O3-type manganese-based anionic redox cathode materials, characterized by high initial sodium content, high capacity, and low cost, are promising candidates for advanced sodium-ion batteries. However, achieving controllable oxygen anionic redox remains challenging due to complex synthesis and a limited understanding of irreversible degradation during cycling. This work introduces a series of O3-type Na1-xLi1/3-xMgxMn2/3O2 (NLMMO, x = 0, 1/12, and 1/6) cathodes exhibiting anionic redox activity, synthesized via precise control over sodium stoichiometry, calcination temperature and atmosphere. Importantly, the partial substitution of magnesium for lithium markedly improves the reversibility of oxygen redox, as evidenced by a significant decrease in oxygen release during charging. Owing to the unique characteristic of these O3-type materials—the absence of phase transitions—the beneficial effect is ascribed to magnesium interlayers migration, which kinetically impedes manganese intralayer migration and vacancy clustering. Limiting the excessive formation of Mn3+ for NLMMO-1/6 leads to excellent cycling stability, demonstrating 85.5% capacity retention over 120 cycles in full cells, a significant improvement compared to the 36.5% retention observed without Mg substitution. These insights advance fundamental understanding of synthesizing O3-type anionic redox cathodes and their redox mechanism, guiding the design of next-generation sodium-ion batteries.
{"title":"Frustrated Oxygen Loss Enabled by Magnesium Migration in O3-Type Anionic Redox Cathodes for Sodium-Ion Batteries","authors":"Shaoyu Yang, Pu Yan, Qinzhe Liu, Zhipeng Chen, Yixiao Qiu, Guangsu Tan, Hao Chen, WenChang Hou, Yiyang Qu, Renshu Wang, Bo Zhang, Zhengyan Lun, Kecheng Cao, Xuerong Liu, Chao Xu","doi":"10.1016/j.ensm.2026.104963","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104963","url":null,"abstract":"O3-type manganese-based anionic redox cathode materials, characterized by high initial sodium content, high capacity, and low cost, are promising candidates for advanced sodium-ion batteries. However, achieving controllable oxygen anionic redox remains challenging due to complex synthesis and a limited understanding of irreversible degradation during cycling. This work introduces a series of O3-type Na<sub>1-x</sub>Li<sub>1/3-x</sub>Mg<sub>x</sub>Mn<sub>2/3</sub>O<sub>2</sub> (NLMMO, x = 0, 1/12, and 1/6) cathodes exhibiting anionic redox activity, synthesized via precise control over sodium stoichiometry, calcination temperature and atmosphere. Importantly, the partial substitution of magnesium for lithium markedly improves the reversibility of oxygen redox, as evidenced by a significant decrease in oxygen release during charging. Owing to the unique characteristic of these O3-type materials—the absence of phase transitions—the beneficial effect is ascribed to magnesium interlayers migration, which kinetically impedes manganese intralayer migration and vacancy clustering. Limiting the excessive formation of Mn<sup>3+</sup> for NLMMO-1/6 leads to excellent cycling stability, demonstrating 85.5% capacity retention over 120 cycles in full cells, a significant improvement compared to the 36.5% retention observed without Mg substitution. These insights advance fundamental understanding of synthesizing O3-type anionic redox cathodes and their redox mechanism, guiding the design of next-generation sodium-ion batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"302 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122281","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 : 2026-02-03DOI: 10.1016/j.ensm.2026.104959
Water-in-salt (WIS) electrolytes offer high energy density and excellent stability in energy conversion and storage. A precise assessment of their str…
盐包水（WIS）电解质具有高能量密度和优异的能量转换和储存稳定性。对他们能力的精确评估……
{"title":"Localized insight into potential-switched structure and hierarchical transport of water-in-salt electrolyte at electrified interfaces","authors":"","doi":"10.1016/j.ensm.2026.104959","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104959","url":null,"abstract":"Water-in-salt (WIS) electrolytes offer high energy density and excellent stability in energy conversion and storage. A precise assessment of their str…","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"66 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101521","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 : 2026-02-03DOI: 10.1016/j.ensm.2026.104960
Minhyung Kwon, Seungyun Jeon, Uichan Hwang, Eunji Kwon, Hee-Kang Shin, Seungho Yu, Dong-Ik Kim, Jihyun Hong, Minah Lee
