Lithium carbonate, a solid discharge product, is closely associated with the discharge performance of oxygen-involved lithium-carbon dioxide batteries that exacerbates concentration polarization and electrode passivation. Although numerous strategies to enhance battery performance have progressed, the mechanistic understanding of lithium carbonate on oxygen-involved lithium-carbon dioxide batteries is still confusing. Herein, the effects of lithium carbonate over past decades are traced, including the lithium carbonate product morphology, reaction pathway, formation intermediate, and growth mechanism. The lithium carbonate nucleation and growth are crucial factors that influence battery performance. This perspective proposes a brand-new growth mechanism coupling of solution and surface mechanisms based on experimental results and theories, which extends the growth space of the product and enhances the discharge capacity. Developing advanced technologies are expected to reveal complex lithium carbonate formation pathways and spearhead advanced oxygen-involved lithium-carbon dioxide batteries.
{"title":"Mechanistic Understanding of the Solid Product in O2-Involved Li-CO2 Batteries","authors":"Aijing Yan, Xu Xiao, Zhuojun Zhang, Zehui Zhao, Yasen Hao, Tenghui Qiu, Peng Tan","doi":"10.1002/bte2.70001","DOIUrl":"https://doi.org/10.1002/bte2.70001","url":null,"abstract":"<p>Lithium carbonate, a solid discharge product, is closely associated with the discharge performance of oxygen-involved lithium-carbon dioxide batteries that exacerbates concentration polarization and electrode passivation. Although numerous strategies to enhance battery performance have progressed, the mechanistic understanding of lithium carbonate on oxygen-involved lithium-carbon dioxide batteries is still confusing. Herein, the effects of lithium carbonate over past decades are traced, including the lithium carbonate product morphology, reaction pathway, formation intermediate, and growth mechanism. The lithium carbonate nucleation and growth are crucial factors that influence battery performance. This perspective proposes a brand-new growth mechanism coupling of solution and surface mechanisms based on experimental results and theories, which extends the growth space of the product and enhances the discharge capacity. Developing advanced technologies are expected to reveal complex lithium carbonate formation pathways and spearhead advanced oxygen-involved lithium-carbon dioxide batteries.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.70001","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632665","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Giuseppe Pascuzzi, Sabrina Trano, Carlotta Francia, Stefano Turri, Federico Bella, Gianmarco Griffini
Potassium batteries are very appealing for stationary applications and domestic use, offering a promising alternative to lithium-ion systems. To improve their safety and environmental impact, gel polymer electrolytes (GPEs) based on bioderived materials can be employed. In this work, a series of biobased membranes are developed by crosslinking pre-oxidized Kraft lignin as bio-based component and poly(ethylene glycol) diglycidyl ether (PEGDGE) as functional linker with 200, 500, and 1000 g mol−1 molecular weight. The influence of PEGDGE chain length on the physicochemical properties and electrochemical performance of GPEs for potassium batteries is investigated. These membranes exhibit thermal stability above 240°C and tunable glass transition temperatures depending on the PEGDGE molecular weight. Their mechanical properties are determined by rheology measurements in dry and swollen states, evidencing a slight decrease of elastic modulus (G′) by increasing PEGDGE chain length. An approximately one-order-of-magnitude lower G′ value is observed in swollen membranes versus their dry counterpart. Upon successful activation of the lignin-based membranes by swelling in the liquid electrolyte embedding potassium salts, these GPEs are tested in potassium metal cell prototypes. These systems exhibit ionic conductivity of ~10−3 S cm−1 at ambient temperature. Interestingly, battery devices equipped with the GPE based on PEGDGE 1000 g mol−1 withstand current densities as high as 1.5 mA cm−2 during operation. Moreover, the same devices reach specific capacities of 130 mAh g‒1 at 0.05 A g−1 in the first 100 cycles and long-term operation for over 2500 cycles, representing outstanding achievements as bio-sourced systems for potassium batteries.
