Shaoxiang Zhang, Rongbing Han, Zhong Lin Wang, Tao Jiang
Water wave energy is a clean, renewable energy source that, unlike fossil fuels, produces no greenhouse gases or other pollutants. This study proposes a novel cantilever oscillating float‐type triboelectric nanogenerator (COF‐TENG) for efficient blue energy harvesting. The cantilevered float structure transfers substantial wave‐induced forces to the internal power generation units, with the float's wave energy absorption efficiency being the primary factor influencing overall power generation. The vertical wave forces on floats of various shapes are analyzed using micro‐amplitude wave theory and the Froude‐Krylov hypothesis, enabling identification of the optimal float geometry under identical conditions. The float's motion under wave excitation is then simulated via computational fluid dynamics (CFD). The optimized float achieves a theoretical energy absorption efficiency of up to 37.7%. Under real wave excitation, the COF‐TENG delivers a maximum output power density of 14.9 W m −3 Hz −1 . Wave energy harvesting further enables self‐powered temperature‐humidity and water quality monitoring. This work provides theoretical guidance for float optimization and offers new insights into blue energy harvesting for self‐powered environmental monitoring.
水波能是一种清洁的可再生能源，与化石燃料不同，它不产生温室气体或其他污染物。本研究提出了一种新型悬臂振荡浮子型摩擦纳米发电机（COF - TENG），用于高效的蓝色能量收集。悬臂浮子结构将大量的波浪力传递给内部发电单元，浮子的波浪能吸收效率是影响整体发电的主要因素。利用微振幅波理论和Froude - Krylov假设分析了不同形状浮子上的垂直波浪力，从而确定了相同条件下的最佳浮子几何形状。然后通过计算流体动力学（CFD）模拟波浪激励下浮子的运动。优化后的浮子理论吸能效率可达37.7%。在实波激励下，COF‐TENG的最大输出功率密度为14.9 W m−3 Hz−1。波浪能收集进一步实现自供电的温度、湿度和水质监测。这项工作为浮子优化提供了理论指导，并为自供电环境监测的蓝色能量收集提供了新的见解。
{"title":"Fur‐Brush Disk Triboelectric Nanogenerator Driven by Cantilever Oscillating Float Mechanism for Near‐Shore Marine Environment Monitoring","authors":"Shaoxiang Zhang, Rongbing Han, Zhong Lin Wang, Tao Jiang","doi":"10.1002/aenm.202503847","DOIUrl":"https://doi.org/10.1002/aenm.202503847","url":null,"abstract":"Water wave energy is a clean, renewable energy source that, unlike fossil fuels, produces no greenhouse gases or other pollutants. This study proposes a novel cantilever oscillating float‐type triboelectric nanogenerator (COF‐TENG) for efficient blue energy harvesting. The cantilevered float structure transfers substantial wave‐induced forces to the internal power generation units, with the float's wave energy absorption efficiency being the primary factor influencing overall power generation. The vertical wave forces on floats of various shapes are analyzed using micro‐amplitude wave theory and the Froude‐Krylov hypothesis, enabling identification of the optimal float geometry under identical conditions. The float's motion under wave excitation is then simulated via computational fluid dynamics (CFD). The optimized float achieves a theoretical energy absorption efficiency of up to 37.7%. Under real wave excitation, the COF‐TENG delivers a maximum output power density of 14.9 W m <jats:sup>−3</jats:sup> Hz <jats:sup>−1</jats:sup> . Wave energy harvesting further enables self‐powered temperature‐humidity and water quality monitoring. This work provides theoretical guidance for float optimization and offers new insights into blue energy harvesting for self‐powered environmental monitoring.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"230 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145731993","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}
This review critically examines recent progress in thermoelectric thin films synthesized by atomic layer deposition (ALD), with emphasis on their transport properties, growth strategies, and challenges. Chalcogenide thin films are discussed as the most direct analogs of conventional bulk thermoelectric materials, where ALD enables precise tuning of thickness, crystallinity, and carrier concentration, allowing comparative evaluation against conventional thin film deposition methods. Doped oxides and ternary oxides, particularly ZnO‐based systems with Al, Ga, or transition‐metal dopants, are highlighted as another important class, combining high‐temperature stability with tunable electronic transport, albeit with lower power factors than chalcogenides. Recent advances in molecular layer deposition have allowed the implementation of ALD/MLD multilayers and superlattices, showing how interface engineering and nanoscale modulation of potential barriers can influence carrier scattering and phonon transport. In parallel, we review precursor chemistry, deposition temperature windows, and process limitations, including environmental and safety considerations, to provide practical guidance for reproducibility and scalability. A comparative analysis with results from other deposition methods underlines that while ALD does not intrinsically outperform other deposition techniques, it offers complementary advantages in conformality and sub‐nanometer composition control, making it a powerful option for complex device architectures. Altogether, the review situates ALD‐grown thin films within the broader thermoelectric landscape, highlighting both their potential and the critical bottlenecks that remain.
