Advanced Energy Materials最新文献_第4页

Oxygen-Doped Carbon Monolayer Intercalation and Selenization Stabilizing 1T-Rich MoS2 to Enable Fast and Durable Sodium-Ion Storage 氧掺杂碳单层嵌入和硒化稳定富t二硫化钼以实现快速和持久的钠离子储存

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-07 DOI: 10.1002/aenm.202503274

Di Wu, Luhai Gai, Deliang Cui, Qilong Wang, Haohai Yu, Ching-Ping Wong, Gang Lian

{"title":"Oxygen-Doped Carbon Monolayer Intercalation and Selenization Stabilizing 1T-Rich MoS2 to Enable Fast and Durable Sodium-Ion Storage","authors":"Di Wu, Luhai Gai, Deliang Cui, Qilong Wang, Haohai Yu, Ching-Ping Wong, Gang Lian","doi":"10.1002/aenm.202503274","DOIUrl":"https://doi.org/10.1002/aenm.202503274","url":null,"abstract":"Metallic 1T-MoS2 is a promising anode for sodium-ion batteries (SIBs) due to its excellent conductivity, abundant active sites, and low adsorption barrier for Na+. Unfortunately, intrinsic metastable features and defect-caused poor structure stability pose an unparalleled challenge in cycle life. Herein, a synergetic strategy of carbon intercalation and selenization is proposed to construct stable 1T-rich MoS2-xSey, which is covalently bonded to intercalated carbon monolayers via C─S/Se and C─O─Mo bonds on reduced graphene oxide (MoS2-xSey/m-C@rGO). The heterostructure expands the interlayer distance for fast Na+ diffusion, provides confined atomic-thickness spacing stabilizing the layered structure, induces the formation of the 1T phase, and promotes charge transfer from carbon monolayers to S atoms. Selenization remediates sulfur vacancies while enabling the stabilization of the 1T phase due to induced lattice strains and electronic structure modulation. Consequently, the electrode delivers a capacity of 242.3 mAh g−1 after 2500 cycles at 5 A g−1, corresponding to a capacity retention of 82.6% relative to the initial capacity at 5 A g−1. The full cell delivers an appealing energy output of 167.7 Wh kg−1 at 183 W kg−1. An atomic-level mechanism of reversible reconstruction is proposed. This work provides valuable insights toward the design of durable, high-rate electrodes in SIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"18 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235392","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

Probing Battery Interfaces and Interphases with Microelectrodes: Spatially and Temporally Resolved Single‐Entity Measurements 用微电极探测电池界面和界面：空间和时间分辨的单实体测量

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-07 DOI: 10.1002/aenm.202504512

Animesh Khaund, Surajit Samui, Bharat Bhushan Upreti, Koushik Barman, Srija Ghosh, Ashutosh Rana, Ramendra Sundar Dey, Kingshuk Roy

{"title":"Probing Battery Interfaces and Interphases with Microelectrodes: Spatially and Temporally Resolved Single‐Entity Measurements","authors":"Animesh Khaund, Surajit Samui, Bharat Bhushan Upreti, Koushik Barman, Srija Ghosh, Ashutosh Rana, Ramendra Sundar Dey, Kingshuk Roy","doi":"10.1002/aenm.202504512","DOIUrl":"https://doi.org/10.1002/aenm.202504512","url":null,"abstract":"Understanding batteries at the level of individual particles and interfaces, where critical electrochemical processes actually occur, remains a grand challenge in energy storage research. Traditional characterization techniques often average over complex, heterogeneous structures, obscuring localized events such as nucleation and phase transformation that ultimately dictate battery performance and degradation. Microelectrodes offer a unique opportunity to overcome this limitation by enabling spatially and temporally resolved probing of electrochemical reactions at the microscale. Their reduced dimensions facilitate rapid steady‐state responses, minimal ohmic‐drop, and hemispherical diffusion, making them ideally suited for investigating fast kinetics, localized transport phenomena, and single‐entity redox behavior under realistic battery operating conditions. This review critically examines the growing role of microelectrodes in battery science: from measuring intrinsic charge transfer and diffusion coefficients to mapping morphological transitions and probing interfacial instabilities. It highlights when integrated with advanced characterization tools and operando platforms, microelectrodes can unravel reaction pathways inaccessible to macroscale techniques. Moving forward, it outlines key research directions where microelectrode‐based platforms can make transformative contributions, particularly in non‐equilibrium systems, emerging chemistries, and data‐integrated diagnostics. By reframing batteries as inherently heterogeneous and dynamic systems, microelectrodes emerge as enabling tools for mechanistic understanding and precision control in next‐generation energy storage technologies.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"55 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235396","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

