. XPS, TEM, and Raman analyses confirm TiO₂ interphase formation. EIS analysis shows 3DP-VTA (half-cell, 100%) has the best performance, followed by 3DP-VTA (full-cell, 74%), 3D-VT (half-cell, 53%), and 2D-VTA (half-cell, 38%). These results highlight the synergistic integration of V₂O₅, Ti₃C₂Tx MXene, and Au within a 3D printed framework, offering a promising strategy for the development of next-generation lithium-ion battery cathodes.
{"title":"In-situ Engineering of Defect-Rich TiO₂ interface with Oxygen Vacancies in V₂O₅-Ti₃C₂Tx-Au Framework for Enhanced Li⁺ Intercalation in 3D-Printed Cathodes","authors":"Saima Batool, Muhammad Idrees, Xingyu Chen, Kaishuai Yang, Li Jialin, Yang Zehao, Junguo Xu","doi":"10.1016/j.ensm.2026.105051","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105051","url":null,"abstract":"The strategic engineering of heterostructured cathodes can significantly enhance lithium-ion storage kinetics and structural stability. Here, we report a 3D-printed V₂O₅-Ti₃C₂T<sub>x</sub>-Au (3DP-VTA) cathode, in which an <em>in-situ</em> TiO₂ interface forms via synergistic interactions between V₂O₅, Ti₃C₂T<sub>x</sub>, and Au nanoparticles. The TiO₂ interface introduces abundant oxygen vacancies that act as Li⁺ adsorption sites. Density functional theory (DFT) calculations confirm the presence of localized mid-gap states with reduced Li⁺ adsorption energy (Eₐ<sub>d</sub> = -0.54 eV) and high orbital hybridization, which enhancing the electronic properties. Au NPs further contribute to interfacial redox dynamics, catalysis, and conductivity, forming Au-Ti intermetallics that act as conductive bridges, reduce interfacial resistance, and reinforce mechanical stability. Compared to pristine V₂O₅ (∼20% capacity), the 2D-VTA configuration doubles performance (∼40%), while 3D printing with Au synergy boosts it five-fold (∼100%) in half-cells. Full-cell assemblies retain ∼68% capacity, over three times higher than V₂O₅, demonstrating the efficacy of architectural and interfacial optimization. Electrochemical kinetics reveal predominantly surface-controlled behavior, with b-values of 0.96/0.84 (anodic/cathodic) and capacitive contributions increasing from 72.6% to 86.1% at 0.2-1.2 mV s⁻¹. XPS, TEM, and Raman analyses confirm TiO₂ interphase formation. EIS analysis shows 3DP-VTA (half-cell, 100%) has the best performance, followed by 3DP-VTA (full-cell, 74%), 3D-VT (half-cell, 53%), and 2D-VTA (half-cell, 38%). These results highlight the synergistic integration of V₂O₅, Ti₃C₂T<sub>x</sub> MXene, and Au within a 3D printed framework, offering a promising strategy for the development of next-generation lithium-ion battery cathodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"10 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493132","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}
Pub Date : 2026-03-22DOI: 10.1016/j.ensm.2026.105052
Ningning Yang, Wenze Cao, Mokai Cui, Zenan Zhao, Penghui Guo, Hao Wang, Jing Wang, Pan Chen, Jin Xiang, Daobin Mu, Huigen Yu, Feng Wu, Guoqiang Tan
High-quality solid-state electrolytes with excellent ionic conductivity and interface compatibility are essential for high-performance solid-state batteries. However, at present, all-solid-state electrolytes severely suffer from low intrinsic ionic conductivity and high interface impedance, while quasi-solid-state electrolytes face great challenges of structural metastability due to the heterogeneity. Here, we propose a new metal-organic ionogel concept for extending solid-state electrolytes and investigate their electrochemical properties in Li metal batteries. A simple sol-gel method is used for metal-organic ionogel self-assembly, in which ferric nitrate trimer reacts with trimeric acid to form ordered mesoporous metal-organic frameworks, while ionic liquid electrolyte is in-situ confined within mesoporous channels. The resulting metal-organic ionogel exhibits a glassy homogeneous structure with fast room-temperature Li-ion conduction (1.02 × 10−3 S cm−1), high electrochemical oxidation potential (4.8 V vs Li/Li+), and excellent thermal stability (300 °C), accordingly demonstrating great potential for Li batteries, where both LiFePO4//Li and LiNi0.8Co0.1Mn0.1O2//Li cells display high initial capacities (160 and 202 mAh g−1) and excellent capacity retention (98.6% and 85.4%) after 200 cycles.
