ACS Energy Letters 最新文献

{"title":"A Safe Electrolyte Enriched with Flame-Retardant Solvents for High-Voltage LiCoO2||Graphite Pouch Cells","authors":"Chao Yang, Xing Zhou, Ruitao Sun, Wenxi Hu, Meilong Wang, Xiaoli Dong, Nan Piao, Jin Han, Wen Chen, Ya You","doi":"10.1021/acsenergylett.4c02466","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02466","url":null,"abstract":"Employing a flame-retardant solvent (FRS) in the electrolyte has shown great potential for improving the safety of lithium-ion batteries (LIBs). Nevertheless, their poor compatibility with salts and commonly used solvents leads to the formation of a heterogeneous system, which drastically limits their concentration in the electrolyte and consequently deteriorates the safety performance. In this work, we employ a bridging solvent diethyl carbonate to raise the solubility of a highly effective FRS, ethoxy pentafluorocyclotriphosphonitrile (PFPN), to a concentration as high as 75 vol % in the electrolyte. The target electrolyte forms a stable N/P-rich cathode–electrolyte interface to protect the electrode from oxygen evolution and transition-metal ion dissolution, thereby enabling the LiCoO₂ cathode to preserve 72% capacity retention over 500 cycles at 4.62 V. Moreover, this electrolyte can effectively delay occurrence time and improve the critical temperature of thermal runaway of 1 Ah LiCoO₂||graphite pouch cells. Our work proposes a new direction for nonflammable electrolytes toward safe and high-energy LIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"11 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448897","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":"Harnessing Vibrationally Assisted Delayed Fluorescence for Enhanced Energy Transfer in Mn-Doped CsPbBr3 Nanocrystals","authors":"Subham Das, Sudipa Aich, Aswathy M, Ranjani Viswanatha","doi":"10.1021/acsenergylett.4c02592","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02592","url":null,"abstract":"This study explores vibrationally assisted delayed fluorescence (VADF) in Mn-doped CsPbBr₃ nanocrystals using Förster resonance energy transfer (FRET). Mn doping enhances the FRET efficiency significantly due to an increase in host fluorescence efficiency, indicating an increase in the radiative pathways due to VADF. We observed that Mn facilitates efficient back-transfer of charge carriers, improving energy transfer to acceptor molecules such as Rhodamine 6G (R6G). The simplicity of tuning optical properties through Mn doping presents a promising method to enhance the energy efficiency in donor–acceptor systems for optoelectronic applications. However, further research on halide concentrations, acceptor molecules, and electron transfer mechanisms is necessary to optimize these systems for effective light energy harvesting.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"2 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448903","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":"Nonflammable Sulfone-Based Electrolytes with Mechanically and Thermally Stable Interfaces Enabling LiNi0.5Mn1.5O4 to Operate at High Temperature","authors":"Tian-Ling Chen, Mengting Liu, Xin-Yu Fan, Yi-Hu Feng, Qiang Liu, Xue-Ru Liu, Hanshen Xin, Peng-Fei Wang","doi":"10.1021/acsenergylett.4c02458","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02458","url":null,"abstract":"The development of high-energy 5 V-class LiNi_0.5Mn_1.5O₄ batteries is severely limited by the instability of the cathode electrolyte interphase (CEI) at high temperature. Herein, we propose a nonflammable sulfone (SL)-based fluorinated hybrid electrolyte to form stable, uniform, and thin CEI layers, enabling Li||LiNi_0.5Mn_1.5O₄ batteries to achieve elevated electrochemical performance at 60 °C. The formed highly stable inorganic-dominated CEI, comprising Li_<i>x</i>SO_<i>y</i>, Li_<i>x</i>BO_<i>y</i>, and LiF inorganic compositions, exhibits good thermal stability and mechanical strength. Moreover, the robust CEI layer effectively shields the LNMO particles from undesirable side-reactions and stabilizes the interface within the LiNi_0.5Mn_1.5O₄ cathode during high-temperature cycling. In contrast to the conventional electrolyte, the Li||LiNi_0.5Mn_1.5O₄ battery employing a nonflammable SL-based electrolyte exhibits a stable capacity retention of 88.5% after 100 cycles at 60 °C free from the risk of thermal runaway. This study reveals valuable insights into advanced electrolyte technology, paving the way for safer applications of Co-free high-energy batteries in the future.