Yingfei Li, Qiu Fang, Yichun Zheng, Liwu Fan, Yang Sun, Xuefeng Wang, Huilin Pan
Sodium (Na)‐ion batteries (NIBs) are emerging as a promising solution for large scale energy storage applications. Among various cathode chemistries, O3‐phase layered transition‐metal oxides stand out for their high energy density, yet their practical deployment is restricted by intricate phase transitions that induce lattice distortion, stress accumulation, and particle cracking, leading to rapid performance degradation. Here, we propose a temperature‐mediated strain‐management strategy to improve the phase reversibility and structural stability of O3‐phase oxide cathodes. Comprehensive structural and dynamic analyses reveal that optimal thermal regulation facilitates lattice strain release, mitigates detrimental stress accumulation that drives irreversible phase transitions, and accelerates Na + diffusion kinetics. As a result, structural degradation, transition‐metal dissolution, and capacity fading are effectively suppressed. This work provides a new perspective on employing external fields to overcome the intrinsic structural instability of layered oxides, offering fundamental insights for rational cathode design and reliable operation of practical NIBs for energy storage.
{"title":"Harnessing Temperature‐Mediated Strain Management to Realize Ultra‐Stable Oxide Cathodes in Na‐Ion Batteries","authors":"Yingfei Li, Qiu Fang, Yichun Zheng, Liwu Fan, Yang Sun, Xuefeng Wang, Huilin Pan","doi":"10.1002/aenm.202506239","DOIUrl":"https://doi.org/10.1002/aenm.202506239","url":null,"abstract":"Sodium (Na)‐ion batteries (NIBs) are emerging as a promising solution for large scale energy storage applications. Among various cathode chemistries, O3‐phase layered transition‐metal oxides stand out for their high energy density, yet their practical deployment is restricted by intricate phase transitions that induce lattice distortion, stress accumulation, and particle cracking, leading to rapid performance degradation. Here, we propose a temperature‐mediated strain‐management strategy to improve the phase reversibility and structural stability of O3‐phase oxide cathodes. Comprehensive structural and dynamic analyses reveal that optimal thermal regulation facilitates lattice strain release, mitigates detrimental stress accumulation that drives irreversible phase transitions, and accelerates Na <jats:sup>+</jats:sup> diffusion kinetics. As a result, structural degradation, transition‐metal dissolution, and capacity fading are effectively suppressed. This work provides a new perspective on employing external fields to overcome the intrinsic structural instability of layered oxides, offering fundamental insights for rational cathode design and reliable operation of practical NIBs for energy storage.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"92 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001576","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}
Potassium‐ion batteries (PIBs) and sodium‐ion batteries (SIBs) are promising next‐generation energy storage technologies because of their abundant and low‐cost raw materials. However, anodes for PIBs/SIBs often exhibit poor cycling stability, mainly due to particle fragmentation, loss of electrical connectivity, and continuous electrolyte decomposition from repetitive solid electrolyte interphase (SEI) formation. To address these challenges, a biomimetic pomegranate‐like core‐shell SnP 2 O 7 @PC anode (CSP‐SnP 2 O 7 @PC) is synthesised through pyrolysis‐driven Kirkendall effect of tin‐based phosphonate metal‐organic framework (MOF). This multi‐scale design integrates several key features. At the molecular scale, the in situ formation of Sn‐P‐O bonds reduces K + diffusion barriers. The nanoscale dispersion of SnP 2 O 7 within conductive carbon matrix promotes efficient electron and ion transport. Furthermore, microscale structural engineering creates pre‐reserved voids to accommodate volume expansion, suppress SEI overgrowth, and prevent cracking. The optimised anode demonstrates exceptional cycling stability, exhibiting ultralow capacity decay rate of 0.0015% per cycle over 16 000 cycles at 5 A g −1 , and also delivers excellent performance in SIBs. Density functional theory and finite element simulations further reveal beneficial electronic structures and stress distribution, providing fundamental insights for designing durable electrodes through crystal and electronic optimisation. Overall, this study presents an innovative strategy for mitigating volume expansion in high‐capacity battery materials.
