In situ electrochemical activation converts carbon disulfide into an organosulfide cathode material for rechargeable lithium-organosulfide batteries

In situ electrochemical activation converts carbon disulfide into an organosulfide cathode material for rechargeable lithium-organosulfide batteries | 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 In situ electrochemical activation converts carbon disulfide into an organosulfide cathode material for rechargeable lithium-organosulfide batteries Dean Shi, YouShuang Zhou, Yang Zhou, YiYang Chen, JunPeng Rao, and 7 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9045027/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted You are reading this latest preprint version Abstract Although carbon disulfide (CS2) exhibits high sulfur content and optimal electrolyte solubility, its intrinsic electrochemical inertness prevents its direct use as an active cathode material, relegating it to a non-capacitive electrolyte additive. In this work, it is found that CS2 can be activated electrochemically to transform into a redox-active cathode material that contributes to reversible capacity in lithium batteries under specific conditions. A coin cell (Li//CS2 battery) using bare carbon paper as the cathode (containing no active material), lithium metal as the anode, and a mixture of commercial liquid electrolyte (1 M LiTFSI in 1,2-dimethoxyethane (DME)/1,3-dioxolane (DOL) (3:1 v/v)) and CS2 as the additive is assembled. When the first-cycle discharge cut-off voltage drops below 1.6 V vs. Li/Li⁺, CS2 can be reduced to form CS2 radicals, which subsequently generate electrochemically active lithium tetrathiooxalate anhydride with thiodicarbonic acid (LTAT) under the present of Li+ ions. And LTAT can serve as a new active material in subsequent battery cycles when the discharge cut-off voltage is restored to the conventional 1.7 V vs. Li/Li⁺ during the following charge–discharge cycles. After CS2 being fully activated, the coin Li//CS2 battery delivers a reversible discharge specific capacity of 163 mAh g-1 (calculated based on the total mass of CS2 initially added in the electrolyte) along with exceptional cycling stability (capacity decay rate of merely 0.0096% per cycle over 6,000 cycles) at a current density of 1.0 mA cm-2 within the voltage range of 1.7 to 3.0 V vs Li/Li⁺. The Li//CS2 flow battery delivers a high reversible capacity of 75.5 Ah L-1 at a current density of 0.3 mA cm-2. And the Li//CS2 pouch cell with CS2 as the cathode material retains a capacity retention rate of 95.7% after 100 cycles at 0.3mA cm-2. This work presents a novel strategy for designing high-performance and high-energy-density storage lithium-organosulfide batteries. Physical sciences/Chemistry/Electrochemistry/Batteries Physical sciences/Energy science and technology/Energy storage/Batteries Full Text Additional Declarations There is NO Competing Interest. Supplementary Files Supportinginformation2026.3.4.docx Supplementary Information Cite Share Download PDF Status: Under Review 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. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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-9045027","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":605555021,"identity":"809fe8d8-f8e7-4293-84fe-6444800b3b5a","order_by":0,"name":"Dean Shi","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA90lEQVRIiWNgGAWjYDCCA0DM2CAhx8bMfPAxhMtgQJQWY352tmRjUrQwJM7s5zGTJkoL3/HmZw9/7rBg3HCYway6sO1OYgN78zYJhpo7OLVInjlmbsx7RoLZ4DBD2u2Zbc8SG3iOlUkwHHuGU4vBjQQzacY2CTaglmO3edsOJzZI5JhJMDYcxq3l/vNvkj/bJHgMDjO2FYO1yL8hoOUGj5kEb5uEhGQzMxszxBYe/Fokz+SUSQO1GPADdUjznHtm3MaTVmyRcAy3Fr7jx7cBHVZX38Z//uNnnrI7sv3shzfe+FCDWwsmYAMRCSRoGAWjYBSMglGACQAi8FYS3HRXbQAAAABJRU5ErkJggg==","orcid":"","institution":"Hubei