J.C. Barbosa, A. Fidalgo-Marijuan, J.C. Dias, R. Gonçalves, M. Salado, C.M. Costa, S. Lanceros-Méndez
{"title":"Corrigendum to “Molecular design of functional polymers for organic radical batteries” [Energy Storage Materials, Volume 60, June 2023, 102841]","authors":"J.C. Barbosa, A. Fidalgo-Marijuan, J.C. Dias, R. Gonçalves, M. Salado, C.M. Costa, S. Lanceros-Méndez","doi":"10.1016/j.ensm.2025.104587","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104587","url":null,"abstract":"Due to an editing mistake, the reference (C. Zens, C. Friebe, U.S. Schubert, M. Richter, S. Kupfer, Tailored Charge Transfer Kinetics in Precursors for Organic Radical Batteries: A Joint Synthetic-Theoretical Approach, ChemSusChem 16 (2023), e202201679) was not placed in the corresponding place. The proper attribution of the reference is as follows:","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"15 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144996083","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}
Can Huang, Tiezhong Liu, Jie Yang, Shuang Hou, Qiang Deng, Lingzhi Zhao
{"title":"Revealing anion-evolution mediated superior bidirectional kinetics in Se-doped CuS1-xSex: a highly reversible conversion-type anode for zinc-ion battery","authors":"Can Huang, Tiezhong Liu, Jie Yang, Shuang Hou, Qiang Deng, Lingzhi Zhao","doi":"10.1016/j.ensm.2025.104590","DOIUrl":"10.1016/j.ensm.2025.104590","url":null,"abstract":"<div><div>Anion doping has been regarded as a promising tactic for facilitating the redox reactions of conversion-type transition metal sulfide (TMS) anodes in rocking-chair zinc-ion battery (RCZIB). However, the evolution pathways of doped anion and the enhancement mechanisms of bidirectional reaction kinetics for anion-doped TMS anodes remain unrevealed during both the conversion and inverse-conversion processes. Herein, Se is selected as an appropriate anion to be doped into CuS (CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub> x</em> = 0.24) to design a highly reversible anode for RCZIB. Theoretical calculations and experimental results reveal that Se-doping significantly enhances the conversion kinetics of CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em> through increased electrical conductivity, optimized Zn<sup>2+</sup> adsorption behavior and reduced reaction energy barriers during discharging. Ex-situ characterizations demonstrate the dynamic evolution of Se anions, which are incorporated into the discharge product (ZnS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em>) during the conversion process. The incorporated Se anions enhance inverse-conversion kinetics during charging via synergistic effects: boosted electrical conductivity, strengthened Cu adsorption capability and facile decomposition for ZnS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em>. Subsequently, Se anions are reversibly re-doped into the regenerated charge product (CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em>) upon reverse-conversion reaction. Benefiting from superior bidirectional reaction kinetics, CuS<sub>1-</sub><em><sub>x</sub></em>Se<em><sub>x</sub></em> exhibits remarkable rate capability as well as long-term cycling stability in both half and full batteries. This exploration provides a new insight into the dynamic evolution of doped-Se and its synergistic enhancement mechanisms in bidirectional kinetics for highly reversible anion-doped TMS anodes in RCZIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104590"},"PeriodicalIF":20.2,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987611","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}
Ove Korjus , Saptarshee Mitra , Quentin Berrod , Victor Vanpeene , Markus Appel , Ludovic Broche , Sandrine Lyonnard , Claire Villevieille