{"title":"Solid Electrolyte Interphase Stabilized Pomegranate SnP 2 O 7 @PC Anodes Realized Through Kirkendall Effect of MOF for Durable Potassium/Sodium‐Ion Batteries","authors":"Huimin Jiang, Qiuju Fu, Xiaoyuan Sang, Hengxing Qiu, Shikai Liu, Quanliang Liu, Yingxin Zhang, Jianjian Lin, Xuebo Zhao","doi":"10.1002/aenm.202505082","DOIUrl":"https://doi.org/10.1002/aenm.202505082","url":null,"abstract":"Potassium‐ion batteries (PIBs) and sodium‐ion batteries (SIBs) are promising next‐generation energy storage technologies because of their abundant and low‐cost raw materials. However, anodes for PIBs/SIBs often exhibit poor cycling stability, mainly due to particle fragmentation, loss of electrical connectivity, and continuous electrolyte decomposition from repetitive solid electrolyte interphase (SEI) formation. To address these challenges, a biomimetic pomegranate‐like core‐shell SnP <jats:sub>2</jats:sub> O <jats:sub>7</jats:sub> @PC anode (CSP‐SnP <jats:sub>2</jats:sub> O <jats:sub>7</jats:sub> @PC) is synthesised through pyrolysis‐driven Kirkendall effect of tin‐based phosphonate metal‐organic framework (MOF). This multi‐scale design integrates several key features. At the molecular scale, the in situ formation of Sn‐P‐O bonds reduces K <jats:sup>+</jats:sup> diffusion barriers. The nanoscale dispersion of SnP <jats:sub>2</jats:sub> O <jats:sub>7</jats:sub> within conductive carbon matrix promotes efficient electron and ion transport. Furthermore, microscale structural engineering creates pre‐reserved voids to accommodate volume expansion, suppress SEI overgrowth, and prevent cracking. The optimised anode demonstrates exceptional cycling stability, exhibiting ultralow capacity decay rate of 0.0015% per cycle over 16 000 cycles at 5 A g <jats:sup>−1</jats:sup> , and also delivers excellent performance in SIBs. Density functional theory and finite element simulations further reveal beneficial electronic structures and stress distribution, providing fundamental insights for designing durable electrodes through crystal and electronic optimisation. Overall, this study presents an innovative strategy for mitigating volume expansion in high‐capacity battery materials.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"142 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001577","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}
Vasiliki Faka, Mohammed Alabdali, Martin A. Lange, Franco M. Zanotto, Can Yildirim, Mikael Dahl Kanedal, Jędrzej Kondek, Matthias Hartmann, Oliver Maus, Dominik Daisenberger, Michael Ryan Hansen, Jozef Keckes, Daniel Rettenwander, Alejandro A. Franco, Wolfgang G. Zeier
Solid-state battery fabrication requires the densification of solid electrolytes to achieve optimal cycling performance and high energy density. However, the underlying compaction mechanisms of these electrolytes remain poorly understood. Here, we investigate the effect of pressure consolidation on the ionic conductor Li6PS5Cl with particle size distributions (PSD) ranging from 4 to 40 µm. Heckel analysis reveals that samples with smaller PSDs exhibit higher compressibility at lower pressures. X-ray diffraction peak profiling shows that applied pressure induces lattice strain, leading to peak broadening, while pair distribution function analysis demonstrates a reduction in coherence length upon pressing. Dark-field X-ray microscopy further provides spatially resolved orientation maps, uncovering intragranular structural variations within individual Li6PS5Cl agglomerates after compression. To better understand the origin of stress fluctuations, we performed discrete element method simulations using the experimental PSDs. The results indicate that smaller particles and broader PSDs experience higher stresses, whereas monodisperse systems do not exhibit significant stress fluctuations with position or particle size. This suggests that the high strain observed cannot be attributed solely to smaller particles, but rather to size inhomogeneity. Overall, these findings highlight that both particle size and its distribution play a critical role in processing solid electrolytes for solid-state batteries.
