Pub Date : 2025-04-22DOI: 10.1016/j.ssi.2025.116829
Vladimir B. Nalbandyan , Alexey Yu. Nikulin , Ivan G. Sheptun , Yuri V. Popov , Igor L. Shukaev
It is now widely assumed that conductivity of solid electrolytes may be markedly enhanced by the “high-entropy” (HE) effect. However, HE electrolytes usually differ from their simpler isomorphs by other factors affecting conductivity: lattice expansion/contraction, mobile ion content, bond ionicity, quality of samples. To attribute enhanced conductivity to the HE effect, all other factors should be identical. This work compares “simple” and “HE” ceramic sodium-ion conductors of two related structure types: P2 Nax(MyTi1-y)O2 and honeycomb-ordered P2S Na2M2TeO6, with similar unit cell data, x values, density, and texture and does not reveal any considerable HE effect. In particular, new Na2M2TeO6 conductors combining three to five divalent M (from the list Mg, Co, Ni, Cu, Zn) show similar conductivities with their monocation analogs. Higher conductivity of the P2-type titanates (2–4 mS/cm at 373 K) is explained by the geometrical effect due to smaller size of octahedral cations and possibility of decreased x values.
{"title":"Sodium ion conductivity of hexagonal layered P2-type phases with multiple cationic substitutions","authors":"Vladimir B. Nalbandyan , Alexey Yu. Nikulin , Ivan G. Sheptun , Yuri V. Popov , Igor L. Shukaev","doi":"10.1016/j.ssi.2025.116829","DOIUrl":"10.1016/j.ssi.2025.116829","url":null,"abstract":"<div><div>It is now widely assumed that conductivity of solid electrolytes may be markedly enhanced by the “high-entropy” (HE) effect. However, HE electrolytes usually differ from their simpler isomorphs by other factors affecting conductivity: lattice expansion/contraction, mobile ion content, bond ionicity, quality of samples. To attribute enhanced conductivity to the HE effect, all other factors should be identical. This work compares “simple” and “HE” ceramic sodium-ion conductors of two related structure types: P2 Na<sub>x</sub>(M<sub>y</sub>Ti<sub>1-y</sub>)O<sub>2</sub> and honeycomb-ordered P2S Na<sub>2</sub>M<sub>2</sub>TeO<sub>6</sub>, with similar unit cell data, x values, density, and texture and does not reveal any considerable HE effect. In particular, new Na<sub>2</sub>M<sub>2</sub>TeO<sub>6</sub> conductors combining three to five divalent M (from the list Mg, Co, Ni, Cu, Zn) show similar conductivities with their monocation analogs. Higher conductivity of the P2-type titanates (2–4 mS/cm at 373 K) is explained by the geometrical effect due to smaller size of octahedral cations and possibility of decreased x values.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"425 ","pages":"Article 116829"},"PeriodicalIF":3.0,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143860452","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}
Pub Date : 2025-04-16DOI: 10.1016/j.ssi.2025.116869
Duy Linh Pham , Jean-Noël Chotard , Virginie Viallet , Matthew R. Suchomel , Francois Fauth , Emmanuelle Suard , Stephanie Croyeau , Marc-David Braida , Thierry Le Mercier , Christian Masquelier
All-solid-state batteries (ASSBs) are emerging as next-generation energy storage solutions due to their potential advantages, including enhanced safety, higher energy density, and broader operational temperature ranges. Among various solid electrolytes, amorphous and crystalline Li4PS4I, have attracted interest due to their predicted high conductivity, and high moisture-tolerance. However, experimental studies have reported a wide variation in conductivity values for Li4PS4I, ranging from 0.03 to 3.5 mS.cm−1 at 298 K which are significantly lower than theoretical predictions. Herein, by employing a combination of X-ray diffraction (XRD), 31P magic-angle spinning nuclear magnetic resonance (31P MAS NMR), electrical impedance spectroscopy (EIS), we demonstrate that controlling the crystallinity of Li4PS4I plays a crucial role in its electrochemical performance. Pair distribution function (PDF) analysis reveals the differences in local atomic arrangements between amorphous and crystalline Li4PS4I. Additionally, the analysis indicates that mechanical milling alters the local environment of PS4 tetrahedra and iodide anions, which may explain the discrepancy in conductivity. Furthermore, ASSBs incorporating amorphous-ceramic Li4PS4I in the cathode composite exhibit enhanced cycling stability compared to amorphous Li4PS4I. These findings underscore the potential of tuning crystallinity as an effective approach to optimize the ionic transport properties and cycling performance of ASSBs, paving the way for further advancements in solid electrolytes.
