Pub Date : 2026-01-08DOI: 10.1007/s40820-025-01918-7
Xu Wang, Zixiang Yang, Yujia Cai, Heng Ma, Jinglei Xu, Rabia Khatoon, Zhizhen Ye, Dashuai Wang, Muhammad Tariq Sajjad, Jianguo Lu
Layered oxides have attracted significant attention as cathodes for sodium-ion batteries (SIBs) due to their compositional versatility and tuneable electrochemical performance. However, these materials still face challenges such as structural phase transitions, Na+/vacancy ordering, and Jahn-Teller distortion effect, resulting in severe capacity decay and sluggish ion kinetics. We develop a novel Cu/Y dual-doping strategy that leads to the formation of "Na-Y" interlayer aggregates, which act as structural pillars within alkali metal layers, enhancing structural stability and disrupting the ordered arrangement of Na+/vacancies. This disruption leads to a unique coexistence of ordered and disordered Na+/vacancy states with near-zero strain, which significantly improves Na+ diffusion kinetics. This structural innovation not only mitigates the unfavorable P2-O2 phase transition but also facilitates rapid ion transport. As a result, the doped material demonstrates exceptional electrochemical performance, including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of ~70 mAh g-1 at 50 C. The discovery of this novel interlayer pillar, along with its role in modulating Na⁺/vacancy arrangements, provides a fresh perspective on engineering layered oxides. It opens up promising new pathways for the structural design of advanced cathode materials toward efficient, stable, and high-rate SIBs.
层状氧化物作为钠离子电池(sib)的阴极材料,由于其成分的通用性和电化学性能的可调性而备受关注。然而,这些材料仍然面临结构相变、Na+/空位有序和Jahn-Teller畸变效应等挑战,导致严重的容量衰减和离子动力学缓慢。我们开发了一种新的Cu/Y双掺杂策略,导致“Na-Y”层间聚集体的形成,这些聚集体在碱金属层内充当结构支柱,增强结构稳定性并破坏Na+/空位的有序排列。这种破坏导致了在接近零应变的情况下有序和无序Na+/空位态的独特共存,显著改善了Na+扩散动力学。这种结构创新不仅减轻了不利的P2-O2相变,而且促进了离子的快速传递。结果,掺杂材料表现出优异的电化学性能,包括在10℃下3000次的超长循环寿命和在50℃下~70 mAh g-1的出色高倍率性能。这种新型层间柱的发现,以及它在调节Na + /空位排列中的作用,为工程层状氧化物提供了一个新的视角。它为高效、稳定和高速率sib的先进阴极材料的结构设计开辟了有希望的新途径。
{"title":"Regulation Engineering of Alkali Metal Interlayer Pillar in P2-Type Cathode for Ultra-High Rate and Long-Term Cycling Sodium-Ion Batteries.","authors":"Xu Wang, Zixiang Yang, Yujia Cai, Heng Ma, Jinglei Xu, Rabia Khatoon, Zhizhen Ye, Dashuai Wang, Muhammad Tariq Sajjad, Jianguo Lu","doi":"10.1007/s40820-025-01918-7","DOIUrl":"10.1007/s40820-025-01918-7","url":null,"abstract":"<p><p>Layered oxides have attracted significant attention as cathodes for sodium-ion batteries (SIBs) due to their compositional versatility and tuneable electrochemical performance. However, these materials still face challenges such as structural phase transitions, Na<sup>+</sup>/vacancy ordering, and Jahn-Teller distortion effect, resulting in severe capacity decay and sluggish ion kinetics. We develop a novel Cu/Y dual-doping strategy that leads to the formation of \"Na-Y\" interlayer aggregates, which act as structural pillars within alkali metal layers, enhancing structural stability and disrupting the ordered arrangement of Na<sup>+</sup>/vacancies. This disruption leads to a unique coexistence of ordered and disordered Na<sup>+</sup>/vacancy states with near-zero strain, which significantly improves Na<sup>+</sup> diffusion kinetics. This structural innovation not only mitigates the unfavorable P2-O2 phase transition but also facilitates rapid ion transport. As a result, the doped material demonstrates exceptional electrochemical performance, including an ultra-long cycle life of 3000 cycles at 10 C and an outstanding high-rate capability of ~70 mAh g<sup>-1</sup> at 50 C. The discovery of this novel interlayer pillar, along with its role in modulating Na⁺/vacancy arrangements, provides a fresh perspective on engineering layered oxides. It opens up promising new pathways for the structural design of advanced cathode materials toward efficient, stable, and high-rate SIBs.</p>","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"18 1","pages":"105"},"PeriodicalIF":36.3,"publicationDate":"2026-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12779844/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145916395","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2026-01-07DOI: 10.1007/s40820-025-02023-5
Zhengqian Jin, Zhenjiang Cao, Li Jin, Shujiang Ding, Kai Xi
High-entropy layered hydroxides (HELHs), an emerging frontier in entropy-stabilized materials derived from layered double hydroxides (LDHs), have captivated attention with their unparalleled tunability, thermodynamic stability, and electrochemical performance. The integration of the high-entropy concept into LDHs empowers HELHs to surmount the constraints of conventional materials through compositional diversity, structurally disordered configurations, and synergistic multi-element interactions. This review systematically embarks on their synthesis methodologies, functional mechanisms, and applications in energy conversion/storage and biomedicine. Advanced synthesis strategies, such as plasma-assisted hydrothermal methods, facilitate precise control over HELH architectures while supporting scalable production. HELHs demonstrate superior electrochemical performance in critical reactions, including oxygen evolution reaction, water oxidation, hydrogen evolution, and glucose electrooxidation. Future directions encompass integrating in situ characterization with simulations, leveraging machine learning for composition screening, and expanding HELHs application through interdisciplinary collaborations. This work establishes a comprehensive roadmap for advancing HELHs as next-generation multifunctional platforms for sustainable energy and biomedical technologies.
{"title":"High-Entropy Layered Hydroxides: Pioneering Synthesis, Mechanistic Insights, and Multifunctional Applications in Sustainable Energy and Biomedicine","authors":"Zhengqian Jin, Zhenjiang Cao, Li Jin, Shujiang Ding, Kai Xi","doi":"10.1007/s40820-025-02023-5","DOIUrl":"10.1007/s40820-025-02023-5","url":null,"abstract":"<div><p>High-entropy layered hydroxides (HELHs), an emerging frontier in entropy-stabilized materials derived from layered double hydroxides (LDHs), have captivated attention with their unparalleled tunability, thermodynamic stability, and electrochemical performance. The integration of the high-entropy concept into LDHs empowers HELHs to surmount the constraints of conventional materials through compositional diversity, structurally disordered configurations, and synergistic multi-element interactions. This review systematically embarks on their synthesis methodologies, functional mechanisms, and applications in energy conversion/storage and biomedicine. Advanced synthesis strategies, such as plasma-assisted hydrothermal methods, facilitate precise control over HELH architectures while supporting scalable production. HELHs demonstrate superior electrochemical performance in critical reactions, including oxygen evolution reaction, water oxidation, hydrogen evolution, and glucose electrooxidation. Future directions encompass integrating in situ characterization with simulations, leveraging machine learning for composition screening, and expanding HELHs application through interdisciplinary collaborations. This work establishes a comprehensive roadmap for advancing HELHs as next-generation multifunctional platforms for sustainable energy and biomedical technologies.</p><div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":714,"journal":{"name":"Nano-Micro Letters","volume":"18 1","pages":""},"PeriodicalIF":36.3,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://link.springer.com/content/pdf/10.1007/s40820-025-02023-5.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145907855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}