Energy Storage Materials最新文献

{"title":"Creating electrostatic shielding effects through dual-salt strategy to regulate coordination environment of Li⁺ and realize high-performance all-solid-state lithium metal batteries","authors":"Li Yang ,&nbsp;Lilian Wang ,&nbsp;Qingxia Hu ,&nbsp;Mou Yang ,&nbsp;Guiquan Zhao ,&nbsp;Yunchun Zha ,&nbsp;Qi An ,&nbsp;Qing Liu ,&nbsp;Haijiao Xie ,&nbsp;Yongjiang Sun ,&nbsp;Lingyan Duan ,&nbsp;Xiaoxiao Zou ,&nbsp;Genfu Zhao ,&nbsp;Hong Guo","doi":"10.1016/j.ensm.2025.104210","DOIUrl":"10.1016/j.ensm.2025.104210","url":null,"abstract":"<div><div>All-solid-state lithium metal batteries with polymer-ceramic solid electrolytes (PCSE) have garnered significant attention due to their high design flexibility. However, their low ionic conductivity and interfacial issues often impede commercialization. This study uses a Polyethylene Oxide-Li_1.5Al_0.5Ge_1.5(PO₄)₃ electrolyte model and introduces K⁺ to create a dual-salt composite polymer solid electrolyte. By establishing an electrostatic shielding effect and adjusting the Li⁺ coordination environment, the electrolyte's performance is enhanced. Theoretical and experimental results indicate that K⁺ does not participate in electrochemical reactions but instead accumulates in specific regions, promoting uniform Li⁺ deposition. Additionally, competitive coordination interactions (K⁺-TFSI⁻-Li⁺) facilitate in-situ decomposition of TFSI⁻ and PF₆⁻, forming a LiF–Li₃N–Li₂O rich SEI with low impedance. Results show that the symmetric cell achieves stable plating/stripping for 1000 h at a current density of 0.2 mA/cm² without short-circuiting, and it is compatible with both LiFePO₄ (LFP) and high-voltage LiNi_0.8Mn_0.1Co_0.1O₂ (NCM811) cathodes. This study constructs a dual-salt composite polymer solid electrolyte, revealing the interactions between molecules and ions within the electrolyte and laying a foundation for the further development of all-solid-state batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104210"},"PeriodicalIF":18.9,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713662","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":"Co-intercalation of solvated Mg2+ in amine-chain-expanded VOPO4 cathodes with fast kinetics under high-voltage condition","authors":"Lingxiao Luo, Liuyan Xia, Shuangshuang Tan, Ruimin Sun, Ze He, Xueting Huang, Zhipeng Gao, Jia Huang, Yongfeng Zhang, Xiaofang Yang, Junyao Xu, Guangsheng Huang, Jingfeng Wang, Fusheng Pan","doi":"10.1016/j.ensm.2025.104209","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104209","url":null,"abstract":"Layered cathode materials represent promising candidates for rechargeable magnesium batteries (RMBs). Among them, hydrated vanadyl phosphate (VOPO₄∙2H₂O) has gained traction due to its relatively high redox potential. However, its limited interlayer spacing leads to sluggish Mg²⁺ diffusion kinetics and low specific capacity. We address this issue by systematically studying various organic molecules as pre-insertion agents. We introduce theoretical descriptors, including molecular orbital energy levels and adsorption energy of organic molecules on VOPO₄ material, to guide the selection of applicable interlayer-expanding agents. Our di-n-butylamine (PD) pre-inserted VOPO₄ (PD-VOPO₄) cathode exhibited an expanded interlayer spacing from 0.746 nm to 1.42 nm and simultaneously delivered superior stability. It delivered an enhanced specific capacity of 118.5 mAh∙g⁻¹ with a high discharge potential of 2.74 V (<em>vs.</em> Mg²⁺/Mg) at 50 mA∙g⁻¹, and retained 81.2% of its capacity over 200 cycles. Theoretical calculations and electrochemical characterizations demonstrated that the PD-VOPO₄ cathode exhibited faster Mg²⁺ migration kinetics and a higher intercalation amount, while ex-situ characterization measurements revealed the co-intercalation mechanism of solvated Mg²⁺. This work offers new insights into the development of high-voltage, stable, and high-capacity layered cathode materials for RMBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"57 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713660","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":"Self-cleaning