{"title":"Crystalline vs. amorphous Li4PS4I: Impact of structure on ionic transport and performances in solid-state battery","authors":"Duy Linh Pham , Jean-Noël Chotard , Virginie Viallet , Matthew R. Suchomel , Francois Fauth , Emmanuelle Suard , Stephanie Croyeau , Marc-David Braida , Thierry Le Mercier , Christian Masquelier","doi":"10.1016/j.ssi.2025.116869","DOIUrl":"10.1016/j.ssi.2025.116869","url":null,"abstract":"<div><div>All-solid-state batteries (ASSBs) are emerging as next-generation energy storage solutions due to their potential advantages, including enhanced safety, higher energy density, and broader operational temperature ranges. Among various solid electrolytes, amorphous and crystalline Li<sub>4</sub>PS<sub>4</sub>I, have attracted interest due to their predicted high conductivity, and high moisture-tolerance. However, experimental studies have reported a wide variation in conductivity values for Li<sub>4</sub>PS<sub>4</sub>I, ranging from 0.03 to 3.5 mS.cm<sup>−1</sup> at 298 K which are significantly lower than theoretical predictions. Herein, by employing a combination of X-ray diffraction (XRD), <sup>31</sup>P magic-angle spinning nuclear magnetic resonance (<sup>31</sup>P MAS NMR), electrical impedance spectroscopy (EIS), we demonstrate that controlling the crystallinity of Li<sub>4</sub>PS<sub>4</sub>I plays a crucial role in its electrochemical performance. Pair distribution function (PDF) analysis reveals the differences in local atomic arrangements between amorphous and crystalline Li<sub>4</sub>PS<sub>4</sub>I. Additionally, the analysis indicates that mechanical milling alters the local environment of PS<sub>4</sub> tetrahedra and iodide anions, which may explain the discrepancy in conductivity. Furthermore, ASSBs incorporating amorphous-ceramic Li<sub>4</sub>PS<sub>4</sub>I in the cathode composite exhibit enhanced cycling stability compared to amorphous Li<sub>4</sub>PS<sub>4</sub>I. These findings underscore the potential of tuning crystallinity as an effective approach to optimize the ionic transport properties and cycling performance of ASSBs, paving the way for further advancements in solid electrolytes.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"425 ","pages":"Article 116869"},"PeriodicalIF":3.0,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143845216","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}
Pub Date : 2025-04-16DOI: 10.1016/j.ssi.2025.116867
Kuan-Ting Wu , Tatsumi Ishihara
The efficient utilization of CO2 emissions for energy storage and chemical synthesis is critical to achieving sustainable development. This study focuses on enhancing the performance of solid oxide electrolysis cells (SOECs) for intermediate-temperature co-electrolysis of CO2 and H2O to produce syngas. A novel infiltration technique was employed to introduce nanoscale binary-oxide catalysts, including lanthanide, transition, and alkaline earth metal oxides, into selected scaffold electrodes. Among these catalysts, cerium oxide (CeO2) exhibited significant improvements in electrolysis current density and electrocatalytic activity when paring with the potential La(Sr)Fe(Mn)O3 (LSFM) perovskite electrode material. Notably, due to the infiltration of CeO2, a marked enhancement in electrolysis current density (> 60 %) can be achieved with exceptional Faradaic efficiency, in comparison to the non-infiltrated cell. The observed performance enhancement can be attributed to reduced internal resistances, improved microstructural connectivity, and increased active surface area. However, controlling the syngas product remains a challenge, with a bias toward H₂ production in all tested cells, primarily due to the strong influence of the water-gas shift reaction. Despite this limitation, the findings underscore the significant potential of Ce-oxide infiltrants as highly active catalysts for advancing CO2/H2O co-electrolysis applications.
