Pub Date : 2026-03-01Epub Date: 2026-02-13DOI: 10.1016/j.ensm.2026.104988
Ying Hui Li , Qiang Qiang Zhang , Bu Guang Zhou, Wei Ding, Xin Yue Guo, Yu Xin Tang, Li Ming Wang, Dong Xiao Ji, Xiao Hong Qin
Fiber zinc–air batteries (FZABs) have emerged as promising power sources for wearable and portable electronics. However, their practical deployment remains limited by persistent anode instability caused by dendrite formation, which hampers further technological advancement. Here, we address this challenge by engineering an even interfacial electric field through the modification of electronically conjugated functional groups in both the fibrous zinc anode and gel electrolyte. This interfacial field is constructed between a positively charged -NH2-functionalized conductive fibrous zinc anode and a negatively charged -COOH-rich gel electrolyte, which promotes uniform Zn2+ flux across the curved fiber surfaces and effectively suppresses dendrite formation. Concurrently, the -COOH-functionalized gel electrolyte enhances the water retention capability of the system. These synergistic effects enable symmetric Zn//Zn cells to achieve stable operation for 280 h at 0.5 mA cm-2. Notably, the FZABs based on this design exhibit an extended cycling life of 55 h at 0.5 mA cm-2 while maintaining a high energy efficiency of 90%, ranking among the top performance metrics reported for flexible FZABs to date. Furthermore, by seamlessly integrating with conventional textiles, this battery demonstrates its applicability in powering a flexible fiber-based sweat glucose monitoring system, thereby establishing a new paradigm for wearable power sources.
光纤锌空气电池(FZABs)已成为可穿戴和便携式电子产品的有前途的电源。然而,由于枝晶形成引起的持续阳极不稳定,限制了它们的实际应用,从而阻碍了技术的进一步发展。在这里,我们通过在纤维锌阳极和凝胶电解质中修饰电子共轭官能团来设计均匀的界面电场来解决这一挑战。该界面场在带正电荷的- nh2功能化导电纤维锌阳极和带负电荷的- cooh富凝胶电解质之间构建,促进了Zn2+在弯曲纤维表面的均匀通量,并有效抑制了枝晶的形成。同时,- cooh功能化的凝胶电解质增强了体系的保水能力。这些协同效应使对称Zn//Zn电池在0.5 mA cm-2下稳定运行280小时。值得注意的是,基于这种设计的FZABs在0.5 mA cm-2下的循环寿命延长了55小时,同时保持了90%的高能效,是迄今为止柔性FZABs的最佳性能指标之一。此外,通过与传统纺织品无缝集成,这种电池证明了它在为柔性纤维汗液葡萄糖监测系统供电方面的适用性,从而为可穿戴电源建立了一个新的范例。
{"title":"Conjugated functional groups engineer buckled interfacial electric field for dendrite-free Zn deposition in fiber Zn-air batteries","authors":"Ying Hui Li , Qiang Qiang Zhang , Bu Guang Zhou, Wei Ding, Xin Yue Guo, Yu Xin Tang, Li Ming Wang, Dong Xiao Ji, Xiao Hong Qin","doi":"10.1016/j.ensm.2026.104988","DOIUrl":"10.1016/j.ensm.2026.104988","url":null,"abstract":"<div><div>Fiber zinc–air batteries (FZABs) have emerged as promising power sources for wearable and portable electronics. However, their practical deployment remains limited by persistent anode instability caused by dendrite formation, which hampers further technological advancement. Here, we address this challenge by engineering an even interfacial electric field through the modification of electronically conjugated functional groups in both the fibrous zinc anode and gel electrolyte. This interfacial field is constructed between a positively charged -NH<sub>2</sub>-functionalized conductive fibrous zinc anode and a negatively charged -COOH-rich gel electrolyte, which promotes uniform Zn<sup>2+</sup> flux across the curved fiber surfaces and effectively suppresses dendrite formation. Concurrently, the -COOH-functionalized gel electrolyte enhances the water retention capability of the system. These synergistic effects enable symmetric Zn//Zn cells to achieve stable operation for 280 h at 0.5 mA cm<sup>-2</sup>. Notably, the FZABs based on this design exhibit an extended cycling life of 55 h at 0.5 mA cm<sup>-2</sup> while maintaining a high energy efficiency of 90%, ranking among the top performance metrics reported for flexible FZABs to date. Furthermore, by seamlessly integrating with conventional textiles, this battery demonstrates its applicability in powering a flexible fiber-based sweat glucose monitoring system, thereby establishing a new paradigm for wearable power sources.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104988"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146209588","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}
Pub Date : 2026-03-01Epub Date: 2026-02-14DOI: 10.1016/j.ensm.2026.104987
Eun Hwan Noh , Seongeun Oh , Hyeri Kang , Miseung Kim , Jee Ho Ha , Ho-Jeong Ji , Won-Jin Kwak , Eunji Lee , Se Hun Joo , Seok Ju Kang
