{"title":"Fast Charging Lithium Metal Battery Based on Lewis Acid/Base Dual-Site Solid Electrolyte Interphase","authors":"Minjian Li, Lianzhan Huang, Boyong Wu, Jinhui Liang, Jiahao Xiang, Tong Yan, Mengli Tao, Li Du, Zhiming Cui, Huiyu Song, Zhenxing Liang","doi":"10.1016/j.ensm.2025.104069","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104069","url":null,"abstract":"The unexpected depletion of anions and the restricted diffusion of Li<sup>+</sup> on the Li anode lead to uncontrolled dendrite growth in Li metal batteries. Solid electrolyte interphase (SEI) engineering has been proven to be an effective method for solving these issues. Herein, a novel SEI layer with Lewis acid/base dual-site is constructed with triisopropanolamine cyclic borate (BON) and LiTFSI (defined as TFBN) to regulate the transport behavior of anions and Li<sup>+</sup>. The electron-deficient boron atom in BON can serve as the Lewis acid site, which anchors the anion to prevent its depletion at the interface. Meanwhile, the electron-rich nitrogen atom can serve as the Lewis base site, which accelerates the transport of Li<sup>+</sup> to facilitate smooth Li deposition. As a result, BON can effectively dissociate lithium salts and regulate the migration behavior of anions and Li<sup>+</sup>. Using this novel SEI layer, Li||Li symmetric batteries can achieve stable cycling for over 1200 h at 1.0 mA cm<sup>−</sup>². Furthermore, the Li||LFP full cells show 93.7% capacity retention after 2000 cycles at an ultrahigh current of 10 C.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"1 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056390","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Minjun Bae, Yoonbin Kim, Yonghwan Kim, Yujin Chang, Juhyung Choi, Seon Jae Hwang, Jun Su Kim, Ho Seok Park, Jeongyeon Lee, Yuanzhe Piao
{"title":"Ultra-high Lithium Reversibility Achieved by Partially Pyrolyzed Polymeric Copper Phthalocyanines for Superior Anode-free Lithium Metal Batteries","authors":"Minjun Bae, Yoonbin Kim, Yonghwan Kim, Yujin Chang, Juhyung Choi, Seon Jae Hwang, Jun Su Kim, Ho Seok Park, Jeongyeon Lee, Yuanzhe Piao","doi":"10.1016/j.ensm.2025.104058","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104058","url":null,"abstract":"Anode-free lithium metal batteries (AFLMB) can maximize the energy density by eliminating active materials, conductive agents and binders from the anode. However, intrinsic issues of lithium (Li) metal anodes, such as non-uniform Li growth, large volume changes and unstable solid electrolyte interphase (SEI), become much pronounced, rapidly degrading the cyclability of AFLMB. Herein, we present a superior three-dimensional (3D) AFLMB host, which takes advantage of partially decomposed polymeric copper phthalocyanines bridged by di-thioether linkers (CuPPc-S) as an ultra-thin surface coating layer. By intensive material characterizations alongside in-situ thermal gravimetric analyses coupled with mass spectrometer, we demonstrate that our controlled pyrolysis results in the formation of partially pyrolyzed CuPPc-S (PP-CuPPc-S), where intrinsic redox active sites of CuPPc-S and newly formed ultra-fine Cu–S inorganic compounds co-exist. The preserved redox active sites can not only improve lithiophilicity, but also facilitate the decomposition of TFSi<sup>⁻</sup>, inducing abundant LiF in the SEI, while Cu–S compounds can serve dual roles as active Li nucleation sites and ionically conductive Li<sub>2</sub>S inducer in the SEI. Benefiting from these components, PP-CuPPc-S coated carbon fiber (PP-CuPPc-S@CF) can form a multifunctional SEI and induce dense Li nucleation, achieving the stable operation of 1000 cycles with a LiFePO<sub>4</sub> cathode in AFLMB configuration.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"74 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056929","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Electrodeposition of metal foils for battery current collectors: status and challenges","authors":"Atsushi Kitada","doi":"10.1016/j.ensm.2025.104073","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104073","url":null,"abstract":"The pursuit of reliable and sustainable energy storage solutions has driven continuous development of rechargeable lithium ion batteries (LIBs). While substantial progress has been made in the exploration of active materials and battery electrolytes, innovation is also necessary in the metal foils used as current collectors, which are crucial for electron transport between the electrode and external circuits. The manufacturing process, particularly shifting from roll process to electrolytic process, i.e. thinner foils with low cost, can offer potential improvements in energy density and cost. However, challenges associated with replacing the rolling process with electrolytic one are not well recognized, even by battery or electroplating researchers. Therefore, this review aims to provide an updated overview of the electrodeposition