Tin (Sn) halide perovskites, typically FASnI3, resemble their lead (Pb)-based counterparts in optoelectronic properties but possess dissimilar crystallization kinetics leading to meager device performance. In this study, we fabricated FASn-halide perovskite solar cells (PSCs) with a high open-circuit voltage (VOC) of 1042 mV and a power conversion efficiency (PCE) of 15.48%, as verified by an independent photovoltaic lab. By employing a comprehensive solvent and surface engineering strategy, we enhanced crystal stability and grain size, reduced trap state density, and improved energy level alignment. This was achieved by introducing tetraethylammonium (TEA+) cation at both surface and bulk grain boundaries, through the post-treatment of perovskite film with a preheated solution mixture of N,N-diethylformamide (DEF) and tetraethylammonium bromide (TEABr) in isopropanol (IPA). This approach also effectively suppressed the notorious Sn2+ to Sn4+ oxidation, resulting in reduced charge carrier trapping at grain boundaries. Moreover, the effectiveness and scalability of this strategy are validated with a 1.02 cm2 active area device, achieving a high PCE of 12.21%. Our findings highlight the potential of Sn-halide PSCs to rival Pb-based PSCs in efficiency and stability, paving the way for more environmentally friendly, Pb-free alternatives.
{"title":"Synergistic Solvent and Surface Engineering to Reduce VOC Loss in Tin Halide Perovskite Solar Cells","authors":"M. Bilal Faheem, Bilawal Khan, Yuchen Zhang, Hansheng Li, Madan Saud, Hanjie Lin, Haining Zhang, Syed Bilal Ahmed, Vanshika Vanshika, Ruosi Qiao, Poojan Kaswekar, Yeqing Wang, Weiwei Zheng, Jr-Hau He, Quinn Qiao","doi":"10.1021/acsenergylett.5c00792","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00792","url":null,"abstract":"Tin (Sn) halide perovskites, typically FASnI<sub>3</sub>, resemble their lead (Pb)-based counterparts in optoelectronic properties but possess dissimilar crystallization kinetics leading to meager device performance. In this study, we fabricated FASn-halide perovskite solar cells (PSCs) with a high open-circuit voltage (<i>V</i><sub>OC</sub>) of 1042 mV and a power conversion efficiency (PCE) of 15.48%, as verified by an independent photovoltaic lab. By employing a comprehensive solvent and surface engineering strategy, we enhanced crystal stability and grain size, reduced trap state density, and improved energy level alignment. This was achieved by introducing tetraethylammonium (TEA<sup>+</sup>) cation at both surface and bulk grain boundaries, through the post-treatment of perovskite film with a preheated solution mixture of <i>N</i>,<i>N</i>-diethylformamide (DEF) and tetraethylammonium bromide (TEABr) in isopropanol (IPA). This approach also effectively suppressed the notorious Sn<sup>2+</sup> to Sn<sup>4+</sup> oxidation, resulting in reduced charge carrier trapping at grain boundaries. Moreover, the effectiveness and scalability of this strategy are validated with a 1.02 cm<sup>2</sup> active area device, achieving a high PCE of 12.21%. Our findings highlight the potential of Sn-halide PSCs to rival Pb-based PSCs in efficiency and stability, paving the way for more environmentally friendly, Pb-free alternatives.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"237 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144329396","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}
Industrially textured perovskite/silicon tandem solar cells are among the most promising candidates for future low-cost photovoltaic deployment. Air-annealing is an inevitable process to fabricate high-quality perovskite films during the hybrid two-step deposition method. However, this process often leads to severe perovskite decomposition on the surface because of moisture exposure and high-temperature. To address this issue, a stabilizing additive─dimethylphenethylsulfonium iodide (DMPESI)─is introduced into the organic salt solution, forming a hydrophobic internal encapsulation layer. As a result, the perovskite surface decomposition is effectively suppressed during the air-annealing process and the resulting perovskite films exhibit significantly enhanced film stability and quality. Consequently, the industrially textured perovskite/silicon tandem solar cells delivered an impressive efficiency of 30.49% (1.21 cm2). Moreover, encapsulated tandem devices retained 84% of their initial efficiency after nearly 1800 h of maximum power point tracking (MPPT) (ISOS-L-1) and 80% after 723 h of damp heat test (ISOS-D-3).
