ACS Energy Letters 最新文献

{"title":"Operando Photoelectron Spectroscopy Analysis of Li6PS5Cl Electrochemical Decomposition Reactions in Solid-State Batteries","authors":"Burak Aktekin, Elmar Kataev, Luise M. Riegger, Raul Garcia-Diez, Zora Chalkley, Juri Becker, Regan G. Wilks, Anja Henss, Marcus Bär, Jürgen Janek","doi":"10.1021/acsenergylett.4c01072","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01072","url":null,"abstract":"It is crucial to understand at which potentials electrolyte decomposition reactions start and which chemical species are present in the subsequently formed decomposition films, e.g., solid electrolyte interphase (SEI). Herein, a new operando experimental approach is introduced to investigate such reactions by employing hard X-ray photoelectron spectroscopy (HAXPES). This approach enables the examination of the SEI formed below a thin metal film (e.g., 6 nm nickel) acting as the working electrode in an electrochemical cell with sulfide-based Li₆PS₅Cl solid electrolyte. Electrolyte reduction reactions already started at 1.75 V (vs Li⁺/Li) and resulted in considerable Li₂S formation, particularly in the voltage range 1.5–1.0 V. A heterogeneous/layered microstructure of the SEI is observed (e.g., preferential Li₂O and Li₂S deposits near the current collector). The reversibility of side reactions is also observed, as Li₂O and Li₂S decompose in the 2–4 V potential window, generating oxidized sulfur species, sulfites, and sulfates.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141462010","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":"Design of a Compact Multicyclic High-Performance Atmospheric Water Harvester for Arid Environments","authors":"Xiangyu Li, Bachir El Fil, Buxuan Li, Gustav Graeber, Adela C. Li, Yang Zhong, Mohammed Alshrah, Chad T. Wilson, Emily Lin","doi":"10.1021/acsenergylett.4c01061","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01061","url":null,"abstract":"Water scarcity remains a grand challenge across the globe. Sorption-based atmospheric water harvesting (SAWH) is an emerging and promising solution for water scarcity, especially in arid and noncoastal regions. Traditional approaches to AWH such as fog harvesting and dewing are often not applicable in an arid environment (<30% relative humidity (RH)), whereas SAWH has demonstrated great potential to provide fresh water under a wide range of climate conditions. Despite advances in materials development, most demonstrated SAWH devices still lack sufficient water production. In this work, we focus on the adsorption bed design to achieve high water production, multicyclic operation, and a compact form factor (high material loading per heat source contact area). The modeling efforts and experimental validation illustrate an optimized design space with a fin-array adsorption bed enabled by high-density waste heat, which promises 5.826 L_water kg_sorbent^–1 day^–1 at 30% RH within a compact 1 L adsorbent bed and commercial adsorbent materials.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461566","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":"Acidity-Governed Rules in the Electrochemical Performance of Fluorinated Benzenes for High-Voltage Lithium Metal Batteries","authors":"Xinlin Li, Xianyang Wu, Hieu A. Doan, Zhenzhen Yang, Rachid Amine, Matthew Li, M. Victoria Bracamonte, Chi-Cheung Su, Khalil Amine","doi":"10.1021/acsenergylett.4c01215","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01215","url":null,"abstract":"Judicious selection of the optimal fluorobenzene (FB) as a nonsolvating cosolvent for lithium metal batteries (LMBs) is reported. We found the key correlation between FB structures and cycling stabilities of cells: increased fluorine substitution of FBs results in higher anodic stability but at the expense of reduced reductive stability, and FBs containing three or more fluorine atoms exhibit insufficient anodic stability in the electrolyte system comprised of fluoroethylene carbonate (FEC) and ethyl methyl carbonate (EMC). More importantly, FBs with higher acidity (lower p<i>K</i>_a) due to protons located between two adjacent fluorine atoms tend to be more susceptible to side reactions during cycling. Our results indicate that difluorobenzenes with no “acidic” proton (DFB2 and DFB4) have emerged as the optimal choice with the desired redox stability in high-voltage LMBs. Nuclear magnetic resonance and X-ray photoelectron spectroscopy confirmed these findings, providing guidance for selecting the most suitable FB variants as nonsolvating cosolvents for high-voltage LMBs.