The practical implementation of aqueous Zn-ion batteries (AZIBs) is hindered by the irreversibility of Zn metal anodes, which suffer from heterogeneous electrodeposition coupled with parasitic hydrogen evolution reactions (HER). While substrate engineering is essential to address this issue, the HER activity of substrates and its modulation to achieve homogeneous Zn nucleation and growth have been largely overlooked. Here, we investigate the interplay between HER suppression and Zn deposition behavior by tailoring surface chemistry of Cu current collectors. Specifically, we introduce a deep eutectic solvent (DES) treatment that simultaneously removes native oxides and forms a choline-derived organic nanolayer on Cu surface as an alternative to conventional acid or thermal pretreatments. This unique interface not only inhibits proton reduction but also promotes conformal Cu–Zn alloy formation, thereby enhancing Zn binding and further suppressing HER. Such dynamic surface evolution collectively mitigates insulating byproducts formation and enables dense Zn growth with enlarged grains (>2 μm) and a thickness closely matching that of Zn foil (106%). Consequently, Zn anodes deposited on DES-treated Cu deliver a cumulative capacity of 5.8 Ah cm-2 at 30% depth of discharge (DOD) and retain 2.2 Ah cm-2 even at 50% DOD, highlighting their potential for practical, high-performance AZIBs.
{"title":"Tailoring electrochemical interface to regulate competition between Zn deposition and hydrogen evolution in aqueous rechargeable batteries","authors":"Minhyung Kwon, Seungyun Jeon, Uichan Hwang, Eunji Kwon, Hee-Kang Shin, Seungho Yu, Dong-Ik Kim, Jihyun Hong, Minah Lee","doi":"10.1016/j.ensm.2026.104960","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104960","url":null,"abstract":"The practical implementation of aqueous Zn-ion batteries (AZIBs) is hindered by the irreversibility of Zn metal anodes, which suffer from heterogeneous electrodeposition coupled with parasitic hydrogen evolution reactions (HER). While substrate engineering is essential to address this issue, the HER activity of substrates and its modulation to achieve homogeneous Zn nucleation and growth have been largely overlooked. Here, we investigate the interplay between HER suppression and Zn deposition behavior by tailoring surface chemistry of Cu current collectors. Specifically, we introduce a deep eutectic solvent (DES) treatment that simultaneously removes native oxides and forms a choline-derived organic nanolayer on Cu surface as an alternative to conventional acid or thermal pretreatments. This unique interface not only inhibits proton reduction but also promotes conformal Cu–Zn alloy formation, thereby enhancing Zn binding and further suppressing HER. Such dynamic surface evolution collectively mitigates insulating byproducts formation and enables dense Zn growth with enlarged grains (>2 μm) and a thickness closely matching that of Zn foil (106%). Consequently, Zn anodes deposited on DES-treated Cu deliver a cumulative capacity of 5.8 Ah cm<sup>-2</sup> at 30% depth of discharge (DOD) and retain 2.2 Ah cm<sup>-2</sup> even at 50% DOD, highlighting their potential for practical, high-performance AZIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"41 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101520","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}
Silicon (Si)-based anode materials are considered the most promising next-generation anodes for lithium-ion batteries (LIBs). Nonetheless, in practical applications, Si anodes have encountered numerous challenges. A homogeneous silicon carbide (SiC) dispersoid was synthesized within the Si-based alloy using vacuum melting, sand milling, and Flash joule heating procedures. The integration of SiC facilitates the simultaneous resolution of key issues: low intrinsic conductivity, unstable solid electrolyte interphase (SEI), and significant volume expansion, which is accomplished by creating a swift and uniform charge-transport network, enhancing interfacial kinetics, and bolstering the mechanical integrity of the electrode, which is attributed to the synergistic effect of a highly conductive network formed by the in-situ generated defective SiC and the metallic phases (Sn/Bi), SiC's advantageous interfacial characteristics, exceptional mechanical strength, and dispersion strengthening effect. The half-cell exhibits an impressive capacity of 1881.69 mAh g−1 and maintains steady cycling for 400 cycles at a current density of 1.5 A g−1. The full cell utilizing Li1.2Ni0.13Co0.13Mn0.54O2, demonstrates a capacity of 251.71 mAh g−1 following 80 cycles at 0.33 A g−1. Meanwhile, excellent cycling stability is attained in all-solid-state batteries, delivering a capacity retention of 81.1% over 150 cycles. This work introduces an innovative triple synergistic mechanism that significantly enhances the electrochemical performance of Si-based anodes, facilitating their efficient manufacture and offering important insights for future investigations.
