{"title":"Deep-learning based prediction of chemo-mechanics and damage in battery active materials","authors":"Zehou Wang , Ying Zhao , Zheng Zhong , Bai-Xiang Xu","doi":"10.1016/j.ensm.2025.104581","DOIUrl":"10.1016/j.ensm.2025.104581","url":null,"abstract":"<div><div>Layer-structured cathode active materials of Li-ion batteries such as <figure><img></figure> (NMC) provide benefits including high specific capacity and energy density. However, NMC materials (secondary particles) consist of randomly oriented grains (primary particles), which features anisotropic lattice chemical strain inside each grain and weak intergranular bonding. During <figure><img></figure> insertion into and extraction from the active material, high stresses arise at the interfaces between primary particles and particle disconnection occurs. Therefore, material microstructure characteristics such as grain orientation and morphology play a critical role in determining cycling performance of the active material. However, resolving particle microstructures with different characteristics remains challenging due to high computational costs and limited statistical generalizability. In this work, ConvLSTM is employed to predict the dynamic evolution of critical physical fields — including <figure><img></figure> concentration, stresses and damage — inside secondary particles with diverse microstructures. First, the microstructure of active particles are generated with a certain number of primary particles, whose sizes and orientations can strictly follow given statistical distributions with binning method, even with limited particle numbers. Second, images carrying essential characteristics of microstructure evolution are incorporated into the model. A hybrid loss combining Mean Squared Error (MSE) and Structural Similarity Index (SSIM) is employed, along with a scheduled sampling training strategy, to enhance prediction accuracy. The model’s out-of-sample predictive performance has also been evaluated. Additionally, a microcrack density-based damage model is also used to assess microstructure damage evolution. This work reveals that the proposed approach achieves highly accurate predictions, providing valuable insights into microstructure behavior.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104581"},"PeriodicalIF":20.2,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145018099","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}
Wenfang Yuan , Lejuan Cai , Lisha Lu , Qian Chen , Mengxiang Han , Zihua Li , Fan Zhang , Yingying Lan , Jian Shang , Bocheng Qiu , Wenlong Wang
{"title":"Reversible Mn3+/Mn2+ redox chemistry for high-rate aqueous manganese-ion batteries","authors":"Wenfang Yuan , Lejuan Cai , Lisha Lu , Qian Chen , Mengxiang Han , Zihua Li , Fan Zhang , Yingying Lan , Jian Shang , Bocheng Qiu , Wenlong Wang","doi":"10.1016/j.ensm.2025.104598","DOIUrl":"10.1016/j.ensm.2025.104598","url":null,"abstract":"<div><div>The Mn<sup>3+</sup>/Mn<sup>2+</sup> redox couple is a promising candidate for high-rate energy storage scenarios owing to its high theoretical voltage and rapid redox kinetics. However, critical challenges such as Mn<sup>3+</sup> disproportionation and shuttle effects in aqueous electrolytes significantly limit practical implementation. Herein, we propose a synergistic strategy integrating coordination optimization and interfacial confinement to achieve highly reversible Mn<sup>3+</sup>/Mn<sup>2+</sup> redox chemistry in a mild aqueous electrolyte. Ethylenediaminetetraacetic coordinating anions are utilized to reshape the first solvation shell of Mn<sup>2+</sup>, stabilizing hydrated Mn<sup>3+</sup> intermediates and enabling a single-electron-dominated redox pathway. A sucrose-derived molecular adsorption layer is engineered on the cathode surface through electrostatic polarity interactions, effectively suppressing Mn<sup>3+</sup> migration into the bulk electrolyte. The well-designed Mn<sup>3+</sup>/Mn<sup>2+</sup> cathode delivers an areal capacity of 0.36 mAh cm<sup>−2</sup> at 4 mA cm<sup>−2</sup> with 81 % capacity retention over 3000 cycles. As proof of concept, a high-rate aqueous Mn-ion battery is assembled by pairing the Mn<sup>3+</sup>/Mn<sup>2+</sup> cathode with a polyimide anode, achieving a specific capacity of 104 mAh g<sup>−1</sup> at 0.5 A g<sup>−1</sup>, exceptional rate capability, and 73.2 % capacity retention after 1000 cycles. This work unveils the directional regulation of manganese redox chemistry by a solvation-interfacial coupling mechanism, offering a design blueprint for next-generation grid-scale energy storage technologies.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104598"},"PeriodicalIF":20.2,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009324","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}
