Yuting Gao, Jie Li, Youchen Hao, Yao Huang, Weiwei Zha, Xiaoliang Zhou, Yinzhu Jiang
Manganese-based Prussian blue analog (MnPBA) shows great potential as a high energy density and low-cost cathode material for sodium-ion batteries (SIBs) due to its electrochemical activity, high redox potential, low-cost raw materials, and facile synthesis. However, its practical application is severely challenged by the high water content (>10 wt%) in the framework and the Jahn–Teller effect from high-spin Mn3+, leading to poor reversibility and rapid capacity decay during cycling. Herein, Cu-substituted MnPBA samples (CuMnPBAs) are successfully synthesized under high-concentration chelation conditions, which reduced the water content and alleviated the Jahn–Teller effect from Mn3+. Accordingly, the optimal 25% Cu-substituted MnPBA (CuMnPBA-25) exhibits a significantly reduced water content of 7.6% and excellent cyclability, maintaining 81.2 mAh g−1 at 1 C after 700 cycles. Furthermore, the CuMnPBA-25/hard carbon (HC) pouch cell exhibits superb capacity retention of 80.9% after 280 cycles. This research provides new insights into the development of highly stable PBAs for practical applications in SIBs.
锰基普鲁士蓝类似物(MnPBA)具有电化学活性高、氧化还原电位高、原料成本低、易于合成等优点,具有作为钠离子电池(sib)正极材料的巨大潜力。然而,其实际应用受到框架中高含水量(>10 wt%)和高自旋Mn3+的Jahn-Teller效应的严重挑战,导致可逆性差,循环过程中容量衰减快。本文在高浓度螯合条件下成功合成了cu取代MnPBA样品(CuMnPBAs),降低了水含量,减轻了Mn3+的Jahn-Teller效应。因此,最佳的25% cu取代MnPBA (CuMnPBA-25)具有显著降低7.6%的含水量和优异的循环性能,在1℃下循环700次后保持81.2 mAh g−1。此外,CuMnPBA-25/硬碳(HC)袋状电池在280次循环后的容量保持率为80.9%。该研究为sib中实际应用的高稳定PBAs的开发提供了新的见解。
{"title":"Boosting the Cycling Stability of Manganese Prussian Blue Analogs by Cu-Substitution and Water Reduction for Sodium-Ion Batteries","authors":"Yuting Gao, Jie Li, Youchen Hao, Yao Huang, Weiwei Zha, Xiaoliang Zhou, Yinzhu Jiang","doi":"10.1002/batt.202500216","DOIUrl":"https://doi.org/10.1002/batt.202500216","url":null,"abstract":"<p>Manganese-based Prussian blue analog (MnPBA) shows great potential as a high energy density and low-cost cathode material for sodium-ion batteries (SIBs) due to its electrochemical activity, high redox potential, low-cost raw materials, and facile synthesis. However, its practical application is severely challenged by the high water content (>10 wt%) in the framework and the Jahn–Teller effect from high-spin Mn<sup>3+</sup>, leading to poor reversibility and rapid capacity decay during cycling. Herein, Cu-substituted MnPBA samples (CuMnPBAs) are successfully synthesized under high-concentration chelation conditions, which reduced the water content and alleviated the Jahn–Teller effect from Mn<sup>3+</sup>. Accordingly, the optimal 25% Cu-substituted MnPBA (CuMnPBA-25) exhibits a significantly reduced water content of 7.6% and excellent cyclability, maintaining 81.2 mAh g<sup>−1</sup> at 1 C after 700 cycles. Furthermore, the CuMnPBA-25/hard carbon (HC) pouch cell exhibits superb capacity retention of 80.9% after 280 cycles. This research provides new insights into the development of highly stable PBAs for practical applications in SIBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533627","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}
Lithium-ion batteries (LIBs) have drawn significant attention in the electric vehicle industry, and activated carbon-based anodes are widely recognized as a cost-effective alternative to conventional anode materials. However, the application of these anode materials is significantly limited by the formation of an unstable solid–electrolyte interface (SEI). This study introduces nutmeg shell waste-derived activated carbon (ACNM) as a viable anode material for LIBs with a particular focus on the role of SEI in determining their electrochemical behavior and battery performance. The hierarchical pore structure in ACNM is achieved through systematic optimization of synthesis parameters, ensuring a balance between surface area and the stability of the SEI. The combination of micropores and mesopores in ACNM effectively minimizes extensive SEI formation and associated capacity loss. The potential of ACNM for LIB anode applications is validated by fabricating anode half cells that exhibit a maximum specific capacity of 610 mAh g−1. The half cells also show good cycling performance with significant rate capability. Using scanning electrochemical microscopy, the local electrochemical activity and formation of the SEI layer are investigated. This study highlights the suitability of ACNM for anode applications in LIBs and the importance of SEI engineering for next-generation LIBs.
