ACS Energy Letters 最新文献

{"title":"Regulating Solvation Shell to Fortify Anion–Cation Coordination for Enhanced Sodium Metal Battery Stability","authors":"Zhangbin Cheng, Zehui Zhang, Feilong Qiu, Zheng Gao, Haijiao Xie, Zhen Xu, Min Jia, Xiaoyu Zhang, Haoshen Zhou","doi":"10.1021/acsenergylett.4c02751","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02751","url":null,"abstract":"The use of sodium metal as an anode presents a promising avenue for high energy density sodium rechargeable batteries given its high specific capacity and low redox potential. However, sodium metal batteries (SMBs) encounter significant challenges, including interfacial parasitic reactions and dendrite growth. Developing a robust solid electrolyte interphase (SEI) is crucial for SMB engineering. This study introduces hydrofluoroether as a diluent in high-concentration electrolytes, effectively modifying the solvation structure to enhance ion-pair coordination, which leads to an inorganic-rich SEI, mitigating sodium depletion and dendrite formation. Consequently, localized high concentration electrolytes achieve a 98.3% Coulombic efficiency in Na||Cu batteries, while the Na||NaFe_1/3Ni_1/3Mn_1/3O₂ battery retains 86.4% capacity after 750 cycles at 1C. Additionally, the Na||Na₃V₂(PO₄)₃ battery achieves an exceptional average Coulombic efficiency of 99.97% at 1C, with a capacity retention of 95.4% after 517 days. This study provides a framework for enhancing efficiency and longevity in SMBs that can be applied to other battery systems.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832579","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":"Unlocking Charge Transfer Limitation toward Advanced Low-Temperature Sodium-Ion Batteries","authors":"Pengfei Zhou, Zhongjun Zhao, Junying Weng, Xiaozhong Wu, Jin Zhou, Zhihui Niu, Rui Feng, Xunzhu Zhou, Jia-Zhao Wang, Shixue Dou, Lin Li","doi":"10.1021/acsenergylett.4c02952","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02952","url":null,"abstract":"Sodium-ion batteries (SIBs) are recognized as promising large-scale energy storage systems but suffer from sluggish kinetics at low temperatures. Herein, we proposed a carbon nanotubes-modified P2-Na_0.67Mn_0.67Ni_0.33O₂ (NMNO-CNTs) cathode and tetrahydrofuran (THF)-containing dimethyl-based electrolyte to unlock the charge transfer limitation of SIBs at low temperatures. A highly conductive network constructed by CNTs ensures fast surface electron transfer. The introduction of THF enables an anion-rich solvation structure, which facilitates the formation of a robust NaF-rich electrode–electrolyte interface with accelerated desolvation and uniform Na deposition. As a result, the Na||NMNO-CNTs cell delivers a capacity of 83.4 mAh g^–1 even after 3600 cycles with a decay rate of 0.002% per cycle at −40 °C. More importantly, the hard carbon||NMNO-CNTs full cell exhibits an energy density of 237.6 Wh kg^–1 with 86.5% retention after 1500 cycles at −40 °C. The work highlights the key role of charge transfer kinetics for advanced low-temperature SIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"244 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142832581","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":"Imaging Ultrafast Charge Transfer at Low-Dimensional Lead Halide Perovskite Heterostructures","authors":"Fabiola Faini, Yaiza Asensio, Federico Visentin, Lucía Olano-Vegas, Martin Hörmann, Luis E. Hueso, Giulio Cerullo, Franco V. A. Camargo, Beatriz Martín-García, Giulia Grancini","doi":"10.1021/acsenergylett.4c02786","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02786","url":null,"abstract":"Addressing interface physics and related photoinduced dynamics is crucial to understand charge carrier paths and losses and ultimately design efficient optoelectronic devices. However, such dynamics are often masked when bulky systems are investigated. In this work, we combine photoluminescence with ultrafast transient absorption microscopy to map charge transfer processes in few-layers-thick heterostructures made of low-dimensional (C₆H₅CH₂CH₂NH₃)₂(CH₃NH₃)_n-1Pb_nI_3n+1 perovskite flakes of different dimensionalities (<i>n</i> = 3) and (<i>n</i> = 1). We observe that the hole transfer process from the (<i>n</i> = 3) to the (<i>n</i> = 1) phase happens after exciton diffusion on a time scale of tens of picoseconds, whereas electron transfer is hindered by the high exciton binding energy and low diffusion coefficient within the (<i>n</i> = 1) phase. This study sets the stage for a deeper understanding needed for the smart development of new heterostructure combinations with different dimensionalities and band alignments.