Liang Xie , Taifan Yang , Jiawei Pan , Weipeng Li , Zhanhui Jia , Xiangwen Gao , Chengyong Shu , Wei Tang
{"title":"Hierarchical LiMn0.6Fe0.4PO4 microspheres with atomic mixture of Fe/Mn derived from (Mn0.6Fe0.4)3(PO4)2·xH2O precursors for high stability lithium ion batteries","authors":"Liang Xie , Taifan Yang , Jiawei Pan , Weipeng Li , Zhanhui Jia , Xiangwen Gao , Chengyong Shu , Wei Tang","doi":"10.1016/j.ensm.2025.104637","DOIUrl":"10.1016/j.ensm.2025.104637","url":null,"abstract":"<div><div>LiMn<sub>x</sub>Fe<sub>1-x</sub>PO<sub>4</sub>/C (LMFP) is one of the most promising alternatives of LiFePO<sub>4</sub> (LFP) for next generation high energy lithium-ion batteries (LIBs) due to its higher working potential. However, when the substitution level of Fe with Mn exceeds half, the resulting inhomogeneous distribution of Fe/Mn may subsequently impede the performance of lithium manganese iron phosphate (LMFP) in terms of its rate capability, long-term cyclability. In this study, a multi-strategy synergistic modification approach was employed to address the aforementioned issues. First of all, the atomic-level mixing of iron and manganese was achieved by synthesizing the microsphere (Mn<sub>0.6</sub>Fe<sub>0.4</sub>)<sub>3</sub>(PO<sub>4</sub>)<sub>3</sub>·xH<sub>2</sub>O precursor while nanoscale primary particles coated with uniform carbon layer were agglomerated into hierarchical LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> microspheres through spray-drying to enhance the tap density and electrical conductivity. XAFS measurements reveal a shorter Fe-O bond length, which is beneficial for maintaining the structural stability of the LMFP. Moreover, in situ XRD analysis confirms the occurrence of complete solid-solution behavior during cycling, which minimizes the transport energy barrier at the interface of the two phases and enhances the kinetic properties. Furthermore, in situ XAFS verifies the redox reactions of transition metals in LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> occur with a high degree of reversibility during electrochemical cycling. Consequently, as prepared microspherical LiMn<sub>0.6</sub>Fe<sub>0.4</sub>PO<sub>4</sub> cathode material demonstrates high tap density (1.28 g ml<sup>−1</sup>), excellent rate performance with a capacity of 137 mAh g<sup>−1</sup> at a high rate of 3C and long cycling stability with capacity retention of 88.5 % after 800 cycles as well as minimal voltage decay of 0.21 mV per cycle.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104637"},"PeriodicalIF":20.2,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145182802","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}
Han Guo , Yipu Guo , Xiaoyang Du , Dan Li , Jing Zhong
{"title":"Interconnected Conductive Networks in Cement Mortar Enable High-Performance Structural Supercapacitors","authors":"Han Guo , Yipu Guo , Xiaoyang Du , Dan Li , Jing Zhong","doi":"10.1016/j.ensm.2025.104630","DOIUrl":"10.1016/j.ensm.2025.104630","url":null,"abstract":"<div><div>Integrating energy storage capabilities into construction materials offers a promising pathway toward multifunctional, self-sustaining infrastructure. Among various approaches, cement-based supercapacitors (CSCs) are particularly attractive due to their inherent compatibility with structural elements, safety, and long cycle life. However, achieving both robust mechanical strength and high electrochemical performance in realistic mortar systems containing aggregates remains a major challenge. Here, we report a scalable design strategy that enables the fabrication of structurally sound and electrochemically active cement mortar electrodes. By incorporating reduced graphene oxide (rGO)-coated conductive aggregates into a carbon nanotube (CNT)–reinforced cement matrix, a three-dimensional hybrid conductive network is formed within the mortar. This architecture enhances charge transport while preserving mechanical integrity. Compression forming and low water-to-cement ratios further reduce porosity, enabling high-performance electrodes with flexural and compressive strengths of 9.72 MPa and 32.22 MPa, respectively—comparable to conventional cement mortars. The resulting symmetric device delivers a volumetric capacitance of 350.0 mF cm⁻³, energy density of 48.5 μWh cm⁻³, and power density of 32.8 mW cm⁻³, with excellent cycling stability (∼100 % retention over 10,000 cycles). This work demonstrates a practical and scalable pathway to multifunctional cement-based materials, opening new possibilities for embedding energy storage into structural components.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104630"},"PeriodicalIF":20.2,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145116640","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}