工业结构钙钛矿/硅串联太阳能电池是未来低成本光伏部署最有前途的候选者之一。空气退火是制备高质量钙钛矿薄膜的必经工艺。然而，由于受潮和高温，这一过程往往会导致表面严重的钙钛矿分解。为了解决这一问题，在有机盐溶液中加入稳定添加剂二甲基苯乙基碘化磺酸（DMPESI），形成疏水的内部包封层。结果表明，在空气退火过程中，钙钛矿的表面分解被有效抑制，得到的钙钛矿薄膜的稳定性和质量显著提高。因此，工业结构钙钛矿/硅串联太阳能电池提供了30.49% （1.21 cm2）的令人印象深刻的效率。此外，封装串联器件在近1800小时的最大功率点跟踪（MPPT） （iso - l -1）和723小时的湿热测试（iso - d -3）后保持了84%的初始效率。
{"title":"Damp-Stable Perovskite/Silicon Tandem Solar Cells with Internal Encapsulating Sulfonium-Based Molecules","authors":"Haowen Luo, Xinrui Han, Bowen Yang, Wennan Ou, Jiajia Suo, Hongfei Sun, Xuntian Zheng, Jiajia Hong, Zijing Chu, Lu Zhao, Shuncheng Yang, Pu Wu, Chenyang Duan, Chenshuaiyu Liu, Manya Li, Ludong Li, Renxing Lin, Wenchi Kong, Hairen Tan","doi":"10.1021/acsenergylett.5c01010","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01010","url":null,"abstract":"Industrially textured perovskite/silicon tandem solar cells are among the most promising candidates for future low-cost photovoltaic deployment. Air-annealing is an inevitable process to fabricate high-quality perovskite films during the hybrid two-step deposition method. However, this process often leads to severe perovskite decomposition on the surface because of moisture exposure and high-temperature. To address this issue, a stabilizing additive─dimethylphenethylsulfonium iodide (DMPESI)─is introduced into the organic salt solution, forming a hydrophobic internal encapsulation layer. As a result, the perovskite surface decomposition is effectively suppressed during the air-annealing process and the resulting perovskite films exhibit significantly enhanced film stability and quality. Consequently, the industrially textured perovskite/silicon tandem solar cells delivered an impressive efficiency of 30.49% (1.21 cm<sup>2</sup>). Moreover, encapsulated tandem devices retained 84% of their initial efficiency after nearly 1800 h of maximum power point tracking (MPPT) (ISOS-L-1) and 80% after 723 h of damp heat test (ISOS-D-3).","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"607 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144329397","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}
Rechargeable sodium ion batteries (SIBs) under extreme conditions are still limited by sluggish Na+ transport/desolvation kinetics and unstable electrode/electrolyte interface, thus leading to rapid capacity decay and a short lifespan. Herein, electrolyte engineering is proposed via solvent–solvent hydrogen bonding interaction between dimethyl sulfite (DMS) and glutaronitrile (GN) solvents for wide-temperature SIBs. The formed hydrogen bonding between DMS and GN solvents not only enhances the antioxidative ability of DMS but also simultaneously promotes the formation of a loose solvation structure by distancing DMS from Na+ ions, facilitating Na+ transport/desolvation kinetics. The well-designed electrolyte exhibits wide-temperature application from −55 to 60 °C in NaNi0.33Fe0.33Mn0.33O2 ||Na half cells, while the improved cycling stability with preactivated hard carbon anode is also obtained from −40 to 45 °C. This work sheds light on intersolvent synergistic effect for wide-temperature electrolyte design, specializing in regulating electrolyte thermodynamic and kinetic behavior.