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"3 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816397","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":"Making Na-Ion Batteries Solid","authors":"Yong-Sheng Hu*,&nbsp; and ,&nbsp;Fei Xie*,&nbsp;","doi":"10.1021/acsenergylett.4c0323010.1021/acsenergylett.4c03230","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03230https://doi.org/10.1021/acsenergylett.4c03230","url":null,"abstract":"","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"9 12","pages":"6081–6083 6081–6083"},"PeriodicalIF":19.3,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850179","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":"Electrochemical Ammonia Synthesis: The Energy Efficiency Challenge","authors":"Yuanyuan Zhou, Xianbiao Fu, Ib Chorkendorff, Jens K. Nørskov","doi":"10.1021/acsenergylett.4c02954","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02954","url":null,"abstract":"We discuss the challenges associated with achieving high energy efficiency in electrochemical ammonia synthesis at near-ambient conditions. The current Li-mediated process has a theoretical maximum energy efficiency of ∼28%, since Li deposition gives rise to a very large effective overpotential. As a starting point toward finding electrocatalysts with lower effective overpotentials, we show that one reason why Li and alkaline earth metals work as N₂ reduction electrocatalysts at ambient conditions is that the thermal elemental processes, N₂ dissociation and NH₃ desorption, are both facile at room temperature for these metals. Many transition metals, which have less negative reduction potentials and thus lower effective overpotentials, can dissociate N₂ at these conditions but they all bind NH₃ too strongly. Strategies to circumvent this problem are discussed, as are the other requirements for a good N₂ reduction electrocatalyst.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"7 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816409","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":"Unleashing High Yield Urea Production by Pulse Electrodeposition of Bi/Cu via Co-reduction of N2 and CO2","authors":"Sukhjot Kaur, Kalpana Garg, Divyani Gupta, Alankar Kafle, Dharmender, Vivekanand Shukla, Rajeev Ahuja, Tharamani C. Nagaiah","doi":"10.1021/acsenergylett.4c02823","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02823","url":null,"abstract":"The expanding agricultural practices rely on carbon- and energy-intensive Bosch–Meiser processes for urea synthesis. Alternatively, electrochemical coupling of CO₂ and N₂ is emerging as a sustainable approach. Unfortunately, the high energy barrier for N₂ and CO₂ cracking for C–N bond coupling limits the urea synthesis efficiency. Herein, we have electrodeposited Bi on Cu foil <i>via</i> triple pulse voltage, and the fabricated Bi(0.01 V)@Cu electrode demonstrates a high yield rate of 646 μg h^–1 mg^–1_cat. of urea with 70.7% Faradaic efficiency at −0.45 V <i>vs</i> RHE. The isotopic labeling experiments assert that the produced urea is solely from the dissolved CO₂ and N₂ gases. More importantly, we have utilized <i>in situ</i> electrochemical Raman spectroscopy and Fourier transform infrared (FTIR) measurements to monitor the real-time formation of urea, further supported by a microelectrochemical approach using a Pt-microelectrode and the results were verified by density functional theory (DFT) analysis. Moving a step forward, plant growth and flowering upon addition of extracted urea have been demonstrated for practical application.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"10 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816400","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":"Making Na-Ion Batteries Solid","authors":"Yong-Sheng Hu, Fei Xie","doi":"10.1021/acsenergylett.4c03230","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03230","url":null,"abstract":"Along with the rapid increase of market penetration rate of electric vehicles (EVs) and the continuous increase in the capacity of installed energy storage systems (ESSs), problems associated with limited and unevenly distributed Li resources are becoming prominent with Li-ion batteries (LIBs) serving as the supporting technology. As an alternative, Na-ion batteries (NIBs) have been widely accepted as an