Tailored Ordering Enables High-Capacity Cathode Materials 订制高容量正极材料

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-07 DOI: 10.1002/aenm.202503660

Tzu-chen Liu, Adolfo Salgado-Casanova, So Yubuchi, Bianca Baldassarri, Muratahan Aykol, Jun Yoshida, Hisatsugu Yamasaki, Yizhou Zhu, Steven B. Torrisi, Chris Wolverton

{"title":"Tailored Ordering Enables High-Capacity Cathode Materials","authors":"Tzu-chen Liu, Adolfo Salgado-Casanova, So Yubuchi, Bianca Baldassarri, Muratahan Aykol, Jun Yoshida, Hisatsugu Yamasaki, Yizhou Zhu, Steven B. Torrisi, Chris Wolverton","doi":"10.1002/aenm.202503660","DOIUrl":"https://doi.org/10.1002/aenm.202503660","url":null,"abstract":"Novel Li-ion battery cathode materials with high capacity and greater compositional flexibility are essential for the growing electric vehicle market. Cathode structures with cation disorder were once considered suboptimal, but recent demonstrations have highlighted their potential in Li1 + xM1 − xO2 chemistries with a wide range of metal combinations M. By relaxing requirements of maintaining ordered Li diffusion pathways, countless multi-metal compositions in LiMO2 may become viable, aiding the quest for high-capacity cobalt-free cathodes. A challenge presented by this freedom in composition space is designing compositions that possess specific, tailored types of both long- and short-range orderings, which can ensure both phase stability and Li diffusion. Ordering design frameworks are proposed based on computational ordering descriptors, which in tandem with low-cost heuristics and elemental statistics can be used to simultaneously achieve compositions that possess favorable phase stability as well as configurations amenable to Li diffusion. Utilizing this computational framework, accompanied by illustrative synthesis and characterization experiments, we not only demonstrate the design of LiCr0.75Fe0.25O2, showcasing initial charge capacity of 234 and 320 mAhg−1 in its 20% Li-excess variant Li1.2Cr0.6Fe0.2O2, but also present the elemental ordering statistics for 32 elements, informed by one of the most extensive first-principles studies of ordering tendencies.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"24 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145241197","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

Stability Challenges and Solutions in Wide‐ and Narrow‐Bandgap Perovskites for All‐Perovskite Tandem Solar Cells 全钙钛矿串联太阳能电池宽带隙和窄带隙钙钛矿的稳定性挑战和解决方案

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-07 DOI: 10.1002/aenm.202503904

Jung Geon Son, Jina Roe, Dong Suk Kim, Jin Young Kim

{"title":"Stability Challenges and Solutions in Wide‐ and Narrow‐Bandgap Perovskites for All‐Perovskite Tandem Solar Cells","authors":"Jung Geon Son, Jina Roe, Dong Suk Kim, Jin Young Kim","doi":"10.1002/aenm.202503904","DOIUrl":"https://doi.org/10.1002/aenm.202503904","url":null,"abstract":"Perovskites possess exceptional optoelectronic properties, including tunable direct bandgaps and long carrier diffusion lengths that render ideal absorbers for tandem solar cell architectures. In all‐perovskite tandem solar cells (APTSCs), the integration of wide‐bandgap (WBG) and narrow‐bandgap (NBG) sub‐cells enables more efficient harvesting of the solar spectrum, leading to certified power conversion efficiencies (PCEs) as high as 30.1%. Despite this progress, ensuring long‐term operational stability remains a major challenge. WBG perovskites are prone to photo‐induced phase segregation and the formation of deep‐level defects, whereas NBG perovskites are vulnerable to Sn2⁺ oxidation and asynchronous crystallization‐based defects. These intrinsic instabilities, compounded by extrinsic stressors such as light, heat, moisture, and oxygen, accelerate performance degradation under practical operating conditions. Achieving durable APTSCs thus requires a comprehensive understanding of degradation mechanisms affecting both WBG and NBG absorbers. This review systematically explores both intrinsic and extrinsic degradation pathways in WBG and NBG perovskites, with particular emphasis on the roles of interfaces, charge‐selective layers, and environmental conditions. Furthermore, we summarize recent advances in mitigation strategies aimed at enhancing the stability of APTSCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"158 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235286","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

