Electrocatalytic upcycling of high-pressure captured CO2

Electrocatalytic upcycling of high-pressure captured CO2 | 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 Physical Sciences - Article Electrocatalytic upcycling of high-pressure captured CO 2 Xu Lu, Liang Huang, Ge Gao, Jiwu Zhao, William Roberts This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-4339066/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract Electrochemical upcycling of captured CO 2 – typically under high pressure – holds significant potential to bridge between CO 2 emissions and hydrocarbon commodities. However, this conceptual CO 2 value chain is yet to be demonstrated. Here, we showcase the valorization of gas-phase high-pressure captured CO 2 (HP-cCO 2 ) into ethylene (C 2 H 4 ) through electrochemical CO 2 reduction (CO 2 R). Guided by theoretical calculations, we devise a single-atom In alloyed Cu catalyst (In 1 /Cu), which, when integrated into a custom-built high-pressure membrane electrode assembly (MEA) under 20 bar, affords up to 85% Faradaic efficiency (FE) and up to 750 mA cm −2 partial current density toward C 2 H 4 . The interplay of theory and high-pressure operando methods links the exceptional performance to the pressure-modulated adsorption configuration of the *CO intermediate, and the elevated CO 2 coverage. We also reveal the pivotal role of pressure in mitigating the salt precipitation – a long-standing challenge in the field – by relocating the bicarbonate formation to the catalyst-membrane interface. This was agreed upon by C 2 H 4 FE that is sustained above 80% for 1,500 hours at 600 mA cm −2 under 20 bar. This proof-of-concept, by electrochemically producing C 2 H 4 from HP-cCO 2 and re-capturing the residue CO 2 , delivers industrial grade 99.9% purity C 2 H 4 and exhibits prospect of turning the otherwise costly CO 2 capture process into a profit. Energy analysis suggested that directly valorizing HP-cCO 2 , instead of depressurizing it to accommodate conventional ambient-pressure CO 2 R and repressurizing the effluents for gas product separation, is essential to minimize the energy consumption. Physical sciences/Chemistry/Electrochemistry/Electrocatalysis Physical sciences/Materials science/Materials for energy and catalysis/Electrocatalysis Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryInformation.pdf Supplementary Information Cite Share Download PDF Status: Posted 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-4339066","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Physical Sciences - Article","associatedPublications":[],"authors":[{"id":328737380,"identity":"b8c373a3-6363-4d8d-9119-5b991a0b5d6c","order_by":0,"name":"Xu 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However, this conceptual CO\u003csub\u003e2\u003c/sub\u003e value chain is yet to be demonstrated. Here, we showcase the valorization of gas-phase high-pressure captured CO\u003csub\u003e2\u003c/sub\u003e (HP-cCO\u003csub\u003e2\u003c/sub\u003e) into ethylene (C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e4\u003c/sub\u003e) through electrochemical CO\u003csub\u003e2\u003c/sub\u003e reduction (CO\u003csub\u003e2\u003c/sub\u003eR). Guided by theoretical calculations, we devise a single-atom In alloyed Cu catalyst (In\u003csub\u003e1\u003c/sub\u003e/Cu), which, when integrated into a custom-built high-pressure membrane electrode assembly (MEA) under 20 bar, affords up to 85% Faradaic efficiency (FE) and up to 750 mA cm\u003csup\u003e−2\u003c/sup\u003e partial current density toward C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e4\u003c/sub\u003e. The interplay of theory and high-pressure \u003ci\u003eoperando\u003c/i\u003e methods links the exceptional performance to the pressure-modulated adsorption configuration of the *CO intermediate, and the elevated CO\u003csub\u003e2\u003c/sub\u003e coverage. We also reveal the pivotal role of pressure in mitigating the salt precipitation – a long-standing challenge in the field – by relocating the bicarbonate formation to the catalyst-membrane interface. This was agreed upon by C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e4\u003c/sub\u003e FE that is sustained above 80% for 1,500 hours at 600 mA cm\u003csub\u003e−2\u003c/sub\u003e under 20 bar. This proof-of-concept, by electrochemically producing C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e4\u003c/sub\u003e from HP-cCO\u003csub\u003e2\u003c/sub\u003e and re-capturing the residue CO\u003csub\u003e2\u003c/sub\u003e, delivers industrial grade 99.9% purity C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e4\u003c/sub\u003e and exhibits prospect of turning the otherwise costly CO\u003csub\u003e2\u003c/sub\u003e capture process into a profit. Energy analysis suggested that directly valorizing HP-cCO\u003csub\u003e2\u003c/sub\u003e, instead of depressurizing it to accommodate conventional ambient-pressure CO\u003csub\u003e2\u003c/sub\u003eR and repressurizing the effluents for gas product separation, is essential to minimize the energy consumption.","manuscriptTitle":"Electrocatalytic upcycling of high-pressure captured CO2","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-07-26 16:06:07","doi":"10.21203/rs.3.rs-4339066/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":"9e8c8bef-f482-48ed-b7c4-22baae6a9686","owner":[],"postedDate":"July 26th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":34797654,"name":"Physical sciences/Chemistry/Electrochemistry/Electrocatalysis"},{"id":34797655,"name":"Physical sciences/Materials science/Materials for energy and catalysis/Electrocatalysis"}],"tags":[],"updatedAt":"2024-11-04T15:37:08+00:00","versionOfRecord":[],"versionCreatedAt":"2024-07-26 16:06:07","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-4339066","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-4339066","identity":"rs-4339066","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}