process for metals, especially stainless steel, aluminum, and titanium, which can be used as current collector foils but currently manufactured by roll process. The first part of the review introduces the basic properties of several current collector metals. The manufacturing process for electroplated copper foil, which is already widely industrialized, is also briefly explained. The second part addresses the current issues of electrodeposition of stainless steel alloys (which are difficult to improve in terms of crystallinity), as well as aluminum and titanium (which cannot be electroplated from aqueous solutions). The final part provides perspectives for “metal on plastic” foils where additional electrolytic treatment should be engaged toward practical use. Overall, this review provides new insights and guidelines for the development of next-generation current collector foil processing that leverage the expertise of electrolytic processes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"74 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143056358","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yifan Xu, Zongzi Jin, Xiangkun Kong, Chi Zhang, Cui Li, Zhiwen Zhuo, Ranran Peng, Chengwei Wang
{"title":"Non-Transition Metal Modulated Reducibility Strategy for Highly Conductive Mixed Electronic and Ionic (LixLa2/3-x/3)TiO3 Perovskite","authors":"Yifan Xu, Zongzi Jin, Xiangkun Kong, Chi Zhang, Cui Li, Zhiwen Zhuo, Ranran Peng, Chengwei Wang","doi":"10.1016/j.ensm.2025.104074","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104074","url":null,"abstract":"In solid-state batteries, mixed electronic and ionic conductors play a crucial role in enhancing electrode charge transfer. This study proposes a strategy for modulating the reducibility of materials to develop stable and highly conductive mixed conductors based on perovskite-type (Li<sub>x</sub>La<sub>2/3-x/3</sub>)TiO<sub>3</sub> oxides. Traditional methods that enhance electronic conductivity through B-site doping with variable valence transition metals have limited improvement on electronic conductivity with presence of significant secondary phases. Therefore, our approach focuses on A-site doping with fixed-valence non-transition metals to affect the reducibility of (Li<sub>x</sub>La<sub>2/3-x/3</sub>)TiO<sub>3</sub>, thereby regulating its electronic conductance properties. Our findings reveal that co-doping with the alkali metal Na and the alkaline earth metal Sr at the Li-site enhances the reducibility of Ti and doubles the electronic conductivity to 2.89 × 10<sup>-3</sup> S/cm compared to the undoped composition. Meanwhile, Na-Sr co-doping improves the reconfiguration of the crystal lattice during the reduction process, so that it exhibits high sintering activity and thermodynamic stability. These factors together contribute to its outstanding rate capability and long cycle stability, enabling it to maintain over 50% of its initial capacity at a 50 C-rate, and demonstrating over 800 stable cycles at a 2.5 C-rate. This strategy provides a new way to develop high-performance mixed-conductor electrode framework materials for improving the electrode kinetic behavior of solid-state batteries and promoting their practical applications.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"572 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050432","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenping Cheng, Liyu Sun, Jie Dong, Zongchang Han, Liang Wei, Linlin Lu, Runjun Sun
{"title":"Application progress and challenges of 1D fiber electrodes in wearable devices","authors":"Wenping Cheng, Liyu Sun, Jie Dong, Zongchang Han, Liang Wei, Linlin Lu, Runjun Sun","doi":"10.1016/j.ensm.2025.104059","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104059","url":null,"abstract":"Fiber electrodes, with their one-dimensional (1D) structure, bring distinct advantages to flexible electronics. Their mechanical flexibility, high conductivity, and weavability make them ideal for energy storage, sensing, and biomedical applications. Unlike rigid electrodes, fiber electrodes support lightweight, comfortable wearables with reliable electrical performance under dynamic conditions. This review explores recent progress and challenges in fiber electrodes, emphasizing material selection, fabrication methods, and applications in energy storage, sensing, and biomedicine. Key materials for fiber electrodes include carbon-based materials, metal nanomaterials, and conductive polymers, with carbon nanotubes and graphene as promising candidates due to their conductivity and mechanical strength. Performance can be further optimized through hybridization and surface modifications. Fiber electrodes show strong potential in supercapacitors and lithium-ion batteries, offering high surface areas and energy densities essential for flexible energy storage. In flexible sensors, fiber electrodes provide precise monitoring of human motion and environmental changes. Their biocompatibility also makes them suitable for wearable medical devices. Challenges remain in balancing conductivity with flexibility, reducing fabrication costs, and ensuring durability. Future research should focus on more efficient, scalable fabrication methods and advanced materials to enhance stability and performance, propelling wearable devices for smart health monitoring and self-powered systems.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"52 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143055286","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ziqi Wei, Dewen Kong, Lijiao Quan, Junhao Huang, Si Chen, Xinchuan Cao, Ruiqin Zhang, Haijing Liu, Lidan Xing, Weishan Li