Redox Mediators for Aqueous Electrolytic Zinc‐Manganese Batteries: Fundamentals and Design Criteria 水电解锌锰电池的氧化还原介质：基本原理和设计标准

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-07 DOI: 10.1002/aenm.202504251

Weijie Fan, Liping Qin, Taghreed F. Altamimi, Zeinhom M. El‐Bahy, Bingan Lu, Shaaban M. Shaaban, Siyu Tian, Zequan Zhao, Jiang Zhou

{"title":"Redox Mediators for Aqueous Electrolytic Zinc‐Manganese Batteries: Fundamentals and Design Criteria","authors":"Weijie Fan, Liping Qin, Taghreed F. Altamimi, Zeinhom M. El‐Bahy, Bingan Lu, Shaaban M. Shaaban, Siyu Tian, Zequan Zhao, Jiang Zhou","doi":"10.1002/aenm.202504251","DOIUrl":"https://doi.org/10.1002/aenm.202504251","url":null,"abstract":"Although aqueous electrolytic zinc‐manganese batteries (AZMBs) have attracted significant attention due to their high theoretical energy density, their practical application has been hindered by the insufficient reversibility of the cathodic Mn2+/MnO2 conversion reaction. Introducing redox mediators (RMs) as electron transfer catalysts enables the conversion of electrochemically inert “dead MnO2” into active Mn2+ ions during discharging, effectively enhancing cathodic reversibility. However, the practical application of RM‐assisted AZMB systems is severely hindered by a limited understanding of the relationship between the fundamental properties of RMs and their reaction kinetics with MnO2. By applying classical Marcus theory, the correlation between the fundamental structures of RMs and their reaction kinetics is elucidated, offering a coherent explanation for the conflict between the thermodynamic and kinetic behaviors of the RM‐assisted MnO2 electroreduction process. Emphases are placed on establishing a theoretical foundation and design paradigms, including the design of organic RM molecules, construction of efficient RM‐based reaction systems, and formulation of shuttle‐free approaches, thereby designing and advancing high‐performance RM‐assisted AZMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"68 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235394","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

Customized Solvation Structure for Stable and Safe Sodium‐Metal Batteries 为稳定和安全的钠金属电池定制的溶剂化结构

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-07 DOI: 10.1002/aenm.202504683

Xiaosheng Song, Xinghui Liang, Myung‐Chan Kim, Yang‐Kook Sun

{"title":"Customized Solvation Structure for Stable and Safe Sodium‐Metal Batteries","authors":"Xiaosheng Song, Xinghui Liang, Myung‐Chan Kim, Yang‐Kook Sun","doi":"10.1002/aenm.202504683","DOIUrl":"https://doi.org/10.1002/aenm.202504683","url":null,"abstract":"Owing to the low cost and high abundance of sodium (Na), significant advancements are made in the field of Na‐based batteries, which are possible through the incorporation of lithium‐ion‐inspired electrodes with different electrolyte chemistries. However, the conventional carbonate electrolytes employed in such systems are flammable, thermally unstable, and prone to severe interfacial side reactions that compromise safety and shorten the overall battery cycle life. This study introduces a flame‐retardant cosolvent strategy, wherein trimethylsilyl phosphite (TMSPi) and nonafluorohexyltrimethoxysilane (NFTOS) are blended into a propylene carbonate (PC)‐based commercial electrolyte, yielding an novel electrolyte system (PCTN) with a tailor‐designed solvation structure. This PCTN electrolyte is found to self‐extinguish upon ignition, in addition to generating a robust NaSiOx/NaF solid electrolyte interphase and a NaPOxFy‐dominated cathode electrolyte interphase. Consequently, the Na|NaNi0.4Fe0.2Mn0.4O2 cell incorporating PCTN retained 90.3% of its initial capacity after 450 cycles at 1 C, outperforming commercial electrolytes. Even at a high operation temperature of 70 °C, a capacity retention of 93.2% is achieved after 100 cycles using PCTN (c.f., 79.9% for a commercial electrolyte). Overall, this work demonstrates a facile, production‐compatible electrolyte design that synchronously enhances the stability of the electrode–electrolyte interface, offering a potential system for incorporation into next‐generation high‐performance Na metal batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"81 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145235395","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

