Energy Storage Materials最新文献_第4页

Spin Polarization in Bi/FeS Heterostructure Enables High-Performance Sodium Ion Storage Bi/FeS异质结构的自旋极化实现高性能钠离子存储

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-09-23 DOI: 10.1016/j.ensm.2025.104631

Jing Chen, Junjie Xiao, Shuxuan Liao, Wei Tan, Yao Liu, Boyu Zhao, Jinghao Zhao, Qiang Li, Xin Li

{"title":"Spin Polarization in Bi/FeS Heterostructure Enables High-Performance Sodium Ion Storage","authors":"Jing Chen, Junjie Xiao, Shuxuan Liao, Wei Tan, Yao Liu, Boyu Zhao, Jinghao Zhao, Qiang Li, Xin Li","doi":"10.1016/j.ensm.2025.104631","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104631","url":null,"abstract":"Bismuth (Bi) has emerged as an appealing anode material in sodium-ion batteries (SIBs), owing to its exceptional volumetric capacity. However, sluggish Na⁺ kinetics remains a critical challenge, which can be mitigated by spin polarization. Yet Bi exhibits strong diamagnetism and lacks viable methods for its spin manipulation. And such manipulation mechanism is difficult to capture using conventional electrochemical characterization methods. Herein, we propose a carbon-coated Bi/FeS heterostructure (Bi/FeS@NSC), where FeS generates metallic Fe0 during the conversion reaction, inducing the emergence of spin polarization. Operando magnetometry reveals that the induced-effect contributes to both significant additional capacity and accelerated charge transfer. Furthermore, the complete sodium storage mechanism and capacity derivation of Bi/FeS@NSC electrode are further elucidated through in situ X-ray diffraction (XRD) and theoretical calculations. Benefiting from this unique design, the Bi/FeS@NSC electrode delivers an outstanding capacity (397.5 mAh g⁻¹ at 40.0 A g⁻¹) and stable cycling performance (265.3 mAh g⁻¹ at 20.0 A g⁻¹ after 2200 cycles). This work provides novel perspectives on spin-polarization regulation and corresponding mechanisms in Bi-based anode materials.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"40 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145127407","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

An Janus-type buffer layer with ion conductive and electron insulative interface enabling dendrite-free solid-state lithium metal batteries 一种具有离子导电和电子绝缘界面的janus型缓冲层，使无枝晶固态锂金属电池成为可能

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-22 DOI: 10.1016/j.ensm.2025.104628

Xiaoxue Zhao, Chao Wang, Yang Li, Dabing Li, Yanling Zhang, Meng Wu, Xiang Qi, Li-Zhen Fan

{"title":"An Janus-type buffer layer with ion conductive and electron insulative interface enabling dendrite-free solid-state lithium metal batteries","authors":"Xiaoxue Zhao, Chao Wang, Yang Li, Dabing Li, Yanling Zhang, Meng Wu, Xiang Qi, Li-Zhen Fan","doi":"10.1016/j.ensm.2025.104628","DOIUrl":"10.1016/j.ensm.2025.104628","url":null,"abstract":"<div><div>The cycle life of garnet-based solid-state lithium-metal batteries is limited by interfacial lithium deposition behaviour. In this study, we propose an innovative buffer layer for the electrolyte-lithium anode interface that combined interfacial dynamics with lithium-metal compatibility. A heterogeneous nanofiber buffer layer of LLZO@MoS2, possessing bifunctional ion transport and electronic insulation, has been successfully developed, effectively regulating the potential distribution at the interface to ensure uniform lithium ion deposition. Meanwhile, LLZO@MoS2composite polymer intermediate layer heterogeneous nanofibers is employed to optimize potential distribution on the lithium metal surface. This design leverages enhanced interfacial compatibility to effectively mitigate electron leakage from Li to LLZO grain boundaries/defects, optimize Li+ transport kinetics, and consequently improve cycling stability at high current densities. The unique buffer layer enables a critical current density (CCD) of 1.5 mA cm−2. The resulting symmetric cells exhibit an impressive 2000 h cycle life at a practical current density of 0.8 mA cm−2. When paired with a variety of cathodes, it provides stable and highly reversible capacity. Specifically, the assembled NCM811 cell has a highly reversible capacity of 188 mAh g−1 at 0.1 C and a good cycle stability of 1000 cycles at 0.5 C. This finding breaks with conventional strategies aimed at improving the overall performance of solid-state lithium-metal batteries with LLZO-based composite electrolytes (LLZO CSE) and significantly optimises the lithium deposition behaviour during cycling.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104628"},"PeriodicalIF":20.2,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145116642","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