all-fluorinated nonflammable electrolyte for high-voltage and high-temperature Li||NCM811 batteries","authors":"Maosheng Li ,&nbsp;Lisi Xu ,&nbsp;Anqi He ,&nbsp;Haijiao Xie ,&nbsp;Kuirong Deng","doi":"10.1016/j.ensm.2025.104208","DOIUrl":"10.1016/j.ensm.2025.104208","url":null,"abstract":"<div><div>All-fluorinated electrolytes with high oxidation stability and favorable flame-retardant property are promising electrolytes for high-voltage Li metal batteries. However, conventional all-fluorinated electrolytes consisting of fluoroethylene carbonate (FEC) and LiPF₆ suffer from grievous decompositions at elevated temperature, which generates reactive species (such as HF and PF₅) and seriously damages interfacial structures of electrodes. Herein, we develop a self-cleaning all-fluorinated nonflammable electrolyte, which employes ethoxy(pentafluoro)cyclotriphosphazene (PFPN) to stabilize PF₆⁻ via intermolecular interactions, restrain the generation of HF, prevent the decomposition of FEC and enhance thermostability of the electrolyte. The strong interactions between PFPN and other components regulate the solvation structures, and bring more PF₆⁻ anions into the primary solvation shell of Li⁺ to construct solid electrolyte interphases (SEIs) and cathode-electrolyte interphases (CEIs), which leads to the fabrication of robust LiF-rich SEIs/CEIs. Benefiting from the above advantages, the designed electrolyte possesses excellent high-temperature interface compatibility with Li metal anodes and NCM811 cathodes, which endows Li||NCM811 batteries with significantly enhanced cycling stability at 60 °C and high cut-off voltage of 4.5 V. This work provides rational design of highly stable electrolytes for Li metal batteries capable of withstanding aggressive operating conditions.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104208"},"PeriodicalIF":18.9,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703034","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":"Constructing highly active sulfur atoms on MoS₂ surface via p-p orbital covalent coupling matching the liquid-solid transition in lithium-sulfur batteries","authors":"Helong Jiang ,&nbsp;Fangyi Chu ,&nbsp;Xiangcun Li ,&nbsp;Bo Zhao ,&nbsp;Gaohong He","doi":"10.1016/j.ensm.2025.104203","DOIUrl":"10.1016/j.ensm.2025.104203","url":null,"abstract":"<div><div>Herein, we propose a strategy involving Co atoms and Mo vacancies to precisely adjust the orbital orientation of sulfur atoms on MoS₂ surface, accurately modulating their interaction with lithium and sulfur sites in polysulfide species for stronger interactions with short-chain polysulfides, thereby promoting efficient liquid-solid conversion. Through a combination of theoretical modeling and experimental validation, multiple electron-deficient sulfur sites are constructed to demonstrate the <em>p</em>_z orbitals of unsaturated surface sulfur atoms couple strongly with the <em>p</em> orbitals of short-chain polysulfides, facilitating formation of selective S-S bonds via enhanced <em>p-p</em> interactions, thereby accelerating the transition kinetics from Li₂S₄ to Li₂S₂/Li₂S. This selective coupling is driven by sulfur molecular orbital occupation, charge distribution, and lattice matching. Moreover, we construct an electrocatalytic membrane composed of vertically aligned MoS₂ nanosheets and carbon nanotube nanochannels to ensure efficient contact between reactants and catalysts, enabling continuous polysulfide conversion. Consequently, the cell shows ultralow capacity decay (0.022 % per cycle over 1000 cycles at 2 C). This study emphasizes manipulation of the 3<em>p</em> orbital orientation of sulfur atoms to form selective dual-coordination, and provides valuable insights for the rational design of advanced electrocatalysts at the atomic level.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104203"},"PeriodicalIF":18.