Akash Kankane , Dhirendra Kumar Rai , S. Janakiraman
{"title":"Synergistic effects of halloysite nanotubes in electrospun PVDF-HFP separator for advanced sodium ion battery","authors":"Akash Kankane , Dhirendra Kumar Rai , S. Janakiraman","doi":"10.1016/j.ssi.2025.116947","DOIUrl":"10.1016/j.ssi.2025.116947","url":null,"abstract":"<div><div>Sodium-ion batteries (SIBs) emerge as a sustainable option for energy storage, standing out as a cost-effective and resource-abundant substitute to lithium-ion batteries (LIBs). However, the development of sustainable SIBs necessitates the innovation of separator materials capable of enhancing battery efficiency and safety. This research highlights the fabrication and characterization of a novel separator made up of polyvinylidene fluoride-<em>co</em>-hexafluoropropylene (PVDF-HFP) filled with halloysite nanotubes (HNTs) via the electrospinning technique for SIBs application. The electrospun composite separator was systematically fabricated and comprehensively characterized to investigate its morphological, electrochemical, thermal and mechanical properties. Field emission scanning electron microscopy (FESEM) analysis revealed a well-dispersed HNTs network within the PVDF-HFP matrix, resulting in a fibrous structure with enhanced mechanical strength (23.6 MPa). Electrochemical performance was evaluated through electrochemical impedance spectroscopy (EIS) and cyclic charge-discharge (GCD). The halloysite filled PVDF-HFP separator demonstrated higher ion conductivity (2.11 mS cm<sup>−1</sup>) and electrochemical stability at ambient temperature, leading to enhanced battery performance, including higher specific capacity (171 mA h g<sup>−1</sup>) at 0.1C-rate. Thermal stability studies confirmed the improved thermal resistance of the composite separator, crucial for maintaining structural integrity under high temperatures. The incorporation of HNTs into the structure of PVDF-HFP contributes to the development of robust and efficient separators for SIBs, facilitating the development of sustainable and scalable energy storage.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116947"},"PeriodicalIF":3.0,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144549722","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Carrier transport in sulfur cathodes of all-solid-state lithium-sulfur batteries: Challenges, strategies, and characterizations","authors":"Haoyue Zhong , Changbao Zhu","doi":"10.1016/j.ssi.2025.116945","DOIUrl":"10.1016/j.ssi.2025.116945","url":null,"abstract":"<div><div>All-solid-state lithium‑sulfur batteries (ASSLSBs) have emerged as promising candidates for next-generation energy storage systems due to their high energy density, excellent safety, and low cost. However, the inherently low electronic and ionic conductivity of sulfur, as well as inadequate solid-solid interfacial contact, leads to sluggish electrochemical reaction kinetics, severely impacting the electrochemical performance of ASSLSBs. To address these challenges, various modification strategies have been developed, focusing on improving charge carrier transport to enhance electrochemical activity and stability of the sulfur cathode. Here, we present a comprehensive review of the key electronic and ionic transport limitations in the sulfur cathode of ASSLSBs, along with the modification strategies and advanced characterization techniques. Finally, we highlight future research directions for the development of sulfur cathodes in realizing high-performance ASSLSBs.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116945"},"PeriodicalIF":3.0,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144562844","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yulia D. Salnikova, Mikhail A. Kamenskii, Elena G. Tolstopyatova, Veniamin V. Kondratiev
{"title":"Aluminum ion doped vanadium oxides as highly stable cathodes for aqueous zinc ion batteries","authors":"Yulia D. Salnikova, Mikhail A. Kamenskii, Elena G. Tolstopyatova, Veniamin V. Kondratiev","doi":"10.1016/j.ssi.2025.116946","DOIUrl":"10.1016/j.ssi.2025.116946","url":null,"abstract":"<div><div>In this work, Al<sup>3+</sup>- doped nanosized layered vanadium oxides (Al<sub>x</sub>V<sub>2</sub>O<sub>5</sub>) with different Al:V ratios have been synthesized by hydrothermal method. The morphology and structure of the obtained compounds were characterized by scanning electron microscopy, X-ray diffraction and X-ray photoelectron spectroscopy. Thin layers of Al-doped vanadium oxide agglomerated in the form of “nanoflowers”. The presence of Al<sup>3+</sup> in the layered structure of the vanadium oxide Al<sub>x</sub>V<sub>2</sub>O<sub>5</sub> with expanded interlayer distance was confirmed. The electrochemical properties of the obtained cathode materials were investigated in coin-type zinc-ion battery cells with a zinc anode in an aqueous solution of 3 M ZnSO<sub>4</sub> by cyclic