Dual-salt-additive reinforced commercial carbonate-based electrolytes for 4.7 V high-voltage practical Li-ion and Li-metal batteries 用于4.7 V高压实用锂离子和锂金属电池的双盐添加剂增强商用碳酸盐基电解质

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-22 DOI: 10.1016/j.ensm.2025.104627

Wei Sun , Qian Yu , Shuai Wang , Wenjun Zhang , Zhongxue Chen , He Miao , Jinliang Yuan , Lan Xia

{"title":"Dual-salt-additive reinforced commercial carbonate-based electrolytes for 4.7 V high-voltage practical Li-ion and Li-metal batteries","authors":"Wei Sun , Qian Yu , Shuai Wang , Wenjun Zhang , Zhongxue Chen , He Miao , Jinliang Yuan , Lan Xia","doi":"10.1016/j.ensm.2025.104627","DOIUrl":"10.1016/j.ensm.2025.104627","url":null,"abstract":"<div><div>The commercial lithium hexafluorophosphate (LiPF6)/carbonate electrolyte system, despite dominating lithium-ion battery technologies for over three decades, remains fundamentally constrained by two critical flaws, including insufficient thermodynamic stability, resulting in aggressive lithium dendrites growth and severe cathode-electrolyte reactions at high voltages, coupled with the instability of the LiPF6 against moisture. Herein, we introduce a dual-salt additive of 0.1 mol L−1 (M) lithium difluorophosphate (LiDFP) and 0.1 M lithium nitrate (LiNO3) into the commercial carbonate electrolyte. Both NO3− and DFP− anions mainly dominate in the first solvation sheath of Li+ and simultaneously enrich in the inner Helmholtz plane (IHP) at the electrode surface, leading to the formation of a uniform and inorganic-rich interphase dominated by LiF, Li3PO4, and Li3N, effectively stabilizing electrode interfaces. Consequently, the optimized electrolyte enables stable Li+ intercalation/deintercalation in graphite anodes, and cycling of over 500 cycles for 4.7 V-class Li||NCM811 batteries. Remarkably, due to the strong interaction between NO3− and H2O molecules, this electrolyte also exhibits astonishing stability toward water. This dual-salt additive strategy bridges the gap between laboratory innovation and industrial practicality, offering a scalable, cost-effective electrolyte engineering solution for next-generation high-voltage lithium metal batteries compatible with existing manufacturing protocols.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104627"},"PeriodicalIF":20.2,"publicationDate":"2025-09-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145103699","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

Schottky-type oxygen defect and orbital engineering of bismuth oxide for boosting sulfur redox kinetics 肖特基型氧缺陷和促进硫氧化还原动力学的氧化铋轨道工程

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-21 DOI: 10.1016/j.ensm.2025.104626

Mingjie Yi , Huanchun Zhang , Yancen Li , Shunyou Hu , Yang Yang , Runcang Sun

{"title":"Schottky-type oxygen defect and orbital engineering of bismuth oxide for boosting sulfur redox kinetics","authors":"Mingjie Yi , Huanchun Zhang , Yancen Li , Shunyou Hu , Yang Yang , Runcang Sun","doi":"10.1016/j.ensm.2025.104626","DOIUrl":"10.1016/j.ensm.2025.104626","url":null,"abstract":"<div><div>Lithium-sulfur (Li||S) batteries face significant challenges due to the shuttle effect and sluggish redox kinetics of lithium polysulfides (LiPSs). In this work, Schottky-type oxygen vacancies-enriched p-block bismuth oxide (S-OVS-Bi2O3) is integrated onto lignin-derived carbon nanofibers (CNFs), forming a functional layer (S-OVS-Bi2O3@CNFs) on the separator of high-performance Li||S batteries. Schottky-type oxygen vacancies induce localized crystal lattice distortions, which in turn alter the spatial distribution of the local electronic density, modify the band structures of S-OVS-Bi2O3, narrow the band gap, and enhance electronic conductivity by promoting interband electron transfer. In situ characterizations confirm that S-OVS-Bi2O3 effectively mitigates the shuttle effect and facilitates the redox reactions of LiPSs. The S-Ovs-Bi2O3@CNFs-based cells exhibit a cyclability of 630 mAh g−1 at 1 C over 1000 cycles with a degradation rate of 0.032 % per cycle, and a high areal capacity of 4.36 mAh cm−2 under a high sulfur loading of 7.0 mg cm−2. This work highlights the influence of Schottky-type-vacancy-induced modulation of the p-orbital electronic configuration and p-band center, which lowers antibonding energy, improves electron occupancy in antibonding orbitals, and optimizes the chemical adsorption for LiPSs, offering valuable insights for the design of future electrocatalysts in energy storage applications.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104626"},"PeriodicalIF":20.2,"publicationDate":"2025-09-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145093708","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

