Urban Košir, Alen Vizintin, Elena Tchernychova, Gregor Kapun, Matteo Gastaldi, Alia Jouhara, Margaud Lecuyer, Claudio Gerbaldi, Miran Gaberšček, Robert Dominko, Sara Drvarič Talian
The push to use metallic lithium-based batteries motivates a shift toward the use of solid polymer electrolytes. To improve the ionic conductivity values of such electrolytes, liquid additives (plasticizers) are usually added. However, the improvement in conductivity comes at the expense of a deterioration of the anode–electrolyte interface, resulting in poorer electrochemical cell performance. In this study, the use of a polymer coating consisting of polyethylene oxide, LiTFSI, and LiNO3 is proposed. The coating shows improved electrochemical performance and stability, delayed cell failure and a more uniform distribution of Li deposits. These improvements are attributed to the increased stability of the solid electrolyte interphase, which is confirmed by using a combination of electrochemical impedance spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. In contrast, it is found that the interphase in uncoated Li electrodes is likely affected by continuous reactions with the plasticizer, further confirming the need to use such protective coatings to achieve long-term operation in practical solid-state Li metal batteries.
{"title":"Polymer Coating for Li-Metal Anode in Polyethylene Oxide-Based Electrolyte Batteries","authors":"Urban Košir, Alen Vizintin, Elena Tchernychova, Gregor Kapun, Matteo Gastaldi, Alia Jouhara, Margaud Lecuyer, Claudio Gerbaldi, Miran Gaberšček, Robert Dominko, Sara Drvarič Talian","doi":"10.1002/batt.202500402","DOIUrl":"https://doi.org/10.1002/batt.202500402","url":null,"abstract":"<p>The push to use metallic lithium-based batteries motivates a shift toward the use of solid polymer electrolytes. To improve the ionic conductivity values of such electrolytes, liquid additives (plasticizers) are usually added. However, the improvement in conductivity comes at the expense of a deterioration of the anode–electrolyte interface, resulting in poorer electrochemical cell performance. In this study, the use of a polymer coating consisting of polyethylene oxide, LiTFSI, and LiNO<sub>3</sub> is proposed. The coating shows improved electrochemical performance and stability, delayed cell failure and a more uniform distribution of Li deposits. These improvements are attributed to the increased stability of the solid electrolyte interphase, which is confirmed by using a combination of electrochemical impedance spectroscopy, scanning electron microscopy, and X-ray photoelectron spectroscopy. In contrast, it is found that the interphase in uncoated Li electrodes is likely affected by continuous reactions with the plasticizer, further confirming the need to use such protective coatings to achieve long-term operation in practical solid-state Li metal batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500402","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533552","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}
Utkarsh Vijay, Francisco Fernandez, Siwar Ben Hadj Ali, Mark Asch, Alejandro A. Franco
Optimizing the manufacturing process of Lithium-Ion Batteries (LIB. Finding efficient approaches that accelerate and replace time-consuming, material scrap-expensive trials-and-error optimization methods is a key area of research. This work presents a comprehensive LIB electrode manufacturing framework that combines physics-based simulations with deep learning. This framework efficiently simulates the manufacturing process of LIB electrodes as a function of their formulation. This framework takes the form of a surrogate manufacturing model able to predict the impact of manufacturing parameters on the electrode microstructure and properties. The model is based on a regressor-inspired variational autoencoder method. The analysis of the data and the predicted electrode functional metrics demonstrates the consistency of the approach with an electrode manufacturing model developed on the basis of physics. The reported framework holds significant promise in paving near real time optimization of LIB electrode manufacturing and supporting the optimization of battery cell design in pilot lines.
{"title":"Surrogate Modeling of Lithium-Ion Battery Electrode Manufacturing by Combining Physics-Based Simulation and Deep Learning","authors":"Utkarsh Vijay, Francisco Fernandez, Siwar Ben Hadj Ali, Mark Asch, Alejandro A. Franco","doi":"10.1002/batt.202500433","DOIUrl":"https://doi.org/10.1002/batt.202500433","url":null,"abstract":"<p>Optimizing the manufacturing process of Lithium-Ion Batteries (LIB. Finding efficient approaches that accelerate and replace time-consuming, material scrap-expensive trials-and-error optimization methods is a key area of research. This work presents a comprehensive LIB electrode manufacturing framework that combines physics-based simulations with deep learning. This framework efficiently simulates the manufacturing process of LIB electrodes as a function of their formulation. This framework takes the form of a surrogate manufacturing model able to predict the impact of manufacturing parameters on the electrode microstructure and properties. The model is based on a regressor-inspired variational autoencoder method. The analysis of the data and the predicted electrode functional metrics demonstrates the consistency of the approach with an electrode manufacturing model developed on the basis of physics. The reported framework holds significant promise in paving near real time optimization of LIB electrode manufacturing and supporting the optimization of battery cell design in pilot lines.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 12","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500433","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145754525","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}
Magnesium (Mg) is an abundant resource, and rechargeable Mg metal batteries (RMMBs) could help to achieve a sustainable society. However, practical Mg batteries require electrolyte materials compatible with both positive and negative Mg metal electrodes. Weakly coordinating anion (WCA)-based electrolytes meet these requirements and have had a groundbreaking impact on this field of research. In this study, the effects of multidentate oligoether additives on the structural characteristics of WCA-based electrolytes are examined. Integrating a linear oligoether of hexaglyme (G6) is found to be particularly effective at enhancing Mg plating/stripping performance, whereas the corresponding cyclic counterparts impart inferior performance. The combined electrochemical and spectroscopic analyses suggest that changes in the coordination environments of Mg2+ in solution with a specific amount of G6 are responsible for the enhanced interfacial charge-transfer kinetics. The results of this study will help guide the design of fully ethereal RMMB electrolytes compatible with highly reactive Mg metal-negative electrodes.
{"title":"Enhanced Reversibility of Mg Plating/Stripping via Solvation Sheath Regulation by a Multidentate Linear Oligoether","authors":"Toshihiko Mandai","doi":"10.1002/batt.202500348","DOIUrl":"https://doi.org/10.1002/batt.202500348","url":null,"abstract":"<p>Magnesium (Mg) is an abundant resource, and rechargeable Mg metal batteries (RMMBs) could help to achieve a sustainable society. However, practical Mg batteries require electrolyte materials compatible with both positive and negative Mg metal electrodes. Weakly coordinating anion (WCA)-based electrolytes meet these requirements and have had a groundbreaking impact on this field of research. In this study, the effects of multidentate oligoether additives on the structural characteristics of WCA-based electrolytes are examined. Integrating a linear oligoether of hexaglyme (G6) is found to be particularly effective at enhancing Mg plating/stripping performance, whereas the corresponding cyclic counterparts impart inferior performance. The combined electrochemical and spectroscopic analyses suggest that changes in the coordination environments of Mg<sup>2+</sup> in solution with a specific amount of G6 are responsible for the enhanced interfacial charge-transfer kinetics. The results of this study will help guide the design of fully ethereal RMMB electrolytes compatible with highly reactive Mg metal-negative electrodes.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 10","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500348","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145271644","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}
The Front Cover shows the layout of the automated robotic battery materials research platform Aurora automating battery electrolyte formulation, battery cell assembly, and battery cell cycling into a stepwise, automated, application-relevant workflow. A large structured dataset with ontologized metadata detailing cell assembly and cycling protocols, alongside corresponding time series cycling data for almost 200 cells is provided as open research data. More information can be found in the Research Article by C. Battaglia and co-workers (DOI: 10.1002/batt.202500151).