{"title":"How Particle Size Affects Consolidation Behavior, Strain and Properties of Li6PS5Cl Fast Ionic Conductors","authors":"Vasiliki Faka, Mohammed Alabdali, Martin A. Lange, Franco M. Zanotto, Can Yildirim, Mikael Dahl Kanedal, Jędrzej Kondek, Matthias Hartmann, Oliver Maus, Dominik Daisenberger, Michael Ryan Hansen, Jozef Keckes, Daniel Rettenwander, Alejandro A. Franco, Wolfgang G. Zeier","doi":"10.1002/aenm.202505186","DOIUrl":"https://doi.org/10.1002/aenm.202505186","url":null,"abstract":"Solid-state battery fabrication requires the densification of solid electrolytes to achieve optimal cycling performance and high energy density. However, the underlying compaction mechanisms of these electrolytes remain poorly understood. Here, we investigate the effect of pressure consolidation on the ionic conductor Li<sub>6</sub>PS<sub>5</sub>Cl with particle size distributions (PSD) ranging from 4 to 40 µm. Heckel analysis reveals that samples with smaller PSDs exhibit higher compressibility at lower pressures. X-ray diffraction peak profiling shows that applied pressure induces lattice strain, leading to peak broadening, while pair distribution function analysis demonstrates a reduction in coherence length upon pressing. Dark-field X-ray microscopy further provides spatially resolved orientation maps, uncovering intragranular structural variations within individual Li<sub>6</sub>PS<sub>5</sub>Cl agglomerates after compression. To better understand the origin of stress fluctuations, we performed discrete element method simulations using the experimental PSDs. The results indicate that smaller particles and broader PSDs experience higher stresses, whereas monodisperse systems do not exhibit significant stress fluctuations with position or particle size. This suggests that the high strain observed cannot be attributed solely to smaller particles, but rather to size inhomogeneity. Overall, these findings highlight that both particle size and its distribution play a critical role in processing solid electrolytes for solid-state batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"57 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"146001562","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}
Yuwei Liu, Sheng Cao, Yuxiang Su, Longqiang Bao, Ruifeng Liang, Yi Liang, Yubing Li, Dong Cai, Bingsuo Zou
Dual‐band electrochromic windows (DEWs) enable selective modulation of visible (VIS) and near‐infrared (NIR) solar radiation, providing an effective strategy to reduce building energy consumption. Conventional electrochromic materials, however, undergo lattice distortion, interfacial stress, and irreversible phase transitions during repeated ion intercalation/deintercalation, which lead to rapid optical degradation. Herein, we report ultra‐stable DEWs based on shear‐phase Nb 2 O 5 with electronic‐structure engineering via W 6+ doping. The 2D shear‐phase framework suppresses phase transitions and volume expansion during cycling, while W 6+ substitution introduces oxygen vacancies and strengthens ion‐lattice coupling through d‐p orbital hybridization. The combination of structural and electronic optimization enhances electronic conductivity and reduces the ion diffusion barrier. As a result, W‐doped Nb 2 O 5 films achieve large optical modulation of 92.3% at 633 nm and 93.8% at 1200 nm, rapid switching (coloration/bleaching: 3.4/2.8 s at 633 nm and 2.4/5.2 s at 1200 nm), excellent bistability, and outstanding cycling stability, with less than 10% optical loss after 100 000 cycles. Simulations demonstrate that these DEWs offer substantial energy‐saving potential under diverse climates, and their integration with photovoltaic‐electrochromic systems enables self‐powered operation. This study establishes the first intrinsic stabilization mechanism for Nb 2 O 5 ‐based dual‐band electrochromism and provides a general design principle for durable, energy‐efficient smart windows.
{"title":"Ultra‐Stable Dual‐Band Electrochromic Windows Enabled by Shear‐Phase Niobium Oxide","authors":"Yuwei Liu, Sheng Cao, Yuxiang Su, Longqiang Bao, Ruifeng Liang, Yi Liang, Yubing Li, Dong Cai, Bingsuo Zou","doi":"10.1002/aenm.202505972","DOIUrl":"https://doi.org/10.1002/aenm.202505972","url":null,"abstract":"Dual‐band electrochromic windows (DEWs) enable selective modulation of visible (VIS) and near‐infrared (NIR) solar radiation, providing an effective strategy to reduce building energy consumption. Conventional electrochromic materials, however, undergo lattice distortion, interfacial stress, and irreversible phase transitions during repeated ion intercalation/deintercalation, which lead to rapid optical degradation. Herein, we report ultra‐stable DEWs based on shear‐phase Nb <jats:sub>2</jats:sub> O <jats:sub>5</jats:sub> with electronic‐structure engineering via W <jats:sup>6+</jats:sup> doping. The 2D shear‐phase framework suppresses phase transitions and volume expansion during cycling, while W <jats:sup>6+</jats:sup> substitution introduces oxygen vacancies and strengthens ion‐lattice coupling through <jats:italic>d‐p</jats:italic> orbital hybridization. The combination of structural and electronic optimization enhances electronic conductivity and reduces the ion diffusion barrier. As a result, W‐doped Nb <jats:sub>2</jats:sub> O <jats:sub>5</jats:sub> films achieve large optical modulation of 92.3% at 633 nm and 93.8% at 1200 nm, rapid switching (coloration/bleaching: 3.4/2.8 s at 633 nm and 2.4/5.2 s at 1200 nm), excellent bistability, and outstanding cycling stability, with less than 10% optical loss after 100 000 cycles. Simulations demonstrate that these DEWs offer substantial energy‐saving potential under diverse climates, and their integration with photovoltaic‐electrochromic systems enables self‐powered operation. This study establishes the first intrinsic stabilization mechanism for Nb <jats:sub>2</jats:sub> O <jats:sub>5</jats:sub> ‐based dual‐band electrochromism and provides a general design principle for durable, energy‐efficient smart windows.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"26 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145993205","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 integration of electrocatalytic 5‐hydroxymethylfurfural (HMF) oxidation with the hydrogen evolution reaction (HER) is a win‐win strategy that enables the concurrent production of high‐value chemicals and low‐energy hydrogen. However, HMF oxidation suffers from competing adsorption between organics and OH − along with continuous redox cycling of active sites, leading to unsatisfactory activity, selectivity, and stability. To address these challenges, we designed a VO 2 /Ni 3 S 2 composite catalyst with rich cationic vacancies and low vanadium content. This catalyst creates Ni─V dual active sites that trigger an alternative reaction pathway. VO 2 /Ni 3 S 2 achieves high HMF conversion (97.1%), Faradaic efficiency (96.0%), and selectivity (98.93%) toward FDCA, along with robust stability. In an integrated HMFOR||HER system using VO 2 /Ni 3 S 2 for both electrodes, a current density of 100 mA cm −2 was attained at a low cell voltage of 1.76 V. Mechanistic studies reveal that VO 2 ‐induced vacancies promote the formation of high‐valence Ni species, while adjacent V sites enhance OH adsorption. This configuration enables balanced co‐adsorption of HMF and OH − . Unlike conventional single‐site Ni catalysis, the Ni─V dual sites optimize the dehydrogenation pathway while preserving the high oxidation state of Ni. This study sheds new light on the catalyst design for energy‐efficient biomass valorization and hydrogen production.