钾电池在固定应用和家庭使用中非常有吸引力,为锂离子系统提供了一个有前途的替代品。为了提高其安全性和环境影响,可以采用基于生物衍生材料的凝胶聚合物电解质(gpe)。在这项工作中,通过交联预氧化硫酸盐木质素作为生物基组分,聚乙二醇二甘油酯醚(PEGDGE)作为功能连接剂,开发了一系列生物基膜,分子量分别为200、500和1000 g mol−1。研究了PEGDGE链长对钾电池用gpe材料理化性能和电化学性能的影响。这些膜在240°C以上表现出热稳定性,并且根据PEGDGE分子量可调节玻璃化转变温度。它们的力学性能是通过在干燥和膨胀状态下的流变学测量来确定的,表明弹性模量(G ')随着PEGDGE链长度的增加而略有下降。与干燥膜相比,肿胀膜的G值大约低一个数量级。在木质素基膜通过溶胀在液体电解质中嵌入钾盐成功激活后,这些gpe在钾金属电池原型中进行了测试。这些体系在环境温度下的离子电导率为~10−3 S cm−1。有趣的是,配备基于PEGDGE 1000 g mol - 1的GPE的电池设备在工作期间可承受高达1.5 mA cm - 2的电流密度。此外,相同的装置在前100次循环中达到130 mAh g- 1的比容量,在0.05 A g- 1下长期运行超过2500次循环,代表了钾电池生物源系统的杰出成就。
{"title":"Elucidating the Interplay Between Structure and Electrochemical Behavior in Lignin-Based Polymer Electrolytes for Potassium Batteries","authors":"Giuseppe Pascuzzi, Sabrina Trano, Carlotta Francia, Stefano Turri, Federico Bella, Gianmarco Griffini","doi":"10.1002/bte2.70002","DOIUrl":"https://doi.org/10.1002/bte2.70002","url":null,"abstract":"<p>Potassium batteries are very appealing for stationary applications and domestic use, offering a promising alternative to lithium-ion systems. To improve their safety and environmental impact, gel polymer electrolytes (GPEs) based on bioderived materials can be employed. In this work, a series of biobased membranes are developed by crosslinking pre-oxidized Kraft lignin as bio-based component and poly(ethylene glycol) diglycidyl ether (PEGDGE) as functional linker with 200, 500, and 1000 g mol<sup>−1</sup> molecular weight. The influence of PEGDGE chain length on the physicochemical properties and electrochemical performance of GPEs for potassium batteries is investigated. These membranes exhibit thermal stability above 240°C and tunable glass transition temperatures depending on the PEGDGE molecular weight. Their mechanical properties are determined by rheology measurements in dry and swollen states, evidencing a slight decrease of elastic modulus (G′) by increasing PEGDGE chain length. An approximately one-order-of-magnitude lower G′ value is observed in swollen membranes versus their dry counterpart. Upon successful activation of the lignin-based membranes by swelling in the liquid electrolyte embedding potassium salts, these GPEs are tested in potassium metal cell prototypes. These systems exhibit ionic conductivity of ~10<sup>−3</sup> S cm<sup>−1</sup> at ambient temperature. Interestingly, battery devices equipped with the GPE based on PEGDGE 1000 g mol<sup>−1</sup> withstand current densities as high as 1.5 mA cm<sup>−2</sup> during operation. Moreover, the same devices reach specific capacities of 130 mAh g<sup>‒1</sup> at 0.05 A g<sup>−1</sup> in the first 100 cycles and long-term operation for over 2500 cycles, representing outstanding achievements as bio-sourced systems for potassium batteries.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.70002","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632667","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sodium-layered oxides are a promising category of cathodes for sodium-ion batteries with high energy densities. The solid-state method is the typical approach to synthesizing these oxides because of its simple procedure and low cost. Although the reaction conditions have usually been understated, the effect of reagents has often been overlooked. Thus, fundamental insight into the chemical reagents is required to perform well. Here we report in situ structural and electrochemical methods of studying the effect of using different reagents. The materials have a composite structure containing layered NaMnO2 and Li2MnO3 components, where oxygen anionic redox can be triggered at high voltage by forming Na–O–Li configurations. The samples synthesized via MnCO3-based precursors form the Li2MnO3 phase at evaluated temperature and perform better than those through MnO2-based precursors. This work demonstrates that the reagents also impact the structure and performance of sodium-layered oxides, which provides new insight into developing high-energy cathode material.