effective new route to supplement the market, especially in the field of energy storage. (1−4) Owing to the great efforts and contributions from various groups over the world, NIBs are now stepping into commercialization with a bright future. In 2024, the first NIB energy storage systems, one with a capacity of 10 MWh (5) in Guangxi province and another with 100 MWh (6) in Hubei province, China, were successfully launched. (Figure 1). Figure 1. (a) 10 MWh and (b) 100 MWh Na-ion battery energy storage systems. Although NIBs are developing steadily and rapidly, thanks to the analogies in their principles and fabrication with LIBs, achieving even higher energy density, longer cycle life, and better safety is critical for the ESS applications. Therefore, a transition from liquid-state to solid-state NIBs is significant and necessary. Solid-state NIBs have some unique advantages compared to liquid-state batteries: 1) inorganic solid electrolytes ensure inherent nonflammability, which highly enhances the safety; 2) solid electrolytes show higher oxidation potential than many organic liquid electrolytes, promising a higher working voltage and energy density; and 3) due to the fluidity of liquid electrolytes, some side reactions continuously occur at the electrode–electrolyte interface during cycling, but when using solid electrolytes, interfacial side reactions can be impeded, and much longer lifespan is expected; and 4) again due to the fluidity of liquid electrolytes, it is easy for short-circuits to occur in the bipolar configuration, however because only aluminum foils are used as current collectors at both the cathode and anode sides, NIBs can be assembled as bipolar cells for higher voltage and energy density. Solid electrolytes make the fabrication of bipolar cells feasible and deliver better performance and lower cost. The key for the development of solid-state NIBs is the solid electrolyte material, which should possess high enough ionic conductivity and flexibility with proper contact with the electrodes to adapt to the strain and guarantee fast Na&lt;sup&gt;+&lt;/sup&gt; diffusion in the bulk and at the interface. Currently, similar to the case with solid-state LIBs, organic solid electrolytes, represented by polymers, and inorganic electrolytes, including oxides, sulfides, and halides, are the most studied types in NIB research. Polymer electrolytes usually have pliable properties with a deformable interface that can keep excellent contact between the electrode and electrolyte, but their room-temperature ionic conductivities require further increase. Ox","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"29 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816402","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":"A Conversation with Ib Chorkendorff","authors":"Prashant V. Kamat","doi":"10.1021/acsenergylett.4c03085","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c03085","url":null,"abstract":"Prof. Ib Chorkendorff is a Professor in the Department of Physics at Danmarks Tekniske Universitet (DTU). His initial research interest focused on surface reactivity of heterogeneous catalysts, and later expanded to include electrocatalysis and photoelectrocatalysis for energy harvesting and conversion. Notably, his seminal contributions to the fundamental understanding of CO&lt;sub&gt;2&lt;/sub&gt; and N&lt;sub&gt;2&lt;/sub&gt; reduction have led to new advances in designing electrocatalytic systems for sustainable fuels. He remains a leading advocate for reducing our carbon footprint through the development of sustainable fuels. The Department of Physics at DTU has been organizing a summer school for students and young researchers for the last two decades. (1) During my recent participation in the 2024 &lt;i&gt;SurfCat&lt;/i&gt; Summer School (Figure 1), I had the opportunity to converse with Prof. Ib Chorkendorff. Figure 1. During a discussion with Ib Chorkendorff at the 2024 &lt;i&gt;SurfCat&lt;/i&gt; Summer School, Kobaek Strand, Denmark. (Photo Courtesy: P. Kamat) &lt;i&gt;PK: What were the early motivations that led you to get interested in electrocatalysis research?