Why are Lead Iodide‐Based Perovskite Precursor Inks Yellow? 为什么碘化铅钙钛矿前驱体油墨是黄色的？

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-06 DOI: 10.1002/aenm.202502813

Ross A. Kerner, Keith P. White, Nikhila Balasubramaniam, Jiselle Y. Ye, Bennett Addison, Rosemary Bramante, Kostas Fykouras, Linn Leppert, Michael F. Toney, Bryon W. Larson, Lance M. Wheeler, Barry P. Rand, Joseph J. Berry, Kai Zhu

{"title":"Why are Lead Iodide‐Based Perovskite Precursor Inks Yellow?","authors":"Ross A. Kerner, Keith P. White, Nikhila Balasubramaniam, Jiselle Y. Ye, Bennett Addison, Rosemary Bramante, Kostas Fykouras, Linn Leppert, Michael F. Toney, Bryon W. Larson, Lance M. Wheeler, Barry P. Rand, Joseph J. Berry, Kai Zhu","doi":"10.1002/aenm.202502813","DOIUrl":"https://doi.org/10.1002/aenm.202502813","url":null,"abstract":"A challenge faced by metal halide perovskite (MHP) photovoltaics is scaling up solution deposition processes to realize rapid and inexpensive manufacturing. The challenge lies in completely understanding and controlling solution speciation, nucleation, and self‐assembly of iodoplumbate complexes during solvent evaporation as the liquid transforms into gels and solids. An accurate description of solution species, at all points in the transformation, is a prerequisite to design robust and reliable processes. Here, the common assumption that initial monoplumbate solution species typically invoked (e.g., [PbI6]4−) are certainly not the origin of optical absorbance at >400 nm wavelengths is disproved, as are many large particles of common “intermediate” iodoplumbate phases with face‐ or edge‐sharing connectivity. Instead, a new perspective is offered, involving (partially) corner‐sharing iodo(poly)plumbates (>1 Pb2+ per complex) that experience highly dynamic chemical environments. It is outlined how the MHP field would benefit by elucidating these phenomena. Future work is required to determine the size and kinetic behavior of polyplumbate species, and contextualize these findings in relation to broader trends in materials chemistry beyond MHPs. Ultimately, a complete explanation for the solution speciation, optical absorbance signatures, and the color of MHP precursor inks remains an open challenge to the community.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"14 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145228933","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

Do Micropower Sources Meet the Needs of the Internet of Things? 微电源满足物联网需求吗？

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-06 DOI: 10.1002/aenm.202503921

Grace Whang, Randy Chen, Jacky T. T. Yu, Christopher Choi, Patricia McNeil, Jérémie Chaillou, Christophe Loyez, Christophe Lethien, Bruce Dunn

引用次数: 0

Room‐Temperature Single Li+ Ion Conducting Organic Solid‐State Electrolyte with 10−4 S cm−1 Conductivity for Lithium‐Metal Batteries 用于锂金属电池的室温单锂离子导电有机固态电解质，电导率为10 - 4 S cm - 1

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-06 DOI: 10.1002/aenm.202504143

