Energy Storage Materials最新文献

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Fine-tuning for rapid capacity estimation of lithium-ion batteries 锂离子电池容量快速估算的微调
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-31 DOI: 10.1016/j.ensm.2025.104425
Benjamin Nowacki, Thomas Schmitt, Phillip Aquino, Chao Hu
{"title":"Fine-tuning for rapid capacity estimation of lithium-ion batteries","authors":"Benjamin Nowacki, Thomas Schmitt, Phillip Aquino, Chao Hu","doi":"10.1016/j.ensm.2025.104425","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104425","url":null,"abstract":"The widespread adoption of large-scale battery-powered technologies, such as electric vehicles and renewable energy storage systems, has led to growing interest in assessing their remaining usability after years of operation. As these systems age, state-of-health estimation becomes crucial for ensuring reliability and safety, and for extending life through second-use applications. However, current methods — spanning physics-based, empirical, and data-driven approaches — face challenges, including insufficient labeled data, high resource costs, and poor generalizability across diverse usage conditions. Data-driven models, in particular, struggle to extrapolate beyond their training domain, limiting their applicability in real-world scenarios. This work develops a fine-tuning framework to address these challenges, enabling rapid capacity estimation using short-duration (<span><math><mrow is=\"true\"><mo is=\"true\">≤</mo><mn is=\"true\">100</mn></mrow></math></span> seconds) features. Tested on two battery chemistries (LFP/Gr and NMC/Gr), the fine-tuned model achieves average mean-absolute-percent-errors of 2.592% and 3.094% on datasets collected from the respective chemistries. Compared to two baseline approaches, direct-transfer and target-only modeling, fine-tuning achieves a 25% reduction in estimation error in the target domain, on average. Domain differences are quantified using statistical measures such as Kullback–Leibler divergence and maximum mean discrepancy. These measures are found to correlate with fine-tuning performance, offering insights into domain compatibility. This study also analyzes the impact of feature selection, hyper-parameter tuning, and labeled data availability on fine-tuning efficacy, providing practical guidelines for real-world applications.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"25 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144747976","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}
引用次数: 0
Single Fluorosilane Ester Additive for F/Si-Enriched Inorganic Interphases Enabling Durable High-Voltage Graphite/LiCoO2 Pouch Cells 富F/ si无机界面的单氟硅烷酯添加剂实现持久的高压石墨/LiCoO2袋状电池
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-31 DOI: 10.1016/j.ensm.2025.104501
Shuai Chen, Lingling Huang, Jiajiong Liang, Haonan Huang, Yuling Fu, Jiayi Li, Xinqi Chen, Haolei Chen, Youhao Liao, Jiarong He, Weishan Li
{"title":"Single Fluorosilane Ester Additive for F/Si-Enriched Inorganic Interphases Enabling Durable High-Voltage Graphite/LiCoO2 Pouch Cells","authors":"Shuai Chen, Lingling Huang, Jiajiong Liang, Haonan Huang, Yuling Fu, Jiayi Li, Xinqi Chen, Haolei Chen, Youhao Liao, Jiarong He, Weishan Li","doi":"10.1016/j.ensm.2025.104501","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104501","url":null,"abstract":"An unstable interphase at the electrode/electrolyte interface poses a critical challenge for conventional carbonate-based electrolytes in achieving both enhanced energy density and long cycle life in lithium-ion batteries (LIBs). This study introduces ethyl 2, 2-difluoro-2-trimethylsilylacetate (DFAE) as a novel electrolyte additive designed to concurrently regulate the interphases of both the LiCoO<sub>2</sub> (LCO) cathode and graphite (Gra) anode. Incorporating 1 % DFAE into the electrolyte significantly improves the capacity