Developing safe electrolytes with an expanded electrochemical stability window (ESW) offers a promising pathway toward practical high-energy-density lithium-metal batteries (LMBs). Here, we propose an intrinsically nonflammable F-rich high-entropy electrolyte consisting of fluorinated ester and phosphazenes. This system strategically integrates the disordered environment of high-entropy design with the low polarization characteristics of fluorination to expand the ESW and regulate the solvation structure. Large-scale molecular dynamics simulations and systematic control experimental results demonstrate that the designed electrolyte minimizes Li+-solvent interaction, which on one hand induces an inorganic-rich interface, and on the other hand accelerates the desolvation kinetics, ensuring that solvents rarely exist in the inner Helmholtz layer. The resulting electrolyte enables commercially viable Li||NCM 811 to operate safely and stably under ultrahigh-voltage (4.8 V) and low-temperature (-20°C) conditions. We believe the results of this work hold reference significance for the design of electrolytes in sodium/potassium/calcium/magnesium batteries.
{"title":"Nonflammable F-rich High-Entropy Electrolytes with Manipulated Solvent Coordination for Intrinsically Safe and High-Energy Lithium Metal Batteries","authors":"Zhiwei Ni, Yuan Li, Zhengran Wang, Suyun Liu, Junjie Liu, Chen Yang, Huizi Zhang, Juan Geng, Chenghui Zhang, Shenglin Xiong, Baojuan Xi, Jinkui Feng","doi":"10.1016/j.ensm.2026.104885","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104885","url":null,"abstract":"Developing safe electrolytes with an expanded electrochemical stability window (ESW) offers a promising pathway toward practical high-energy-density lithium-metal batteries (LMBs). Here, we propose an intrinsically nonflammable F-rich high-entropy electrolyte consisting of fluorinated ester and phosphazenes. This system strategically integrates the disordered environment of high-entropy design with the low polarization characteristics of fluorination to expand the ESW and regulate the solvation structure. Large-scale molecular dynamics simulations and systematic control experimental results demonstrate that the designed electrolyte minimizes Li<sup>+</sup>-solvent interaction, which on one hand induces an inorganic-rich interface, and on the other hand accelerates the desolvation kinetics, ensuring that solvents rarely exist in the inner Helmholtz layer. The resulting electrolyte enables commercially viable Li||NCM 811 to operate safely and stably under ultrahigh-voltage (4.8 V) and low-temperature (-20°C) conditions. We believe the results of this work hold reference significance for the design of electrolytes in sodium/potassium/calcium/magnesium batteries.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"84 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145938123","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 : 2026-01-09DOI: 10.1016/j.ensm.2026.104890
Diego Pugliese , Roberto Staffieri , Federico Bella
The transition toward sustainable and high-performance batteries requires not only advances in materials and architectures, but also the adoption of systematic approaches to experimental design. This review highlights the role of design of experiments (DoE) as a versatile and powerful methodology to accelerate innovation in the battery field. By replacing trial-and-error strategies with statistically sound frameworks, DoE enables the exploration of multiple variables and their interactions, offering deeper insights into complex phenomena that govern synthesis, performance, safety, recycling, and lifetime of batteries. Applications reviewed span from the optimization of electrode formulations and cathode synthesis to advanced thermal management strategies and recycling processes of end-of-life batteries. Across these domains, DoE has proven to reduce experimental redundancy, enhance reproducibility, and guide the identification of optimal operating conditions. The review also illustrates how DoE can act as a bridge between laboratory-scale research and industrial scalability, providing tools that are essential for the development of next-generation energy storage technologies. By presenting a comprehensive overview of its impact, this article aims to inspire researchers to embrace DoE as a cornerstone for systematic innovation, fostering both scientific progress and sustainable deployment of electrochemical energy storage.