{"title":"Investigating the densification of Li6PS5Cl solid electrolyte through multi-scale characterization techniques","authors":"Ove Korjus , Saptarshee Mitra , Quentin Berrod , Victor Vanpeene , Markus Appel , Ludovic Broche , Sandrine Lyonnard , Claire Villevieille","doi":"10.1016/j.ensm.2025.104589","DOIUrl":"10.1016/j.ensm.2025.104589","url":null,"abstract":"<div><div>Li<sub>6</sub>PS<sub>5</sub>Cl (LPSCl) has recently gained attention as a promising solid-state electrolyte for batteries. However, the mechanisms underlying the “cold sintering” process in LPSCl remain poorly understood. In this study, we performed <em>in situ</em> densification of LPSCl while simultaneously measuring electrochemical impedance spectroscopy and micro-tomography to gain deeper insights into “cold sintering” process and to correlate the ionic conduction with the three-dimensional microstructure of the solid electrolyte. We observed that the large (secondary) particles are fracturing, while the grain boundary (GB) conductivity is improving due to better contact between grains. We have found that during the pressure application (up to 510 MPa from 76.2 MPa) at room temperature, the conductivity increases 2.45 times (up to 1.66 mS cm<sup>−1</sup>). From an in-depth electrochemical impedance and quasielastic neutron scattering (QENS) investigation, we show that the conductivity enhancement primarily arises from improved GB contact, with the bulk material remaining largely unaffected – that is, unsintered. However, the Li<sup>+</sup>conductivity is not limited by bulk but by GB resistance. The electrolyte’s conductivity without any GB contribution is estimated from QENS results with the Nernst-Einstein equation to be 5.3 mS cm<sup>−1</sup>, giving us the maximum conductivity that could be reached with shaping without modifying the bulk of the material.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104589"},"PeriodicalIF":20.2,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144987613","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}
Xinyu Wang , Yiran Ying , Yuanbiao Gong , Shengmei Chen , Shuyun Wang , Weijia Wang , Juan Antonio Zapien , Longtao Ma , Min Zhu
{"title":"Piezoelectric gradient electrolytes for environmentally adaptive and stable zinc batteries","authors":"Xinyu Wang , Yiran Ying , Yuanbiao Gong , Shengmei Chen , Shuyun Wang , Weijia Wang , Juan Antonio Zapien , Longtao Ma , Min Zhu","doi":"10.1016/j.ensm.2025.104586","DOIUrl":"10.1016/j.ensm.2025.104586","url":null,"abstract":"<div><div>Solid polymer electrolyte-based zinc batteries are promising candidates for next-generation electrochemical energy storage due to their cost-effectiveness, enhanced safety and high theoretical energy density. However, their practical deployment is severely hindered by sluggish Zn<sup>2+</sup> ion mobility, poor interfacial compatibility and uneven electric field distribution. To address the persistent challenges, this work presents a novel asymmetric piezoelectric electrolyte, engineered by the strategic vertical distribution of piezoelectric barium titanate (BTO) nanofillers within a polyvinylidene fluoride (PVDF)-based polymer matrix. This design introduces a built-in gradient electric field across the electrolyte thickness, leveraging the electromechanical properties of BTO to regulate ion transport and interfacial dynamics. On the Zn anode-facing side, the BTO-rich region with a high dielectric constant and enhanced local polarization, promotes zinc salt dissociation and generates a directional electric field that promotes uniform Zn<sup>2+</sup> flux. This configuration effectively suppresses dendrite formation and mitigates localized charge accumulation. Conversely, the MnO<sub>2</sub> cathode-facing side comprises a softer, polymer-rich phase with lower BTO content, ensuring better interfacial compliance and reduced contact resistance, which is crucial for facilitating efficient ion transport without inducing excessive polarization. As a result, the asymmetric architecture achieves an impressive ionic conductivity of 1.39 mS·cm<sup>-1</sup> and a high Zn<sup>2+</sup> transference number of 0.69 at room temperature, outperforming conventional SPEs. ZnǀǀZn symmetric cells exhibit outstanding cycle stability, sustaining operation for over 1500 h, while Zn||MnO<sub>2</sub> full batteries demonstrate stable cycling over 1200 cycles. Notably, the battery performs reliably across a wide temperature range from -30 °C to 60 °C, demonstrating strong adaptability to harsh environments. This work provides a scalable and effective strategy for overcoming key limitations in Zn-based batteries by introducing a functionally asymmetric, piezoelectric electrolyte structure. This advancement paves the way for the development of safe, durable, and high-efficiency zinc-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104586"},"PeriodicalIF":20.2,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928470","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}