{"title":"Advances in Thermoelectric Thin Films Grown by Atomic Layer Deposition: A Critical Review of Performance and Challenges","authors":"Jorge Luis Vazquez‐Arce, Dong‐Ho Shin, Shuyue Yao, Shiyang He, Kornelius Nielsch, Amin Bahrami","doi":"10.1002/aenm.202502982","DOIUrl":"https://doi.org/10.1002/aenm.202502982","url":null,"abstract":"This review critically examines recent progress in thermoelectric thin films synthesized by atomic layer deposition (ALD), with emphasis on their transport properties, growth strategies, and challenges. Chalcogenide thin films are discussed as the most direct analogs of conventional bulk thermoelectric materials, where ALD enables precise tuning of thickness, crystallinity, and carrier concentration, allowing comparative evaluation against conventional thin film deposition methods. Doped oxides and ternary oxides, particularly ZnO‐based systems with Al, Ga, or transition‐metal dopants, are highlighted as another important class, combining high‐temperature stability with tunable electronic transport, albeit with lower power factors than chalcogenides. Recent advances in molecular layer deposition have allowed the implementation of ALD/MLD multilayers and superlattices, showing how interface engineering and nanoscale modulation of potential barriers can influence carrier scattering and phonon transport. In parallel, we review precursor chemistry, deposition temperature windows, and process limitations, including environmental and safety considerations, to provide practical guidance for reproducibility and scalability. A comparative analysis with results from other deposition methods underlines that while ALD does not intrinsically outperform other deposition techniques, it offers complementary advantages in conformality and sub‐nanometer composition control, making it a powerful option for complex device architectures. Altogether, the review situates ALD‐grown thin films within the broader thermoelectric landscape, highlighting both their potential and the critical bottlenecks that remain.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"9 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145731995","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}
Shengxiang Kang, Jiyao Zhang, Haojie Liang, Jiaming Huang, Zhiwei Ren, Teng He, Xiaohui Liu, Jing Zhang, Yuejin Zhu, Kuan Liu, Gang Li, Like Huang
Perovskite solar cells (PSCs) face challenges in long‐term stability, especially under reverse bias. Here, a water‐soluble vanadium pentoxide (V 2 O 5‐x ) hole‐collecting layer (HCL) is introduced into inverted PSCs to improve the photovoltaic performance and multiple‐scenario stability under operational, thermal recycle, and reverse bias. V 2 O 5‐x annealed at 50–250°C are characterized for multiple physical properties, revealing that 150°C annealing optimizes oxygen vacancy to reduce trap density and improve interface carrier collection. The champion device based on (FA 0.83 MA 0.17 ) 0.95 Cs 0.05 Pb(I 0.95 Br 0.05 ) 3 absorber achieves power conversion efficiency (PCE) of 23.3% with negligible hysteresis (HI = 0.64%) and good stability (retains ∼88% of initial PCE after 1000 h of storage). Further, with Cs 0.05 MA 0.1 FA 0.85 PbI 3 as absorber, the PCE of the device can be further improved to be 25.88% with an HI of 3.26%, superior to the device without V 2 O 5‐x (PCE = 24.94%, HI = 5.47%). Moreover, the operational and thermal cycling stability of the device has been obviously improved. Crucially, V 2 O 5‐x enhances the reverse breakdown voltage from about |−2| to |−6| V, endowing the device with higher reverse bias stability and tolerance to the shadow effect. These results demonstrate that V 2 O 5‐x can simultaneously boost PCE and stability of PSCs, offering a promising route toward efficient and durable PSCs.
钙钛矿太阳能电池（PSCs）在长期稳定性方面面临挑战，特别是在反向偏压下。本研究将水溶性五氧化二钒（v2o - 5 - x）空穴收集层（HCL）引入到倒置PSCs中，以提高光伏性能和在操作、热循环和反向偏压下的多场景稳定性。在50-250°C退火的V 2o - 5‐x具有多种物理性质，表明150°C退火优化了氧空位，降低了陷阱密度，改善了界面载流子收集。基于（FA 0.83 MA 0.17） 0.95 Cs 0.05 Pb(I 0.95 Br 0.05) 3吸收体的champion器件实现了23.3%的功率转换效率（PCE），迟滞可以忽略不计（HI = 0.64%），稳定性良好（存储1000 h后保持初始PCE的~ 88%）。此外，以c0.05 MA 0.1 FA 0.85 pbi3为吸收剂时，器件的PCE为25.88%，HI为3.26%，优于无v2o - x的器件（PCE = 24.94%, HI = 5.47%）。同时，器件的工作稳定性和热循环稳定性也得到了明显的提高。至关重要的是，v2o5‐x将反向击穿电压从约|−2|提高到|−6| V，使器件具有更高的反向偏置稳定性和对阴影效应的容错性。这些结果表明，v2o5‐x可以同时提高PCE和PSCs的稳定性，为制备高效耐用的PSCs提供了一条有希望的途径。
{"title":"Water‐Soluble V 2 O 5‐x Enables Efficient Inverted Perovskite Solar Cells With High Operational and Reverse Bias Stability","authors":"Shengxiang Kang, Jiyao Zhang, Haojie Liang, Jiaming Huang, Zhiwei Ren, Teng He, Xiaohui Liu, Jing Zhang, Yuejin Zhu, Kuan Liu, Gang Li, Like Huang","doi":"10.1002/aenm.202506005","DOIUrl":"https://doi.org/10.1002/aenm.202506005","url":null,"abstract":"Perovskite solar cells (PSCs) face challenges in long‐term stability, especially under reverse bias. Here, a water‐soluble vanadium pentoxide (V <jats:sub>2</jats:sub> O <jats:sub>5‐x</jats:sub> ) hole‐collecting layer (HCL) is introduced into inverted PSCs to improve the photovoltaic performance and multiple‐scenario stability under operational, thermal recycle, and reverse bias. V <jats:sub>2</jats:sub> O <jats:sub>5‐x</jats:sub> annealed at 50–250°C are characterized for multiple physical properties, revealing that 150°C annealing optimizes oxygen vacancy to reduce trap density and improve interface carrier collection. The champion device based on (FA <jats:sub>0.83</jats:sub> MA <jats:sub>0.17</jats:sub> ) <jats:sub>0.95</jats:sub> Cs <jats:sub>0.05</jats:sub> Pb(I <jats:sub>0.95</jats:sub> Br <jats:sub>0.05</jats:sub> ) <jats:sub>3</jats:sub> absorber achieves power conversion efficiency (PCE) of 23.3% with negligible hysteresis (HI = 0.64%) and good stability (retains ∼88% of initial PCE after 1000 h of storage). Further, with Cs <jats:sub>0.05</jats:sub> MA <jats:sub>0.1</jats:sub> FA <jats:sub>0.85</jats:sub> PbI <jats:sub>3</jats:sub> as absorber, the PCE of the device can be further improved to be 25.88% with an HI of 3.26%, superior to the device without V <jats:sub>2</jats:sub> O <jats:sub>5‐x</jats:sub> (PCE = 24.94%, HI = 5.47%). Moreover, the operational and thermal cycling stability of the device has been obviously improved. Crucially, V <jats:sub>2</jats:sub> O <jats:sub>5‐x</jats:sub> enhances the reverse breakdown voltage from about |−2| to |−6| V, endowing the device with higher reverse bias stability and tolerance to the shadow effect. These results demonstrate that V <jats:sub>2</jats:sub> O <jats:sub>5‐x</jats:sub> can simultaneously boost PCE and stability of PSCs, offering a promising route toward efficient and durable PSCs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"13 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145731992","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}
With the increasing dependence of national development on power grids, a self‐powered grid security system is urgently needed for the long‐term safe operation of transmission lines. To provide sustainable power for the system, a rolling‐magnet‐based energy harvester (RMEH) is proposed by utilizing the mechanical energy in a rolling magnet, as triggered by the alternating‐current magnetic field from the transmission line. Due to the compact structural design and rapid magnetic‐field variation from the rolling motion, RMEH achieves an average power density of up to 128.5 W/m 3 and 0.14 W/kg in volume and mass, respectively, which stands far ahead of other reported studies so far. Furthermore, the trajectory of the magnet rolling is numerically calculated by kinetic equations, confirming a high degree of consistency between experimental and simulation results. Based on the theoretical analysis and experimental results, the effects of current amplitude and magnetic sheet thickness on the output performance are investigated. Moreover, RMEH can create a self‐powered smart grid security system with multiple functions including bird repelling, aviation obstacle indication, and wireless monitoring, demonstrating a broad prospect on the future grid security systems for transmission lines.
{"title":"High‐Power‐Density Rolling‐Magnet Based Energy Harvesting from Transmission Lines","authors":"Jinhong Dai, Shaoshuai He, Yiru Wang, Xin Xia, Zuoqing Luo, Chuanyang Li, Yanpeng Hao, Yunlong Zi","doi":"10.1002/aenm.202504837","DOIUrl":"https://doi.org/10.1002/aenm.202504837","url":null,"abstract":"With the increasing dependence of national development on power grids, a self‐powered grid security system is urgently needed for the long‐term safe operation of transmission lines. To provide sustainable power for the system, a rolling‐magnet‐based energy harvester (RMEH) is proposed by utilizing the mechanical energy in a rolling magnet, as triggered by the alternating‐current magnetic field from the transmission line. Due to the compact structural design and rapid magnetic‐field variation from the rolling motion, RMEH achieves an average power density of up to 128.5 W/m <jats:sup>3</jats:sup> and 0.14 W/kg in volume and mass, respectively, which stands far ahead of other reported studies so far. Furthermore, the trajectory of the magnet rolling is numerically calculated by kinetic equations, confirming a high degree of consistency between experimental and simulation results. Based on the theoretical analysis and experimental results, the effects of current amplitude and magnetic sheet thickness on the output performance are investigated. Moreover, RMEH can create a self‐powered smart grid security system with multiple functions including bird repelling, aviation obstacle indication, and wireless monitoring, demonstrating a broad prospect on the future grid security systems for transmission lines.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"12 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145731994","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}
Thick electrodes are essential for achieving high‐energy‐density lithium‐ion batteries, yet their performance is often constrained by transport limitations. A central factor is the carbon‐binder domain (CBD), which plays a dual role in electrode. It provides electronic pathways but simultaneously impedes ionic transport. The coexistence of pores between active materials and nanoscale pores within the CBD has previously been recognized, but their individual contributions have not been quantitatively resolved. Here, we introduce the Dual‐Pore Transmission Line Model (DTLM), which separates ionic transport into two parallel pathways through interparticle and CBD pores. DTLM provides a physically grounded and domain‐resolved interpretation of porosity–tortuosity behavior, offering additional insight beyond what can be obtained from conventional Bruggeman relations or transmission line models. Guided by this framework, we design an optimized electrode formulation with 2 wt.% carbon black (CB), moderate milling, and a reduced binder‐to‐CB ratio. This formulation maintains CBD pore accessibility, reduces both electronic and ionic resistance, and substantially improves rate capability in high‐loading (10.0 mAh cm −2 ) and low‐porosity (20%) electrodes. Beyond this demonstration, DTLM offers a transferable framework for microstructure‐guided design of next‐generation thick electrodes and delivers quantitative insight into how electronic and ionic transport are balanced within multiscale pore networks.