{"title":"From materials to management: The expanding role of design of experiments in advanced battery technologies","authors":"Diego Pugliese , Roberto Staffieri , Federico Bella","doi":"10.1016/j.ensm.2026.104890","DOIUrl":"10.1016/j.ensm.2026.104890","url":null,"abstract":"<div><div>The transition toward sustainable and high-performance batteries requires not only advances in materials and architectures, but also the adoption of systematic approaches to experimental design. This review highlights the role of design of experiments (DoE) as a versatile and powerful methodology to accelerate innovation in the battery field. By replacing trial-and-error strategies with statistically sound frameworks, DoE enables the exploration of multiple variables and their interactions, offering deeper insights into complex phenomena that govern synthesis, performance, safety, recycling, and lifetime of batteries. Applications reviewed span from the optimization of electrode formulations and cathode synthesis to advanced thermal management strategies and recycling processes of end-of-life batteries. Across these domains, DoE has proven to reduce experimental redundancy, enhance reproducibility, and guide the identification of optimal operating conditions. The review also illustrates how DoE can act as a bridge between laboratory-scale research and industrial scalability, providing tools that are essential for the development of next-generation energy storage technologies. By presenting a comprehensive overview of its impact, this article aims to inspire researchers to embrace DoE as a cornerstone for systematic innovation, fostering both scientific progress and sustainable deployment of electrochemical energy storage.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104890"},"PeriodicalIF":20.2,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145955477","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 : 2026-01-09DOI: 10.1016/j.ensm.2026.104891
Gawon Lee , Minchang Go , Hanqun Wang , Chang-Min Choi , Hee-Soo Kim , Jemok Lee , Un-Hyuck Kim , Chong Seung Yoon
A structural investigation of an archetypal mid-Ni layered cathode, LiNi0.6Co0.2Mn0.2O2, charged to voltages between 4.3 V and 4.7 V, is performed to assess its structural stability at deep charge levels and determine its suitability for high-voltage cycling. Besides interparticle cracks, cracks within primary particles start to form above 4.5 V. The microstructure of primary particles is characterized by alternating bands of defect-free regions and areas containing numerous structural faults, likely caused by uneven Li ion extraction. Intraparticle cracks often originate at the boundary of these banded regions. Additionally, an unreported intermediate phase appears within the defective band. Electrochemical data confirm that 4.5 V (210 mAh g-1 at 0.1 C) is probably the limit at which LiNi0.6Co0.2Mn0.2O2 can be cycled without major capacity loss. This study reveals that the structural degradation of LiNi0.6Co0.2Mn0.2O2 during deep charging is highly localized due to the selective extraction of Li ions. Therefore, reducing the Li concentration difference at the cathode surface would prevent the formation of localized defective zones and enhance the cycling stability of LiNi0.6Co0.2Mn0.2O2 above 4.5 V.
本文对中镍层状阴极LiNi0.6Co0.2Mn0.2O2在4.3 V ~ 4.7 V充电时的结构进行了研究，以评估其在深电荷水平下的结构稳定性，并确定其在高压循环中的适用性。在4.5 V以上，除了颗粒间裂纹外，初级颗粒内部也开始形成裂纹。初生颗粒的微观结构表现为无缺陷区和含有大量结构断层的区域交替存在，这可能是由于Li离子提取不均匀造成的。颗粒内裂纹通常起源于这些带状区域的边界。此外，一个未报道的中间相出现在缺陷带内。电化学数据证实，4.5 V （210 mAh g-1, 0.1 C）可能是LiNi0.6Co0.2Mn0.2O2在没有重大容量损失的情况下循环的极限。研究表明，由于Li离子的选择性萃取，LiNi0.6Co0.2Mn0.2O2在深度充电过程中的结构降解是高度局域化的。因此，减小阴极表面的Li浓度差可以防止局部缺陷区的形成，提高LiNi0.6Co0.2Mn0.2O2在4.5 V以上的循环稳定性。
{"title":"Localized defective zone formation driven by selective Li+ extraction defines the high-voltage threshold of LiNi0.6Co0.2Mn0.2O2","authors":"Gawon Lee , Minchang Go , Hanqun Wang , Chang-Min Choi , Hee-Soo Kim , Jemok Lee , Un-Hyuck Kim , Chong Seung Yoon","doi":"10.1016/j.ensm.2026.104891","DOIUrl":"10.1016/j.ensm.2026.104891","url":null,"abstract":"<div><div>A structural investigation of an archetypal mid-Ni layered cathode, LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub>, charged to voltages between 4.3 V and 4.7 V, is performed to assess its structural stability at deep charge levels and determine its suitability for high-voltage cycling. Besides