voltammetry and galvanostatic charge/discharge. The initial capacity of the cathodes depended on the aluminum content (<em>x</em>-values). The highest initial capacity of 383 mAh·g<sup>−1</sup> at a current density of 1.0 A·g<sup>−1</sup> was observed for Al<sub>0.060</sub>V<sub>2</sub>O<sub>5</sub>, which degraded faster due to the lower content of Al<sup>3+</sup> ions, and the capacity retention was 89 % of the initial value. Al<sub>0.072</sub>V<sub>2</sub>O<sub>5</sub> had the lowest initial discharge capacity (196 mAh·g<sup>−1</sup>), but was the most stable with a capacity retention of 98 % (192 mAh·g<sup>−1</sup> after 100 cycles) and 96 % (189 mAh·g<sup>−1</sup> after 300 cycles). Except for the first cycle, the coulombic efficiency of all cathodes is close to 100 %, confirming the perfect reversibility of the charge/discharge process.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116946"},"PeriodicalIF":3.0,"publicationDate":"2025-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144562843","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Change of electrochemical potential and entropy of Li around an edge dislocation in solid electrolytes","authors":"Kyuichi Yasui, Koichi Hamamoto","doi":"10.1016/j.ssi.2025.116950","DOIUrl":"10.1016/j.ssi.2025.116950","url":null,"abstract":"<div><div>The equations of the electrochemical potential and entropy of Li atoms near an edge dislocation inside solid electrolytes are derived. Although a stress field becomes complex in the presence of many dislocations in polycrystalline materials, the equations are still valid and the qualitative conclusions are robust at least for lower dislocation density than about <span><math><msup><mn>10</mn><mn>16</mn></msup></math></span> <span><math><msup><mi>m</mi><mrow><mo>−</mo><mn>2</mn></mrow></msup></math></span>. As the modified electrochemical potential of <span><math><msup><mi>Li</mi><mo>+</mo></msup></math></span> ions in a stress field is spatially uniform at equilibrium in solid electrolytes due to the high mobility of <span><math><msup><mi>Li</mi><mo>+</mo></msup></math></span> ions, the spatial variations of the entropies associated with the stress and electric-potential field are obtained. From the increase in the local entropy by a positively charged dislocation, the concentration of Frenkel pairs of <span><math><msup><mi>Li</mi><mo>+</mo></msup></math></span> interstitials and vacancies is derived, which could be considerably higher near the dislocation. It could be the reason for higher ionic conductivity along a dislocation. It is suggested that a dislocation should be positively charged in an ionic conductor of positive ions in the absence of impurities. When the dilation due to <span><math><msup><mi>Li</mi><mo>+</mo></msup></math></span> interstitials is relatively large, reduction or oxidation of the solid electrolyte may possibly occur near a dislocation although considerable diffusion of atoms and electrons is necessary for it.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116950"},"PeriodicalIF":3.0,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144549720","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Garnet solid electrolytes: Material design, microstructural engineering, and pathways to high-energy density solid-state lithium batteries","authors":"Xin Chen , Ning Zhao , Zhiqing Jia , Xiangxin Guo","doi":"10.1016/j.ssi.2025.116943","DOIUrl":"10.1016/j.ssi.2025.116943","url":null,"abstract":"<div><div>Garnet-type Li<sub>7</sub>La<sub>3</sub>Zr<sub>2</sub>O<sub>12</sub> (LLZO) solid electrolytes have been identified as potential candidates for high-energy solid-state lithium batteries due to their distinguished ionic conductivity, wide-ranging electrochemical stability, and compatibility with lithium metal. This review provides a systematic examination of the structure-property relationships of LLZO, with a specific focus on the pivotal role of grain boundary engineering in improving ionic conductivity. Advanced doping strategies, encompassing single/multi-ion substitution and anion-cation co-doping, are evaluated for their impact on stabilizing the cubic phase and optimizing lithium vacancy distribution. Innovations in sintering techniques and LLZO film fabrication methods are emphasized for their contributions to achieving high ionic conductivity and ultrathin thickness. Moreover, the design of ultrathin flexible organic-inorganic composite electrolytes is discussed to tackle challenges associated with mechanical brittleness and industrialization. The critical evaluations of ionic conductivity enhancement, ultrathin electrolyte fabrication strategies, and scalability challenges provide insightful references for the advancement of LLZO-based solid-state batteries toward high energy density and industrial practicality.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116943"},"PeriodicalIF":3.0,"publicationDate":"2025-07-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144549723","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
