{"title":"Advanced Aqueous Electrolytes for Aluminum-Ion Batteries: Challenges and Opportunities","authors":"Michael Ruby Raj, Karim Zaghib, Gibaek Lee","doi":"10.1016/j.ensm.2025.104211","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104211","url":null,"abstract":"With the rapid growth in global energy demand, renewable energy has emerged as a promising solution. However, the intermittency and irregularity of renewable energy sources pose significant challenges for next-generation, large-scale energy-storage systems. Aqueous rechargeable batteries with multivalent cations have attracted attention as candidates for grid-scale energy storage because of their high energy densities enabled by their multi-electron redox reactions, low cost, operational safety, and environmentally benign nature. Among such batteries, rechargeable aqueous aluminum-ion batteries (AAIBs) show promise, offering high gravimetric and volumetric capacities (2981 mAh g<sup>−1</sup> and 8056 mAh cm<sup>−3</sup>, respectively) through a three-electron redox process. However, the practical application of AAIBs remains constrained by several critical challenges, including parasitic chemical reactions between the Al anode surface and the electrolyte, sluggish reaction kinetics of Al³⁺ ions, low reversibility and poor utilization of the Al anode, as well as instability in the crystal structure due to the high charge density of Al³⁺ ions. These issues contribute to poor cycling life and inferior rate performance in AAIBs. To address these limitations, research has focused on advanced strategies, such as the design of aqueous electrolytes to extend the output voltage window and improve the electrochemical stability window (ESW), pre-addition or pre-intercalation of multivalent ion, and structural optimization of active materials to enhance kinetics with electrolytes. This review highlights the latest progress in the field of advanced aqueous electrolyte design, covering approaches such as metal alloy strategies, eutectic engineering, amorphization, electrolyte additive modulation, hybrid electrolyte optimization, and surface modification technologies. These strategies are employed to control the overpotential and reduce the polarization–voltage gap to achieve high Al plating/stripping reversibility in AAIBs. Furthermore, the challenges, limitations, and promising pathways for enhancing performance in advanced aqueous environments are discussed. Finally, critical challenges and prospects for advanced aqueous electrolyte design and anodic surface modification strategies in AAIBs are proposed to inspire future research directions.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"870 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723846","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}
Younghoon Jo, Hongjun Chang, Chaeyeon Ha, Hyeongjun Choi, Taesun Song, Yeonghoon Kim, Janghyuk Moon, Young-Jun Kim
{"title":"Prolonged Cycle Life of Composite Cathodes via Ionically Permeable Li3PO4 Surface Engineering on Conductive Agents to Suppress Degradation of Sulfide Solid Electrolytes","authors":"Younghoon Jo, Hongjun Chang, Chaeyeon Ha, Hyeongjun Choi, Taesun Song, Yeonghoon Kim, Janghyuk Moon, Young-Jun Kim","doi":"10.1016/j.ensm.2025.104193","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104193","url":null,"abstract":"Sulfide-based all-solid-state batteries (ASSBs) are promising candidates for next-generation energy storage systems owing to their notable ionic conductivity and stability against explosions. However, the low chemical stability of sulfide-based solid electrolytes (SSE) causes problems at their interfaces with other electrode components. Among them, addressing the side reactions between conductive agents and SSEs is crucial for commercialization. Herein, a conductive agent surface-modified with Li<sub>3</sub>PO<sub>4</sub> is employed to enhance the interfacial stability of SSEs. Density functional theory-based analysis reveals that Li<sub>3</sub>PO<sub>4</sub>, characterized by strong inter-element bonding, exhibits high ionic conductivity and stability at the interface with SSEs. Electrochemical measurements confirm that Li<sub>3</sub>PO<sub>4</sub>-coated conductive agents suppress the interfacial decomposition of SSEs, thereby securing the targeted ionic conductivity in the composite cathode. Consequently, ASSBs adopting surface-engineered conductive agents demonstrate remarkable rate capability (153.6 mAh g<sup>−1</sup> at 2 C) and cycle performance (88.8 % retention over 1000 cycles) with a high areal capacity (4 mAh cm<sup>−2</sup>). This study provides a novel concept for conductive agents that enhance charge transport characteristics and mitigate SSE degradation, paving the way for the development of long cycle life ASSBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"61 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143703032","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}