retention across different cell configurations: from 36% to 84% in LCO/Li half-cells, from 57% to 96% in Gra/Li half-cell, and from 50% to 80% in LCO/Gra full-cell. Theoretical calculations and spectroscopic analyses demonstrate that DFAE preferentially undergoes redox reactions, leading to the formation of stable F/Si-enriched cathode electrolyte interphase (CEI) on LCO and solid electrolyte interphase (SEI) on graphite. This F/Si-rich nature enhances the structural robustness of the CEI/SEI, suppresses high-voltage-induced electrolyte degradation, and promotes efficient Li<sup>+</sup> (de)intercalation dynamics. Furthermore, DFAE exhibits strong affinity for detrimental F<sup>−</sup> ions, effectively scavenging acidic species and preserving the surface integrity of the LCO cathode. <em>In-situ</em> XRD analysis reveals that the CEI/SEI generated by DFAE significantly enhances the cycling reversibility of the LCO/Gra full-cell, facilitating more uniform Li<sup>+</sup> (de)intercalation and maintaining the overall integrity of both electrodes. The dual interphase modulation enabled by a single DFAE additive provides valuable insights into screening electrolyte additive for high-energy-density LIBs with superior performance.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"287 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144747919","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}
引用次数: 0
High-efficiency NaCl presodiation agent for sodium-ion batteries 钠离子电池用高效NaCl预沉淀剂
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-29 DOI: 10.1016/j.ensm.2025.104500
Le Hu, Pei Hu, Qiongfang Zhang, Jianlong Cong, Wei Su, Yibin Ren, Yuelin Kong, Junyao Zhang, Zhen Li, Yunhui Huang
{"title":"High-efficiency NaCl presodiation agent for sodium-ion batteries","authors":"Le Hu, Pei Hu, Qiongfang Zhang, Jianlong Cong, Wei Su, Yibin Ren, Yuelin Kong, Junyao Zhang, Zhen Li, Yunhui Huang","doi":"10.1016/j.ensm.2025.104500","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104500","url":null,"abstract":"In the ordinary sodium-ion batteries, irreversible sodium loss during the initial cycle is inevitable, significantly reducing the initial Coulombic efficiency and operational lifespan. In this work, sodium chloride (NaCl) was developed as a low-cost, non-toxic and high-efficient presodiation agent for Na-ion batteries. The facilely prepared NaCl/Ketjen Black composite can deliver a presodiation capacity of 457 mAh g<sup>−1</sup> below 4.2 V. Innovatively, instead of direct cathode incorporation, NaCl is applied as a presodiation layer on commercial polypropylene separators, ensuring homogeneous sodium compensation while avoiding structural damage to the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode. In Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>||hard carbon full cells, this approach fully offsets initial sodium loss, achieving a 46.8% increase in initial discharge capacity (115 mAh g<sup>−1</sup>) and an ideal 100% initial Coulombic efficiency. Mechanistic studies confirm NaCl’s irreversible decomposition without harmful Cl<sub>2</sub> byproducts, while residual Cl species do not impede charge transfer. The strategy boosts energy density by 29% (186 Wh kg<sup>−1</sup>) and demonstrates scalability for practical applications. This work presents a cost-effective and industrially scalable strategy to mitigate irreversible sodium loss, advancing the development of high-energy-density and long-cycle-life sodium-ion batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"710 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720214","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}
引用次数: 0
Challenges and rational design approaches of high-energy-density rechargeable zinc-sulfur batteries 高能量密度可充电锌硫电池的挑战与合理设计途径
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-28 DOI: 10.1016/j.ensm.2025.104498
Jiguo Tu , Jing Wang , Libo Chen , Dongbai Sun , Wei Wang