厚电极对于实现高能量密度锂离子电池至关重要，但其性能往往受到传输限制的制约。一个中心因素是碳结合剂结构域（CBD），它在电极中起双重作用。它提供了电子途径，但同时阻碍了离子传递。生物多样性公约中活性物质和纳米级孔隙的共存已经被认识到，但它们各自的贡献尚未得到定量解决。在这里，我们引入了双孔传输线模型（DTLM），该模型将离子传输分为两个平行的途径，分别通过颗粒间孔和CBD孔。DTLM为孔隙度-弯曲度行为提供了物理基础和域解析解释，提供了传统Bruggeman关系或传输线模型所无法获得的额外见解。在此框架的指导下，我们设计了一种优化的电极配方，其中含有2 wt.%的炭黑（CB），适度的铣削，以及降低粘合剂与CB的比例。该配方保持了CBD孔隙的可达性，降低了电子和离子阻力，并大大提高了高负载（10.0 mAh cm - 2）和低孔隙率（20%）电极的速率能力。除了这个演示之外，DTLM为下一代厚电极的微结构指导设计提供了一个可转移的框架，并提供了对多尺度孔隙网络中电子和离子传输如何平衡的定量见解。
{"title":"Thick Electrode Design Enabled by a Carbon–Binder Domain–Resolved Dual‐Pore Transmission Line Model for Lithium‐Ion Batteries","authors":"Byeong‐Jin Jeon, Hyeon Jeong, Suhui Yoon, Seungho Park, Junehyun Im, Kyeong‐Min Jeong","doi":"10.1002/aenm.202505334","DOIUrl":"https://doi.org/10.1002/aenm.202505334","url":null,"abstract":"Thick electrodes are essential for achieving high‐energy‐density lithium‐ion batteries, yet their performance is often constrained by transport limitations. A central factor is the carbon‐binder domain (CBD), which plays a dual role in electrode. It provides electronic pathways but simultaneously impedes ionic transport. The coexistence of pores between active materials and nanoscale pores within the CBD has previously been recognized, but their individual contributions have not been quantitatively resolved. Here, we introduce the Dual‐Pore Transmission Line Model (DTLM), which separates ionic transport into two parallel pathways through interparticle and CBD pores. DTLM provides a physically grounded and domain‐resolved interpretation of porosity–tortuosity behavior, offering additional insight beyond what can be obtained from conventional Bruggeman relations or transmission line models. Guided by this framework, we design an optimized electrode formulation with 2 wt.% carbon black (CB), moderate milling, and a reduced binder‐to‐CB ratio. This formulation maintains CBD pore accessibility, reduces both electronic and ionic resistance, and substantially improves rate capability in high‐loading (10.0 mAh cm <jats:sup>−2</jats:sup> ) and low‐porosity (20%) electrodes. Beyond this demonstration, DTLM offers a transferable framework for microstructure‐guided design of next‐generation thick electrodes and delivers quantitative insight into how electronic and ionic transport are balanced within multiscale pore networks.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"1 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732015","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}
Layered oxide cathodes with activated anionic redox reaction (ARR) have been considered as promising candidates for high‐energy‐density sodium‐ion batteries (SIBs) due to their high reversible capacity. Unfortunately, they suffer from irreversible oxygen release, successive electrolyte decomposition, severe transition metal dissolution, and crystal structure degradation, resulting in unsatisfactory sodium storage performance. Herein, the highly reversible ARR in Na 0.67 Li 0.24 Mn 0.66 Zn 0.05 Ti 0.05 O 2 (NLMZTO) is realized through the incorporation of multifunctional electrolyte additive (ethoxy (pentafluoro) cyclotriphosphazene, PFPN) into a traditional ester‐based electrolyte. The PFPN additive regulates the anion‐reinforced solvation structure, promotes the formation of a robust N/P‐rich cathode‐electrolyte interphase, and scavenges highly reactive oxygen species, which facilitates the formation of robust interfacial chemistry, suppresses continuous side reactions, and accelerates the desolvation kinetics. These combined effects effectively solve the key challenge for layered oxide cathodes with activated ARR. Consequently, the capacity retention of NLMZTO is significantly increased from 25.0% to 81.6% after 600 cycles at a high cut‐off voltage of 4.5 V. More importantly, the hard carbon||NLMZTO full cell delivers a high energy density of 472.6 Wh kg −1 and superior cycling performance, demonstrating the feasibility of PFPN in SIBs. This work provides valuable guidance in interfacial chemistry engineering employing multifunctional electrolyte additives for highly reversible ARR in layered oxide cathodes for high‐energy‐density SIBs.
