Energy Storage Materials最新文献

{"title":"A cross-linked AB-type alternating perfluoroalkyl-ethylene oxide polymer electrolyte for high-performance all-solid-state lithium-metal batteries","authors":"Alem Gebrelibanos Hailu ,&nbsp;Ljalem Hadush Abraha ,&nbsp;Zishuo Zhao ,&nbsp;Doosoo Kim ,&nbsp;Siddhartha Nanda ,&nbsp;Hadi Khani","doi":"10.1016/j.ensm.2025.104485","DOIUrl":"10.1016/j.ensm.2025.104485","url":null,"abstract":"<div><div>Poly(ethylene oxide) (PEO) derivatives are attractive Li⁺-conducting solid polymer electrolytes (SPEs) due to their high lithium salt solubility but face challenges with low ionic conductivity and interfacial stability. In contrast, fluorinated polymers offer superior chemical and mechanical stability but limited salt solubility and conductivity. To address these challenges, we developed a cross-linked AB-type alternating copolymer electrolyte, poly(TEGDVE-OFDIB)-LiTFSI, via iodo-ene photopolymerization of triethylene glycol divinyl ether (TEGDVE) and octafluoro-1,4-diiodobutane (OFDIB) in the presence of LiTFSI. TEGDVE enhances film flexibility and cross-linking while enabling Li⁺ transport through sequential Li⁺ coordination and decoordination, whereas OFDIB serves as both a structural spacer and electrostatic mediator, with its negative electrostatic potential stabilizing the electrochemical interface while facilitating Li⁺ conduction between TEGDVE units. The resulting SPE achieves a Li⁺ conductivity of 1.3 × 10⁻⁴ S cm⁻¹, a transference number of 0.55, and a stability window of 4.98 V at 40 ℃. All solid-state lithium-metal batteries (ASSLMBs) with a LiFePO₄ cathode and the SPE retain 100 % capacity over 500 cycles at 0.5C. With an NMC811 cathode, the cell delivers an initial capacity of 157.7 mAh g⁻¹ with 80 % capacity retention after 100 cycles. This work establishes iodo-ene polymerization as a versatile strategy for designing high-performance AB-type alternating copolymer electrolytes for ASSLMBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104485"},"PeriodicalIF":18.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685108","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":"Highly synergistic electrocatalysis and confinement of covalently bonded heterostructures enable high-efficient-stable Li−S batteries","authors":"Tong Wang ,&nbsp;Jiang Zhong ,&nbsp;Xinwei Huang ,&nbsp;Junfan Zhang ,&nbsp;Zenan Zhao ,&nbsp;Chuguang Yu ,&nbsp;Jing Wang ,&nbsp;Jinhui Cao ,&nbsp;Chang-Jiang Yao ,&nbsp;Jia-Qi Huang ,&nbsp;Feng Wu ,&nbsp;Guoqiang Tan","doi":"10.1016/j.ensm.2025.104477","DOIUrl":"10.1016/j.ensm.2025.104477","url":null,"abstract":"<div><div>Li₂S, as a high-capacity Li-containing cathode, can avoid the use of metallic Li in batteries, so as to improve cycle-life and safety. However, intrinsic low electrical conductivity, high activation barrier and serious polysulfide dissolution of Li₂S limit its performance output. Here, we propose a chemical cyclization crosslinking strategy to construct a covalently bonded Li₂S−cyclized polyacrylonitrile (cPAN) heterostructure, aiming to facilitate fast Li₂S activation and electron/ion transport as well as high volumetric accommodation. The obtained structure features crystalline Li₂S wrapped by conformal cPAN layer via robust Li−N bonding, forming compact Li₂S@cPAN core-shell nanocomposite. Systematic studies demonstrate distinguished synergistic electrocatalysis and confinement on Li₂S, where the bridge-like heterostructure composed of strong and abundant Li−N bonds facilitates fast electron/ion transport and Li₂S dissociation, and the core-shell nanostructure with elastic and dense cPAN enhances volumetric efficiency for accommodating sulfur species. Owing to improvement on both electrocatalysis and domain effects, this cathode design enables promising electrochemical performance. An optimal Li₂S@cPAN cathode exhibits a dramatically reduced activation potential (2.7 V), a largely increased output capacity (730 mAh g⁻¹), and an obviously improved cycling stability (500 cycles). This Li₂S@cPAN cathode demonstrates the great application potential for high-efficient-stable Li−S batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104477"},"PeriodicalIF":18.9,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144693796","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":"Excess-lithium-free