{"title":"Challenges and rational design approaches of high-energy-density rechargeable zinc-sulfur batteries","authors":"Jiguo Tu ,&nbsp;Jing Wang ,&nbsp;Libo Chen ,&nbsp;Dongbai Sun ,&nbsp;Wei Wang","doi":"10.1016/j.ensm.2025.104498","DOIUrl":"10.1016/j.ensm.2025.104498","url":null,"abstract":"<div><div>Rechargeable zinc-sulfur (Zn-S) batteries have attracted considerable attention owing to their advantages of low cost, high safety, and high energy density. Despite facing critical challenges such as low electrical conductivity, sluggish reaction kinetics, and polysulfide shuttle effect, the latest advancements in active material design and electrolyte engineering have brought about significant breakthroughs. In this review, we first delve into the electrochemistry differences and key challenges of Zn-S batteries in both aqueous and nonaqueous electrolyte systems. Then, several effective approaches at the cathode side, including electrocatalytic function, host architecture design, selenium/tellurium incorporating, hybrid configuration with Cu<sup>2+</sup> charge carrier, and electrolyte engineering, are summarized to improve reaction kinetics and cycling stability. Further breakthroughs will rely on integrating S structure/morphology regulation, interface design, anode optimization and multi-scale characterizations. This review contributes to more comprehensive understanding in the reaction mechanisms and constructive strategies, which is expected to further facilitate the rapid development and practical application of high-energy-density Zn-S batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104498"},"PeriodicalIF":20.2,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720215","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}
引用次数: 0
Designing bionic ion pumps in the electrolyte for stable Zn metal anodes 稳定锌金属阳极电解液仿生离子泵的设计
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-28 DOI: 10.1016/j.ensm.2025.104499
Yanjiao Cao , Shifeng Huang , Yaodong Huo , Zihan Liu , Mengjing Li , Penghui Tian , Tuotuo Ma , Xiaojun Gu , Yuliang Gao
{"title":"Designing bionic ion pumps in the electrolyte for stable Zn metal anodes","authors":"Yanjiao Cao ,&nbsp;Shifeng Huang ,&nbsp;Yaodong Huo ,&nbsp;Zihan Liu ,&nbsp;Mengjing Li ,&nbsp;Penghui Tian ,&nbsp;Tuotuo Ma ,&nbsp;Xiaojun Gu ,&nbsp;Yuliang Gao","doi":"10.1016/j.ensm.2025.104499","DOIUrl":"10.1016/j.ensm.2025.104499","url":null,"abstract":"<div><div>Zn metal anodes with dendrite growth that driven by heterogeneous ion distribution, limit their application in high-energy-density batteries. Here, we pioneer liquid metal-organic framework (MOF) as a built-in bionic ion pump into the electrolyte, unlike conventional solid MOF, to stabilize Zn metal anodes. The inherent pores of liquid MOF of UiO-66 and the strong electrostatic interactions between the oxygen-containing atoms and Zn<sup>2+</sup> can effectively promote the homogenization and pumping of Zn<sup>2+</sup>, thus achieving the uniform bulk ion distribution. Meanwhile, the exposed metal sites and the anchoring effect of -CH<sub>2</sub> on OTf⁻ further strengthen ion regulation effect. Consequently, Zn dendrites are effectively suppressed, and the V<sub>2</sub>O<sub>5</sub>||Zn pouch cell exhibits a capacity retention of 80.1 % and low gassing behavior after 600 cycles at 1 A g⁻<sup>1</sup> compared to the control group (56.6 %). Remarkably, the liquid UiO-66 also demonstrates universal applicability in Li and Na metal anodes, where the capacity retention of the LiFePO<sub>4</sub>||Li cell improves from 57.8 % to 92.8 % after 150 cycles, and the Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>||Na cell shows an increase from 82.7 % to 94.1 % after 5600 cycles.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104499"},"PeriodicalIF":20.2,"publicationDate":"2025-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144720216","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}