Achieving ultra-high active material loading in lithium iron phosphate (LiFePO₄, LFP) cathodes is essential for enhancing the performance of LFP-based lithium-ion batteries. However, conventional cathodes typically contain around 20% inactive binders and conductive additives. Here, we present a bifunctional binder composed of poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and polyethylene glycol (PEG), reinforced with single-walled carbon nanotubes (SWCNTs) to provide strong adhesion, thermal stability, and high electronic conductivity while minimizing inactive content. By optimizing the PEDOT:PSS/PEG ratio, LFP cathodes with 4 wt% binder reach 96% active material loading, delivering a specific capacity of ∼160 mAh g⁻¹ and excellent rate performance (∼106 mAh g⁻¹ at 8 C). Incorporating SWCNTs enables further reduction of binder content to 2 wt% while maintaining robust cohesion and high conductivity, resulting in strong rate capability of ∼131 mAh g⁻¹ at 8 C and stable cycling over 1000 cycles. Even electrodes with 99% active material operate reliably on a graphite-coated Al current collector, achieving ∼132 mAh g⁻¹ at 8 C and ∼3.5 mAh cm⁻² areal capacity. Furthermore, full-cell evaluations with graphite anodes confirm the practical applicability of this binder system, achieving ∼125 mAh g⁻¹ at 8 C and long-term cycling stability even at 60 °C.
在磷酸铁锂(LiFePO₄,LFP)阴极中实现超高活性物质负载对于提高LFP基锂离子电池的性能至关重要。然而,传统的阴极通常含有约20%的非活性粘合剂和导电添加剂。在这里,我们提出了一种双功能粘合剂,由聚(3,4-乙烯二氧噻吩)聚苯乙烯磺酸盐(PEDOT:PSS)和聚乙二醇(PEG)组成,用单壁碳纳米管(SWCNTs)增强,以提供强附着力、热稳定性和高电子导电性,同时最大限度地减少非活性含量。通过优化PEDOT:PSS/PEG比率,4 wt%粘合剂的LFP阴极达到96%的活性物质负载,提供约160 mAh g⁻¹的比容量和出色的速率性能(8℃时约106 mAh g⁻¹)。加入SWCNTs可以进一步将粘合剂含量降低到2 wt%,同时保持强大的凝聚力和高导电性,从而在8℃时产生强大的速率能力- 131 mAh g⁻¹,并在1000次循环中稳定循环。即使是含有99%活性材料的电极,在石墨涂层的铝集流器上也能可靠地工作,在8℃时达到~ 132 mAh g⁻¹和~ 3.5 mAh cm⁻²的面积容量。此外,石墨阳极的全电池评估证实了这种粘合剂系统的实际适用性,在8℃下可以达到~ 125 mAh g⁻¹,即使在60℃下也可以长期循环稳定。
{"title":"Enabling ultra-high-loading LiFePO4 cathodes via a conductive binder architecture with minimized inactive content","authors":"Eun Hwan Noh , Seongeun Oh , Hyeri Kang , Miseung Kim , Jee Ho Ha , Ho-Jeong Ji , Won-Jin Kwak , Eunji Lee , Se Hun Joo , Seok Ju Kang","doi":"10.1016/j.ensm.2026.104987","DOIUrl":"10.1016/j.ensm.2026.104987","url":null,"abstract":"<div><div>Achieving ultra-high active material loading in lithium iron phosphate (LiFePO₄, LFP) cathodes is essential for enhancing the performance of LFP-based lithium-ion batteries. However, conventional cathodes typically contain around 20% inactive binders and conductive additives. Here, we present a bifunctional binder composed of poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) and polyethylene glycol (PEG), reinforced with single-walled carbon nanotubes (SWCNTs) to provide strong adhesion, thermal stability, and high electronic conductivity while minimizing inactive content. By optimizing the PEDOT:PSS/PEG ratio, LFP cathodes with 4 wt% binder reach 96% active material loading, delivering a specific capacity of ∼160 mAh g⁻¹ and excellent rate performance (∼106 mAh g⁻¹ at 8 C). Incorporating SWCNTs enables further reduction of binder content to 2 wt% while maintaining robust cohesion and high conductivity, resulting in strong rate capability of ∼131 mAh g⁻¹ at 8 C and stable cycling over 1000 cycles. Even electrodes with 99% active material operate reliably on a graphite-coated Al current collector, achieving ∼132 mAh g⁻¹ at 8 C and ∼3.5 mAh cm⁻² areal capacity. Furthermore, full-cell evaluations with graphite anodes confirm the practical applicability of this binder system, achieving ∼125 mAh g⁻¹ at 8 C and long-term cycling stability even at 60 °C.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104987"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146209590","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}
Pub Date : 2026-03-01Epub Date: 2026-01-30DOI: 10.1016/j.ensm.2026.104945
Chunhui Bi , Congzhen Xie , Qingyu Wang , Daoming Zhang , An Zhong , Hangchuan Cai , Yongxia Han , Jing Fu , Qi Li , Rui Wang