LLZO enabling fast ion conduction and ultra-low interfacial resistance for solid-state lithium metal batteries","authors":"Mohammad Nasir ,&nbsp;Jun Seo ,&nbsp;Jae In Song ,&nbsp;Yong Seok Choi ,&nbsp;Hee Jung Park","doi":"10.1016/j.ensm.2025.104482","DOIUrl":"10.1016/j.ensm.2025.104482","url":null,"abstract":"<div><div>Garnet-type La_6.25Ga_0.25La₃ZrO₁₂ (LLZO:Ga) is a leading solid electrolyte for next-generation solid-state lithium batteries (SSLBs), yet its widespread adoption is hindered by the routine need for excess lithium and protective powder coverings during synthesis, both of which increase costs and compromise interface stability. Here, we present a scalable, excess-lithium-free synthesis of LLZO:Ga that achieves ultrafast Li-ion conductivity of 1.64(3) × 10^–3 S/cm at 25 °C, surpassing many Li-rich counterparts. Molecular dynamics simulations reveal that excess lithium blocks diffusion pathways, hindering ion mobility and cooperative hopping. Remarkably, the zero-Li-excess LLZO:Ga delivers ultralow interfacial resistance (∼5 Ω·cm²) in symmetric Li|LLZO:Ga|Li cells, enabling stable cycling beyond 700 h at 0.2 mA/cm² with minimal overpotential (∼60 mV). Full cells paired with LiFePO₄ retain ∼96 % capacity over 80 cycles (at 0.1C), demonstrating practical viability. This work establishes a new benchmark in solid electrolyte design, achieving high conductivity, stable interfaces, and scalable processability without lithium excess.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104482"},"PeriodicalIF":20.2,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678198","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":"Pyrrolidine ionic liquid enables dynamic EDL regulation for highly stable aqueous Zn Ion capacitors","authors":"Kailimai Su ,&nbsp;Zongkun Bian ,&nbsp;Yongbiao Mu ,&nbsp;Zhibin Lu ,&nbsp;Yan Wang ,&nbsp;Ming Li ,&nbsp;Jingxin Zhao ,&nbsp;Junwei Lang ,&nbsp;Bingang Xu","doi":"10.1016/j.ensm.2025.104480","DOIUrl":"10.1016/j.ensm.2025.104480","url":null,"abstract":"<div><div>Aqueous Zn-based energy storage devices have garnered significant attention and research interest owing to their numerous advantages, including low cost, inherent safety, and eco-friendliness. Nevertheless, detrimental Zn dendrites and side reactions triggered by the water-rich electric double layer (EDL) and unstable solid electrolyte interface (SEI) are still the critical factors that limit the service life of Zn-ion energy storage systems. In this paper, we constructed a dynamic EDL structure under varying interface charges by using a N‑butyl‑N-methylpyrrolidine tetrafluoroborate (Py14BF4) ionic liquid (IL) as an electrolyte additive. On one hand, the strong interaction between the Py14BF4 and H2O disrupted the H-bonds between the H2O molecules in both the diffusion layer and the outer Helmholtz layer (OHL) of the EDL, thereby suppressing the activity of H2O. On the other hand, the stronger adsorption energy for Zn of Py14BF4, along with its lower energy level of the lowest unoccupied molecular orbital (LUMO), is utilized to modulate the ion/molecule composition of the HL of the EDL, and promote the in-situ formation of a self-healing organic-inorganic hybrid SEI protective layer. Based on this, the introduction of Py14BF4 effectively alleviates the dendrites and side reactions issues of Zn anode during the long-term cycling process, and the Zn//Zn battery shows a highly stable life of 3300 h at 0.5 mA cm-2. Impressively, the Zn//AC capacitor exhibits ultra-long cycle stability at 5 A g-1 with a capacity retention rate of 93 % after 60,000 cycles.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104480"},"PeriodicalIF":18.9,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144678197","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":"A medium-entropy Li-garnet solid electrolyte with ultrahigh ionic conductivity and outstanding electrochemical stability for solid-state batteries","authors":"Muhammad Umair ,&nbsp;Hafiz Talha Hasnain Rana ,&nbsp;Suzhu Yu ,&nbsp;Jun Wei","doi":"10.1016/j.ensm.2025.104484","DOIUrl":"10.1016/j.ensm.2025.104484","url":null,"abstract":"<div><div>Solid-state batteries (SSBs) have gained attention as a next-generation energy storage technology, with solid-state