{"title":"Constructing All-Climate Hybrid Sodium Ion/Metal Batteries through Intersolvent Synergistic Effect","authors":"Yiwen Gao, Haifeng Tu, Jiangyan Xue, Yan Wang, Shiqi Zhang, Suwan Lu, Lingwang Liu, Keyang Peng, Guochao Sun, Guangye Wu, Peng Ding, Yi Yang, Zhicheng Wang, Jingjing Xu, Xiaodong Wu","doi":"10.1021/acsenergylett.5c01080","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01080","url":null,"abstract":"Rechargeable sodium ion batteries (SIBs) under extreme conditions are still limited by sluggish Na<sup>+</sup> transport/desolvation kinetics and unstable electrode/electrolyte interface, thus leading to rapid capacity decay and a short lifespan. Herein, electrolyte engineering is proposed via solvent–solvent hydrogen bonding interaction between dimethyl sulfite (DMS) and glutaronitrile (GN) solvents for wide-temperature SIBs. The formed hydrogen bonding between DMS and GN solvents not only enhances the antioxidative ability of DMS but also simultaneously promotes the formation of a loose solvation structure by distancing DMS from Na<sup>+</sup> ions, facilitating Na<sup>+</sup> transport/desolvation kinetics. The well-designed electrolyte exhibits wide-temperature application from −55 to 60 °C in NaNi<sub>0.33</sub>Fe<sub>0.33</sub>Mn<sub>0.33</sub>O<sub>2</sub> ||Na half cells, while the improved cycling stability with preactivated hard carbon anode is also obtained from −40 to 45 °C. This work sheds light on intersolvent synergistic effect for wide-temperature electrolyte design, specializing in regulating electrolyte thermodynamic and kinetic behavior.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"15 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144329399","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}
Pub Date : 2025-06-19DOI: 10.1021/acsenergylett.5c01213
Yameen Ahmed, Wanlong Wang, Mohammad Reza Kokaba, Augusto Amaro, Vishal Yeddu, Hannah Gartside, Muhammad Awais, Sergey Dayneko, Dongyang Zhang, Hayley C. Parkin, I Teng Cheong, Victor Marrugat-Arnal, Alexandre G. Brolo, Makhsud I. Saidaminov
Scalable fabrication of perovskite solar cells (PSCs) in ambient air is important toward widespread industrial adoption. While spiro-OMeTAD-based PSCs perform well, they lack long-term stability, and alternative hole transport layers often trade efficiency for durability. Here we report high molecular weight poly(triarylamine) (HMW PTAA)-based PSCs fabricated in ambient air using scalable techniques, achieving 23.7% efficiency for 0.049 cm2 solar cells and 22.2% for 10.23 cm2 mini-modules, representing, to our knowledge, the highest values reported for scalable n-i-p PTAA-based perovskite photovoltaics made in ambient conditions. The HMW PTAA spontaneously forms a contact-area-reduced (CAR) interface with perovskite, enhancing charge collection and suppressing recombination. Despite reduced adhesion, the CAR interface improves PSC stability; devices retain 83% of their efficiency after 1000 h of operation at maximum power point at 55 ± 5 °C, and 77% after 1100 h of thermal stress at 85 °C. We attribute this resilience to strain-relieving interfacial voids created by the CAR interface.
{"title":"PTAA/Perovskite Contact-Area Reduced Solar Modules","authors":"Yameen Ahmed, Wanlong Wang, Mohammad Reza Kokaba, Augusto Amaro, Vishal Yeddu, Hannah Gartside, Muhammad Awais, Sergey Dayneko, Dongyang Zhang, Hayley C. Parkin, I Teng Cheong, Victor Marrugat-Arnal, Alexandre G. Brolo, Makhsud I. Saidaminov","doi":"10.1021/acsenergylett.5c01213","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01213","url":null,"abstract":"Scalable fabrication of perovskite solar cells (PSCs) in ambient air is important toward widespread industrial adoption. While spiro-OMeTAD-based PSCs perform well, they lack long-term stability, and alternative hole transport layers often trade efficiency for durability. Here we report high molecular weight poly(triarylamine) (HMW PTAA)-based PSCs fabricated in ambient air using scalable techniques, achieving 23.7% efficiency for 0.049 cm<sup>2</sup> solar cells and 22.2% for 10.23 cm<sup>2</sup> mini-modules, representing, to our knowledge, the highest values reported for scalable <i>n-i-p</i> PTAA-based perovskite photovoltaics made in ambient conditions. The HMW PTAA spontaneously forms a contact-area-reduced (CAR) interface with perovskite, enhancing charge collection and suppressing recombination. Despite reduced adhesion, the CAR interface improves PSC stability; devices retain 83% of their efficiency after 1000 h of operation at maximum power point at 55 ± 5 °C, and 77% after 1100 h of thermal stress at 85 °C. We attribute this resilience to strain-relieving interfacial voids created by the CAR interface.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"234 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144319705","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}
Pub Date : 2025-06-18DOI: 10.1021/acsenergylett.5c01147
Xing Zhou, Chao Yang, Wenxi Hu, Jin Han, Ya You
Thermal safety is a key bottleneck in the development of high-energy-density batteries, primarily due to the high volatility and flammability of organic electrolytes. Efforts to enhance battery safety focuses largely on making electrolytes flame-retardant to prevent ignition. However, the direct correlation between electrolyte nonflammability and battery thermal safety could be misleading, as the intricate cell environment may deviate the actual battery safety performance from the material-level design. Therefore, clarifying other influential factors beyond flammability and establishing multiscale and quantitative assessment metrics are highly crucial. In this Perspective we discuss the key factors and characterization methods for evaluating the thermal safety of electrolytes from the material to the cell level and simultaneously provide insights into standardization of measurement protocols. Finally, a brief outlook on future directions in electrolyte thermal safety assessment is presented. This perspective may inspire more efforts toward advanced characterization techniques and comprehensive safety evaluation frameworks, further paving the way for safer and more reliable energy storage technologies in the future.