interparticle cracks, cracks within primary particles start to form above 4.5 V. The microstructure of primary particles is characterized by alternating bands of defect-free regions and areas containing numerous structural faults, likely caused by uneven Li ion extraction. Intraparticle cracks often originate at the boundary of these banded regions. Additionally, an unreported intermediate phase appears within the defective band. Electrochemical data confirm that 4.5 V (210 mAh g<sup>-1</sup> at 0.1 C) is probably the limit at which LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> can be cycled without major capacity loss. This study reveals that the structural degradation of LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> during deep charging is highly localized due to the selective extraction of Li ions. Therefore, reducing the Li concentration difference at the cathode surface would prevent the formation of localized defective zones and enhance the cycling stability of LiNi<sub>0.6</sub>Co<sub>0.2</sub>Mn<sub>0.2</sub>O<sub>2</sub> above 4.5 V.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104891"},"PeriodicalIF":20.2,"publicationDate":"2026-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145949872","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 : 2026-01-08DOI: 10.1016/j.ensm.2026.104886
Jianhui Chen , Xiaoxia Chen , Bo Xu , Libin Chen , Chenyu Wang , Cuilian Wen , Erhong Song , Baisheng Sa , Musheng Wu , Chuying Ouyang
Sodium-ion batteries (SIBs) present a compelling lithium-ion alternative, leveraging abundant sodium reserves and shared main-group chemistry for grid-scale storage and electric vehicles. Hard carbon (HC) is the prime sodium host among carbon-based materials, exhibiting superior thermodynamic stability during charge transfer over traditional graphite. However, complex organic precursors for HC anodes require precise control of structural evolution during carbonization to optimize ideal electrochemical performance. This work provides an independently developed Neural Network Potential (NNP) model for CHON-containing systems combined with experimental characterizations to reveal the pivotal role of oxygen contents in HC. Crucially, nitric acid pre-oxidation of pitch precursors elevates carbonized HC capacity from 300 to 350 mAh/g mainly in the plateau stage. Enhanced oxygen content increases carbonyl/carboxyl/ester group density, triggering intra-/inter-molecular crosslinking during carbonization. The results highlight that the resultant CO2/CO/H2 release generates radially propagating percolation pores within the carbon matrix, directly boosting sodium storage plateau capacity. Additionally, lateral and longitudinal dimensions of nanographitic crystallites modulate pore evolution during stacking as well. These atomistic insights into functional group transformations and nanographitic crystallites enable targeted HC structure optimization, advancing high-performance SIB electrode materials.
{"title":"Atomistic mechanisms of oxygen-containing functional groups in hard carbon precursors for enhanced sodium storage performance","authors":"Jianhui Chen , Xiaoxia Chen , Bo Xu , Libin Chen , Chenyu Wang , Cuilian Wen , Erhong Song , Baisheng Sa , Musheng Wu , Chuying Ouyang","doi":"10.1016/j.ensm.2026.104886","DOIUrl":"10.1016/j.ensm.2026.104886","url":null,"abstract":"<div><div>Sodium-ion batteries (SIBs) present a compelling lithium-ion alternative, leveraging abundant sodium reserves and shared main-group chemistry for grid-scale storage and electric vehicles. Hard carbon (HC) is the prime sodium host among carbon-based materials, exhibiting superior thermodynamic stability during charge transfer over traditional graphite. However, complex organic precursors for HC anodes require precise control of structural evolution during carbonization to optimize ideal electrochemical performance. This work provides an independently developed Neural Network Potential (NNP) model for CHON-containing systems combined with experimental characterizations to reveal the pivotal role of oxygen contents in HC. Crucially, nitric acid pre-oxidation of pitch precursors elevates carbonized HC capacity from 300 to 350 mAh/g mainly in the plateau stage. Enhanced oxygen content increases carbonyl/carboxyl/ester group density, triggering intra-/inter-molecular crosslinking during carbonization. The results highlight that the resultant CO<sub>2</sub>/CO/H<sub>2</sub> release generates radially propagating percolation pores within the carbon matrix, directly boosting sodium storage plateau capacity. Additionally, lateral and longitudinal dimensions of nanographitic crystallites modulate pore evolution during stacking as well. These atomistic insights into functional group transformations and nanographitic crystallites enable targeted HC structure optimization, advancing high-performance SIB electrode materials.