硅基负极材料被认为是最有前途的下一代锂离子电池负极材料。然而，在实际应用中，硅阳极遇到了许多挑战。采用真空熔炼、砂磨和闪速焦耳加热工艺，在硅基合金中合成了均匀的碳化硅分散体。SiC的集成有助于同时解决关键问题：低固有电导率，不稳定的固体电解质界面相（SEI），以及显著的体积膨胀，这是通过创建快速均匀的电荷传输网络来实现的，增强了界面动力学，增强了电极的机械完整性，这是由于原位生成的缺陷SiC和金属相（Sn/Bi）形成的高导电性网络的协同作用，SiC的有利界面特性。优异的机械强度和分散强化效果。该半电池的容量为1881.69 mAh g−1，在电流密度为1.5 a g−1的情况下可稳定循环400次。使用Li1.2Ni0.13Co0.13Mn0.54O2的完整电池在0.33 a g - 1下循环80次后的容量为251.71 mAh g - 1。同时，在全固态电池中获得了出色的循环稳定性，在150次循环中提供81.1%的容量保持率。这项工作引入了一种创新的三重协同机制，显著提高了硅基阳极的电化学性能，促进了它们的高效制造，并为未来的研究提供了重要的见解。
{"title":"Flash joule heating Driven In-Situ Dispersoid Synthesis: Mechanical-Interfacial-Conductive Coupling Mechanisms in Silicon-Based Anodes","authors":"D.R. Lan, P.Y. Ou, S.Q. Pei, K.J. Liu, C.C. Li, M.C. Zhang, Y.X. Liu, S.N. He, L.N. She, Y.X. Yang, W.B. Du, H.G. Pan","doi":"10.1016/j.ensm.2026.104956","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104956","url":null,"abstract":"Silicon (Si)-based anode materials are considered the most promising next-generation anodes for lithium-ion batteries (LIBs). Nonetheless, in practical applications, Si anodes have encountered numerous challenges. A homogeneous silicon carbide (SiC) dispersoid was synthesized within the Si-based alloy using vacuum melting, sand milling, and Flash joule heating procedures. The integration of SiC facilitates the simultaneous resolution of key issues: low intrinsic conductivity, unstable solid electrolyte interphase (SEI), and significant volume expansion, which is accomplished by creating a swift and uniform charge-transport network, enhancing interfacial kinetics, and bolstering the mechanical integrity of the electrode, which is attributed to the synergistic effect of a highly conductive network formed by the in-situ generated defective SiC and the metallic phases (Sn/Bi), SiC's advantageous interfacial characteristics, exceptional mechanical strength, and dispersion strengthening effect. The half-cell exhibits an impressive capacity of 1881.69 mAh g<sup>−1</sup> and maintains steady cycling for 400 cycles at a current density of 1.5 A g<sup>−1</sup>. The full cell utilizing Li<sub>1.2</sub>Ni<sub>0.13</sub>Co<sub>0.13</sub>Mn<sub>0.54</sub>O<sub>2</sub>, demonstrates a capacity of 251.71 mAh g<sup>−1</sup> following 80 cycles at 0.33 A g<sup>−1</sup>. Meanwhile, excellent cycling stability is attained in all-solid-state batteries, delivering a capacity retention of 81.1% over 150 cycles. This work introduces an innovative triple synergistic mechanism that significantly enhances the electrochemical performance of Si-based anodes, facilitating their efficient manufacture and offering important insights for future investigations.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"95 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101523","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.ensm.2026.104953
Jiayi Yang, Yangqian Zhang, Han Liu, Yaqi Liao, Chihon Leung, Rongfeng Chen, Ying Wei, Le Hu, Mengyuan Zhou, Gang Sun, Ziping Wu, Henghui Xu, Zhenbo Wang, Shaoming Huang, Yang Ren
