{"title":"Performance Prediction Models with Improved Accuracy and Generalizability for Organic Cathode-Active Materials of Lithium-Ion Battery","authors":"Rika Yamamoto, Yasuhiko Igarashi, Hiroaki Imai, Taisei Sakata, Shuntaro Miyakawa, Shino Yoshizaki, Takaya Saito, Yuya Oaki","doi":"10.1002/batt.202500288","DOIUrl":"10.1002/batt.202500288","url":null,"abstract":"<p>Development of organic energy storage requires enhancing performances of active materials. In particular, reaction potential and specific capacity of cathode-active materials have significant impact on energy density of organic lithium-ion battery. However, discovery of new compounds for active materials based on professional experience and intuition meets the limitation of huge search space of organic molecules. The performance predictors enable efficient discovery of new potential compounds. Although the predictors of potential, capacity, and energy density (models G1) are prepared in the previous work, these become older and have problems. In the present work, the updated models G2 have been constructed to improve the accuracy, usability, and generalizability. The models G2 are prepared by sparse modeling for small data combining machine learning and chemical insight on the training data set with adding new data. The updated models are validated using a new test data set and data-scientific methods. The improved predictors contribute to efficient exploration of new cathode-active materials to realize high-performance batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 9","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500288","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144935482","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}
{"title":"ZnO-gCN Coated Separator for Modulating the Solid-Electrolyte Interphase on Lithium Metal Anodes","authors":"Rashmi Yadav, Ankush Kumar Singh, Rosy","doi":"10.1002/batt.202500128","DOIUrl":"10.1002/batt.202500128","url":null,"abstract":"<p>Lithium metal batteries are recognized as potential candidates for the next-generation energy storage system. Nevertheless, their chemical reactivity, volumetric changes, and dendritic deposition profoundly influence their performance. Introducing an artificial solid-electrolyte interphase (ASEI) is one of the most effective ways to tackle this interfacial instability. However, due to unparalleled reactivity, the direct interfacial engineering of lithium is challenging. Herein, the modification of the polypropylene (PP) separator with lithiophilic zinc oxide (ZnO) and graphitic carbon nitride (gCN) is reported as an indirect yet effective strategy to tackle the interfacial instability of lithium. This work substantiates that ZnO.gCN PP modulates the electrolyte uptake, ionic conductivity, and Li<sup>+</sup> transportation and reacts with the lithium metal to form an ASEI having rigid inorganic materials, leading to much lower nucleation overpotential, reduced polarization, and remarkable cycling stability of more than 500 cycles at 1 mA cm<sup>−2</sup>. The GITT studies further manifested the improved mass and charge-transfer kinetics of Li<sup>+</sup> in the presence of ZnO.gCN PP. The postcycling high-resolution scanning electron microscopy and X-ray photoelectron spectroscopy analysis confirmed that the enhanced electrochemical performance resulted from uniform Li plating/stripping and suppressed electrolyte degradation. Furthermore, the practicality of ZnO.gCN PP is demonstrated through the significantly improved electrochemical performance of NCM811.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 7","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144635008","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}
Frank Tietz, Philipp Odenwald, Doris Sebold, Mareen Schaller, Thorben Böger, Jan Köttgen, Qianli Ma, Sylvio Indris, Wolfgang G. Zeier, Oana Cojocaru-Mirédin, Dina Fattakhova-Rohlfing
{"title":"Impact of Microstructural Properties on Ionic and Heat Transport in NaSICON Glass Ceramics","authors":"Frank Tietz, Philipp Odenwald, Doris Sebold, Mareen Schaller, Thorben Böger, Jan Köttgen, Qianli Ma, Sylvio Indris, Wolfgang G. Zeier, Oana Cojocaru-Mirédin, Dina Fattakhova-Rohlfing","doi":"10.1002/batt.202500093","DOIUrl":"10.1002/batt.202500093","url":null,"abstract":"<p>Two composition series of Zr-deficient NaSICON materials are investigated with respect to their ionic and thermal transport properties. The bulk conductivity varies between 1.4 and 6.6 mS cm<sup>−1</sup>. The total conductivity showdecreasing values with increasing Zr deficiency due to the impact of the increasing fraction of glass phase. The calculated grain boundary conductivity is about two orders of magnitude lower than the total conductivity but does not correspond to the conductivity of any known glass composition of