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104886"},"PeriodicalIF":20.2,"publicationDate":"2026-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145947737","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 : 2026-01-07DOI: 10.1016/j.ensm.2026.104882
Wen Yu , Zhitao Kang , Zonghang Liu , Nanping Deng , Xiaofan Feng , Jiaxuan Zhang , Bowen Cheng , Weimin Kang
For advancing lithium metal batteries (LMBs) toward practical deployment, polymer-based electrolytes are generally regarded to possess better interfacial compatibility and formability than the inorganic counterparts. In fact, poly(ethylene oxide) (PEO)-based electrolytes suffer from severe stress relaxation behavior, rendering them incapable of rapidly accommodating the repetitive volume fluctuations. Here, we report a mechanically robust and self-adaptive solid electrolyte engineered with the physical-chemical dual networks comprising the curled fiber networks and dynamic hydrogen bonds with polymer matrix. The intermolecular interactions and competitive coordination of composite interface phases endow the obtained electrolytes with high ionic conductivity (1.4 × 10−4 S cm−1 at 30 °C), exceptional ductility (340%), high compressive resilience (81.58%) and low stress relaxation (384.11 s). Furthermore, this study also features an operando and quantitative measurement of the stress evolution in all-solid-state LMBs during cycling. It reveals the electrochemical-mechanical behaviors of the polymer-based electrolytes and the difference in stress-strain regulation priorities between polymer and inorganic electrolytes. These features enable the excellent cycling performance in Li-Li symmetric battery (4000 h at 0.2 mA cm−2) and ultra-low external pressure pouch cell. This work offers a promising strategy toward high-performance all-solid-state LMBs through the stress-adaptive and toughened polymer electrolytes.
为了推进锂金属电池的实际应用，聚合物电解质通常被认为比无机电解质具有更好的界面相容性和成形性。事实上，基于聚环氧乙烯醇（PEO）的电解质具有严重的应力松弛行为，使其无法快速适应重复的体积波动。在这里，我们报告了一种机械坚固和自适应的固体电解质，它由卷曲的纤维网络和聚合物基质的动态氢键组成的物理-化学双网络工程。复合界面相的分子间相互作用和竞争配位使电解质具有高离子电导率（30°C时为1.4 × 10−4 S cm−1）、优异的延展性（340%）、高压缩回弹性（81.55%）和低应力松弛（384.11 S）。此外，本研究还对全固态lmb在循环过程中的应力演化进行了操作和定量测量。揭示了聚合物电解质的电化学-力学行为以及聚合物电解质与无机电解质在应力-应变调节优先级上的差异。这些特性使得锂离子对称电池（在0.2 mA cm−2下可循环4000小时）和超低外压袋电池具有优异的循环性能。这项工作为通过应力自适应和增韧聚合物电解质实现高性能全固态lmb提供了一个有希望的策略。
{"title":"Physical-chemical dual networks enabled mechanically robust solid electrolytes for stress-strain regulation","authors":"Wen Yu , Zhitao Kang , Zonghang Liu , Nanping Deng , Xiaofan Feng , Jiaxuan Zhang , Bowen Cheng , Weimin Kang","doi":"10.1016/j.ensm.2026.104882","DOIUrl":"10.1016/j.ensm.2026.104882","url":null,"abstract":"<div><div>For advancing lithium metal batteries (LMBs) toward practical deployment, polymer-based electrolytes are generally regarded to possess better interfacial compatibility and formability than the inorganic counterparts. In fact, poly(ethylene oxide) (PEO)-based electrolytes suffer from severe stress relaxation behavior, rendering them incapable of rapidly accommodating the repetitive volume fluctuations. Here, we report a mechanically robust and self-adaptive solid electrolyte engineered with the physical-chemical dual networks comprising the curled fiber networks and dynamic hydrogen bonds with polymer matrix. The intermolecular interactions and competitive coordination of composite interface phases endow the obtained electrolytes with high ionic conductivity (1.4 × 10<sup>−4</sup> S cm<sup>−1</sup> at 30 °C), exceptional ductility (340%), high compressive resilience (81.58%) and low stress relaxation (384.11 s). Furthermore, this study also features an operando and quantitative measurement of the stress evolution in all-solid-state LMBs during cycling. It reveals the electrochemical-mechanical behaviors of the polymer-based electrolytes and the difference in stress-strain regulation priorities between polymer and inorganic electrolytes. These features enable the excellent cycling performance in Li-Li symmetric battery (4000 h at 0.2 mA cm<sup>−2</sup>) and ultra-low external pressure pouch cell. This work offers a promising strategy toward high-performance all-solid-state LMBs through the stress-adaptive and toughened polymer electrolytes.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104882"},"PeriodicalIF":20.2,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145920539","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 : 2026-01-07DOI: 10.1016/j.ensm.2026.104879