University","correspondingAuthor":true,"prefix":"","firstName":"Dean","middleName":"","lastName":"Shi","suffix":""},{"id":605555022,"identity":"934e9647-2c79-4609-8a20-1910fa5d8e57","order_by":1,"name":"YouShuang Zhou","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"YouShuang","middleName":"","lastName":"Zhou","suffix":""},{"id":605555023,"identity":"106a21f5-09d9-4889-8463-f4b26996308a","order_by":2,"name":"Yang Zhou","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"Yang","middleName":"","lastName":"Zhou","suffix":""},{"id":605555024,"identity":"ef05fba4-b301-4a50-afd3-0ebb76fd6068","order_by":3,"name":"YiYang Chen","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"YiYang","middleName":"","lastName":"Chen","suffix":""},{"id":605555025,"identity":"b56fb637-c43f-463d-b5f9-b068a2e9834c","order_by":4,"name":"JunPeng Rao","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"JunPeng","middleName":"","lastName":"Rao","suffix":""},{"id":605555026,"identity":"4ff5038f-46c7-4438-b028-5e89732abb3c","order_by":5,"name":"ZhaoYang Wei","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"ZhaoYang","middleName":"","lastName":"Wei","suffix":""},{"id":605555027,"identity":"f1174777-6c1b-408e-b3e6-a8db1ea51870","order_by":6,"name":"WeiWei Lei","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"WeiWei","middleName":"","lastName":"Lei","suffix":""},{"id":605555028,"identity":"f5045d6b-ce87-4858-81d3-78e431e792b6","order_by":7,"name":"YouFang Zhang","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"YouFang","middleName":"","lastName":"Zhang","suffix":""},{"id":605555029,"identity":"fdf2ac9c-0b4e-4a18-bc2d-9c9f3162c802","order_by":8,"name":"Jun You","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"Jun","middleName":"","lastName":"You","suffix":""},{"id":605555030,"identity":"d60e3b8e-6e66-408a-a06d-5c8437ac9306","order_by":9,"name":"Qunchao Zhang","email":"","orcid":"","institution":"Hubei University","correspondingAuthor":false,"prefix":"","firstName":"Qunchao","middleName":"","lastName":"Zhang","suffix":""},{"id":605555031,"identity":"6c418eac-f796-44b9-b044-d279aed65112","order_by":10,"name":"Robert K.Y. 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In this work, it is found that CS2 can be activated electrochemically to transform into a redox-active cathode material that contributes to reversible capacity in lithium batteries under specific conditions. A coin cell (Li//CS2 battery) using bare carbon paper as the cathode (containing no active material), lithium metal as the anode, and a mixture of commercial liquid electrolyte (1 M LiTFSI in 1,2-dimethoxyethane (DME)/1,3-dioxolane (DOL) (3:1 v/v)) and CS2 as the additive is assembled. When the first-cycle discharge cut-off voltage drops below 1.6 V vs. Li/Li⁺, CS2 can be reduced to form CS2 radicals, which subsequently generate electrochemically active lithium tetrathiooxalate anhydride with thiodicarbonic acid (LTAT) under the present of Li+ ions. And LTAT can serve as a new active material in subsequent battery cycles when the discharge cut-off voltage is restored to the conventional 1.7 V vs. Li/Li⁺ during the following charge–discharge cycles. After CS2 being fully activated, the coin Li//CS2 battery delivers a reversible discharge specific capacity of 163 mAh g-1 (calculated based on the total mass of CS2 initially added in the electrolyte) along with exceptional cycling stability (capacity decay rate of merely 0.0096% per cycle over 6,000 cycles) at a current density of 1.0 mA cm-2 within the voltage range of 1.7 to 3.0 V vs Li/Li⁺. The Li//CS2 flow battery delivers a high reversible capacity of 75.5 Ah L-1 at a current density of 0.3 mA cm-2. And the Li//CS2 pouch cell with CS2 as the cathode material retains a capacity retention rate of 95.7% after 100 cycles at 0.3mA cm-2. 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