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"232 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142448171","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":"Controlling Intermediate Phase Formation to Enhance Photovoltaic Performance of Inverted FA-Based Perovskite Solar Cells","authors":"Chaohui Li, Hyoungwon Park, Shudi Qiu, Fabian Streller, Kaicheng Zhang, Zijian Peng, Jiwon Byun, Jingjing Tian, Santanu Maiti, Zhiqiang Xie, Lirong Dong, Chao Liu, Vincent M. Le Corre, Ying Shang, Jianchang Wu, Jiyun Zhang, Mingjie Feng, Andreas Späth, Karen Forberich, Andres Osvet, Thomas Heumueller, Silke H. Christiansen, Marcus Halik, Rainer H. Fink, Tobias Unruh, Ning Li, Larry Lüer, Christoph J. Brabec","doi":"10.1021/acsenergylett.4c02580","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02580","url":null,"abstract":"Formamidinium (FA)-based perovskites exhibit significant potential for highly efficient photovoltaics due to their promising optoelectronic properties and optimal bandgap. However, the undesired inactive phase arises from multiple crystal nucleation pathways formed by various intermediate phases during the film formation process, persistently accompanying it. FA-based perovskites frequently struggle to form uniform, highly crystalline films. This challenge complicates the development of reliable and highly reproducible crystallization processes for perovskites and the establishment of guidelines for controlling the α-phase formation. In this work, we investigate the role of poly(acrylonitril-<i>co</i>-methyl acrylate) (PAM) to simultaneously control nucleation and subsequent α-phase crystallization. This successfully demonstrates the regulation of oriented crystal growth through the creation of a PAM-PbI₂ intermediate. Ultimately, PAM-modified p–i–n architecture devices obtain a promising power conversion efficiency (PCE) of 25.30%, with <i>V</i>_OC (1.211 V), achieving 95% of the detailed balance limit. Additionally, PAM-modified devices maintain ≥90% of the initial efficiency for 1000 h under 1 sun and 65 °C operation.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"44 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444159","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":"Identifying the Critical Oxygenated Functional Groups on Graphene Oxide for Efficient Water Dissociation in Bipolar Membranes","authors":"Fanxu Meng, Jiangzhou Qin, Qinghao Wu, Huiwang Dai, Pan Zhu, Tian Tang, Lixia Zhang, Zishuai Bill Zhang, Kuichang Zuo","doi":"10.1021/acsenergylett.4c02677","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02677","url":null,"abstract":"Bipolar membranes (BPMs) are emerging options for kinetically accelerating water dissociation (WD) in electrochemical applications. Graphene oxide (GO) with abundant oxygenated functional groups is an efficient catalyst within BPMs to decrease the transmembrane potential. However, the dominant catalytic sites on GO for WD in BPMs have not been experimentally identified, and the reported simulative calculation results are controversial. Herein, we prepared carboxylated and partially hydroxylated GO-based BPMs, and for the first time quantitatively unraveled the correlativity between WD performance and carboxyl group content with tailor-designed experiments. By using a simple mechanical ball milling method, we further improved the bulk density of carboxyl on the GO catalyst, which achieved excellent WD performance during an operation of over 130 h operation. This study provides a subtle and facile strategy for catalyst design to advance BPM technologies.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"79 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444167","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":"Surface Defect Recovery in Perovskite Nanocrystals with Excess Halide for Core–Shell Structure","authors":"Dong Hyeon Lee, Woo Hyeon Jeong, Seokhyun Choung, Ji Won Jang, Gyudong Lee, Hochan Song, Sanghun Han, Gyeong Eun Seok, Jihoon Kim, Myeonggeun Han, Jeong Woo Han, Hyosung Choi, Jongmin Choi, Bo Ram Lee, Yong-Young Noh","doi":"10.1021/acsenergylett.4c01870","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01870","url":null,"abstract":"We present a method to synthesize stable and uniform high-quality perovskite nanocrystals (PNCs) by using excess halide to recover surface defects in CsPbBr₃/ZnS core/shell nanocrystals. Use of <i>N</i>-bromosuccinimide as a halide donor recovered surface halide vacancies of bare CsPbBr₃ PNCs during the growth of the ZnS shell, as confirmed by DFT calculations. This approach achieves a high photoluminescence quantum yield of nearly 1, and significantly increases the stability of PNCs under adverse conditions such as high humidity and elevated temperature. CsPbBr₃/ZnS PNC light-emitting diodes demonstrated outstanding luminous characteristics, with a remarkable external quantum efficiency of 12.77% and a maximum luminance of 1449 cd m^–2 at 517 nm. These characteristics of the PNCs will have a wide variety of applications and will help enable development of highly efficient optoelectronic devices.