sodium silicates/phosphates. Nuclear magnetic resonance reveals three <sup>23</sup>Na relaxation rates, the fastest of which is attributed to the NaSICON phase and the two slower relaxation rates to sodium orthophosphates and the glass phase. Thermal conductivity varies between 0.9 and 1.0 W m<sup>−1</sup> K<sup>−1</sup> at 25 °C. At elevated temperatures, a clear trend is observed toward lower thermal conductivity with a higher glass fraction. In addition, atom probe tomography is applied to precisely quantify the composition of specific microstructural regions found within the glassy phase. A scanning electron microscopy study of the surfaces of sintered pellets shows an increasing amount of glass phase between the NaSICON particles with increasing Zr deficiency. Furthermore, a time-dependent phase separation is observed in relation to the dynamic formation and dissolution of Na<sub>3</sub>PO<sub>4</sub> domains.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 6","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500093","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144339085","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}
Abirdu Woreka Nemaga, Claude Guery, Michael Molinari, Jean Michel, Mathieu Morcrette, Jeremy Mallet
{"title":"Tailored Synthesis of Conformal Si–Al Coatings on TiO2 Nanotubes for Hybrid Negative Electrodes of Lithium-Ion Batteries","authors":"Abirdu Woreka Nemaga, Claude Guery, Michael Molinari, Jean Michel, Mathieu Morcrette, Jeremy Mallet","doi":"10.1002/batt.202500017","DOIUrl":"10.1002/batt.202500017","url":null,"abstract":"<p>An original synthesis route has been developed to optimize silicon's utility in replacing graphite as anode material in Li-ion batteries. This involves blending silicon with aluminum to enhance its conductivity. The silicon–aluminum is codeposited on a nanoporous titanium dioxide nanotube matrix, which serves as an active current collector, thereby eliminating the need for inactive binders and ensuring robust mechanical stability during cycling. The nanostructured negative electrode is fabricated through two electrochemical synthesis steps: first, the anodization of a titanium foil, followed by the coelectrodeposition of silicon and aluminum using a room temperature ionic liquid electrolyte. This coelectrodeposition enables the in situ integration of aluminum into the silicon deposit. The resulting Si–Al/TiO<sub>2</sub> nanotube nanocomposite anode exhibits improved cyclic stability and enhanced rate capability. The observed enhancement in battery electrochemical performance underscores the significance of this electrochemical process in fabricating such nanostructured silicon negative composite electrodes.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 9","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144934837","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}
Kenta Watanabe, Han-Seul Kim, Kazuhiro Hikima, Naoki Matsui, Kota Suzuki, Hiroyuki Muto, Atsunori Matsuda, Ryoji Kanno, Masaaki Hirayama
{"title":"Self-Closing of Cracks Generated in Microstructure-Controlled 400 μm-Thick Composite Cathodes for All-Solid-State Batteries: Observed by In Situ Scanning Electron Microscopy with Energy-Dispersive X-Ray Spectroscopy","authors":"Kenta Watanabe, Han-Seul Kim, Kazuhiro Hikima, Naoki Matsui, Kota Suzuki, Hiroyuki Muto, Atsunori Matsuda, Ryoji Kanno, Masaaki Hirayama","doi":"10.1002/batt.202500119","DOIUrl":"10.1002/batt.202500119","url":null,"abstract":"<p>All-solid-state batteries (ASSBs) are a promising next-generation secondary battery technology. To achieve high energy and power densities, the thickness of composite electrodes must be increased. The microstructure and mechanical properties of the composites must be carefully controlled to ensure sufficient contact between particles. The 400 μm-thick LiCoO<sub>2</sub>-Li<sub>10.35</sub>Ge<sub>1.35</sub>P<sub>1.65</sub>S<sub>12</sub> (LCO–LGPS) composites are fabricated using LGPS with various particle sizes. The composites using small-sized LGPS particles exhibited higher capacity and retention than those using large-sized particles. <i>In situ</i> cross-sectional scanning electron microscopy with energy-dispersive X-ray spectroscopy reveals that the cracks generated during charging demonstrated self-closing during discharge in the composite with small-sized LGPS regardless of the generated locations, leading to high-capacity retention. However, this self-closing is not observed in the composite using large-sized LGPS. The self-closing behavior depends on the microstructure and mechanical properties of ASSBs. Furthermore, this self-closing finding provides new strategies for designing the microstructure and mechanical properties of ASSBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 6","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500119","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144339185","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}