锂离子电池(LIBs)在电动汽车行业受到了广泛的关注,活性炭基阳极被广泛认为是一种具有成本效益的替代传统阳极材料。然而,这些阳极材料的应用受到不稳定固体-电解质界面(SEI)形成的严重限制。本研究介绍了肉豆蔻壳废弃物衍生活性炭(ACNM)作为锂离子电池的可行阳极材料,并特别关注SEI在确定其电化学行为和电池性能方面的作用。ACNM中的分层孔结构是通过系统优化合成参数实现的,保证了表面面积和SEI稳定性之间的平衡。ACNM中微孔和介孔的结合有效地减少了大面积SEI的形成和相关的产能损失。ACNM在锂电池阳极应用的潜力通过制造最大比容量为610 mAh g−1的阳极半电池得到验证。半电池也表现出良好的循环性能和显著的速率能力。利用扫描电化学显微镜研究了SEI层的局部电化学活性和形成过程。这项研究强调了ACNM在锂离子电池阳极应用中的适用性,以及SEI工程对下一代锂离子电池的重要性。
{"title":"Impact of the Stable Solid–Electrolyte Interphase in Sustainable and High-Performance Lithium-Ion Battery Anodes","authors":"Merin Pulikkottil, Rakhi Raghavan Baby, Seema Ansari","doi":"10.1002/batt.202500228","DOIUrl":"https://doi.org/10.1002/batt.202500228","url":null,"abstract":"<p>Lithium-ion batteries (LIBs) have drawn significant attention in the electric vehicle industry, and activated carbon-based anodes are widely recognized as a cost-effective alternative to conventional anode materials. However, the application of these anode materials is significantly limited by the formation of an unstable solid–electrolyte interface (SEI). This study introduces nutmeg shell waste-derived activated carbon (ACNM) as a viable anode material for LIBs with a particular focus on the role of SEI in determining their electrochemical behavior and battery performance. The hierarchical pore structure in ACNM is achieved through systematic optimization of synthesis parameters, ensuring a balance between surface area and the stability of the SEI. The combination of micropores and mesopores in ACNM effectively minimizes extensive SEI formation and associated capacity loss. The potential of ACNM for LIB anode applications is validated by fabricating anode half cells that exhibit a maximum specific capacity of 610 mAh g<sup>−1</sup>. The half cells also show good cycling performance with significant rate capability. Using scanning electrochemical microscopy, the local electrochemical activity and formation of the SEI layer are investigated. This study highlights the suitability of ACNM for anode applications in LIBs and the importance of SEI engineering for next-generation LIBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533558","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}
Garnet-type Li6.4La3Zr1.4Ta0.6O12 solid-state electrolytes (SSEs) have attracted considerable attention for solid-state lithium metal batteries (SSLMBs) due to their high ionic conductivity, wide electrochemical window, and excellent stability towards lithium. However, poor interfacial contact hinders charge transport and increases impedance. Herein, introducing only 1.0 wt% BiBr3 into molten lithium at 280 °C in situ forms a mixed ion–electronic conductor (MIEC) of Li3Bi and LiBr, significantly enhancing wettability. Thanks to its uniqueness, the modified symmetric cell achieves a remarkably low interfacial resistance (15.7 Ω cm2) compared to pristine lithium (1280.3 Ω cm2). Furthermore, lithiophilic Li3Bi with high ionic conductivity improves the interfacial adhesion and regulates the Li nucleation. Meanwhile, the lithiophobic LiBr, with high interfacial energy against Li, enables effective suppression of the growth of Li dendrites by promoting the lateral growth of deposited Li metal. Therefore, it achieves a high critical current density (1.4 mA cm−2) and stable cycling over 1100 h, at 0.1 mA cm−2 at room temperature. When paired with a LiFePO4 cathode, the cell retains 91.6% of its initial capacity after 300 cycles at 0.5 C, demonstrating excellent cycling stability. These findings suggest that the incorporation of 1.0 wt% BiBr3 effectively constructs a superlithiophilic interface on garnet electrolyte, offering a simple and effective strategy for high-performance SSLMBs.