{"title":"Ni─V Dual Sites Boost Nucleophilic Electrooxidation Coupling With Cathodic Hydrogen Production","authors":"Mengran Zeng, Haeseong Jang, Zijian Li, Xiaoyue Zhu, Wenquan Zhang, Wenlie Lin, Jaephil Cho, Shangguo Liu, Xien Liu, Qing Qin","doi":"10.1002/aenm.202505773","DOIUrl":"https://doi.org/10.1002/aenm.202505773","url":null,"abstract":"The integration of electrocatalytic 5‐hydroxymethylfurfural (HMF) oxidation with the hydrogen evolution reaction (HER) is a win‐win strategy that enables the concurrent production of high‐value chemicals and low‐energy hydrogen. However, HMF oxidation suffers from competing adsorption between organics and OH <jats:sup>−</jats:sup> along with continuous redox cycling of active sites, leading to unsatisfactory activity, selectivity, and stability. To address these challenges, we designed a VO <jats:sub>2</jats:sub> /Ni <jats:sub>3</jats:sub> S <jats:sub>2</jats:sub> composite catalyst with rich cationic vacancies and low vanadium content. This catalyst creates Ni─V dual active sites that trigger an alternative reaction pathway. VO <jats:sub>2</jats:sub> /Ni <jats:sub>3</jats:sub> S <jats:sub>2</jats:sub> achieves high HMF conversion (97.1%), Faradaic efficiency (96.0%), and selectivity (98.93%) toward FDCA, along with robust stability. In an integrated HMFOR||HER system using VO <jats:sub>2</jats:sub> /Ni <jats:sub>3</jats:sub> S <jats:sub>2</jats:sub> for both electrodes, a current density of 100 mA cm <jats:sup>−2</jats:sup> was attained at a low cell voltage of 1.76 V. Mechanistic studies reveal that VO <jats:sub>2</jats:sub> ‐induced vacancies promote the formation of high‐valence Ni species, while adjacent V sites enhance OH adsorption. This configuration enables balanced co‐adsorption of HMF and OH <jats:sup>−</jats:sup> . Unlike conventional single‐site Ni catalysis, the Ni─V dual sites optimize the dehydrogenation pathway while preserving the high oxidation state of Ni. This study sheds new light on the catalyst design for energy‐efficient biomass valorization and hydrogen production.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"49 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145993179","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}
Michael Wolf, Benjamin vom Hau, Rebecca Wilhelm, Matti M. Kaye, Aaron Stoeckle, Johannes Kriegler, Florian Schmidt, Stefan Stojcevic, Korbinian Huber, Simon Lux
This study presents a novel dry‐coating process for the scalable production of sulfidic ASSB cathodes within a dry room environment. Composite powders, consisting of 82.0 wt% NCM85 and 0.5 wt% PTFE, are mixed and fibrillated using a twin‐screw extruder. Dry‐coated cathode films are manufactured using a two‐roll calender through a single high‐shear calendering step. The study explores the impact of processing parameters on the morphology of electrodes and cell performance. Furthermore, the findings are compared to a slurry reference. Increasing the process temperature and reducing the line load enhances PTFE fibrillation and mitigates CAM particle cracking. These adjustments improve electrode homogeneity, density, and CAM–SE interface contact. The improvements are attributed to the deformation of LPSCl particles under shear stress, especially at higher temperatures. XPS analysis reveals temperature‐driven degradation of LPSCl, forming Li 2 S. Despite lower electronic conductivity, dry‐coated cathodes exhibit superior ionic conductivity compared to the slurry reference. Single‐layer pouch cells with dry‐coated cathodes demonstrate enhanced initial capacity, ICE, and discharge rate capability. Optimal performance is achieved with electrodes produced with high extrusion temperature (100°C), medium calender temperature (60°C), and low line load (50 N mm −1 ).
