ACS Energy Letters 最新文献

Tracking Local pH Dynamics during Water Electrolysis via In-Line Continuous Flow Raman Spectroscopy

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.5c00582

Raul A. Marquez, Jay T. Bender, Shashwati C. da Cunha, Ashton M. Aleman, Amaresh Sahu, Venkat Ganesan, Delia J. Milliron, Joaquin Resasco, Thomas F. Jaramillo, C. Buddie Mullins

{"title":"Tracking Local pH Dynamics during Water Electrolysis via In-Line Continuous Flow Raman Spectroscopy","authors":"Raul A. Marquez, Jay T. Bender, Shashwati C. da Cunha, Ashton M. Aleman, Amaresh Sahu, Venkat Ganesan, Delia J. Milliron, Joaquin Resasco, Thomas F. Jaramillo, C. Buddie Mullins","doi":"10.1021/acsenergylett.5c00582","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00582","url":null,"abstract":"The performance of electrochemical devices, which play a critical role in decarbonization efforts, is often governed by proton-coupled electron transfer reactions at the electrode–electrolyte interface. These reactions are highly sensitive to the complex and dynamic microenvironment present at the electrode surface. However, characterizing this environment─particularly monitoring interfacial pH and its evolution under reaction conditions─remains challenging, necessitating the development of advanced analytical tools. Here, we introduce in-line continuous flow Raman spectroscopy (CFRS) as a spectroelectrochemical platform for quantifying interfacial pH swings generated during water-splitting. By monitoring phosphate ion speciation and controlling the hydrodynamics with a flow cell, we measure pH swings as a function of current density, flow rate, and distance from the electrode. Comparison with theoretical models reveals the impact of bulk pH, boundary layer thickness, and bubble dynamics at high current densities. Collectively, these findings establish CFRS as a platform for quantitatively investigating pH dynamics, offering critical insights for advancing electrochemical energy conversion technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766429","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

Buried SnI2 Induces Gradient Heterojunctions in Sn–Pb Perovskite Solar Cells

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-03 DOI: 10.1021/acsenergylett.5c00305

Xuewei Liu, Jia Xu, Chenxu Zhao, Fan Shen, Pengchen Zou, Yijun Wang, Bozhang Ji, Xingjie Guan, Xu Pan, Jianxi Yao

引用次数: 0

Disconnected Lithium Metal Damages Solid-State Electrolytes

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c00101

Diana Avadanii, Steffen Ganschow, Markus Stypa, Sonja Müller, Sabrina Lang, Dominik Kramer, Christoph Kirchlechner, Reiner Mönig

引用次数: 0

Vacancy-Catalyzed Cation Homogenization for High-Performance AgBiS2 Nanocrystal Solar Cells

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c00506

Yang Liu, Zitao Ni, Lucheng Peng, Hao Wu, Zeke Liu, Yongjie Wang, Wanli Ma, Gerasimos Konstantatos

引用次数: 0

Interlayer Cationic Defect Engineering in Lamellar Vanadate Cathodes Enables Ultralong-Lifespan Magnesium-Ion Batteries

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-02 DOI: 10.1021/acsenergylett.5c00380

Fuyu Chen, Kaifeng Huang, Hong-Yi Li, Qing Zhong, Jili Yue, Jiang Diao, Zhongting Wang, Guangsheng Huang, Bin Jiang, Fusheng Pan

{"title":"Interlayer Cationic Defect Engineering in Lamellar Vanadate Cathodes Enables Ultralong-Lifespan Magnesium-Ion Batteries","authors":"Fuyu Chen, Kaifeng Huang, Hong-Yi Li, Qing Zhong, Jili Yue, Jiang Diao, Zhongting Wang, Guangsheng Huang, Bin Jiang, Fusheng Pan","doi":"10.1021/acsenergylett.5c00380","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00380","url":null,"abstract":"The rate performance and lifespan of rechargeable magnesium-ion batteries (RMIBs) are limited by the low ionic conductivity and poor structural stability of the cathode materials. Herein, we introduce interlayer cationic defect engineering to enhance the diffusion dynamics and structural integrity of vanadate cathodes for the RMIBs. Through interlayer Mg2+ doping, we synthesized a defect-engineered cathode material (d-MgNVO) that establishes optimized migration pathways. Lattice defects confine ionic migration within the vanadate framework and reconstruct short, rapid, and reversible migration pathways, increasing the Mg2+ diffusion coefficient to 10–11–10–13 cm2 s–1. The d-MgNVO cathode exhibits a capacity of 198 mAh g–1 at 0.05 A g–1 and 73 mAh g–1 at 3.0 A g–1, showcasing good rate capability; the PTCDA//d-MgNVO full cell achieves a long lifespan of 5,000 cycles at 1.0 A g–1 with 79% capacity retention. These findings highlight interlayer cationic defect engineering as a promising strategy for high-performance, long-lasting RMIBs and other secondary batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"32 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758594","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

