ACS Energy Letters 最新文献

Diketopyrrolopyrroles Act as Redox Mediators in Lithium–Sulfur Batteries 二酮吡咯在锂硫电池中的氧化还原介质作用

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-17 DOI: 10.1021/acsenergylett.5c01262

Joanne S. Searle, Ferdinando Malagreca, Benjamin M. G. Denison, Alexander J. Kibler, Darren A. Walsh, Lee R. Johnson, David B. Amabilino, Graham N. Newton

{"title":"Diketopyrrolopyrroles Act as Redox Mediators in Lithium–Sulfur Batteries","authors":"Joanne S. Searle, Ferdinando Malagreca, Benjamin M. G. Denison, Alexander J. Kibler, Darren A. Walsh, Lee R. Johnson, David B. Amabilino, Graham N. Newton","doi":"10.1021/acsenergylett.5c01262","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01262","url":null,"abstract":"Lithium–sulfur (Li–S) batteries are among the most promising next-generation energy storage technologies, offering gravimetric energy densities greater than those of state-of-the-art lithium-ion batteries. However, widespread commercialization of the technology is hindered by challenges related to the multistep redox chemistry of sulfur. The addition of diketopyrollopyrroles (DPPs) to Li–S battery electrolytes can improve cell performance; however, their mechanism of action remains unclear. Here, we use a range of electrochemical methods to elucidate the mechanism through which DPPs affect the performance of the Li–S batteries. Electrochemical analysis demonstrates the importance of DPP redox potentials in enhancing the redox kinetics of polysulfide reduction, with analytical measurements confirming this is via a redox mediation process in which electrons are shuttled between polysulfide intermediates and the underlying current collector via the DPP molecule. We show that DPP derivatives that are not redox active at the potentials associated with the multi-step interconversion of sulfur and lithium sulfide in Li–S batteries do not show the same effect. Galvanostatic analysis confirms that the enhancement of the kinetics of polysulfide conversion translates to the operation of Li–S batteries, which show an improvement in the discharge capacity after the addition of the additives.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"64 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066968","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Probing Capacity Decay in Vanadium Oxide Cathodes of Aqueous Zinc-Ion Batteries Using Operando EQCM-D 用EQCM-D探测水锌离子电池氧化钒阴极容量衰减

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-16 DOI: 10.1021/acsenergylett.5c00901

Zijian Li, Yuexin Liu, Shu Yang, Zhenghui Pan, Congcong Liu, Xiaoli Zhao, Xiaowei Yang

{"title":"Probing Capacity Decay in Vanadium Oxide Cathodes of Aqueous Zinc-Ion Batteries Using Operando EQCM-D","authors":"Zijian Li, Yuexin Liu, Shu Yang, Zhenghui Pan, Congcong Liu, Xiaoli Zhao, Xiaowei Yang","doi":"10.1021/acsenergylett.5c00901","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00901","url":null,"abstract":"Zn-ion batteries are promising for their safety and cost-effectiveness. Vanadium-based compounds are notable due to their layered structure and polyvalent nature, enabling high-rate capability and large capacity. The type and properties of charge carriers critically influence the structural and performance stability of vanadium-based electrodes, which, however, remain obscure. Herein, we elucidate the H+-dominated intercalation mechanism of vanadium oxide and its correlation with capacity degradation via an electrochemical quartz crystal microbalance investigation. By tracking real-time mass changes and ion diffusion during the electrochemical process, we demonstrate that H+ is the predominant shuttling cation. H+ intercalation generates OH– at the electrode–electrolyte interface, causing alkaline dissolution of vanadium oxide and the capacity decay. With nanosized modification, the dissolution can be mitigated. The electrode exhibits a capacity retention of 98.2% after 2000 cycles at 5 A g–1. This study deepens the understanding of vanadium oxide’s charge storage, guiding the design of high-performance aqueous batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"36 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066575","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

Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries 一种实际可行的制造硫化物基全固态电池的溶液工艺的溶剂粘合剂工程

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-16 DOI: 10.1021/acsenergylett.5c00762