Tuning additive functionality via a molecular-by-design strategy: Acyl silanes for stable high-nickel cobalt-lean cathodes in lithium-based batteries 通过分子设计策略调整添加剂功能：用于锂基电池中稳定的高镍钴贫阴极的酰基硅烷

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-20 DOI: 10.1016/j.ensm.2025.104622

Mamta Sham Lal , Yogendra Kumar , Yury Glagovsky , Robin Kumar , Dmitry Bravo-Zhivotovskii , Yitzhak Apeloig , Xiulin Fan , Doron Aurbach , Malachi Noked

{"title":"Tuning additive functionality via a molecular-by-design strategy: Acyl silanes for stable high-nickel cobalt-lean cathodes in lithium-based batteries","authors":"Mamta Sham Lal , Yogendra Kumar , Yury Glagovsky , Robin Kumar , Dmitry Bravo-Zhivotovskii , Yitzhak Apeloig , Xiulin Fan , Doron Aurbach , Malachi Noked","doi":"10.1016/j.ensm.2025.104622","DOIUrl":"10.1016/j.ensm.2025.104622","url":null,"abstract":"<div><div>Developing multifunctional electrolyte additives is essential for stabilizing high-nickel cobalt-lean cathodes, which are prone to interphase instability and parasitic side reactions, particularly at elevated voltages. Herein, a molecular-by-design strategy is presented that enables systematic tuning of interphase chemistry and hydrofluoric acid (HF) scavenging capability via single-bond (Si–X, X = Me, Me2N, F) variation within an acyl silane framework. Three structurally analogous yet functionally distinct additives were synthesized: di-tert-butyl methyl adamantoyl silane ((Me)tBu2SiCOAd; Ad is 1-Ad), (di-methyl amino) di-tert-butyl adamantoyl silane ((Me2N)tBu2SiCOAd), and di-tert-butyl fluoro adamantoyl silane ((F)tBu2SiCOAd). In Li||LiNi0.9Co0.05Mn0.05O2 (Li||NCM90) cells with carbonate-based electrolyte, (Me2N)tBu2SiCOAd, significantly improves cycling stability, delivering 90 % capacity retention after 200 cycles at 1C and 4.3 V (30 % improvement over the blank), and 80 % retention at 4.4 V (42 % improvement). This enhancement is attributed to its multifunctionality: stable interphase formation and effective HF scavenging via the Si-N bond. Conversely, (Me)tBu2SiCOAd contributes only to interphase formation, while (F)tBu2SiCOAd is ineffective. These findings are supported by theoretical simulations, which reveal a low activation barrier for HF scavenging by (Me2N)tBu2SiCOAd and explain the inert behavior of (F)tBu2SiCOAd. Overall, this study demonstrates how targeted single-bond modulation enables precise molecular tuning of additive functionality in high-nickel cobalt-lean systems.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104622"},"PeriodicalIF":20.2,"publicationDate":"2025-09-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145089591","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

Hydrofluoric-fixation separators through hydrogarnet electrolyte bonded by silane for long-cycling lithium metal batteries 长循环锂金属电池用硅烷键合石榴石电解液固氢氟分离器

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-19 DOI: 10.1016/j.ensm.2025.104625

Yaqiong Zhu , Ye Zeng , Dezhi Yang , Zhiqian Hou , Hansong Yang , Xi Gong , Yanan Yang , Tao Zhang

{"title":"Hydrofluoric-fixation separators through hydrogarnet electrolyte bonded by silane for long-cycling lithium metal batteries","authors":"Yaqiong Zhu , Ye Zeng , Dezhi Yang , Zhiqian Hou , Hansong Yang , Xi Gong , Yanan Yang , Tao Zhang","doi":"10.1016/j.ensm.2025.104625","DOIUrl":"10.1016/j.ensm.2025.104625","url":null,"abstract":"<div><div>Lithium metal batteries (LMBs) with high-voltage cathodes easily suffer from electrode structure degeneration caused by hydrogen fluoride (HF) attack, especially in electrolytes with high moisture content. Herein, we report a hydrofluoric-fixation bifunctional separator, in which 3-aminopropyltriethoxysilane (APTES) - modified hydrogarnet electrolyte (Li1.5La3Zr1.5Ta0.5O7(OH)5) serves as a functional layer on a polypropylene (PP) separator surface. The silane acts as fixation sites for HF via Si-F bond formation, effectively eliminating HF in the electrolyte and inhibiting cathode degradations. Simultaneously, the hydrogarnet electrolyte enhances lithium-ion transfer kinetics owing to its high ionic conductivity, leading to suppressions of lithium dendrites. As a result, symmetric Li cells employing PP@LH-A separators exhibit stable cycling for 2000 h at 5 mA cm-2. Li/LiNi0.6Co0.2Mn0.2O2 (NCM622) cells possess a capacity retention rate of 78.2 % at 2 C after 500 cycles, even in the electrolytes containing 500 ppm of water. This strategy offers a promising approach for HF fixation in high-voltage lithium metal batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104625"},"PeriodicalIF":20.2,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083686","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