Rongrong Guo , Xiaoyun Xu , Songmei Li , Yangyang Cheng , Junwei An , Mei Yu , Jinyan Zhong , Juan Du , Shubin Yang , Bin Li
{"title":"Elevating operation voltage of LiTFSI-electrolyte via a universal passivation strategy for high-voltage lithium-metal batteries","authors":"Rongrong Guo , Xiaoyun Xu , Songmei Li , Yangyang Cheng , Junwei An , Mei Yu , Jinyan Zhong , Juan Du , Shubin Yang , Bin Li","doi":"10.1016/j.ensm.2025.104588","DOIUrl":"10.1016/j.ensm.2025.104588","url":null,"abstract":"<div><div>Lithium bis((trifluoromethyl)sulfonyl)azanide (LiTFSI) based electrolytes have become the preferred electrolytes for lithium metal batteries (LMBs) due to their exceptional anode stability and ionic conductivity. However, challenges including unstable cathode electrolyte interface (CEI) formation and aluminum current collector (AlCC) corrosion have hindered the application of LiTFSI-based electrolyte in high-voltage LMBs. In this work, a universal passivation strategy is proposed and achieved with additive 8-hydroxyquinoline (8-HQ) in LiTFSI based electrolyte (ED-HQ). The 8-HQ additive preferentially decomposes on the cathode surface to generate Li<sub>3</sub>N, inducing the formation of inorganic-rich CEI with a uniform thickness of only 10 nm. The dense and homogeneous inorganic-rich CEI enables the cycling stability of the cathode. Meanwhile, the 8-HQ additive shows strong adsorption on the AlCC surface, which promotes the formation of a composite passivation layer consisting of an Aluminum-8-hydroxyquinoline (Alq<sub>3</sub>) chelate layer and an AlF<sub>3</sub>/LiF inorganic layer, increasing the stable operating voltage of AlCC to 4.9 V and reducing the corrosion current density to one tenth. As a result, the joint effects enable Li||LiFePO<sub>4</sub> cells with ED-HQ electrolyte to achieve 89.8% capacity retention after 500 cycles at an elevated cutoff voltage of 4.5 V, demonstrating a viable pathway toward stable high-voltage LMB operation.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104588"},"PeriodicalIF":20.2,"publicationDate":"2025-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144931203","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}
Sheng Guo , Hao Luo , Zhe Gao , Yizheng Ding , Shiwen Wang , Pengcheng Wang , Feihong Wang , Jizhong Cao , Yajie Song , Ning Ren , Mi Lu
{"title":"Embedded sensing: The neural frontier and early-warning revolution in battery safety monitoring","authors":"Sheng Guo , Hao Luo , Zhe Gao , Yizheng Ding , Shiwen Wang , Pengcheng Wang , Feihong Wang , Jizhong Cao , Yajie Song , Ning Ren , Mi Lu","doi":"10.1016/j.ensm.2025.104582","DOIUrl":"10.1016/j.ensm.2025.104582","url":null,"abstract":"<div><div>The rapid proliferation of battery systems has positioned thermal runaway prevention as a crucial technological imperative. In-situ sensor-based monitoring frameworks enable real-time tracking of internal parameters, thereby providing early warnings and interventions for thermal management. However, conventional sensors, limited by their unidimensional architectures, struggle to accurately capture the intricate interplay among thermal, mechanical, and chemical fields. This limitation results in significant blind spots when predicting battery degradation under multiphysics conditions over the entire lifecycle. Consequently, advancing multi-parameter sensing technologies and developing multidimensional sensing architectures become essential for achieving comprehensive battery safety monitoring. From an embedded sensing perspective, this review systematically examines critical challenges related to chemical compatibility, measurement accuracy, and multi-parameter monitoring encountered during sensor integration. It provides a detailed elaboration on the operating principles and practical applications of thermocouples, optical fiber sensors, and thin-film sensors in batteries. To address technological bottlenecks, such as risks to structural integrity, electrolyte-induced performance degradation, and limitations in single-parameter monitoring, we propose strategies that include sensor miniaturization, the selection of chemically robust materials, integrated multidimensional in-situ platforms, and the incorporation of artificial intelligence (AI) technologies. This review advances comprehensive understanding of battery multidimensional sensing systems, significantly enhancing active safety engineering and multiphysics diagnostic frameworks.