Reversible Dual Anionic-Redox Chemistry in NaCrSSe with Fast Charging Capability

Reversible Dual Anionic-Redox Chemistry in NaCrSSe with Fast Charging Capability | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Reversible Dual Anionic-Redox Chemistry in NaCrSSe with Fast Charging Capability Ding-Ren Shi, Zulipiya Shadike, Tian Wang, Si-Yu Yang, He-Yi Xia, and 15 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-40019/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 01 Aug, 2021 Read the published version in Journal of Power Sources → Version 1 posted You are reading this latest preprint version Abstract Utilizing the anionic redox reaction opens new approaches for the development of new battery cathode materials with extra capacities. Although, it suffers from several obstacles such as voltage hysteresis and sluggish kinetics. In this paper, a new layered chalcogenide-based on dual anionic-redox reaction is reported. The newly designed layered NaCrSSe exhibits the capacity of almost all Na+ intercalation/deintercalation (137 mAh g-1 at 50 mA g-1), and a unique charge/discharge feature with a small polarization of 0.15 V and high energy efficiencies of ~92% in initial cycles. Furthermore, a superior high-rate charge capacity of 115.5mAh g-1 (83.7% retention) was achieved at 27.8 C (4000 mA g-1), which is impressive in all bulk materials for sodium-ion batteries. Systematic characterization studies on structure evolution and DFT calculation show the charge compensation of S and Se anions during cycling. These results will enrich the anion redox chemistry and provide valuable information for developing new anion redox based cathode materials with high capacity and fast kinetics. Physical Chemistry Catalysis Energy Engineering chalcogenide-based dual anionic-redox reaction batteries cathode materials Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Full Text Additional Declarations There is NO Competing Interest. Supplementary Files ESI.pdf supplementary information Cite Share Download PDF Status: Published Journal Publication published 01 Aug, 2021 Read the published version in Journal of Power Sources → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-40019","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":791780,"identity":"2b7e1c46-da6a-4767-a7f9-9d27263377fd","order_by":0,"name":"Ding-Ren Shi","email":"","orcid":"","institution":"Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Ding-Ren","middleName":"","lastName":"Shi","suffix":""},{"id":791781,"identity":"70896e80-c9d5-4f4f-88d7-6e3dc7b27043","order_by":1,"name":"Zulipiya Shadike","email":"","orcid":"","institution":"Chemistry Division, Brookhaven National Laboratory","correspondingAuthor":false,"submittingAuthor":false,"prefix":"","firstName":"Zulipiya","middleName":"","lastName":"Shadike","suffix":""},{"id":791782,"identity":"c7f64fe5-dcac-4286-a5ae-8f6de9338bda","order_by":2,"name":"Tian Wang","email":"","orcid":"","institution":"Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Fudan University, Shanghai 200433, P. 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07:30:59","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-40019/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-40019/v1","draftVersion":[],"editorialEvents":[{"content":"https://doi.org/10.1016/j.jpowsour.2021.230022","type":"published","date":"2021-08-01T20:55:18+00:00"}],"editorialNote":"","failedWorkflow":false,"files":[{"id":1566857,"identity":"4a6afcb1-665f-49e5-b2da-b4b19758dc6f","added_by":"auto","created_at":"2020-07-15 15:59:47","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":605059,"visible":true,"origin":"","legend":"Structure of pristine NaCrSSe. (a) HAADF-STEM and (c) ABF-STEM image of the pristine NaCrSSe viewed along [110] projection. (b) Average image intensity profiles of the regions designated by the red line in (a) and its corresponding blue line in (c). (d) Synchrotron XRD patterns of the pristine NaCrSSe powder (red circle), calculated profile (black solid line), and their difference (violet solid line), Bragg positions are indicated as vertical tick marks. (e) EDX analysis of NaCrSSe powder, up: SEM image (scale bar represents 10 μm) and face EDX analysis results, down: corresponding elemental mapping images of Cr (red), Na (blue), Se (violet) and S (green). ","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-40019/v1/1.png"},{"id":1566858,"identity":"727cb8b7-443b-4bf2-87df-7e23ae93ce0c","added_by":"auto","created_at":"2020-07-15 15:59:47","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":168423,"visible":true,"origin":"","legend":"Electrochemical performance of NaCrSSe as cathode material for sodium-ion battery. (a) The first galvanostatic charge curves of NaCrS2 (green), NaCrS1.5Se0.5 (cyan), NaCrSSe (black) and NaCrS0.5Se1.5 (orange) at a rate of 50 mAh g-1, with their calculated voltage platforms (black dash lines). (b) Galvanostatic charge/discharge curves for the first three cycles at a rate of 50 mA g-1. (c) Cycle coulombic and energy efficiencies for the first 5 cycles. (d) Rata capacity at varied current densities. (e) Cyclic voltammograms of the NaCrSSe electrodes for various sweep rates. (f) Na+ diffusion coefficients as a function of stoichiometry from GITT. (g) Impedance spectra of a NaCrSSe pellet (mass: 0.4810 g, diameter: 12 mm, thickness: 1.302 mm) at 25 ℃, the equivalent circuits used for fitting the impedance spectra is inserted in the figure. ","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-40019/v1/2.png"},{"id":1566859,"identity":"dfd628b2-f586-4b10-b43f-5659af3d25ca","added_by":"auto","created_at":"2020-07-15 