石榴石型Li6.4La3Zr1.4Ta0.6O12固态电解质(sse)因其高离子电导率、宽电化学窗口和优异的锂稳定性而受到固态锂金属电池(sslmb)的广泛关注。然而,不良的界面接触阻碍了电荷传输并增加了阻抗。在280°C的温度下,将1.0 wt%的BiBr3原位引入熔融锂中,形成Li3Bi和LiBr的混合离子电子导体(MIEC),显著提高了润湿性。由于其独特性,与原始锂(1280.3 Ω cm2)相比,改进的对称电池具有非常低的界面电阻(15.7 Ω cm2)。此外,具有高离子电导率的亲锂性Li3Bi提高了界面附着力,调控了锂的成核。同时,疏锂的LiBr对锂具有较高的界面能,通过促进沉积的锂金属的横向生长,有效抑制了锂枝晶的生长。因此,它实现了高临界电流密度(1.4 mA cm - 2)和稳定循环超过1100小时,在0.1 mA cm - 2室温下。当与LiFePO4阴极配对时,电池在0.5 C下循环300次后仍保持其初始容量的91.6%,表现出出色的循环稳定性。这些发现表明,1.0 wt% BiBr3的加入有效地在石榴石电解质上构建了一个超亲锂界面,为高性能sslmb提供了一种简单有效的策略。
{"title":"Less is More: 1.0 wt% BiBr3 Enabled a Superlithiophlic Interface on Garnet for Solid-State Batteries","authors":"Jiaoli Peng, Zhipeng Wang, Wei Gong, Hongquan Song, Mingpeng Yu","doi":"10.1002/batt.202500240","DOIUrl":"https://doi.org/10.1002/batt.202500240","url":null,"abstract":"<p>Garnet-type Li<sub>6.4</sub>La<sub>3</sub>Zr<sub>1.4</sub>Ta<sub>0.6</sub>O<sub>12</sub> solid-state electrolytes (SSEs) have attracted considerable attention for solid-state lithium metal batteries (SSLMBs) due to their high ionic conductivity, wide electrochemical window, and excellent stability towards lithium. However, poor interfacial contact hinders charge transport and increases impedance. Herein, introducing only 1.0 wt% BiBr<sub>3</sub> into molten lithium at 280 °C in situ forms a mixed ion–electronic conductor (MIEC) of Li<sub>3</sub>Bi and LiBr, significantly enhancing wettability. Thanks to its uniqueness, the modified symmetric cell achieves a remarkably low interfacial resistance (15.7 Ω cm<sup>2</sup>) compared to pristine lithium (1280.3 Ω cm<sup>2</sup>). Furthermore, lithiophilic Li<sub>3</sub>Bi with high ionic conductivity improves the interfacial adhesion and regulates the Li nucleation. Meanwhile, the lithiophobic LiBr, with high interfacial energy against Li, enables effective suppression of the growth of Li dendrites by promoting the lateral growth of deposited Li metal. Therefore, it achieves a high critical current density (1.4 mA cm<sup>−2</sup>) and stable cycling over 1100 h, at 0.1 mA cm<sup>−2</sup> at room temperature. When paired with a LiFePO<sub>4</sub> cathode, the cell retains 91.6% of its initial capacity after 300 cycles at 0.5 C, demonstrating excellent cycling stability. These findings suggest that the incorporation of 1.0 wt% BiBr<sub>3</sub> effectively constructs a superlithiophilic interface on garnet electrolyte, offering a simple and effective strategy for high-performance SSLMBs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533554","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}
Young-Hoon Lee, Hyeonjun An, Eunbin Park, Yung-Eun Sung, Seung-Ho Yu
There has been growing interest in aqueous batteries, which are considered safer and more cost-effective compared to Li-ion batteries. Among them, aqueous Sn-ion batteries have emerged as promising alternatives because of their high specific capacity and wide voltage window. Despite these numerous advantages, in aqueous-based electrolytes, significant variations in metal growth behavior with temperature lead to severe performance degradation, necessitating a fundamental investigation into the underlying mechanisms to develop high-performance aqueous batteries capable of operating across a wide temperature range. Therefore, this study for the first time examines the temperature-dependent Sn metal plating and stripping behavior in aqueous Sn-ion batteries. The results indicate that, at low temperatures, uneven pits are formed during stripping, leading to a rough and nonuniform surface. These pits serve as nucleation sites for deposition during plating, further exacerbating surface irregularities. In contrast, at high temperatures, stripping occurs uniformly along the grain boundaries and grain surfaces, resulting in a smooth and homogeneous surface. Similarly, plating under high-temperature conditions leads to uniform Sn deposition. In contrast, the corrosion tests reveal that pits form on the electrode surface under high-temperature conditions, leading to deterioration. These findings are expected to contribute to the development of high-performance aqueous Sn-ion batteries.