{"title":"The Synthesis Effects on the Performance of P2-Na0.6Li0.27Mn0.73O2 Cathode Material for Sodium-Ion Batteries","authors":"Cuihong Zeng, Ziqin Zhang, Jiming Peng, Jia Qiao, Qichang Pan, Fenghua Zheng, Youguo Huang, Hongqiang Wang, Qingyu Li, Sijiang Hu","doi":"10.1002/bte2.70000","DOIUrl":"https://doi.org/10.1002/bte2.70000","url":null,"abstract":"<p>Sodium-layered oxides are a promising category of cathodes for sodium-ion batteries with high energy densities. The solid-state method is the typical approach to synthesizing these oxides because of its simple procedure and low cost. Although the reaction conditions have usually been understated, the effect of reagents has often been overlooked. Thus, fundamental insight into the chemical reagents is required to perform well. Here we report in situ structural and electrochemical methods of studying the effect of using different reagents. The materials have a composite structure containing layered NaMnO<sub>2</sub> and Li<sub>2</sub>MnO<sub>3</sub> components, where oxygen anionic redox can be triggered at high voltage by forming Na–O–Li configurations. The samples synthesized via MnCO<sub>3</sub>-based precursors form the Li<sub>2</sub>MnO<sub>3</sub> phase at evaluated temperature and perform better than those through MnO<sub>2</sub>-based precursors. This work demonstrates that the reagents also impact the structure and performance of sodium-layered oxides, which provides new insight into developing high-energy cathode material.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.70000","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143632666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Murugavel Kathiresan, Abishek Kumar Lakshmi, Natarajan Angulakshmi, Sara Garcia-Ballesteros, Federico Bella, A. Manuel Stephan
Although lithium-ion batteries (LIBs) have found an unprecedented place among portable electronic devices owing to their attractive properties such as high energy density, single cell voltage, long shelf-life, etc., their application in electric vehicles still requires further improvements in terms of power density, better safety, and fast-charging ability (i.e., 15 min charging) for long driving range. The challenges of fast charging of LIBs have limitations such as low lithium-ion transport in the bulk and solid electrode/electrolyte interfaces, which are mainly influenced by the ionic conductivity of the electrolyte. Therefore, electrolyte engineering plays a key role in enhancing the fast-charging capability of LIBs. Here, we synthesize a novel propionic acid-based viologen that contains a 4,4′-bipyridinium unit and a terminal carboxylic acid group with positive charges that confine PF6‒ anions and accelerate the migration of lithium ions due to electrostatic repulsion, thus increasing the overall rate capability. The LiFePO4/Li cells with 0.25% of viologen added to the electrolyte show a discharge capacity of 110 mAh g‒1 at 6C with 95% of capacity retention even after 500 cycles. The added viologen not only enhances the electrochemical properties, but also significantly reduces the self-extinguishing time.
尽管锂离子电池(LIBs)凭借其高能量密度、单节电压、长保质期等吸引人的特性在便携式电子设备中占据了前所未有的地位,但其在电动汽车中的应用仍需要在功率密度、更好的安全性和长行驶里程的快速充电能力(即充电15分钟)方面进一步改进。锂离子电池快速充电的挑战在于锂离子在体积和固体电极/电解质界面中的低输运,这主要受电解质离子电导率的影响。因此,电解质工程对提高锂离子电池的快速充电能力起着至关重要的作用。在这里,我们合成了一种新的丙酸基紫胶,它含有一个4,4 ' -联吡啶单元和一个带正电荷的末端羧基,它限制了PF6 -阴离子,并由于静电排斥加速了锂离子的迁移,从而提高了整体的速率能力。在电解液中添加0.25%紫素的LiFePO4/Li电池在6C下的放电容量为110 mAh g-1,即使在500次循环后仍保持95%的容量。添加紫外光不仅提高了电化学性能,而且显著缩短了自熄时间。
{"title":"Viologen as an Electrolyte Additive for Extreme Fast Charging of Lithium-Ion Batteries","authors":"Murugavel Kathiresan, Abishek Kumar Lakshmi, Natarajan Angulakshmi, Sara Garcia-Ballesteros, Federico Bella, A. Manuel Stephan","doi":"10.1002/bte2.20240039","DOIUrl":"https://doi.org/10.1002/bte2.20240039","url":null,"abstract":"<p>Although lithium-ion batteries (LIBs) have found an unprecedented place among portable electronic devices owing to their attractive properties such as high energy density, single cell voltage, long shelf-life, etc., their application in electric vehicles still requires further improvements in terms of power density, better safety, and fast-charging ability (i.e., 15 min charging) for long driving range. The challenges of fast charging of LIBs have limitations such as low lithium-ion transport in the bulk and solid electrode/electrolyte interfaces, which are mainly influenced by the ionic conductivity of the electrolyte. Therefore, electrolyte engineering plays a key role in enhancing the fast-charging capability of LIBs. Here, we synthesize a novel propionic acid-based viologen that contains a 4,4′-bipyridinium unit and a terminal carboxylic acid group with positive charges that confine PF<sub>6</sub><sup>‒</sup> anions and accelerate the migration of lithium ions due to electrostatic repulsion, thus increasing the overall rate capability. The LiFePO<sub>4</sub>/Li cells with 0.25% of viologen added to the electrolyte show a discharge capacity of 110 mAh g<sup>‒1</sup> at 6C with 95% of capacity retention even after 500 cycles. The added viologen not only enhances the electrochemical properties, but also significantly reduces the self-extinguishing time.