D. Chatzogiannakis , O. Arcelus , E. Ayerbe , P. Ghorbanzade , B. Ricci , I. de Meatza , M. Casas-Cabanas , M. Rosa Palacin
{"title":"Key design considerations for blended electrodes in Li-ion batteries","authors":"D. Chatzogiannakis , O. Arcelus , E. Ayerbe , P. Ghorbanzade , B. Ricci , I. de Meatza , M. Casas-Cabanas , M. Rosa Palacin","doi":"10.1016/j.ssi.2025.116942","DOIUrl":"10.1016/j.ssi.2025.116942","url":null,"abstract":"<div><div>Blended electrodes, containing two or more active materials, are already a key part of commercial battery cells, especially ones used in EVs. Yet, surprisingly, research on them at a fundamental level remains limited. This work aims to shed light on their unique characteristics, discuss how best to study them, and offer practical guidelines for designing them effectively. A particular emphasis is placed in specific cell designs to study them, such as the decoupled blend cell. This allows the study of each material separately within the same system, helping to assess effective rates. Beyond experimental techniques, this work also touches on modeling approaches for blended electrodes aiming at predicting performance, fine-tune material combinations, and accelerate the development of better electrode formulations. By combining all these strategies, a deeper understanding of blended electrodes should be achieved, ultimately enabling improving battery performance, longevity, and efficiency. Given their growing role in commercial energy storage, continued research is essential to unlock their full potential and push battery technology forward.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116942"},"PeriodicalIF":3.0,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144514186","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Current-overpotential relationships from electrochemical impedance spectroscopy (EIS) under DC bias – A tutorial exercise applied to a Pt||YSZ electrode","authors":"Stine Roen , Ragnar Strandbakke , Truls Norby","doi":"10.1016/j.ssi.2025.116939","DOIUrl":"10.1016/j.ssi.2025.116939","url":null,"abstract":"<div><div>Electrochemical impedance spectroscopy (EIS) of electrode polarisation offers the possibility to delineate overpotentials into ohmic, charge transfer kinetic, and transport and other mass transfer contributions, commonly applied and interpreted under open circuit conditions. It is sometimes also applied under DC bias, as it in principle then can provide information about net anodic or cathodic processes. However, the impedances so obtained are seldomly converted to overpotentials and therefore remain as qualitative indicators only. Here, we tutorially derive formalism of converting resistances from EIS under DC bias properly into overpotential contributions to the total overpotential, allowing identification of their origins from their dependencies on the current. We illustrate the methodology by generated model current-voltage curves and then apply it to an experimental data set for a Pt electrode on an yttria-stabilised zirconia (YSZ) oxide ion conducting electrolyte. The result reveals that a dominating electrode polarisation easily taken to reflect mass transfer in fact behaves like a second charge transfer step following Butler-Volmer kinetics, allowing us to hypothesise a new model for the O<sub>2</sub>,Pt||YSZ electrode. Our tutorial exercise is applicable to both liquid- and solid-state electrochemistry and should apply equally also to EIS under DC bias of any types of junctions.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116939"},"PeriodicalIF":3.0,"publicationDate":"2025-06-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144513635","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Amit Bhattacharya , Ji-young Ock , Tao Wang , James T. Bamford , Rachel A. Segalman , Sheng Dai , Alexei P. Sokolov , Xi Chelsea Chen , Raphaële J. Clément
{"title":"Critical role of polymer-ceramic ion exchange for high conductivity composite electrolytes","authors":"Amit Bhattacharya , Ji-young Ock , Tao Wang , James T. Bamford , Rachel A. Segalman , Sheng Dai , Alexei P. Sokolov , Xi Chelsea Chen , Raphaële J. Clément","doi":"10.1016/j.ssi.2025.116938","DOIUrl":"10.1016/j.ssi.2025.116938","url":null,"abstract":"<div><div>Polymer-ceramic composites offer a path to enhance the transport and mechanical properties of solid electrolytes. However, an in-depth understanding of the extent and role of ion transport along and across polymer-ceramic interfaces in these systems is lacking. We have recently shown that Li-conducting Li<sub>0.11</sub>Na<sub>0.24</sub>K<sub>0.02</sub>La<sub>0.43</sub>TiO<sub>2.82</sub> (LMTO) nanorods can be prepared by a molten flux method, and the addition of 30–50 weight (wt.)