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677802","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":"Achieving superior high-temperature capacitance performance in aromatic polyetherimide with bulky fluorine substituent","authors":"Xinru Yang, Yang Feng, Peiyan Liu, Liuhao Jiang, Shuo Zhang, Yifan Wu, Shengtao Li","doi":"10.1016/j.ensm.2025.104206","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104206","url":null,"abstract":"The rapid development of electronic and electrical power equipment has increased the demand for dielectric materials with high-temperature energy storage performances. However, the mutual restrictions imposed by the glass transition temperature (<em>T</em>_g) and bandgap (<em>E</em>_g) limit the use of commercial polyetherimide (PEI) under extreme conditions. In this work, we propose a strategic modular structure design to balance a high <em>T</em>_g and large <em>E</em>_g by modulating the substituents in the biphenyl structure of modified PEI. Both experimental results and theoretical simulations indicates that owing to its electron-withdrawing nature, a bulky -CF₃ substituent not only increase the bandgap but also decreases the conjugation effect of the biphenyl structure, while having a minimal effect on <em>T</em>_g. This significantly shortens the hopping distance of the carriers, ultimately improving the high-temperature breakdown strength (<em>E</em>_b) and thus the capacitance performance of PEI. The modified PEI with the bulky -CF₃ achieves a discharge energy density (<em>U</em>_e) of 8.01 J/cm³ with an efficiency (<em>η</em>) of 91.9% at 150 °C and an <em>U</em>_e of 5.3 J/cm³ with an <em>η</em> of 90.4% at 200 °C, which exceeds the performance of most of current high-temperature dielectric polymers. The results of this study provide technical support for the developing of high-performance, flexible dielectric capacitors.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"57 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695827","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":"Achieving excellent energy storage properties in lead-free ceramics via competing FE/AFE phase coexistence","authors":"Zhongqian Lv ,&nbsp;Bing Han ,&nbsp;Zhen Liu ,&nbsp;Shaobo Guo ,&nbsp;Kai Dai ,&nbsp;Fei Cao ,&nbsp;Zhigao Hu ,&nbsp;Genshui Wang","doi":"10.1016/j.ensm.2025.104205","DOIUrl":"10.1016/j.ensm.2025.104205","url":null,"abstract":"<div><div>Dielectric capacitors are widely utilized in large-scale power systems, including applications in medical and military fields. However, their relatively low energy storage density limits further advancements in miniaturization and integration. Therefore, improving the energy storage density of dielectric capacitors is of paramount importance. In this work, novel lead-free Na_0.70Sr_0.15Nb_0.75Ta_0.25O₃ (NSNT) ceramics were designed, which exhibit a unique combination of relaxor ferroelectric (FE) N phase and stabilized antiferroelectric (AFE) P phase, as confirmed through local structural analysis. The competing FE/AFE phase coexistence is attributed to the discrepancy in ion valence and radius. As a result, the NSNT ceramics demonstrate exceptional energy storage performance, featuring a recoverable energy density (<em>W</em>_rec) of 10.45 J/cm³ and an energy efficiency (<em>η</em>) of 83.0 % at 850 kV/cm, along with excellent stability. These outstanding energy storage properties not only confirm the promising application prospects of NN-based ceramics with competing FE/AFE phase coexistence, but also provide an innovative approach for advancing high-performance ceramic capacitors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104205"},"PeriodicalIF":18.9,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695826","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":"Three birds with one stone: Reducing gases manipulate surface reconstruction of Li-rich Mn-based oxide cathodes for high-energy lithium-ion batteries","authors":"Kejie Jin ,&nbsp;Liaoliao Li ,&nbsp;Hao Tian ,&nbsp;Mengxing Su ,&nbsp;Yang Yang ,&nbsp;Zhijun Wu ,&nbsp;Shengnan He ,&nbsp;Yanxia Liu ,&nbsp;Chao Zheng ,&nbsp;Jiantuo Gan ,&nbsp;Wubin Du ,&nbsp;Liaona She ,&nbsp;Yaxiong Yang ,&nbsp;Mingchang Zhang ,&nbsp;Hongge Pan","doi":"10.1016/j.ensm.2025.104202","DOIUrl":"10.1016/j.ensm.2025.104202","url":null,"abstract":"<div><div>Energy storage through additional anionic redox can