{"title":"Refined Film-Forming Additive Overcomes Polytetrafluoroethylene Challenges in Dry-Processed High-Loading Lithium-Ion Batteries","authors":"Ziqi Wei, Dewen Kong, Lijiao Quan, Junhao Huang, Si Chen, Xinchuan Cao, Ruiqin Zhang, Haijing Liu, Lidan Xing, Weishan Li","doi":"10.1016/j.ensm.2025.104071","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104071","url":null,"abstract":"The demand for high-energy-density lithium-ion batteries (LIBs) has led to progress in producing high-loading electrodes using dry-process, reducing costs and energy consumption related to toxic solvents used in wet-process. Polytetrafluoroethylene (PTFE), commonly used as a binder in dry electrodes, offers excellent adhesion and thermal stability but poses difficulties for graphite anodes due to substantial initial irreversible capacity loss caused by reductive decomposition (∼1.2 V vs. Li/Li<sup>+</sup>). This study introduces a novel approach showing the problem of PTFE reduction can be mitigated by incorporating N-phenyl-bis(trifluoromethanesulfonimide) (PTFSI), an electrolyte additive with strong reducibility and superior film-forming properties. PTFSI creates a protective solid-electrolyte interphase (SEI) layer on both graphite and PTFE surfaces, successfully inhibiting PTFE decomposition without introducing inert substances. The innovative method allowed high-loading pouch cells (LiNi<sub>0.75</sub>Mn<sub>0.25</sub>O<sub>2</sub>/graphite) to achieve an initial discharge capacity of 227.7 mAh and a Coulombic efficiency of 78.2%, with an energy density of 258.7 Wh/kg. After 400 cycles, the cells maintained a capacity of 183.4 mAh, retaining 80.5% of their original capacity. The findings highlight the potential impact of PTFSI in significantly improving next-generation high-loading LIBs, addressing challenges with high-loading electrodes and advancing efficient and durable energy storage systems critical for electric vehicles and large-scale energy storage applications.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"39 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Haochen Dong, Tingzhou Yang, Chuangwei Liu, Dan Luo, Ning Liu, Yunnan Gao, Zhenjia Shi, Yongguang Zhang, Zhongwei Chen
{"title":"Controllable and scalable prelithiation of dry silicon-based anodes for high-energy-density lithium-ion batteries","authors":"Haochen Dong, Tingzhou Yang, Chuangwei Liu, Dan Luo, Ning Liu, Yunnan Gao, Zhenjia Shi, Yongguang Zhang, Zhongwei Chen","doi":"10.1016/j.ensm.2025.104072","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104072","url":null,"abstract":"High-energy-density batteries using high mass loaded silicon (Si)-based anode are of great interest to battery manufacturers as a transition toward next-generation storage technology. However, the huge volume expansion and insufficient cation utilization accompanied by low initial Coulombic efficiency of the anode limit the battery performance. Herein, a cost-effective and controllable clinging prelithiation strategy for high-loaded dry Si-based electrodes is proposed to achieve a homogeneous prelithiation process with improved structural stability and higher initial Coulombic efficiency. The sufficient interior space enabled by dry electrode technology and uniformly distributed lithiated alloy phases can tolerate large volume changes and avoid irreversible capacity loss, thereby improving Li utilization and enhancing cycle stability. With this prelithiation strategy, initial Coulombic efficiency (ICE) can be improved by 22.3%-25.1% to around 100% even under a high-loading Si-based anode of 16.51 mg cm<sup>-2</sup> with reduced open circuit voltage. Therefore, the assembled full cell paired with both electrodes fabricated via dry electrode technology further exhibits an improved ICE of 98.73% with high capacity retention of 88.15% over 300 cycles, suggesting that dry electrode technology combined with the prelithiation method is suitable for optimizing high Si loading anode for next-generation high energy density batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"49 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143050416","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhanxu Zheng, Bingying Pei, Lei Zhang, Xinxin Cao, Shuquan Liang