The growing demand for mainstream dielectric energy storage technologies requires dielectric polymers capable of stable operation at high temperature, which is limited by the inherent contradiction between thermal resistance and high-temperature insulation. While structural optimization of the main-chain can mitigate the trade-off, it nevertheless fails to disentangle the contradiction. Herein, we report a puzzle-like molecular design that assembles specific substituents on the original polymer backbone. We found that the structure and bonding sites of the substituents have a significant impact on their steric hindrance and electron-withdrawing effect, which is related to the electrical and thermal properties of polymers. Consequently, the optimal structure, by means of maintaining the polymer backbone, decouples the pending contradictions, and thus achieves excellent high-temperature capacitive performance, i.e., at 150 and 200°C, the discharged energy density exceeded 6.33 and 5.42 J cm−3 respectively, with the efficiency above 90%. This polymer design strategy has universality and is also applicable to other material fields, such as packaging dielectrics.
{"title":"Polymer dielectrics with customized substituent for high temperature capacitive energy storage","authors":"Chunhui Bi , Congzhen Xie , Qingyu Wang , Daoming Zhang , An Zhong , Hangchuan Cai , Yongxia Han , Jing Fu , Qi Li , Rui Wang","doi":"10.1016/j.ensm.2026.104945","DOIUrl":"10.1016/j.ensm.2026.104945","url":null,"abstract":"<div><div>The growing demand for mainstream dielectric energy storage technologies requires dielectric polymers capable of stable operation at high temperature, which is limited by the inherent contradiction between thermal resistance and high-temperature insulation. While structural optimization of the main-chain can mitigate the trade-off, it nevertheless fails to disentangle the contradiction. Herein, we report a puzzle-like molecular design that assembles specific substituents on the original polymer backbone. We found that the structure and bonding sites of the substituents have a significant impact on their steric hindrance and electron-withdrawing effect, which is related to the electrical and thermal properties of polymers. Consequently, the optimal structure, by means of maintaining the polymer backbone, decouples the pending contradictions, and thus achieves excellent high-temperature capacitive performance, <em>i.e.</em>, at 150 and 200°C, the discharged energy density exceeded 6.33 and 5.42 J cm<sup>−3</sup> respectively, with the efficiency above 90%. This polymer design strategy has universality and is also applicable to other material fields, such as packaging dielectrics.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104945"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146089605","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}
Silicon (Si)-based anode materials are considered the most promising next-generation anodes for lithium-ion batteries (LIBs). Nonetheless, in practical applications, Si anodes have encountered numerous challenges. A homogeneous silicon carbide (SiC) dispersoid was synthesized within the Si-based alloy using vacuum melting, sand milling, and Flash joule heating procedures. The integration of SiC facilitates the simultaneous resolution of key issues: low intrinsic conductivity, unstable solid electrolyte interphase (SEI), and significant volume expansion, which is accomplished by creating a swift and uniform charge-transport network, enhancing interfacial kinetics, and bolstering the mechanical integrity of the electrode, which is attributed to the synergistic effect of a highly conductive network formed by the in-situ generated defective SiC and the metallic phases (Sn/Bi), SiC's advantageous interfacial characteristics, exceptional mechanical strength, and dispersion strengthening effect. The half-cell exhibits an impressive capacity of 1881.69 mAh g−1 and maintains steady cycling for 400 cycles at a current density of 1.5 A g−1. The full cell utilizing Li1.2Ni0.13Co0.13Mn0.54O2, demonstrates a capacity of 251.71 mAh g−1 following 80 cycles at 0.33 A g−1. Meanwhile, excellent cycling stability is attained in all-solid-state batteries, delivering a capacity retention of 81.1% over 150 cycles. This work introduces an innovative triple synergistic mechanism that significantly enhances the electrochemical performance of Si-based anodes, facilitating their efficient manufacture and offering important insights for future investigations.