Xinhua Zheng , Song Wu , Ruihao Luo , Mohsin Ali , Bibo Han , Jifei Sun , Yuan Yuan , Shikai Liu , Faxing Wang , Yuping Wu , Mingjie Wu , Wei Chen
The advancement of high voltage and capacity manganese dioxide (MnO2) cathode of aqueous zinc-manganese (Zn-MnO2) batteries is widely recognized as a commendable endeavor, yet it is very challenging to improve their energy density and reversibility. Herein, we develop a MnO2 cathode with hybrid charge storage chemistries of both insertion/extraction and deposition/dissolution, resulting in high areal capacity and discharge voltage. Theoretical calculations and characterizations suggest that the deposited MnO2 can repair and compensate the decayed MnO2 in the insertion chemistry. The pre-loaded MnO2 provides a seed layer and additional active sites for the deposition/dissolution chemistry. The hybrid Zn-MnO2 battery exhibits a durability over 1200 cycles at 10 mAh cm−2, and nearly 350 stable cycles at a high areal capacity of 50 mAh cm−2. Notably, it displays high energy and power densities of 344 Wh kg−1 and 6.8 kW kg−1, respectively, based on the Zn anode and MnO2 cathode. The large-scale Zn-MnO2 full battery exhibits stable cycling performance at a capacity of 500 mAh, achieving a practical energy density of 51.3 Wh kg−1. The battery pack integrated with a photovoltaic panel showcases practical energy storage capabilities and enhanced safety features. The superior Zn-MnO2 battery enlightens an area towards the next generation large-scale energy storage applications.
高电压、高容量二氧化锰（MnO2）水相锌锰（Zn-MnO2）电池阴极的发展是一项值得称赞的努力，但提高其能量密度和可逆性是非常具有挑战性的。在此，我们开发了一种具有插入/提取和沉积/溶解混合电荷存储化学性质的二氧化锰阴极，从而获得高面积容量和放电电压。理论计算和表征表明，沉积的MnO2可以修复和补偿插入化学中衰减的MnO2。预加载的二氧化锰为沉积/溶解化学提供了种子层和额外的活性位点。混合锌-二氧化锰电池在10 mAh cm - 2下的耐久性超过1200次，在50 mAh cm - 2的高面积容量下稳定循环近350次。值得注意的是，基于Zn阳极和MnO2阴极，它的能量和功率密度分别为344 Wh kg - 1和6.8 kW kg - 1。大规模锌-二氧化锰电池在500毫安时具有稳定的循环性能，实现了51.3 Wh kg−1的实用能量密度。集成了光伏板的电池组展示了实用的储能能力和增强的安全特性。优异的Zn-MnO2电池为下一代大规模储能应用开辟了新的领域。
{"title":"Hybrid charge storage chemistries for energetic Zn-MnO2 batteries","authors":"Xinhua Zheng , Song Wu , Ruihao Luo , Mohsin Ali , Bibo Han , Jifei Sun , Yuan Yuan , Shikai Liu , Faxing Wang , Yuping Wu , Mingjie Wu , Wei Chen","doi":"10.1016/j.ensm.2026.104879","DOIUrl":"10.1016/j.ensm.2026.104879","url":null,"abstract":"<div><div>The advancement of high voltage and capacity manganese dioxide (MnO<sub>2</sub>) cathode of aqueous zinc-manganese (Zn-MnO<sub>2</sub>) batteries is widely recognized as a commendable endeavor, yet it is very challenging to improve their energy density and reversibility. Herein, we develop a MnO<sub>2</sub> cathode with hybrid charge storage chemistries of both insertion/extraction and deposition/dissolution, resulting in high areal capacity and discharge voltage. Theoretical calculations and characterizations suggest that the deposited MnO<sub>2</sub> can repair and compensate the decayed MnO<sub>2</sub> in the insertion chemistry. The pre-loaded MnO<sub>2</sub> provides a seed layer and additional active sites for the deposition/dissolution chemistry. The hybrid Zn-MnO<sub>2</sub> battery exhibits a durability over 1200 cycles at 10 mAh cm<sup>−2</sup>, and nearly 350 stable cycles at a high areal capacity of 50 mAh cm<sup>−2</sup>. Notably, it displays high energy and power densities of 344 Wh kg<sup>−1</sup> and 6.8 kW kg<sup>−1</sup>, respectively, based on the Zn anode and MnO<sub>2</sub> cathode. The large-scale Zn-MnO<sub>2</sub> full battery exhibits stable cycling performance at a capacity of 500 mAh, achieving a practical energy density of 51.3 Wh kg<sup>−1</sup>. The battery pack integrated with a photovoltaic panel showcases practical energy storage capabilities and enhanced safety features. The superior Zn-MnO<sub>2</sub> battery enlightens an area towards the next generation large-scale energy storage applications.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104879"},"PeriodicalIF":20.2,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146036146","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 : 2026-01-07DOI: 10.1016/j.ensm.2026.104883