Li Yang , Lilian Wang , Qingxia Hu , Mou Yang , Guiquan Zhao , Yunchun Zha , Qi An , Qing Liu , Haijiao Xie , Yongjiang Sun , Lingyan Duan , Xiaoxiao Zou , Genfu Zhao , Hong Guo
{"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 , Lilian Wang , Qingxia Hu , Mou Yang , Guiquan Zhao , Yunchun Zha , Qi An , Qing Liu , Haijiao Xie , Yongjiang Sun , Lingyan Duan , Xiaoxiao Zou , Genfu Zhao , 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<sub>1.5</sub>Al<sub>0.5</sub>Ge<sub>1.5</sub>(PO<sub>4</sub>)<sub>3</sub> electrolyte model and introduces K⁺ to create a dual-salt composite polymer solid electrolyte. By establishing an electrostatic shielding effect and adjusting the Li<sup>+</sup> 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 PF<sub>6</sub>⁻, 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/cm<sup>2</sup> without short-circuiting, and it is compatible with both LiFePO<sub>4</sub> (LFP) and high-voltage LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> (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 (VOPO<sub>4</sub>∙2H<sub>2</sub>O) has gained traction due to its relatively high redox potential. However, its limited interlayer spacing leads to sluggish Mg<sup>2+</sup> 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 VOPO<sub>4</sub> material, to guide the selection of applicable interlayer-expanding agents. Our di-n-butylamine (PD) pre-inserted VOPO<sub>4</sub> (PD-VOPO<sub>4</sub>) 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<sup>−1</sup> with a high discharge potential of 2.74 V (<em>vs.</em> Mg<sup>2+</sup>/Mg) at 50 mA∙g<sup>−1</sup>, and retained 81.2% of its capacity over 200 cycles. Theoretical calculations and electrochemical characterizations demonstrated that the PD-VOPO<sub>4</sub> cathode exhibited faster Mg<sup>2+</sup> migration kinetics and a higher intercalation amount, while ex-situ characterization measurements revealed the co-intercalation mechanism of solvated Mg<sup>2+</sup>. 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}
Maosheng Li , Lisi Xu , Anqi He , Haijiao Xie , Kuirong Deng
{"title":"Self-cleaning all-fluorinated nonflammable electrolyte for high-voltage and high-temperature Li||NCM811 batteries","authors":"Maosheng Li , Lisi Xu , Anqi He , Haijiao Xie , 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 LiPF<sub>6</sub> suffer from grievous decompositions at elevated temperature, which generates reactive species (such as HF and PF<sub>5</sub>) 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 PF<sub>6</sub><sup>−</sup> 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 PF<sub>6</sub><sup>−</sup> anions into the primary solvation shell of Li<sup>+</sup> 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}
Jesús Chacón-Borrero, Xuede Qi, Xuesong Zhang, Armando Berlanga-Vázquez, Xingqi Chang, Guillem Montaña-Mora, Karol V. Mejía-Centeno, Helena Rabelo Freitas, María Chiara Spadaro, Jordi Arbiol, Jordi Llorca, Pablo Guardia, Xueqiang Qi, Chao Yue Zhang, Andreu Cabot
{"title":"Enhanced Lithium Polysulfide Adsorption and Reaction with Cobalt-Doped Spinel Additives for Robust Lithium-Sulfur Batteries","authors":"Jesús Chacón-Borrero, Xuede Qi, Xuesong Zhang, Armando Berlanga-Vázquez, Xingqi Chang, Guillem Montaña-Mora, Karol V. Mejía-Centeno, Helena Rabelo Freitas, María Chiara Spadaro, Jordi Arbiol, Jordi Llorca, Pablo Guardia, Xueqiang Qi, Chao Yue Zhang, Andreu Cabot","doi":"10.1016/j.ensm.2025.104207","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104207","url":null,"abstract":"Sulfur-based cathodes offer a promising high-energy-density alternative to conventional lithium-ion batteries. However, their commercial viability is hindered by limited stability due to the gradual loss of active sulfur during cycling. This study addresses this challenge by introducing a cobalt-doped spinel oxide as a catalytic additive, designed to enhance the performance and stability of sulfur cathodes with minimized cobalt usage. Small amounts of cobalt doping improve the adsorption of sulfur species through stronger electronic interactions with antibonding orbitals and accelerate charge transfer, thereby promoting more efficient sulfur redox reactions. Cobalt also lowers the energy barrier for Li<sub>2</sub>S formation, a critical step in the cycling process. Specifically, Co-doped MnFe<sub>2</sub>O<sub>4</sub> with 2.4 wt% Co demonstrates a remarkable initial capacity of 1302 mAh/g at 0.1C, excellent rate capability with 700 mAh/g at 4C, and stable cycling performance with an average capacity decay of just 0.03 % per cycle at 0.5C over 200 cycles. Overall, this work underscores the potential of cobalt-doped spinel structures as catalytic additives to mitigate the limitations of sulfur cathodes, paving the way for more stable and high-performance lithium-sulfur batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"183 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695825","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}