Yingshuai Wang , Runqing Ou , Yuhang Xin, Jingjing Yang, Feng Wu, Hongcai Gao
{"title":"Towards advanced Fe-based phosphates cathode with ultra-fast redox reaction kinetics and suppressed voltage hysteresis","authors":"Yingshuai Wang , Runqing Ou , Yuhang Xin, Jingjing Yang, Feng Wu, Hongcai Gao","doi":"10.1016/j.ensm.2025.104635","DOIUrl":"10.1016/j.ensm.2025.104635","url":null,"abstract":"<div><div>Voltage hysteresis has been regarded as a crucial challenge to achieve the application of ultra-fast charge/discharge sodium-ion batteries (SIBs), which drastically minimizes capacity output and degrades energy efficiency. Unfortunately, relevant research for suppressing the issue is mainly conducted in layered oxide cathodes, but the internal mechanism and suppression strategy of voltage hysteresis in polyanionic systems are often overlooked. Herein, this work proposes a dual strategy of Fe-defect and V-substitution to improve the redox reaction kinetics and suppress voltage hysteresis in Na<sub>3</sub>Fe<sub>1.85</sub>V<sub>0.1</sub>(PO<sub>4</sub>)P<sub>2</sub>O<sub>7</sub> (NF1.85V0.1PP). The dual strategy can facilitate the sluggish diffusion kinetics of sodium ions and improve redox reversibility while enhancing the stability of crystal structure by constructing rigid VO<sub>6</sub>. Consequently, NF1.85V0.1PP cathode exhibits excellent high-rate capability (101.3 mAh g<sup>−1</sup> at 1C and 68.8 mAh g<sup>−1</sup> at 50C) and remarkable cycling stability (decay-free for 3000 cycles under an ultra-high current density of 50C). Moreover, systematic in-situ/ex-situ characterizations reveal that the suppressed voltage hysteresis originates primarily from improved diffusion kinetics of the two-phase reaction process rather than the solid solution reaction process. This work sheds new light on the targeted improvement of redox reaction kinetics and suppression of voltage hysteresis to achieve high-performance SIBs.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104635"},"PeriodicalIF":20.2,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145153844","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}
Yongcong Huang, Fangchang Zhang, Xin Xu, Yanfang Wang, Peisong Sun, Kuan Jing, Feng Wu, Zibing An, Xiaodong Han, Yulin Cao, Yan Liu, Xingqun Liao, Yingzhi Li, Zhenghe Xu, Zhouguang Lu
{"title":"Enthalpy-mediated local structural ordering stabilizes O3-type layered cathode for sodium-ion batteries","authors":"Yongcong Huang, Fangchang Zhang, Xin Xu, Yanfang Wang, Peisong Sun, Kuan Jing, Feng Wu, Zibing An, Xiaodong Han, Yulin Cao, Yan Liu, Xingqun Liao, Yingzhi Li, Zhenghe Xu, Zhouguang Lu","doi":"10.1016/j.ensm.2025.104641","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104641","url":null,"abstract":"O3-type Na<sub>0.9</sub>Ni<sub>0.4</sub>Fe<sub>0.1</sub>Mn<sub>0.5</sub>O<sub>2</sub> (NFM) is a promising candidate material for sodium-ion batteries (SIBs) because of high theoretical capacity (220 mAh g<sup>−1</sup>), but largely suffers from rapid capacity decay due to severe phase transition caused by unstable transition metal (TM) layer gliding and anisotropic lattice strain accumulation upon cycling. Herein, we propose an enthalpy-doping strategy to precisely manipulate the local coordination ordering structure, thereby stabilize the TMO<sub>6</sub> octahedral framework in the O3-type Na<sub>0.9</sub>Ni<sub>0.35</sub>Zn<sub>0.05</sub>Fe<sub>0.1</sub>Mn<sub>0.3</sub>Ti<sub>0.2</sub>O<sub>2</sub> (NZFMT). Our findings demonstrate that the negative enthalpy characteristics of dopants reduce the <em>ΔH<sub>mix</sub></em> of TM layers, thereby strengthening cation-anion interactions and promoting the formation of an ordered lattice structure. As anticipated, this tailored structure strategy favorably stabilizes layered structure to resist severe phase transition, leading to remarkable electrochemical improvements. The optimized NZFMT delivers a high capacity of 162.3 mAh g<sup>−1</sup> with a prominent capacity retention of 96.3% after 100 cycles at 1 C (vs. 62.5% for NFM). Furthermore, the practical feasibility of an Ampere-hour-scale NZFMT||HC pouch cell is demonstrated by an energy density of 148 Wh kg<sup>−1</sup>, along with outstanding cycling stability (80.5% retention after 200 cycles at 0.5 C), outperforming many state-of-the-art O3-type cathodes. This work provides a universal enthalpy-mediated stabilization approach for designing high-energy-density SIB cathodes.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"93 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145194941","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}