Fei Hu , Yineng Zhao , Xinhao Li , In Won Yeu , Alexander Urban , Wyatt E. Tenhaeff
Anode-free lithium metal batteries, containing no excess Li metal and utilizing only the cathode’s Li inventory, promise extreme energy densities. Realization of practical anode-free Li batteries, however, is constrained by the poor reversibility of Li metal electrodeposition and rapid depletion of the Li inventory in the form of “dead” Li. To address these issues, conventional Cu current collectors were modified with ultrathin dual-layer coatings to construct a lithiophobic artificial solid electrolyte interface (ASEI) atop a lithiophilic metallic alloy layer. The lithophilic layer consisting of LixAu alloys reduced the Li nucleation overpotential, inducing continuous and homogenous Li deposition on the current collector. The lithiophobic ASEI composed of MgF2 conferred superior Li dendrite suppression stability due to its high interfacial energy, resulting in less Li penetration into the SEI. Conventional Cu current collectors coated with ultrathin Au and MgF2 films provided an enhanced Coulombic efficiency of 99.2 % over 350 cycles in a Li||Cu cell, compared to only ∼98.4 % from baseline samples employing conventional, bare Cu current collectors. More importantly, when the coated copper current collectors were incorporated into anode-free LiFePO4 full cells, the average initial CE and capacity retention were improved by ∼8.2 % and 30.1 %, respectively. The high energy density of the cell was maintained given the thinness of the layers (<50 nm in total). This ultrathin dual layer design provides a pathway to practical, reversible anode-free Li batteries while preserving extreme energy densities.
{"title":"Combining ultrathin lithiophobic and lithiophilic interlayers to enhance the reversibility of anode-free lithium metal batteries","authors":"Fei Hu , Yineng Zhao , Xinhao Li , In Won Yeu , Alexander Urban , Wyatt E. Tenhaeff","doi":"10.1016/j.ensm.2026.104883","DOIUrl":"10.1016/j.ensm.2026.104883","url":null,"abstract":"<div><div>Anode-free lithium metal batteries, containing no excess Li metal and utilizing only the cathode’s Li inventory, promise extreme energy densities. Realization of practical anode-free Li batteries, however, is constrained by the poor reversibility of Li metal electrodeposition and rapid depletion of the Li inventory in the form of “dead” Li. To address these issues, conventional Cu current collectors were modified with ultrathin dual-layer coatings to construct a lithiophobic artificial solid electrolyte interface (ASEI) atop a lithiophilic metallic alloy layer. The lithophilic layer consisting of Li<sub>x</sub>Au alloys reduced the Li nucleation overpotential, inducing continuous and homogenous Li deposition on the current collector. The lithiophobic ASEI composed of MgF<sub>2</sub> conferred superior Li dendrite suppression stability due to its high interfacial energy, resulting in less Li penetration into the SEI. Conventional Cu current collectors coated with ultrathin Au and MgF<sub>2</sub> films provided an enhanced Coulombic efficiency of 99.2 % over 350 cycles in a Li||Cu cell, compared to only ∼98.4 % from baseline samples employing conventional, bare Cu current collectors. More importantly, when the coated copper current collectors were incorporated into anode-free LiFePO<sub>4</sub> full cells, the average initial CE and capacity retention were improved by ∼8.2 % and 30.1 %, respectively. The high energy density of the cell was maintained given the thinness of the layers (<50 nm in total). This ultrathin dual layer design provides a pathway to practical, reversible anode-free Li batteries while preserving extreme energy densities.</div></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"85 ","pages":"Article 104883"},"PeriodicalIF":20.2,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145937481","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 : 2026-01-07DOI: 10.1016/j.ensm.2026.104884
Shakti Singh, Prisca Putri Elesta, Jinhwan Yoon