{"title":"Temperature-Dependent Morphological Evolution of Sn Metal Anode for Aqueous Sn-Ion Batteries","authors":"Young-Hoon Lee, Hyeonjun An, Eunbin Park, Yung-Eun Sung, Seung-Ho Yu","doi":"10.1002/batt.202500230","DOIUrl":"https://doi.org/10.1002/batt.202500230","url":null,"abstract":"<p>There has been growing interest in aqueous batteries, which are considered safer and more cost-effective compared to Li-ion batteries. Among them, aqueous Sn-ion batteries have emerged as promising alternatives because of their high specific capacity and wide voltage window. Despite these numerous advantages, in aqueous-based electrolytes, significant variations in metal growth behavior with temperature lead to severe performance degradation, necessitating a fundamental investigation into the underlying mechanisms to develop high-performance aqueous batteries capable of operating across a wide temperature range. Therefore, this study for the first time examines the temperature-dependent Sn metal plating and stripping behavior in aqueous Sn-ion batteries. The results indicate that, at low temperatures, uneven pits are formed during stripping, leading to a rough and nonuniform surface. These pits serve as nucleation sites for deposition during plating, further exacerbating surface irregularities. In contrast, at high temperatures, stripping occurs uniformly along the grain boundaries and grain surfaces, resulting in a smooth and homogeneous surface. Similarly, plating under high-temperature conditions leads to uniform Sn deposition. In contrast, the corrosion tests reveal that pits form on the electrode surface under high-temperature conditions, leading to deterioration. These findings are expected to contribute to the development of high-performance aqueous Sn-ion batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500230","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533675","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}
Ha Young Ko, Jesik Park, Joo Young Lee, Yong Joon Park
All-solid-state batteries (ASSBs) with sulfide electrolytes are promising for next-generation battery systems owing to their superior safety and favorable electrochemical properties. However, interfacial instability between the oxide cathode and sulfide electrolyte induces undesirable side reactions, degrading cell performance. This study develops a sulfurized LiNbO3 coating to stabilize this interface. While conventional LiNbO3 coatings reduce interfacial side reactions, their limited compatibility with sulfide electrolytes, due to Li-ion chemical potential differences, hinders ion transport. The sulfurized LiNbO3 coating improves compatibility, acting as a buffer that reduces the Li-ion potential gradient and enhances interfacial conductivity. The coating effectively suppresses side reactions, lowering cathode degradation and interfacial resistance. A simple and cost-effective sulfur treatment process is used, where sulfur sublimation at 300 °C forms a sulfurized outer layer on the coating. Electrochemical evaluations of the coating reveal significant capacity, rate capability, and cyclic performance improvements over conventional LiNbO3 coatings. These findings underscore sulfur treatment as an effective method for stabilizing interfaces and enabling smooth Li-ion transport, highlighting the advantages of the sulfurized LiNbO3 coating method. Overall, sulfurized LiNbO3 coatings offer scalable solutions to interfacial challenges in sulfide-based ASSBs, thereby promoting improved performance and commercialization of solid-state battery systems.