Joo Hyeong Suh , Hong Rim Shin , Taehee Kim , Dong Ki Kim , Ki Jae Kim , Jong-Won Lee , Min-Sik Park
{"title":"Mitigating the fast-charging limitations of graphite anodes via g-C3N4 surface engineering","authors":"Joo Hyeong Suh , Hong Rim Shin , Taehee Kim , Dong Ki Kim , Ki Jae Kim , Jong-Won Lee , Min-Sik Park","doi":"10.1016/j.ensm.2025.104596","DOIUrl":"10.1016/j.ensm.2025.104596","url":null,"abstract":"<div><div>With the rapid expansion of the electric vehicle (EV) market, the demand for fast-charging lithium-ion batteries (LIBs) has increased considerably to extend the driving range and reduce charging time. However, commercial graphite (Gr) anodes suffer from slow interfacial kinetics under fast-charging conditions, ultimately causing Li plating on their surfaces, which results in significant capacity losses and safety concerns. Herein, a surface engineering approach using graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) is introduced to modify Gr anodes. Three-dimensional electrochemical modeling at particle- and electrode-levels has identified critical requirements for functional surface coatings that effectively improve the fast-charging capability. By conducting a simple chemical exfoliation process followed by a post-heat treatment, g-C<sub>3</sub>N<sub>4</sub> nanoplates form a functional surface layer on Gr particles, which reduces the activation energy for Li⁺ adsorption and migration during charging. Hence, g-C<sub>3</sub>N<sub>4</sub>-decorated Gr (g-C<sub>3</sub>N<sub>4</sub>@Gr) exhibits a lower overpotential and effectively suppresses Li plating under fast-charging conditions. When paired with a commercial LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> cathode in a full-cell configuration, the g-C<sub>3</sub>N<sub>4</sub>@Gr anode demonstrates stable cycling performance for up to 300 cycles, achieving an 80 % state of charge in only 6.8 min. This study clearly describes the fast-charging mechanism in commercial Gr anodes and a practical strategy for advancing fast-charging LIB technology.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104596"},"PeriodicalIF":20.2,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145009327","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}
Zhiying Fang , Jiapei Li , Lizhi Xiang , Kunlun Liu , Yicai Pan , Xiaoge Li , Dewu Lin , Kaiping Zhu , Cuiping Han , Yagang Yao , Pan Xue , Jie Han , Guo Hong
{"title":"Kinetic regulation of Zn(002) textured interfaces for highly reversible Zn–iodine batteries","authors":"Zhiying Fang , Jiapei Li , Lizhi Xiang , Kunlun Liu , Yicai Pan , Xiaoge Li , Dewu Lin , Kaiping Zhu , Cuiping Han , Yagang Yao , Pan Xue , Jie Han , Guo Hong","doi":"10.1016/j.ensm.2025.104592","DOIUrl":"10.1016/j.ensm.2025.104592","url":null,"abstract":"<div><div>The commercialization of zinc-ion batteries is severely hindered by anode instability, as hydrogen evolution reactions and Zn dendrite growth lead to low Coulombic efficiency and short cycle life. Here, we propose a kinetic regulation strategy of spatial electrostatic field layer (EFL), based on the conjugated system of tetrasulfonated cobalt phthalocyanine (CoPcS<sub>4</sub>), to enhance the preferred Zn(002)-oriented deposition. Experimental characterizations and theoretical calculations confirm that CoPcS<sub>4</sub> can preferentially adsorb on the electrode surface and form a stable solid electrolyte interface, which prevents zinc anode from the direct contact with aqueous electrolyte. The conjugated planar structure of CoPcS<sub>4</sub> further generates a delocalized EFL, which promotes Zn<sup>2+</sup> desolvation, accelerates ion transport, and ensures uniform electric field distribution. Moreover, it can effectively promote the preferred Zn(002) deposition and maintains a dense, smooth anode surface during cycling. This strategy achieves excellent cycling stability of 3500 cycles in Zn//Zn symmetry cells under extreme condition of 50 mA cm<sup>−2</sup>. In a Zn//I<sub>2</sub> battery, it demonstrates exceptional stability even at an ultra-high current density of 50 C, highlighting its great potential in massive energy storage.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104592"},"PeriodicalIF":20.2,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007223","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}