本研究提出了一种在干燥室内环境下可扩展生产硫化物ASSB阴极的新型干涂工艺。复合粉末，由82.0 wt% NCM85和0.5 wt% PTFE组成，使用双螺杆挤出机混合和纤化。干涂阴极薄膜是使用双辊压延机通过一个单一的高剪切压延步骤制造的。该研究探讨了加工参数对电极形态和电池性能的影响。此外，研究结果与泥浆参考进行了比较。提高工艺温度和降低生产线负荷可以增强PTFE的纤颤，减轻CAM颗粒的开裂。这些调整改善了电极均匀性、密度和CAM-SE界面接触。这种改善是由于LPSCl颗粒在剪切应力下的变形，特别是在高温下。XPS分析揭示了温度驱动的LPSCl降解，形成Li 2s，尽管电子电导率较低，但与浆液对照相比，干涂阴极表现出优异的离子电导率。采用干涂阴极的单层袋状电池显示出增强的初始容量、ICE和放电速率能力。在高挤压温度（100°C），中等压延温度（60°C）和低线负载（50 N mm−1）下生产的电极可实现最佳性能。
{"title":"Impact of Extrusion and Direct Calendering on Dry‐Coated Cathodes for Sulfidic All‐Solid‐State Batteries","authors":"Michael Wolf, Benjamin vom Hau, Rebecca Wilhelm, Matti M. Kaye, Aaron Stoeckle, Johannes Kriegler, Florian Schmidt, Stefan Stojcevic, Korbinian Huber, Simon Lux","doi":"10.1002/aenm.202506443","DOIUrl":"https://doi.org/10.1002/aenm.202506443","url":null,"abstract":"This study presents a novel dry‐coating process for the scalable production of sulfidic ASSB cathodes within a dry room environment. Composite powders, consisting of 82.0 wt% NCM85 and 0.5 wt% PTFE, are mixed and fibrillated using a twin‐screw extruder. Dry‐coated cathode films are manufactured using a two‐roll calender through a single high‐shear calendering step. The study explores the impact of processing parameters on the morphology of electrodes and cell performance. Furthermore, the findings are compared to a slurry reference. Increasing the process temperature and reducing the line load enhances PTFE fibrillation and mitigates CAM particle cracking. These adjustments improve electrode homogeneity, density, and CAM–SE interface contact. The improvements are attributed to the deformation of LPSCl particles under shear stress, especially at higher temperatures. XPS analysis reveals temperature‐driven degradation of LPSCl, forming Li <jats:sub>2</jats:sub> S. Despite lower electronic conductivity, dry‐coated cathodes exhibit superior ionic conductivity compared to the slurry reference. Single‐layer pouch cells with dry‐coated cathodes demonstrate enhanced initial capacity, ICE, and discharge rate capability. Optimal performance is achieved with electrodes produced with high extrusion temperature (100°C), medium calender temperature (60°C), and low line load (50 N mm <jats:sup>−</jats:sup> <jats:sup>1</jats:sup> ).","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"85 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145993204","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}
Jonas Wortmann, Larry Luer, Chao Liu, Jerrit Wagner, Tobias Osterrieder, Simon Arnold, Jens Hauch, Thomas Heumüller, Christoph J. Brabec
Organic Photovoltaic (OPV) devices show a large gap between laboratory-recorded cells with over 20% efficiency and commercial roll-to-roll printed modules reaching a maximum half that efficiency. A novel OPV material not only needs high efficiency, but must be processable in architectures suited for large-scale applications and provide sufficient stability under various stress factors. We present a holistic screening protocol to cover all relevant aspects of OPV material development. Using machine learning techniques together with systematic experimental protocols, only a minimum amount of a novel semiconductor is necessary. We utilize process parameters, optical features, and IV data to explore the processing window, benchmark process stability, and enable structure-property predictions. We implement a combinatorial degradation protocol that investigates key stress factors, like temperature, oxygen, and illumination, at different stages of device fabrication. Testing partially finished devices, conventional and inverted architectures, as well as hole-only and electron-only devices, enables the identification of individual layers responsible for degradation. The protocol includes a solvent test to investigate processability with green solvents. The systematic data collected in this protocol provides a general and reliable basis for material development and the imminent creation of digital twins for OPV.