具有优异离子电导率和界面兼容性的高质量固态电解质是高性能固态电池必不可少的材料。然而，目前全固态电解质存在着固有离子电导率低、界面阻抗高的问题，而准固态电解质由于其非均质性而面临着结构亚稳态的巨大挑战。在此，我们提出了一种新的金属有机离子凝胶概念来扩展固态电解质，并研究了它们在锂金属电池中的电化学性能。采用简单的溶胶-凝胶法进行金属-有机离子凝胶自组装，硝酸三聚铁与三聚酸反应形成有序的介孔金属-有机框架，而离子液体电解质被原位限制在介孔通道内。所制备的金属有机离子凝胶具有玻璃状均匀结构，具有快速室温锂离子传导（1.02 × 10−3 S cm−1）、高电化学氧化电位（4.8 V vs Li/Li+）和优异的热稳定性（300°C），因此显示了锂电池的巨大潜力，其中LiFePO4//Li和LiNi0.8Co0.1Mn0.1O2//Li电池在200次循环后具有高初始容量（160和202 mAh g−1）和优异的容量保持率（98.6%和85.4%）。
{"title":"Metal-organic ionogel nanocomposite electrolytes for efficient and stable solid-state lithium batteries","authors":"Ningning Yang, Wenze Cao, Mokai Cui, Zenan Zhao, Penghui Guo, Hao Wang, Jing Wang, Pan Chen, Jin Xiang, Daobin Mu, Huigen Yu, Feng Wu, Guoqiang Tan","doi":"10.1016/j.ensm.2026.105052","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105052","url":null,"abstract":"High-quality solid-state electrolytes with excellent ionic conductivity and interface compatibility are essential for high-performance solid-state batteries. However, at present, all-solid-state electrolytes severely suffer from low intrinsic ionic conductivity and high interface impedance, while quasi-solid-state electrolytes face great challenges of structural metastability due to the heterogeneity. Here, we propose a new metal-organic ionogel concept for extending solid-state electrolytes and investigate their electrochemical properties in Li metal batteries. A simple sol-gel method is used for metal-organic ionogel self-assembly, in which ferric nitrate trimer reacts with trimeric acid to form ordered mesoporous metal-organic frameworks, while ionic liquid electrolyte is in-situ confined within mesoporous channels. The resulting metal-organic ionogel exhibits a glassy homogeneous structure with fast room-temperature Li-ion conduction (1.02 × 10<sup>−3</sup> S cm<sup>−1</sup>), high electrochemical oxidation potential (4.8 V vs Li/Li<sup>+</sup>), and excellent thermal stability (300 °C), accordingly demonstrating great potential for Li batteries, where both LiFePO<sub>4</sub>//Li and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub>//Li cells display high initial capacities (160 and 202 mAh g<sup>−1</sup>) and excellent capacity retention (98.6% and 85.4%) after 200 cycles.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"83 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493131","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}
The rapid proliferation of spent lithium-ion batteries (LIBs) is driving the demand for sustainable recycling. Hydrometallurgy serves as the dominant recycling approach with proven efficiency and industrial potential. However, the exploration of metal value disparities that beneficial for flexible application orientation have been largely overlooked. Herein, we pioneered a value-gradient separation strategy for the closed-loop recycling of ternary cathode. The proposed malonic acid-glycine system exhibits synergistic dynamic coordination and differential precipitation mechanism, where malonic acid drives selective separation through differential complexation and glycine promotes localized ligand aggregation to mediate Ni-Co coprecipitation. This process yields two distinctly segregated phases of Li-Mn-enriched leachate and Ni-Co-enriched precipitate, achieving a notable separation factor (SFLi−Mn/Ni-Co) of 133.3. This facilitates the formation and flexible applications of layered Li2MnO3 cathode and Ni-Co oxide catalyst. The approach demonstrates broad compatibility with diverse battery materials and amino acid coordinators, and offers validated techno-economic advantages, establishing it as a viable pathway for advancing spent ternary LIB recycling.
{"title":"Synergic dynamic coordination and differential precipitation for value-gradient separation of Li-Mn/Ni-Co from spent lithium-ion batteries","authors":"Yilei Zheng, Hui Shi, Xingyu Hu, Bingzhong Zhang, Xingtong Zhou, Liming Yang, Wei Ren, Penghui Shao, Xubiao Luo","doi":"10.1016/j.ensm.2026.105039","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.105039","url":null,"abstract":"The rapid proliferation of spent lithium-ion batteries (LIBs) is driving the demand for sustainable recycling. Hydrometallurgy serves as the dominant recycling approach with proven efficiency and industrial potential. However, the exploration of metal value disparities that beneficial for flexible application orientation have been largely overlooked. Herein, we pioneered a value-gradient separation strategy for the closed-loop recycling of ternary cathode. The proposed malonic acid-glycine system exhibits synergistic dynamic coordination and differential precipitation mechanism, where malonic acid drives selective separation through differential complexation and glycine promotes localized ligand aggregation to mediate Ni-Co coprecipitation. This process yields two distinctly segregated phases of Li-Mn-enriched leachate and Ni-Co-enriched precipitate, achieving a notable separation factor (SF<sub>Li−Mn/Ni-Co</sub>) of 133.3. This facilitates the formation and flexible applications of layered Li<sub>2</sub>MnO<sub>3</sub> cathode and Ni-Co oxide catalyst. The approach demonstrates broad compatibility with diverse battery materials and amino acid coordinators, and offers validated techno-economic advantages, establishing it as a viable pathway for advancing spent ternary LIB recycling.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"50 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"147493134","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}
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