ACS Energy Letters 最新文献

Reconfiguring Polymer Chain for Regulating Na+ Solvation Structure in a Gel Polymer Electrolyte toward Sodium Metal Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-28 DOI: 10.1021/acsenergylett.5c00331

Yan Yuan, Huan Liu, Lei Zhang, Zhao Fang, Jiaxin Luo, Yaxin Kong, Long Kong, Hai Lu

{"title":"Reconfiguring Polymer Chain for Regulating Na+ Solvation Structure in a Gel Polymer Electrolyte toward Sodium Metal Batteries","authors":"Yan Yuan, Huan Liu, Lei Zhang, Zhao Fang, Jiaxin Luo, Yaxin Kong, Long Kong, Hai Lu","doi":"10.1021/acsenergylett.5c00331","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00331","url":null,"abstract":"Gel polymer electrolytes (GPEs) instead of liquid electrolytes can greatly improve the lifespan and safety of sodium metal batteries (SMBs). However, inferior interface stability against Na metal and sluggish reaction kinetics restrict their practical use. Herein, a cross-linked GPE (c-GPE) is proposed by in situ copolymerization of ethoxylated trimethylolpropane triacrylate (ETT) and trifluoroethyl methacrylate (TM) in a liquid electrolyte. The uniquely fabricated c-GPE exhibits impressive ionic conductivity, a wide electrochemical window, low flammability, and favorable Na metal compatibility. Particularly, the functional copolymer chain regulates the Na+ solvation structure with lower desolvation energy by a strong cation-dipole (in polymer) interaction. Consequently, full cells based on the Na3V2(PO4)3 (NVP) cathode (NVP|c-GPE|Na) display an ultralong cycle life (>3000 cycles), remarkable rate capability (up to 15C), and wide temperature adaptability. The work offers new insight into constructing a Na+ coordination environment, achieving more facile desolvation by the polymer chain design of the GPE used for developing advanced SMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"66 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143724012","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Constriction and Contact Impedance of Ceramic Solid Electrolytes

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-28 DOI: 10.1021/acsenergylett.5c00032

Md Salman Rabbi Limon, Curtis Wesley Duffee, Zeeshan Ahmad

{"title":"Constriction and Contact Impedance of Ceramic Solid Electrolytes","authors":"Md Salman Rabbi Limon, Curtis Wesley Duffee, Zeeshan Ahmad","doi":"10.1021/acsenergylett.5c00032","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00032","url":null,"abstract":"The development of solid-state batteries (SSBs) is hindered by degradation at solid–solid interfaces due to void formation and contact loss, resulting in increased impedance. We systematically investigate the roles of real and unrecoverable interfacial contact areas at the electrode/Li6PS5Cl interface in driving the impedance rise. By controlling contact geometries and applied pressures, we identify their distinct contributions to the impedance and quantify their influence on the interfacial resistance and transport. Experiments reveal that interfacial resistance follows power law scaling, with exponents of −1 for recoverable contact area and −0.5 to −0.67 for pressure, respectively. Moreover, distributed contacts result in lower impedance due to smaller potential gradients and a more uniform electrical potential distribution. Simulations of the geometries with unrecoverable contact loss predict interfacial resistances in agreement with experiments. Our work highlights the influence of unrecoverable and recoverable contact losses on SSB impedance while quantifying the effectiveness of mitigation strategies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"41 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723838","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Structural Feature Design for Carbon Materials toward Sodium Storage: Insights and Prospects

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-27 DOI: 10.1021/acsenergylett.5c00231

Shaorui Chen, Tianzhao Hu, Tong Yu, Xianyou Luo, Lei Zhang, Feng Li

{"title":"Structural Feature Design for Carbon Materials toward Sodium Storage: Insights and Prospects","authors":"Shaorui Chen, Tianzhao Hu, Tong Yu, Xianyou Luo, Lei Zhang, Feng Li","doi":"10.1021/acsenergylett.5c00231","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00231","url":null,"abstract":"Sodium-ion batteries are an attractive alternative to lithium-ion batteries due to the abundance and cost-effectiveness and are suitable for large-scale energy storage. Carbon materials, notable for their availability, economic viability, high capacity, and stability, stand out as potential anode materials. The sodium storage performance of carbon materials is inherently determined by their structural features. Manipulating these features is key to optimizing the storage behavior. This Perspective systematically evaluates the classification and structural distinctions of existing carbon-based materials for sodium-ion batteries, summarizing different sodium storage processes and electrochemical behaviors. Structural features are categorized into intrinsic (e.g., arrangement and distribution of carbon atoms) and extrinsic (e.g., heteroatoms). The sodium storage processes and behaviors associated with these features and the corresponding regulation strategies are explored in depth. Finally, the challenges and future directions for developing high-performance carbon anodes are proposed, aiming to provide actionable insights for advancing research and commercialization efforts.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"49 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723839","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Steric Hindrance Manipulation in Polymer Electrolytes toward Wide-Temperature Solid-State Lithium Metal Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-27 DOI: 10.1021/acsenergylett.4c03602