硅基负极材料被认为是最有前途的下一代锂离子电池负极材料。然而,在实际应用中,硅阳极遇到了许多挑战。采用真空熔炼、砂磨和闪速焦耳加热工艺,在硅基合金中合成了均匀的碳化硅分散体。SiC的集成有助于同时解决关键问题:低固有电导率,不稳定的固体电解质界面相(SEI),以及显著的体积膨胀,这是通过创建快速均匀的电荷传输网络来实现的,增强了界面动力学,增强了电极的机械完整性,这是由于原位生成的缺陷SiC和金属相(Sn/Bi)形成的高导电性网络的协同作用,SiC的有利界面特性。优异的机械强度和分散强化效果。该半电池的容量为1881.69 mAh g−1,在电流密度为1.5 a g−1的情况下可稳定循环400次。使用Li1.2Ni0.13Co0.13Mn0.54O2的完整电池在0.33 a g - 1下循环80次后的容量为251.71 mAh g - 1。同时,在全固态电池中获得了出色的循环稳定性,在150次循环中提供81.1%的容量保持率。这项工作引入了一种创新的三重协同机制,显著提高了硅基阳极的电化学性能,促进了它们的高效制造,并为未来的研究提供了重要的见解。
{"title":"Flash joule heating driven in-situ dispersoid synthesis: Mechanical-interfacial-conductive coupling mechanisms in silicon-based anodes","authors":"D.R. Lan, P.Y. Ou, S.Q. Pei, K.J. Liu, C.C. Li, M.C. Zhang, Y.X. Liu, S.N. He, L.N. She, Y.X. Yang, W.B. Du, H.G. Pan","doi":"10.1016/j.ensm.2026.104956","DOIUrl":"10.1016/j.ensm.2026.104956","url":null,"abstract":"<div><div>Silicon (Si)-based anode materials are considered the most promising next-generation anodes for lithium-ion batteries (LIBs). Nonetheless, in practical applications, Si anodes have encountered numerous challenges. A homogeneous silicon carbide (SiC) dispersoid was synthesized within the Si-based alloy using vacuum melting, sand milling, and Flash joule heating procedures. The integration of SiC facilitates the simultaneous resolution of key issues: low intrinsic conductivity, unstable solid electrolyte interphase (SEI), and significant volume expansion, which is accomplished by creating a swift and uniform charge-transport network, enhancing interfacial kinetics, and bolstering the mechanical integrity of the electrode, which is attributed to the synergistic effect of a highly conductive network formed by the in-situ generated defective SiC and the metallic phases (Sn/Bi), SiC's advantageous interfacial characteristics, exceptional mechanical strength, and dispersion strengthening effect. The half-cell exhibits an impressive capacity of 1881.69 mAh g<sup>−1</sup> and maintains steady cycling for 400 cycles at a current density of 1.5 A g<sup>−1</sup>. The full cell utilizing Li<sub>1.2</sub>Ni<sub>0.13</sub>Co<sub>0.13</sub>Mn<sub>0.54</sub>O<sub>2</sub>, demonstrates a capacity of 251.71 mAh g<sup>−1</sup> following 80 cycles at 0.33 A g<sup>−1</sup>. Meanwhile, excellent cycling stability is attained in all-solid-state batteries, delivering a capacity retention of 81.1% over 150 cycles. This work introduces an innovative triple synergistic mechanism that significantly enhances the electrochemical performance of Si-based anodes, facilitating their efficient manufacture and offering important insights for future investigations.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104956"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146101523","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}
The practical implementation of lithium-sulfur (Li-S) batteries with high energy density and low cost faces significant challenges stemming from the inherent sluggish redox kinetics and inefficient conversion reactions of lithium polysulfides (LiPSs). Recent breakthroughs in dual-atom catalysts (DACs) have opened new avenues for addressing these limitations, as these materials exhibit uniquely tailored electronic configurations, pronounced synergistic effects between active sites, and unparalleled atomic utilization efficiency. This comprehensive review critically examines the latest advancements in DACs applications for Li-S batteries, with particular emphasis on their multifunctional roles in LiPSs adsorption/conversion, shuttle mitigation and Li+ deposition. Through meticulous engineering of coordination environments, spatial distributions of active centers, and substrate structures, DACs verify extraordinary capabilities in accelerating sulfur conversion kinetics, facilitating charge transfer processes, and enhancing long-term cycling stability. Combining state-of-the-art theoretical calculation with characterization techniques, the discussion further unravels the fundamental catalytic mechanisms of DACs under extreme operating conditions. Finally, the review concludes by identifying existing challenges and future research directions. Most importantly, by establishing clear structure-performance correlations and synthesizing latest developments in DACs frontier, the contribution not only provides actionable guidelines for catalyst design but lays a theoretical foundation for rational development of advanced energy storage technologies.