Jihoon Oh, Seung Ho Choi, Heejin Kim, Woo Jun Chung, Minkwan Kim, Inwoo Kim, Taeyong Lee, Jieun Lee, Dong Ok Kim, Sunung Moon, Donghoon Kim, Jang Wook Choi

{"title":"Solvent–Binder Engineering for a Practically Viable Solution Process for Fabricating Sulfide-Based All-Solid-State Batteries","authors":"Jihoon Oh, Seung Ho Choi, Heejin Kim, Woo Jun Chung, Minkwan Kim, Inwoo Kim, Taeyong Lee, Jieun Lee, Dong Ok Kim, Sunung Moon, Donghoon Kim, Jang Wook Choi","doi":"10.1021/acsenergylett.5c00762","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00762","url":null,"abstract":"The commercial viability of sulfide all-solid-state batteries (ASSBs) has been hindered by limited solvent compatibility in solution processing as sulfide solid electrolytes (SEs) degrade in polar solvents. This constraint significantly restricts binder selection, which is critical for both performance─particularly at low pressures─and processability. This study addresses this critical issue by investigating thermoplastic polyurethane (TPU) as a binder dissolved in 1,6-dichlorohexane (DCH), a solvent specifically tailored for sulfide ASSBs. TPU demonstrates outstanding adhesion properties in composite anode, cathode, and SE layers, which not only enhance the long-term cycling performance but also enable double-cast solution processing with minimal binder content for electrode-SE layer manufacturing. A silicon-graphite (Si-Gr)-based pouch-cell fabricated through this solution process maintained 80% capacity retention over 100 cycles under practical conditions (40 μm SE layer, 25 °C, and 2 MPa), validating its practical feasibility. The successful implementation of this optimized solvent–binding system for solution processing represents a significant advancement toward practical ASSB technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"74 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144067087","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

Charge Transfer from Perovskite Quantum Dots to Multifunctional Ligands with Tethered Molecular Species 钙钛矿量子点与系链分子的多功能配体之间的电荷转移

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00881

Mariam Kurashvili, Lena S. Stickel, Jordi Llusar, Christian Wilhelm, Fabian Felixberger, Ivana Ivanović-Burmazović, Ivan Infante, Jochen Feldmann, Quinten A. Akkerman

{"title":"Charge Transfer from Perovskite Quantum Dots to Multifunctional Ligands with Tethered Molecular Species","authors":"Mariam Kurashvili, Lena S. Stickel, Jordi Llusar, Christian Wilhelm, Fabian Felixberger, Ivana Ivanović-Burmazović, Ivan Infante, Jochen Feldmann, Quinten A. Akkerman","doi":"10.1021/acsenergylett.5c00881","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00881","url":null,"abstract":"Perovskite quantum dots (pQDs) are promising materials for optoelectronic and photocatalytic applications due to their unique optical properties. To enhance charge carrier extraction or injection, donor/acceptor molecules can be tethered to the pQD. These molecules must strongly bind to the ionic surfaces of pQDs without compromising colloidal stability. This is achieved by using multifunctional ligands containing a quaternary ammonium binding group for strong pQD surface attachment, a long tail group for colloidal stability, and a functional group near the pQD surface. Such pQDs with ferrocene-functionalized ligands show fast photoexcited hole transfer with near-unity efficiency. Density functional theory calculations reveal how ferrocene’s molecular structure reorganizes following hole transfer, affecting its charge separation efficiency. This approach can also be extended to photoexcited electron and energy transfer processes with pQDs. Therefore, this strategy offers a blueprint for creating efficient pQD–molecular hybrids for applications like photocatalysis.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066443","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

Rational Design of Phosphate Cathodes with Improved Na-storage Performance 提高na存储性能的磷酸盐阴极的合理设计

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00653

Xusheng Zhang, Huican Mao, Zhao Chen, Lin Zhou, Lilu Liu, Mingxuan Wu, Zilong Lv, Zhihao Zhang, Yukun Zhong, Yong-Sheng Hu, Junmei Zhao