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"23 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440710","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":"Sequential Linker Installation in Metal–Organic Frameworks","authors":"Zongsu Han,&nbsp;Yihao Yang,&nbsp;Joshua Rushlow,&nbsp;Rong-Ran Liang and Hong-Cai Zhou*,&nbsp;","doi":"10.1021/acs.accounts.4c0056410.1021/acs.accounts.4c00564","DOIUrl":"https://doi.org/10.1021/acs.accounts.4c00564https://doi.org/10.1021/acs.accounts.4c00564","url":null,"abstract":"&lt;p &gt;Metal–organic frameworks (MOFs) represent a sophisticated blend of inorganic and organic components, promoting the development of coordination chemistry greatly and offering a versatile platform for tailored functionalities. By combining various metal nodes, organic linkers, and functional guests, MOFs provide numerous pathways for their design, synthesis, and customization. Among these, sequential linker installation (SLI) stands out as a novel and crucial strategy, enabling the precise integration of desired properties and functions at the atomic scale. SLI enhances structural diversity and stability while facilitating the meticulous construction of robust frameworks by leveraging open metal sites and functional organic linkers at targeted locations. Compared to the direct synthesis of MOFs, postsynthetic modification methods allow for precise regulation of their structures and corresponding properties. While unlike conventional postsynthetic modification methods, SLI requires the careful selection of linkers and framework design to ensure precise positioning for installation, which gives rise to the well-designed and ordered positions for the installed linkers, confirmed directly by X-ray diffraction technology.&lt;/p&gt;&lt;p &gt;Recent advancements in MOF synthesis have led to the creation of increasingly tailored flexible matrix structures, particularly due to the diverse connection modes of multicore metal clusters, especially for the Zr&lt;sub&gt;6&lt;/sub&gt; cluster. The spatial hindrance of certain ligands has resulted in the formation of unsaturated metal clusters and various missing linker pockets. Examples of these advanced MOFs include PCN-606, PCN-608, PCN-609, PCN-700, and PCN-808, which feature specific open metal sites and certain framework flexibility conducive to SLI. Strategically positioned open metal sites within these frameworks serve as predetermined anchor points for desired functional molecules, while the frameworks’ flexibility can accommodate molecules of varying sizes to a certain extent, enlarging the scopes of application greatly. This precise positioning of functional groups enables the creation of tailored sites for enhanced applications, such as adsorption, catalysis, and recognition.&lt;/p&gt;&lt;p &gt;In this Account, we delve into the intricate process of designing and synthesizing MOFs with appropriate missing-linker pockets for the aforementioned applications. We discuss the meticulous selection of functional linkers and the methods used to insert them into the corresponding missing-linker pockets within the MOFs. Additionally, we explore the diverse properties and functionalities of the resulting MOFs, focusing on their adsorptive, catalytic, and recognition performance. Furthermore, we provide insights into the future trajectory of SLI methods, complemented by our recent works. This Account not only reviews the evolution of the SLI method but also underscores its practical applications across various functional domains, paving a ration","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"57 21","pages":"3217–3226 3217–3226"},"PeriodicalIF":16.4,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.accounts.4c00564","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142577580","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Research Trends and Future Perspectives on Zn-Ion Batteries Using Ga-Based Liquid Metal Coatings on Zn Anodes","authors":"Seungwoo Hong, Zungsun Choi, Byungil Hwang, Aleksandar Matic","doi":"10.1021/acsenergylett.4c02191","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02191","url":null,"abstract":"Zn-ion