{"title":"Emerging of dual-atom electrocatalysts advancing lithium-sulfur batteries: recent advances, challenges and perspectives","authors":"Xuting Li , Zhenxiang Zhao , Shuheng Yuan , Junhao Cheng , Wenshuo Hou , Linrui Hou , Fengwei Liu , Changzhou Yuan","doi":"10.1016/j.ensm.2026.104965","DOIUrl":"10.1016/j.ensm.2026.104965","url":null,"abstract":"<div><div>The practical implementation of lithium-sulfur (Li-S) batteries with high energy density and low cost faces significant challenges stemming from the inherent sluggish redox kinetics and inefficient conversion reactions of lithium polysulfides (LiPSs). Recent breakthroughs in dual-atom catalysts (DACs) have opened new avenues for addressing these limitations, as these materials exhibit uniquely tailored electronic configurations, pronounced synergistic effects between active sites, and unparalleled atomic utilization efficiency. This comprehensive review critically examines the latest advancements in DACs applications for Li-S batteries, with particular emphasis on their multifunctional roles in LiPSs adsorption/conversion, shuttle mitigation and Li<sup>+</sup> deposition. Through meticulous engineering of coordination environments, spatial distributions of active centers, and substrate structures, DACs verify extraordinary capabilities in accelerating sulfur conversion kinetics, facilitating charge transfer processes, and enhancing long-term cycling stability. Combining state-of-the-art theoretical calculation with characterization techniques, the discussion further unravels the fundamental catalytic mechanisms of DACs under extreme operating conditions. Finally, the review concludes by identifying existing challenges and future research directions. Most importantly, by establishing clear structure-performance correlations and synthesizing latest developments in DACs frontier, the contribution not only provides actionable guidelines for catalyst design but lays a theoretical foundation for rational development of advanced energy storage technologies.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104965"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146122280","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}
Pub Date : 2026-03-01Epub Date: 2026-02-07DOI: 10.1016/j.ensm.2026.104970
Chong Xu , Gong Cheng , Shuang Liu , Guang Ma , Dongyuan Zhang , Junjie Fu , Ye Wang , Zhengkun Xie , Weihua Chen , Yongfeng Li
Lithium-sulfur (Li-S) batteries with sulfurized polyacrylonitrile (SPAN) cathodes hold promises for high energy density but face critical challenges in conventional ether/ester electrolytes, including polysulfide dissolution, shuttle effects and incompatibility with lithium metal anodes. To address these issues, a systematic siloxane electrolyte screening strategy serves as the core of this work. Here, we propose a siloxane-based localized high-concentration electrolyte (4 M LiFSI PTTS/TTE (7:3 by volume), PT73) to address these issues. By leveraging the unique d-p orbital conjugation of siloxanes and tailored steric hindrance from propyl terminal groups, PT73 weakens Li⁺-solvent coordination while promoting anion-dominated solvation structures, thereby forming a robust inorganic-rich SEI and suppressing polysulfide dissolution. Electrochemically, Li||Cu cells with PT73 achieve 98.7 % average Coulombic efficiency (CE) and retain 98.2 % CE over 720 cycles. Li-SPAN full cells (4.4 mg cm-2 sulfur loading) maintain 91.1 % capacity retention after 120 cycles. This screening paradigm provides a rational framework for siloxane electrolyte design, accelerating high-energy-density Li-S battery development.