{"title":"Designing highly active electrode by infiltration technique for co-electrolysis of CO2 and H2O","authors":"Kuan-Ting Wu , Tatsumi Ishihara","doi":"10.1016/j.ssi.2025.116867","DOIUrl":"10.1016/j.ssi.2025.116867","url":null,"abstract":"<div><div>The efficient utilization of CO<sub>2</sub> emissions for energy storage and chemical synthesis is critical to achieving sustainable development. This study focuses on enhancing the performance of solid oxide electrolysis cells (SOECs) for intermediate-temperature co-electrolysis of CO<sub>2</sub> and H<sub>2</sub>O to produce syngas. A novel infiltration technique was employed to introduce nanoscale binary-oxide catalysts, including lanthanide, transition, and alkaline earth metal oxides, into selected scaffold electrodes. Among these catalysts, cerium oxide (CeO<sub>2</sub>) exhibited significant improvements in electrolysis current density and electrocatalytic activity when paring with the potential La(Sr)Fe(Mn)O<sub>3</sub> (LSFM) perovskite electrode material. Notably, due to the infiltration of CeO<sub>2</sub>, a marked enhancement in electrolysis current density (> 60 %) can be achieved with exceptional Faradaic efficiency, in comparison to the non-infiltrated cell. The observed performance enhancement can be attributed to reduced internal resistances, improved microstructural connectivity, and increased active surface area. However, controlling the syngas product remains a challenge, with a bias toward H₂ production in all tested cells, primarily due to the strong influence of the water-gas shift reaction. Despite this limitation, the findings underscore the significant potential of Ce-oxide infiltrants as highly active catalysts for advancing CO<sub>2</sub>/H<sub>2</sub>O co-electrolysis applications.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"425 ","pages":"Article 116867"},"PeriodicalIF":3.0,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143845214","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}
Pub Date : 2025-04-15DOI: 10.1016/j.ssi.2025.116850
P.J. Nunes , Wojciech Zając , Katarzyna Styszko , Sónia Pereira , Elvira Fortunato , V. de Zea Bermudez , M. Fernandes
In this work, novel di-ureasil hybrid materials doped with three room-temperature ionic liquids (RTILs) (1-methylimidazolium chloride ([MIm]Cl), 1-ethyl-3-methylimidazolium chloride ([EMIm]Cl), and 1-butyl-3-methylimidazolium chloride ([BMIm]Cl)) are synthesized by the sol-gel method, and their potential as ormolytes in electrochromic devices (ECDs) is evaluated. The ECDs developed exhibit high visible and near-infrared (NIR) transparency, fast switching times, and good coloration efficiency and memory effect, allowing us to foresee their application in energy-efficient smart electrochromic windows.
{"title":"Novel ormolytes for smart electrochromic windows for energy-efficient buildings","authors":"P.J. Nunes , Wojciech Zając , Katarzyna Styszko , Sónia Pereira , Elvira Fortunato , V. de Zea Bermudez , M. Fernandes","doi":"10.1016/j.ssi.2025.116850","DOIUrl":"10.1016/j.ssi.2025.116850","url":null,"abstract":"<div><div>In this work, novel di-ureasil hybrid materials doped with three room-temperature ionic liquids (RTILs) (1-methylimidazolium chloride ([MIm]Cl), 1-ethyl-3-methylimidazolium chloride ([EMIm]Cl), and 1-butyl-3-methylimidazolium chloride ([BMIm]Cl)) are synthesized by the sol-gel method, and their potential as ormolytes in electrochromic devices (ECDs) is evaluated. The ECDs developed exhibit high visible and near-infrared (NIR) transparency, fast switching times, and good coloration efficiency and memory effect, allowing us to foresee their application in energy-efficient smart electrochromic windows.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116850"},"PeriodicalIF":3.0,"publicationDate":"2025-04-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143828800","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}
Pub Date : 2025-04-12DOI: 10.1016/j.ssi.2025.116866
Chanachai Pattanathummasid , Ryoji Asahi , Alex Kutana , Kazuhiro Mori , Toshiyuki Matsunaga , Tsuyoshi Takami
Tuning the atomic arrangement in mixed-anion compounds is one of the key research areas in solid-state chemistry, as it enables the understanding of the structure-property relationship. In this study, we proposed a strategy for fluorine ordering in an oxyfluoride compound with an n = 1 Ruddlesden-Popper (RP) structure, An+1BnO3n+1-xF2x, by aliovalent doping at the A-site. The framework structure based on Ba2(Sn/Zr)O4-xF2x was selected, because oxygen and fluorine occupy all three anion positions—equatorial, apical, and interstitial. To analyze the materials, we used a combination of high-resolution neutron diffraction, synchrotron X-ray diffraction, electrochemical testing, and computational analyses. Our findings show that doping potassium leads to fluorine ordering at the interstitial sites. This ordering occurs to balance the electronic charge at the anion positions, following the electrostatic valence rule. As a result, the electrochemical properties of the compound change: the electrical conductivity increases and the activation energy decreases. These results offer new insights and suggest a strategy for controlling the atomic arrangement in mixed-anion compounds, opening possibilities for designing materials with tailored properties.