Clarifying the microscopic origin of Mn3+ ion instability in cathode oxides 澄清阴极氧化物中Mn3+离子不稳定性的微观成因

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-19 DOI: 10.1016/j.ensm.2025.104624

Yin Huang , Liang Xue , Jiangfeng Huang , He Zhu , Hongfei Zheng , Lei Yu , Chao Wang , Pan Xiong , Jingwen Sun , Yongsheng Fu , Jun Lu , Junwu Zhu

{"title":"Clarifying the microscopic origin of Mn3+ ion instability in cathode oxides","authors":"Yin Huang , Liang Xue , Jiangfeng Huang , He Zhu , Hongfei Zheng , Lei Yu , Chao Wang , Pan Xiong , Jingwen Sun , Yongsheng Fu , Jun Lu , Junwu Zhu","doi":"10.1016/j.ensm.2025.104624","DOIUrl":"10.1016/j.ensm.2025.104624","url":null,"abstract":"<div><div>The pronounced mobility of Mn3+ ions in oxygen sublattice critically limits the utilization of Mn3+/Mn4+ redox couples for cathode materials. While Mn3+ instability has historically long been associated with their inherent Jahn-Teller (JT) effect, the microstructural features and electronic-state evolutions underlying the Mn migration remain insufficiently understood, hindering the development of effective Mn stabilization strategies. Here, we demonstrate that the Mn3+ site instability is not an inherent property of the JT effect but closely depends on their local coordination environment. Using spinel LiMn2O4 as a research model, we experimentally demonstrate that Mn migration induced by coordination instability preferentially occurs within the 0–50% SOC, where both Li vacancies and a high concentration of Mn3+ ions coexist. Under these structural conditions, weakly hybridized oxygen orbitals aligned with elongated Mn3+–O bonds act as electronic donors, stabilizing the linear Mn–O–Mn configuration in the degraded state. This electronic stabilization reduces the energetic penalty for Mn migration, thereby uncovering the microscopic origin of site instability that drives Mn3+ migration.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104624"},"PeriodicalIF":20.2,"publicationDate":"2025-09-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083687","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

A brief review of engineering “balance” challenges for electrolytes of all-solid-state lithium-metal battery 综述全固态锂金属电池电解液的工程“平衡”挑战

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-18 DOI: 10.1016/j.ensm.2025.104623

Yaohui Liang , Zhiwei Xu , Xu Xiao , Nan Chen

{"title":"A brief review of engineering “balance” challenges for electrolytes of all-solid-state lithium-metal battery","authors":"Yaohui Liang , Zhiwei Xu , Xu Xiao , Nan Chen","doi":"10.1016/j.ensm.2025.104623","DOIUrl":"10.1016/j.ensm.2025.104623","url":null,"abstract":"<div><div>Solid-state electrolytes are promising in enhancing safety and energy density of lithium-metal batteries. Significant progress made in recent years calls for a fresh perspective on the electrolyte development to guide future research. After thorough investigation and analysis, we propose that the current bottleneck lies in property “balance” to achieve practical applications of solid electrolytes. In this review, we present the state art of inorganic solid electrolytes, polymer electrolytes, and hybrid solid electrolytes, and discuss the strategies to “balance” the properties of those electrolytes especially the advanced preparation methods and sophisticated structural designs. Firstly, we provide an overview of different types of solid-state electrolytes, highlighting their potential benefits. Then we delve into their separated challenges faced by the proposed paired properties with correlation. For inorganics, we explore the balance between cost and conductivity, interphase e- and Li+ transportation, thickness and mechanical property. As for polymers, we examine the balance between Li+ transference number and conductivity, mechanical property and conductivity, anodic and cathodic stability. Furthermore, we summarize effective strategies for constructing hybrid solid electrolytes with low interfacial resistance and high Li+ conductivity. Lastly, we offer comments and expectations on the future development of solid electrolytes based on “balance” strategy.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104623"},"PeriodicalIF":20.2,"publicationDate":"2025-09-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145083688","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

