Ralf Schmidt, Tom Boenke, Paul Härtel, Susanne Dörfler, Thomas Abendroth, Holger Althues, Stefan Kaskel
{"title":"High Shear Dispersion Techniques for Up-Scaling and Controllable Cathode Morphology in High Performance Li−S Pouch Cells","authors":"Ralf Schmidt, Tom Boenke, Paul Härtel, Susanne Dörfler, Thomas Abendroth, Holger Althues, Stefan Kaskel","doi":"10.1002/batt.202400768","DOIUrl":"10.1002/batt.202400768","url":null,"abstract":"<p>The lithium sulfur (Li−S) cell chemistry is promising due to the high specific capacity of its active materials resulting in high specific energy cells. In the past years, the number of publications on practical prototype cells have increased, already reporting high specific energies over 400 Wh kg<sup>−1</sup> with low electrolyte-to-sulfur (E : S) ratios. To enable the complex conversion chemistry at low E : S ratios, the cathode porosity adaption is crucial and depends for example on the suspension blending procedure. There are several methods and devices to prepare suspensions for battery electrodes, e. g. dissolver and planetary mixers. In this study, a standard laboratory blender with low shear forces (EL1) is compared with a high shear mixer (HSM) for preparing porous carbon-sulfur suspensions in a relevant scale. In this study, the influence of the slurry preparation on the final performance is investigated by coating via slot die on a roll-to-roll device to produce carbon-sulfur-cathodes. The electrodes are characterized via optical and mechanical measurements. Electrochemical analysis is conducted using coin cells for pre-evaluation as well as multi-layered pouch cells with reduced electrolyte volume (3.0 μl mg(S)<sup>−1</sup>). It could be shown that the HSM enables increased binder dispersion and enhanced density leading to improved cycle life.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400768","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144809280","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}
Junqi Wang, Peng Wu, Ke Wang, Yiren Zhong, Gaoming Sun, Yuanchun Ji, Yuan Ma, Yanjiao Ma
{"title":"Composite (bi-)metallic oxides with heterostructure and heteroatom-doped porous carbon as advanced potassium-ion battery anodes","authors":"Junqi Wang, Peng Wu, Ke Wang, Yiren Zhong, Gaoming Sun, Yuanchun Ji, Yuan Ma, Yanjiao Ma","doi":"10.1002/batt.202400779","DOIUrl":"10.1002/batt.202400779","url":null,"abstract":"<p>In this work, a scalable two-step synthesis method was employed to develop transition metal oxide/carbon composites that exhibit excellent electrochemical performance as the anode of potassium-ion batteries. The functionalized metal-organic framework precursor was combined with molecular silicotungstic acid clusters (SiW9) during thermal conversion, and embedded into in-situ formed porous carbon matrix to form a multi-component CoWO<sub>4</sub>/WO<sub>3</sub>-C composite material with N-doping. Benefiting from unique compositional and structural features, the resulting composite exhibits an appealing potassium-ion storage performance, such as, large specific capacity of ca. 1500 mAh/g after 600 cycles and excellent rate capability, i. e., delivering reversible capacity over 200 mAh/g even at the high-rate of 2.0 A/g.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144809274","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}
Svenja Both, Dr. Simon Hein, Dr. Timo Danner, Prof. Dr. Arnulf Latz
{"title":"Modeling Oxygen Loss and Phase Transformation in Ni-Rich Cathode Materials: Impact of Electrode Microstructure","authors":"Svenja Both, Dr. Simon Hein, Dr. Timo Danner, Prof. Dr. Arnulf Latz","doi":"10.1002/batt.202400802","DOIUrl":"10.1002/batt.202400802","url":null,"abstract":"<p>Nickel-Manganese-Cobalt (NMC) oxides are widely used as cathode materials in lithium-ion batteries. While increasing the nickel content increases the available capacity in a given voltage window, it also reduces the structural stability of the material when cycled to high cutoff voltages. Oxygen release from the crystal structure as well as a layered-to-rocksalt phase transformation of the layered oxide material cause capacity loss and impedance rise. In this work, we propose a continuum approach to model oxygen release and the associated phase transformation using a 1+1D model informed by atomistic simulations to predict the thickness of reconstructed active material over time. An efficient interface model allows us to combine this approach with 3D microstructure-resolved simulations in order to study the effect of a resistive layer on a real cathode microstructure. This novel workflow enables us to investigate the effect of individual electrode properties on the phase transformation and guide future electrode design.