Lithium thioantimonate argyrodite solid electrolytes, Li6+xMxSb1–xS5I (M=Si, Ge), are promising candidates for all-solid-state batteries due to their exceptional ionic conductivity. However, limited mechanistic understanding hinders the rational design of these materials. In this study, we systematically investigate the underlying Li-ion conduction mechanisms and propose a cation-disorder-driven design strategy using machine-learned interatomic potentials (MLIPs). While inter-cage migration via the Wyckoff 16e (T4) site remains significant, enhanced inter-cage migration through Wyckoff 48 h (T2) sites induced by Si and Ge dopants emerges as a critical factor for achieving high ionic conductivity. Additionally, Si and Ge exhibit distinct inductive effects: Si requires higher substitution to activate T2 pathways, while Ge achieves optimal conductivity at lower levels. Co-substitution of Si and Ge further increases cation disorder, yielding ionic conductivity up to ~50 mS/cm. This study demonstrates the effectiveness of MLIPs in elucidating conduction mechanisms and facilitating the rational design of advanced argyrodite electrolytes.
硫代锑酸锂银晶固体电解质Li6+ xMxSb1-xS5I （M=Si, Ge）由于其优异的离子导电性，是全固态电池的有希望的候选者。然而，有限的机械理解阻碍了这些材料的合理设计。在这项研究中，我们系统地研究了潜在的锂离子传导机制，并提出了一种利用机器学习原子间电位（MLIPs）的阳离子无序驱动设计策略。虽然通过Wyckoff 16e （T4）位点的笼间迁移仍然很明显，但Si和Ge掺杂剂诱导的通过Wyckoff 48h （T2）位点的笼间迁移增强是实现高离子电导率的关键因素。此外，Si和Ge表现出不同的诱导效应：Si需要更高的取代来激活T2通路，而Ge在较低水平下获得最佳导电性。Si和Ge的共取代进一步增加了阳离子的无序性，离子电导率高达~50 mS/cm。该研究证明了MLIPs在阐明导电机制和促进先进银晶电解质合理设计方面的有效性。
{"title":"Design Principles for Cation-Disordered Superionic Thioantimonate Argyrodite Solid Electrolytes","authors":"Kanguk Park, Myeongcho Jang, Eunji Kwon, Yongheum Lee, Hun-Gi Jung, Kyung Yoon Chung, Seung-Ho Yu, Seungho Yu","doi":"10.1016/j.nanoen.2026.111777","DOIUrl":"https://doi.org/10.1016/j.nanoen.2026.111777","url":null,"abstract":"Lithium thioantimonate argyrodite solid electrolytes, Li<sub>6+x</sub>M<sub>x</sub>Sb<sub>1–x</sub>S<sub>5</sub>I (M=Si, Ge), are promising candidates for all-solid-state batteries due to their exceptional ionic conductivity. However, limited mechanistic understanding hinders the rational design of these materials. In this study, we systematically investigate the underlying Li-ion conduction mechanisms and propose a cation-disorder-driven design strategy using machine-learned interatomic potentials (MLIPs). While inter-cage migration via the Wyckoff 16e (T4) site remains significant, enhanced inter-cage migration through Wyckoff 48<!-- --> <!-- -->h (T2) sites induced by Si and Ge dopants emerges as a critical factor for achieving high ionic conductivity. Additionally, Si and Ge exhibit distinct inductive effects: Si requires higher substitution to activate T2 pathways, while Ge achieves optimal conductivity at lower levels. Co-substitution of Si and Ge further increases cation disorder, yielding ionic conductivity up to ~50 mS/cm. This study demonstrates the effectiveness of MLIPs in elucidating conduction mechanisms and facilitating the rational design of advanced argyrodite electrolytes.","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"83 1","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122283","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 presence of silver ions (Ag+) in industrial wastewater not only leads to the waste of resources but also poses significant environmental risks. Traditional adsorbent materials generally face technical limitations in complex wastewater systems, such as poor selectivity and instability under acidic conditions. Tunnel-structured MnO2 (OMS-2) nanomaterial has been known as a versatile adsorbent to various ionic species due to its high surface area; however, its internal sub-nanosized tunnel space with a theoretical potential for ion accommodation, exhibits sluggish adsorption kinetics due to the high energy barrier associated with demanded structural distortion upon ion intercalation. In this study, we report a strategy of K+ pre-intercalation into OMS-2 tunnels, which leverages the ionic similarity between K+ and Ag+, i.e. similar physical size and monovalent charge, to suppress structural distortion and facilitate Ag+–K+ ion exchange within the internal tunnels. As such, we not only extend OMS-2’s adsorption sites from its surface to internal tunnels with high efficiency and high selectivity, but also transform adsorbed Ag+ into efficient atomic catalysts for oxygen reduction reactions confined within the tunnel micropores. Consequently, a technological bridge from wastewater purification to energy conversion is established, demonstrating the bi-functionality future of the as-proposed strategy and material of interest.