{"title":"Assessment of Thermal Safety for Organic Electrolytes: from Material to Cell Level","authors":"Xing Zhou, Chao Yang, Wenxi Hu, Jin Han, Ya You","doi":"10.1021/acsenergylett.5c01147","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01147","url":null,"abstract":"Thermal safety is a key bottleneck in the development of high-energy-density batteries, primarily due to the high volatility and flammability of organic electrolytes. Efforts to enhance battery safety focuses largely on making electrolytes flame-retardant to prevent ignition. However, the direct correlation between electrolyte nonflammability and battery thermal safety could be misleading, as the intricate cell environment may deviate the actual battery safety performance from the material-level design. Therefore, clarifying other influential factors beyond flammability and establishing multiscale and quantitative assessment metrics are highly crucial. In this Perspective we discuss the key factors and characterization methods for evaluating the thermal safety of electrolytes from the material to the cell level and simultaneously provide insights into standardization of measurement protocols. Finally, a brief outlook on future directions in electrolyte thermal safety assessment is presented. This perspective may inspire more efforts toward advanced characterization techniques and comprehensive safety evaluation frameworks, further paving the way for safer and more reliable energy storage technologies in the future.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311890","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}
Pub Date : 2025-06-17DOI: 10.1021/acsenergylett.5c01329
Xinzhe Xue, Yat Li
Electrolytic MnO2 batteries based on a two-electron-transfer Mn2+/MnO2 conversion reaction have been attracting growing research interests for large-scale applications due to high voltage and high capacity. However, the low Mn2+/MnO2 conversion efficiency caused by incomplete MnO2 dissolution hinders its practical applications. Recently, redox mediation chemistry has been introduced to improve Mn2+/MnO2 conversion capacity by orders of magnitude. However, as an emerging key strategy, the complex solid–liquid conversion mechanism, the interactions between the redox mediator and the Mn-based species, and the influence of the interfacial environment remain poorly understood. This perspective article aims to discuss critical evaluation criteria, outline key research directions, and summarize relevant characterization methods for redox mediation chemistry in Mn2+/MnO2 conversion. Several future focuses on design principles for high-energy Mn-based cathode materials are proposed. We hope to use a Mn2+/MnO2 system as a model platform to deepen scientific understanding of redox-mediated conversion reactions and inspire broader research in this field.