{"title":"Modification of Cathode Surface for Sulfide Electrolyte-Based All-Solid-State Batteries Using Sulfurized LiNbO3 Coating","authors":"Ha Young Ko, Jesik Park, Joo Young Lee, Yong Joon Park","doi":"10.1002/batt.202500188","DOIUrl":"https://doi.org/10.1002/batt.202500188","url":null,"abstract":"<p>All-solid-state batteries (ASSBs) with sulfide electrolytes are promising for next-generation battery systems owing to their superior safety and favorable electrochemical properties. However, interfacial instability between the oxide cathode and sulfide electrolyte induces undesirable side reactions, degrading cell performance. This study develops a sulfurized LiNbO<sub>3</sub> coating to stabilize this interface. While conventional LiNbO<sub>3</sub> coatings reduce interfacial side reactions, their limited compatibility with sulfide electrolytes, due to Li-ion chemical potential differences, hinders ion transport. The sulfurized LiNbO<sub>3</sub> coating improves compatibility, acting as a buffer that reduces the Li-ion potential gradient and enhances interfacial conductivity. The coating effectively suppresses side reactions, lowering cathode degradation and interfacial resistance. A simple and cost-effective sulfur treatment process is used, where sulfur sublimation at 300 °C forms a sulfurized outer layer on the coating. Electrochemical evaluations of the coating reveal significant capacity, rate capability, and cyclic performance improvements over conventional LiNbO<sub>3</sub> coatings. These findings underscore sulfur treatment as an effective method for stabilizing interfaces and enabling smooth Li-ion transport, highlighting the advantages of the sulfurized LiNbO<sub>3</sub> coating method. Overall, sulfurized LiNbO<sub>3</sub> coatings offer scalable solutions to interfacial challenges in sulfide-based ASSBs, thereby promoting improved performance and commercialization of solid-state battery systems.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533673","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}
Tommi Hendrik Aalto, Roham Talei, Kathrin Küster, Guido Schmitz, Oliver Clemens
In this study, conductive, fluorine and antimony codoped tin oxide nanoparticles (FATO-NPs) are highlighted as a possible alternative for conductive carbon additives in fluoride ion batteries, successfully circumventing oxidative side reactions. Since good cyclability with high and stable discharge capacities is achieved with both types of conductive additive at a high stack pressure of 180 MPa, it is concluded that conductive carbon is well-suited for high-voltage fluoride ion batteries, contrary to prior assumptions. However, FATO-NP-based cathodes outperform those based on conductive carbon at lower stack pressures of 50 MPa, emphasizing the importance of avoiding carbon fluorination at low stack pressures.
{"title":"Toward Carbon-Free Cathodes for Fluoride Ion Batteries: Deconvoluting Effects of Active Material and Conductive Additive on Charging and Cyclic Stability","authors":"Tommi Hendrik Aalto, Roham Talei, Kathrin Küster, Guido Schmitz, Oliver Clemens","doi":"10.1002/batt.202500195","DOIUrl":"https://doi.org/10.1002/batt.202500195","url":null,"abstract":"<p>In this study, conductive, fluorine and antimony codoped tin oxide nanoparticles (FATO-NPs) are highlighted as a possible alternative for conductive carbon additives in fluoride ion batteries, successfully circumventing oxidative side reactions. Since good cyclability with high and stable discharge capacities is achieved with both types of conductive additive at a high stack pressure of 180 MPa, it is concluded that conductive carbon is well-suited for high-voltage fluoride ion batteries, contrary to prior assumptions. However, FATO-NP-based cathodes outperform those based on conductive carbon at lower stack pressures of 50 MPa, emphasizing the importance of avoiding carbon fluorination at low stack pressures.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500195","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533757","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}
Li–CO2/O2 batteries hold tremendous promises for energy storage and conversion systems, attributed to their high theoretical energy density and economic viability. Nevertheless, their widespread application is hindered by high overpotential and compromised cycling stability. Herein, ruthenium (Ru)-doped copper-based metal organic frameworks (HKUST) octahedral particles (Ru@HKUST) are synthesized as the cathode catalyst for Li–CO2/O2 batteries. The Ru@HKUST matrix rich in free channels provides unimpeded gas permeation and substantial adsorption spaces for CO2/O2. A synergistic interaction between HKUST and Ru significantly enhances the kinetic conversion of Li2CO3 upon cycles, thereby markedly boosting the capacity and extending the cycle life of Li–CO2/O2 batteries. A high discharge capacity of 19 437 mAh g−1 is achieved at 2 V cutoff voltage in the Li–CO2/O2 cell with Ru@HKUST under a constant current density of 200 mA g−1. The cells exhibit a superior catalytic efficiency with reduced charge plateaus of 4.1 V for over 100 cycles at a fixed capacity of 1000 mAh g−1, demonstrating excellent electrochemical properties and paving the way for advanced battery technology.
