Qinghua Gui , Jinzhong Li , Bowen Jin , Peng Liu , Kun Yu , Jiarui Zhang , Lei Mao
{"title":"Cross-scale investigation of overcharge-induced thermal runaway propagation mechanism in sodium-ion batteries under multi-module configuration","authors":"Qinghua Gui , Jinzhong Li , Bowen Jin , Peng Liu , Kun Yu , Jiarui Zhang , Lei Mao","doi":"10.1016/j.jechem.2025.08.042","DOIUrl":"10.1016/j.jechem.2025.08.042","url":null,"abstract":"<div><div>In electrochemical energy storage systems, the sodium-ion battery is typically integrated in the form of a “cell-module-cluster”, but its cross-scale thermal runaway triggering risk and the propagation mechanism remain unclear. This study reveals the cross-scale thermal runaway triggering and propagation behavior of sodium-ion batteries of “cell-module-cluster” under overcharge conditions, and investigates the effects of key factors, including module spacing, triggering cell location, and heat dissipation condition, on the thermal runaway propagation behavior. Results demonstrate that the thermal runaway propagation in a module containing the overcharged cell follows a sequential triggering mode, while thermal runaway in the downstream module exhibits a simultaneous triggering mode with greater severity. Furthermore, increasing the module spacing or enhancing the heat dissipation capacity can effectively reduce the heat accumulation and prevent the trigger of thermal runaway. On the above basis, the multi-dimensional evaluation strategy is proposed to quantitatively assess the hazard of sodium-ion battery cluster thermal runaway. The findings serve as a foundation for the safe design of sodium-ion batteries in energy storage systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 13-28"},"PeriodicalIF":14.9,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145048168","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhiyuan Liu, Xin Wang, Xuan Xie, Yue Li, Hui Peng, Guofu Ma, Ziqiang Lei
{"title":"Dual-regulation of pore confinement and mouth size for enhanced sodium storage in hard carbon","authors":"Zhiyuan Liu, Xin Wang, Xuan Xie, Yue Li, Hui Peng, Guofu Ma, Ziqiang Lei","doi":"10.1016/j.jechem.2025.08.038","DOIUrl":"10.1016/j.jechem.2025.08.038","url":null,"abstract":"<div><div>Hard carbon (HC) remains a leading anode candidate for sodium-ion storage, yet its application is hindered by low initial Coulombic efficiency (ICE) and limited plateau capacity due to uncontrolled defect density and open porosity. Here, we propose a scalable dual-regulation strategy that simultaneously tunes pore mouth size and defect chemistry to enhance sodium storage performance. Using phenol-formaldehyde resin as the carbon precursor and phosphorus pentoxide (P<sub>2</sub>O<sub>5</sub>) as a bifunctional sacrificial template and dopant source, we synthesize phosphorus-functionalized hard carbon (PF-PHC) featuring a high density of closed pores with well-confined sub-nanometer pore entrances. The in-situ sublimation of P<sub>2</sub>O<sub>5</sub> during pyrolysis promotes the formation of closed-pore architectures, while residual phosphorus atoms effectively passivate vacancy-type defects, thereby reducing irreversible Na<sup>+</sup> adsorption and mitigating excessive solid electrolyte interphase (SEI) formation. As a result, PF-PHC achieves an ICE of 89.3% and a plateau capacity of 289 mAh g<sup>−1</sup>. In-situ characterizations reveal that regulating pore mouth dimensions decouples Na<sup>+</sup> and solvent access, enabling highly selective ion transport and stable interfacial chemistry. Sodium-ion hybrid capacitors (SIHCs) assembled based on PF-PHC deliver exceptional rate performance and outstanding long-term cycling stability, retaining 98.2% after 10,000 cycles at 2 A g<sup>−1</sup>. This study establishes pore mouth engineering as a robust and scalable design principle for advancing next-generation HC-based sodium storage materials.