引用次数: 0
Facile Gel Polymer Electrolyte Enabling Fast Charging of Quasi-Solid-State Lithium Metal Batteries at −40°C 在- 40°C下实现准固态锂金属电池快速充电的易溶凝胶聚合物电解质
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-27 DOI: 10.1016/j.ensm.2025.104494
Xuanfeng Chen, Shuai Zhao, Weihong Liang, Feixiang Wu
{"title":"Facile Gel Polymer Electrolyte Enabling Fast Charging of Quasi-Solid-State Lithium Metal Batteries at −40°C","authors":"Xuanfeng Chen, Shuai Zhao, Weihong Liang, Feixiang Wu","doi":"10.1016/j.ensm.2025.104494","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104494","url":null,"abstract":"Gel polymer electrolytes (GPEs) are promising for lithium metal batteries (LMBs) due to their high ionic conductivity and excellent mechanical properties. However, conventional GPEs often underperform at low temperatures and high rates. Herein, we develop a low-temperature fast-charging GPE (LFGPE) by incorporating LiPO<sub>2</sub>F<sub>2</sub> as an additive into a LiBF<sub>4</sub>/DOL/FEC-based precursor. The LFGPE exhibits a high ionic conductivity of 0.49 mS cm<sup>−1</sup> (−40°C). Notably, LiPO<sub>2</sub>F<sub>2</sub> participates in Li<sup>+</sup> solvation structures at −40°C, competing with poly-DOL and BF<sub>4</sub><sup>−</sup>, which weakens their tight coordination with Li<sup>+</sup>. Moreover, LiPO<sub>2</sub>F<sub>2</sub> exhibits a narrow gap of HOMO-LOMO energy level, preferentially decomposing and inducing formation of P-containing solid electrolyte interphase (SEI). Thus, the LFGPE system generates inorganic-rich SEI containing Li<sub>3</sub>PO<sub>4</sub>, which accelerates Li<sup>+</sup> desolvation and Li<sup>+</sup> migration across the SEI, improving Li<sup>+</sup> transport kinetics and interfacial stability at −40°C. Consequently, Li//LiCoO<sub>2</sub> (LCO) cells with the LFGPE yield a high reversible capacity of 128 mAh g<sup>−1</sup> at 1 C (−40°C). Impressively, the LFGPE even enables Li//LCO cells to sustain over 200 cycles under 3 C charging/1 C discharging at −40°C. This work offers an effective approach of simultaneously enhancing ion transport kinetics and interfacial stability to develop quasi-solid-state LMBs with low-temperature fast charging capability.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"47 17 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144712439","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}
引用次数: 0
Quantitative Decoupling of Electrode Expansion, Electrolyte Depletion, and Dead Sodium in Low-Temperature Storage Cylindrical Sodium-Ion Cell 低温圆柱形钠离子电池中电极膨胀、电解液耗竭和死钠的定量解耦
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-27 DOI: 10.1016/j.ensm.2025.104495
Chaofan Tang, Xingming Fan, Jin Shi, Juya Zhong, Qinmeng Wang, Xueyi Guo
{"title":"Quantitative Decoupling of Electrode Expansion, Electrolyte Depletion, and Dead Sodium in Low-Temperature Storage Cylindrical Sodium-Ion Cell","authors":"Chaofan Tang, Xingming Fan, Jin Shi, Juya Zhong, Qinmeng Wang, Xueyi Guo","doi":"10.1016/j.ensm.2025.104495","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104495","url":null,"abstract":"Sodium-ion batteries (SIBs) exhibit promising potential for low temperature (LT) energy storage, yet their capacity decay mechanisms under LT conditions remain insufficiently investigated. Herein, we report the coupled mechanisms of Full cell - Electrode - Material/Interface, and quantitative analysis of electrode expansion, electrolyte depletion, and dead sodium of 100% SOC NaCuFeMnO<sub>2</sub> || Hard Carbon cylindrical SIBs during prolonged storage at -20 ℃. Based on multimodal in situ/ex situ characterization methodologies, we found a new capacity fade mechanism of LT storage, which reversible capacity loss (1-3 months) dominated by electrolyte depletion and charge transfer polarization, transitioning to irreversible capacity loss caused by