{"title":"Siloxane electrolyte molecular design for lithium-sulfur batteries","authors":"Chong Xu , Gong Cheng , Shuang Liu , Guang Ma , Dongyuan Zhang , Junjie Fu , Ye Wang , Zhengkun Xie , Weihua Chen , Yongfeng Li","doi":"10.1016/j.ensm.2026.104970","DOIUrl":"10.1016/j.ensm.2026.104970","url":null,"abstract":"<div><div>Lithium-sulfur (Li-S) batteries with sulfurized polyacrylonitrile (SPAN) cathodes hold promises for high energy density but face critical challenges in conventional ether/ester electrolytes, including polysulfide dissolution, shuttle effects and incompatibility with lithium metal anodes. To address these issues, a systematic siloxane electrolyte screening strategy serves as the core of this work. Here, we propose a siloxane-based localized high-concentration electrolyte (4 M LiFSI PTTS/TTE (7:3 by volume), PT73) to address these issues. By leveraging the unique <em><span>d</span>-p</em> orbital conjugation of siloxanes and tailored steric hindrance from propyl terminal groups, PT73 weakens Li⁺-solvent coordination while promoting anion-dominated solvation structures, thereby forming a robust inorganic-rich SEI and suppressing polysulfide dissolution. Electrochemically, Li||Cu cells with PT73 achieve 98.7 % average Coulombic efficiency (CE) and retain 98.2 % CE over 720 cycles. Li-SPAN full cells (4.4 mg cm<sup>-2</sup> sulfur loading) maintain 91.1 % capacity retention after 120 cycles. This screening paradigm provides a rational framework for siloxane electrolyte design, accelerating high-energy-density Li-S battery development.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104970"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146135236","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}
Pub Date : 2026-03-01Epub Date: 2026-01-28DOI: 10.1016/j.ensm.2026.104933
Qirui Wang , Jie Gao , Lei Mao , Yan Lyu
Inhomogeneous degradation is a critical factor leading to performance decay and safety risks in lithium-ion batteries. Multi-regional physical information of Lithium-ion batteries facilitates the analysis of inhomogeneous degradation processes, yet its spatio-temporal evolution remains challenging to probe non-invasively. In this study, a magnetic field sensing methodology is proposed to map and analyze regional degradation with spatio-temporal evolution. A Regional Magnetic Feature Selection and Integration (RMFSI) strategy was developed to construct an optimized magnetic feature matrix that shows strong correlation with the state of health (SOH). Then, a quantitative link between macroscopic magnetic response and electrochemical degradation was established through differential magnetic capacity (dB/dV) analysis. Moreover, spatio-temporal evolution mapping of regional magnetic fields revealed a progressive behavior from localized failure to widespread, inhomogeneous degradation throughout the cell. The heightened sensitive response for regions identified by this approach was finally validated by post-mortem scanning electron microscopy (SEM) analysis. It provides a non-invasive methodology for elucidating dynamic degradation, which is promising for early safety warnings and spatial management strategies in future battery systems.
{"title":"Magnetic field sensing of inhomogeneous degradation in Lithium-ion batteries with spatio-temporal evolution","authors":"Qirui Wang , Jie Gao , Lei Mao , Yan Lyu","doi":"10.1016/j.ensm.2026.104933","DOIUrl":"10.1016/j.ensm.2026.104933","url":null,"abstract":"<div><div>Inhomogeneous degradation is a critical factor leading to performance decay and safety risks in lithium-ion batteries. Multi-regional physical information of Lithium-ion batteries facilitates the analysis of inhomogeneous degradation processes, yet its spatio-temporal evolution remains challenging to probe non-invasively. In this study, a magnetic field sensing methodology is proposed to map and analyze regional degradation with spatio-temporal evolution. A Regional Magnetic Feature Selection and Integration (RMFSI) strategy was developed to construct an optimized magnetic feature matrix that shows strong correlation with the state of health (SOH). Then, a quantitative link between macroscopic magnetic response and electrochemical degradation was established through differential magnetic capacity (dB/dV) analysis. Moreover, spatio-temporal evolution mapping of regional magnetic fields revealed a progressive behavior from localized failure to widespread, inhomogeneous degradation throughout the cell. The heightened sensitive response for regions identified by this approach was finally validated by post-mortem scanning electron microscopy (SEM) analysis. It provides a non-invasive methodology for elucidating dynamic degradation, which is promising for early safety warnings and spatial management strategies in future battery systems.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104933"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146072528","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}
Pub Date : 2026-03-01Epub Date: 2026-01-19DOI: 10.1016/j.ensm.2026.104914
Xinyu Luo , Haoyu Wang , Mingjun Cen , Tiantian Fang , Shuya Zhang , Rui Yan , Wenchao Peng , Yang Li , Qicheng Zhang , Xiaobin Fan
Rechargeable aqueous zinc-manganese batteries (AZMBs) have received widespread attention as next-generation large-scale energy storage devices. However, there is still some controversy regarding the energy storage mechanism of the cathode materials. The deposition of manganese ions on the cathode is facilitated by the byproduct zinc hydroxide sulfate (ZHS), and both this process and the ion intercalation mechanism contribute substantially to the capacity. Herein, by constructing an alkaline and manganese-free substrate to decouple mechanisms, the capacity fading issues and resolution strategies based on the ZHS-assisted manganese deposition mechanism are comprehensively investigated. An "acid-in-alkali" substrate (AlO-ZnO) was designed with the fundamental principles of using the alkali (ZnO) to assist in manganese deposition and the acid (AlO) to aid in manganese dissolution. Specifically, Brønsted acidic sites (AlO) within the alkaline substrate structure capitalize on the proton self-limiting effect to generate a localized acidic environment at the cathode, in order to inhibit and activate dead Mn for enhanced energy density and cycle life. As a result, long-term cycle stability (2000 cycles with 98% retention) and high-rate performance are achieved. This work provides a new perspective for significantly improving the cycle stability of AZMBs and upgrading the mechanism cognition.