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141461564","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":"Correction to “Inelastic Deformation in Methylammonium Lead Iodide Perovskite and Mitigation by Additives during Thermal Cycling”","authors":"Anton A. Samoylov, Matthew Dailey, Yanan Li, Patrick J. Lohr, Sean Raglow, Adam D. Printz","doi":"10.1021/acsenergylett.4c01603","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01603","url":null,"abstract":"Pages 2101 and 2104. The authors discovered an error in the calculation of the biaxial moduli derived from the slopes of the stress curves in Figure S1. In our calculations of the moduli using eq 2, we inadvertently had inverted the slopes of the linear elastic region (i.e., we used <i></i><span style=\"color: inherit;\"></span><span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"&gt;&lt;mfrac&gt;&lt;mrow&gt;&lt;mi mathvariant=\"normal\"&gt;d&lt;/mi&gt;&lt;mi&gt;T&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi mathvariant=\"normal\"&gt;d&lt;/mi&gt;&lt;mi&gt;&amp;#x3C3;&lt;/mi&gt;&lt;/mrow&gt;&lt;/mfrac&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"><nobr aria-hidden=\"true\"><span overflow=\"scroll\" style=\"width: 1.286em; display: inline-block;\"><span style=\"display: inline-block; position: relative; width: 1.179em; height: 0px; font-size: 110%;\"><span style=\"position: absolute; clip: rect(1.126em, 1001.18em, 2.73em, -999.997em); top: -2.19em; left: 0em;\"><span><span><span style=\"display: inline-block; position: relative; width: 0.965em; height: 0px; margin-right: 0.11em; margin-left: 0.11em;\"><span style=\"position: absolute; clip: rect(3.372em, 1000.8em, 4.174em, -999.997em); top: -4.436em; left: 50%; margin-left: -0.425em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">d</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝑇<span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.11em;\"></span></span></span><span style=\"display: inline-block; width: 0px; height: 4.013em;\"></span></span><span style=\"position: absolute; clip: rect(3.372em, 1000.75em, 4.174em, -999.997em); top: -3.634em; left: 50%; margin-left: -0.372em;\"><span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\">d</span><span style=\"font-size: 70.7%; font-family: STIXMathJax_Normal-italic;\">𝜎<span style=\"display: inline-block; overflow: hidden; height: 1px; width: 0.003em;\"></span></span></span><span style=\"display: inline-block; width: 0px; height: 4.013em;\"></span></span><span style=\"position: absolute; clip: rect(0.858em, 1000.97em, 1.233em, -999.997em); top: -1.281em; left: 0em;\"><span style=\"display: inline-block; overflow: hidden; vertical-align: 0em; border-top: 1.3px solid; width: 0.965em; height: 0px;\"></span><span style=\"display: inline-block; width: 0px; height: 1.072em;\"></span></span></span></span></span><span style=\"display: inline-block; width: 0px; height: 2.195em;\"></span></span></span><span style=\"display: inline-block; overflow: hidden; vertical-align: -0.468em; border-left: 0px solid; width: 0px; height: 1.532em;\"></span></span></nobr><span role=\"presentation\"><math display=\"inline\" overflow=\"scroll\" xmlns=\"http://www.w3.org/1998/Math/MathML\"><mfrac><mrow><mi mathvariant=\"normal\">d</mi><mi>T</mi></mrow><mrow><mi mathvariant=\"normal\">d</mi><mi>σ</mi></mrow></mfrac></math></span></span><script type=\"math/mml\"><math ","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448893","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":"Oxide-Based Nanoporous Interlayer for Durable Anodic Interface in All-Solid-State Lithium Metal Batteries","authors":"Dayoung Jun, Seong Gyu Lee, Ji Eun Jung, Kyu Seok Kim, Haena Yim, Hyuksoo Shin, Jungho Lee, Yun Jung Lee","doi":"10.1021/acsenergylett.4c01360","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01360","url":null,"abstract":"Highly promising Li metal all-solid-state batteries (ASSBs) with enhanced safety and energy density have been plagued by interfacial degradation caused by the high reactivity and dendritic growth of Li at the anodic