Cyrus Kirwa, Evelyna Wang, Seoung‐Bum Son, Juliane Preimesberger, Fulya Dogan Key, Yaocai Bai, Krzysztof Pupek, Hongmei Luo, Matthew Keyser, Jaclyn Coyle
{"title":"Addressing Inherent Challenges to Chemical Relithiation of Cycled End‐of‐Life Cathode Materials","authors":"Cyrus Kirwa, Evelyna Wang, Seoung‐Bum Son, Juliane Preimesberger, Fulya Dogan Key, Yaocai Bai, Krzysztof Pupek, Hongmei Luo, Matthew Keyser, Jaclyn Coyle","doi":"10.1002/aenm.202501809","DOIUrl":"https://doi.org/10.1002/aenm.202501809","url":null,"abstract":"Recycling end‐of‐life (EOL) lithium‐ion batteries (LIBs) is important to retain valuable resources from critical materials present in EOL battery waste. Direct recycling methods offer an opportunity to recover intact valuable cathode materials with minimal re‐processing. An important step of the direct recycling process is relithiation which is used to restore lithium content to EOL cathode materials. However, little has been done to study how preprocessing steps such as washing or binder removal may affect relithiation methods in the direct recycling process. Here, the evolution of fluorine byproducts left over from preprocessing steps during a low‐temperature chemical redox mediator relithiation process is tracked. A facile washing step is presented as a solution for mediating adverse effects of surface contamination on the chemical relithiation performance. The structure, lithium content, and electrochemical performance of relithiated EOL NMC 622 material that underwent a pre‐relithiation washing step to remove fluorine byproducts is shown to match that of pristine NMC 622. In this work, it is showed that redox mediator relithiation as a part of a direct recycling process is a promising low energy method that can be applied to EOL material with inherent surface impurities if the proper pre‐relithiation processing steps are implemented.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144370594","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}
Pan Zeng, Xiaoqin Li, Bo Zhao, Jiechang Gao, Wei Feng, Qingyuan Wang, Yingze Song
{"title":"Electronic Structure Engineering in Electrocatalysts: Enabling Regulated Redox Mediation for Advanced Lithium‐Sulfur Chemistry","authors":"Pan Zeng, Xiaoqin Li, Bo Zhao, Jiechang Gao, Wei Feng, Qingyuan Wang, Yingze Song","doi":"10.1002/aenm.202501603","DOIUrl":"https://doi.org/10.1002/aenm.202501603","url":null,"abstract":"The practical deployment of lithium‐sulfur (Li–S) battery is fundamentally constrained by the intrinsic shuttle effect and the kinetically sluggish conversion of lithium polysulfides (LiPSs). To mitigate these challenges, rational design of advanced electrocatalysts capable of dual‐functional LiPSs immobilization and catalytic conversion has been recognized as a pivotal solution. Critically, the catalytic efficacy of electrocatalysts is intrinsically governed by their electronic structure characteristics, which dictate adsorption energies, charge transfer dynamics, and reaction pathway selectivity during the redox process. However, a systematic review correlating electronic modulation strategies with mechanistic enhancements in Li–S chemistry still remains absent. This review emphasizes recent advances in the fascinating strategies to tailor the electronic structure of electrocatalysts, including but not limited to <jats:italic>d</jats:italic>‐band position, <jats:italic>d</jats:italic>‐band valence electron/vacancy, spin state, e<jats:sub>g</jats:sub>/t<jats:sub>2g</jats:sub> orbitals, electron filling of anti‐bonding, <jats:italic>p</jats:italic>‐band, <jats:italic>d‐p</jats:italic> orbital hybridization, <jats:italic>f</jats:italic>‐orbital, and geometric structure engineering. The fundamental relationships between electronic structure and catalytic activity are discussed in detail, highlighting mechanistic insights into the origins of enhanced activity. Finally, the major challenges in modulating electronic structure are summarized, and an outlook for further development of electronic structure strategies is briefly proposed. This review can afford cutting‐edge insights into the electronic structure regulation in Li–S chemistry.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"4 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144370481","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}