{"title":"\"Acid-in-Alkali\" structure for regulating dynamic evolution of manganese in Zn–Mn batteries","authors":"Xinyu Luo , Haoyu Wang , Mingjun Cen , Tiantian Fang , Shuya Zhang , Rui Yan , Wenchao Peng , Yang Li , Qicheng Zhang , Xiaobin Fan","doi":"10.1016/j.ensm.2026.104914","DOIUrl":"10.1016/j.ensm.2026.104914","url":null,"abstract":"<div><div>Rechargeable aqueous zinc-manganese batteries (AZMBs) have received widespread attention as next-generation large-scale energy storage devices. However, there is still some controversy regarding the energy storage mechanism of the cathode materials. The deposition of manganese ions on the cathode is facilitated by the byproduct zinc hydroxide sulfate (ZHS), and both this process and the ion intercalation mechanism contribute substantially to the capacity. Herein, by constructing an alkaline and manganese-free substrate to decouple mechanisms, the capacity fading issues and resolution strategies based on the ZHS-assisted manganese deposition mechanism are comprehensively investigated. An \"acid-in-alkali\" substrate (AlO-ZnO) was designed with the fundamental principles of using the alkali (ZnO) to assist in manganese deposition and the acid (AlO) to aid in manganese dissolution. Specifically, Brønsted acidic sites (AlO) within the alkaline substrate structure capitalize on the proton self-limiting effect to generate a localized acidic environment at the cathode, in order to inhibit and activate dead Mn for enhanced energy density and cycle life. As a result, long-term cycle stability (2000 cycles with 98% retention) and high-rate performance are achieved. This work provides a new perspective for significantly improving the cycle stability of AZMBs and upgrading the mechanism cognition.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104914"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145995085","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}
Pub Date : 2026-03-01Epub Date: 2026-01-26DOI: 10.1016/j.ensm.2026.104926
Jianrong Lin , Wenxuan Hu , Jian Yang , Yonggang Hu , Siyuan Ma , Lixuan Pan , Fangmei Wen , Meifang Ding , Shijun Tang , Yiming Wei , Zhengliang Gong , Yong Yang
Lithium-ion batteries exhibit distinct degradation mechanisms under calendar and cycle aging, making it essential to establish correlations between key electrochemical performance metrics and evolution of underlying physicochemical properties. In this study, LiFePO4/graphite pouch cells are subjected to both cycle aging and calendar aging (at 100% State-of-Charge) at 65 °C. Throughout the aging processes, the capacity decay, impedance variation, and the evolution of solid electrolyte interphase (SEI) are quantitatively analyzed. The capacity fading follows a 0.5-power law relationship with time during cycle aging and a logarithmic trend during calendar aging. Both aging modes could be divided into two distinct stages based on SEI evolutions. In Stage Ⅰ, the growth of inorganic SEI components far exceeds that of its organic components, accompanied by a significant decrease in both capacity and impedance. The SEI even undergoes a drastic structural reconstruction during cycle aging. In Stage Ⅱ, the SEI composition stabilizes, and its thickness increases gradually, accompanied by a slower rate of capacity fade. Notably, in this stage, a strong linear correlation is observed between capacity loss and the reciprocal of SEI capacitance (1/CSEI) for both aging modes, which enables CSEI to serve as a key descriptor for evaluating battery health state.