interface. Herein, a structurally immutable nanoporous oxide material, specifically Li₄Ti₅O₁₂ (LTO), is proposed as a protective shield to ensure interfacial stability in the Li metal anode. The LTO interlayer at the anodic interface exhibits sufficient electronic and ionic transfer kinetics upon lithiation to 0 V, enabling the Li deposit to penetrate through the LTO interlayer to the Li anode. The separation of Li from the solid electrolyte (SE) suppresses the increase in interfacial resistance caused by voids, dead Li, and SE decomposition, while the structural stability of the LTO ensures long-term cycling. Leveraging the physical and electrochemical robustness of LTO, this protection persists for over 300 cycles in full-cells at a substantial current density of 4.275 mA cm^–2 and a capacity of 3 mAh cm^–2.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448803","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":"Designing Better Flow Batteries: An Overview on Fifty Years’ Research","authors":"Changkun Zhang, Zhizhang Yuan, Xianfeng Li","doi":"10.1021/acsenergylett.4c00773","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c00773","url":null,"abstract":"Flow batteries (FBs) are very promising options for long duration energy storage (LDES) due to their attractive features of the decoupled energy and power rating, scalability, and long lifetime. Since the first modern FB was proposed by NSNA in 1973, FBs have developed rapidly in extensive basic research on the key materials, stack, demonstration trials, and even commercial implementation. Meanwhile, as prime candidates for the LDES, FBs still meet several challenges for industrialization: cost and performance concerns, which require that we increase the FB duration and consider some “green” and recycle resources. This review aims at providing the milestones in FB development over the 50 years of research and critical analysis of the different types of FB technologies. The directions in the science and engineering of FBs are finally presented with a future goal of achieving FBs’ commercialization.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448908","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":"Topological Considerations in Electrolyte Additives for Passivating Silicon Anodes with Hybrid Solid–Electrolyte Interphases","authors":"Youngmin Ko, Jiwoong Bae, Gan Chen, Michael A. Baird, Jiajun Yan, Liana Klivansky, Dong-Min Kim, Stephen E. Trask, Marco-Tulio Fonseca Rodrigues, Gerard M. Carroll, Nathan R. Neale, Brett A. Helms","doi":"10.1021/acsenergylett.4c01331","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01331","url":null,"abstract":"Unlike most anodes used in high energy density batteries, lithiated Si does not form long-lasting passivating solid-electrolyte interphases (SEI) during formation or on charge due to SEI delamination, reconstruction, or dissolution. As a result, electrolyte degradation is continuous and results in a permanent loss of the Li inventory, shortening the useful life of the battery. Here, we show that perfluoroether electrolyte additives featuring either sulfonyl fluorides or trifluorovinyl ethers, when introduced in prescribed amounts to locally superconcentrated electrolytes, exhibit preferential reactivity at Si during formation due to their higher reduction potential than salts and solvents, creating a hybrid SEI that is simultaneously enriched with LiF and organics tethered to the reactive functionality. While both reactive motifs are effective in creating a hybrid SEI, perfluoroether additives bearing sulfonyl fluorides show more substantial integration. More important, however, is the combined influence of additive topology on anchoring efficacy and tether flexibility between anchoring sites on SEI resiliency. Top-performing Si|LFP cells featuring ditopic additive-enriched SEI improve capacity retention by as much as 45% over 100 cycles when compared to additive-free cells.