Muhammad Imran , Zhongsheng Dai , Fiaz Hussain , Wei Xia , Renjie Chen , Feng Wu , Li Li
{"title":"Chemical competing diffusion for ultra-high voltage LiCoO2","authors":"Muhammad Imran , Zhongsheng Dai , Fiaz Hussain , Wei Xia , Renjie Chen , Feng Wu , Li Li","doi":"10.1016/j.ensm.2025.104594","DOIUrl":"10.1016/j.ensm.2025.104594","url":null,"abstract":"<div><div>Elevating the operation voltage (≥4.6 V) is essential to realize higher energy density LiCoO<sub>2</sub> (LCO) based lithium-ion batteries (LIBs). However, higher cut-off voltage is inevitably accompanied by more severe material degradation from the surface to the bulk. Herein, a complexing doping strategy involving in trace multi-element (Ti, Mo, W and Mg) in LCO was proposed. Particularly, due to the limited vacancies produced by the LCO precursor during lithiation, a special competitive doping phenomenon of above elements were happened. The Mg content decreased sharply with the doping depth, while other elements are uniformly distributed throughout the particle. Therefore, a high-entropy zone was established in LCO surface, which could serve as “interface rivet” to elevate the surface stability. Furthermore, the other doping elements with high bonding energy to oxygen could act as “oxygen anchor” to enhance the bulk integrity. As a result, this robust LCO structure greatly enhanced the Li-ion diffusion dynamics, enabling the modified sample exhibited remarkable rate performance. Half-cells employing the modified LCO exhibited 80 % capacity retention after 300 cycles, and the capacity retention of full cell is 90 % after 400 cycles. This work provided a promising way for commercializing LCO material at high voltage and fast charging for LIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104594"},"PeriodicalIF":20.2,"publicationDate":"2025-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145007201","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}
Renju Dou , Xiaoyan Ren , Qin Wang , Zizheng Cheng , Zhijian Cao , Chengjiang Lin , Xiaozheng Duan , Jidong Zhang , Lehui Lu
{"title":"A low-melting solid electrolyte with grain-boundary fluidity for solid-state batteries","authors":"Renju Dou , Xiaoyan Ren , Qin Wang , Zizheng Cheng , Zhijian Cao , Chengjiang Lin , Xiaozheng Duan , Jidong Zhang , Lehui Lu","doi":"10.1016/j.ensm.2025.104591","DOIUrl":"10.1016/j.ensm.2025.104591","url":null,"abstract":"<div><div>Solid electrolytes (SEs) are urgently needed as key components of solid-state batteries (SSBs). However, the limited physical contact between the SE and electrode gives rise to interfacial issues, causing interrupted charge transport and significant resistance at the interface. In this study, we propose a co-crystalline SE, Li(GLN)<sub>2</sub>BF<sub>4</sub> (GLN, glutaronitrile), exhibiting a combination of properties not found in conventional ceramics, notably a low melting point of 60 °C and its grain-boundary fluidity. These features facilitate intimate interfacial contact without external pressure, thereby enabling liquid-like Li<sup>+</sup> conduction for high-performance SSBs. Consequently, this SE exhibits an ionic conductivity of 1.43 × 10<sup>−4</sup> S cm<sup>−1</sup> at 30 °C and a lithium-ion transference number of 0.74. Importantly, it exhibits superior structural stability during electrochemical cycling as evidenced by in-situ wide-angle X-ray scattering. Benefitting from these properties, Li||Li symmetric cells exhibit stable operation for 600 h, while Li||LiFePO<sub>4</sub> cells retain 92.3 % of its initial capacity after 400 cycles, all operating at room temperature and under zero externally applied pressure. This work paves new avenues for exploring co-crystalline substances that can concurrently achieve interfacial compatibility and chemical stability, in contrast to ceramic electrolytes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104591"},"PeriodicalIF":20.2,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145003319","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}