Li-CO2 /O2电池由于其高理论能量密度和经济可行性,在能量存储和转换系统方面有着巨大的前景。然而,它们的广泛应用受到高过电位和破坏循环稳定性的阻碍。本文合成了钌(Ru)掺杂铜基金属有机骨架(HKUST)八面体粒子(Ru@HKUST)作为Li-CO2 /O2电池的阴极催化剂。富含自由通道的Ru@HKUST基质为CO2/O2提供了畅通的气体渗透和大量的吸附空间。科大与Ru之间的协同作用显著提高了Li2CO3在循环时的动力学转化,从而显著提高了Li-CO2 /O2电池的容量和延长了循环寿命。在200 mA g−1的恒流密度下,在2 V的截止电压下,在含有Ru@HKUST的Li-CO2 /O2电池中获得了19 437 mAh g−1的高放电容量。在1000 mAh g - 1的固定容量下,该电池表现出了卓越的催化效率,在100次循环中降低了4.1 V的充电平台,展示了优异的电化学性能,为先进的电池技术铺平了道路。
{"title":"Promoting the Energy Conversion of Li–CO2/O2 Batteries via Ru-Doped HKUST with Substantial Adsorption and Excellent Catalytic Effect","authors":"Ke Li, Ningning Zhu, Xueqi Tan, Xuechun Li, Yifan Xu, Enyi Zhang, Ziqiang Bi, Jou-Hyeon Ahn, Sheng Ju, Xiaohui Zhao","doi":"10.1002/batt.202500296","DOIUrl":"https://doi.org/10.1002/batt.202500296","url":null,"abstract":"<p>Li–CO<sub>2</sub>/O<sub>2</sub> batteries hold tremendous promises for energy storage and conversion systems, attributed to their high theoretical energy density and economic viability. Nevertheless, their widespread application is hindered by high overpotential and compromised cycling stability. Herein, ruthenium (Ru)-doped copper-based metal organic frameworks (HKUST) octahedral particles (Ru@HKUST) are synthesized as the cathode catalyst for Li–CO<sub>2</sub>/O<sub>2</sub> batteries. The Ru@HKUST matrix rich in free channels provides unimpeded gas permeation and substantial adsorption spaces for CO<sub>2</sub>/O<sub>2</sub>. A synergistic interaction between HKUST and Ru significantly enhances the kinetic conversion of Li<sub>2</sub>CO<sub>3</sub> upon cycles, thereby markedly boosting the capacity and extending the cycle life of Li–CO<sub>2</sub>/O<sub>2</sub> batteries. A high discharge capacity of 19 437 mAh g<sup>−1</sup> is achieved at 2 V cutoff voltage in the Li–CO<sub>2</sub>/O<sub>2</sub> cell with Ru@HKUST under a constant current density of 200 mA g<sup>−1</sup>. The cells exhibit a superior catalytic efficiency with reduced charge plateaus of 4.1 V for over 100 cycles at a fixed capacity of 1000 mAh g<sup>−1</sup>, demonstrating excellent electrochemical properties and paving the way for advanced battery technology.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533668","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}
Shungui Deng, Mohammad Jafarpour, Frank Nüesch, Chuanfang Zhang, Jakob Heier
In the pursuit of durable lithium–sulfur (Li–S) batteries, considerable research has been devoted to extending cycle life by developing advanced cathode materials. However, there exists a common overcharging problem which leads to the disfunction of Li–S batteries but has been largely overlooked. This study systematically investigates the overcharging failure and its underlying mechanisms. Experimental results reveal that failure comes from a soft internal short circuit (ISCs) caused by excessive lithium dendrite growth, primarily driven by the sulfur cathode rather than the lithium anode. Electrochemical processes during overcharging are examined, revealing the generation of a specific by-product. By analyzing the structural properties of the sulfur cathode such as topography and pore connectivity, and through combined experiments and theoretical simulations, the complex mechanisms through which the cathode influences lithium dendrite growth are elucidated. Finally, an effective "interlayer" strategy is proposed to mitigate the overcharging failure. This work sheds light on the overcharging mechanisms and emphasizes the critical importance of cathode design in improving the safety and reliability of Li–S batteries.