As one of the most promising solid-state polymer electrolytes (SPEs), Polyacrylonitrile (PAN)-based SPEs suffer from unstable interfaces due to their highly reactivity with lithium metal anode. Here, the molecular chain of the PAN polymer is tailored through surface-basicity-guided reactions of Li7La3Zr1.4Ta0.6O12 (LLZTO) and an electrostatic shielding effect of 1-Ethyl-3-methylimidazolium cation (EMIM⁺), effectively mitigating its reactivity with Li. The alkalinity of LLZTO catalyze PAN dehydrocyanation, transforming –CN groups to π-conjugated –C=N/–C=C– bonds, thus decreasing its inherent reactivity with the Li metal. Then, the positive EMIM⁺ with an electron-delocalized π-network electrostatically connect with polarized –C=N sites, shielding the direct contact of –CN groups with Li, further alleviating parasitic reactions. As a result, the Li//Li symmetric cells deliver high critical current density of 3.0 mA cm−2 and maintain stable Li plating/stripping over 2000 h. The Li//LFP cell delivers a high capacity retention of 87.53% after 1200 cycles at 2C, and the pouch battery presents excellent cycling and safety performance. This work provides a promising approach to enable the stable operation of solid-state lithium metal batteries via incorporating the electron-delocalized π-network.
{"title":"Electron-Delocalized π-Network Enables Low-Reactive Polyacrylonitrile-based Solid-State Electrolytes for Lithium Metal Batteries","authors":"Jiayi Yang, Yangqian Zhang, Han Liu, Yaqi Liao, Chihon Leung, Rongfeng Chen, Ying Wei, Le Hu, Mengyuan Zhou, Gang Sun, Ziping Wu, Henghui Xu, Zhenbo Wang, Shaoming Huang, Yang Ren","doi":"10.1016/j.ensm.2026.104953","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104953","url":null,"abstract":"As one of the most promising solid-state polymer electrolytes (SPEs), Polyacrylonitrile (PAN)-based SPEs suffer from unstable interfaces due to their highly reactivity with lithium metal anode. Here, the molecular chain of the PAN polymer is tailored through surface-basicity-guided reactions of Li<sub>7</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> (LLZTO) and an electrostatic shielding effect of 1-Ethyl-3-methylimidazolium cation (EMIM⁺), effectively mitigating its reactivity with Li. The alkalinity of LLZTO catalyze PAN dehydrocyanation, transforming –C<img alt=\"triple bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/tbnd.gif\" style=\"vertical-align:middle\"/>N groups to π-conjugated –C=N/–C=C– bonds, thus decreasing its inherent reactivity with the Li metal. Then, the positive EMIM⁺ with an electron-delocalized π-network electrostatically connect with polarized –C=N sites, shielding the direct contact of –C<img alt=\"triple bond\" src=\"https://sdfestaticassets-us-east-1.sciencedirectassets.com/shared-assets/55/entities/tbnd.gif\" style=\"vertical-align:middle\"/>N groups with Li, further alleviating parasitic reactions. As a result, the Li//Li symmetric cells deliver high critical current density of 3.0 mA cm<sup>−2</sup> and maintain stable Li plating/stripping over 2000 h. The Li//LFP cell delivers a high capacity retention of 87.53% after 1200 cycles at 2C, and the pouch battery presents excellent cycling and safety performance. This work provides a promising approach to enable the stable operation of solid-state lithium metal batteries via incorporating the electron-delocalized π-network.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"42 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146095933","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}
N groups to π-conjugated –C=N/–C=C– bonds, thus decreasing its inherent reactivity with the Li metal. Then, the positive EMIM⁺ with an electron-delocalized π-network electrostatically connect with polarized –C=N sites, shielding the direct contact of –C
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