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 1-12"},"PeriodicalIF":14.9,"publicationDate":"2025-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145048167","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Entropy-stabilized oxides with d10 and s0p0 cations as heterostructured photocatalysts with high work function: Experiments and first-principles calculations","authors":"Jacqueline Hidalgo-Jiménez , Taner Akbay , Motonori Watanabe , Katsuhiko Saito , Qixin Guo , Tatsumi Ishihara , Kaveh Edalati","doi":"10.1016/j.jechem.2025.08.033","DOIUrl":"10.1016/j.jechem.2025.08.033","url":null,"abstract":"<div><div>Elements from the right side of the periodic table, including cations with <em>d</em><sup>10</sup> and <em>s</em><sup>0</sup><em>p</em><sup>0</sup> configurations, have been shown to improve photocatalytic activity in various photocatalysts either as dopants or principal elements. This study introduces the first medium- and high-entropy oxide photocatalysts accommodating only <em>d</em><sup>10</sup> and <em>s</em><sup>0</sup><em>p</em><sup>0</sup> cations. The designated oxides, AlZnGaO<sub>4</sub> and AlZnGaSnBiO<sub>7.5</sub> (dual-phase heterostructure of AlZnGaO<sub>4</sub> and 1/2Sn<sub>2</sub>Bi<sub>2</sub>O<sub>7</sub>), demonstrate good optical properties and promising photocatalytic activity for water conversion to hydrogen and CO<sub>2</sub> conversion to methane compared to entropy-stabilized cations containing only <em>d</em><sup>0</sup> or <em>d</em><sup>0</sup>+<em>d</em><sup>10</sup> configurations. The good activity of these oxides was ascribed to their high work function, which was supported by experimental analysis and first-principles calculations. Moreover, AlZnGaSnBiO<sub>7.5</sub> exhibited enhanced activity compared to AlZnGaO<sub>4</sub> due to the creation of type II heterojunctions and resultant higher charge carrier separation and lifetime. This study introduces the significance of <em>d</em><sup>10</sup>+<em>s</em><sup>0</sup><em>p</em><sup>0</sup> cationic configuration, high work function, and inherent heterojunctions on the design of advanced high-entropy photocatalysts with high photocatalytic activity.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 954-968"},"PeriodicalIF":14.9,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026915","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yunfei Huan , Yanzheng He , Zhenkang Wang , Haoqing Ji , Sisi Liu , Lifang Zhang , Xiaowei Shen , Jie Liu , Mengfan Wang , Tao Qian , Chenglin Yan
{"title":"Weakened ionization electrolyte with n-hexane additive enabling high activity of lithium-mediated nitrogen fixation","authors":"Yunfei Huan , Yanzheng He , Zhenkang Wang , Haoqing Ji , Sisi Liu , Lifang Zhang , Xiaowei Shen , Jie Liu , Mengfan Wang , Tao Qian , Chenglin Yan","doi":"10.1016/j.jechem.2025.08.037","DOIUrl":"10.1016/j.jechem.2025.08.037","url":null,"abstract":"<div><div>Lithium-mediated nitrogen reduction reaction (LMNRR) is a promising route for sustainable ammonia synthesis, but the generation of excessive solid electrolyte interphase (SEI) severely limits its efficiency. Here, we tackle this challenge by introducing <em>n</em>-hexane as an electrolyte additive to weaken LiClO<sub>4</sub> ionization, achieving minimized dissociation via squeezed solvation shells with compact ion pairs. Molecular dynamics simulations and experimental characterizations reveal that <em>n</em>-hexane enriches anion coordination around Li<sup>+</sup>, endowing the electrolyte with robust anti-reduction capability. This suppresses SEI overgrowth, reduces interfacial resistance, and accelerates N<sub>2</sub> diffusion. Consequently, a thinner, inorganic-rich SEI is formed, enabling high nitrogen flux and rapid active Li<sub>3</sub>N generation kinetics. Consequently, the proof-of-concept system achieves unprecedentedly high Faradaic efficiency of 53.8 %±8.2 % at 10 mA cm<sup>−2</sup> and NH<sub>3</sub> yield rate of 88.57±9.5 nmol s<sup>−1</sup> cm<sup>−2</sup> under ambient conditions, making a giant step further toward industrializing the electrochemical ammonia production.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 39-46"},"PeriodicalIF":14.9,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145048169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Xinxin Li , Long Zhou , Dazheng Chen , Weidong Zhu , He Xi , Hang Dong , Wenming Chai , Hui Wang , Chunxiang Zhu , Jincheng Zhang , Yue Hao , Chunfu Zhang