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202400802","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144811403","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}
Eunbin Park, Jiwon Jeong, Yung-Eun Sung, Seung-Ho Yu
{"title":"Cover Picture: Green Electrolytes for Aqueous Ion Batteries: Towards High-Energy and Low-Temperature Applications (Batteries & Supercaps 2/2025)","authors":"Eunbin Park, Jiwon Jeong, Yung-Eun Sung, Seung-Ho Yu","doi":"10.1002/batt.202580201","DOIUrl":"10.1002/batt.202580201","url":null,"abstract":"<p><b>The Front Cover</b> illustrates the five key electrolytes discussed in this Review of green aqueous ion batteries by Y.-E. Sung, S.-H. Yu and co-workers (DOI: 10.1002/batt.202400579). At the center of the illustration is a cylindrical aqueous battery, symbolizing the paper's two major themes: high-energy and low-temperature operation. It is placed in the middle of a green forest, surrounded by hydrogel, eutectic, additive/cosolvent, water-in-salt, and molecular crowding electrolytes.\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 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202580201","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431522","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}
Mohammed Alabdali, Franco M. Zanotto, Benoît Notredame, Virginie Viallet, Vincent Seznec, Alejandro A. Franco
{"title":"Cover Feature: Experimental and Computational Analysis of Slurry-Based Manufacturing of Solid-State Battery Composite Cathode (Batteries & Supercaps 2/2025)","authors":"Mohammed Alabdali, Franco M. Zanotto, Benoît Notredame, Virginie Viallet, Vincent Seznec, Alejandro A. Franco","doi":"10.1002/batt.202580202","DOIUrl":"10.1002/batt.202580202","url":null,"abstract":"<p><b>The Cover Feature</b> showcases the manufacturing journey of solid-state battery composite electrodes, capturing the transition of the microstructure across key stages: slurry, drying, and calendering. It features a modeling workflow for battery cathodes composed of LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> and Li<sub>6</sub>PS<sub>5</sub>Cl, unveiling the impact of processing on microstructural evolution, with results validated against experimental data. More information can be found in the Research Article by A. A. Franco and co-workers (DOI: 10.1002/batt.202400709).\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 2","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202580202","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431523","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":"Dynamic Mechanism of Short Peptide Additive Regulating Solvation Microenvironment of Zinc Ions","authors":"Yuting Li, Danyang Xiong, Jiabao Zhu, Yulan Mou, Jinrong Yang, Xiao He","doi":"10.1002/batt.202400735","DOIUrl":"10.1002/batt.202400735","url":null,"abstract":"<p>The optimization electrolyte strategy through molecular additives to improve the stability of aqueous zinc-ion batteries (AZIBs), which changes the solvation structure of hydrated zinc ions (Zn<sup>2+</sup>), generally relies on experimental trial and error, because the precise mechanism by which these additives alter the coordination environment of Zn<sup>2+</sup> remains elusive. Here, we select the oligopeptide of mono-, di-, tri-, and tetra-glycine, as electrolyte additives to optimize the Zn<sup>2+</sup> solvation microenvironment in AZIBs. Contrary to traditional views, we find that these additives modify the solvated structure of the Zn<sup>2+</sup> by substituting sulfate ion (SO<sub>4</sub><sup>2−</sup>) in