interface deterioration and dead sodium accumulation (&gt;3 months). Interestingly, we quantitatively analyzed the changes in the expansion rate and dead sodium content of the anode electrode at different positions (inner, center, and outer region) and revealed unprecedented heterogeneous degradation patterns: anode electrode degradation dominates system failure, inner region and exhibit higher expansion and greater dead sodium accumulation compared to center and outer regions. Consequently, optimizing cell performance under LT conditions necessitates careful optimization of coating parameters, winding architectures, and electrolyte filling volumes during cell design.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"188 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144712440","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}
引用次数: 0
Bilayer Interphases Engineering Enabling Practical Anode-Free Lithium Metal Batteries 实现实用无阳极锂金属电池的双层界面工程
IF 20.4 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-27 DOI: 10.1016/j.ensm.2025.104497
Fan Hu, Lin Chen, Bin Liao, Hao Guo, Haikuo Wang, Hongshuai Cao, Xiaoping Ouyang
{"title":"Bilayer Interphases Engineering Enabling Practical Anode-Free Lithium Metal Batteries","authors":"Fan Hu, Lin Chen, Bin Liao, Hao Guo, Haikuo Wang, Hongshuai Cao, Xiaoping Ouyang","doi":"10.1016/j.ensm.2025.104497","DOIUrl":"https://doi.org/10.1016/j.ensm.2025.104497","url":null,"abstract":"The continuous lithium consumption between the interphase of electrolyte and lithium metal has primary influence for limited lifespan of anode-free lithium metal batteries (AFLMBs). Herein, an effective concept of using bilayer interphase engineering to regulate the nanoscale structure of the deposited Li has been proposed to enhance the cycling lifespan of AFLMBs. The nanoscale bilayer structure is tailored through magnetron sputtering: the inner layer is dominated by high-entropy alloy (HEA, CuInCdSnZn) to improve lithiophilicity while the outer layer contains LiF to improve homogeneity, leading to reversible Li plating/stripping and mitigated reconstruction of solid-electrolyte interphase (SEI). Benefiting from the bilayer design, the coin cell consisting of a Cu-HEA-F anode and a high-loading cathode (NCM811, 10.5 mg cm<sup>−2</sup>) performs 35 cycles at discharge rates of 0.5 C, significantly outperforming for bare Cu. Large-capacity pouch cells (1.5/2.5 Ah) with high-loading cathode (7.6 mAh cm<sup>−2</sup>, single side) and lean electrolyte of 1.6 g Ah<sup>−1</sup>, achieve high-energy density of 360/380 Wh kg<sup>−1</sup> and lifespan about 20 cycles.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"53 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2025-07-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144712438","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}
引用次数: 0
Design of d/p-band center regulation guided by suppressing electron interference for ultra-stable iron/manganese-based mixed phosphate cathode 抑制电子干扰的超稳定铁/锰基混合磷酸盐阴极d/p波段中心调控设计
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-26 DOI: 10.1016/j.ensm.2025.104496
Yian Wang , Yulei Sui , Wenbin Fei , Mengting Deng , Yichao Shi , Zonglin Yang , Zhiyi Hu , Xiaoping Zhang , Shengkui Zhong , Ling Wu
{"title":"Design of d/p-band center regulation guided by suppressing electron interference for ultra-stable iron/manganese-based mixed phosphate cathode","authors":"Yian Wang ,&nbsp;Yulei Sui ,&nbsp;Wenbin Fei ,&nbsp;Mengting Deng ,&nbsp;Yichao Shi ,&nbsp;Zonglin Yang ,&nbsp;Zhiyi Hu ,&nbsp;Xiaoping Zhang ,&nbsp;Shengkui Zhong ,&nbsp;Ling Wu","doi":"10.1016/j.ensm.2025.104496","DOIUrl":"10.1016/j.ensm.2025.104496","url":null,"abstract":"<div><div>Iron/manganese-based mixed phosphate, characterized by its remarkable energy density and structural stability, emerges as a formidable contender for the next generation of commercial sodium-ion battery