{"title":"K+ pre-intercalated octahedral molecular sieves enabling Ag+-specific adsorption and ORR electrocatalysis","authors":"Qing Tang, Xuemei Zeng, Yaqing Guo, Wenjun Song, Yun Li, Yiner Cai, Jie Xu, Yifei Yuan","doi":"10.1016/j.nanoen.2026.111778","DOIUrl":"https://doi.org/10.1016/j.nanoen.2026.111778","url":null,"abstract":"The presence of silver ions (Ag<sup>+</sup>) in industrial wastewater not only leads to the waste of resources but also poses significant environmental risks. Traditional adsorbent materials generally face technical limitations in complex wastewater systems, such as poor selectivity and instability under acidic conditions. Tunnel-structured MnO<sub>2</sub> (OMS-2) nanomaterial has been known as a versatile adsorbent to various ionic species due to its high surface area; however, its internal sub-nanosized tunnel space with a theoretical potential for ion accommodation, exhibits sluggish adsorption kinetics due to the high energy barrier associated with demanded structural distortion upon ion intercalation. In this study, we report a strategy of K<sup>+</sup> pre-intercalation into OMS-2 tunnels, which leverages the ionic similarity between K<sup>+</sup> and Ag<sup>+</sup>, <em>i.e.</em> similar physical size and monovalent charge, to suppress structural distortion and facilitate Ag<sup>+</sup>–K<sup>+</sup> ion exchange within the internal tunnels. As such, we not only extend OMS-2’s adsorption sites from its surface to internal tunnels with high efficiency and high selectivity, but also transform adsorbed Ag<sup>+</sup> into efficient atomic catalysts for oxygen reduction reactions confined within the tunnel micropores. Consequently, a technological bridge from wastewater purification to energy conversion is established, demonstrating the bi-functionality future of the as-proposed strategy and material of interest.","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"89 1","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122282","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 : 2026-02-05DOI: 10.1016/j.nanoen.2026.111779
Robert Kuphal, Jingjing Liu, Li Yang, Nader Marendian Hagh, Umamaheswari Janakiraman, Chengcheng Fang
The development of high-energy lithium metal batteries (LMBs) requires cathode areal capacities exceeding 4 mAh cm-2, ultra-thin lithium (Li) foil (<50 μm), and over 500 cycles with 80% capacity retention to achieve commercially viable applications. While significant advances in electrolyte formulation, pressure control, and interfacial engineering have improved LMB performance, the interplay among cathode capacity loading, Li utilization, and cycle life remains underexplored in practical cell configurations. Here, we investigate the impact of cathode capacity loading on electrochemical reversibility, Li loss mechanisms, and cycle life using a 20 μm Li anode. Li||Cu half-cell analysis benchmarks Coulombic efficiency (CE) behavior across varied Li cycling capacities. We find that while higher cathode loadings (4 - 5 mAh cm-2) yield higher Li cycling CE, they also result in greater cumulative Li loss and faster degradation from solid-electrolyte interphase (SEI) formation and inactive Li. These cells require ≥99.8% CE to achieve 500 cycles with 80% of capacity retention, compared to ~99.6% for lower-capacity designs (2 mAh cm-2). Full cell studies with LiNi0.8Mn0.1Co0.1O2 (NMC811) reveal further deviations from Li-metal estimation, attributed to increased cathode polarization at higher loadings. A quantitative inverse linear relationship is established between cathode capacity loading and achievable cycle life. These findings highlight the importance of standardized testing conditions for evaluating improvement strategies and provide practical design guidance for integrating high-loading cathodes with ultra-thin Li anodes, advancing the realization of high-energy LMB systems.
高能锂金属电池（lmb）的发展需要阴极面积容量超过4 mAh cm-2，超薄锂（Li）箔（<50 μm），超过500次循环，80%的容量保留，以实现商业上可行的应用。虽然电解质配方、压力控制和界面工程方面的重大进展改善了LMB的性能，但在实际电池配置中，阴极容量负载、锂离子利用率和循环寿命之间的相互作用仍未得到充分探讨。在这里，我们研究了阴极容量负载对电化学可逆性、锂损失机制和循环寿命的影响，使用20 μm的锂阳极。Cu半电池分析基准库仑效率（CE）行为在不同的锂循环容量。我们发现，虽然更高的阴极负载（4 - 5 mAh cm-2）产生更高的锂循环CE，但它们也导致更大的累积锂损失和更快的固体电解质间相（SEI）形成和非活性锂的降解。这些电池需要≥99.8%的CE才能达到500次循环，并保持80%的容量，而低容量设计的CE为~99.6%（2 mAh cm-2）。用LiNi0.8Mn0.1Co0.1O2 （NMC811）进行的全电池研究进一步揭示了与锂金属估计的偏差，这归因于高负载下阴极极化的增加。在阴极容量负载与可实现循环寿命之间建立了定量的反比线性关系。这些发现强调了标准化测试条件对评估改进策略的重要性，并为将高负载阴极与超薄锂阳极集成在一起，推进高能LMB系统的实现提供了实用的设计指导。