batteries (ZIBs) are considered promising alternatives to conventional Li-ion secondary batteries due to their high safety, environmental friendliness, and cost-effectiveness. Despite these advantages, uneven metal plating and stripping, dendrite formation, and passivation and corrosion owing to the hydrogen evolution reaction (HER) have hindered the practical implementation of ZIBs. A promising route for overcoming these problems involves coating the Zn anode with eutectic gallium indium (EGaIn)-based liquid metal (LM) with a strong Zn affinity and growth direction tenability. Despite considerable research on EGaIn-coated Zn anodes for ZIBs, this topic has not been comprehensively reviewed. Hence, this Review introduces the application of LMs to ZIBs and particularly discusses the mitigation of stability issues using LM and the fundamental processes related to Zn anodes. We summarize the progress in this field and suggest promising future research directions to advance ZIBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"40 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142440657","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":"Solvation Sheath Reorganization by Alkyl Chain Tuning Promises Lean-Electrolyte Li–S Batteries","authors":"Zixiong Shi, Simil Thomas, Dong Guo, Zhengnan Tian, Zhiming Zhao, Yizhou Wang, Abdul-Hamid Emwas, Nimer Wehbe, Georgian Melinte, Osman M. Bakr, Omar F. Mohammed, Husam N. Alshareef","doi":"10.1021/acsenergylett.4c02049","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02049","url":null,"abstract":"Sparsely solvating electrolyte (SSE), which can achieve a quasi-solid-phase sulfur reaction path, stands out as a promising strategy to alleviate the dependence on electrolyte usage and construct lean-electrolyte lithium–sulfur (Li–S) batteries. Nonetheless, its formation relies upon a high dosage of salt and diluent, thereby leading to increased electrolyte cost. To this end, we herein customize a localized SSE (LSSE) featuring a low ratio of salt-to-solvent and diluent-to-solvent through alkyl chain tuning. A multimodal 2D nuclear magnetic resonance technique is developed to unveil the Li-ion solvation sheath reorganization, which is crucial for studying the coordination and dynamics in liquid electrolytes. LSSE affords an anion-derived solid electrolyte interface and effective restriction of the shuttling effect; hence, our Li–S batteries can sustain a steady operation under 4 μL mg_S^–1 and 3 mg cm^–2. Our work opens a new avenue for advancing SSE design in the pursuit of pragmatic lean-electrolyte Li–S batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"21 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142436367","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":"Dual-Function ZnO-Li3TaO4 Surface Modification of Single-Crystalline Ni-Rich Cathodes for All-Solid-State Batteries","authors":"Jun Pyo Son, Jae-Seung Kim, Chang-Gi Lee, Juhyoun Park, Jong Seok Kim, Se-Ho Kim, Baptiste Gault, Dong-Hwa Seo, Yoon Seok Jung","doi":"10.1021/acsenergylett.4c02016","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c02016","url":null,"abstract":"Herein, we introduce a ZnO–Li₃TaO₄ composite coating designed to stabilize single-crystalline LiNi_0.95Co_0.03Mn_0.015Al_0.005O₂ (sNCMA) in ASSBs with Li₆PS₅Cl. This dual-function coating establishes a Ta-rich surface layer and Zn-doped near-surface regions, as verified by detailed analyses, including atom probe tomography and transmission electron microscopy. The ZnO-Li₃TaO₄ coating markedly enhances both interfacial and structural stabilities, showcasing an exceptional performance in sNCMA|Li₆PS₅Cl|(Li–In) cells at 30 °C (initial discharge capacity of 196 mA h g^–1 with 82.7% capacity retention after 1000 cycles), exceeding the performance of both uncoated or only Li₃TaO₄-coated sNCMA (only 82.5 or 84.2%, respectively, after 200 cycles). The protective role of ZnO-Li₃TaO₄ is corroborated by electrochemical impedance spectroscopy and ex situ X-ray photoelectron spectroscopy. Finally, density functional theory calculations and comparative tests with oxidatively inert Li₂ZrCl₆ catholytes elucidate the enhanced performance mechanism, specifically, the suppression of Ni²⁺ migration by Zn doping, emphasizing the importance of cathode structural stability in all-solid-state batteries.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":"44 1","pages":""},"PeriodicalIF":22.0,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439268","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}