Solid State Ionics最新文献

{"title":"Investigating the impact of solid electrolyte particle size/void shape in modulating lithium-ion conduction pathways within graphite composite electrodes using in situ X-ray computed tomography","authors":"Yong Jun Park ,&nbsp;Seunghoon Yang ,&nbsp;Toshiki Watanabe ,&nbsp;Kentaro Yamamoto ,&nbsp;Atsushi Sakuda ,&nbsp;Akitoshi Hayashi ,&nbsp;Masahiro Tatsumisago ,&nbsp;Mukesh Kumar ,&nbsp;Neha Thakur ,&nbsp;Toshiyuki Matsunaga ,&nbsp;Yoshiharu Uchimoto","doi":"10.1016/j.ssi.2025.116975","DOIUrl":"10.1016/j.ssi.2025.116975","url":null,"abstract":"<div><div>Although all-solid-state batteries (ASSBs) have superior safety and higher energy density than conventional lithium-ion batteries (LIBs), concern regarding inadequate power density originate from the poor Li-ion conduction in composite electrode, especially at high C-rate. Tortuosity of solid electrolyte (SE) within the composite electrode has been considered as one of the major components which influence their electrochemical performance. However, research based on structural information for composite electrodes under actual pressure conditions is not sufficient. Here, we investigated the effect of solid electrolyte particle size on the voids and tortuosity of solid electrolyte in composite electrode and electrochemical performance of composite electrodes using in situ X-ray computed tomography. The results showed that fine Li₃PS₄ resulted in better packing and lowering tortuosity to increasing pressure compared to large Li₃PS₄, which enhanced the electrochemical performance, especially at higher pressure. A detailed analysis on shapes of voids revealed that plate-like voids with low elongation and flatness disappeared and more spherical voids with high elongation and flatness were emerged as external pressure increased. In addition, the voids in the composite electrode using fine Li₃PS₄ particles were less likely to interfere with Li-ion conduction pathways, which improved overall battery performance. This study highlights the important role of SE particle size in optimizing ASSB performance through improved microstructural properties.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116975"},"PeriodicalIF":3.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720845","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":"Migration energies of the constituent ions in LaAlO3","authors":"Robert A. Jackson ,&nbsp;Peter Fielitz ,&nbsp;Günter Borchardt","doi":"10.1016/j.ssi.2025.116974","DOIUrl":"10.1016/j.ssi.2025.116974","url":null,"abstract":"<div><div>The calculated migration energies of the constituent elements of LaAlO₃ are comparable to the corresponding calculated migration energies of LaGaO₃ available in the literature. The resulting calculated ranking of the migration energies, <span><math><mi>Δ</mi><msubsup><mi>E</mi><mi>m</mi><mtext>Oxygen</mtext></msubsup><mo>&lt;</mo><mi>Δ</mi><msubsup><mi>E</mi><mi>m</mi><mtext>A site cation</mtext></msubsup><mo>&lt;</mo><mi>Δ</mi><msubsup><mi>E</mi><mi>m</mi><mtext>B site cation</mtext></msubsup></math></span>, is valid for various nominally undoped oxide perovskites (ABO₃). From this ranking it must be concluded that for a specific temperature the ranking of the self-diffusivities of the constituent elements in nominally undoped oxide perovskites reads <span><math><msub><mi>D</mi><mtext>Oxygen</mtext></msub><mo>≫</mo><msub><mi>D</mi><mtext>A site cation</mtext></msub><mo>≫</mo><msub><mi>D</mi><mtext>B site cation</mtext></msub></math></span>. The low cation mobilities in undoped oxide perovskites hamper the experimental determination of the diffusivities of the cations considerably. That is predominantly true for the B site elements which probably migrate via an antisite mechanism in the A sublattice. This conjecture is rationalized by an appropriate mechanistic model which is principally valid for any ternary oxide system with very different defect concentrations and cation mobilities in the two cation sublattices.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116974"},"PeriodicalIF":3.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720879","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":"Ethyl difluoroacetate additive engineering for fast-charging and durable graphite anodes in lithium-ion batteries","authors":"Bin Li ,&nbsp;Wenlin Gong ,&nbsp;Mingyao Yang ,&nbsp;Si Lin ,&nbsp;Yan Liu ,&nbsp;Jiayi Su ,&nbsp;Jie Zhang ,&nbsp;Guocong Liu","doi":"10.1016/j.ssi.2025.116986","DOIUrl":"10.1016/j.ssi.2025.116986","url":null,"abstract":"<div><div>The practical application of fast-charging lithium-ion batteries is hindered by interfacial instability at graphite anodes, primarily due to uncontrolled electrolyte decomposition and the formation of resistive solid electrolyte interphase (SEI) layers. Herein, we report ethyl difluoroacetate (EDFA) as a fluorinated additive