the preexistence of Zn<sup>2+</sup>-SO<sub>4</sub><sup>2−</sup> ion pair, rather than water molecules in the first solvation shell, due to a high energy barrier to replace one of the coordinated water molecules of Zn<sup>2+</sup>. This observation is consistent with recent experimental result of the attenuating influence of glycine on the interaction between Zn<sup>2+</sup> and SO<sub>4</sub><sup>2−</sup> confirmed by Fourier-transform infrared spectroscopy. For the multifunctional triglycine, its favorable conformation is disrupted to accommodate the direct coordination of oxygen atoms with Zn<sup>2+</sup>, and Zn<sup>2+</sup> is observed to migrate between distinct sites along the triglycine backbone. This work provides theoretical principles to rationally design advanced electrolytes for solvation modulation with high performance AZIBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 7","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144635280","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":"Bolstering the Rate Performance of Co-Free Ni-Rich Layered Oxide Cathode through a Rapid Heating Method","authors":"Soumyadip Mitra, Thilini Rathnayaka Mudiyanselage, Xijue Wang, Gaurav Lohar, Deepak Dubal, Chandran Sudakar","doi":"10.1002/batt.202400782","DOIUrl":"10.1002/batt.202400782","url":null,"abstract":"<p>The growing demand for high-energy density Ni-rich cathode materials, driven by the rise in lithium-ion batteries for electric vehicles and electronics necessitates fast, efficient production methods. Traditional methods for Ni-rich cathodes are energy-intensive, taking up to 24 hours, which increases costs and CO<sub>2</sub> emissions. In contrast, this study introduces a Co-free Ni-rich layered oxide cathode (LiNi<sub>0.9</sub>Fe<sub>0.05</sub>Al<sub>0.05</sub>O<sub>2</sub> (NFA)) synthesis using a rapid microwave heating technique. This method takes just 2.5 hours, including heating and dwell time, while consuming minimal electricity. The microwave-annealed cathodes exhibits a well-ordered layered structure with fewer defects compared to those produced by traditional calcination (21 h). Furthermore, these cathodes display superior discharge capacities across all C-rates (e. g. 157 mAh g<sup>−1</sup> at 1 C-rate and 129 mAh g<sup>−1</sup> at 10 C-rate) and retain 78.1 % specific capacity after 100 cycles at high current density (1 C-rate). This study paves the way for the rapid, energy-efficient synthesis of high-performance cathode materials for advanced lithium-ion batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144811191","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":"Investigating Lithium Segregation in Nickel-Rich Layered Oxides via Atom Probe Tomography and its Impact on Performance","authors":"Peddi Mahender Reddy, Sasikala Natarajan, Nagini Macha, Raghavan Gopalan, Sahana B Moodakare","doi":"10.1002/batt.202400752","DOIUrl":"10.1002/batt.202400752","url":null,"abstract":"<p>Nickel-rich LiNi<sub>0.8</sub>Co<sub>0.15</sub>Al<sub>0.05</sub>O<sub>2</sub> (NCA) is a promising alternative to LiNi<sub>1−x−y</sub>Co<sub>x</sub>Mn<sub>y</sub>O<sub>2</sub> (NMC) with x + y≤0.2, providing high specific energy and power density, making it ideal for long-range electric vehicles. However, the formation of surface residual impurities and extreme sensitivity to moisture are detrimental to the large-scale synthesis and electrochemical performance of NCA. This paper investigates the formation of Li<sub>2</sub>CO<sub>3</sub> surface impurities and the elemental distribution of lithium within the secondary particle in NCA synthesized with different lithium-to-transition metal ratios. X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and Raman spectroscopy confirm the presence of Li<sub>2</sub>CO<sub>3</sub> on the surface of NCA prepared with 3 % excess lithium. Atom probe tomography (APT) analysis of the particle interior confirms the absence of carbonaceous products within the hierarchical structure. Instead, it reveals the segregation of lithium ions into discrete regions, which leads to the poor electrochemical performance of NCA synthesized with excess Li. Upon storage, the structural and electrochemical deterioration is more pronounced in NCA with a 3 % excess of lithium than the one prepared without excess lithium, as confirmed by XRD, Raman imaging, and electrochemical galvanostatic charge-discharge testing.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144811038","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}