deliver ultrahigh specific capacities of Lithium-rich manganese-based oxides cathode materials (LRMO). The commercial application of LRMO is hampered by several drawbacks, including structure degradation, continuous capacity and voltage decay, sluggish kinetics and severe irreversible oxygen release, stemming from generation of O₂ⁿ⁻ (0 ≤ <em>n</em> &lt; 2) species during deep oxidation. Notably, relying solely on a single modification strategy only partially address the problems of LRMO materials. Herein, one-step phosphatizing-assisted interface engineering strategy was successfully implemented, simultaneously fabricating oxygen vacancies, spinel-like structure and an ionic conductor Li₃PO₄ capping layer on the surface. Among them, the formation of oxygen vacancies is accompanied by the production of a spinel phase buffer layer, which inhibits the generation of O–O dimers and oxygen loss, contributing to the stability and reversibility of anionic redox reactions. The lithium ions conductive protective layer of Li₃PO₄ accelerates Li⁺ diffusion rate while suppressing harmful interfacial side-reactions between the electrode and electrolyte. More importantly, the incorporation of P into the subsurface lattice regulates the local electron configuration and activates oxygen redox. As a result, the modification LRMO demonstrates an impressive reversible capacity of 312.9 mAh <em>g</em>⁻¹, with excellent capacity retention of 91.87 % at 1 C and 82.43 % at 2 C after 500 cycles, respectively. The mult-ianionic redox mechanism provides an effective and straightforward method to stabilizing LRMO for next-generation high-energy lithium-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104202"},"PeriodicalIF":18.9,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675287","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":"Epitaxial growth of the (101) plane: High stability and dendrite-free Zn anode achieved by “one stone, two birds” strategy","authors":"Youyi Li ,&nbsp;Yuhan Liu ,&nbsp;Kun-Peng Wang ,&nbsp;Zhenyu Xiao ,&nbsp;Qi Zhang ,&nbsp;Lei Wang ,&nbsp;Volodymyr Turkevych","doi":"10.1016/j.ensm.2025.104204","DOIUrl":"10.1016/j.ensm.2025.104204","url":null,"abstract":"<div><div>The performance of zinc ion batteries (ZIBs) is significantly constrained by dendrite growth and side reactions on the Zn anode. While epitaxial growth is an efficient strategy to stabilize the Zn anode by directing crystal alignment, the direct contact between the exposed crystal and electrolyte results in severe parasitic reactions. Here, we present a selective etching strategy on Zn anodes (denoted as ACE-Zn) that preferentially exposes the (101) plane, which features strong epitaxial growth characteristics to facilitate stably dense stacking of Zn atoms. Notably, the (101) plane also promotes the formation of a ZnS solid electrolyte interphase (SEI). This ZnS SEI exhibits high hydrophilicity and an ultrathin structure, contributing to exceptional ion transfer rate and isolating the Zn anode from water-related side reactions. As a result, ACE-Zn symmetric cells achieve an impressive cycle life of 4920 h at 0.5 mAh cm⁻² and 0.5 mA cm⁻², along with a high average Coulombic efficiency (CE) of 99.93 % over 3500 cycles. Furthermore, V-EG//ACE-Zn button-cells demonstrate prolonged cycle life of 7600 cycles at 10 A g⁻¹. We believe this “one stone, two birds” strategy will provide new insights into texturing preferential planes and constructing SEI to stabilize Zn anodes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104204"},"PeriodicalIF":18.9,"publicationDate":"2025-03-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677803","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":"Upcycling of spent LiCoO2/Graphite/Cu mixtures: Cu-doping with contrary gradient distribution towards high-rate and prolonged-cyclability","authors":"Hai Lei ,&nbsp;Xinwei Cui ,&nbsp;Jiexiang Li ,&nbsp;Zihao Zeng ,&nbsp;Chao Zhu ,&nbsp;Xiaobo Ji ,&nbsp;Wei Sun ,&nbsp;Yue Yang ,&nbsp;Peng Ge","doi":"10.1016/j.ensm.2025.104201","DOIUrl":"10.1016/j.ensm.2025.104201","url":null,"abstract":"<div><div>Attracted by remarkable environmental/economic