for conventional LiPF₆/EC-EMC electrolytes to address these challenges. Electrochemical measurements demonstrate that EDFA undergoes preferential reduction to form a stable, fluorine-rich SEI, which enhances interfacial stability and facilitates Li⁺ transport. As a result, graphite/Li half-cells with EDFA exhibit significantly improved performance, with capacity retention increasing from 81.8 % to 93.4 % after 100 cycles and 3C-rate capacity rising from 49.1 to 99.5 mAh·g⁻¹. SEM, TEM, and XPS analyses confirm the formation of a uniform, compact and fluorine-rich SEI that mitigates parasitic reactions and reduces impedance. This work provides a viable strategy to enhance fast-charging performance in commercial battery systems through additive engineering.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116986"},"PeriodicalIF":3.3,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720846","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":"High temperature oxygen exchange reaction on dense and porous La0.6Sr0.4CoO3-δ electrodes: An overview of the experimental evidence for modeling","authors":"Tatsuya Kawada","doi":"10.1016/j.ssi.2025.116973","DOIUrl":"10.1016/j.ssi.2025.116973","url":null,"abstract":"&lt;div&gt;&lt;div&gt;Oxygen exchange kinetics was investigated to model the current-potential relationship of mixed conducting oxide electrodes used in SOFC and SOEC. Focusing on La&lt;sub&gt;0.6&lt;/sub&gt;Sr&lt;sub&gt;0.4&lt;/sub&gt;CoO&lt;sub&gt;3&lt;/sub&gt; as a model material, experimental evidence so far obtained in our group were summarized and reanalyzed. The reaction order analysis suggested a complex reaction mechanism, for which we came to think of two series kinetics, surface process and subsurface process. The former refers to an exchange process between gas-phase oxygen molecules and some sort of surface oxygen species. The latter refers to the exchange of surface oxygen with bulk oxide ions, and the reaction barrier is not necessarily oxygen transport, but may be electron transport/transfer for oxygen in/ex-corporation This hypothesis appeared to resolve some of our remaining questions regarding the experimental results, such as scattered &lt;em&gt;p&lt;/em&gt;&lt;sub&gt;O&lt;sub&gt;2&lt;/sub&gt;&lt;/sub&gt; dependence in high partial pressure range, the higher isotope exchange rates than electrochemical impedance, and the reaction rate enhancement in the presence of the LaSrCoO&lt;sub&gt;4&lt;/sub&gt; phase. While a single piece of such experimental evidence is insufficient to prove the hypothesis, considering all the results together provides strong support. We then tried to separate the contributions of surface and subsurface processes by measuring the surface oxygen potential using a porous oxygen sensor. 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{"title":"When ions are in charge: Generalized ionic impedance spectroscopy for characterizing energy materials and devices","authors":"Paul Nizet ,&nbsp;Francesco Chiabrera ,&nbsp;Alex Morata ,&nbsp;Albert Tarancón","doi":"10.1016/j.ssi.2025.116972","DOIUrl":"10.1016/j.ssi.2025.116972","url":null,"abstract":"<div><div>Electrochemical Impedance Spectroscopy (EIS) is the conventional technique for studying the electrical response of individual materials or complete energy devices such as batteries, fuel cells, and supercapacitors. However, EIS has several limitations, including its spatial resolution, the description of ion insertion phenomena (especially when multiple ion species are involved), and the presence of porous electrodes. In this paper, Generalized Ionic Impedance Spectroscopy (GIIS) is proposed to address these issues by complementing traditional EIS to analyze ionic concentration changes under an AC voltage stimulus. A broad range of characterization techniques can be employed to analyze such ionic concentration variations, as these significantly modify the functional properties of the material, such as optical, magnetic, and electrical behavior. Some of these techniques also offer high spatial resolution, enabling lateral and depth profiling analysis. This study provides a theoretical framework for the development of GIIS in the field of energy, analyzing battery-like and fuel cell-like devices while resolving the major limitations of EIS mentioned above. The proven versatility of GIIS opens new pathways for the detailed characterization of energy materials and devices, advancing the understanding of low-frequency fundamental electrochemical processes and broadening the scope of their applications. While many of the discussed cases are experimentally validated, others are presented as perspectives of GIIS applications.