{"title":"Advancing Mn2+/MnO2 Conversion Chemistry through Redox Mediation: Mechanistic Insights and Outlook","authors":"Xinzhe Xue, Yat Li","doi":"10.1021/acsenergylett.5c01329","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01329","url":null,"abstract":"Electrolytic MnO<sub>2</sub> batteries based on a two-electron-transfer Mn<sup>2+</sup>/MnO<sub>2</sub> conversion reaction have been attracting growing research interests for large-scale applications due to high voltage and high capacity. However, the low Mn<sup>2+</sup>/MnO<sub>2</sub> conversion efficiency caused by incomplete MnO<sub>2</sub> dissolution hinders its practical applications. Recently, redox mediation chemistry has been introduced to improve Mn<sup>2+</sup>/MnO<sub>2</sub> conversion capacity by orders of magnitude. However, as an emerging key strategy, the complex solid–liquid conversion mechanism, the interactions between the redox mediator and the Mn-based species, and the influence of the interfacial environment remain poorly understood. This perspective article aims to discuss critical evaluation criteria, outline key research directions, and summarize relevant characterization methods for redox mediation chemistry in Mn<sup>2+</sup>/MnO<sub>2</sub> conversion. Several future focuses on design principles for high-energy Mn-based cathode materials are proposed. We hope to use a Mn<sup>2+</sup>/MnO<sub>2</sub> system as a model platform to deepen scientific understanding of redox-mediated conversion reactions and inspire broader research in this field.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"34 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144305226","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}
Pub Date : 2025-06-17DOI: 10.1021/acsenergylett.5c00960
Ting Xiong, Yaoxin Zhang, Wee Siang Vincent Lee
Aqueous zinc ion batteries (ZIBs) have garnered substantial research interest owing to their utilization of aqueous electrolytes, high theoretical zinc capacity, economically viable and widely accessible zinc resources, and ease of material handling. However, several challenges remain, such as low capacity, unsatisfactory energy density, and poor stability, which necessitate further research. Recently, defective engineering has emerged as a promising strategy in the development of ZIBs. This Review highlights the recent advancements in employing defective engineering toward high performing aqueous ZIBs, detailing its implications on various cathode, anode, electrolyte additives, current collectors, and separators. We will also discuss methodologies to incorporate defects and elucidate the underlying mechanisms by which defective engineering enhances battery performance. Furthermore, we outline future research directions of defective engineering in the development of aqueous zinc ion batteries.
{"title":"Defective Engineering As a Promising Strategy for Advanced Aqueous Zn Ion Batteries","authors":"Ting Xiong, Yaoxin Zhang, Wee Siang Vincent Lee","doi":"10.1021/acsenergylett.5c00960","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00960","url":null,"abstract":"Aqueous zinc ion batteries (ZIBs) have garnered substantial research interest owing to their utilization of aqueous electrolytes, high theoretical zinc capacity, economically viable and widely accessible zinc resources, and ease of material handling. However, several challenges remain, such as low capacity, unsatisfactory energy density, and poor stability, which necessitate further research. Recently, defective engineering has emerged as a promising strategy in the development of ZIBs. This Review highlights the recent advancements in employing defective engineering toward high performing aqueous ZIBs, detailing its implications on various cathode, anode, electrolyte additives, current collectors, and separators. We will also discuss methodologies to incorporate defects and elucidate the underlying mechanisms by which defective engineering enhances battery performance. Furthermore, we outline future research directions of defective engineering in the development of aqueous zinc ion batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144311891","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}
Pub Date : 2025-06-16DOI: 10.1021/acsenergylett.5c01012
Jinxu Qiu, Hongliang Li, Tao Wu, Yaxuan He, Rongrui Xu, Yuezhen Hua, Yu Zhao, Jie Shu, Keyu Xie, Yanhua Cui
The growing trend of unmanned monitoring and the widespread popularity of intelligent automation necessitate higher energy storage for self-powered microbatteries. All-solid-state thin-film lithium batteries offer significant advantages in size and integration but are still subject to their low-voltage plateau (<3.3 V) and microampere-level capacity (≤0.2 mWh). Herein, we proposed the crystal-facet engineering combined with the substrate anchoring effect to address critical structure variation in the 4.6 V LiCoO2 film. The rotated (003) basal plane effectively relieves internal stress and the Li+ migration energy barrier, contributing to strengthened continuous migration channels and a structure skeleton in Nb2O5@LCO nanosheets. Therefore, the additive-free full cell exhibits excellent cyclability, retains 72.5% capacity retention over 500 cycles at 1.4 C between 3.0 and 4.6 V, and has a high energy density of 1.148 mWh cm–2 in a 3.5 cm2 thin-film cell. This study provides a prototype method for tailoring desired compatible thin film electrode materials for further on-chip microdevices.