{"title":"Quantifying aging kinetics in LiFePO4/graphite pouch cells: Cycle aging vs calendar aging via a novel impedance descriptor","authors":"Jianrong Lin , Wenxuan Hu , Jian Yang , Yonggang Hu , Siyuan Ma , Lixuan Pan , Fangmei Wen , Meifang Ding , Shijun Tang , Yiming Wei , Zhengliang Gong , Yong Yang","doi":"10.1016/j.ensm.2026.104926","DOIUrl":"10.1016/j.ensm.2026.104926","url":null,"abstract":"<div><div>Lithium-ion batteries exhibit distinct degradation mechanisms under calendar and cycle aging, making it essential to establish correlations between key electrochemical performance metrics and evolution of underlying physicochemical properties. In this study, LiFePO<sub>4</sub>/graphite pouch cells are subjected to both cycle aging and calendar aging (at 100% State-of-Charge) at 65 °C. Throughout the aging processes, the capacity decay, impedance variation, and the evolution of solid electrolyte interphase (SEI) are quantitatively analyzed. The capacity fading follows a 0.5-power law relationship with time during cycle aging and a logarithmic trend during calendar aging. Both aging modes could be divided into two distinct stages based on SEI evolutions. In Stage Ⅰ, the growth of inorganic SEI components far exceeds that of its organic components, accompanied by a significant decrease in both capacity and impedance. The SEI even undergoes a drastic structural reconstruction during cycle aging. In Stage Ⅱ, the SEI composition stabilizes, and its thickness increases gradually, accompanied by a slower rate of capacity fade. Notably, in this stage, a strong linear correlation is observed between capacity loss and the reciprocal of SEI capacitance (1/C<sub>SEI</sub>) for both aging modes, which enables C<sub>SEI</sub> to serve as a key descriptor for evaluating battery health state.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104926"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146047996","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}
Pub Date : 2026-03-01Epub Date: 2026-01-27DOI: 10.1016/j.ensm.2026.104929
Fenqiang Luo , Taiyu Lyu , Jie Liu , Dechao Wang , Darya O. Klimchuk , Pavel B. Sorokin , Lei Tao , Zhifeng Zheng
The structure of hard carbon somehow determines the Na storage mechanism and directly affects its rate capability and initial Coulombic efficiency (ICE) in Na-ion batteries. Herein, we fabricate hierarchical graphitized carbon fibers via flash Joule heating within seconds. The fiber presents a uniform graphitized shell layer and a disordered core layer, which can maximize the Na intercalation capacity and reversibility. Combined with advanced spectroscopic techniques, we clearly observe that metallic Na clusters are uniformly stored in the outer layer at a low-voltage plateau. Such Na storage mechanism shortens ion transport distance and enhances reaction kinetics. As a result, the carbon fiber exhibits the highest ICE (97.7% at 50 mA g-1) and fast charging capability (4 mins charging). A single-layer pouch cell with a low N/P ratio can be cycled stably 1000 times at 1C. To our knowledge, this Na+ storage is reported for the first time, providing new insights into the rational design of hard carbon.
{"title":"Rapid flash heating of hard carbon: enhanced sodium storage via hierarchical graphitization","authors":"Fenqiang Luo , Taiyu Lyu , Jie Liu , Dechao Wang , Darya O. Klimchuk , Pavel B. Sorokin , Lei Tao , Zhifeng Zheng","doi":"10.1016/j.ensm.2026.104929","DOIUrl":"10.1016/j.ensm.2026.104929","url":null,"abstract":"<div><div>The structure of hard carbon somehow determines the Na storage mechanism and directly affects its rate capability and initial <em>Coulombic</em> efficiency (ICE) in Na-ion batteries. Herein, we fabricate hierarchical graphitized carbon fibers via flash Joule heating within seconds. The fiber presents a uniform graphitized shell layer and a disordered core layer, which can maximize the Na intercalation capacity and reversibility. Combined with advanced spectroscopic techniques, we clearly observe that metallic Na clusters are uniformly stored in the outer layer at a low-voltage plateau. Such Na storage mechanism shortens ion transport distance and enhances reaction kinetics. As a result, the carbon fiber exhibits the highest ICE (97.7% at 50 mA g<sup>-1</sup>) and fast charging capability (4 mins charging). A single-layer pouch cell with a low N/P ratio can be cycled stably 1000 times at 1C. To our knowledge, this Na<sup>+</sup> storage is reported for the first time, providing new insights into the rational design of hard carbon.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"86 ","pages":"Article 104929"},"PeriodicalIF":20.2,"publicationDate":"2026-03-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146185528","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}