{"title":"Insights into the Overcharge-Induced Failure Mechanism of Lithium–Sulfur Batteries","authors":"Shungui Deng, Mohammad Jafarpour, Frank Nüesch, Chuanfang Zhang, Jakob Heier","doi":"10.1002/batt.202500350","DOIUrl":"https://doi.org/10.1002/batt.202500350","url":null,"abstract":"<p>In the pursuit of durable lithium–sulfur (Li–S) batteries, considerable research has been devoted to extending cycle life by developing advanced cathode materials. However, there exists a common overcharging problem which leads to the disfunction of Li–S batteries but has been largely overlooked. This study systematically investigates the overcharging failure and its underlying mechanisms. Experimental results reveal that failure comes from a soft internal short circuit (ISCs) caused by excessive lithium dendrite growth, primarily driven by the sulfur cathode rather than the lithium anode. Electrochemical processes during overcharging are examined, revealing the generation of a specific by-product. By analyzing the structural properties of the sulfur cathode such as topography and pore connectivity, and through combined experiments and theoretical simulations, the complex mechanisms through which the cathode influences lithium dendrite growth are elucidated. Finally, an effective \"interlayer\" strategy is proposed to mitigate the overcharging failure. This work sheds light on the overcharging mechanisms and emphasizes the critical importance of cathode design in improving the safety and reliability of Li–S batteries.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500350","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533373","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}
Li Tao, Chun Li, Xuejun Lu, Rameez Ahmad Mir, Nieves López-Salas, Jian Liu
Aqueous zinc (Zn)-ion capacitors (AZICs) have addressed considerable attention due to their high energy density, low toxicity, and rich abundance of Zn metal. However, the development of ultra-long cycle life and high energy density AZICs is often hindered by the lack of adequately optimized active carbon (AC) electrodes and compatible electrolytes. Herein, high-performance, free-standing AC electrodes for AZICs are derived from sustainable precursors—adenine and D-ribose—using magnesium chloride hexahydrate as an activation agent via a eutectic template strategy. Furthermore, an aqueous hybrid electrolyte tailored to the designed AC electrodes is developed, significantly enhancing the stability and cycle life of AZICs. The resulting AZIC achieves a high specific capacity of 164.39 F g−1 at 0.1 A g−1 and a magnificently long cell life of over 50 000 cycles with nearly 94.5% capacitance retention at 10 000th cycles, and 76.3% at 50 000th cycle. The pouch cell assembly also demonstrates comparable specific capacitance and energy density to the coin cell, underscoring the potential of large-scale applications of AZICs.
含水锌离子电容器(AZICs)因其高能量密度、低毒性和丰富的锌金属丰度而受到广泛关注。然而,超长循环寿命和高能量密度azic的发展往往受到缺乏充分优化的活性炭(AC)电极和兼容电解质的阻碍。本文采用共晶模板策略,采用六水氯化镁作为活化剂,从可持续前体腺嘌呤和d -核苷酸中获得高性能、独立的azic交流电极。此外,针对所设计的交流电极开发了一种适合的水混合电解质,显著提高了azic的稳定性和循环寿命。得到的AZIC在0.1 ag−1下的比容量达到164.39 F g−1,电池寿命超过5万次,在1万次循环时电容保持率接近94.5%,在5万次循环时电容保持率为76.3%。袋状电池组件也显示出与硬币电池相当的比电容和能量密度,强调了azic大规模应用的潜力。
{"title":"Adenine and D-Ribose Coderived Activated Carbon with N-Methyl-2-Pyrrolidone-Modified Aqueous Electrolyte for Long-Life Zinc-Ion Capacitors","authors":"Li Tao, Chun Li, Xuejun Lu, Rameez Ahmad Mir, Nieves López-Salas, Jian Liu","doi":"10.1002/batt.202500161","DOIUrl":"https://doi.org/10.1002/batt.202500161","url":null,"abstract":"<p>Aqueous zinc (Zn)-ion capacitors (AZICs) have addressed considerable attention due to their high energy density, low toxicity, and rich abundance of Zn metal. However, the development of ultra-long cycle life and high energy density AZICs is often hindered by the lack of adequately optimized active carbon (AC) electrodes and compatible electrolytes. Herein, high-performance, free-standing AC electrodes for AZICs are derived from sustainable precursors—adenine and D-ribose—using magnesium chloride hexahydrate as an activation agent via a eutectic template strategy. Furthermore, an aqueous hybrid electrolyte tailored to the designed AC electrodes is developed, significantly enhancing the stability and cycle life of AZICs. The resulting AZIC achieves a high specific capacity of 164.39 F g<sup>−1</sup> at 0.1 A g<sup>−1</sup> and a magnificently long cell life of over 50 000 cycles with nearly 94.5% capacitance retention at 10 000<sup>th</sup> cycles, and 76.3% at 50 000<sup>th</sup> cycle. The pouch cell assembly also demonstrates comparable specific capacitance and energy density to the coin cell, underscoring the potential of large-scale applications of AZICs.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533546","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}
This study examines the thermal, transport, and electrochemical properties of Rochelle salt (SPTa, KNaC4H4O6·4H2O) aqueous solutions for energy storage applications. SPTa exhibits eutectic melting (−38 °C), crystallization, density variations (e.g., 0.25 g cm−3 at 25 °C for 2.0 mol dm−3), and high ionic conductivity (70 mS cm−1 at 25 °C for 1.0 mol dm−3), which increases with temperature and concentration. Ionic transport follows the Arrhenius and Vogel–Fulcher–Tammann models, indicating low activation energies for ion mobility, especially below 8 °C. The Walden plot analysis suggests that most ions remain dissociated in the solution, while the thermodynamic parameters from the activated state of viscosity indicate strong chelation and molecular structuring effects. Cyclic voltammetry of symmetric supercapacitors with activated carbon electrodes in 1.0 mol dm−3 SPTa confirms double-layer capacitive behavior with a 2.5 V electrochemical window. Galvanostatic charge/discharge tests reveal an energy density of 35 Wh kg−1, excellent cycling stability (10 000 cycles), and high coulombic efficiency (>97%). Electrolyte evaporation and electrode degradation require further optimization for long-term stability. These findings highlight SPTa as a cost-effective and sustainable candidate for electrochemical energy storage.