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240039","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145012937","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The increasing amounts of end-of-life lithium-ion batteries (EOL LIBs) require novel and safe solutions allowing for the minimisation of health and environmental hazards. Arguably, the best approach to the problem of EOL LIBs is recycling and recovery of the metals contained within the cells. This allows the diversion of the EOL battery cells from the environment and the recovery of precious metals that can be reused in the manufacturing of new products, allowing the reduction of the requirements of virgin materials from the mining industry. The most significant hindrance to the recycling process of EOL LIBs is their unstable chemical nature and significant safety hazards related to opening the air-tight casings. To minimise these issues, the end-of-life cells must be stabilised in one of the few available ways. This review aims at a comprehensive presentation of the studied chemical methods of EOL LIB cell discharge and stabilisation. The advantages and disadvantages of the method and its variations are discussed based on the literature published to date. The literature review found that a significant number of authors make use of chemical stabilisation techniques without proper comprehension of the associated risks. Many authors focus solely on the cheapest and fastest way to stop a cell from producing an electrical charge without extra thought given to the downstream recycling processes of safety hazards related to the proposed stabilisation method. Only a few studies highlighted the risks and problems associated with chemical stabilisation techniques.
{"title":"A Review of the Use of Chemical Stabilisation Methods for Lithium-Ion Batteries","authors":"Mark D. Williams-Wynn, Marcin H. Durski","doi":"10.1002/bte2.20240086","DOIUrl":"https://doi.org/10.1002/bte2.20240086","url":null,"abstract":"<p>The increasing amounts of end-of-life lithium-ion batteries (EOL LIBs) require novel and safe solutions allowing for the minimisation of health and environmental hazards. Arguably, the best approach to the problem of EOL LIBs is recycling and recovery of the metals contained within the cells. This allows the diversion of the EOL battery cells from the environment and the recovery of precious metals that can be reused in the manufacturing of new products, allowing the reduction of the requirements of virgin materials from the mining industry. The most significant hindrance to the recycling process of EOL LIBs is their unstable chemical nature and significant safety hazards related to opening the air-tight casings. To minimise these issues, the end-of-life cells must be stabilised in one of the few available ways. This review aims at a comprehensive presentation of the studied chemical methods of EOL LIB cell discharge and stabilisation. The advantages and disadvantages of the method and its variations are discussed based on the literature published to date. The literature review found that a significant number of authors make use of chemical stabilisation techniques without proper comprehension of the associated risks. Many authors focus solely on the cheapest and fastest way to stop a cell from producing an electrical charge without extra thought given to the downstream recycling processes of safety hazards related to the proposed stabilisation method. Only a few studies highlighted the risks and problems associated with chemical stabilisation techniques.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240086","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145012695","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Employing functional additives can facilitate the formation of stable solid electrolyte interphase (SEI), which has emerged as a promising strategy to improve the electrochemical properties of lithium metal batteries (LMBs). Typical SEI containing inorganic components, such as lithium fluoride (LiF) and lithium nitride (LiNxOy and Li3N), have been confirmed to construct an ideal SEI for LMBs. Here, we designed and synthesized a novel molecule named BTFN to act as an SEI-forming additive containing fluorine and nitro groups. The strong electron-withdrawing effect greatly reduces the lowest unoccupied molecular orbital (LUMO) energy, facilitating its preferential decomposition during the SEI-forming process. An SEI with rich LiF, LiNxOy, and Li3N forms after its preferential and complete decomposition, greatly enhancing stabilization and uniformity. The lifespan of symmetric LMBs with BTFN significantly increases more than 12 times under the same conditions; the Li/SPE/LFP full batteries cycle more than four times the contrast batteries with a capacity retention of 99.7%. This work provides some experiences and opinions for exploring complex SEI-forming additives.