&lt;/i&gt; IC: From a young age, I was deeply interested in energy and energy conversion. This interest dates back to my high school days in the 1970s in Denmark, when car-free Sundays were introduced due to gasoline and oil shortages─an energy vulnerability that left a lasting impression on me. During my studies, I specialized in surface science, though without focusing specifically on energy, as the crisis had subsided for the time being. While working on my master’s degree, I had the opportunity to spend six months at Haldor Topsoe A/S, a Danish catalyst manufacturer. This experience helped me realize what I wanted to pursue as a career. After completing my Ph.D. in surface science of rare earth metals and their alloys, I did my postdoctoral work with John Yates at the University of Pittsburgh, where I earned experience on surface reactions and catalysis. In the early part of my career, I focused on single-crystal surface reactions and thermal catalysis, supported by collaborations with Haldor Topsoe, who encouraged more rigorous teaching of these subjects at DTU. By the turn of the century, I returned to my passion for energy, initiating a project called “Towards a Hydrogen Society”, where fuel cells were seen as an efficient energy source. Initially, electrochemistry held little appeal for me, as I associated it mainly with corrosion of automobiles and electroplating, both of which I found uninteresting. However, from an energy perspective, new possibilities opened up, and I began exploring fundamental single-crystal studies, fuel cells, and eventually photoelectrocatalysis. In recent years, my work has focused on energy conversion─particularly water splitting─and the challenge of coupling protons directly to CO&lt;sub&gt;2&lt;/sub&gt; or N&lt;sub&gt;2&lt;/sub&gt; to produce chemicals and fuels. My approach has generally been based on my background in sur","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"13 2 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816401","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":"Your Best Single-Junction Solar Cell Does Not Always Make an Efficient Tandem Partner","authors":"Lorelle M. Mansfield, Jacob J. Cordell, Sirazul Haque, William E. McMahon, Emily L. Warren","doi":"10.1021/acsenergylett.4c02706","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02706","url":null,"abstract":"Tandem solar cells, where multiple single-junction cells are combined optically in series, provide a path to making cells with high areal efficiencies, with multiple material systems capable of achieving greater than 30% efficiency under 1-sun conditions. However, there are many different material combinations and configurations used to make a tandem, and it can be challenging to understand how advances in one material system will impact the performance of a tandem device. We have built an open-source calculator based on the spectral efficiency metric proposed by Yu et al. to easily enable calculation of spectral efficiency for single junctions and predicted maximum efficiency of tandem pairs, accounting for different optical and electrical coupling between the top and bottom junctions.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"42 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816347","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":"Emerging Trends and Future Opportunities for Battery Recycling","authors":"Jarom G. Sederholm, Lin Li, Zheng Liu, Kai-Wei Lan, En Ju Cho, Yashraj Gurumukhi, Mohammed Jubair Dipto, Alexander Ahmari, Jin Yu, Megan Haynes, Nenad Miljkovic, Nicola H. Perry, Pingfeng Wang, Paul V. Braun, Marta C. Hatzell","doi":"10.1021/acsenergylett.4c02198","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02198","url":null,"abstract":"The global lithium-ion battery recycling capacity needs to increase by a factor of 50 in the next decade to meet the projected adoption of electric vehicles. During this expansion of recycling capacity, it is unclear which technologies are most appropriate to reduce costs and environmental impacts. Here, we describe the current and future recycling capacity situation and summarize methods for quantifying costs and environmental impacts of battery recycling methods with a focus on cathode active materials. Second use, electrification of pyrometallurgy and hydrometallurgy, direct recycling, and electrochemical recycling methods are discussed as leading-edge methods for overcoming state of the art battery recycling challenges. The paper ends with a discussion of future issues and considerations regarding solid-state batteries and co-optimization of battery design for recycling.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"29 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-12-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142815980","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}