{"title":"Enhancing fluoride-ion conduction via doping-induced anionic ordering in an n = 1 Ba-based Ruddlesden-Popper oxyfluoride structure","authors":"Chanachai Pattanathummasid , Ryoji Asahi , Alex Kutana , Kazuhiro Mori , Toshiyuki Matsunaga , Tsuyoshi Takami","doi":"10.1016/j.ssi.2025.116866","DOIUrl":"10.1016/j.ssi.2025.116866","url":null,"abstract":"<div><div>Tuning the atomic arrangement in mixed-anion compounds is one of the key research areas in solid-state chemistry, as it enables the understanding of the structure-property relationship. In this study, we proposed a strategy for fluorine ordering in an oxyfluoride compound with an <em>n</em> = 1 Ruddlesden-Popper (RP) structure, A<sub><em>n</em>+1</sub>B<sub><em>n</em></sub>O<sub>3<em>n</em>+1-<em>x</em></sub>F<sub>2<em>x</em></sub>, by aliovalent doping at the A-site. The framework structure based on Ba<sub>2</sub>(Sn/Zr)O<sub>4-<em>x</em></sub>F<sub>2<em>x</em></sub> was selected, because oxygen and fluorine occupy all three anion positions—equatorial, apical, and interstitial. To analyze the materials, we used a combination of high-resolution neutron diffraction, synchrotron X-ray diffraction, electrochemical testing, and computational analyses. Our findings show that doping potassium leads to fluorine ordering at the interstitial sites. This ordering occurs to balance the electronic charge at the anion positions, following the electrostatic valence rule. As a result, the electrochemical properties of the compound change: the electrical conductivity increases and the activation energy decreases. These results offer new insights and suggest a strategy for controlling the atomic arrangement in mixed-anion compounds, opening possibilities for designing materials with tailored properties.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116866"},"PeriodicalIF":3.0,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820534","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}
Pub Date : 2025-04-12DOI: 10.1016/j.ssi.2025.116865
Jiao Wang , Xun Yang , Xiao-fan Song , Chun Li , He-fa Zhu
Due to its excellent mechanical, thermal, chemical and dielectric properties, zirconia (ZrO2) is widely used in gas sensors, solid oxide fuel cells, high-durability coatings, catalysts, as well as in mechanical engineering, aerospace and dental fields. Compared with other ceramics, zirconia has excellent wear resistance, and after polishing, zirconia maintains a low surface roughness for a long time. At present, most of the researches on the mechanical properties of ZrO2 doping are concentrated in the experimental stage, and the first-principle calculations are mainly focused on the optical properties, thermoelectric properties and thermodynamic properties of ZrO2. Therefore, based on density functional theory, this paper constructs a ZrO2 model through Materials Studio software, conducts convergence tests on the model, studies the electronic structure and bonding of ZrO2, calculates the mechanical properties of ZrO2 after doping different concentrations of CeO2, and analyzes the effects of doping concentrations on mechanical properties and elastic wave velocity from the atomic scale.