{"title":"Additive engineering for colloid stabilization and crystallization control in slot-die coated large-area solar modules","authors":"Xinxin Li , Long Zhou , Dazheng Chen , Weidong Zhu , He Xi , Hang Dong , Wenming Chai , Hui Wang , Chunxiang Zhu , Jincheng Zhang , Yue Hao , Chunfu Zhang","doi":"10.1016/j.jechem.2025.08.028","DOIUrl":"10.1016/j.jechem.2025.08.028","url":null,"abstract":"<div><div>Scalable fabrication of homogeneous perovskite films remains crucial for bridging the efficiency gap between lab-scale solar cells and commercial solar modules. To tackle this issue, we introduce <em>N</em>-Cyano-4-methyl-<em>N</em>-phenylbenzenesulfonamide (CMPS) additives into perovskite precursors, enabling slot-die coating of large-area modules under ambient conditions. CMPS suppresses colloidal aggregation and delays crystallization, yielding high-quality uniform films. Small-area devices (0.07 cm<sup>2</sup> aperture area) incorporating CMPS exhibited a significant efficiency increase from 22.07 % to 24.58 %. Corresponding encapsulated devices maintained 85 % of their initial power conversion efficiency (PCE, average 23.56 %) after 1500 h of continuous maximum power point (MPP) tracking under one-sun illumination at 50–55 °C. Furthermore, we demonstrate impressive efficiency of perovskite solar modules, achieving 20.57 % (52 cm<sup>2</sup> aperture area) for 10 cm × 10 cm mini-modules and 17.02 % (260 cm<sup>2</sup> aperture area) for 21 cm × 21 cm sub-modules, representing the state-of-the-art performance for solution-processed devices at these scales.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 935-943"},"PeriodicalIF":14.9,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026913","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yang Wang , Fangxiong Deng , Shaowei Ouyang , Can Jiang , Huangxu Li
{"title":"Current progress of Na4Fe3(PO4)2(P2O7): Key issues, modifications, and perspectives","authors":"Yang Wang , Fangxiong Deng , Shaowei Ouyang , Can Jiang , Huangxu Li","doi":"10.1016/j.jechem.2025.08.027","DOIUrl":"10.1016/j.jechem.2025.08.027","url":null,"abstract":"<div><div>The sodium-ion battery (SIB) cathode material, Na<sub>4</sub>Fe<sub>3</sub>(PO<sub>4</sub>)<sub>2</sub>(P<sub>2</sub>O<sub>7</sub>) (NFPP), has become a focal material in both academia and industry due to its low cost, long lifespan, and high safety. In the recent three years, substantial efforts have been devoted to promoting the practical applications of NFPP by optimizing its electrochemical performance and disclosing the reaction mechanisms. Various modification strategies and their effect mechanisms have been explored, and the performance evaluation of NFPP has progressively advanced from laboratory-scale coin cells to practical pouch cell configurations. Nevertheless, there remains a lack of systematic reviews comprehensively assessing the developmental status and application readiness of NFPP. This review critically examines NFPP’s fundamental structural characteristics and proposes four key development issues. Then, the latest research advances are introduced with explicit differentiation of design strategies and their mechanistic impacts. Notably, we provide a dedicated discussion on NFPP’s current pouch cell performance metrics, while highlighting two critical yet underexplored research directions (enhancing air stability and improving tap density) for commercial viability.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 914-934"},"PeriodicalIF":14.9,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Weijie Zheng , Jingzhou Ling , Shiru Li , Tian Wen , Zhibiao Cui , Dong Shu , Xiuhua Li , Honghong Cheng , Fan Zhang , Tao Meng
{"title":"Electrochemical phase reconstruction of biomimetic MnO2 structure to enhance sodium-ion storage kinetics in aqueous systems","authors":"Weijie Zheng , Jingzhou Ling , Shiru Li , Tian Wen , Zhibiao Cui , Dong Shu , Xiuhua Li , Honghong Cheng , Fan Zhang , Tao Meng","doi":"10.1016/j.jechem.2025.08.026","DOIUrl":"10.1016/j.jechem.2025.08.026","url":null,"abstract":"<div><div>The application of conventional manganese dioxide (MnO<sub>2</sub>) materials in sodium-ion supercapacitors (Na-SCs) is considerably limited by their low conductivity and structural instability. Biomimetic morphology engineering can optimize the electrochemical performance of MnO<sub>2</sub>. Here, based on the metal-organic frameworks (MOFs)-derived method and