ACS Energy Letters 最新文献

{"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 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.","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}

{"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 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.","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}

{"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}

{"title":"Toward Reliable Reference Electrode Calibration In Alkaline Solution","authors":"Kousik Das, J. Niklas Hausmann, Matthias Driess, Prashanth W. Menezes","doi":"10.1021/acsenergylett.5c01269","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01269","url":null,"abstract":"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\u0000Reference Electrode Calibration In\u0000Alkaline 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","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"70 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144305228","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}

{"title":"Upcycling of Air-Degraded Ni-Rich Cathodes via In Situ Surface Reconstruction","authors":"Mengshan Xu, Mei Zhao, Min Hong, Mengting Zheng, Jianwei Nai, Xinyong Tao, Tiefeng Liu","doi":"10.1021/acsenergylett.5c00581","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c00581","url":null,"abstract":"Ni-rich cathodes are well-known for their high specific capacity but require extremely dry conditions for prolonged storage due to their inherent sensitivity to tiny amounts of moisture in the atmosphere. Once LiOH/Li₂CO₃ is formed from exposure to moisture on the cathode surface, these impurities unavoidably obstruct Li insertion into/extraction out of bulk electrodes and simultaneously cause a further loss of the active Li source. In this work, we propose to convert the LiOH/Li₂CO₃ layer on spent NCM82 particles (S-NCM82) into a high-kinetic Li₃PO₄/LiF interphase via a simple phosphide reaction in aqueous LiPO₂F₂ solution. Meanwhile, such a conformal interphase prevents side reactions with electrolytes and alleviates structural strain during the service. The regenerated NCM82 electrode (R-NCM82) demonstrates a high specific capacity of 102 mAh/g at 5C, surpassing the 79 mAh/g observed in the pristine NCM82 (P-NCM82). Additionally, the R-NCM82//Gr full-cell exhibits 76% of its initial capacity after 300 cycles at 1C. This conversion process is easily scalable and could inspire the development of upcycling techniques for regenerating various spent electrodes.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"25 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278766","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}

{"title":"Photoelectrochemical Solar Fuels: What’s Next?","authors":"Kevin Sivula","doi":"10.1021/acsenergylett.5c01404","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01404","url":null,"abstract":"Figure 1. Abstract illustration of a PEC cell. Text-to-image generation from Microsoft Bing image creator was used, in part, to create this image. Figure 2. Simplified schematics of some typical semiconductor electrode architectures: (a) classic n-type semiconductor photoanode, (b) cocatalyst decorated photoanode, (c) a protected photoelectrode with a wide band gap semiconductor overlayer, and (d) a heterojunction photoanode. Electrode structures with continuous metal overlayers (with a work function Φ_M that controls the band bending/photopotential in the semiconductor) are also shown: (e) Schottky junction-biased electrode and (f) PV-biased electrode. This article references 14 other publications. Early View Article. This article has not yet been cited by other publications.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"27 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278772","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}

{"title":"Crack-Engineered Microporous Layer for Mitigating Cathode Flooding in Polymer Electrolyte Fuel Cells","authors":"Young Je Park, Won Young Choi, Seong Hyun Park, Hyunguk Choi, Seo Won Choi, Jy-Young Jyoung, Eunsook Lee, Jae-ll Park, Min Jae Ko, Kang Taek Lee, Chi-Young Jung","doi":"10.1021/acsenergylett.5c01202","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01202","url":null,"abstract":"Crack engineering within the microporous layer (MPL) of the gas diffusion layer (GDL) has emerged as a promising strategy to alleviate severe cathode flooding in polymer electrolyte fuel cells (PEFCs), especially under high current operation. Here, we report a connected-crack MPL architecture that forms continuous liquid water highways, extending from the catalyst layer (CL) to the GDL backing layer, effectively separating the liquid/gas transport. Three-dimensional reconstruction using X-ray computed tomography reveals that the microengineered cracks significantly reduce flooding at the CL-MPL interface by providing efficient drainage. Compared to the noncrack GDL, the connected-crack GDL (C-GDL) exhibits 20% higher peak power density of 1.23 W cm^–2. Pore-scale simulations further validate the antiflooding capabilities of C-GDL, showing a 25-fold enhancement in water removal. This crack-engineered GDL thus offers an efficient and scalable route to water management challenges, enabling robust and high-performance PEFCs suitable for heavy-duty vehicle electrification.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"12 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278768","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}