electrolytes (SSEs) serving as a key component in their development. Garnet-type SSEs, known for their high stability, face limitations due to low ionic conductivity. High-entropy ceramics, with intrinsic structural disorder and tunable compositions, offer a pathway to overcome these challenges. In this study, we innovatively design and develop a medium-entropy garnet-type SSE of Li₆La₃Zr_0.5Ti_0.5Ta_0.5Nb_0.5O₁₂ (LLZTTNO) by partially substituting Zr with Ti, Ta, and Nb. The incorporation of these multiple elements introduces lattice disorder and facilitates fast ion transport through low-energy diffusion pathways, therefore, greatly enhances the electrochemical performance of the SSE. Consequently, LLZTTNO demonstrates excellent ionic conductivity (1.52 × 10^–3 S cm^-1), a low Li-ion activation energy for Li⁺ transport (0.18 eV), and minimal electronic conductivity (6.88 × 10^–10 S cm^-1). A Li-graphite (Li-C) composite was employed as an anode to enhance interfacial compatibility between the solid electrolyte and electrode. The Li-C/LLZTTNO/Li-C symmetric cell demonstrates long-term lithium plating/stripping for over 3600 h at 0.1 mA cm^-2, and achieves a critical current density of 2.5 mA cm^-2. The Li-C/LLZTTNO/LFP full cell also delivers a specific capacity of 143.87 mAh g^-1 and retains 83.4 % of its capacity over 150 cycles at a 0.1 C rate. This work supports the potential application of medium-entropy garnet SSEs for next-generation SSBs, providing valuable insights into their electrochemical performance and stability.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104484"},"PeriodicalIF":18.9,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685111","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":"Thermal switches for lithium-ion battery thermal management: Principle, performance and application","authors":"Peihang Li ,&nbsp;Mingjian Xu ,&nbsp;Xiaojie Guo ,&nbsp;Pengjun Zheng ,&nbsp;Weiping Qu ,&nbsp;Chengshuai Xu ,&nbsp;Da Liu ,&nbsp;WenHui Gan ,&nbsp;Deqiu Zou","doi":"10.1016/j.ensm.2025.104481","DOIUrl":"10.1016/j.ensm.2025.104481","url":null,"abstract":"<div><div>Lithium-ion battery (LIB) is increasingly deployed in a wide range of applications. However, its temperature sensitivity presents two critical challenges: all-climate thermal management for efficient heat dissipation in high temperature environments and insulation in low temperature environments, and reversible protection for thermal runaway (TR). Thermal switches, as intelligent thermal management devices, have been shown to effectively address both challenges. Specifically, external thermal switches enable all-climate thermal management to reconcile low- and high-temperature operation, while internal thermal switches achieve reversible TR protection through temperature-responsive electrochemical modulation. This review discusses LIB thermal management (LIBTM) strategies based on thermal switches, detailing the operational principles of both external and internal thermal switches, and their critical roles in enhancing battery performance and safety across wide temperature ranges. The necessity of employing thermal switches in LIBTM systems is first explained, and their operational mechanisms, along with classification criteria, are introduced. The distinct action mechanisms of external and internal thermal switches are then analyzed, with an evaluation of their respective impacts on LIB performance. Finally, current challenges are identified, potential solutions are proposed, and key directions for future research in this emerging field are outlined.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104481"},"PeriodicalIF":20.2,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685110","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":"Unveiling the Peierls effect during electrochemical delithiation/lithiation process in magnesium (2,5-dilithium-oxy)-terephthalate using combined experimental and computational studies","authors":"Alia Jouhara,&nbsp;Eric Quarez,&nbsp;Nicolas Gautier,&nbsp;Florent Boucher,&nbsp;Etienne Janod,&nbsp;Nicolas Dupré,&nbsp;Joël Gaubicher,&nbsp;Philippe Poizot","doi":"10.1016/j.ensm.2025.104456","DOIUrl":"10.1016/j.ensm.2025.104456","url":null,"abstract":"<div><div>Organic host electrode materials offer a promising route for