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104582"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924302","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":"Deciphering the capacitive behavior of heteroatom–doped carbon materials with small mesopores","authors":"Xiang Cai , Kuixuan Zhang , Wangxu Chen, Xinqi Hu","doi":"10.1016/j.ensm.2025.104584","DOIUrl":"10.1016/j.ensm.2025.104584","url":null,"abstract":"<div><div>The charge storage processes of heteroatom–doped carbon materials with small mesopores (2 ∼ 4 nm) occur by both double–layer capacitance and pseudocapacitance. Yet, owing to the ambiguous understanding on how electrolyte ions affect their capacitive behavior, it is hard to form a unified design principle to guide the selection of electrolytes, with the purpose of boosting supercapacitors. Herein, an all–in–one carbon electrode with abundant oxygen–containing groups and an average pore size of 2.5 nm was used as a model electrode to investigate the capacitive behavior of this class of carbon materials. It is found that in ammonium acetate aqueous electrolyte the model electrode shows a significantly increased specific capacitance, and an ion exchange mechanism dominates charge storage. Acetate anions with a larger ion radius can better match small mesopores in size and thus increase double–layer capacitance due to the suppression of the “over–screening” effect in the first adsorbed layer on carbon surfaces. Besides, ammonium cations forms hydrogen bonds with oxygen–containing groups maximizing the Gibbs free energy change related to faradic reactions, which enhances pseudocapacitance. Our work elaborated the effect of electrolyte ions on the capacitance of heteroatom–doped carbon materials with small mesopores and provided new understanding on designing high–performance aqueous supercapacitors.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104584"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924339","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}
Bo Yu , Luo Fei , Mengfei Li , Zhiyuan Ma , Bingshu Guo , Junchen Chen , Xingyang Wang , Zhiyu Xue , Liujiang Zhou , John Wang
{"title":"Ultrathin lithium metal anodes for high-efficiency lithium batteries: synergizing surface LiF and Lithiophilic alloying","authors":"Bo Yu , Luo Fei , Mengfei Li , Zhiyuan Ma , Bingshu Guo , Junchen Chen , Xingyang Wang , Zhiyu Xue , Liujiang Zhou , John Wang","doi":"10.1016/j.ensm.2025.104579","DOIUrl":"10.1016/j.ensm.2025.104579","url":null,"abstract":"<div><div>Lithium metal batteries are considered one of the most promising candidates for next-generation energy storage systems. However, challenges such as dendrite formation, unstable cycling, and low lithium utilization have severely hindered their practical implementation. Herein, we propose a universal and scalable strategy for fabricating ultrathin lithium anodes by integrating lithiophilic alloys and metal fluoride coatings onto current collectors through a simple SnF<sub>2</sub>-based gas-phase reaction. A roll-to-roll system enables scalable production on various metal substrates, as demonstrated by Ni mesh coated with Ni<sub>3</sub>Sn<sub>2</sub> and NiF<sub>2</sub>. Electrochemical lithium deposition and molten infusion induce in situ Li-Sn alloy formation and LiF surface migration, which synergistically enable uniform plating, interface stabilization, and high lithium utilization. The resulting anodes deliver tunable areal capacities of 3–10 mAh cm<sup>−2</sup>, effectively overcoming the fabrication limitations of lithium foils thinner than 50 μm and significantly reducing lithium consumption. Specifically, ultrathin lithium anodes with a capacity of 3.4 mAh cm<sup>−2</sup> exhibit stable cycling over 2200 h in symmetric cells. Full cells with LiFePO<sub>4</sub> cathodes deliver an average Coulombic efficiency of 99.8 % over 200 cycles at 0.5 C.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104579"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928508","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}