Yuankai Ren , Ming Huang , Genlin Liu , Yun Zhao , Billy Wu , Yatish Patel , Frederic Cegla , Bo Lan
{"title":"Decoding coupled mechanical–electrochemical responses in multi-layer batteries via generalized ultrasonic dynamics","authors":"Yuankai Ren , Ming Huang , Genlin Liu , Yun Zhao , Billy Wu , Yatish Patel , Frederic Cegla , Bo Lan","doi":"10.1016/j.ensm.2025.104618","DOIUrl":"10.1016/j.ensm.2025.104618","url":null,"abstract":"<div><div>Characterizing and understanding internal battery physics is essential for stability, safety, and recyclability. Ultrasound provides a non-destructive solution by encoding battery dynamics into mechanical waves. However, the complex multi-layer structure and coupled mechanical–electrochemical behaviors of commercial cells hinder standardized and physically interpretable ultrasonic testing. This study presents a unified ultrasonic framework for multi-layer pouch cells, linking wave dynamics to battery structures, materials, and states across frequency and time domains. Inspired by electrochemical impedance spectroscopy, we examine structure- and state–waveform relationships of batteries under various excitation conditions, decoding ultrasonic responses related to mechanical and electrochemical factors in a generalizable manner. Using first-principles modeling and frequency sweep experiments, we identify battery-specific frequency bandstructures and wave modulation signatures tied to cell architecture and cathode chemistry, allowing mechanical discrimination of these factors in electrochemically steady states. In-operando tests demonstrate that changes in localized ultrasonic resonance associated with shifting bandstructure can map variations in battery state of charge, with the evolution of anode material stiffness as a key driving mechanism. This work establishes a physics-grounded foundation for understanding wave–battery interactions and is expected to guide the development of high-sensitivity, task-specific tools and diagnostic strategies across the in-laboratory, post-manufacture, and in-service stages of a battery’s lifecycle.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104618"},"PeriodicalIF":20.2,"publicationDate":"2025-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145103726","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}
Hebang Li, Lulu Deng, Yanhui Zhang, Kui Chen, Yuanlong Guo, Qinqin Xu, Mingwei Xu, Haibo Xie, Lei Wang
{"title":"Synergistic Biomass Electrolyte via Mechanochemistry Enables Ultralong-Life Dendrite-Free Zinc Anodes","authors":"Hebang Li, Lulu Deng, Yanhui Zhang, Kui Chen, Yuanlong Guo, Qinqin Xu, Mingwei Xu, Haibo Xie, Lei Wang","doi":"10.1016/j.ensm.2025.104639","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104639","url":null,"abstract":"Zinc metal, a promising anode for aqueous zinc-ion batteries (AZIBs) due to its high capacity, low cost, and safety, suffers from irreversibility caused by side reactions and dendrite growth. While electrolyte additives offer a solution, designing low-cost, green additives remains challenging. Herein, we introduce a novel, multifunctional electrolyte (CSZE) prepared via a solvent-free ball milling mechanochemical process using microcrystalline cellulose (MCC), succinic anhydride (SAD), and ZnSO₄ (ZS). This one-pot solid-phase synthesis leverages ZS as both catalyst and electrolyte solute. The resulting cellulose succinate ester (CSAE) and succinic acid (SA) exhibit a synergistic effect, promoting close Zn²⁺ binding and uniform deposition, surpassing the performance of either component alone. Carboxyl and hydroxyl groups within CSAE/SA facilitate strong adsorption on the Zn anode, effectively shielding it from dendrite formation and corrosion. Consequently, the Zn anode achieves exceptional reversibility for 3666 h at 1 mA cm⁻²/1 mAh cm⁻². Paired with a MnO₂ cathode, the full cell retains 79.75% capacity after 4000 cycles at 5 A g⁻¹. Life-cycle assessment further demonstrates a 22.64% reduction in global warming potential versus conventional electrolytes. This work presents a sustainable strategy utilizing abundant lignocellulosic biomass for high-performance, reversible AZIBs.