{"title":"The influence of Ce element doping on the mechanical properties of ZrO2 ceramic from first-principles calculations","authors":"Jiao Wang , Xun Yang , Xiao-fan Song , Chun Li , He-fa Zhu","doi":"10.1016/j.ssi.2025.116865","DOIUrl":"10.1016/j.ssi.2025.116865","url":null,"abstract":"<div><div>Due to its excellent mechanical, thermal, chemical and dielectric properties, zirconia (ZrO<sub>2</sub>) is widely used in gas sensors, solid oxide fuel cells, high-durability coatings, catalysts, as well as in mechanical engineering, aerospace and dental fields. Compared with other ceramics, zirconia has excellent wear resistance, and after polishing, zirconia maintains a low surface roughness for a long time. At present, most of the researches on the mechanical properties of ZrO<sub>2</sub> doping are concentrated in the experimental stage, and the first-principle calculations are mainly focused on the optical properties, thermoelectric properties and thermodynamic properties of ZrO<sub>2</sub>. Therefore, based on density functional theory, this paper constructs a ZrO<sub>2</sub> model through Materials Studio software, conducts convergence tests on the model, studies the electronic structure and bonding of ZrO<sub>2</sub>, calculates the mechanical properties of ZrO<sub>2</sub> after doping different concentrations of CeO<sub>2</sub>, and analyzes the effects of doping concentrations on mechanical properties and elastic wave velocity from the atomic scale.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116865"},"PeriodicalIF":3.0,"publicationDate":"2025-04-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820535","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}
Pub Date : 2025-04-11DOI: 10.1016/j.ssi.2025.116853
Zixuan Yuan , Qing-Tao Hu , Weijie Wang , Guangxin Wu , Changchun Liu , Hao Chen , He-Zhang Chen , Ying-de Huang , Wenjie Yang
With the explosion of the lithium-ion battery market, the requirement for lithium resources is growing promptly, even though traditional lithium extraction methods are inefficient and research focuses on lithium extraction from brines, efficiently extracting lithium from lithium-rich aluminum electrolytes (LRAE) is crucial. This study explores a novel approach to recover lithium from lithium-containing aluminum electrolytes through hydrochloric acid dissolution and ion-exchange adsorption, aiming to achieve high-value use of hazardous waste. The research examines the influence of various parameters-covering the effects of factors such as hydrochloric acid concentration, reaction time, reaction temperature, and liquid-solid ratio. Including the important role of these factors in the reaction process and outcome, as well as their impact on the entire process. The dissolution rate via hydrochloric acid dissolution. A dissolution efficiency of approximately 76.48 % for lithium was achieved within 90 min using a 2 mol/L hydrochloric acid solution at a temperature of 75 °C, while maintaining a liquid-to-solid ratio of 45:1. Additionally, polymer-loaded PVC-H1.6Mn1.6O4 films were synthesized through a hydrothermal reaction utilizing the dissolution solution as the precursor. The optimal adsorption performance of the PVC-H1.6Mn1.6O4 film was observed at mass concentration of 12 % for both PVC and the precursor. The adsorption equilibrium was attained after 480 min, resulting in a lithium ion adsorption capacity of 381.82 mg/m2. After five cycles of adsorption experiments, the lithium adsorption ability of the PVC-H1.6Mn1.6O4 film in lithium-rich aluminum electrolyte solutions was determined to be 96.80 %, indicating a decrease of 3.20 % compared to the initial lithium adsorption.
{"title":"Study on Li+ adsorption performance using PVC-H1.6Mn1.6O4 film in lithium-rich aluminum electrolyte","authors":"Zixuan Yuan , Qing-Tao Hu , Weijie Wang , Guangxin Wu , Changchun Liu , Hao Chen , He-Zhang Chen , Ying-de Huang , Wenjie Yang","doi":"10.1016/j.ssi.2025.116853","DOIUrl":"10.1016/j.ssi.2025.116853","url":null,"abstract":"<div><div>With the explosion of the lithium-ion battery market, the requirement for lithium resources is growing promptly, even though traditional lithium extraction methods are inefficient and research focuses on lithium extraction from brines, efficiently extracting lithium from lithium-rich aluminum electrolytes (LRAE) is crucial. This study explores a novel approach to recover lithium from lithium-containing aluminum electrolytes through hydrochloric acid dissolution and ion-exchange adsorption, aiming to achieve high-value use of hazardous waste. The research examines the influence of various parameters-covering the effects of factors such as hydrochloric acid concentration, reaction time, reaction temperature, and liquid-solid ratio. Including the important role of these factors in the reaction process and outcome, as well as their impact on the entire process. The dissolution rate via hydrochloric acid dissolution. A dissolution efficiency of approximately 76.48 % for lithium was achieved within 90 min using a 2 mol/L hydrochloric acid solution at a temperature of 75 °C, while maintaining a liquid-to-solid ratio of 45:1. Additionally, polymer-loaded PVC-H<sub>1.6</sub>Mn<sub>1.6</sub>O<sub>4</sub> films were synthesized through a hydrothermal reaction utilizing the dissolution solution as the precursor. The optimal adsorption performance of the PVC-H<sub>1.6</sub>Mn<sub>1.6</sub>O<sub>4</sub> film was observed at mass concentration of 12 % for both PVC and the precursor. The adsorption equilibrium was attained after 480 min, resulting in a lithium ion adsorption capacity of 381.82 mg/m<sup>2</sup>. After five cycles of adsorption experiments, the lithium adsorption ability of the PVC-H<sub>1.6</sub>Mn<sub>1.6</sub>O<sub>4</sub> film in lithium-rich aluminum electrolyte solutions was determined to be 96.80 %, indicating a decrease of 3.20 % compared to the initial lithium adsorption.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116853"},"PeriodicalIF":3.0,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143820533","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}