{"title":"Ultrastable Gel Polymer Lithium Metal Batteries With Novel Nitro-Substituted Hexafluoride SEI-Forming Additive","authors":"Shuoning Zhang, Zichen Wang, Yinuo Yu, Shengyu Qin, Yunxiao Ren, Jiajun Chen, Jiale Liu, Lanying Zhang, Wei Hu, Huai Yang","doi":"10.1002/bte2.20240081","DOIUrl":"https://doi.org/10.1002/bte2.20240081","url":null,"abstract":"<p>Employing functional additives can facilitate the formation of stable solid electrolyte interphase (SEI), which has emerged as a promising strategy to improve the electrochemical properties of lithium metal batteries (LMBs). Typical SEI containing inorganic components, such as lithium fluoride (LiF) and lithium nitride (LiN<sub><i>x</i></sub>O<sub><i>y</i></sub> and Li<sub>3</sub>N), have been confirmed to construct an ideal SEI for LMBs. Here, we designed and synthesized a novel molecule named BTFN to act as an SEI-forming additive containing fluorine and nitro groups. The strong electron-withdrawing effect greatly reduces the lowest unoccupied molecular orbital (LUMO) energy, facilitating its preferential decomposition during the SEI-forming process. An SEI with rich LiF, LiN<sub><i>x</i></sub>O<sub><i>y</i></sub>, and Li<sub>3</sub>N forms after its preferential and complete decomposition, greatly enhancing stabilization and uniformity. The lifespan of symmetric LMBs with BTFN significantly increases more than 12 times under the same conditions; the Li/SPE/LFP full batteries cycle more than four times the contrast batteries with a capacity retention of 99.7%. This work provides some experiences and opinions for exploring complex SEI-forming additives.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240081","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145012068","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junyoung Heo, Hawon Gu, Changhee Lee, Junghwan Sung, Dong-Hee Kim, Jiye Han, Yeong-Seok Oh, Seongki Ahn, Il Jeon, Jun-Woo Park
Although lithium–sulfur batteries (LSBs) are promising next-generation secondary batteries, their mass commercialization has not yet been achieved primarily owing to critical issues such as the “shuttle effect” of soluble lithium polysulfides (LiPSs) and uncontrollable Li dendrite growth. Thus, most reviews on LSBs are focused on strategies for inhibiting shuttle behavior and achieving dendrite-free LSBs to improve the cycle life and Coulombic efficiency of LSBs. However, LSBs have various promising advantages, including an ultrahigh energy density (2600 Wh kg−1), cost-effectiveness, environmental friendliness, low weight, and flexible attributes, which suggest the feasibility of their current and near-future practical applications in fields that require these characteristics, irrespective of their moderate lifespan. Here, for the first time, challenges impeding the current and near-future applications of LSBs are comprehensively addressed. In particular, the latest progress and novel materials based on their electrochemical characteristics are summarized, with a focus on the gravimetric/volumetric energy density (capacity), loading mass and sulfur content in cathodes, electrolyte-to-sulfur ratios, rate capability, and maximization of these advantageous characteristics for applications in specific areas. Additionally, potential areas for practical applications of LSBs are suggested, with insights for improving LSB performances from a different standpoint and facilitating their integration into various application domains.