J.C. Barbosa, A. Fidalgo-Marijuan, J.C. Dias, R. Gonçalves, M. Salado, C.M. Costa, S. Lanceros-Méndez
{"title":"Corrigendum to “Molecular design of functional polymers for organic radical batteries” [Energy Storage Materials, Volume 60, June 2023, 102841]","authors":"J.C. Barbosa, A. Fidalgo-Marijuan, J.C. Dias, R. Gonçalves, M. Salado, C.M. Costa, S. Lanceros-Méndez","doi":"10.1016/j.ensm.2025.104587","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104587","url":null,"abstract":"Due to an editing mistake, the reference (C. Zens, C. Friebe, U.S. Schubert, M. Richter, S. Kupfer, Tailored Charge Transfer Kinetics in Precursors for Organic Radical Batteries: A Joint Synthetic-Theoretical Approach, ChemSusChem 16 (2023), e202201679) was not placed in the corresponding place. The proper attribution of the reference is as follows:","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"15 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144996083","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}
Can Huang, Tiezhong Liu, Jie Yang, Shuang Hou, Qiang Deng, Lingzhi Zhao
{"title":"Revealing anion-evolution mediated superior bidirectional kinetics in Se-doped CuS1-xSex: a highly reversible conversion-type anode for zinc-ion battery","authors":"Can Huang, Tiezhong Liu, Jie Yang, Shuang Hou, Qiang Deng, Lingzhi Zhao","doi":"10.1016/j.ensm.2025.104590","DOIUrl":"10.1016/j.ensm.2025.104590","url":null,"abstract":"<div><div>Anion doping has been regarded as a promising tactic for facilitating the redox reactions of conversion-type transition metal sulfide (TMS) anodes in rocking-chair zinc-ion battery (RCZIB). However, the evolution pathways of doped anion and the enhancement mechanisms of bidirectional reaction kinetics for anion-doped TMS anodes remain unrevealed during both the conversion and inverse-conversion processes. Herein, Se is selected as an appropriate anion to be doped into CuS (CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub> x</em> = 0.24) to design a highly reversible anode for RCZIB. Theoretical calculations and experimental results reveal that Se-doping significantly enhances the conversion kinetics of CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em> through increased electrical conductivity, optimized Zn<sup>2+</sup> adsorption behavior and reduced reaction energy barriers during discharging. Ex-situ characterizations demonstrate the dynamic evolution of Se anions, which are incorporated into the discharge product (ZnS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em>) during the conversion process. The incorporated Se anions enhance inverse-conversion kinetics during charging via synergistic effects: boosted electrical conductivity, strengthened Cu adsorption capability and facile decomposition for ZnS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em>. Subsequently, Se anions are reversibly re-doped into the regenerated charge product (CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em>) upon reverse-conversion reaction. Benefiting from superior bidirectional reaction kinetics, CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em> exhibits remarkable rate capability as well as long-term cycling stability in both half and full batteries. This exploration provides a new insight into the dynamic evolution of doped-Se and its synergistic enhancement mechanisms in bidirectional kinetics for highly reversible anion-doped TMS anodes in RCZIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104590"},"PeriodicalIF":20.2,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987611","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}
Ove Korjus , Saptarshee Mitra , Quentin Berrod , Victor Vanpeene , Markus Appel , Ludovic Broche , Sandrine Lyonnard , Claire Villevieille