cathode materials. However, due to the 3d<sup>5</sup> electronic configuration of Mn<sup>2+</sup>, the d-orbitals are in a half-filled state, which results in uneven charge distribution. Therefore, we propose the design of d/p-band center regulation for Na<sub>4</sub>Fe<sub>2</sub>Mn(PO<sub>4</sub>)<sub>2</sub>(P<sub>2</sub>O<sub>7</sub>). As a result, the electronic interference resulting from electronic localization is effectively mitigated. Through lattice reconstruction, the internal strain within the material is alleviated, and the Mn Jahn-Teller synergistic distortion is effectively suppressed, thereby enhancing the structural stability and electronic transition capability. Furthermore, the introduction of defect engineering for charge compensation alleviates the restricted diffusion of sodium ions due to the exacerbation of P<sub>2</sub>O<sub>7</sub> distortion. Based on this, the modified iron/manganese-based mixed phosphate shows high energy density and ultra-long cycle stability, indicating significant potential for large-scale applications in sodium-ion batteries.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104496"},"PeriodicalIF":20.2,"publicationDate":"2025-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144710848","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}
引用次数: 0
High-valent cation-mediated inorganic-rich gradient SEI for highly stable solid state polymer lithium metal batteries 高稳定固态聚合物锂金属电池中高价阳离子介导的富无机梯度SEI
IF 20.2 1区 材料科学
Energy Storage Materials Pub Date : 2025-07-26 DOI: 10.1016/j.ensm.2025.104493
Pengfei Zhai , Shuangquan Qu , Zidan Cao , Heng Mao
{"title":"High-valent cation-mediated inorganic-rich gradient SEI for highly stable solid state polymer lithium metal batteries","authors":"Pengfei Zhai ,&nbsp;Shuangquan Qu ,&nbsp;Zidan Cao ,&nbsp;Heng Mao","doi":"10.1016/j.ensm.2025.104493","DOIUrl":"10.1016/j.ensm.2025.104493","url":null,"abstract":"<div><div>Solid-state polymer lithium metal batteries (SSPLMBs) are widely regarded as the most promising next-generation energy storage technologies due to the high energy density and intrinsic safety. However, common organic-rich solid electrolyte interphase (SEI) exhibits the inhomogeneous and sluggish Li<sup>+</sup> transport at the lithium anode interface, and the high nucleation barrier for lithium atoms, collectively promoting Li dendritic growth, thereby hindering the large-scale deployment of SSPLMBs. Herein, we propose a high-valence cation-mediated strategy to construct an inorganic-rich gradient (SEI) by introducing In(NO<sub>3</sub>)<sub>3</sub> as an additive into a polyethylene oxide-based electrolyte (PEO-In(NO<sub>3</sub>)<sub>3</sub>). Specifically, trivalent In<sup>3+</sup> reacts with lithium to form a lithiophilic Li-In alloy underlayer, while simultaneously mediating anion enrichment at the lithium anode interface via enhanced electrostatic attraction, which facilitates formation of a lithiophobic top layer enriched with anion-derived LiF/Li<sub>3</sub>N components. The inorganic-rich gradient SEI architecture is established, and superior Li<sup>+</sup> diffusion kinetics and reduced energy barrier for lithium atom nucleation are achieved, synergistically enabling homogeneous lithium deposition morphology. Consequently, over one order of magnitude improvement in the lifespan of Li|PEO-In(NO<sub>3</sub>)<sub>3</sub>|LFP cell is achieved, demonstrating a 78.3 % capacity retention after 1000 cycles at 1 C, as compared to Li|PEO|LFP cell with common SEI. This study presents a novel avenue to the rational design of inorganic-rich gradient SEI.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"81 ","pages":"Article 104493"},"PeriodicalIF":20.2,"publicationDate":"2025-07-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144710652","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}
引用次数: 0
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