{"title":"Recent Advances in Achieving High Energy/Power Density of Lithium–Sulfur Batteries for Current and Near-Future Applications","authors":"Junyoung Heo, Hawon Gu, Changhee Lee, Junghwan Sung, Dong-Hee Kim, Jiye Han, Yeong-Seok Oh, Seongki Ahn, Il Jeon, Jun-Woo Park","doi":"10.1002/bte2.20240051","DOIUrl":"https://doi.org/10.1002/bte2.20240051","url":null,"abstract":"<p>Although lithium–sulfur batteries (LSBs) are promising next-generation secondary batteries, their mass commercialization has not yet been achieved primarily owing to critical issues such as the “shuttle effect” of soluble lithium polysulfides (LiPSs) and uncontrollable Li dendrite growth. Thus, most reviews on LSBs are focused on strategies for inhibiting shuttle behavior and achieving dendrite-free LSBs to improve the cycle life and Coulombic efficiency of LSBs. However, LSBs have various promising advantages, including an ultrahigh energy density (2600 Wh kg<sup>−1</sup>), cost-effectiveness, environmental friendliness, low weight, and flexible attributes, which suggest the feasibility of their current and near-future practical applications in fields that require these characteristics, irrespective of their moderate lifespan. Here, for the first time, challenges impeding the current and near-future applications of LSBs are comprehensively addressed. In particular, the latest progress and novel materials based on their electrochemical characteristics are summarized, with a focus on the gravimetric/volumetric energy density (capacity), loading mass and sulfur content in cathodes, electrolyte-to-sulfur ratios, rate capability, and maximization of these advantageous characteristics for applications in specific areas. Additionally, potential areas for practical applications of LSBs are suggested, with insights for improving LSB performances from a different standpoint and facilitating their integration into various application domains.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240051","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145012356","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sangjun Son, Jihong Kim, Sung Min Wi, Sungsan Kang, Younghyun Cho, Jong Bae Park, A-Rang Jang, Sangyeon Pak, Young-Woo Lee
Micro-supercapacitors (mSCs) have emerged as next-generation energy storage components suitable for portable, flexible, and eco-friendly electronic device system. In particular, electric double-layer (EDL) mSCs utilizing flexible graphene electrodes have gained significant attention due to their quick and efficient charge/discharge capabilities. Despite significant progress in fabricating mSCs, particularly through the development of laser-induced graphene (LIG) for creating 3D porous electrodes, challenges remain in increasing both energy and power densities. One promising strategy to address these challenges is the incorporation of pseudo-capacitive materials into the 3D graphene structure. However, conventional methods for embedding pseudo-capacitive materials often involve complex and additional labor-intensive steps to the manufacturing process. In this work, we introduce a high-speed mSC fabrication method (< 5 min) that employs a continuous laser-scribing process to directly integrate Mn2O3, a pseudo-capacitive material, onto LIG electrodes, forming hierarchical Mn2O3/LIG structure. By precisely controlling the fabrication parameter, this approach can significantly improve the electrochemical performance by optimizing the density and thickness of Mn2O3, leading to 550.5% increase in capacitance and energy density compared to the LIG electrode. Additionally, the mSCs exhibit outstanding cyclic (> 88% @ 20,000 cycles) and mechanical stability (@ bending radius of 5 mm), confirming their potential for seamless integration into electronic circuits. This innovation not only simplifies the production process of high-performance mSCs but also broadens their potential applications in sustainable and compact electronic device system.