具有活化阴离子氧化还原反应（ARR）的层状氧化物阴极由于其高可逆容量而被认为是高能量密度钠离子电池（sib）的有希望的候选者。不幸的是，它们遭受不可逆的氧释放，连续的电解质分解，严重的过渡金属溶解和晶体结构退化，导致不理想的钠存储性能。本文通过在传统的酯基电解质中加入多功能电解质添加剂乙氧基（五氟）环三磷腈（PFPN），实现了Na 0.67 Li 0.24 Mn 0.66 Zn 0.05 Ti 0.05 o2 （NLMZTO）中的高可逆ARR。PFPN添加剂调节了阴离子增强的溶剂化结构，促进了强大的富N/P阴极电解质界面相的形成，并清除了高活性的氧，从而促进了强大的界面化学的形成，抑制了连续的副反应，加速了脱溶动力学。这些综合效应有效地解决了具有活化ARR的层状氧化物阴极的关键挑战。因此，在4.5 V的高截止电压下，经过600次循环后，NLMZTO的容量保持率从25.0%显著提高到81.6%。更重要的是，硬碳||NLMZTO全电池具有472.6 Wh kg−1的高能量密度和优异的循环性能，证明了PFPN在sib中的可行性。这项工作为界面化学工程提供了有价值的指导，使用多功能电解质添加剂在高能量密度sib层状氧化物阴极中进行高可逆的ARR。
{"title":"Solvation Chemistry‐Driven Interfacial Engineering Enables Reversible Anionic Redox in Sodium‐Layered Oxide Cathodes","authors":"Yiran Sun, Xunzhu Zhou, Junying Weng, Honghe Yu, Xiaozhong Wu, Zhen Zhou, Jin Zhou, Jiazhao Wang, Lin Li, Shixue Dou, Pengfei Zhou","doi":"10.1002/aenm.202504397","DOIUrl":"https://doi.org/10.1002/aenm.202504397","url":null,"abstract":"Layered oxide cathodes with activated anionic redox reaction (ARR) have been considered as promising candidates for high‐energy‐density sodium‐ion batteries (SIBs) due to their high reversible capacity. Unfortunately, they suffer from irreversible oxygen release, successive electrolyte decomposition, severe transition metal dissolution, and crystal structure degradation, resulting in unsatisfactory sodium storage performance. Herein, the highly reversible ARR in Na <jats:sub>0.67</jats:sub> Li <jats:sub>0.24</jats:sub> Mn <jats:sub>0.66</jats:sub> Zn <jats:sub>0.05</jats:sub> Ti <jats:sub>0.05</jats:sub> O <jats:sub>2</jats:sub> (NLMZTO) is realized through the incorporation of multifunctional electrolyte additive (ethoxy (pentafluoro) cyclotriphosphazene, PFPN) into a traditional ester‐based electrolyte. The PFPN additive regulates the anion‐reinforced solvation structure, promotes the formation of a robust N/P‐rich cathode‐electrolyte interphase, and scavenges highly reactive oxygen species, which facilitates the formation of robust interfacial chemistry, suppresses continuous side reactions, and accelerates the desolvation kinetics. These combined effects effectively solve the key challenge for layered oxide cathodes with activated ARR. Consequently, the capacity retention of NLMZTO is significantly increased from 25.0% to 81.6% after 600 cycles at a high cut‐off voltage of 4.5 V. More importantly, the hard carbon||NLMZTO full cell delivers a high energy density of 472.6 Wh kg <jats:sup>−1</jats:sup> and superior cycling performance, demonstrating the feasibility of PFPN in SIBs. This work provides valuable guidance in interfacial chemistry engineering employing multifunctional electrolyte additives for highly reversible ARR in layered oxide cathodes for high‐energy‐density SIBs.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"149 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732016","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}
Jeong‐Myeong Yoon, Pugalenthiyar Thondaiman, Je‐Hyeon Han, Young‐Han Lee, Do‐Hyeon Kim, Cheol‐Min Park
Lithium all‐solid‐state batteries (LASSBs) with sulfide‐type solid electrolytes (SEs) offer enhanced safety and higher energy densities compared to conventional Li‐ion batteries. However, Li‐metal anodes are incompatible with sulfide‐type SEs and prone to dendrite formation, which severely limits their practical applicability. Although various strategies, including the use of Li‐free, carbon‐based, alloy‐based, or oxide‐based anodes, as well as interfacial protection layers, have been explored, they typically deliver poor rate performance and suffer from dendrite growth. Herein, we introduce a Li–Ga compound anode, specifically the LiGa phase, predicted through density functional theory simulations, which exhibits dendrite‐free behavior, high ionic/electronic conductivities, stable operation at low stack pressures, room temperature stability, and excellent interfacial compatibility with SEs. Benefiting from these properties, a full cell comprising a LiGa anode and the LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cathode (LiGa|NCM622) delivers a high areal capacity of 14.47 mAh cm −2 at a high cathode loading of 100 mg cm −2 , along with fast rate capability and stable cycling at a low stack pressure of 3 MPa at room temperature. Furthermore, a LiGa|NCM622 pouch cell demonstrates outstanding electrochemical performance, highlighting the potential of LiGa as a high‐performance anode for next‐generation LASSBs, with the concept broadly applicable to diverse Li‐based compounds.
