Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene

Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene | 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 Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene Weiming Wan, zitong zhang, youran wang, liujia zhang, Zhendong Liu This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-8230494/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 Non-thermal plasma (NTP) is a promising approach for activating methane at room temperature, enabling its direct conversion to ethylene under mild conditions. However, the high energy consumption and the trade-off between methane conversion and ethylene selectivity limit its industrial application. Herein, we report a pure-silica self-pillared pentasil (SPP) zeolite catalyst that enables efficient methane conversion to ethylene under NTP activation at room temperature. This plasma-catalytic system achieves an exceptional ethylene selectivity of 58.8% with an energy yield of 52 mmol/MJ at atmospheric pressure. Mechanistic studies reveal that isolated hydroxyl groups on the SPP catalyst stabilize gaseous methyl radicals, promoting C–C coupling and methane dissociation. The confined plasma between catalyst granules selectively suppresses further hydrogenation and methylation of the key C 2 H 5 intermediate, thereby achieving high ethylene selectivity. By optimizing reaction conditions, an ethylene yield of 40% was achieved, surpassing the benchmarks of both plasma and thermal catalytic processes. Physical sciences/Chemistry/Catalysis/Heterogeneous catalysis Physical sciences/Chemistry/Catalysis/Catalytic mechanisms Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupportingInformation1128.docx Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene-SI 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-8230494","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":555876362,"identity":"cdecd7c2-1176-462f-9123-401a95b2b046","order_by":0,"name":"Weiming Wan","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA5ElEQVRIie3NsQrCMBCA4ZNCp6BrS0Vf4USoCEJfJSI4iTi5KgiZBNf6Dg6dnBMEXapdA13sriC4KDhYs7jFugnmhzsI5OMATKafDYEAWIKrBy9ObPoNUREsRnC33zqX0braqqwu4s6gVpa0dB3pSDzsuyGmpB2eI+4yaLqSWl6oIT4f+CnJCcp9xBsMupGktkV0JDn56UOR+Mi7DCaficyvwIskc+CCAcVPJJCn1n2urtgopgensYyzmacj7mLQxNsjDTDZZNlt3KmXdz1x1ZF3DlU7n9K0EACo8IIfTSaT6e96AoB+VK9aKwfmAAAAAElFTkSuQmCC","orcid":"","institution":"Lanzhou University","correspondingAuthor":true,"prefix":"","firstName":"Weiming","middleName":"","lastName":"Wan","suffix":""},{"id":555876363,"identity":"f1ef35b5-38a2-4fab-b488-6a7a585db643","order_by":1,"name":"zitong zhang","email":"","orcid":"","institution":"Lanzhou University","correspondingAuthor":false,"prefix":"","firstName":"zitong","middleName":"","lastName":"zhang","suffix":""},{"id":555876364,"identity":"26838f73-9e77-4231-b3dd-c43de8275248","order_by":2,"name":"youran wang","email":"","orcid":"","institution":"Tsinghua University","correspondingAuthor":false,"prefix":"","firstName":"youran","middleName":"","lastName":"wang","suffix":""},{"id":555876365,"identity":"1daf3e06-2cb5-4edf-8969-ce1b45b3cf93","order_by":3,"name":"liujia zhang","email":"","orcid":"","institution":"Lanzhou University","correspondingAuthor":false,"prefix":"","firstName":"liujia","middleName":"","lastName":"zhang","suffix":""},{"id":555876366,"identity":"74be8347-9b58-4b78-9d8c-9fcf60c2a6d4","order_by":4,"name":"Zhendong Liu","email":"","orcid":"https://orcid.org/0000-0002-3364-2523","institution":"Tsinghua University","correspondingAuthor":false,"prefix":"","firstName":"Zhendong","middleName":"","lastName":"Liu","suffix":""}],"badges":[],"createdAt":"2025-11-28 12:50:14","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-8230494/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-8230494/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":97673632,"identity":"b3323185-c0d5-41b6-8916-daf0235c29aa","added_by":"auto","created_at":"2025-12-08 09:40:52","extension":"docx","order_by":0,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":3430515,"visible":true,"origin":"","legend":"","description":"","filename":"Manuscript1128.docx","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/a1fb4af5fa8d70407c6d78c6.docx"},{"id":97649052,"identity":"9eef753c-6431-4f70-85eb-a97e1726ccbf","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"json","order_by":1,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":6310,"visible":true,"origin":"","legend":"","description":"","filename":"NCOMMS2596559.json","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/fd31127aeb52723d8de18f4f.json"},{"id":97673984,"identity":"8d8e9518-540a-496d-9189-84ad8701bc56","added_by":"auto","created_at":"2025-12-08 09:42:03","extension":"docx","order_by":2,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":10450000,"visible":true,"origin":"","legend":"","description":"","filename":"SupportingInformation1128.docx","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/2d646fa8eba40b76f8f55df5.docx"},{"id":97649054,"identity":"ff860d58-158a-469e-bee3-604006027be3","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"xml","order_by":3,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":112169,"visible":true,"origin":"","legend":"","description":"","filename":"NCOMMS25965590enriched.xml","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/03e5b103c6d34de82a6196ac.xml"},{"id":97674140,"identity":"ff8950a3-fc74-4565-b6c5-0a5f4b970813","added_by":"auto","created_at":"2025-12-08 09:42:28","extension":"jpeg","order_by":4,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":525656,"visible":true,"origin":"","legend":"","description":"","filename":"floatimage1.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/2671b8575159260747c7e7f4.jpeg"},{"id":97673993,"identity":"6b96118e-9a37-415a-aa2b-4008030a5986","added_by":"auto","created_at":"2025-12-08 09:42:05","extension":"jpeg","order_by":5,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":623208,"visible":true,"origin":"","legend":"","description":"","filename":"floatimage2.