Xinran Hu, Wenxi Hu, Deda Peng, Xiaowei Liu, Xing Zhou, Meilong Wang, Yongyuan Zhou, Prof. Jin Han, Prof. Tiefeng Liu, Prof. Ya You
{"title":"Stabilizing Cathode-Electrolyte Interface by Low-Cost Ethyl Methylsulfone Co-Solvent for High-Voltage Sodium-ion Batteries","authors":"Xinran Hu, Wenxi Hu, Deda Peng, Xiaowei Liu, Xing Zhou, Meilong Wang, Yongyuan Zhou, Prof. Jin Han, Prof. Tiefeng Liu, Prof. Ya You","doi":"10.1002/batt.202400778","DOIUrl":"10.1002/batt.202400778","url":null,"abstract":"<p>Raising the upper cut-off voltage of cathode is an effective method to improve the energy density of sodium-ion batteries (SIBs). However, the high upper cut-off voltage could cause severe side reactions and injure the cycle life of SIBs as the absence of stable cathode-electrolyte interface. Some fluorinated co-solvents have been ever employed and proven effective in stabilizing the cathode-electrolyte interface to support the normal operation of SIBs under a high upper cut-off voltage. However, the high-cost of fluorinated co-solvents would notably improve battery expenses. In this study, a low-cost co-solvent called ethyl methylsulfone (EMS) is introduced into the electrolyte for the Na<sub>0.67</sub>Mn<sub>0.8</sub>Cu<sub>0.2</sub>O<sub>2</sub> cathode with a high upper cut-off voltage of 4.5 V. It is found that a stable and uniform cathode-electrolyte interface (CEI) forms on the cathode, which mitigates the cathode degradation and enhances the cycling stability of cathode. Consequently, this cathode with the designed electrolyte achieves a high capacity retention of 83.2 % after 750 cycles at a current density of 1 C (1 C=110 mAh g<sup>−1</sup>). This work provides valuable insights into the development of electrolytes for sodium-ion batteries working at high-voltage.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144811249","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}
Kun Rui, Ke Chen, Yakai Chen, Wenhao Si, Jiliang Liu, Yan Yan, Huijuan Lin, Cong Zhao, Jixin Zhu
{"title":"Synergy in Commercial Brass Reinforced Carbon Hybrids Interlayer towards Highly Reversible Zn Anodes","authors":"Kun Rui, Ke Chen, Yakai Chen, Wenhao Si, Jiliang Liu, Yan Yan, Huijuan Lin, Cong Zhao, Jixin Zhu","doi":"10.1002/batt.202400792","DOIUrl":"10.1002/batt.202400792","url":null,"abstract":"<p>Aqueous Zn-ion batteries (AZIBs) have served as a promising candidate for next-generation energy storage applications. Nonetheless, interfacial issues concerning the metallic Zn anode including hydrogen evolution reaction (HER), chemical corrosion, and dendrite growth remain to be carefully addressed. Herein, we present a facile and cost-effective strategy to implant carbon nanotube (CNT) framework with a commercial brass alloy as the protective interlayer. The conductive network constructed by interconnected CNTs ensures an optimal electric field distribution over the entire electrode surface. The embedded brass alloy not only inhibits the aggregation of CNTs, but also mitigates surface corrosion through its abundance of chemically inert Cu sites. Leveraging the synergy within the carbon hybrids featuring high Zn-affinity and abundant nucleation sites for Zn<sup>2+</sup>, lowered energy barriers and promoted redox kinetics for Zn deposition enable highly stabilized and reversible Zn anodes. As a result, symmetric cells demonstrate extended cycling lifespan of 3000 h and 1200 h at 2 mA cm<sup>−2</sup> and 5 mA cm<sup>−2</sup> for 1 mAh cm<sup>−2</sup>, respectively. Furthermore, the optimized Zn||MnO<sub>2</sub> full cells exhibit impressive cycling stability for 1000 cycles at 2 A g<sup>−1</sup>.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 8","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144811291","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}