Xingyu Hu , Hui Shi , Yilei Zheng , Penghui Shao , Liming Yang , Xubiao Luo
{"title":"Precise Ni/Co separation from spent Li-Ion batteries: Revealing the pivotal role of H2O in deep eutectic solvents","authors":"Xingyu Hu , Hui Shi , Yilei Zheng , Penghui Shao , Liming Yang , Xubiao Luo","doi":"10.1016/j.ensm.2025.104585","DOIUrl":"10.1016/j.ensm.2025.104585","url":null,"abstract":"<div><div>The sustainable recovery of valuable metals from end-of-life lithium-ion batteries (LIBs) has become essential for relieving the supply-demand contradiction of key resources. However, the high similarity in physicochemical properties of transition metals poses a fundamental challenge for the selective recycling. Here we proposed a facile strategy for defining the demarcation line of precipitation/dissolution behavior for precise Ni/Co separation. A malonic acid-based deep eutectic solvent (DES) is developed, emphasizing the H<sub>2</sub>O-mediated competitive coordination and differentiated solubility. We discovered the distinctive formation of [Ni(H<sub>2</sub>O)<sub>6</sub>]<sup>2+</sup> and [CoCl<sub>4</sub>]<sup>2-</sup> in the DES-20 % H<sub>2</sub>O system. Furthermore, the <em>K</em><sub>sp</sub> differences of the Ni-complex and Co-complex in the C<sub>3</sub>H<sub>2</sub>O<sub>4</sub><sup>2-</sup>-rich environment was effectively magnified. These significant differences synergistically enable the generation of C<sub>3</sub>H<sub>2</sub>NiO<sub>4</sub>·2H<sub>2</sub>O precipitation (∼ 99.9 % purity), achieving a remarkable Ni/Co separation factor of 125, which guarantees sequential separation of all metals. This universal methodology along with in-depth mechanism understanding provides a guideline toward value-added recovery of LIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104585"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144928631","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}
Haizhou Zhao , Sizhe Wang , Sihang Xia , Fei Liang , Yancheng Yang , Ji Qian , Haojie Song , Chao Yang , Renjie Chen
{"title":"Engineering the future of silicon-based all-solid-state lithium-ion batteries: Current barriers and innovative solutions","authors":"Haizhou Zhao , Sizhe Wang , Sihang Xia , Fei Liang , Yancheng Yang , Ji Qian , Haojie Song , Chao Yang , Renjie Chen","doi":"10.1016/j.ensm.2025.104583","DOIUrl":"10.1016/j.ensm.2025.104583","url":null,"abstract":"<div><div>As a leading contender for advanced energy storage systems, silicon-based all-solid-state lithium-ion batteries (Si-ASSLIBs) have garnered critical research frontier due to their demonstrated capacity to offer enhanced energy density and superior thermal stability and safety compared to conventional lithium-ion batteries. However, Si-ASSLIBs still faces challenges in practical applications, such as cell failure due to the significant volume expansion of silicon. Innovatively, we highlight that pressure plays two critical roles in Si-ASSLIBs. Herein, we systematically review the recent advances and challenges in Si-ASSLIBs, with a particular emphasis on their industrialization pathways. The research progress of Si-ASSLIBs is comprehensively summarized, and different silicon anodes and their electrochemical performance optimization strategies are presented. Next, we systematically summarize the mechanical properties, simulation, and morphological/structural characterization approaches pertaining to volume expansion in Si-ASSLIBs. Crucially, we propose that fabrication pressure pre-stabilizes electrode interfaces, while operational pressure dynamically regulates stress evolution. In order to promote the scaled-up industrial production of Si-ASSLIBs, we summarize the current state of research on the pre-lithiation process and present our views for industrialization. As a core enabler, pre-lithiation technology is rigorously evaluated via scalable production pathways, establishing design standards and an industrial roadmap. Finally, the challenges and opportunities for achieving high energy density Si-ASSLIBs and future developments are outlined. This review outlooks the challenges, opportunities, and future directions for advanced Si-ASSLIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104583"},"PeriodicalIF":20.2,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144924340","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}