Haicheng Li, Bo Gao, Liu Yang, Shibo Wang, Kun Gao, Wei Shi, Fengxian Cao, Xiang Chen, Wenhao Li, Yao Li, Bowen Yang, Chang Wang, Wenhao Li, Cao Yu, Xiaohong Zhang, Xinbo Yang
{"title":"Magnesium Oxide Buffer Layer for Over 32% Efficiency Four-Terminal Perovskite/Silicon Tandem Solar Cells","authors":"Haicheng Li, Bo Gao, Liu Yang, Shibo Wang, Kun Gao, Wei Shi, Fengxian Cao, Xiang Chen, Wenhao Li, Yao Li, Bowen Yang, Chang Wang, Wenhao Li, Cao Yu, Xiaohong Zhang, Xinbo Yang","doi":"10.1002/aenm.202501762","DOIUrl":"https://doi.org/10.1002/aenm.202501762","url":null,"abstract":"Perovskite/silicon tandem solar cells have emerged as a promising candidate for next-generation photovoltaics, offering a pathway to surpass the efficiency limits of single-junction devices. However, the integration of a buffer layer between the electron transport layer and the transparent electrode is critical for maintaining structural integrity and optimizing charge extraction and stability. Here, the fabrication of a chemically stable and multifunctional buffer layer, magnesium oxide (MgO<sub>x</sub>), via thermal evaporation is demonstrated in four-terminal perovskite/silicon tandem solar cells. The introduction of MgO<sub>x</sub> enhances electron extraction while effectively mitigating damage caused by the sputtering process used for subsequent layers. As a result, the optimized device achieves a power conversion efficiency exceeding 32%, along with exceptional operational stability, MgO<sub>x</sub> device retains 80% of its initial efficiency after 400 h of continuous MPPT testing. This work highlights the pivotal role of buffer layer engineering in advancing high-performance tandem solar cells and provides a scalable route toward efficient and durable perovskite/silicon photovoltaics.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"17 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144370832","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}
Xiaomei Huo, Guowei Gao, Boxin Li, Zhenkai Zhou, Kaiqian Shu, Jingxuan Bi, Zhuzhu Du, Longhua Xu, Wei Ai
{"title":"Manipulating Zn2+ Depletion Zones and Deposition Kinetics via Self‐Concentrating Micro‐Reservoirs for Ah‐Scale Zn Metal Batteries","authors":"Xiaomei Huo, Guowei Gao, Boxin Li, Zhenkai Zhou, Kaiqian Shu, Jingxuan Bi, Zhuzhu Du, Longhua Xu, Wei Ai","doi":"10.1002/aenm.202502238","DOIUrl":"https://doi.org/10.1002/aenm.202502238","url":null,"abstract":"The glass fiber separator is a critical component in Zn metal batteries (ZMBs), but its disordered pores inadequately regulate the flow of anions and cations, leading to uncontrolled dendrite growth. Herein, the integration of ion self‐concentrating zincized hectorite (Zn‐HEC) layers into the separator is introduced and their crucial role in managing ion distribution and solvation on the surface of the Zn anode during battery operation is revealed. Density functional theory demonstrates that Zn‐HEC possesses a notable Zn<jats:sup>2+</jats:sup> self‐concentration capability, acting as microzone Zn<jats:sup>2+</jats:sup> reservoirs that promote rapid and even Zn<jats:sup>2+</jats:sup> transport. This feature prevents the formation of Zn<jats:sup>2+</jats:sup>‐depleted zones during Zn deposition. Moreover, the incorporated Zn‐HEC effectively curtails the migration of SO<jats:sub>4</jats:sub><jats:sup>2−</jats:sup> and significantly minimizes the desolvation barrier of hydrated Zn<jats:sup>2+</jats:sup>. Consequently, Zn‐HEC facilitates uniform Zn deposition along the (002) crystal planes of the Zn anode, enabling a lifespan of over 2000 h at 20 mA cm<jats:sup>−2</jats:sup> for 5 mAh cm<jats:sup>−2</jats:sup> and a cycle life of 500 h at an extraordinarily high rate of 50 mA cm<jats:sup>−2</jats:sup> (10 mAh cm<jats:sup>−2</jats:sup>). Moreover, the I<jats:sub>2</jats:sub>||GF@Zn‐HEC||Zn pouch cell with 1.6 Ah capacity exhibits outstanding cycling stability for 200 cycles. This study introduces a new approach for optimizing Zn deposition in next‐generation ZMBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"657 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144478979","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}