Willy Shun Kai Bong, Naoya Ishida, Shoko Kitabayashi, Masaki Shimada, Koji Kawamoto, Takuhiro Miyuki, Minoru Kuzuhara
{"title":"Unlocking the Potential of Li-Rich Mn-Based Oxides: Surpassing 300 mAh g−1 at Room Temperature in All-Solid-State Batteries","authors":"Willy Shun Kai Bong, Naoya Ishida, Shoko Kitabayashi, Masaki Shimada, Koji Kawamoto, Takuhiro Miyuki, Minoru Kuzuhara","doi":"10.1002/batt.202500059","DOIUrl":"10.1002/batt.202500059","url":null,"abstract":"<p>This study presents a comprehensive assessment of the temperature-dependent electrochemical performance of LiNbO<sub>3</sub>-coated lithium-rich manganese-based oxide (LRMO) cathodes in all-solid-state batteries (ASSBs). The effects of temperature and activation on the performance of LRMO cathodes are systematically investigated through electrochemical characterization and X-ray diffraction and X-ray absorption near-edge structure analyses. LRMO activation significantly improves electronic conductivity by facilitating lithium intercalation within the sulfide-based solid electrolyte (SE). This conductivity enhancement reduces cell resistance more effectively than an elevation in temperature alone. Because of the low conductivity of LRMO at room temperature (≈10<sup>−6</sup> S cm<sup>−1</sup>), improving the composite cathode's conductivity is critical for reducing cell resistance and enabling LRMO activation. Two strategies are proposed to achieve this: the addition of carbon additives to enhance the electronic conductivity and the application of a LiNbO<sub>3</sub> coating to stabilize the interface between the cathode active material and the SE, thereby minimizing resistance. With these improvements, LiNbO<sub>3</sub>-coated LRMO cathodes with conductive additives achieve a high discharge capacity of over 300 mAh g<sup>−1</sup> after 30 cycles at 25 °C. These findings provide valuable insights into optimizing next-generation LRMO-based cathodes and advancing high-performance energy storage systems for ASSBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 9","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144935436","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}
Adam Mackowiak, Przemyslaw Galek, Paweł Jezowski, Krzysztof Fic
{"title":"Unraveling the Effects of Redox-Active Electrolytes on Carbon Electrodes in Li-Ion Capacitor","authors":"Adam Mackowiak, Przemyslaw Galek, Paweł Jezowski, Krzysztof Fic","doi":"10.1002/batt.202400822","DOIUrl":"10.1002/batt.202400822","url":null,"abstract":"<p>The quest for efficient and sustainable energy storage solutions has generated significant interest in lithium-ion capacitors (LICs) due to their balanced power and energy characteristics. This study explores the performance of carbon electrodes in LICs prelithiated with a redox-active electrolyte containing lithium thiocyanate (LiSCN). The impact of thiocyanate on electrode performance is investigated utilizing step potential electrochemical spectroscopy (SPECS) and the galvanostatic intermittent titration technique (GITT). In the studied conditions, the thiocyanate reaction proceeds with an efficiency of ≈81%, resulting in a capacity of 301 mAh g<sup>−1</sup> for the positive electrode. Notably, the presence of thiocyanates significantly reduces the resistance of the negative electrode by 30%. Therefore, the addition of LiSCN facilitates lithium intercalation in the negative graphite electrode, enhancing capacity and reducing resistance. The SPECS technique reveals distinct intercalation stages and improved ion diffusion, while GITT confirms these findings with diffusion coefficients. Overall, the study demonstrates the efficacy of using redox-active electrolytes in LICs, presenting a viable path for optimizing their performance in future applications.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 9","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400822","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144935494","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}
Andreas Röck, Margret Wohlfahrt-Mehrens, Peter Axmann, Alice Hoffmann