{"title":"Pore Structure in Hard Carbon: from Recognition to Regulation","authors":"Zhanxu Zheng, Bingying Pei, Lei Zhang, Xinxin Cao, Shuquan Liang","doi":"10.1016/j.ensm.2025.104068","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104068","url":null,"abstract":"Hard carbon (HC) has garnered significant attention as the most commercially promising anode material for sodium-ion batteries (SIBs), owing to its wide distribution, low cost, and abundant resources. However, challenges have arisen in recent years regarding its application in SIBs due to variations in Na storage mechanisms and performance resulting from its diverse microstructure. The diversity of microstructures in HC, resulting from different precursor systems, presents a formidable challenge to the elucidation of the mechanism and regulation of Na storage in HC. A comprehensive understanding of the diverse pore structures in HC is pivotal for rational modulation of its structure and performance, as well as for comprehending its Na storage mechanism. This review initially discusses the classification, structure, and characterization methods of nanopores in HC. Subsequently, it elucidates the relationship between these nanopores and their electrochemical properties, encompassing open pores, closed pores, and sieving pores. Finally, it introduces and prospects common approaches for manipulating disordered carbon multi-structure. This review is anticipated to offer a viable research direction for the field of HC, facilitating the rational design of high-capacity carbon anodes, and accelerating the industrialization process of SIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"61 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044626","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Nonflammable F/N synergistic electrolyte boosting high-voltage Li metal batteries in wide temperature range","authors":"Yilu Wu, Qinghui Zhang, Ning Wang, Kuirong Deng","doi":"10.1016/j.ensm.2025.104066","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104066","url":null,"abstract":"High-voltage Li metal batteries are promising energy storage technologies owing to their high energy densities (>400 Wh kg<sup>−1</sup>). However, high-voltage Li metal batteries with conventional electrolytes suffer from poor interface stability, inferior cycle performance and low security. Herein, we develop a rational design of nonflammable fluorinated amide electrolyte via the synergetic combination of F/N donating solvents to construct robust and highly conductive solid electrolyte interphases (SEIs) and cathode-electrolyte interphases (CEIs) with high LiF and Li<sub>3</sub>N content, which effectively enhance the interfacial stability and ionic conductivity of Li metal anodes and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cathodes. More anions are brought into the primary solvation shell of Li<sup>+</sup> to participate in the formation of SEIs/CEIs by tuning the intermolecular interactions. As a result, extremely stable and high-efficiency cycle of Li metal anodes in Li||Li cells and Li||Cu cells is achieved. The performance of Li||NCM811 cells is markedly boosted under high voltage (4.7 V) and in wide temperature range (−20 °C to 60 °C), which display stable cycling over 650 cycles and excellent rate capability up to 20 C. This work sheds new lights on F/N synergetic effect and intermolecular interactions of electrolytes for Li metal batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"22 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044630","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Reevaluating feature selection in phase field models for battery performance: A call for robust statistical approaches","authors":"Yoshiyasu Takefuji","doi":"10.1016/j.ensm.2025.104060","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104060","url":null,"abstract":"Han and Lin's phase field model for lithium-ion batteries utilizes LASSO regression to analyze battery performance during galvanostatic cycling, aiming to simplify the relationship between parameters and Coulombic efficiency. Despite demonstrating accuracy, this paper critiques the reliance on LASSO for feature selection, highlighting its potential inadequacy in capturing nonlinear interactions within chemical properties. Traditional performance metrics, such as MAE, RMSE, and R², provide limited insights regarding individual feature contributions and the nuanced relationships present in the data. This paper advocates for adopting nonparametric statistical methods, such as Spearman's correlation and Kendall's tau, which can better elucidate complex variable associations and validate feature importance. Incorporating these methods will enhance the robustness of findings, promoting a clearer understanding of battery performance dynamics.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"27 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143044677","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}