本研究考察了罗谢尔盐(SPTa, KNaC4H4O6·4H2O)水溶液在储能应用中的热、输运和电化学性能。SPTa表现出共晶熔化(- 38°C)、结晶、密度变化(例如,在25°C下,2.0 mol dm - 3为0.25 g cm - 3)和高离子电导率(在25°C下,1.0 mol dm - 3为70 mS cm - 1),其随温度和浓度的增加而增加。离子传输遵循Arrhenius和Vogel-Fulcher-Tammann模型,表明离子迁移的活化能较低,特别是在8°C以下。Walden图分析表明,大多数离子在溶液中保持解离,而粘度激活状态的热力学参数表明有很强的螯合作用和分子结构效应。采用活性炭电极的对称超级电容器在1.0 mol dm−3 SPTa环境下的循环伏安法证实了其在2.5 V电化学窗口下的双层电容行为。恒流充放电测试显示能量密度为35 Wh kg - 1,具有优异的循环稳定性(10,000次循环)和高库仑效率(97%)。电解液蒸发和电极降解需要进一步优化长期稳定性。这些发现突出了SPTa作为一种具有成本效益和可持续性的电化学储能候选材料。
{"title":"Exploring Rochelle Salt Aqueous Solutions for Supercapacitors: Transport, Stability, and Performance","authors":"Hamza Kahri, Chalal Tachouaft, Yanzhuo Li, Ziwei Chen, Mérièm Anouti, Georgios Nikiforidis","doi":"10.1002/batt.202500259","DOIUrl":"https://doi.org/10.1002/batt.202500259","url":null,"abstract":"<p>This study examines the thermal, transport, and electrochemical properties of Rochelle salt (SPTa, KNaC<sub>4</sub>H<sub>4</sub>O<sub>6</sub>·4H<sub>2</sub>O) aqueous solutions for energy storage applications. SPTa exhibits eutectic melting (−38 °C), crystallization, density variations (e.g., 0.25 g cm<sup>−3</sup> at 25 °C for 2.0 mol dm<sup>−3</sup>), and high ionic conductivity (70 mS cm<sup>−1</sup> at 25 °C for 1.0 mol dm<sup>−3</sup>), which increases with temperature and concentration. Ionic transport follows the Arrhenius and Vogel–Fulcher–Tammann models, indicating low activation energies for ion mobility, especially below 8 °C. The Walden plot analysis suggests that most ions remain dissociated in the solution, while the thermodynamic parameters from the activated state of viscosity indicate strong chelation and molecular structuring effects. Cyclic voltammetry of symmetric supercapacitors with activated carbon electrodes in 1.0 mol dm<sup>−3</sup> SPTa confirms double-layer capacitive behavior with a 2.5 V electrochemical window. Galvanostatic charge/discharge tests reveal an energy density of 35 Wh kg<sup>−1</sup>, excellent cycling stability (10 000 cycles), and high coulombic efficiency (>97%). Electrolyte evaporation and electrode degradation require further optimization for long-term stability. These findings highlight SPTa as a cost-effective and sustainable candidate for electrochemical energy storage.</p>","PeriodicalId":132,"journal":{"name":"Batteries & Supercaps","volume":"8 11","pages":""},"PeriodicalIF":4.7,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://chemistry-europe.onlinelibrary.wiley.com/doi/epdf/10.1002/batt.202500259","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145533547","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}