{"title":"Improving Gr/SiO Negative Electrode Formulations: Effect of Active Material, Binders, and Single-Walled Carbon Nanotubes","authors":"Andreas Röck, Margret Wohlfahrt-Mehrens, Peter Axmann, Alice Hoffmann","doi":"10.1002/batt.202400764","DOIUrl":"10.1002/batt.202400764","url":null,"abstract":"<p>With the growing demand for high-energy-density lithium-ion batteries, silicon oxide (SiO) has emerged as a promising anode material due to its high specific capacity. However, its use entails high irreversible losses and mechanical stress. Pre-lithiated SiO (Li-SiO) blended with graphite enables electrodes with rather low irreversible losses, high specific capacity, and less mechanical stress. However, so far, insights about processing Li-SiO are missing in literature. This work deals with Gr/SiO negative electrodes containing 20 wt% SiO in the active mass. We investigate the effects of different suspension formulations on their rheological properties and the electrochemical performance of the electrodes. Our findings prove superior electrochemical properties of anodes made from Li-SiO compared to pristine SiO. However, we show that the basicity of suspensions containing Li-SiO causes challenges for their processability. The integration of single-walled carbon nanotubes is shown to be essential for counteracting the adverse effects and enabling electrodes with enhanced adhesion, reduced irreversible losses, and stable cycling. A good cell performance is demonstrated with electrodes containing as much as 96.8% of active mass. Our findings provide essential insights into the correlation between formulation, processability, and electrochemical performance of Gr/SiO blends, supporting the development of industrial-scale production processes.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400764","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144809241","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}
Luca Minnetti, Faduma M. Maddar, Anupriya K. Haridas, Matthew Capener, Francesco Nobili, Ivana Hasa
{"title":"Cover Feature: Assessing Manufacturing-Performance Correlation On LiMn0.7Fe0.3PO4 Electrodes For Application In Upscaled Li-Ion Battery Cells (Batteries & Supercaps 4/2025)","authors":"Luca Minnetti, Faduma M. Maddar, Anupriya K. Haridas, Matthew Capener, Francesco Nobili, Ivana Hasa","doi":"10.1002/batt.202580402","DOIUrl":"10.1002/batt.202580402","url":null,"abstract":"<p><b>Process parameters</b>, often overlooked in lab-scale studies, play a crucial role in shaping manufacturing–performance correlations when scaling up battery cell components. The Research Article by I. Hasa and co-workers (DOI: 10.1002/batt.202400645) examines the influence of conductive additives and electrode manufacturing parameters, bridging the gap between academic research and industrial applications for a more accurate assessment of electrode performance under realistic conditions.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 4","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202580402","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826741","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}
Abdul Shakoor, Muhammad Adnan, Muhammad Luqman, Muhammad Ahmed Khan, Shahid M. Ramay, Farooq Ahmad, Shahid Atiq
{"title":"Synergistic Improvements in Ionic Conductivity, Diffusion Dynamics, and Transference Numbers for LaNiO3/MXene Supercapacitor Electrodes","authors":"Abdul Shakoor, Muhammad Adnan, Muhammad Luqman, Muhammad Ahmed Khan, Shahid M. Ramay, Farooq Ahmad, Shahid Atiq","doi":"10.1002/batt.202500014","DOIUrl":"10.1002/batt.202500014","url":null,"abstract":"<p>Supercapacitors are crucial for bridging energy storage gaps, offering rapid charge/discharge rates, long cycle life, and high power density, key for renewable energy systems and electric vehicles. This study incorporated MXene (Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub>) into LaNiO<sub>3</sub> (PLNO) at 0, 10, 20, and 30 wt% via solvothermal synthesis. X-ray diffraction confirmed a simple cubic phase across all samples. BET analysis and FESEM revealed mesoporous structures and reduced grain sizes due to MXene inclusion, contributing to enhanced electrochemical performance. Elemental analysis via EDS matched expected stoichiometry. Cyclic voltammetry indicated battery-type behavior, with the LNO-III sample achieving the highest capacity of 541.60 C g<sup>−1</sup> at 2.5 mV s<sup>−1</sup>. Galvanostatic charge/discharge profiles showed increasing discharge times with higher MXene content. The Ragone plot highlighted excellent energy and power densities of 84.30 Wh kg<sup>−1</sup> and 2125 W kg<sup>−1</sup> at 2.5 A g<sup>−1</sup>. Long-term testing demonstrated strong cycle stability, with 88.12% retention over 10 000 cycles. Electrochemical impedance spectroscopy showed low charge transfer resistance (0.84 Ω), short relaxation time (17 ms), high ion diffusion rate (9.5 × 10<sup>−13</sup> m<sup>2</sup> s<sup>−1</sup>), good ionic conductivity (6.3 × 10<sup>−</sup><sup>3</sup> S cm<sup>−1</sup>), and a transference number (t<sub>+</sub>) of 0.3. These results confirm the potential of MXene-modified PLNO as a promising electrode for high-performance supercapacitors.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 9","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-04-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144935411","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}