Helong Jiang , Fangyi Chu , Xiangcun Li , Bo Zhao , Gaohong He
{"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 , Fangyi Chu , Xiangcun Li , Bo Zhao , 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 MoS<sub>2</sub> 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><sub>z</sub> 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 Li<sub>2</sub>S<sub>4</sub> to Li<sub>2</sub>S<sub>2</sub>/Li<sub>2</sub>S. 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}
Xinru Yang, Yang Feng, Peiyan Liu, Liuhao Jiang, Shuo Zhang, Yifan Wu, Shengtao Li
{"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><sub>g</sub>) and bandgap (<em>E</em><sub>g</sub>) 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><sub>g</sub> and large <em>E</em><sub>g</sub> 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 -CF<sub>3</sub> 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><sub>g</sub>. This significantly shortens the hopping distance of the carriers, ultimately improving the high-temperature breakdown strength (<em>E</em><sub>b</sub>) and thus the capacitance performance of PEI. The modified PEI with the bulky -CF<sub>3</sub> achieves a discharge energy density (<em>U</em><sub>e</sub>) of 8.01 J/cm<sup>3</sup> with an efficiency (<em>η</em>) of 91.9% at 150 °C and an <em>U</em><sub>e</sub> of 5.3 J/cm<sup>3</sup> 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}
Zhongqian Lv , Bing Han , Zhen Liu , Shaobo Guo , Kai Dai , Fei Cao , Zhigao Hu , Genshui Wang
{"title":"Achieving excellent energy storage properties in lead-free ceramics via competing FE/AFE phase coexistence","authors":"Zhongqian Lv , Bing Han , Zhen Liu , Shaobo Guo , Kai Dai , Fei Cao , Zhigao Hu , 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<sub>0.70</sub>Sr<sub>0.15</sub>Nb<sub>0.75</sub>Ta<sub>0.25</sub>O<sub>3</sub> (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><sub>rec</sub>) 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}
Fan Wang, Ming Zhang, Zixuan Fang, Haiping Zhou, Jintian Wu, Ziqiang Xu, Naixun Zhou, Yihang Zhang, Zhi Zeng, Mengqiang Wu
{"title":"Mechano-Electrical Buffer Layer at Grain Boundary Induced Solid State Electrolyte with Ultra-High Mechanical Strength and Electrical Insulation for Stable Lithium Metal Batteries","authors":"Fan Wang, Ming Zhang, Zixuan Fang, Haiping Zhou, Jintian Wu, Ziqiang Xu, Naixun Zhou, Yihang Zhang, Zhi Zeng, Mengqiang Wu","doi":"10.1016/j.ensm.2025.104198","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104198","url":null,"abstract":"The high sintering temperature, low mechanical properties and instability of lithium metal have consistently hindered the practicality of Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> (LATP) solid-state electrolytes (SSEs). Herein, a meticulously designed mechano-electrical buffer layer is constructed at grain boundaries (GBs) of LATP by introducing Li<sub>2</sub>B<sub>4</sub>O<sub>7</sub> (LBO) glass-ceramic. LBO can generate a liquid phase with high Young's modulus and low electronic conductivity at GBs to simultaneously reduce sintering temperature, and enhance the mechanical strength and electrical insulation of LATP. The construction of a mechano-electrical buffer layer at GBs leads to three significant achievements: the reduced sintering temperature from 950 to 750 °C, the enhanced mechanical strength from 9.9 to 117.5 MPa, and the decreased electronic conductivity from 1.2 × 10<sup>-9</sup> to 1.5 × 10<sup>-10</sup> S cm<sup>-1</sup>. When coupled with a solid polymer electrolyte, it effectively protects LATP from internal microcrack propagation and electron attack. Remarkably, the critical current density (CCD) of the modified LATP can reach 2 mA cm<sup>-2</sup>. Moreover, the lithium metal battery with LiFePO<sub>4</sub> demonstrates outstanding stability of more than 1000 cycles with a capacity retention of 93.3% at 0.2C. This work provides new insights into improving the performance of SSEs by enhancing both mechanical strength and electrical insulation.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"70 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143677801","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}