% LMTO to a bis[(trifluoromethyl)sulfonyl]imide-vinyl ethylene carbonate-based single-ion conducting (SIC) polymer electrolyte leads to a two-fold enhancement in Li-ion conductivity, from 1.4 to 3.0 × 10<sup>−5</sup> S/cm at 30 °C. In the present study, we use NMR methods to identify the Li-ion transport pathways and determine the timescale of chemical exchange between the SIC polymer and LMTO ceramic components. Tracer exchange NMR indicates preferential transport through the polymer or polymer-interfacial regions, and exchange spectroscopy (EXSY) and a new isotope exchange method reveal negligible Li exchange between the SIC polymer and LMTO ceramic up to several days. Here, LMTO nanorods act as a passive filler. Our results further highlight that significant (e.g., 10- or 100-fold) conductivity enhancements in composite electrolytes can only be achieved 1) with ionically-conductive fillers, and 2) when both the ceramic and polymer components <em>actively</em> participate in long-range transport. For this, fast interfacial ion exchange is needed. This leads us to introduce a critical interfacial ion exchange time to evaluate whether a filler actively contributes to conduction in a composite electrolyte, and screen for promising polymer-ceramic pairings to accelerate the development of high conductivity solid electrolytes.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116938"},"PeriodicalIF":3.0,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144480850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Michael L. Machala , Dawei Zhang , Di Chen , Hongyang Su , Zixuan Guan , Hanshi Li , Yunzhi Liu , Joonsuk Park , Robert Sinclair , Ethan Crumlin , Hendrik Bluhm , William C. Chueh
{"title":"Reducing the degradation rate and surface segregation of (La0.5Sr0.5)FeO3−δ electrodes in ambient air through multilayering","authors":"Michael L. Machala , Dawei Zhang , Di Chen , Hongyang Su , Zixuan Guan , Hanshi Li , Yunzhi Liu , Joonsuk Park , Robert Sinclair , Ethan Crumlin , Hendrik Bluhm , William C. Chueh","doi":"10.1016/j.ssi.2025.116940","DOIUrl":"10.1016/j.ssi.2025.116940","url":null,"abstract":"<div><div>Transition metal perovskite oxides are employed as air electrode catalysts for solid-oxide fuel cells and electrolyzers. However, degradation linked to cation segregation and precipitation involving alkaline-earth substituents limits their commercialization. In this work, we engineered a multilayer electrode consisting of an ultrathin (La<sub>1−x</sub>Sr<sub>x</sub>)FeO<sub>3−δ</sub> catalyst overlayer (x = 0, 0.5), a cation-migration-suppression Pr<sub>0.1</sub>Ce<sub>0.9</sub>O<sub>2−δ</sub> layer, and a bulk-transport (La<sub>0.5</sub>Sr<sub>0.5</sub>)FeO<sub>3−δ</sub> layer. This “trilayer” electrode structure enables the surface reactivity and stability to be optimized independently from the bulk transport: an architecture that mitigates the segregation of available Sr and other cations from the bulk reservoir and their subsequent precipitation at the solid–gas interface. This trilayer architecture reduced surface reaction resistance and long-term degradation by over an order of magnitude at 650 <span><math><msup><mrow></mrow><mo>°</mo></msup><mi>C</mi></math></span> over 48 h. The approach offers a general pathway for designing multilayer electrode coatings with decoupled catalytic and transport functionalities.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116940"},"PeriodicalIF":3.0,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144472291","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Ion emission efficiency of Ag+ ions from silver ion-conducting glass under atmospheric pressure","authors":"Daigo Ito, Daisuke Urushihara, Yusuke Daiko","doi":"10.1016/j.ssi.2025.116941","DOIUrl":"10.1016/j.ssi.2025.116941","url":null,"abstract":"<div><div>By sharpening ion-conductive glass and applying a high voltage, conducting species ions are released from the glass tip. The ion emission of Ag<sup>+</sup> ions under atmospheric pressure was investigated. Under atmospheric pressure, there is a possibility that various ions are produced as a result of corona discharge. To analyze the efficiency of Ag<sup>+</sup> ion emission from the tip of sharpening glass, a quartz crystal microbalance was used to simultaneously measure the mass of the emitted ions and the ion current value. In an air atmosphere at room temperature, the efficiency of Ag<sup>+</sup> ion emission was only ∼20 %. The efficiency tended to decrease further in an oxygen atmosphere. On the other hand, the emission efficiency reaches approximately 100 % in N<sub>2</sub> atmosphere. The efficiency of Ag<sup>+</sup> ion emission under atmospheric pressure with various conditions are discussed in this paper.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"428 ","pages":"Article 116941"},"PeriodicalIF":3.0,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144338517","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}