Rak Hyeon Choi, Akshay Gurumoorthi, Sangwon Bae, Chang Yun Son, Hye Ryung Byon

{"title":"Room‐Temperature Single Li+ Ion Conducting Organic Solid‐State Electrolyte with 10−4 S cm−1 Conductivity for Lithium‐Metal Batteries","authors":"Rak Hyeon Choi, Akshay Gurumoorthi, Sangwon Bae, Chang Yun Son, Hye Ryung Byon","doi":"10.1002/aenm.202504143","DOIUrl":"https://doi.org/10.1002/aenm.202504143","url":null,"abstract":"Covalent organic frameworks (COFs) are promising solid‐state electrolytes (SSEs) for lithium (Li)‐metal batteries due to their tunable structures, ordered nanochannels, and suppressed segmental motion, which support Li⁺ ion transport at ambient temperatures. However, pellet‐type COF‐based SSEs have exhibited low ionic conductivity, attributed to suboptimal ion transport pathways, limited crystallinity, and extensive grain boundary formation. Here, a 20 µm‐thick disulfonate‐functionalized COF (COFds) film is presented that achieves an ionic conductivity of 1.0 × 10‒4 S cm‒1 at 25 °C. The integration of immobile disulfonate anions and carbonyl groups enables inter‐subchannel Li⁺ hopping with minimal spatial separation. Molecular dynamics (MD) simulations under applied fields confirm that the molecular design facilitates optimized Li⁺ conduction pathways. Solution‐phase synthesis enabled COFds films with high crystallinity, uniform morphology, and smooth surfaces, which enhanced electrochemical performance. As a result, symmetric Li cells with the COFds film showed stable cycling for over 1300 h at 25 °C, while full cells with LiFePO4 cathodes retained ≈95% capacity and 99.999% Coulombic efficiency over 300 cycles at 0.2 C. This study highlights the importance of integrating molecular and structural engineering for developing COF‐based SSEs in Li‐metal batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145228910","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

Electrolyte‐Driven Suppression of Oxygen Dimerization and Oxygen Evolution in High‐Voltage Li‐Ion Batteries 高压锂离子电池中电解液驱动的氧二聚抑制和析氧

IF 27.8 1区材料科学

Advanced Energy Materials Pub Date : 2025-10-06 DOI: 10.1002/aenm.202503180

Jeongin Lee, Jihyun Kim, Daehyun Kim, Hosik Lee, Do Sol Cheong, Mideum Kim, Dongho Jang, Jonghak Kim, Jisu Lee, Chihyun Hwang, Seo‐Hyun Jung, Hyun‐Kon Song

{"title":"Electrolyte‐Driven Suppression of Oxygen Dimerization and Oxygen Evolution in High‐Voltage Li‐Ion Batteries","authors":"Jeongin Lee, Jihyun Kim, Daehyun Kim, Hosik Lee, Do Sol Cheong, Mideum Kim, Dongho Jang, Jonghak Kim, Jisu Lee, Chihyun Hwang, Seo‐Hyun Jung, Hyun‐Kon Song","doi":"10.1002/aenm.202503180","DOIUrl":"https://doi.org/10.1002/aenm.202503180","url":null,"abstract":"High‐voltage operation of Ni‐rich layered cathodes in lithium‐ion batteries (LIBs) induces oxygen redox reactions, leading to singlet oxygen evolution, interfacial degradation, and electrolyte decomposition. While cathode engineering has been extensively explored to mitigate these challenges, electrolyte‐based strategies for directly regulating oxygen redox remain limited. To address this limitation, an anthracene‐functionalized cyanoethyl polyvinyl alcohol (An‐PVA‐CN) gel polymer electrolyte (GPE) is developed, offering dual functionalities: anchoring oxidized surface oxygen and scavenging singlet oxygen. The anthracene moiety binds to oxidized lattice oxygen prior to O–O dimer formation, forming a stable Ni─O─C bridging structure that suppresses singlet oxygen release. It also acts as an effective scavenger for any singlet oxygen generated. Simultaneously, the electron‐rich nitrile groups coordinate with transition metals, suppressing over‐oxidation of Ni during charging. Spectroscopic and computational analyses confirm the suppression of oxygen redox and stabilization of surface oxygen species. By regulating charge compensation via transition metal redox while inhibiting oxygen redox, oxygen gas evolution and transition metal dissolution are effectively mitigated. As a result, An‐PVA‐CN GPE enables 81% capacity retention over 500 cycles at 4.55 V in full‐cell configurations. This work demonstrates a rare electrolyte‐centered approach to oxygen redox regulation and offers a promising design strategy for stabilizing high‐voltage LIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"120 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-10-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145228931","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