advantages, the direct regeneration of spent LiCoO₂ (LCO) has been regarded as potential recycling method. However, limited by small-size and various designing-models, spent batteries are always industrially dismantled to obtain complex mixture, containing LCO, graphite, Cu-impurities, etc. Thus, exploring the synergetic effect of graphite removing and Cu-doping behaviors/threshold is crucial for the practical commercial production about spent mixture. Herein, spent mixtures are utilized to regenerate high-voltage LCO. Assisted by graphite self-heating and Li-vacancies, the doping-temperature and diffusion energy-barrier are lowering, facilitating Cu-atoms doping into bulk-phase. After optimizing Cu-content (0.7 wt.%), bulk-oriented doping at Li/Co sites is achieved with contrary gradient Cu-atoms distribution. Unique doping behaviors induce the evolution of morphology/lattice stability and the expanding of interlayer spacing. The as-optimized sample delivers a high capacity of 177.59 mAh g^-1 at 0.2 C. Even at 5.0 C after 500 cycles, its capacity could reach up to 154.8 mAh g^-1 with ∼82.4% retention. Supporting by electronic structure analysis, unique doping behaviors served as important roles in enhancing electronic conductivity and lowering O 2p band center. Given this, the work is expected to offer significant guidance of direct commercial regeneration, and shed light on the clear Cu-doping behaviors with threshold-value.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104201"},"PeriodicalIF":18.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675241","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":"Enabling efficient guiding of Li diffusion/plating toward high-performance lithium metal batteries by utilizing a gradient Janus interlayer","authors":"Tzu-Chi Chuang ,&nbsp;Rupan Bera ,&nbsp;Yi-Ting Wu ,&nbsp;Shih-Yu Chen ,&nbsp;I-Yu Tsao ,&nbsp;Jeng-Kuei Chang ,&nbsp;Ching-Yuan Su","doi":"10.1016/j.ensm.2025.104196","DOIUrl":"10.1016/j.ensm.2025.104196","url":null,"abstract":"<div><div>Lithium metal batteries (LMBs) face significant challenges, including dendrite growth and degradation during cycling. Two effective strategies to address these issues involve utilizing a nano-structured current collector as a lithium host and forming an ideal solid-electrolyte interphase (SEI) as an artificial anode modifier. However, synthesizing an anode modifier that offers high cycling stability and efficient lithium diffusion/storage via a well-controlled deposition method remains challenging. This study presents a binder-free and novel gradient Janus interlayer(GJL) as anode modifier comprising gradient layered composite of fluorinated graphene (FECG) and intrinsic graphene (ECG), deposited through electrophoretic deposition (EPD). The gradient Janus structure provides separate ionic and electronic transport pathways. The top FECG layer with LiF-rich species enhances both electrolyte wettability and lithium ion transport for uniform Li plating, while the underlying ECG layer facilitates efficient electron transfer. Also, a thin CuF₂-riched functional layer is designed to connecting the GJL to the copper substrate, ensures strong adhesion to the copper substrate without using any binder, enabling stable lithium deposition and improved structural integrity. The GJL as anode modifier demonstrates outstanding electrochemical performance, showing a low nucleation overpotential of 42.17 mV and stable polarization over 600 h. After 325 cycles, the Coulombic efficiency reached 97.2 %, indicating excellent stability. In full-cell testing, the specific capacity exceeded 120 mAh/g after 150 cycles, with 72 % capacity retention after 160 cycles. Overall, this innovative composite multilayer ASEI offers a promising solution to overcome the challenges of anode-free lithium metal batteries (AFLB), paving the way for safer and higher-energy-density battery technologies.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"77 ","pages":"Article 104196"},"PeriodicalIF":18.9,"publicationDate":"2025-03-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675284","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}