与传统锂离子电池相比，采用硫化物型固体电解质的全固态锂电池（lassb）具有更高的安全性和能量密度。然而，锂金属阳极与硫化物型se不相容，容易形成枝晶，这严重限制了它们的实际应用。尽管已经探索了各种策略，包括使用无锂、碳基、合金基或氧化物基阳极以及界面保护层，但它们通常具有较差的速率性能，并且受到枝晶生长的影响。本文介绍了一种Li-Ga复合阳极，特别是通过密度泛函理论模拟预测的LiGa相，它具有无枝晶行为、高离子/电子电导率、低堆叠压力下稳定运行、室温稳定性以及与SEs的良好界面相容性。得益于这些特性，由LiGa阳极和LiNi 0.6 Co 0.2 Mn 0.2 O 2 （NCM622）阴极（LiGa|NCM622）组成的全电池在阴极负载为100 mg cm - 2时具有14.47 mAh cm - 2的高面容量，以及在室温下3 MPa的低堆叠压力下的快速速率能力和稳定循环。此外，LiGa|NCM622袋状电池表现出出色的电化学性能，突出了LiGa作为下一代lassb高性能阳极的潜力，其概念广泛适用于各种锂基化合物。
{"title":"Highly Conductive and Dendrite‐Free Li–Ga Compound Anodes for High‐Performance Lithium All‐Solid‐State Batteries","authors":"Jeong‐Myeong Yoon, Pugalenthiyar Thondaiman, Je‐Hyeon Han, Young‐Han Lee, Do‐Hyeon Kim, Cheol‐Min Park","doi":"10.1002/aenm.202505248","DOIUrl":"https://doi.org/10.1002/aenm.202505248","url":null,"abstract":"Lithium all‐solid‐state batteries (LASSBs) with sulfide‐type solid electrolytes (SEs) offer enhanced safety and higher energy densities compared to conventional Li‐ion batteries. However, Li‐metal anodes are incompatible with sulfide‐type SEs and prone to dendrite formation, which severely limits their practical applicability. Although various strategies, including the use of Li‐free, carbon‐based, alloy‐based, or oxide‐based anodes, as well as interfacial protection layers, have been explored, they typically deliver poor rate performance and suffer from dendrite growth. Herein, we introduce a Li–Ga compound anode, specifically the LiGa phase, predicted through density functional theory simulations, which exhibits dendrite‐free behavior, high ionic/electronic conductivities, stable operation at low stack pressures, room temperature stability, and excellent interfacial compatibility with SEs. Benefiting from these properties, a full cell comprising a LiGa anode and the LiNi <jats:sub>0.6</jats:sub> Co <jats:sub>0.2</jats:sub> Mn <jats:sub>0.2</jats:sub> O <jats:sub>2</jats:sub> (NCM622) cathode (LiGa|NCM622) delivers a high areal capacity of 14.47 mAh cm <jats:sup>−2</jats:sup> at a high cathode loading of 100 mg cm <jats:sup>−2</jats:sup> , along with fast rate capability and stable cycling at a low stack pressure of 3 MPa at room temperature. Furthermore, a LiGa|NCM622 pouch cell demonstrates outstanding electrochemical performance, highlighting the potential of LiGa as a high‐performance anode for next‐generation LASSBs, with the concept broadly applicable to diverse Li‐based compounds.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"10 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732017","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}
Herao Wang, Zicheng Luo, Yangyang Cheng, Menghong Li, Yulong He, Yuxuan Gao, Zhiguo Du, Shubin Yang, Bin Li
Long‐term electrochemical energy storage devices of lithium battery demand electrolytes that simultaneously ensure operational functionality and suppress self‐discharge during idle periods. In this work, a binary phase‐change electrolyte (B‐PCE) integrating dimethyl dodecanedioate (DDCA) and fluoroethylene carbonate (FEC) is proposed. The B‐PCE exhibits temperature‐adaptive functionality through an 18.65°C phase transition, prolonging storage properties and enhancing operational performance. The B‐PCE achieves unprecedented over 2000‐fold ionic conductivity modulation, maintaining 0.23 mS cm −1 at 25°C for efficient operation, while collapsing to 8.8 × 10 −5 mS cm −1 at 0°C to block parasitic reactions. This drastic change is accompanied by a transformation in solvation structures from solvent‐separated ion pairs to contact ion pairs and aggregates, which significantly elevates charge transfer resistance. Furthermore, it has been confirmed that the FEC‐derived LiF‐rich SEI formation on lithium metal anodes is effective in suppressing interfacial side reactions. In lithium metal batteries (LiFePO 4 ‖Li) full cells, B‐PCE delivers an ultralow daily self‐discharge rate of 0.02% after stabilization at 0°C with a projected 5.9‐year long‐shelf‐life, surpassing conventional electrolytes by 11.3‐fold. Concurrently, it exhibits exceptional cycling stability with lithium metal anodes, maintaining 82% capacity retention after 200 cycles at 1 C and high‐rate capability of 117.5 mAh g −1 at 5 C.