Post-Treatment Free Yttrium Phosphotungstate Anode Interfacial Material for Organic Solar Cells with 20.55% Efficiency 用于效率为 20.55% 的有机太阳能电池的无后处理磷钨酸钇阳极界面材料

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-04-01 DOI: 10.1021/acsenergylett.5c00482

Xingjian Dai, Ben Fan, Weilin Zhou, Yinfeng Li, Xiaopeng Xu, Qiang Peng

{"title":"Post-Treatment Free Yttrium Phosphotungstate Anode Interfacial Material for Organic Solar Cells with 20.55% Efficiency","authors":"Xingjian Dai, Ben Fan, Weilin Zhou, Yinfeng Li, Xiaopeng Xu, Qiang Peng","doi":"10.1021/acsenergylett.5c00482","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00482","url":null,"abstract":"Hole transport layers (HTLs) play a crucial role in organic solar cells, yet achieving high performance while maintaining simple processing requirements remains challenging. Here, we report a facile strategy utilizing yttrium-doped phosphotungstate (YPWO) as an efficient HTL material, prepared through a straightforward solution process without requiring post-treatment. The incorporation of yttrium enhances molecular stacking and reduces defect states, resulting in improved charge transport properties and suppressed recombination losses. YPWO-based devices achieve a power conversion efficiency (PCE) of 20.55% (certified efficiency of 20.30%), attributed to optimized energy level alignment, reduced trap states, and improved charge carrier mobility. Additionally, YPWO demonstrates thickness tolerance and compatibility across various photovoltaic systems, achieving PCEs exceeding 19% with different photoactive layers. This work presents a viable strategy for developing efficient HTL materials, offering a practical pathway toward commercially viable organic solar cells through simplified processing.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"107 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758530","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

Multicomponent Solvent Engineered Spatially Uniform 2D/3D Perovskite Heterojunction for Solar Cells

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-31 DOI: 10.1021/acsenergylett.5c00393

Yinghao Xu, Shaokuan Gong, Zhinan Zhang, Shaofu Wang, Shengjie Du, Dexin Pu, Wenbo Li, Yang Zheng, Ke Wu, Ti Wang, Weijun Ke, Xingzhong Zhao, Wei Liu, Guojia Fang, Xihan Chen, Zhenhua Yu

{"title":"Multicomponent Solvent Engineered Spatially Uniform 2D/3D Perovskite Heterojunction for Solar Cells","authors":"Yinghao Xu, Shaokuan Gong, Zhinan Zhang, Shaofu Wang, Shengjie Du, Dexin Pu, Wenbo Li, Yang Zheng, Ke Wu, Ti Wang, Weijun Ke, Xingzhong Zhao, Wei Liu, Guojia Fang, Xihan Chen, Zhenhua Yu","doi":"10.1021/acsenergylett.5c00393","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00393","url":null,"abstract":"This study introduces a multicomponent solvent engineering approach for constructing high-quality 2D/3D metal halide perovskite (MHP) heterostructures, addressing vertical inhomogeneity in ultrathin 2D capping layers for perovskite solar cells (PSCs). Through synergistic solvent coordination, isopropyl alcohol spatially confines 2D layer formation at the 3D perovskite surface, while dimethyl sulfoxide induces controlled 3D matrix dissolution to enable vertical phase propagation. Acetonitrile optimizes solvent penetration dynamics, achieving 2D layers with exceptional spatial homogeneity across multiple cation systems. The optimized PDAI2-derived 2D/3D architecture demonstrates a certified power conversion efficiency (PCE) of 25.57% (champion 26.14%) with an 85.62% fill factor, attributed to enhanced interfacial charge transport at the C60/perovskite junction through reduced nonradiative recombination. The spatially uniform 2D capping layer confers remarkable operational stability, retaining 92% initial PCE after 5,000 h dark aging and 90% efficiency following 1,700 h maximum power point tracking under continuous 1-sun illumination.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143744864","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