Haeryang Lim, Nam In Kim, Giwon Shin, Jaehun Lee, Sungryong Kim, Shin-Woo Myeong, Chiho Kim, Sung Mook Choi, Taiho Park
{"title":"Poly(fluorene)-Based Anion Exchange Membrane Demonstrating Excellent Durability at 1.5 A cm‒2 for 2400 h in Water Electrolyzers (Adv. Energy Mater. 24/2025)","authors":"Haeryang Lim, Nam In Kim, Giwon Shin, Jaehun Lee, Sungryong Kim, Shin-Woo Myeong, Chiho Kim, Sung Mook Choi, Taiho Park","doi":"10.1002/aenm.202570106","DOIUrl":"https://doi.org/10.1002/aenm.202570106","url":null,"abstract":"<p><b>Water Electrolyzers</b></p><p>In article number 2501038, Chiho Kim, Sung Mook Choi, Taiho Park, and co-workers developed a poly(fluorene)-based anion exchange membrane (AEM) for water electrolyzer (WE). The AEM with a simple structure and an interstitial alkyl chain exhibits superior hydroxide conductivity, excellent mechanical properties, and exceptional alkaline stability, demonstrating remarkable long-term durability of AEMWE.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 24","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570106","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144367299","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Benjamin Schumm, Arthur Dupuy, Milena Lux, Christian Girsule, Susanne Dörfler, Florian Schmidt, Magdalena Fiedler, Maria Rosner, Felix Hippauf, Stefan Kaskel
{"title":"Dry Battery Electrode Technology: From Early Concepts to Industrial Applications (Adv. Energy Mater. 24/2025)","authors":"Benjamin Schumm, Arthur Dupuy, Milena Lux, Christian Girsule, Susanne Dörfler, Florian Schmidt, Magdalena Fiedler, Maria Rosner, Felix Hippauf, Stefan Kaskel","doi":"10.1002/aenm.202570102","DOIUrl":"https://doi.org/10.1002/aenm.202570102","url":null,"abstract":"<p><b>Dry Battery Electrodes</b></p><p>In article number 2406011, Benjamin Schumm, Stefan Kaskel, and co-workers provide an in-depth literature review on dry coating as a promising approach toward environmentally friendly and efficient battery electrode production. The review focuses on polytetrafluoroethylene binder based dry film methods and summarizes the historical background, recent developments for lithium-ion and next-generation batteries, as well as approaches for upscaling and the challenges of the method.\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"15 24","pages":""},"PeriodicalIF":24.4,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/aenm.202570102","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144367529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ze‐Nong Zhang, Xiao‐Hui Wang, Qiu‐Yu Du, Qing‐Ling Hong, Xuan Ai, Yu Chen, Shu‐Ni Li
{"title":"Defect‐Rich AuCu/CuS Nanowires Heterojunction for Light‐Enhanced Sulfur Ion Electrooxidation Coupled Nitrite Electroreduction","authors":"Ze‐Nong Zhang, Xiao‐Hui Wang, Qiu‐Yu Du, Qing‐Ling Hong, Xuan Ai, Yu Chen, Shu‐Ni Li","doi":"10.1002/aenm.202500176","DOIUrl":"https://doi.org/10.1002/aenm.202500176","url":null,"abstract":"The nitrite electroreduction reaction (NO<jats:sub>2</jats:sub>ERR) offers a promising pathway for ammonia (NH<jats:sub>3</jats:sub>) synthesis and the remediation of nitrite pollutants. Copper (Cu)‐based nanomaterials have demonstrated significant potential as NO<jats:sub>2</jats:sub>ERR catalysts, but their catalytic activity and durability are hindered by limitations in the hydrogenation process. In this work, alloying and post‐sulfurization strategies are employed to synthesize AuCu/CuS nanowires (NWs), which feature abundant amorphous active sites and distinct electronic structures. AuCu/CuS NWs exhibit high electroactivity for both NO<jats:sub>2</jats:sub>ERR (Faradaic efficiency: 95.26%; NH<jats:sub>3</jats:sub> yield: 2.54 mg h<jats:sup>−1</jats:sup> g<jats:sub>cat</jats:sub><jats:sup>−1</jats:sup>) and sulfur ion electrooxidation reaction (SEOR, oxidation potential: −0.05 V at 10 mA cm<jats:sup>−2</jats:sup>). In situ characterization and theoretical calculations explain that amorphous CuS can modify the electronic property of AuCu alloy, thereby optimizing the adsorption of active hydrogen and nitrogen‐containing intermediates. Using AuCu/CuS NWs as a bifunctional electrocatalyst, the assembled NO<jats:sub>2</jats:sub>ERR||SEOR two‐electrode system only requires the electrolysis voltage of 0.77 V to obtain the current density of 10 mA cm<jats:sup>−2</jats:sup>, accompanied by the co‐production of sulfur and NH<jats:sub>3</jats:sub>. Under light irradiation conditions, the electrolysis voltage of the NO<jats:sub>2</jats:sub>ERR||SEOR two‐electrode system is further reduced under light irradiation conditions. This study offers a novel approach for the co‐generation of value‐added products through NO<jats:sub>2</jats:sub>ERR coupled with SEOR.