The development of new proton exchange membranes (PEM) for electrochemical devices have attracted researcher's attention in the pursuit for more sustainable and cost-effective technologies for clean energy production and conversion. In this work, new doped chitosan (CS) membranes were prepared by the casting method. Chitosan is an abundant, biodegradable and non-toxic material, and as a membrane, a sustainable and cheaper alternative to those perfluorinated and commonly used, such as Nafion. Three different ionic liquids were employed as dopants, ([EMIM][OTf], [EMIM][FSI] and [MIMH][HSO4]), in various concentrations and up to 50 wt% load. The new membranes were characterized by ATR-FTIR, thermogravimetry, using TGA and DSC techniques to assess their thermal properties, and by SEM, to analyse their surface morphology. Proton conduction properties of the new membranes were assessed by Electrochemical Impedance Spectroscopy (EIS). The new doped membranes showed an increase in the proton conduction compared with pristine chitosan membranes. The incorporation of ionic liquids into chitosan membranes improved their proton conductivity and thermal properties, with [EMIM][OTf] and [MIMH][HSO4] showing the most promising results. A 2-fold increment in the proton conduction was generally observed with the increase of the temperature from 30 to 60 °C. The best proton conductivity was found at 60 °C for the membrane doped with [EMIM][OTf], with a value of 47 mS.cm−1.
{"title":"New proton exchange membranes based on ionic liquid doped chitosan","authors":"Naima Naffati , Fátima C. Teixeira , António P.S. Teixeira , C.M. Rangel","doi":"10.1016/j.ssi.2025.116852","DOIUrl":"10.1016/j.ssi.2025.116852","url":null,"abstract":"<div><div>The development of new proton exchange membranes (PEM) for electrochemical devices have attracted researcher's attention in the pursuit for more sustainable and cost-effective technologies for clean energy production and conversion. In this work, new doped chitosan (CS) membranes were prepared by the casting method. Chitosan is an abundant, biodegradable and non-toxic material, and as a membrane, a sustainable and cheaper alternative to those perfluorinated and commonly used, such as Nafion. Three different ionic liquids were employed as dopants, ([EMIM][OTf], [EMIM][FSI] and [MIMH][HSO<sub>4</sub>]), in various concentrations and up to 50 wt% load. The new membranes were characterized by ATR-FTIR, thermogravimetry, using TGA and DSC techniques to assess their thermal properties, and by SEM, to analyse their surface morphology. Proton conduction properties of the new membranes were assessed by Electrochemical Impedance Spectroscopy (EIS). The new doped membranes showed an increase in the proton conduction compared with pristine chitosan membranes. The incorporation of ionic liquids into chitosan membranes improved their proton conductivity and thermal properties, with [EMIM][OTf] and [MIMH][HSO<sub>4</sub>] showing the most promising results. A 2-fold increment in the proton conduction was generally observed with the increase of the temperature from 30 to 60 °C. The best proton conductivity was found at 60 °C for the membrane doped with [EMIM][OTf], with a value of 47 mS.cm<sup>−1</sup>.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116852"},"PeriodicalIF":3.0,"publicationDate":"2025-04-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143799013","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}
Pub Date : 2025-04-07DOI: 10.1016/j.ssi.2025.116858
Zixuan Wang, Jialong Fu, Xin Guo
Polymer electrolytes have been extensively studied due to their high safety, low cost, and ease of processing, and they have received significant attention in the development of solid-state lithium batteries with high energy density and enhanced safety. An ideal polymer-based electrolyte must exhibit a combination of properties, with fast ion conduction being particularly critical. This paper reviews the lithium-ion conduction mechanisms in solid, composite, and quasi-solid polymer electrolytes. The effects of inorganic fillers on Li+ conduction in composite polymer electrolytes, as well as the effects of liquid plasticizers on Li+ conduction in quasi-solid polymer electrolytes, are discussed. In addition, the application prospects of polymer electrolytes in high energy density, high safety solid-state lithium metal batteries are explored. Finally, the challenges and perspectives for the development of high-performance lithium batteries using polymer electrolytes are presented.