electrochemical reconstruction, a coral-like MnO<sub>2</sub> structure integrated with a functional nitrogen-doped carbon (NC) coating is designed for Na-SC application. The bioinspired coral-like structure captures numerous electrolyte ions and increases the Na<sup>+</sup> concentration on the electrode surface, which is beneficial for optimizing the Na<sup>+</sup> transport pathway and accelerating the electrode reaction kinetics. Moreover, the coral-like crosslinked structure effectively enhances the mechanical properties, enabling the maintenance of the structure of MnO<sub>2</sub>-based electrodes during long-term operation. Furthermore, in/ex-situ characterizations are performed to elucidate the mechanism of lattice transformation during electrochemical phase reconstruction. Additionally, the theoretical calculation and simulation results reveal the ion/electron dynamics in the fabricated electrode. The prepared electrode demonstrates excellent capacitance storage ability (340.7 F g<sup>−1</sup> at 0.5 A g<sup>−1</sup>) and cycling stability (85.1 % capacitance retention after 10,000 cycles). The assembled hybrid device exhibits exceptional life-span (82.0 % capacitance retention after 10,000 cycles) and exceptional energy density (36.5 Wh kg<sup>−1</sup>). This study provides a reliable biomimetic morphology design strategy for MnO<sub>2</sub> cathodes, paving the way for the fabrication of high-performance Na-SCs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"112 ","pages":"Pages 29-38"},"PeriodicalIF":14.9,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145048170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fengchun Zhou , Yunfei Huan , Sisi Liu , Yanzheng He , Qiyang Cheng , Mengfan Wang , Chenglin Yan , Tao Qian
{"title":"Platinum-based electrocatalysts for efficient ammonia oxidation in low-temperature direct ammonia fuel cells: Insight into intrinsic mechanisms, activity regulation, and challenges","authors":"Fengchun Zhou , Yunfei Huan , Sisi Liu , Yanzheng He , Qiyang Cheng , Mengfan Wang , Chenglin Yan , Tao Qian","doi":"10.1016/j.jechem.2025.08.025","DOIUrl":"10.1016/j.jechem.2025.08.025","url":null,"abstract":"<div><div>Over recent decades, fuel cell technologies have emerged as viable solutions to address the energy and environmental challenges stemming from fossil fuel dependence. Especially, ammonia has gained increasing attention as an attractive alternative to hydrogen, offering comparable energy density while maintaining carbon-free characteristics, along with superior storage and transport properties that give direct ammonia fuel cells (DAFCs) distinct safety advantages over hydrogen-based systems. Central to this technology is the anodic ammonia oxidation reaction (AOR), where platinum (Pt) remains the most efficient catalyst after years of intensive research. This review offers a comprehensive overview of Pt-based AOR electrocatalysts with potential for application in low-temperature DAFCs. Following an introductory section highlighting key historical developments and catalytic breakthroughs, a fundamental understanding of low-temperature DAFC operation and AOR mechanisms is systematically presented. Subsequently, it outlines the advancements in Pt-based catalysts from simple monometallic systems to sophisticated multimetallic alloys and composites, highlighting material innovations and performance enhancements. Afterward, key challenges and future research directions for advancing AOR electrocatalysts are identified, with the aim of providing valuable guidance for developing practical, high-performance, and low-temperature DAFC systems.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 979-1003"},"PeriodicalIF":14.9,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145044063","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junyi Han , Yini Long , Jiaming Li , Xiao Yu , Nan Li , Shaoyu Zhang , Jiaqi Li , Hedong Gu , Zhanhong Yang