{"title":"Investigating the densification of Li6PS5Cl solid electrolyte through multi-scale characterization techniques","authors":"Ove Korjus , Saptarshee Mitra , Quentin Berrod , Victor Vanpeene , Markus Appel , Ludovic Broche , Sandrine Lyonnard , Claire Villevieille","doi":"10.1016/j.ensm.2025.104589","DOIUrl":"10.1016/j.ensm.2025.104589","url":null,"abstract":"<div><div>Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) has recently gained attention as a promising solid-state electrolyte for batteries. However, the mechanisms underlying the “cold sintering” process in LPSCl remain poorly understood. In this study, we performed <em>in situ</em> densification of LPSCl while simultaneously measuring electrochemical impedance spectroscopy and micro-tomography to gain deeper insights into “cold sintering” process and to correlate the ionic conduction with the three-dimensional microstructure of the solid electrolyte. We observed that the large (secondary) particles are fracturing, while the grain boundary (GB) conductivity is improving due to better contact between grains. We have found that during the pressure application (up to 510 MPa from 76.2 MPa) at room temperature, the conductivity increases 2.45 times (up to 1.66 mS cm<sup>−1</sup>). From an in-depth electrochemical impedance and quasielastic neutron scattering (QENS) investigation, we show that the conductivity enhancement primarily arises from improved GB contact, with the bulk material remaining largely unaffected – that is, unsintered. However, the Li<sup>+</sup>conductivity is not limited by bulk but by GB resistance. The electrolyte’s conductivity without any GB contribution is estimated from QENS results with the Nernst-Einstein equation to be 5.3 mS cm<sup>−1</sup>, giving us the maximum conductivity that could be reached with shaping without modifying the bulk of the material.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104589"},"PeriodicalIF":20.2,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987613","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}
Xinyu Wang , Yiran Ying , Yuanbiao Gong , Shengmei Chen , Shuyun Wang , Weijia Wang , Juan Antonio Zapien , Longtao Ma , Min Zhu
{"title":"Piezoelectric gradient electrolytes for environmentally adaptive and stable zinc batteries","authors":"Xinyu Wang , Yiran Ying , Yuanbiao Gong , Shengmei Chen , Shuyun Wang , Weijia Wang , Juan Antonio Zapien , Longtao Ma , Min Zhu","doi":"10.1016/j.ensm.2025.104586","DOIUrl":"10.1016/j.ensm.2025.104586","url":null,"abstract":"<div><div>Solid polymer electrolyte-based zinc batteries are promising candidates for next-generation electrochemical energy storage due to their cost-effectiveness, enhanced safety and high theoretical energy density. However, their practical deployment is severely hindered by sluggish Zn<sup>2+</sup> ion mobility, poor interfacial compatibility and uneven electric field distribution. To address the persistent challenges, this work presents a novel asymmetric piezoelectric electrolyte, engineered by the strategic vertical distribution of piezoelectric barium titanate (BTO) nanofillers within a polyvinylidene fluoride (PVDF)-based polymer matrix. This design introduces a built-in gradient electric field across the electrolyte thickness, leveraging the electromechanical properties of BTO to regulate ion transport and interfacial dynamics. On the Zn anode-facing side, the BTO-rich region with a high dielectric constant and enhanced local polarization, promotes zinc salt dissociation and generates a directional electric field that promotes uniform Zn<sup>2+</sup> flux. This configuration effectively suppresses dendrite formation and mitigates localized charge accumulation. Conversely, the MnO<sub>2</sub> cathode-facing side comprises a softer, polymer-rich phase with lower BTO content, ensuring better interfacial compliance and reduced contact resistance, which is crucial for facilitating efficient ion transport without inducing excessive polarization. As a result, the asymmetric architecture achieves an impressive ionic conductivity of 1.39 mS·cm<sup>-1</sup> and a high Zn<sup>2+</sup> transference number of 0.69 at room temperature, outperforming conventional SPEs. ZnǀǀZn symmetric cells exhibit outstanding cycle stability, sustaining operation for over 1500 h, while Zn||MnO<sub>2</sub> full batteries demonstrate stable cycling over 1200 cycles. Notably, the battery performs reliably across a wide temperature range from -30 °C to 60 °C, demonstrating strong adaptability to harsh environments. This work provides a scalable and effective strategy for overcoming key limitations in Zn-based batteries by introducing a functionally asymmetric, piezoelectric electrolyte structure. This advancement paves the way for the development of safe, durable, and high-efficiency zinc-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104586"},"PeriodicalIF":20.2,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928470","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}