15:59:47","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":361377,"visible":true,"origin":"","legend":"Structure revolution of NaCrSSe. (a) Ex-situ XRD patterns of NaCrSSe at different charge/discharge states in the first cycle, the violet lines represent the patterns of pristine and discharged NaCrSSe and green line represents that of charged CrSSe, their corresponding peaks are also marked by violet and green respectively. (b) DFT calculated formation energies of NaxCrSSe at different x values. (c) HAADF-STEM, and (d) ABF-STEM image of the charged CrSSe viewed along [110] projection. (e) Synchrotron XRD patterns of the charged NaCrSSe powder (red circle), calculated profile (black solid line), and their difference (violet solid line). Bragg positions are indicated as vertical tick marks, a schematic of CrSSe along [110] projection is inserted in the figure. ","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-40019/v1/3.png"},{"id":1566860,"identity":"683bed62-7520-4793-ab07-69f4ee816d48","added_by":"auto","created_at":"2020-07-15 15:59:48","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":264930,"visible":true,"origin":"","legend":"Ex situ XAS and xPDF. (a)-(c) Cr, Se and S K-edge XANES spectra of NaCrSSe electrodes at various charge/discharge states which include pristine, half charged (HF, charged to a capacity of 70 mAh g-1), full charged (FC, full charged to 3.3 V), half discharged (HD, discharged to a capacity of 70 mAh g-1 after full charged) and full discharged (FD, full discharged to 1.5 V after full charged). (d)-(f) Corresponding FT-EXAFS spectra of Cr, Se and S. (g) xPDF within a range of 2.0-5.0 Å, the coordination of an S/Se in a NaCrSSe structure showed on the right. The first three peaks are marked with green, violet and yellow dashed line, the corresponding distances are represented with the same color lines in the illustrations on the right. ","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-40019/v1/4.png"},{"id":1566861,"identity":"a4b88581-fa34-4f25-9348-ada3f8b35fda","added_by":"auto","created_at":"2020-07-15 15:59:48","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":277822,"visible":true,"origin":"","legend":"Dimers and cation migration. (a) Cr 2p, (b) Se 3d and (c) S 2p XPS core peaks of NaCrSSe electrode at different charge/discharge states. (d) Raman spectra of NaCrSSe at different charge/discharge states. The data from FeS2 and CH3-S-S-S-CH3 are included for comparison. The Raman spectrum of CrSe2 was reproduced from ref38. (e) Calculated total energy of CrSSe with different amount of Cr migration. (f) Color STEM image of charged NaCrSSe (CrSSe). Scale bar refer to 1nm. ","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-40019/v1/5.png"},{"id":1566862,"identity":"642c1573-0037-42ad-9d65-58af78a9e4c1","added_by":"auto","created_at":"2020-07-15 15:59:48","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":116009,"visible":true,"origin":"","legend":"The density of states. (a), (b) Calculated density of states of NaCrSSe and 4 CrSSe is shown on the right, which is used to represent the charge contribution near the 5 Fermi level. (c) Schematic of density of states. (d) The charge compensation per atom 6 of NaCrSSe (calculated by Bader charges) and NaCrS2 (ref 11). 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Although, it suffers from several obstacles such as voltage hysteresis and sluggish kinetics. In this paper, a new layered chalcogenide-based on dual anionic-redox reaction is reported. The newly designed layered NaCrSSe exhibits the capacity of almost all Na+ intercalation/deintercalation (137 mAh g-1 at 50 mA g-1), and a unique charge/discharge feature with a small polarization of 0.15 V and high energy efficiencies of ~92% in initial cycles. Furthermore, a superior high-rate charge capacity of 115.5mAh g-1 (83.7% retention) was achieved at 27.8 C (4000 mA g-1), which is impressive in all bulk materials for sodium-ion batteries. Systematic characterization studies on structure evolution and DFT calculation show the charge compensation of S and Se anions during cycling. These results will enrich the anion redox chemistry and provide valuable information for developing new anion redox based cathode materials with high capacity and fast kinetics.","manuscriptTitle":"Reversible Dual Anionic-Redox Chemistry in NaCrSSe with Fast Charging Capability","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2020-07-15 15:59:46","doi":"10.21203/rs.3.rs-40019/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"a7d10ea7-8f9c-44c1-a0fa-6094c767d0ac","owner":[],"postedDate":"July 15th, 2020","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"published-in-journal","subjectAreas":[{"id":160399,"name":"Physical Chemistry"},{"id":160400,"name":"Catalysis"},{"id":160401,"name":"Energy Engineering"}],"tags":[],"updatedAt":"2021-07-27T20:55:18+00:00","versionOfRecord":{"articleIdentity":"rs-40019","link":"https://doi.org/10.1016/j.jpowsour.2021.230022","journal":{"identity":"journal-of-power-sources","isVorOnly":true,"title":"Journal of Power Sources"},"publishedOn":"2021-08-01 20:55:18","publishedOnDateReadable":"August 1st, 2021"},"versionCreatedAt":"2020-07-15 15:59:46","video":"","vorDoi":"10.1016/j.jpowsour.2021.230022","vorDoiUrl":"https://doi.org/10.1016/j.jpowsour.2021.230022","workflowStages":[]},"version":"v1","identity":"rs-40019","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-40019","identity":"rs-40019","version":["v1"]},"buildId":"7rjqhiLT3MXkJMwkYKINL","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}