锂电池的长期电化学储能装置需要同时保证运行功能和抑制闲置期间的自放电的电解质。在这项工作中，提出了一种整合二甲基十二烷二酸酯（DDCA）和氟碳酸乙烯（FEC）的二元相变电解质（B - PCE）。B - PCE通过18.65°C的相变表现出温度自适应功能，延长了存储性能并提高了操作性能。B - PCE实现了前所未有的超过2000倍的离子电导率调制，在25°C时保持0.23 mS cm - 1以有效运行，而在0°C时坍塌到8.8 × 10 - 5 mS cm - 1以阻止寄生反应。这种剧烈的变化伴随着溶剂化结构的转变，从溶剂分离的离子对到接触离子对和聚集体，这显著提高了电荷转移阻力。此外，还证实了FEC衍生的富liff SEI在锂金属阳极上的形成对抑制界面副反应是有效的。在锂金属电池（lifepo4‖Li）全电池中，B‐PCE在0°C稳定后提供了0.02%的超低日自放电率，预计保质期为5.9年，超过传统电解质11.3倍。同时，它具有优异的锂金属阳极循环稳定性，在1℃下循环200次后保持82%的容量保持，在5℃下保持117.5 mAh g - 1的高倍率容量。
{"title":"Prolonging Storage Shelf‐Life of Lithium Metal Batteries with Phase‐Change Electrolyte","authors":"Herao Wang, Zicheng Luo, Yangyang Cheng, Menghong Li, Yulong He, Yuxuan Gao, Zhiguo Du, Shubin Yang, Bin Li","doi":"10.1002/aenm.202505116","DOIUrl":"https://doi.org/10.1002/aenm.202505116","url":null,"abstract":"Long‐term electrochemical energy storage devices of lithium battery demand electrolytes that simultaneously ensure operational functionality and suppress self‐discharge during idle periods. In this work, a binary phase‐change electrolyte (B‐PCE) integrating dimethyl dodecanedioate (DDCA) and fluoroethylene carbonate (FEC) is proposed. The B‐PCE exhibits temperature‐adaptive functionality through an 18.65°C phase transition, prolonging storage properties and enhancing operational performance. The B‐PCE achieves unprecedented over 2000‐fold ionic conductivity modulation, maintaining 0.23 mS cm <jats:sup>−1</jats:sup> at 25°C for efficient operation, while collapsing to 8.8 × 10 <jats:sup>−5</jats:sup> mS cm <jats:sup>−1</jats:sup> at 0°C to block parasitic reactions. This drastic change is accompanied by a transformation in solvation structures from solvent‐separated ion pairs to contact ion pairs and aggregates, which significantly elevates charge transfer resistance. Furthermore, it has been confirmed that the FEC‐derived LiF‐rich SEI formation on lithium metal anodes is effective in suppressing interfacial side reactions. In lithium metal batteries (LiFePO <jats:sub>4</jats:sub> ‖Li) full cells, B‐PCE delivers an ultralow daily self‐discharge rate of 0.02% after stabilization at 0°C with a projected 5.9‐year long‐shelf‐life, surpassing conventional electrolytes by 11.3‐fold. Concurrently, it exhibits exceptional cycling stability with lithium metal anodes, maintaining 82% capacity retention after 200 cycles at 1 C and high‐rate capability of 117.5 mAh g <jats:sup>−1</jats:sup> at 5 C.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"39 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145731991","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}
Yu Su, Kongxiang Wang, Xiang Guan, Yumao Wu, Hong Zhang, Fengxian Xie, Junhao Chu
In recent years, machine learning (ML) has emerged as a versatile tool for accelerating the development of perovskite solar cells (PSCs). A key challenge, however, lies in the scarcity of researchers possessing deep expertise in both material science and artificial intelligence. Pivotal to bridging this gap is ML descriptors, mediating between the empirical language of materials and the numerical inputs for ML algorithms. By translating domain knowledge into computationally tractable forms, the descriptors significantly enhance the model interpretability and empower researchers to uncover the underlying physical mechanisms governing behavior of PSCs. Therefore, it is crucial to overview the efforts translating the structure, property of perovskite materials and performance of PSCs into numerical descriptors compatible with ML models. This review summarized (1) the encoding of crystal structure in perovskites; (2) the quantification of microstructures in perovskite films; (3) the stability assessment of perovskite materials and devices. By synthesizing progress in these aspects, this work lays a solid foundation for constructing a universal model to elucidate the structure‐property‐performance relationships in PSCs, especially in forward prediction and backward inference.