{"title":"Quantifying capacity loading - cycle life relationship in lithium metal batteries","authors":"Robert Kuphal, Jingjing Liu, Li Yang, Nader Marendian Hagh, Umamaheswari Janakiraman, Chengcheng Fang","doi":"10.1016/j.nanoen.2026.111779","DOIUrl":"https://doi.org/10.1016/j.nanoen.2026.111779","url":null,"abstract":"The development of high-energy lithium metal batteries (LMBs) requires cathode areal capacities exceeding 4 mAh cm<sup>-2</sup>, ultra-thin lithium (Li) foil (<50 μm), and over 500 cycles with 80% capacity retention to achieve commercially viable applications. While significant advances in electrolyte formulation, pressure control, and interfacial engineering have improved LMB performance, the interplay among cathode capacity loading, Li utilization, and cycle life remains underexplored in practical cell configurations. Here, we investigate the impact of cathode capacity loading on electrochemical reversibility, Li loss mechanisms, and cycle life using a 20 μm Li anode. Li||Cu half-cell analysis benchmarks Coulombic efficiency (CE) behavior across varied Li cycling capacities. We find that while higher cathode loadings (4 - 5 mAh cm<sup>-2</sup>) yield higher Li cycling CE, they also result in greater cumulative Li loss and faster degradation from solid-electrolyte interphase (SEI) formation and inactive Li. These cells require ≥99.8% CE to achieve 500 cycles with 80% of capacity retention, compared to ~99.6% for lower-capacity designs (2 mAh cm<sup>-2</sup>). Full cell studies with LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (NMC811) reveal further deviations from Li-metal estimation, attributed to increased cathode polarization at higher loadings. A quantitative inverse linear relationship is established between cathode capacity loading and achievable cycle life. These findings highlight the importance of standardized testing conditions for evaluating improvement strategies and provide practical design guidance for integrating high-loading cathodes with ultra-thin Li anodes, advancing the realization of high-energy LMB systems.","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"47 1","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122284","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 : 2026-02-01DOI: 10.1016/j.nanoen.2026.111771
Huimin Qi, Siyao Qin, Zhipeng Zhang, Zifei Meng, Long Zheng, Xucong Wang, Xiangcheng Chu, Fang Wang, Li Zheng, Xiangyu Chen
The self-polarization approach for fabricating poly(vinylidene fluoride) (PVDF)-based piezoelectric materials can avoid drawbacks of post-poling treatment, such as high energy consumption, electrical breakdown, and depolarization. In this work, a core–shell nanofiller with abundant surface hydroxyl groups is prepared as the dopant for sufficiently inducing local self-polarization for the 3D printed PVDF film. Hydrogen bonding between these groups and PVDF molecular chains promotes β-phase crystallization and enables local polarization anchoring. Furthermore, the shear field at the nozzle tip of 3D printer can be utilized for orienting the nanorod-induced self-polarization. Simultaneously, the induced shear and tensile stresses facilitate PVDF molecular chain extension and β-phase crystallization, achieving macroscopic self-polarization in the out-of-plane direction. Benefiting from this synergistic strategy, the composite film exhibits excellent long-term polarization stability and a high piezoelectric coefficient of 117.3 pC/N, which exceeds all the previously reported self-polarization PVDF films. This study offers an effective strategy for developing high-performance piezoelectric composites without polarization treatment. Owing to its high piezoelectric output performance, this PVDF film can be used for mechanical energy harvesting and motion signal sensing in various conditions.
{"title":"High-Performance Self-Polarized PVDF film Based on One-Dimensional Core-Shell Nanofiller and Direct Ink Writing 3D Printing","authors":"Huimin Qi, Siyao Qin, Zhipeng Zhang, Zifei Meng, Long Zheng, Xucong Wang, Xiangcheng Chu, Fang Wang, Li Zheng, Xiangyu Chen","doi":"10.1016/j.nanoen.2026.111771","DOIUrl":"https://doi.org/10.1016/j.nanoen.2026.111771","url":null,"abstract":"The self-polarization approach for fabricating poly(vinylidene fluoride) (PVDF)-based piezoelectric materials can avoid drawbacks of post-poling treatment, such as high energy consumption, electrical breakdown, and depolarization. In this work, a core–shell nanofiller with abundant surface hydroxyl groups is prepared as the dopant for sufficiently inducing local self-polarization for the 3D printed PVDF film. Hydrogen bonding between these groups and PVDF molecular chains promotes β-phase crystallization and enables local polarization anchoring. Furthermore, the shear field at the nozzle tip of 3D printer can be utilized for orienting the nanorod-induced self-polarization. Simultaneously, the induced shear and tensile stresses facilitate PVDF molecular chain extension and β-phase crystallization, achieving macroscopic self-polarization in the out-of-plane direction. Benefiting from this synergistic strategy, the composite film exhibits excellent long-term polarization stability and a high piezoelectric coefficient of 117.3 pC/N, which exceeds all the previously reported self-polarization PVDF films. This study offers an effective strategy for developing high-performance piezoelectric composites without polarization treatment. Owing to its high piezoelectric output performance, this PVDF film can be used for mechanical energy harvesting and motion signal sensing in various conditions.","PeriodicalId":394,"journal":{"name":"Nano Energy","volume":"8 1","pages":""},"PeriodicalIF":17.6,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146110644","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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