The growing demand for compact and portable energy storage solutions for wearable devices has led to the development of conformal and deformable high-performance microsupercapacitors (MSCs). However, traditional MSCs face challenges in achieving high deformability without compromising performance. Herein, we present a soft electrode system comprising multiwalled carbon nanotubes/manganese phosphate nanoneedles/poly(3,4-ethylenedioxythiophene):polystyrene sulfonate within an Ecoflex matrix. This system is prepared via phosphoric acid treatment, which forms nanoneedles with high aspect ratios, resulting in an enhanced surface area and porosity. Additionally, an ionogel containing a zwitterionic moiety is employed as an MSC electrolyte to ensure high conductivity and strong interfacial bonding. The fabricated MSC exhibits exceptional performance, with a specific capacitance of 304.2 mF cm−2, energy density of 82.8 µWh cm−2, and power density of 699.7 µW cm−2. The capacitance retention exceeds 95%, even at 300% stretching, which is attributed to the intrinsic stretchability of the MSC. Furthermore, the present MSC device demonstrates outstanding reproducibility and stability, retaining 95.7% of its initial capacitance after 10,000 charge-discharge cycles and 97.8% after being stored for 21 days. This MSC can be interfaced with a microcontroller unit to facilitate wireless charging and discharging via a smartphone, thereby enabling the remote operation of healthcare devices.
{"title":"Highly intrinsically stretchable microsupercapacitor achieved by a post-growth-engineered electrode and zwitterionic ionogel electrolyte","authors":"Shakti Singh, Prisca Putri Elesta, Jinhwan Yoon","doi":"10.1016/j.ensm.2026.104884","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104884","url":null,"abstract":"The growing demand for compact and portable energy storage solutions for wearable devices has led to the development of conformal and deformable high-performance microsupercapacitors (MSCs). However, traditional MSCs face challenges in achieving high deformability without compromising performance. Herein, we present a soft electrode system comprising multiwalled carbon nanotubes/manganese phosphate nanoneedles/poly(3,4-ethylenedioxythiophene):polystyrene sulfonate within an Ecoflex matrix. This system is prepared via phosphoric acid treatment, which forms nanoneedles with high aspect ratios, resulting in an enhanced surface area and porosity. Additionally, an ionogel containing a zwitterionic moiety is employed as an MSC electrolyte to ensure high conductivity and strong interfacial bonding. The fabricated MSC exhibits exceptional performance, with a specific capacitance of 304.2 mF cm<sup>−2</sup>, energy density of 82.8 µWh cm<sup>−2</sup>, and power density of 699.7 µW cm<sup>−2</sup>. The capacitance retention exceeds 95%, even at 300% stretching, which is attributed to the intrinsic stretchability of the MSC. Furthermore, the present MSC device demonstrates outstanding reproducibility and stability, retaining 95.7% of its initial capacitance after 10,000 charge-discharge cycles and 97.8% after being stored for 21 days. This MSC can be interfaced with a microcontroller unit to facilitate wireless charging and discharging via a smartphone, thereby enabling the remote operation of healthcare devices.","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"263 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145937479","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 : 2026-01-06DOI: 10.1016/j.ensm.2026.104877
Xin Gao, Ya Chen, Bin Fang, Xiaodong Chen, Runjing Xu, Tao Meng, Ling Huang, Peiyi Ji, Long Bao, Hongchao Sun, Lifeng Cui, Gang Tan, Guoxiu Wang
{"title":"Engineering Ultra-Stable Composite Cathodes via Multifunctional Conductive Additive Architectures to Stabilize Li6PS5Cl-Based All-Solid-State Lithium Batteries","authors":"Xin Gao, Ya Chen, Bin Fang, Xiaodong Chen, Runjing Xu, Tao Meng, Ling Huang, Peiyi Ji, Long Bao, Hongchao Sun, Lifeng Cui, Gang Tan, Guoxiu Wang","doi":"10.1016/j.ensm.2026.104877","DOIUrl":"https://doi.org/10.1016/j.ensm.2026.104877","url":null,"abstract":"","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":"29 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2026-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145902960","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}
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