the development of sustainable secondary batteries, with reduced resource dependency and eco-friendly synthesis. However, the understanding of insertion mechanisms remains complex, primarily due to the challenges associated with resolving the crystal structures of these materials especially with lithiated structures. This study investigates the phase transformation pathways occurring in magnesium (2,5-dilithium-oxy)-terephthalate during the electrochemical reversible extraction/uptake of lithium. A combination of advanced techniques, including electron diffraction tomography, powder X-ray diffraction, and density functional theory calculations, was successfully employed to elucidate the crystal structure of this electrode material. The structure exhibits a compact layered arrangement (2.189 g cm⁻³) and a distinctive coordination environment surrounding the phenolate group, which involves both Li⁺ and Mg²⁺ ions. The Mg²⁺ ion, exhibiting a high ionic potential, mitigates the donor inductive effect of the conjugated CO⁻/CO₂⁻ groups, resulting in a high working potential for this <em>n</em>-type redox-active organic skeleton, comparable to that of LiFePO₄. The electrochemical solid-state process, studied using <em>operando</em> synchrotron X-ray diffraction, revealed an asymmetric delithiation/lithiation mechanism, linked to Peierls-distorted π-stacks of radicals, confirmed by DFT calculations and electron spin resonance experiments. Finally, analysis of the electronic structure of the semiquinone Mg(Li₁)-<em>p</em>-DHT^• phase, with spin-coupled diamagnetic dimers, showed that removal of the second electron (resulting in the quinone form) is unfavorable due to the weakening or destruction of the carboxylate C<em>=</em>O bond. This observation sheds light on the limited capacity of <em>p</em>-DHT-based compounds, which typically reach only half of their theoretical capacity due to the occurrence of the Kolbe electrolysis reaction.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104456"},"PeriodicalIF":20.2,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144677749","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":"Synergistic nano-micro structuring boosts high-Ni cathode performance for all-solid-state lithium-ion batteries","authors":"Hyungyeon Cha ,&nbsp;Hyomyung Lee ,&nbsp;Wooyoung Jin ,&nbsp;Sujong Chae ,&nbsp;Ohjoon Kwon ,&nbsp;Jaephil Cho ,&nbsp;Namhyung Kim","doi":"10.1016/j.ensm.2025.104470","DOIUrl":"10.1016/j.ensm.2025.104470","url":null,"abstract":"<div><div>Grid-scale energy storage has emerged as a critical component for modern power systems, so batteries are at the forefront of this technological revolution. This trend delves into the long-duration, higher energy and safer energy storage system. All-solid-state lithium-ion battery system is one of the promising candidates for addressing this challenges, and high-Ni material is notable cathode due to its high energy density and high technical maturity for practical applications. However, their performances in solid electrolyte system still cannot achieve the performance levels that are attained in the conventional liquid electrolyte system with severe reaction inhomogenity. Therefore, for the effective utilization and prolonged lifespan of high-Ni cathode materials in all-solid-state lithium-ion batteries, careful design of particles in both nano-scale and micro-scale is necessary. In this work, we designed three different LiNi_0.8Co_0.1Mn_0.1O₂ (Polycrystalline, single-crystal, cluster with twin boundaries) by tuning the nanostructure and microstructure and revealed how these particles are utilized in all-solid-state lithium-ion battery system. We found that the intentionally synthesized defects at particle surface can enhance Li-ion diffusivity, and single crystal structure greatly improves reaction homogeneity. We also demonstrate comparative studies of these high-Ni particles in both liquid and solid electrolyte system. These results provide opportunities for gaining insights into how to design high-Ni materials for the future all-solid-state lithium-ion battery system.