Jie Huang, Bin Qiu, Feng Xu, Jinyu Gao, Peixin Zhang, Chuanxin He, Hongwei Mi

{"title":"Steric Hindrance Manipulation in Polymer Electrolytes toward Wide-Temperature Solid-State Lithium Metal Batteries","authors":"Jie Huang, Bin Qiu, Feng Xu, Jinyu Gao, Peixin Zhang, Chuanxin He, Hongwei Mi","doi":"10.1021/acsenergylett.4c03602","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03602","url":null,"abstract":"Solid-state lithium metal batteries (LMBs) based on polymer electrolytes have become a hot topic for next-generation energy storage owing to their high specific energy, flexibility, and simple preparation process. However, poor electrolyte–electrode interface reactions and intrinsically slow Li+ transfer kinetics limit the development of solid-state LMBs. Here, a tris(4-fluorophenyl)phosphine (T4FPP) additive with strong steric hindrance and weak coordination is introduced to remodel the Li+ coordination environment to facilitate electrolyte bulk and interface charge transfer. Furthermore, theoretical analysis combined with in situ/ex situ characterizations demonstrate that the addition of T4FPP helps to construct an anion-dominated solvation structure through molecular crowding and form a LiF/Li2O-rich SEI layer. Ultimately, the LFP|Li full cell based on the T4FPP modified electrolyte works normally even at 10 C with a reversible specific capacity of 88.9 mAh g–1. Simultaneously, the electrochemical performance at 0–60 °C further verified the wide temperature range adaptability of the electrolyte.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"183 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143724014","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Lattice-Matched Ta3N5/Nb5N6 Interface Enables a Bulk Charge Separation Efficiency of Close to 100%

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-27 DOI: 10.1021/acsenergylett.5c00603

Yitong Liu, Zeyu Fan, Ronghua Li, Andraž Mavrič, Iztok Arčon, Matjaz Valant, Gregor Kapun, Beibei Zhang, Chao Feng, Zemin Zhang, Tingxi Chen, Yanning Zhang, Yanbo Li

{"title":"Lattice-Matched Ta3N5/Nb5N6 Interface Enables a Bulk Charge Separation Efficiency of Close to 100%","authors":"Yitong Liu, Zeyu Fan, Ronghua Li, Andraž Mavrič, Iztok Arčon, Matjaz Valant, Gregor Kapun, Beibei Zhang, Chao Feng, Zemin Zhang, Tingxi Chen, Yanning Zhang, Yanbo Li","doi":"10.1021/acsenergylett.5c00603","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00603","url":null,"abstract":"The interface between the semiconductor light absorber and the metal electrode is critical for facilitating the extraction of photogenerated charges in photoelectrodes. Achieving a lattice-matched semiconductor/electrode interface with low defect density is highly desirable but remains a challenge for Ta3N5 photoanodes. In this study, we synthesized niobium nitride thin film electrodes with controllable crystallographic phases to achieve a lattice-matched Ta3N5/Nb5N6 back contact. This results in an enhanced crystallinity of the Ta3N5 film and reduced interfacial defect density. Consequently, the photoanode with the lattice-matched back contact attains a record half-cell solar-to-hydrogen conversion efficiency of 4.1%, attributed to the bulk carrier separation efficiency of nearly 100%. This work highlights lattice-matching as an effective strategy to enhance the efficiency of thin film-based solar energy conversion devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"72 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713427","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Operando Optical Microscopy for Visualization of Dendrite Growth in an Argyrodite LPSCl–Polymer Composite Electrolyte

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-27 DOI: 10.1021/acsenergylett.5c00281

Xiuyu Jin, Di Huang, Qiusu Miao, Ziting Zhu, Wei Tong, Alvaro Videla, Gao Liu

引用次数: 0

Polyoxometalates (POMs) as Proton Conductors

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-27 DOI: 10.1021/acsenergylett.5c00373

Apu Saha, Rupam Sahoo, Shyam Chand Pal, Sayaka Uchida, Madhab C. Das

引用次数: 0

Integration of Microstructural Image Data into Machine Learning Models for Advancing High-Performance Perovskite Solar Cell Design

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-26 DOI: 10.1021/acsenergylett.5c00626

Haotian Liu, Antai Yang, Chengquan Zhong, Xu Zhu, Hao Meng, Zhuo Feng, Jixin Tang, Chen Yang, Jingzi Zhang, Jiakai Liu, Kailong Hu, Xi Lin