{"title":"Machine Learning Descriptors for Mapping Structure‐Property‐Performance Relationships of Perovskite Solar Cells","authors":"Yu Su, Kongxiang Wang, Xiang Guan, Yumao Wu, Hong Zhang, Fengxian Xie, Junhao Chu","doi":"10.1002/aenm.202505294","DOIUrl":"https://doi.org/10.1002/aenm.202505294","url":null,"abstract":"In recent years, machine learning (ML) has emerged as a versatile tool for accelerating the development of perovskite solar cells (PSCs). A key challenge, however, lies in the scarcity of researchers possessing deep expertise in both material science and artificial intelligence. Pivotal to bridging this gap is ML descriptors, mediating between the empirical language of materials and the numerical inputs for ML algorithms. By translating domain knowledge into computationally tractable forms, the descriptors significantly enhance the model interpretability and empower researchers to uncover the underlying physical mechanisms governing behavior of PSCs. Therefore, it is crucial to overview the efforts translating the structure, property of perovskite materials and performance of PSCs into numerical descriptors compatible with ML models. This review summarized (1) the encoding of crystal structure in perovskites; (2) the quantification of microstructures in perovskite films; (3) the stability assessment of perovskite materials and devices. By synthesizing progress in these aspects, this work lays a solid foundation for constructing a universal model to elucidate the structure‐property‐performance relationships in PSCs, especially in forward prediction and backward inference.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"66 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145732018","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}
Solid‐state lithium metal batteries (SS‐LMBs) are restrained currently by their ionic conductivity, interface stability, and lithium dendrite penetration. Here, a high‐voltage SS‐LMB is enabled by a tailored functional composite electrolyte, which achieves a synergistic enhancement effect of “free radical scavenging–ion transport regulating–interface stabilizing.” This electrolyte obtained by embedding fluoro (F) and phenol (Ar─OH) dual‐hybrid ZIF‐8 into a PVDF‐HFP matrix exhibits a high room temperature ionic conductivity of 6.7 × 10 −4 S cm −1 (E a = 0.19 eV) and an electrochemical stability window above 5 V. The Ar─OH groups can effectively scavenge superoxide radicals (O 2− ·) to suppress side reactions in NCM811‐based batteries. Active sites from triazole‐Zn coordination can specifically adsorb TFSI − (adsorption energy −2.45 eV) to enhance the Li + transference number (0.68). The F groups can preferentially decompose to form an inorganic F/N‐enriched solid electrolyte interface (SEI) layer with 65.8% LiF and 68.5% Li 3 N content. The assembled NCM811‐based SS‐LMB achieved an initial capacity of 177 mAh g −1 under 4.6 V high voltage, with a capacity retention of 76% after 300 cycles (1C). These results jointly reveal that this synergistic effect Fluoro and Phenol Dual‐hybrid MOF, High‐Voltage, Solid Electrolyte, Triple Enhancement Effect of functional groups is a promising strategy for the development of high‐performance batteries.
固态锂金属电池（SS - lmb）目前受到离子电导率、界面稳定性和锂枝晶穿透性的限制。在这里，高电压SS - LMB是由定制的功能性复合电解质实现的，它实现了“自由基清除-离子传输调节-界面稳定”的协同增强效应。通过将氟(F)和苯酚（Ar─OH）双杂化ZIF‐8包埋在PVDF‐HFP基质中得到的电解质，其室温离子电导率高达6.7 × 10−4 S cm−1 (ea = 0.19 eV)，电化学稳定窗口高于5 V。Ar─OH基团能有效清除超氧自由基（o2−·），抑制NCM811电池的副反应。三唑-锌配位的活性位点可以特异性吸附TFSI -（吸附能- 2.45 eV），提高Li +转移数（0.68）。F基团可以优先分解形成无机富F/N固体电解质界面（SEI）层，其LiF含量为65.8%，li3n含量为68.5%。组装的基于NCM811的SS - LMB在4.6 V高压下获得了177 mAh g - 1的初始容量，在300次循环后容量保持率为76% （1C）。这些结果共同揭示了氟和酚双杂化MOF、高压、固体电解质、官能团三重增强效应的协同效应是一种很有前途的高性能电池发展策略。
{"title":"Triple Enhancement Effect of Fluoro and Phenol Dual‐Hybrid MOF in High‐Voltage Solid‐State Lithium Metal Batteries","authors":"Yixian Xiao, Jiaxing Zhang, Yinuo Yu, Jiajun Chen, Xinzhao Xia, Zhifeng Gan, Xiaoli Cao, Wei Hu, Huai Yang","doi":"10.1002/aenm.202505438","DOIUrl":"https://doi.org/10.1002/aenm.202505438","url":null,"abstract":"Solid‐state lithium metal batteries (SS‐LMBs) are restrained currently by their ionic conductivity, interface stability, and lithium dendrite penetration. Here, a high‐voltage SS‐LMB is enabled by a tailored functional composite electrolyte, which achieves a synergistic enhancement effect of “free radical scavenging–ion transport regulating–interface stabilizing.” This electrolyte obtained by embedding fluoro (F) and phenol (Ar─OH) dual‐hybrid ZIF‐8 into a PVDF‐HFP matrix exhibits a high room temperature ionic conductivity of 6.7 × 10 <jats:sup>−4</jats:sup> S cm <jats:sup>−1</jats:sup> (E <jats:sub>a</jats:sub> = 0.19 eV) and an electrochemical stability window above 5 V. The Ar─OH groups can effectively scavenge superoxide radicals (O <jats:sub>2</jats:sub> <jats:sup>−</jats:sup> ·) to suppress side reactions in NCM811‐based batteries. Active sites from triazole‐Zn coordination can specifically adsorb TFSI <jats:sup>−</jats:sup> (adsorption energy −2.45 eV) to enhance the Li <jats:sup>+</jats:sup> transference number (0.68). The F groups can preferentially decompose to form an inorganic F/N‐enriched solid electrolyte interface (SEI) layer with 65.8% LiF and 68.5% Li <jats:sub>3</jats:sub> N content. The assembled NCM811‐based SS‐LMB achieved an initial capacity of 177 mAh g <jats:sup>−1</jats:sup> under 4.6 V high voltage, with a capacity retention of 76% after 300 cycles (1C). These results jointly reveal that this synergistic effect Fluoro and Phenol Dual‐hybrid MOF, High‐Voltage, Solid Electrolyte, Triple Enhancement Effect of functional groups is a promising strategy for the development of high‐performance batteries.","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":"19 1","pages":""},"PeriodicalIF":27.8,"publicationDate":"2025-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145717398","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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