{"title":"Hierarchically Assembled Mn2O3/Porous Graphene Electrodes Synthesized via High Speed and Continuous Laser-Scribing Strategy for High-Performance Microsupercapacitors","authors":"Sangjun Son, Jihong Kim, Sung Min Wi, Sungsan Kang, Younghyun Cho, Jong Bae Park, A-Rang Jang, Sangyeon Pak, Young-Woo Lee","doi":"10.1002/bte2.20240079","DOIUrl":"https://doi.org/10.1002/bte2.20240079","url":null,"abstract":"<p>Micro-supercapacitors (mSCs) have emerged as next-generation energy storage components suitable for portable, flexible, and eco-friendly electronic device system. In particular, electric double-layer (EDL) mSCs utilizing flexible graphene electrodes have gained significant attention due to their quick and efficient charge/discharge capabilities. Despite significant progress in fabricating mSCs, particularly through the development of laser-induced graphene (LIG) for creating 3D porous electrodes, challenges remain in increasing both energy and power densities. One promising strategy to address these challenges is the incorporation of pseudo-capacitive materials into the 3D graphene structure. However, conventional methods for embedding pseudo-capacitive materials often involve complex and additional labor-intensive steps to the manufacturing process. In this work, we introduce a high-speed mSC fabrication method (< 5 min) that employs a continuous laser-scribing process to directly integrate Mn<sub>2</sub>O<sub>3</sub>, a pseudo-capacitive material, onto LIG electrodes, forming hierarchical Mn<sub>2</sub>O<sub>3</sub>/LIG structure. By precisely controlling the fabrication parameter, this approach can significantly improve the electrochemical performance by optimizing the density and thickness of Mn<sub>2</sub>O<sub>3</sub>, leading to 550.5% increase in capacitance and energy density compared to the LIG electrode. Additionally, the mSCs exhibit outstanding cyclic (> 88% @ 20,000 cycles) and mechanical stability (@ bending radius of 5 mm), confirming their potential for seamless integration into electronic circuits. This innovation not only simplifies the production process of high-performance mSCs but also broadens their potential applications in sustainable and compact electronic device system.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240079","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145013101","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Norshahirah Mohamad Saidi, Muhammad Amirul Aizat Mohd Abdah, Muhammad Norhaffis Mustafa, Rashmi Walvekar, Mohammad Khalid, Ajit Khosla
Silicon (Si)-based materials have emerged as promising alternatives to graphite anodes in lithium-ion (Li-ion) batteries due to their exceptionally high theoretical capacity. However, their practical deployment remains constrained by challenges such as significant volume changes during lithiation, poor electrical conductivity, and the instability of the solid electrolyte interphase (SEI). This review critically examines recent advancements in Si-based nanostructures to enhance stability and electrochemical performance. Distinct from prior studies, it highlights the application of Si anodes in commercial domains, including electric vehicles, consumer electronics, and renewable energy storage systems, where prolonged cycle life and improved power density are crucial. Special emphasis is placed on emerging fabrication techniques, particularly scalable and cost-effective methods such as electrospinning and sol–gel processes, which show promise for industrial adoption. By addressing both the technical innovations and economic considerations surrounding Si anodes, this review provides a comprehensive roadmap for overcoming existing barriers, paving the way for next-generation, high-performance batteries.
{"title":"Advancements in Silicon Anodes for Enhanced Lithium-Ion Batteries Performance: Innovations Toward Next-Gen Superbatteries","authors":"Norshahirah Mohamad Saidi, Muhammad Amirul Aizat Mohd Abdah, Muhammad Norhaffis Mustafa, Rashmi Walvekar, Mohammad Khalid, Ajit Khosla","doi":"10.1002/bte2.20240048","DOIUrl":"https://doi.org/10.1002/bte2.20240048","url":null,"abstract":"<p>Silicon (Si)-based materials have emerged as promising alternatives to graphite anodes in lithium-ion (Li-ion) batteries due to their exceptionally high theoretical capacity. However, their practical deployment remains constrained by challenges such as significant volume changes during lithiation, poor electrical conductivity, and the instability of the solid electrolyte interphase (SEI). This review critically examines recent advancements in Si-based nanostructures to enhance stability and electrochemical performance. Distinct from prior studies, it highlights the application of Si anodes in commercial domains, including electric vehicles, consumer electronics, and renewable energy storage systems, where prolonged cycle life and improved power density are crucial. Special emphasis is placed on emerging fabrication techniques, particularly scalable and cost-effective methods such as electrospinning and sol–gel processes, which show promise for industrial adoption. By addressing both the technical innovations and economic considerations surrounding Si anodes, this review provides a comprehensive roadmap for overcoming existing barriers, paving the way for next-generation, high-performance batteries.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240048","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145013128","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Due to the strong affinity between the solvent and Li+, the desolvation process of Li+ at the interface as a rate-controlling step slows down, which greatly reduces the low-temperature electrochemical performance of lithium-ion batteries (LIBs) and thus limits its wide application in energy storage. Herein, to improve the low-temperature tolerance, a localized high-concentration electrolyte based on weak solvation (Wb-LHCE) has been designed by adding a diluent hexafluorobenzene (FB) in a weak solvating solvent tetrahydrofuran (THF). Combining theoretical calculations with characterization tests, it is found that with the addition of diluent FB, the dipole–dipole interaction between the diluent and the solvent causes FB to compete with Li+ for THF. This competition causes the solvent to move away from Li+, weakening the binding energy between Li+ and THF, whereas the anions are transported into the solvation shell of Li+, forming an anion-rich solvation structure. In addition to accelerating the Li+ desolvation process, this unique solvation structure optimizes the composition of the CEI film, making it thin, dense, homogeneous, and rich in inorganic components, and thus improving the interfacial stability of the battery. As a result, the assembled LiFePO4/Li half-cell shows excellent electrochemical performances at low temperature. That is, it can maintain a high discharge specific capacity of 124.2 mAh g−1 after 100 cycles at a rate of 0.2C at −20°C. This provides an attractive avenue for the design of advanced low-temperature electrolytes and improvement of battery tolerance to harsh conditions.