{"title":"Integration of Microstructural Image Data into Machine Learning Models for Advancing High-Performance Perovskite Solar Cell Design","authors":"Haotian Liu, Antai Yang, Chengquan Zhong, Xu Zhu, Hao Meng, Zhuo Feng, Jixin Tang, Chen Yang, Jingzi Zhang, Jiakai Liu, Kailong Hu, Xi Lin","doi":"10.1021/acsenergylett.5c00626","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00626","url":null,"abstract":"Perovskite microstructure is one of the key factors limiting the effectiveness of current machine learning (ML) approaches for designing perovskite solar cells (PSCs) with high power conversion efficiency (PCE). This work develops a multimodal convolutional neural network to extract microstructural features from scanning electron microscopy (SEM) images of perovskite thin films. The model dynamically adjusts the weights of different modal information, including material composition, processing techniques, and microstructure, to enhance predictive accuracy. The model achieves an impressive coefficient of determination (R2) of 0.79 on the 1,583 SEM images data set. By introducing six SEM image features to describe the grain size of PSCs, we found that a grain boundary length density (GBLD) below 5.96 and an equivalent circular diameter (ECD) above 0.83 significantly enhance the PCE. Additional experiments confirmed the effectiveness of the results, and by improving these parameters to alter the crystallization, the PCE was increased to 24.61%, and the consistency of the results demonstrated the effectiveness and rationality of the multimodal model.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"59 1","pages":"1884-1891"},"PeriodicalIF":22.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713429","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Comprehensive Crystal Structural Insights into Phase Evolution of Spinel Co-Free Lithium Nickel Manganese Oxide

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-26 DOI: 10.1021/acsenergylett.5c00271

Jiguo Tu, Bokun Zhang, Yan Li, Xiaoyun Wang, Shuqiang Jiao

{"title":"Comprehensive Crystal Structural Insights into Phase Evolution of Spinel Co-Free Lithium Nickel Manganese Oxide","authors":"Jiguo Tu, Bokun Zhang, Yan Li, Xiaoyun Wang, Shuqiang Jiao","doi":"10.1021/acsenergylett.5c00271","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00271","url":null,"abstract":"High-voltage Co-free LiNi0.5Mn1.5O4 (LNMO) is considered a promising candidate for next-generation high-performance lithium-ion batteries. However, there is a significant absence of full understanding of elaborate evolution of crystal structures. This review article aims to thoroughly examine the latest advancements in state-of-the-art LNMO and establish a systematic framework that outlines the varied phase evolution mechanisms under different synthesis conditions and during cycling from the perspective of the crystal structure. First, an analysis of the intrinsic structural properties of LNMO is conducted for optimizing the synthesis process, including crystal orientation, oxygen deficiency, disorder–order transition, and surface phase reconstruction under various synthesis conditions. Then, the phase transformation mechanisms during cycling have been systematically elucidated to develop strategies to mitigate any detrimental effects and improve the electrochemical performance. Finally, the insights into further development directions in LNMO are offered at relevant length scales from the crystal structure level to the electrode level.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":"1892-1910"},"PeriodicalIF":22.0,"publicationDate":"2025-03-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713428","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

An Active and Durable Misfit-Layered Air Electrode for Reversible Protonic Ceramic Electrochemical Cells

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-25 DOI: 10.1021/acsenergylett.4c03562

Xirui Zhang, Yangsen Xu, Kang Xu, Liyan Chen, Feng Zhu, Fan He, Zhiwei Du, Wei Yuan, Yu Chen

{"title":"An Active and Durable Misfit-Layered Air Electrode for Reversible Protonic Ceramic Electrochemical Cells","authors":"Xirui Zhang, Yangsen Xu, Kang Xu, Liyan Chen, Feng Zhu, Fan He, Zhiwei Du, Wei Yuan, Yu Chen","doi":"10.1021/acsenergylett.4c03562","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03562","url":null,"abstract":"Developing air electrode materials with high catalytic activity and durability of oxygen reduction/evolution reactions is an important solution to address the performance and stability problems of reversible protonic ceramic electrochemical cells (R-PCECs). This work reports an active and durable misfit-layered air electrode with a chemical formula of Ca3Co3.8Mo0.2O9+δ. A low area-specific resistance of 0.13 Ω cm2 with reasonable operation stability over 100 h is achieved in the air with 30% steam at 650 °C, likely attributed to the fast surface exchange kinetics and bulk diffusion processes. A single cell with this electrode demonstrates outstanding performance in fuel cell and electrolysis modes, with a peak power density of 1.62 W cm–2 and an electrolysis current density of −2.98 A cm–2 at 650 °C. Most notably, Mo ions doped in air electrodes significantly enhance the cell’s operational reversibility stability, with no observed performance degradation after 52 reversible cycles and over 200 h in dual modes of fuel and electrolysis cell tests.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"20 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143695828","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0