Surface Engineered BiVO4 for Photoelectrochemical Alkene Epoxidation via Bromine Mediation

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-31 DOI: 10.1021/acsenergylett.5c00389

Qingjie Wang, Linxiao Wu, Haiwen Shi, Jingshan Luo

{"title":"Surface Engineered BiVO4 for Photoelectrochemical Alkene Epoxidation via Bromine Mediation","authors":"Qingjie Wang, Linxiao Wu, Haiwen Shi, Jingshan Luo","doi":"10.1021/acsenergylett.5c00389","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00389","url":null,"abstract":"Selective epoxidation of alkenes is essential in organic synthesis, yet achieving it under mild conditions presents significant challenges. Photoelectrochemical (PEC) alkene epoxidation driven by hypobromite (BrO–, Br+) formation offers a green and sustainable route, and enhancing Br+ production is essential for achieving high product selectivity. A synergistic strategy that integrates water oxidation to hydrogen peroxide with bromide oxidation to bromine (Br2) using a surface engineered BiVO4 photoanode is presented. In situ generated H2O2 and Br2 yield BrO–, which serves as an active brominating (Br+) agent for alkene epoxidation. Consequently, the surface engineered BiVO4 photoanode achieves over 98.1 ± 0.79% conversion rate and 91.9 ± 0.99% selectivity across various alkenes. An unbiased PEC tandem device is constructed by coupling a BiVO4 photoanode for styrene epoxidation with a Cu2O photocathode for hydrogen production, achieving simultaneous styrene oxide production with 86.4% selectivity and hydrogen production. Our work provides new insights into PEC organic synthesis and hydrogen production.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736669","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

Triphenylamine-Based Hole-Transporting Ligands for 2D/3D FAPbI3 Perovskite Solar Cells

IF 22 1区材料科学

ACS Energy Letters Pub Date : 2025-03-30 DOI: 10.1021/acsenergylett.5c00471

Huaiman Cao, Tianshu Li, Liangyu Zhao, Yue Qiang, Xufan Zheng, Shouye Dai, Yulong Chen, Yong Zhu, Liang Zhao, Rui Cai, Zhiguang Sun, Fei Li, Yingguo Yang, Lijun Zhang, Hin-Lap Yip, Ze Yu

{"title":"Triphenylamine-Based Hole-Transporting Ligands for 2D/3D FAPbI3 Perovskite Solar Cells","authors":"Huaiman Cao, Tianshu Li, Liangyu Zhao, Yue Qiang, Xufan Zheng, Shouye Dai, Yulong Chen, Yong Zhu, Liang Zhao, Rui Cai, Zhiguang Sun, Fei Li, Yingguo Yang, Lijun Zhang, Hin-Lap Yip, Ze Yu","doi":"10.1021/acsenergylett.5c00471","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00471","url":null,"abstract":"Two-dimensional (2D) perovskites suffer from poor charge transport due to the insulating nature of typically used organic spacers. Here, we develop a triphenylamine (TPA)-functionalized semiconducting ligand, namely, DPA-PEAI, in which the TPA moiety is tethered to the ethylammonium cation. Crystallographic analysis of n = 1 2D perovskite (DPA-PEA)2PbI4 reveals that the propeller-like geometry and enriched phenyl rings of the TPA tail enable the formation of multifarious π-stacking interconnections between neighboring ligands. Theoretical calculations further unveil that both the binding energy and hole transfer integral are augmented between the adjacent DPA-PEA cations, in contrast to the widely used phenylethylammonium (PEA) counterpart. This cross-electronic coupling feature allows the formation of multiple hole-transfer pathways within DPA-PEA-based 2D perovskites, enabling efficient out-of-plane charge transport, as confirmed by a set of characterizations. As a consequence, 2D/3D FAPbI3-based PSCs employing DPA-PEAI afford a champion efficiency of 25.7%, which ranks among the best efficiencies reported for conjugative ligands.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"72 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-03-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143736670","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

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