{"title":"Rational Design of Phosphate Cathodes with Improved Na-storage Performance","authors":"Xusheng Zhang, Huican Mao, Zhao Chen, Lin Zhou, Lilu Liu, Mingxuan Wu, Zilong Lv, Zhihao Zhang, Yukun Zhong, Yong-Sheng Hu, Junmei Zhao","doi":"10.1021/acsenergylett.5c00653","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00653","url":null,"abstract":"As a typical Na-superionic conductor (NASICON), the Na3+xV2–xMnx(PO4)3 cathodes have a high capacity of over 120 mA g–1 owing to the multielectron reaction. However, these cathodes always show structural degradation and sluggish Na-ion diffusion kinetics derived from the Jahn-Teller distortion of Mn. Here, Al3+ was first used to replace Mn2+ in Na3.5V1.5Mn0.5(PO4)3, which could significantly reduce the Jahn-Teller distortion through regulating the MnO6 local crystal structure and enhancing Mn–O bond strength. Additionally, Al3+ could also increase the electronic conductivity and the Na-ion migration ability. As a result, the as-prepared Na3.3V1.5Mn0.3Al0.2(PO4)3 cathode achieved a high-rate capacity of 96.8 mAh g–1 at 20 C and a high-capacity retention of 88.8% after 3000 cycles at 10 C. The application prospects of Na3.3V1.5Mn0.3Al0.2(PO4)3 cathode were further confirmed by a scale-up synthesis, and a 21700-type cylindrical cell showed an excellent cycling performance of over 80% capacity retention after 4000 cycles at 1 C.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"120 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066442","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

Regulating Bond Structure in Polyanion Cathode for Long-Cycle-Life Sodium-Ion Batteries 长循环寿命钠离子电池聚阴离子阴极键结构调控研究

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00769

Shuoshuo Cheng, Yibing Zhang, Peng Lv, Shiyu Li, Ying Bai

引用次数: 0

Hidden Acidification Challenges in Electrochemical Ocean Decarbonization 电化学海洋脱碳中潜在的酸化挑战

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00900

Wei Zhang, Adnan Ozden, Yu Yang, Aoni Xu, Fengwang Li

引用次数: 0

Visualizing Electron Transport and Interface Evolution of Li3InCl6-Based Composite Cathode for All-Solid-State Batteries 全固态电池用li3incl6基复合阴极的电子传递与界面演化可视化

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00174

Rui Li, Yanpei Fan, Xiaotong Liu, Jiewen Li, Haodong Zhang, Lin Lin, Zhenbin Wang, Bohua Wen

{"title":"Visualizing Electron Transport and Interface Evolution of Li3InCl6-Based Composite Cathode for All-Solid-State Batteries","authors":"Rui Li, Yanpei Fan, Xiaotong Liu, Jiewen Li, Haodong Zhang, Lin Lin, Zhenbin Wang, Bohua Wen","doi":"10.1021/acsenergylett.5c00174","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00174","url":null,"abstract":"All-solid-state batteries (ASSBs) promise higher energy density and improved safety, but stable solid electrolyte-electrode interfaces remain a key challenge. Mixed ionic-electronic conducting interphases cause degradation, limiting the cathode lifetime. Here, we employ operando electrochemical atomic force microscopy based on modified Kelvin probe force microscopy to visualize nanoscale electron transport and dynamic evolution of the composite cathode interface. By analyzing the contact current (Ic) distribution, we distinguish the interfacial stability of Li3InCl6 (LIC)-based cathodes with LiNi0.8Mn0.1Co0.1O2, both coated and uncoated with LiNbO3, and conductive carbon additives. Operando studies, combined with interfacial mechanical property mapping, reveal that the Ic heterogeneity and magnitude critically influence degradation. In LIC-based cathodes, decomposed organic interphases enhance electron transport, driving the formation of high-modulus inorganic species that accelerate LIC breakdown. These findings link microscopic electron transport and interface evolution to electrochemical performance, offering insights for designing stable interphases to advance ASSB technology.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"30 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144066441","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

Epitaxial Growth of High-Quality Perovskite Heterojunctions for Direct-Conversion X-ray Detectors 用于直接转换x射线探测器的高质量钙钛矿异质结外延生长