{"title":"Accelerating the Development of Organic Solar Cells: A Standardized Protocol with Machine Learning Integration","authors":"Jonas Wortmann, Larry Luer, Chao Liu, Jerrit Wagner, Tobias Osterrieder, Simon Arnold, Jens Hauch, Thomas Heumüller, Christoph J. Brabec","doi":"10.1002/aenm.202506139","DOIUrl":"https://doi.org/10.1002/aenm.202506139","url":null,"abstract":"Organic Photovoltaic (OPV) devices show a large gap between laboratory-recorded cells with over 20% efficiency and commercial roll-to-roll printed modules reaching a maximum half that efficiency. A novel OPV material not only needs high efficiency, but must be processable in architectures suited for large-scale applications and provide sufficient stability under various stress factors. We present a holistic screening protocol to cover all relevant aspects of OPV material development. Using machine learning techniques together with systematic experimental protocols, only a minimum amount of a novel semiconductor is necessary. We utilize process parameters, optical features, and IV data to explore the processing window, benchmark process stability, and enable structure-property predictions. We implement a combinatorial degradation protocol that investigates key stress factors, like temperature, oxygen, and illumination, at different stages of device fabrication. Testing partially finished devices, conventional and inverted architectures, as well as hole-only and electron-only devices, enables the identification of individual layers responsible for degradation. The protocol includes a solvent test to investigate processability with green solvents. The systematic data collected in this protocol provides a general and reliable basis for material development and the imminent creation of digital twins for OPV.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145972344","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}
Ni-rich layered oxides and Li-rich layered oxides are technologically important high-capacity cathode materials for constructing high-energy-density batteries. However, their practical application is severely limited by interfacial instability and structural degradation during cycling. Herein, an organic-inorganic hybrid polymer (PHM-T) composed of titanium-oxo clusters (TOCs) cross-linked polyurethane is proposed to stabilize high-capacity layered oxides. Rationally designing the soft and hard domains of polyurethane endows PHM-T with high mechanical strength, excellent electrolyte tolerance, and strong cathode affinity. When employed as a surface coating layer, PHM-T acts as an artificial cathode electrolyte interphase and dramatically improves the structural and compositional stabilities of both Ni-rich layered oxides and Li-rich layered oxides. With the suppressed lattice distortion and transition-metal dissolution, the PHM-T coated LiNi0.8Mn0.1Co0.1O2 achieves enhanced rate capability (149.8 mAh g−1 at 10 C) and cycling stability (78% capacity retention after 200 cycles at 1 C). More impressively, the TOC cross-linked polymer can serve directly as a reinforced binder, enabling one-step surface modification and electrode fabrication without the pre-coating process, offering a convenient and industrially Binder engineering, Cathode-electrolyte interphase, Layered cathode materials, Nanocluster cross-linked polymer, interfacial engineeringcompatible “two-in-one” interfacial-engineering route to develop high-performance batteries.
富镍层状氧化物和富锂层状氧化物是构建高能量密度电池的技术重要的高容量正极材料。然而，它们的实际应用受到循环过程中界面不稳定性和结构退化的严重限制。本文提出了一种由钛-氧簇（TOCs）交联聚氨酯组成的有机-无机杂化聚合物（PHM-T）来稳定高容量层状氧化物。合理设计聚氨酯的软、硬畴，使PHM-T具有较高的机械强度、优异的电解质耐受性和较强的阴极亲和力。当PHM-T用作表面涂层时，作为人工阴极电解质界面，显著提高了富镍层状氧化物和富锂层状氧化物的结构和组成稳定性。在抑制了晶格变形和过渡金属溶解的情况下，PHM-T涂层的LiNi0.8Mn0.1Co0.1O2获得了更高的倍率性能（10℃下149.8 mAh g−1）和循环稳定性（1℃下200次循环后78%的容量保持率）。更令人印象深刻的是，TOC交联聚合物可以直接用作增强粘合剂，无需预涂覆过程即可一步表面改性和电极制造，为粘合剂工程、阴极-电解质界面、层状阴极材料、纳米簇交联聚合物、界面工程兼容的“二合一”界面工程提供了方便和工业化的途径，以开发高性能电池。