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116972"},"PeriodicalIF":3.0,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144702473","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":"High Oxide-ion Conductivity in Cubic Perovskite Na- and Ga-doped BaZrO3","authors":"Akanksha Yadav ,&nbsp;Yeting Wen ,&nbsp;Xi Yang ,&nbsp;Dunji Yu ,&nbsp;Yan Chen ,&nbsp;Kevin Huang","doi":"10.1016/j.ssi.2025.116976","DOIUrl":"10.1016/j.ssi.2025.116976","url":null,"abstract":"<div><div>Solid oxide ion electrolytes (SOEs) play a crucial role in determining the operating temperature, cost, and lifetime of solid oxide electrochemical devices. The most competitive SOEs are typically found in cubic-structured fluorides (e.g., ZrO₂-based and CeO₂-based) and perovskites (e.g., LaGaO₃-based and Ba(<em>Zr</em>,<em>Ce</em>)O₃-based). However, the discovery of new high-conductivity SOE systems has been very limited in the history of solid state ionics. Here, we explore a new cubic-structured perovskite, Ba_1-xNa_xZr_1-xGa_xO_3-x (BNZG), as a potential oxide-ion conductor. Compared to La_0.8Sr_0.2Ga_0.8Mg_0.2O_2.8 (LSGM), a state-of-the-art perovskite electrolyte, BNZG exhibits a comparable bulk ionic conductivity (∼0.01 S/cm at 600°C) while reducing Ga content by 40 %. Additionally, compared to BaZr_0.8Y_0.2O_2.9 (BZY), another widely studied perovskite electrolyte, BNZG shows excellent sinterability at lower temperatures. Ab Initio molecular dynamics (AIMD) simulations suggest that BNZG is an oxide-ion conductor, particularly at higher temperatures, which is also confirmed by high oxide-ion transport number (&gt;0.99) and conductivity independent of oxygen and water vapor partial pressures. Furthermore, BNZG is stable in CO₂/air and compatible with active perovskite cathodes such as La_1-xSr_xCoO_3-δ without the use of barrier layer. We also show that the high grain-boundary resistance originated from Ga segregation could be one critical issue for BNZG application in intermediate temperature solid oxide cells.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116976"},"PeriodicalIF":3.0,"publicationDate":"2025-07-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144702474","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":"Phase field simulation of effect of ceramic composite separator on the growth of lithium dendrites","authors":"Chuanxiang Zhang ,&nbsp;Hao Zhang ,&nbsp;Qingyang Hu ,&nbsp;Yuhan Zhang ,&nbsp;Zhixin Liu ,&nbsp;Xingxu Gao ,&nbsp;Tao Wang","doi":"10.1016/j.ssi.2025.116966","DOIUrl":"10.1016/j.ssi.2025.116966","url":null,"abstract":"<div><div>The uncontrollable growth of lithium dendrites has a huge impact on the practical application of lithium metal batteries. The separator is an integral element of the battery and fulfils two functions: firstly, it ensures the normal operation of the battery, and secondly, it is effective in inhibiting the growth of lithium dendrites. The present paper proposes the establishment of a two-dimensional phase field model, with the objective of investigating the effects of the ceramic composite diaphragm phase and the PE separator diaphragm phase on lithium dendrite growth. This investigation is conducted under conditions of stress and temperature fields. It has been shown that the elastic modulus of ceramic particles is greater than that of lithium metal. Therefore, the ceramic separator can effectively prevent the growth of lithium dendrites under stress-coupled conditions. In addition, at higher temperatures, it is beneficial to the transport of lithium ions and increases the deposition of lithium dendrites in the tip and non-tip regions, thereby reducing the length of lithium dendrites at high temperatures. This study reveals the important influence of the ceramic separator on inhibiting the growth of lithium dendrites under the conditions of stress field and temperature field.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116966"},"PeriodicalIF":3.0,"publicationDate":"2025-07-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144695115","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":"Electrophoretically deposited polymer-in-ceramic electrolyte comprising polymerized ionic liquid","authors":"Moran Lifshitz ,&nbsp;Anna Greenbaum ,&nbsp;Inbar Anconina ,&nbsp;Thomas Leirikh ,&nbsp;Mounesha Garaga Nagendrachar ,&nbsp;Ivan Popov ,&nbsp;Harmandeep Singh ,&nbsp;Gaukhar Toleutay ,&nbsp;Yuri Feldman ,&nbsp;Alexei P. Sokolov ,&nbsp;Steve Greenbaum ,&nbsp;Diana Golodnitsky","doi":"10.1016/j.ssi.2025.116971","DOIUrl":"10.1016/j.ssi.2025.116971","url":null,"abstract":"<div><div>Composite solid electrolytes, in which superionic ceramics materials are combined with ion-conducting polymers, could revolutionize electrochemical-energy-storage devices enabling higher energy density, providing greater stability during operation and enhanced safety. However, the interfacial resistance between the ceramic and polymer phases strongly suppresses the ionic conductivity and presents the main obstacle for the practical uses.