由于溶剂与Li+之间的强亲和力,Li+在界面处的脱溶过程作为一个速率控制步骤减慢,这大大降低了锂离子电池(LIBs)的低温电化学性能,从而限制了其在储能领域的广泛应用。为了提高低温耐受性,在弱溶剂四氢呋喃(THF)中加入稀释剂六氟苯(FB),设计了基于弱溶剂化的局部高浓度电解质(Wb-LHCE)。理论计算与表征试验相结合,发现当稀释剂FB加入后,稀释剂与溶剂之间的偶极-偶极相互作用导致FB与Li+竞争THF。这种竞争导致溶剂远离Li+,减弱Li+和THF之间的结合能,而阴离子被转移到Li+的溶剂化壳层,形成一个富含阴离子的溶剂化结构。这种独特的溶剂化结构除了加速Li+的脱溶过程外,还优化了CEI膜的组成,使其薄、致密、均匀,并富含无机成分,从而提高了电池的界面稳定性。结果表明,组装后的LiFePO4/Li半电池在低温下表现出优异的电化学性能。即在−20℃下,以0.2C的倍率放电100次后,可保持124.2 mAh g−1的高放电比容量。这为设计先进的低温电解质和提高电池对恶劣条件的耐受性提供了一条有吸引力的途径。
{"title":"Improving Low-Temperature Tolerance of a Lithium-Ion Battery by a Localized High-Concentration Electrolyte Based on the Weak Solvation Effect","authors":"Jinlong Sun, Yijie Yao, Xiaoling Cui, Jing Luo, Junwei Zhang, Yanjun Zhao, Hui Wang, Junfei Zhou, Junlong Zhu, Yinong Wang, Chunlei Li, Ningshuang Zhang, Lijuan Zhang, Shiyou Li, Dongni Zhao","doi":"10.1002/bte2.20240106","DOIUrl":"https://doi.org/10.1002/bte2.20240106","url":null,"abstract":"<p>Due to the strong affinity between the solvent and Li<sup>+</sup>, the desolvation process of Li<sup>+</sup> at the interface as a rate-controlling step slows down, which greatly reduces the low-temperature electrochemical performance of lithium-ion batteries (LIBs) and thus limits its wide application in energy storage. Herein, to improve the low-temperature tolerance, a localized high-concentration electrolyte based on weak solvation (Wb-LHCE) has been designed by adding a diluent hexafluorobenzene (FB) in a weak solvating solvent tetrahydrofuran (THF). Combining theoretical calculations with characterization tests, it is found that with the addition of diluent FB, the dipole–dipole interaction between the diluent and the solvent causes FB to compete with Li<sup>+</sup> for THF. This competition causes the solvent to move away from Li<sup>+</sup>, weakening the binding energy between Li<sup>+</sup> and THF, whereas the anions are transported into the solvation shell of Li<sup>+</sup>, forming an anion-rich solvation structure. In addition to accelerating the Li<sup>+</sup> desolvation process, this unique solvation structure optimizes the composition of the CEI film, making it thin, dense, homogeneous, and rich in inorganic components, and thus improving the interfacial stability of the battery. As a result, the assembled LiFePO<sub>4</sub>/Li half-cell shows excellent electrochemical performances at low temperature. That is, it can maintain a high discharge specific capacity of 124.2 mAh g<sup>−1</sup> after 100 cycles at a rate of 0.2C at −20°C. This provides an attractive avenue for the design of advanced low-temperature electrolytes and improvement of battery tolerance to harsh conditions.</p>","PeriodicalId":8807,"journal":{"name":"Battery Energy","volume":"4 5","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/bte2.20240106","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145013129","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}