{"title":"Thiol-thione tautomerism-mediated electrolyte additive engineering for stable Zn metal anodes","authors":"Junyi Han , Yini Long , Jiaming Li , Xiao Yu , Nan Li , Shaoyu Zhang , Jiaqi Li , Hedong Gu , Zhanhong Yang","doi":"10.1016/j.jechem.2025.08.029","DOIUrl":"10.1016/j.jechem.2025.08.029","url":null,"abstract":"<div><div>Aqueous zinc-ion batteries (AZIBs) have garnered significant attention as promising candidates for grid-scale energy storage. However, the interfacial instability of zinc anodes caused by the hydrogen evolution reaction (HER) and aqueous electrolyte corrosion severely restricts their practical implementation. This study introduces 2-mercaptothiazoline (MT) as a dynamic electrolyte additive, leveraging its thiol-thione tautomerism for interfacial stabilization. Theoretical calculations and experimental investigations reveal that MT can adsorb onto the zinc surface to form a protective layer to suppress corrosion. Simultaneously, the spatial effect of the thiazoline ring prevents excessive molecular aggregation while enabling homogeneous Zn<sup>2+</sup> electrodeposition. The electronegativity difference between sulfur and nitrogen atoms induces localized polarization, strengthening electronic interactions with the metal surface to accelerate Zn<sup>2+</sup> reduction kinetics and inhibit side reactions. Consequently, smooth and low-porosity Zn deposits with enhanced interfacial stability are achieved. The optimized Zn//Zn symmetric cells exhibit extraordinary cycling stability exceeding 1800 h at 0.5 mA cm<sup>−2</sup>, 0.5 mAh cm<sup>−2</sup>, while sustaining 400 h of operation at 28.5 % depth of discharge (DOD). Zn//MnO<sub>2</sub> full cells incorporating MT additive maintain 122.6 mAh g<sup>−1</sup> capacity retention after 500 cycles (1 A g<sup>−1</sup>). This work provides a facile yet effective strategy for stabilizing Zn metal-based batteries through synergistic interface engineering.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 896-903"},"PeriodicalIF":14.9,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026928","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jiahao Xiang, Minjian Li, Mianrui Li, Lianzhan Huang, Sucheng Liu, Jinhui Liang, Li Du, Zhiming Cui, Huiyu Song, Zhenxing Liang
{"title":"Durable 4.5 V sodium metal batteries stabilized by negatively charged metal–organic frameworks in gel polymer electrolyte","authors":"Jiahao Xiang, Minjian Li, Mianrui Li, Lianzhan Huang, Sucheng Liu, Jinhui Liang, Li Du, Zhiming Cui, Huiyu Song, Zhenxing Liang","doi":"10.1016/j.jechem.2025.07.089","DOIUrl":"10.1016/j.jechem.2025.07.089","url":null,"abstract":"<div><div>The development of high-voltage sodium metal batteries faces significant challenges, including high desolvation energy and detrimental interfacial side reactions at elevated voltages. These issues critically impede Na<sup>+</sup> transport kinetics and compromise high voltage stability, but can be addressed by strategically modifying the Na<sup>+</sup> solvation structure. Herein, we report a metal–organic framework (MOF)-based strategy to reconfigure the Na<sup>+</sup> solvation structure specifically for enhanced high-voltage stability and Na<sup>+</sup> transport. A composite gel polymer electrolyte (MPVHF) is engineered by incorporating UiO-66-(COONa)<sub>2</sub> into a polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) matrix, followed by liquid electrolyte infiltration. The densely arrayed carboxylate groups (–COO<sup>−</sup>) on the MOF ligands exert strong electrostatic interactions with Na<sup>+</sup>, effectively weakening the coordination bonds between Na<sup>+</sup> and solvent molecules. This targeted solvation regulation significantly mitigates interfacial side reactions and promotes the formation of a robust, stable electrode–electrolyte interphase crucial for high-voltage operation. Consequently, the MPVHF electrolyte achieves a wide electrochemical stability window extending to 4.93 V and a high Na<sup>+</sup> transference number of 0.74. The Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>2</sub>F<sub>3</sub> (NVPF)||Na full cells employing MPVHF exhibit stable cycling at 4.5 V cut-off for 1300 cycles at 4 C. This work presents an effective approach to tailor Na<sup>+</sup> coordination and transport for high-voltage and fast-charging sodium metal batteries.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"111 ","pages":"Pages 886-895"},"PeriodicalIF":14.9,"publicationDate":"2025-08-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145026929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}