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104470"},"PeriodicalIF":18.9,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144677753","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":"Emerging non-carbon cathodes for advanced mild aqueous Zn-ion capacitors","authors":"Cuiqin Fang ,&nbsp;Zhenguo Gao ,&nbsp;Tiandi Chen ,&nbsp;Yaopeng Wu ,&nbsp;Yuejiao Chen ,&nbsp;Bingang Xu","doi":"10.1016/j.ensm.2025.104476","DOIUrl":"10.1016/j.ensm.2025.104476","url":null,"abstract":"<div><div>Conventional Zn-ion capacitors (ZICs) predominantly utilize carbonaceous cathodes in carbon//Zn configurations, leveraging surface-dominated ion adsorption/desorption to deliver high power density and prolonged cycle life. As carbon-based systems approach their performance ceiling, cathode evolution is increasingly pivoting toward non-carbon materials. While prior reviews have acknowledged their existence, a comprehensive review remains absent. Herein, this review systematically charts the paradigm shift to non-carbon cathodes, dissecting their Zn-ion storage mechanisms and performance landscapes. Emerging non-carbon cathodes are categorized as pseudocapacitive-type (MXenes, transition metal compounds, organics, etc.) and battery-type (V/Mn-based compounds, Prussian blue analogs), with rigorous evaluation of voltage window, specific capacitance, energy/power density, rate capability, and cycle stability. Persistent scientific challenges, including restricted theoretical capacitance, suboptimal electrolyte compatibility, material dissolution, structural degradation, and sluggish storage kinetics, are critically discussed. The review further analyzes optimization strategies across material design, structural modulation, and electrolyte formulation refinement to solve these challenges. Looking forward, we propose targeted research priorities to propel non-carbon cathodes beyond current constraints. This review underscores the translational potential of non-carbon cathodes in redefining the performance frontiers of mild aqueous ZICs, ultimately harmonizing high energy/power density, ultrafast storage kinetics, and robust durability.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104476"},"PeriodicalIF":18.9,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144670064","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":"A bioinspired flexible hydrogel electrolyte with β-sheet–directed interphase for dendrite-free Zn metal batteries","authors":"Panpan Shen ,&nbsp;Shilin Xu ,&nbsp;Dehua Li ,&nbsp;Yuting Lin ,&nbsp;Yue Zhang ,&nbsp;Junjie Huang ,&nbsp;Xun Wang ,&nbsp;Jianhong Xu ,&nbsp;Weiyu Teng ,&nbsp;Yaoxi Shen ,&nbsp;Mingyu Liu ,&nbsp;Zhen Shen ,&nbsp;Yi Hu","doi":"10.1016/j.ensm.2025.104464","DOIUrl":"10.1016/j.ensm.2025.104464","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZIBs) have attracted growing attention due to their intrinsic safety, low cost, and environmental compatibility. However, challenges such as zinc dendrite formation, electrode passivation, and parasitic side reactions continue to impede long-term cycling stability. Inspired by conformational transitions in natural proteins, we propose a biomimetic interfacial engineering strategy by introducing silk fibroin (SF) into a hydrogel electrolyte. Upon solvent induction, SF undergoes a structural transition from α-helix to β-sheet, forming a dense, ionically conductive interphase on the Zn anode. The ordered β-sheet network, enriched with Zn-affinitive polar groups, modulates Zn²⁺ solvation, guides deposition along the (002) crystal plane, and suppresses dendrite growth and side reactions. Density functional theory (DFT) and molecular dynamics (MD) simulations reveal the mechanism of solvation structure reconstruction and interfacial stabilization. Benefiting from this design, the β-SF hydrogel electrolyte enables stable Zn plating/stripping over 2500 hours at 1 mA cm⁻², while the Zn//MnO₂ full cell retains 93.8 % capacity after 1500 cycles at 1.0 A <em>g</em>⁻¹. Moreover, the fibrous and flexible configuration exhibits excellent mechanical durability and device compatibility. This work presents a protein-based interfacial strategy driven by conformational regulation, offering a new pathway toward high-performance, durable, and flexible AZIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104464"},"PeriodicalIF":18.9,"publicationDate":"2025-07-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144669908","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}