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-15 DOI: 10.1021/acsenergylett.5c00938

Yang He, Sheng Gao, Bo Zhao, Huiwen Chen, Ziyao Zhu, Mingrui Yu, Yang Zhang, Yang Li, Martin Stolterfoht, Xueqing Yang, Xingzhu Wang, Yunlong Li

{"title":"Epitaxial Growth of High-Quality Perovskite Heterojunctions for Direct-Conversion X-ray Detectors","authors":"Yang He, Sheng Gao, Bo Zhao, Huiwen Chen, Ziyao Zhu, Mingrui Yu, Yang Zhang, Yang Li, Martin Stolterfoht, Xueqing Yang, Xingzhu Wang, Yunlong Li","doi":"10.1021/acsenergylett.5c00938","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00938","url":null,"abstract":"Three-dimensional metal halide perovskites (3D-MHPs) have emerged as potential semiconductors for direct-conversion X-ray detectors. However, excessive ion migration in 3D-MHPs compromises device stability, hindering practical deployment. While perovskite heterojunctions have been explored to suppress ion migration, their effectiveness are often limited by challenges in fabricating high-quality heterojunctions, resulting in suboptimal charge collection compared to individual perovskite crystals. In this work, a liquid-phase interfacial array-epitaxial growth method was developed to construct high-quality MAPbBr3/MAPbI3 heterojunctions for direct X-ray detectors. The heterojunction crystal exhibit a serrated, ultrathick transition region that enhances X-ray response by increasing the interfacial contact area between MAPbBr3 and MAPbI3. Consequently, the fabricated detectors demonstrate stable operational performance, a high sensitivity of 0.99 × 106 μC Gyair–1 cm–2, and an ultralow detection limit of 0.56 nGyair s–1. Furthermore, the built-in electric field enables self-powered X-ray detection at 0 V bias, achieving a sensitivity of 1.16 × 103 μC Gyair–1 cm–2.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"8 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143979874","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

Phase Evolution Extension of Cu2ZnSn(S,Se)4 Absorber Boosting the Efficiency of Kesterite Solar Cells to 14.99% Cu2ZnSn(S,Se)4吸收体的相变扩展将Kesterite太阳能电池效率提高到14.99%

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-05-14 DOI: 10.1021/acsenergylett.5c01007

Ge Yao, Zucheng Wu, Dongxing Kou, Bingyin Kong, Hao Wei, Zhipeng Shao, Wenhui Zhou, Zhengji Zhou, Shengjie Yuan, Yafang Qi, Litao Han, Guanglei Cui, Sixin Wu

{"title":"Phase Evolution Extension of Cu2ZnSn(S,Se)4 Absorber Boosting the Efficiency of Kesterite Solar Cells to 14.99%","authors":"Ge Yao, Zucheng Wu, Dongxing Kou, Bingyin Kong, Hao Wei, Zhipeng Shao, Wenhui Zhou, Zhengji Zhou, Shengjie Yuan, Yafang Qi, Litao Han, Guanglei Cui, Sixin Wu","doi":"10.1021/acsenergylett.5c01007","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01007","url":null,"abstract":"The presence of secondary phases and a high concentration of deep-level defects led to a large open-circuit voltage deficit (Voc,deficit) for Cu2ZnSn(S,Se)4 (CZTSSe) solar cells. Here we regulate the phase evolution from CZTS to CZTSSe in the initial selenization stage to obtain high-quality absorber with minimal defects and secondary phases. By adding the bidentate chelation structured mercaptopropionic acid (MPA) into the air-prepared 2-methoxyethanol (MOE) precursor solution, large CZTS colloidal particles and dense precursor films are prepared. During the initial selenization stage, the reduced nucleation sites can decrease selenium–molecule interactions and extend the phase evolution process. This extension makes the heterogeneous nucleation more controllable, fostering uniform element distribution and enhanced growth of permeating the large-grain layer. These benefits demonstrate a substantial increase in device efficiency up to 14.99% (certified at 14.38%) with a reduced Voc,deficit of 281.18 mV. The findings are of great significance for further efficiency leaps of kesterite solar cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"122 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143945621","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