{"title":"Construction of Longitudinal (003) Textured Low-Strain Diffusion Channel in 4.6 V LiCoO2-Based All-Solid-State Thin Film Battery for Microelectronic Systems","authors":"Jinxu Qiu, Hongliang Li, Tao Wu, Yaxuan He, Rongrui Xu, Yuezhen Hua, Yu Zhao, Jie Shu, Keyu Xie, Yanhua Cui","doi":"10.1021/acsenergylett.5c01012","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01012","url":null,"abstract":"The growing trend of unmanned monitoring and the widespread popularity of intelligent automation necessitate higher energy storage for self-powered microbatteries. All-solid-state thin-film lithium batteries offer significant advantages in size and integration but are still subject to their low-voltage plateau (<3.3 V) and microampere-level capacity (≤0.2 mWh). Herein, we proposed the crystal-facet engineering combined with the substrate anchoring effect to address critical structure variation in the 4.6 V LiCoO<sub>2</sub> film. The rotated (003) basal plane effectively relieves internal stress and the Li<sup>+</sup> migration energy barrier, contributing to strengthened continuous migration channels and a structure skeleton in Nb<sub>2</sub>O<sub>5</sub>@LCO nanosheets. Therefore, the additive-free full cell exhibits excellent cyclability, retains 72.5% capacity retention over 500 cycles at 1.4 C between 3.0 and 4.6 V, and has a high energy density of 1.148 mWh cm<sup>–2</sup> in a 3.5 cm<sup>2</sup> thin-film cell. This study provides a prototype method for tailoring desired compatible thin film electrode materials for further on-chip microdevices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"66 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144305227","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}
Pub Date : 2025-06-16DOI: 10.1021/acsenergylett.5c01446
Mehran Arzani, Hamidreza Mahdavi, Vikas Berry
Beyond traditional electrolytes, innovative electrolytes with molecular porosity to selectively embed ions can provide a protective shield to increase their mobility for enhanced battery efficiency. The molecular structure of these porous liquid-based electrolytes (PLEs) can be designed to provide permanent, empty, and selective porous media. In this Perspective, we show the potential and design principles of porous liquids (PLs) that can enable their incorporation into all ion batteries. The porous structure of PLs increases their surface area exposure to ions for their selective shielding from dendrite formation, enhancing their mobility/conductivity, thus also addressing challenges with thermal instability and safety risks associated with conventional electrolytes. This work proposes a roadmap for PLE development, emphasizing molecular design, target mechanisms, and computational studies aligned with specific battery chemistries to enhance the energy density and extended cycle life.
{"title":"Engineering Porous Liquids for Enhanced Ion Mobility and Stable Battery Electrolytes","authors":"Mehran Arzani, Hamidreza Mahdavi, Vikas Berry","doi":"10.1021/acsenergylett.5c01446","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01446","url":null,"abstract":"Beyond traditional electrolytes, innovative electrolytes with molecular porosity to selectively embed ions can provide a protective shield to increase their mobility for enhanced battery efficiency. The molecular structure of these porous liquid-based electrolytes (PLEs) can be designed to provide permanent, empty, and selective porous media. In this Perspective, we show the potential and design principles of porous liquids (PLs) that can enable their incorporation into all ion batteries. The porous structure of PLs increases their surface area exposure to ions for their selective shielding from dendrite formation, enhancing their mobility/conductivity, thus also addressing challenges with thermal instability and safety risks associated with conventional electrolytes. This work proposes a roadmap for PLE development, emphasizing molecular design, target mechanisms, and computational studies aligned with specific battery chemistries to enhance the energy density and extended cycle life.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"14 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144305229","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}