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448796","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":"Nitrogen Doping-Induced Structural Distortion in LaMnO3 Enhances Oxygen Reduction and Oxygen Evolution Reactions","authors":"Soumi Mondal, Shreya Sarkar, Mohd Riyaz, Manaswita Kar, Adrian C. Fortuin, Surishi Vashishth, Risov Das, M. Eswaramoorthy, Denis Kramer, Sebastian C. Peter","doi":"10.1021/acsenergylett.4c01206","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01206","url":null,"abstract":"Nitrogen-doped perovskites (LaMnO₃) were designed as bifunctional catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Nitridation led to O-substitution in LaMnO₃, creating distortion in the LaMnO₃ structure and generating oxygen vacancies. N-doping facilitated an increase of Mn³⁺ content, enhancing ORR and OER activities. LaMnO₃ with 4 h of nitridation exhibits 3.35 and 1.75 times higher specific and mass activities in comparison to pristine LaMnO₃ (highest reported among perovskite oxides). The enhancement in catalytic activity is attributed to the increase of Mn³⁺ content and distorted Mn–O, leading to compressive strain. The substitution of N at the crystal lattice of perovskite stabilizes the intermediates through a combination of strain and charge modulation of the active Mn center, which causes the enhancement in ORR and OER performance. The bifunctional character of the catalyst was further evaluated for practical zinc–air battery applications in which nitrogen-doped LaMnO₃ undergoes steady operation up to 500 cycles in harsh industrial conditions of 6 M KOH.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448933","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 Neutral Zinc–Iron Flow Battery with Long Lifespan and High Power Density","authors":"Ze Chen, Tianyu Li, Congxin Xie, Xianfeng Li","doi":"10.1021/acsenergylett.4c01424","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01424","url":null,"abstract":"Neutral zinc–iron flow batteries (ZIFBs) remain attractive due to features of low cost, abundant reserves, and mild operating medium. However, the ZIFBs based on Fe(CN)₆^3–/Fe(CN)₆^4– catholyte suffer from Zn₂Fe(CN)₆ precipitation due to the Zn²⁺ crossover from the anolyte. Even worse, the opposite charge properties of positive and negative active species enable a big contradiction in the design of a suitable membrane. Herein, sodium citrate (Cit) was introduced to coordinate with Zn²⁺, which effectively alleviated the crossover and precipitation issues. Meanwhile, the redox species exhibited considerable kinetics and reversibility with a good capability of hydrogen evolution inhibition. As a result, the assembled battery demonstrated a high energy efficiency of 89.5% at 40 mA cm^–2 and operated for 400 cycles with an average Coulombic efficiency of 99.8%. Even at 100 mA cm^–2, the battery showed an energy efficiency of over 80%. This paper provides a possible solution toward a low-cost and sustainable grid energy storage.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141445026","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":"Understanding Limitations in Electrochemical Conversion to CO at Low CO2 Concentrations","authors":"Danielle A. Henckel, Prantik Saha, Sunil Rajana, Carlos Baez-Cotto, Audrey K. Taylor, Zengcai Liu, Michael G. Resch, Richard I. Masel, K. C. Neyerlin","doi":"10.1021/acsenergylett.4c01224","DOIUrl":"https://doi.org/10.1021/acsenergylett.4c01224","url":null,"abstract":"Low-temperature electrochemical CO₂ reduction has demonstrated high selectivity for CO when devices are operated with pure CO₂ streams. However, there is currently a dearth of knowledge for systems operating below 30% CO₂, a regime interesting for coupling electrochemical devices with CO₂ point sources. Here we examine the influence of ionomer chemistry and cell operating conditions on the CO selectivity at low CO₂ concentrations. Utilizing advanced electrochemical diagnostics, values for cathode catalyst layer ionic resistance and electrocatalyst capacitance as a function of relative humidity (RH) were extracted and correlated with selectivity and catalyst utilization. Staying above 20% CO₂ concentration with at least a 50% cathode RH resulted in &gt;95% CO/H₂ selectivity regardless of the ionomer chemistry. At 10% CO₂, however, &gt;95% CO/H₂ selectivity was only obtained at 95% RH under scenarios where the resulting electrode morphology enabled high catalyst utilization.","PeriodicalId":16,"journal":{"name":"ACS Energy Letters ","volume":null,"pages":null},"PeriodicalIF":22.0,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141448839","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}