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"50 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144370498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Impact of Cathode Microstructure on Sulfur Redox Kinetics in Lithium–Sulfur Batteries","authors":"Kameron Liao, Arumugam Manthiram","doi":"10.1002/aenm.202502062","DOIUrl":"https://doi.org/10.1002/aenm.202502062","url":null,"abstract":"Lithium–sulfur (Li–S) batteries offer high theoretical energy density and employ earth-abundant sulfur, making them a promising next-generation energy storage technology. Although essential for practical energy densities, high sulfur loadings, and lean-electrolyte contents lead to poor sulfur kinetics/utilization and cycle life. This study highlights the critical role of electrode microstructure in resolving these challenges. The particle morphology and size of a ketjenblack/sulfur composite are controlled through a scalable spray-drying procedure (SD-KB/S), producing an optimized cathode structure with uniform sulfur distribution and enhanced mechanical integrity with minimal electrode cracking. At a sulfur loading of 4 mg cm<sup>−2</sup> and an electrolyte-to-sulfur (E/S) ratio of 6, SD-KB/S cathodes exhibit stable cycling performance, retaining a capacity of 768 mA h g<sup>−1</sup> after 100 cycles, contrasting severe capacity fade with conventional electrodes. A cell overpotential deconvolution unveils that the activation overpotential (typically the largest barrier in conventional cells) is notably reduced in SD-KB/S cells. Although the concentration overpotential is also reduced with SD-KB/S, it becomes a prominent contributor to cell polarization, revealing the need to consider diffusional limitations in practical Li–S batteries. This work emphasizes the importance of advancing electrode and catalyst design concurrently—rather than sole catalyst development—to achieve high-performance and commercially viable Li–S batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"16 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144340965","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}
Bo Pang, Guihui Xie, Huimin Zhao, Fujun Cui, Chengbo Liu, Wanting Chen, Xiaoming Yan, Xuemei Wu, Gaohong He
{"title":"SCOF Hollow Fiber Constructing Ion Selective Conduction Nano-Pipeline Network for Vanadium Redox Flow Batteries","authors":"Bo Pang, Guihui Xie, Huimin Zhao, Fujun Cui, Chengbo Liu, Wanting Chen, Xiaoming Yan, Xuemei Wu, Gaohong He","doi":"10.1002/aenm.202500523","DOIUrl":"https://doi.org/10.1002/aenm.202500523","url":null,"abstract":"Hollow covalent organic frameworks (COFs) can decrease the resistance of proton conduction, however, the current micro-spherical or nano-rod morphology makes COFs only act as a disperse phase in membranes due to low aspect ratio. Herein, hollow fiber morphology of sulfonated covalent organic framework (HF-SCOF) is fabricated for the first time via a dissolution-diffusion control of monomers in different solvents during the electrospinning-solvothermal synthesis. The HF-SCOF mat is long-range orientated, with water/acid uptake in core cavity layer, and abundant sulfonic acid groups and protonated secondary amine along shell layer, thus establish continuous H<sup>+</sup>/V<sup>n+</sup> ion selective conduction nano-pipeline network in the membrane to maximize the advantages of SCOFs materials. Densified by sulfonated polybenzimidazole, the composite membrane exhibits excellent performance of vanadium redox flow battery. The energy efficiency reaches 81.9% at a high current density of 200 mA cm<sup>−2</sup>, and keeps stable during 1000 charging/discharging cycles, surpassing the performance of currently reported COFs-based membranes.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"70 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144341016","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}