{"title":"Stabilizing High-Capacity Layered Cathode Materials via Nanocluster Cross-Linked Polymer","authors":"Shuchang Liu, Yanru Zeng, Hao Wang, Cuimiao Wang, Rongrong Zhang, Chaozhi Wang, Jingqin Cui, Xiaoliang Fang","doi":"10.1002/aenm.202506402","DOIUrl":"https://doi.org/10.1002/aenm.202506402","url":null,"abstract":"Ni-rich layered oxides and Li-rich layered oxides are technologically important high-capacity cathode materials for constructing high-energy-density batteries. However, their practical application is severely limited by interfacial instability and structural degradation during cycling. Herein, an organic-inorganic hybrid polymer (PHM-T) composed of titanium-oxo clusters (TOCs) cross-linked polyurethane is proposed to stabilize high-capacity layered oxides. Rationally designing the soft and hard domains of polyurethane endows PHM-T with high mechanical strength, excellent electrolyte tolerance, and strong cathode affinity. When employed as a surface coating layer, PHM-T acts as an artificial cathode electrolyte interphase and dramatically improves the structural and compositional stabilities of both Ni-rich layered oxides and Li-rich layered oxides. With the suppressed lattice distortion and transition-metal dissolution, the PHM-T coated LiNi<sub>0.8</sub>Mn<sub>0.1</sub>Co<sub>0.1</sub>O<sub>2</sub> achieves enhanced rate capability (149.8 mAh g<sup>−1</sup> at 10 C) and cycling stability (78% capacity retention after 200 cycles at 1 C). More impressively, the TOC cross-linked polymer can serve directly as a reinforced binder, enabling one-step surface modification and electrode fabrication without the pre-coating process, offering a convenient and industrially Binder engineering, Cathode-electrolyte interphase, Layered cathode materials, Nanocluster cross-linked polymer, interfacial engineeringcompatible “two-in-one” interfacial-engineering route to develop high-performance batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"270 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145972346","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}
Fangzhen Han, Chuanshun Xing, Ming-Yu Chen, Xin Liu, Kai Jiang, Yijie Wang, Hai-sheng Su, Yiqun Du, Wenqiang Gao, Hong Liu, Weijia Zhou
Tuning the adsorption behavior of key reaction intermediates is the crucial pathway for optimizing the performance of Cu-based catalysts in electrochemical nitrate reduction to ammonia. Constructing tandem catalytic sites by alloying to regulate the adsorption properties of nitrate and protons is regarded as a key approach to enhancing the performance of NH3-oriented conversion. However, constructing the self-tandem catalytic sites merely on the Cu surface remains a challenge. Here, we report a Cu-based catalyst featuring unsaturated defect sites on its surface. This catalyst achieves an NH3 Faradaic efficiency approaching 92.37% and a production rate of 2.0 mmol cm−2 h−1 at −0.4 V versus the reversible hydrogen electrode. Through electrokinetic analysis, in situ spectroscopic investigation, and theoretical calculations, we reveal that this catalyst realizes efficient self-tandem catalysis via its dual active sites, in which the Cu(111) facet serves as the active site for selective nitrate adsorption, while the engineered surface unsaturated defect sites promote water activation to supply protons. This synergistic effect not only optimizes the proton-coupled electron transfer step (identified as the rate-determining step) but also balances the surface coverage of nitrate and protons. These findings hold significant guiding implications for designing effective Cu-based self-tandem catalytic sites in electrochemical nitrate reduction.
{"title":"Self-Tandem Catalysis of Unsaturated Cu with Dual Active Sites for Efficient Ammonia Electrosynthesis","authors":"Fangzhen Han, Chuanshun Xing, Ming-Yu Chen, Xin Liu, Kai Jiang, Yijie Wang, Hai-sheng Su, Yiqun Du, Wenqiang Gao, Hong Liu, Weijia Zhou","doi":"10.1002/aenm.202506098","DOIUrl":"https://doi.org/10.1002/aenm.202506098","url":null,"abstract":"Tuning the adsorption behavior of key reaction intermediates is the crucial pathway for optimizing the performance of Cu-based catalysts in electrochemical nitrate reduction to ammonia. Constructing tandem catalytic sites by alloying to regulate the adsorption properties of nitrate and protons is regarded as a key approach to enhancing the performance of NH<sub>3</sub>-oriented conversion. However, constructing the self-tandem catalytic sites merely on the Cu surface remains a challenge. Here, we report a Cu-based catalyst featuring unsaturated defect sites on its surface. This catalyst achieves an NH<sub>3</sub> Faradaic efficiency approaching 92.37% and a production rate of 2.0 mmol cm<sup>−2</sup> h<sup>−1</sup> at −0.4 V versus the reversible hydrogen electrode. Through electrokinetic analysis, in situ spectroscopic investigation, and theoretical calculations, we reveal that this catalyst realizes efficient self-tandem catalysis via its dual active sites, in which the Cu(111) facet serves as the active site for selective nitrate adsorption, while the engineered surface unsaturated defect sites promote water activation to supply protons. This synergistic effect not only optimizes the proton-coupled electron transfer step (identified as the rate-determining step) but also balances the surface coverage of nitrate and protons. These findings hold significant guiding implications for designing effective Cu-based self-tandem catalytic sites in electrochemical nitrate reduction.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"76 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145972474","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}