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"18 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145195103","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":"Hydrogen Bonding at MXene/Electrolyte Interface Enables Stable Ammonium Ion Energy Storage","authors":"Xiaofeng Zhang, Qian Zhang, Zihua Wang, Peiao Lu, Jiakun Luo, Wei Xu, Yuhang Zhao, Yichen Zhang, Kui-Qing Peng","doi":"10.1016/j.ensm.2025.104638","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104638","url":null,"abstract":"Aqueous ammonium ion (NH<sub>4</sub><sup>+</sup>) hybrid supercapacitors (AAHSCs) have attracted much attention due to their environmental friendliness and excellent electrochemical performance, but the mechanism of NH<sub>4</sub><sup>+</sup> energy storage of AAHSCs has been unknown. In this work, Ti<sub>3</sub>C<sub>2</sub>T<em><sub>x</sub></em> films were prepared by vacuum filtration and used as cathode materials for AAHSC. The charge storage mechanism of Ti<sub>3</sub>C<sub>2</sub>T<em><sub>x</sub></em> films in different electrolyte solutions was systematically analyzed by means of ex-situ techniques and theoretical calculations. These analyses revealed an H–bonding (N–H…O) interaction between NH<sub>4</sub><sup>+</sup> and oxygen-containing functional groups, elucidating the reason for the excellent electrochemical performance of AAHSCs. DFT and MD calculations further verified the existence of H–bonds, which act as a channel for charge transfer and facilitate the transfer of electrons from NH<sub>4</sub><sup>+</sup> to O–atoms. The Ti<sub>3</sub>C<sub>2</sub>T<em><sub>x</sub></em> film//AC-AAHSC assembled with 1 M (NH<sub>4</sub>)<sub>2</sub>SO<sub>4</sub> as the electrolyte solution has a high specific capacitance of 84.3 F/g at a current density of 1 A/g and excellent cycling stability of 96.2% (10,000 cycles). It has a high energy density of 108 Wh/kg at a power density of 2,160 W/kg. This work lays the theoretical foundation for the construction of high-performance MXene-based AAHSCs devices.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"6 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189165","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}
Ying Li, Yingzi Hua, Shuangyang Cai, Rong Zhou, Mengyao Wang, Zhenzhen Wei, Yan Zhao
{"title":"Separator’s Contribution to the Ion Transport in Lithium Batteries","authors":"Ying Li, Yingzi Hua, Shuangyang Cai, Rong Zhou, Mengyao Wang, Zhenzhen Wei, Yan Zhao","doi":"10.1016/j.ensm.2025.104636","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104636","url":null,"abstract":"The performance and safety of lithium batteries are heavily dependent on the transport efficiency and deposition uniformity of lithium ions (Li<sup>+</sup>). As an essential component of lithium batteries, the separator’s physical structure and chemical characteristics significantly affect Li<sup>+</sup> transport. Herein, the influence of separators on Li<sup>+</sup> transport and design strategies for ion transport regulation are first elaborated at the mechanistic level along the Li<sup>+</sup> transport path. Subsequently, the research progress of the current work on Li<sup>+</sup> transport regulation is systematically reviewed by categorizing the improvement approaches, with comprehensive discussions on their respective advantages, limitations, and application scopes. Finally, it is concluded that future research should focus on the multifunctionalization with performance breakthroughs, as well as the cost, reliability and compatibility for industrial implementation, in order to transform laboratory innovations into industrial applications.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"32 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145189169","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}
Hao Tong, Libo Li, Yangmingyue Zhao, Hang Yang, Suo Li, Zhixuan Wang, Wenhao Xu, Wenyi Lu, Xiangrui Deng