{"title":"Electrochromic Harvester for All-Day Energy Savings in Buildings","authors":"Wenhao Wang, Long Wang, Shenghao Jin, Tao Xie, Gu Liu, Zhen Meng, Tonghao Liu, Yina Cui, Haoyuan Zhang, Weiguo Liu, Zhenyi Gao, Boxiang Wang, Liuying Wang","doi":"10.1021/acsenergylett.5c01153","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01153","url":null,"abstract":"Technologies that can simultaneously capture energy from outer space and the sun have garnered extensive interest in recent years. However, the utilization of these two energy sources is challenged by their conflicting spectral requirements, making it difficult to capture both in a single device or material. Here, an adaptive energy harvester coupling photothermal conversion and radiative cooling utilizing photonic metastructure electrodes in conjunction with reversible metal electrodeposition technology for all-day continuous energy harnessing is reported. The harvester demonstrates sustained bistability for over 30 days with large emissivity contrast (0.82 at 3–5 μm, 0.66 at 7.5–13 μm), robust environmental durability, and scalability (100 cm²) for switching between heating and cooling states. World-wide energy simulations show that it can significantly reduce energy consumption in buildings by up to 21.4%, amounting to a savings of 95.8 GJ year-round. This harvester offers a promising method to utilize heat source and heat sink, sun and outer space, to improve sustainability and reduce carbon foot print of the Earth.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278767","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}

{"title":"Photoelectrochemical Solar Fuels: What’s Next?","authors":"Kevin Sivula*, ","doi":"10.1021/acsenergylett.5c0140410.1021/acsenergylett.5c01404","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01404https://doi.org/10.1021/acsenergylett.5c01404","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 6","pages":"2877–2879 2877–2879"},"PeriodicalIF":19.3,"publicationDate":"2025-06-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144269565","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}

{"title":"Electroswitchable Noble-Metal-Free Catalysis for Molecular Solar Thermal Systems","authors":"Evanie Franz, Georg Fickenscher, Erik J. Schulze, Daniel Krappmann, Anna Weidlich, Tobias Luchs, Andreas Dreuw, Andreas Hirsch, Olaf Brummel, Jörg Libuda","doi":"10.1021/acsenergylett.5c01341","DOIUrl":"https://doi.org/10.1021/acsenergylett.5c01341","url":null,"abstract":"Molecular solar thermal (MOST) systems convert solar energy into chemical energy via a simple unimolecular reaction, enabling efficient energy storage. However, controlling the energy release remains a challenge. Here, we present an electroswitchable, noble-metal-free hybrid catalyst that enables energy release with high activity and selectivity. The MOST system is <i>p</i>-methoxyphenyl-ethyl ester-norbornadiene (mPENBD), which is photoconverted to its energy-rich quadricyclane isomer (mPEQC). A Co^II porphyrin derivative, anchored as a self-assembled monolayer (SAM) on an atomically defined Co₃O₄(111) electrode, catalyzes the back-conversion of mPEQC to mPENBD with exceptional selectivity. Over 100 cycles, no side products were detected, and only minimal deactivation occurred. Most importantly, catalytic activity can be switched on and off via electrode potential due to the reversible conversion between an active Co^II porphyrin SAM and an inactive Co^I porphyrin SAM. This electroswitchable catalyst enables precise control of energy release in MOST-based solar energy storage systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"223 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144278769","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}