</div><div>In the current article, an attempt has been made to improve composite conductivity by significantly increasing ceramic concentration in combination with the polymerized ionic liquid (PolyIL). The film was prepared by the electrophoretic deposition method. We believe this is the first demonstration of a PolyIL as a multifunctional additive in EPD, enabling both field-driven deposition and an integrated electrolyte architecture that ensures mechanical cohesion and continuous ion transport pathways. We deposited thirty-micron-thick composite film, which contains more than 90 wt% of LAGP. It has porous structure, in which single ceramic particles and their aggregates are coated by PolyIL. Broad Band Dielectric Spectroscopy method is used for the understanding of ion transport in composite polymer-in-ceramic electrolyte. We observed no improvement in conductivity and assign this to the dominating effect of interfacial energy barriers limiting Li transport in composites.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116971"},"PeriodicalIF":3.0,"publicationDate":"2025-07-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144685903","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":"Exploring the reaction process and properties of γ-Ce2S3 derived from pure and Na-doped CeO2 sulfurization with CS2","authors":"Fusheng Song ,&nbsp;Hongbing Wei ,&nbsp;Zongyang Shen ,&nbsp;Zhumei Wang ,&nbsp;Yueming Li","doi":"10.1016/j.ssi.2025.116965","DOIUrl":"10.1016/j.ssi.2025.116965","url":null,"abstract":"<div><div>The sulfurization pathways of pure and Na-doped CeO₂ with CS₂ were investigated to elucidate the mechanism by which Na⁺ doping lowers <em>γ</em>-Ce₂S₃ synthesis temperature. For undoped CeO₂, the synthesis of <em>γ</em>-Ce₂S₃ typically encompasses three primary steps: (1) deoxidation, where oxygen in CeO₂ is substituted by sulfur to form CeS₂; (2) reduction of CeS₂ to <em>α</em>-Ce₂S₃; (3) a phase transition sequence from <em>α</em>-Ce₂S₃ to <em>β</em>-Ce₂S₃, and subsequently to <em>γ</em>-Ce₂S₃. This process requires a high synthesis temperature of up to 1300 °C. Remarkably, Na⁺ introduction fundamentally altered this pathway, bypassing <em>α</em> and <em>β</em> intermediates to directly yield pure <em>γ</em>-Ce₂S₃ at 900 °C. This is attributed to Na⁺-promoted formation of NaCeS₂ and Ce₂O₂S intermediates that facilitate direct <em>γ</em>-phase crystallization. The resultant <em>γ</em>-[Na]-Ce₂S₃ solid solution exhibits modified band structure and enhanced thermal stability compared to undoped <em>γ</em>-Ce₂S₃.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116965"},"PeriodicalIF":3.0,"publicationDate":"2025-07-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144679942","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":"Li3BO3 decoration endows fast reaction kinetics of LiFePO4 cathode for lithium ion batteries","authors":"Kaihua Li,&nbsp;Jiajin Li,&nbsp;Haoyu Qi,&nbsp;Jinze Song,&nbsp;Diaohan Wang,&nbsp;Lijun Fu,&nbsp;Yuping Wu","doi":"10.1016/j.ssi.2025.116944","DOIUrl":"10.1016/j.ssi.2025.116944","url":null,"abstract":"<div><div>Olivine-type lithium iron phosphate is widely used as a cathode material for lithium-ion batteries because of its moderate operating voltage, excellent stability, and high safety. However, the high rate capability of LiFePO₄ is limited by its low electrical conductivity. Additionally, its interface and internal structure would degrade under high-rate conditions. To address these issues, Li₃BO₃ was prepared via sol-gel method as the surface decoration to enhance the rate performance of LiFePO₄. The Li₃BO₃ decorated LiFePO₄ (B-LiFePO₄) maintains the structural integrity during cycling under large current densities, furthermore, it induces the formation of favorable cathode-electrolyte interface (CEI) with less Li₂CO₃ and more Li₂O contents, and reduces the activation energy of Li⁺ diffusion in the CEI layer and charge transfer, thus the high capacity and long cycle performances of LiFePO₄ are achieved when cycled at high current densities. At ambient environment and 30C, B-LiFePO₄ delivers a high reversible capacity of 63.1 mAh g⁻¹, and a capacity retention of 90 % can be realized over 600 cycles at 1C. In contrast, the original LiFePO₄ delivers only 27.8 mAh g⁻¹ at 30C and a capacity retention of 67.2 % after 600 cycles at 1C. Besides, B-LiFePO₄ demonstrates good low temperature performance, it exhibits high capacities of 122.1 and 80.7 mAh g⁻¹ at 1C, 0 °C and − 20 °C, respectively. This study provides a simple method to enhance the reaction kinetics of LiFePO₄ cathode, which would benefit the development of LiFePO₄ based lithium ion batteries with high rate performance.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"429 ","pages":"Article 116944"},"PeriodicalIF":3.0,"publicationDate":"2025-07-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144671017","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}