Pub Date : 2025-06-16DOI: 10.1021/acsenergylett.5c01269
Kousik Das, J. Niklas Hausmann, Matthias Driess, Prashanth W. Menezes
Figure 1. a) A chart showing the distribution of different reference electrode calibration processes from 2014 to 2023 (Web of science). b) The range of calibration values for Hg/Hg<sub>2</sub>Cl<sub>2</sub>, Ag/AgCl and Hg/HgO reference electrodes in 0.1 and 1 M KOH solution obtained from the literature. The values represent the total range of calibration values observed for the same reference electrode in the same measuring solution. The experimental calibration values and the corresponding literature are tabulated in Tables S1–S3. Figure 2. a) The change in measured potential of a 1 M KOH solution with time in the open air. The potentials were measured with a Hg/HgO electrode containing 1 M NaOH solution against a Gaskatel Hydroflex RHE electrode. b) Calibration potential of Hg/HgO reference electrode (1 M NaOH internal solution) measured against Pt/H<sub>2</sub> electrode under different H<sub>2</sub> flow. All measurements were conducted with stirring except the black line. The measurements for the blue and black lines were performed under the same H<sub>2</sub> flow. c) Distribution of experimental calibration values for Hg/Hg<sub>2</sub>Cl<sub>2</sub>, Ag/AgCl and Hg/HgO reference electrodes in 1 M KOH and 0.1 M KOH solution. The literature calibration values and their corresponding references were tabulated in Tables S1–S3. Figure 3. Comparison of pH values obtained from different measurements and their corresponding error in potential for KOH solution. Figure 4. a) Comparison of calibration potential of a Hg/HgO reference electrode (1 M NaOH internal solution) obtained from the equation-based method and experiment-based method for KOH solution. b) Comparison of the calibration potential of a modified, liquid junction free Hg/HgO reference electrode obtained from the equation-based method and experiment-based method for KOH solution. The standard deviations in experiment-based measurements were determined from four independent measurements. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsenergylett.5c01269. Materials and methods, descriptive notes, tables (calibration potentials, KOH molality, hydroxide ion activity coefficient and water activity, potentials), and figures (experimental setup, change in measured potential, <sup>29</sup>Si NMR spectra, pH values, potentials) (PDF) Toward Reliable Reference Electrode Calibration In Alkaline Solution <span> 1 </span><span> views </span> <span> 0 </span><span> shares </span> <span> 0 </span><span> downloads </span> Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. M.D. headed the pro
图1所示。a) 2014年至2023年不同基准电极校准过程的分布图（Web of science）。b)从文献中得到的Hg/Hg2Cl2、Ag/AgCl和Hg/HgO参考电极在0.1和1m KOH溶液中的校准值范围。这些值表示在相同的测量溶液中对相同的参比电极观察到的校准值的总范围。实验标定值及相关文献见表S1-S3。图2。a) 1 M KOH溶液在露天中随时间的测量电位变化。用含有1 M NaOH溶液的Hg/HgO电极对Gaskatel Hydroflex RHE电极测量电位。b)不同H2流量下Hg/HgO参比电极（1m NaOH内溶液）对Pt/H2电极标定电位的测量。除黑线外，所有测量均在搅拌状态下进行。蓝线和黑线的测量是在相同的H2流量下进行的。c) Hg/Hg2Cl2、Ag/AgCl和Hg/HgO参比电极在1m KOH和0.1 M KOH溶液中的实验定标值分布。文献校正值及相应参考文献见表S1-S3。图3。比较不同测量得到的pH值及其相应的KOH溶液电位误差。图4。a) KOH溶液中基于方程法和基于实验法得到的Hg/HgO参比电极（1 M NaOH内溶液）标定电位的比较。b) KOH溶液中基于方程法和基于实验法得到的改进的无液结Hg/HgO参比电极标定电位的比较。基于实验的测量的标准差由四个独立的测量确定。支持信息可在https://pubs.acs.org/doi/10.1021/acsenergylett.5c01269免费获取。材料和方法，描述性注释，表格（校准电位，KOH摩尔浓度，氢氧根离子活度系数和水活度，电位），和数字（实验设置，测量电位的变化，29Si核磁共振光谱，pH值，电位）（PDF）迈向可靠的参考电极校准在碱性溶液1视图0共享0下载大多数电子支持信息文件是可用的，无需订阅ACS网络版。这些文件可以通过文章下载用于研究用途（如果相关文章有公共使用许可链接，该许可可以允许其他用途）。如有其他用途，可通过RightsLink权限系统http://pubs.acs.org/page/copyright/permissions.html向ACS申请。医学博士领导了这个项目。P.W.M.和M.D.设计了实验。K.D.做了所有的实验。K.D和J.N.H.在所有作者的意见下撰写了这份手稿。所有作者都认可了手稿的最终版本。本项目由德国卓越战略（EXC 2008/1-390540038 - UniSysCat）资助。J.N.H和P.W.M.感谢德国联邦教育和研究部在“Catlab”项目（03EW0015A/B）框架下的支持。本文引用了40个其他出版物。这篇文章尚未被其他出版物引用。
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