Surface Lattice Regulation Drives Energy Coupling to Stabilize High-Energy Mn-based Prussian Blue Analogue Cathode 表面晶格调节驱动能量耦合以稳定高能锰基普鲁士蓝模拟阴极

IF 20.4 1区材料科学

Energy Storage Materials Pub Date : 2025-09-17 DOI: 10.1016/j.ensm.2025.104621

Chunhui Zhong, Fan Li, Haohong Chen, Yuncai Chen, Guobin Zhang, Haijun Zhang, Qingxia Liu

{"title":"Surface Lattice Regulation Drives Energy Coupling to Stabilize High-Energy Mn-based Prussian Blue Analogue Cathode","authors":"Chunhui Zhong, Fan Li, Haohong Chen, Yuncai Chen, Guobin Zhang, Haijun Zhang, Qingxia Liu","doi":"10.1016/j.ensm.2025.104621","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104621","url":null,"abstract":"Sodium-ion batteries (SIBs) are considered as competitive candidates for energy storage applications due to their abundant resources and low cost. Na2Mn[Fe(CN)6] (NaMnPB) is an ideal cathode material for SIBs because of its high theoretical energy density. However, it usually suffers from sluggish reaction kinetic and rapid capacity fading due to manganese (Mn) Jahn-Teller distortion. To address these issues, a surface lattice contraction strategy induced by surface [Fe(CN)6] vacancies is proposed. The surface [Fe(CN)6] vacancies lead to a charge imbalance and facilitate d-electron compensation from Fe to Mn, which drives the energy coupling of low-spin Fe2+ and high-spin Mn2+ and promotes the redox activity of Mn2+/Mn3+. Consequently, the π-backdonation in the low-spin Fe−C unit and the π-donation in the high-spin Mn−N unit work synergistically, mitigating the continuous electron delocalization of Mn2+ and the associated Jahn-Teller distortion. This approach stabilizes the NaMnPB structure while maintaining its inherent high discharge potential without elements doping. The as-prepared NaMnPB□-3 delivers a high specific capacity of 148.97 mAh/g with a corresponding energy density of 464.40 Wh/kg at a current density of 15 mA/g. Furthermore, the full-cell assembled with NaMnPB□-3 and hard carbon demonstrates high energy density, superior rate capability, and excellent cycling performance, indicating its potential for large-scale energy storage systems. This research provides valuable insights into stabilizing high-energy Mn-based cathodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"16 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145078539","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

Bifunctional cationic polyelectrolyte additive enables dendrite-free and shuttle-suppressed zinc-bromine batteries 双功能阳离子聚电解质添加剂实现无枝晶和抑制穿梭的锌-溴电池

IF 20.2 1区材料科学

Energy Storage Materials Pub Date : 2025-09-16 DOI: 10.1016/j.ensm.2025.104620

Xiaofei Miao , Jingye Chen , Xiaolin Zheng , Huiqi Li , Lei Zhang

{"title":"Bifunctional cationic polyelectrolyte additive enables dendrite-free and shuttle-suppressed zinc-bromine batteries","authors":"Xiaofei Miao , Jingye Chen , Xiaolin Zheng , Huiqi Li , Lei Zhang","doi":"10.1016/j.ensm.2025.104620","DOIUrl":"10.1016/j.ensm.2025.104620","url":null,"abstract":"<div><div>Zinc-bromine (Zn-Br2) batteries are attractive candidates for large-scale energy storage owing to their low cost and high energy density. However, their practical deployment remains impeded by the zinc dendrites growth and polybromide shuttle diffusion effects, which compromise long-term cycling and energy efficiency. Herein, we introduce a low-concentration, bifunctional polyelectrolyte additive, polyquaternium-6 (P-6), that simultaneously addresses both challenges. Electrochemical analyses, in-situ Raman spectroscopy, and theoretical computation reveal that P-6 selectively adsorbs on Zn (002)/(100) facets, facilitating uniform Zn deposition along the kinetically favourable (101) orientation while suppressing dendrite formation via electrostatic shielding. Simultaneously, P-6 forms stable complexes with Br3- and Br5-, effectively inhibiting their shuttle diffusion. Consequently, Zn-Br2 battery incorporating only 0.65 wt. % P-6 (∼44 mM) delivers a high capacity of ∼1300 μAh cm-2 and exhibit outstanding stability over 1500 cycles with >98 % Coulombic efficiency. This bifunctional electrolyte strategy effectively addresses interfacial challenge in Zn-Br2 batteries and may serve as a guiding principle for the design of additives in broader aqueous halogen-based system.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104620"},"PeriodicalIF":20.2,"publicationDate":"2025-09-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145072084","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