HyunWoo Chang, Jae Hyun Ryu, KwangHo Lee, JeongHan Roh, SangJae Lee, Junu Bak, DongWon Shin, MinJun Kim, HyunWoo Yang, Won Bo Lee, EunAe Cho
Promotion of atomic ordering in Pt-based intermetallic compounds (IMCs) is a proven strategy to enhance catalytic activity and durability, for the cathode catalysts in proton exchange membrane fuel cells (PEMFCs). However, achieving higher atomic ordering typically requires elevated temperature annealing, which induces nanoparticles (NPs) sintering and surface area loss, resulting in a challenge for catalyst design. Here, we demonstrate that Zn incorporation in L10-PtCo IMCs promotes the ordering, endowing the enhanced stability and activity. Machine learning interatomic potential (MLIP) simulations reveal that Zn lowers vacancy formation energies and modifies atomic migration, thereby accelerating ordering during annealing. These results are validated experimentally by X-ray-based analyses. Electrochemical measurements show that L10-Zn-PtCo/ZnNC achieves a mass activity (MA) of 1.76 A mgPt−1 at 0.9 VRHE, outperforming Pt/C (0.24 A mgPt−1). In single-cell tests, it delivers 438 mA cm−2 at 0.7 V, surpassing Pt/C (293 mA cm−2). After 30 000 cycles, it retains 89.7% initial current density, compared with only 54.6% retention for Pt/C. By integrating ML-guided design with experimental validation, this work establishes a rational strategy to engineer atomically ordered Pt-based IMCs under practical conditions, advancing the development of efficient electrocatalysts.
提高pt基金属间化合物（IMCs）的原子有序性是质子交换膜燃料电池（pemfc）阴极催化剂提高催化活性和耐久性的一种有效策略。然而，实现更高的原子有序通常需要高温退火，这会导致纳米颗粒（NPs）烧结和表面积损失，从而给催化剂设计带来挑战。在这里，我们证明了Zn在L10-PtCo IMCs中的掺入促进了有序，赋予了增强的稳定性和活性。机器学习原子间势（MLIP）模拟表明，Zn降低了空位形成能，改变了原子迁移，从而加速了退火过程中的有序。这些结果通过基于x射线的实验分析得到了验证。电化学测量表明，L10-Zn-PtCo/ZnNC在0.9 VRHE下的质量活度（MA）为1.76 a mgPt−1，优于Pt/C （0.24 a mgPt−1）。在单电池测试中，它在0.7 V下提供438 mA cm - 2，超过Pt/C （293 mA cm - 2）。经过3万次循环后，它保持了89.7%的初始电流密度，而Pt/C只保持了54.6%。通过将机器学习引导设计与实验验证相结合，本工作建立了在实际条件下设计原子有序pt基IMCs的合理策略，推动了高效电催化剂的发展。
{"title":"Machine Learning-Guided Design of L10-PtCo Intermetallic Catalysts: Zn-Mediated Atomic Ordering","authors":"HyunWoo Chang, Jae Hyun Ryu, KwangHo Lee, JeongHan Roh, SangJae Lee, Junu Bak, DongWon Shin, MinJun Kim, HyunWoo Yang, Won Bo Lee, EunAe Cho","doi":"10.1002/aenm.202505211","DOIUrl":"https://doi.org/10.1002/aenm.202505211","url":null,"abstract":"Promotion of atomic ordering in Pt-based intermetallic compounds (IMCs) is a proven strategy to enhance catalytic activity and durability, for the cathode catalysts in proton exchange membrane fuel cells (PEMFCs). However, achieving higher atomic ordering typically requires elevated temperature annealing, which induces nanoparticles (NPs) sintering and surface area loss, resulting in a challenge for catalyst design. Here, we demonstrate that Zn incorporation in L1<sub>0</sub>-PtCo IMCs promotes the ordering, endowing the enhanced stability and activity. Machine learning interatomic potential (MLIP) simulations reveal that Zn lowers vacancy formation energies and modifies atomic migration, thereby accelerating ordering during annealing. These results are validated experimentally by X-ray-based analyses. Electrochemical measurements show that L1<sub>0</sub>-Zn-PtCo/ZnNC achieves a mass activity (MA) of 1.76 A mg<sub>Pt</sub><sup>−1</sup> at 0.9 V<sub>RHE</sub>, outperforming Pt/C (0.24 A mg<sub>Pt</sub><sup>−1</sup>). In single-cell tests, it delivers 438 mA cm<sup>−2</sup> at 0.7 V, surpassing Pt/C (293 mA cm<sup>−2</sup>). After 30 000 cycles, it retains 89.7% initial current density, compared with only 54.6% retention for Pt/C. By integrating ML-guided design with experimental validation, this work establishes a rational strategy to engineer atomically ordered Pt-based IMCs under practical conditions, advancing the development of efficient electrocatalysts.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"81 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2026-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145972638","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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