{"title":"Conduction of lithium ions in polymer-based electrolytes","authors":"Zixuan Wang, Jialong Fu, Xin Guo","doi":"10.1016/j.ssi.2025.116858","DOIUrl":"10.1016/j.ssi.2025.116858","url":null,"abstract":"<div><div>Polymer electrolytes have been extensively studied due to their high safety, low cost, and ease of processing, and they have received significant attention in the development of solid-state lithium batteries with high energy density and enhanced safety. An ideal polymer-based electrolyte must exhibit a combination of properties, with fast ion conduction being particularly critical. This paper reviews the lithium-ion conduction mechanisms in solid, composite, and quasi-solid polymer electrolytes. The effects of inorganic fillers on Li<sup>+</sup> conduction in composite polymer electrolytes, as well as the effects of liquid plasticizers on Li<sup>+</sup> conduction in quasi-solid polymer electrolytes, are discussed. In addition, the application prospects of polymer electrolytes in high energy density, high safety solid-state lithium metal batteries are explored. Finally, the challenges and perspectives for the development of high-performance lithium batteries using polymer electrolytes are presented.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116858"},"PeriodicalIF":3.0,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143785485","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-07DOI: 10.1016/j.ssi.2025.116857
Baogang Liu , Chengdong Wei , Fenning Zhao , Jian Xu , Jihong Li , Hongtao Xue , Fuling Tang
The structure and nature of the interface between the electrode and the discharge product have an important impact on the performance of Lithium‑sulfur (LiS) batteries. We investigated the effects of transition metals Ti and V doped into FeS2 on the high-rate performance of the interface formed with Li2S(110). Using the first-principles calculations, we have investigated the interface between FeS2(001) with doping transition metal Ti and V, and Li2S(110). The investigation covered aspects such as lattice structure, electrochemical properties, diffusion of Li+ at the interface, distribution of charge, and work function. The results indicate that doping with transition metals Ti and V reduces the Li+ diffusion barrier. The interfacial density of states introduces metallic properties. Additionally, analysis of work function revealed that Ti doping promotes the establishment of an internal electric field in the interfacial structure which accelerates cycling and migration of Li+. This study enhances our understanding of interfacial structure and electrochemical properties between cathode host material and Li2S.
{"title":"Electronic and Li-ion diffusion properties in Fe0.875M0.125S2 (M = Ti, V)(001)|Li2S(110) interface by the first-principles study","authors":"Baogang Liu , Chengdong Wei , Fenning Zhao , Jian Xu , Jihong Li , Hongtao Xue , Fuling Tang","doi":"10.1016/j.ssi.2025.116857","DOIUrl":"10.1016/j.ssi.2025.116857","url":null,"abstract":"<div><div>The structure and nature of the interface between the electrode and the discharge product have an important impact on the performance of Lithium‑sulfur (Li<img>S) batteries. We investigated the effects of transition metals Ti and V doped into FeS<sub>2</sub> on the high-rate performance of the interface formed with Li<sub>2</sub>S(110). Using the first-principles calculations, we have investigated the interface between FeS<sub>2</sub>(001) with doping transition metal Ti and V, and Li<sub>2</sub>S(110). The investigation covered aspects such as lattice structure, electrochemical properties, diffusion of Li<sup>+</sup> at the interface, distribution of charge, and work function. The results indicate that doping with transition metals Ti and V reduces the Li<sup>+</sup> diffusion barrier. The interfacial density of states introduces metallic properties. Additionally, analysis of work function revealed that Ti doping promotes the establishment of an internal electric field in the interfacial structure which accelerates cycling and migration of Li<sup>+</sup>. This study enhances our understanding of interfacial structure and electrochemical properties between cathode host material and Li<sub>2</sub>S.</div></div>","PeriodicalId":431,"journal":{"name":"Solid State Ionics","volume":"424 ","pages":"Article 116857"},"PeriodicalIF":3.0,"publicationDate":"2025-04-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143785484","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}
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