{"title":"UV-Assisted Rapid Polymerization of Poly(Tannic Acid)-Silver Layers for Design Lithiophilic Layers in Anode-Free Lithium Metal Batteries","authors":"Hao Tong, Libo Li, Yangmingyue Zhao, Hang Yang, Suo Li, Zhixuan Wang, Wenhao Xu, Wenyi Lu, Xiangrui Deng","doi":"10.1016/j.ensm.2025.104633","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104633","url":null,"abstract":"Anode-free lithium metal batteries (AFLMBs) enhance energy density by using bare copper (Cu) foils as the anode. However, they face challenges due to irreversible lithium (Li) plating caused by the inherent lithiophobicity of the materials. In this study, we present an ultraviolet-assisted in-situ polymerization strategy to create a poly(tannic acid) film embedded with silver (Ag) nanospheres (PTA@Ag-Cu) in just 15 minutes. The PTA film improves the wettability of the electrolyte, reducing the contact angle by 50.6%, and accelerates Li<sup>+</sup> desolvation. The Ag nanoparticles (21 nm) lower the nucleation overpotential to 10 mV compared to 150 mV for bare Cu, through the formation of a lithiophilic LiAg alloy. The charge-transfer dynamics and embedded electric fields, which are verified by density functional theory (DFT), contribute to the uniform deposition of Li, as evidenced by in situ optical microscopy. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) indicates a synergistic regulation of Li<sup>+</sup> flux at the atomic level by the combination of Ag and molecular-level interactions from PTA. The PTA@Ag-Cu||LiFePO<sub>4</sub> configuration achieves 61.2% capacity retention after 100 cycles at a rate of 1 C-rate without pre-lithiation. The preparation of PTA@Ag-Cu using UV-assisted polymerization is economical, time-saving, and suitable for large-scale production. This work introduces a photo-induced dual-functional interface that addresses AFLMB degradation through integrated electric field engineering, making it compatible with roll-to-roll battery manufacturing.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"9 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145134612","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}
Xingmin He , Shuai Zheng , Kai Sun , Yi He , Dan Yang , Anmin Wang , Yasen Hao , Peng Tan
{"title":"Operando electrode-scale stress characterization revealing the Li+ insertion mechanism of graphite anode","authors":"Xingmin He , Shuai Zheng , Kai Sun , Yi He , Dan Yang , Anmin Wang , Yasen Hao , Peng Tan","doi":"10.1016/j.ensm.2025.104629","DOIUrl":"10.1016/j.ensm.2025.104629","url":null,"abstract":"<div><div>As a preferred anode material for lithium-ion batteries, a deeper understanding of the lithiation mechanism in graphite is essential for advancing novel optimization strategies. In this study, the lattice evolution information traditionally obtained through techniques such as X-ray diffraction and neutron powder diffraction is innovatively translated into stress signals for analysis, providing mechanical insights into the Li⁺ intercalation mechanism in graphite. The dynamic lithiation behavior of graphite particle assemblies is simulated using the Monte Carlo method, and combined with in situ X-ray diffraction and high-resolution transmission electron microscopy, the mechanical–electrochemical mapping relationship during lithiation is systematically elucidated. The lithiation process of graphite exhibits three distinct mechanical stages: C→LiC<sub>30</sub>, LiC<sub>30</sub>→LiC<sub>12</sub>, and LiC<sub>12</sub>→LiC<sub>6</sub>. Notably, during the transitions between the first/second and second/third stages, significantly differentiated mechanical signatures are observed, which deviate from theoretical predictions. Further analysis reveals that the former originates from a rapid phase separation process, while the latter is driven by lattice reconstruction induced by lithium intercalation. These two phenomena can be well explained by the Rüdorff–Hofmann interlayer intercalation model and the Daumas–Herold domain wall migration mechanism, respectively. The presence of such stage-specific mechanical responses suggests that distinct intercalation mechanisms govern different stages of graphite lithiation. The experimental findings presented in this work contribute to a multidimensional and comprehensive understanding of the graphite lithiation mechanism.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"82 ","pages":"Article 104629"},"PeriodicalIF":20.2,"publicationDate":"2025-09-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145116641","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}