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/652b742cba1fd0734a48ea6a.jpeg"},{"id":97649061,"identity":"d68ba909-a1c9-4bf5-bdff-9b546c0294d8","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"jpeg","order_by":6,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":1150052,"visible":true,"origin":"","legend":"","description":"","filename":"floatimage3.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/280d0907b16a306f240824db.jpeg"},{"id":97673902,"identity":"6e5258f2-a89f-40f9-a1d8-f92f346eaa6b","added_by":"auto","created_at":"2025-12-08 09:41:51","extension":"jpeg","order_by":7,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":765486,"visible":true,"origin":"","legend":"","description":"","filename":"floatimage4.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/f38f38231f4aa112a0058364.jpeg"},{"id":97672896,"identity":"59736283-e70e-4a25-96f2-6f1d67e76844","added_by":"auto","created_at":"2025-12-08 09:39:01","extension":"jpeg","order_by":8,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":281046,"visible":true,"origin":"","legend":"","description":"","filename":"floatimage5.jpeg","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/25fdb96a9b5a85e634b67b25.jpeg"},{"id":97649059,"identity":"d22186b3-4bce-4c9b-88dc-254ecfe7b388","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"png","order_by":9,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":97003,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage1.png","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/a272a5057dd4f87f1284128f.png"},{"id":97649056,"identity":"3451255f-4ece-4314-907e-267b06230614","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"png","order_by":10,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":115815,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage2.png","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/8c1ab8c0c2d25067971968b2.png"},{"id":97649062,"identity":"4e8ee19a-e07a-4014-882e-5d4663687e26","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"png","order_by":11,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":171041,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage3.png","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/ff6ae51544e15a682e8ff713.png"},{"id":97673985,"identity":"6f6cae81-38f5-4b44-9eff-81d4231f6ffb","added_by":"auto","created_at":"2025-12-08 09:42:03","extension":"png","order_by":12,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":116893,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage4.png","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/b238afc019d464e489af16f5.png"},{"id":97649067,"identity":"ba7f5b36-01d6-43cb-97f6-347495165f8b","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"png","order_by":13,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":38318,"visible":true,"origin":"","legend":"","description":"","filename":"Onlinefloatimage5.png","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/70cf9294bdc5df70ad043076.png"},{"id":97649064,"identity":"b4d3ef3c-e477-4a39-9861-3628c5e39547","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"xml","order_by":14,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":110443,"visible":true,"origin":"","legend":"","description":"","filename":"NCOMMS25965590structuring.xml","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/89e91c74b8732ccad0e5fab4.xml"},{"id":97649068,"identity":"b916a1c6-0eb4-4886-b55b-7bb0913faa14","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"html","order_by":15,"title":"","display":"","copyAsset":false,"role":"acdc-reference","size":117487,"visible":true,"origin":"","legend":"","description":"","filename":"earlyproof.html","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/2e0577a35870456076661c7a.html"},{"id":97678894,"identity":"e9c6cb00-5e85-47bd-8198-6629d4e956a4","added_by":"auto","created_at":"2025-12-08 09:56:33","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":1000184,"visible":true,"origin":"","legend":"","description":"","filename":"Manuscript1128.pdf","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1_covered_6300f5cc-9cf2-4690-85bb-de72cc0ee201.pdf"},{"id":97649055,"identity":"d28c0e76-ae78-4fbf-92b7-e48c37a43e38","added_by":"auto","created_at":"2025-12-08 05:39:08","extension":"docx","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":10450000,"visible":true,"origin":"","legend":"Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene-SI","description":"","filename":"SupportingInformation1128.docx","url":"https://assets-eu.researchsquare.com/files/rs-8230494/v1/725a3be5d5daaac3d1ffbedf.docx"}],"financialInterests":"There is \u003cb\u003eNO\u003c/b\u003e Competing Interest.","formattedTitle":"Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"nature-portfolio","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"","title":"Nature Portfolio","twitterHandle":"","acdcEnabled":false,"dfaEnabled":false,"editorialSystem":"ejp","reportingPortfolio":"","inReviewEnabled":true,"inReviewRevisionsEnabled":false},"keywords":"","lastPublishedDoi":"10.21203/rs.3.rs-8230494/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-8230494/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eNon-thermal plasma (NTP) is a promising approach for activating methane at room temperature, enabling its direct conversion to ethylene under mild conditions. However, the high energy consumption and the trade-off between methane conversion and ethylene selectivity limit its industrial application. Herein, we report a pure-silica self-pillared pentasil (SPP) zeolite catalyst that enables efficient methane conversion to ethylene under NTP activation at room temperature. This plasma-catalytic system achieves an exceptional ethylene selectivity of 58.8% with an energy yield of 52 mmol/MJ at atmospheric pressure. Mechanistic studies reveal that isolated hydroxyl groups on the SPP catalyst stabilize gaseous methyl radicals, promoting C\u0026ndash;C coupling and methane dissociation. The confined plasma between catalyst granules selectively suppresses further hydrogenation and methylation of the key C\u003csub\u003e2\u003c/sub\u003eH\u003csub\u003e5\u003c/sub\u003e intermediate, thereby achieving high ethylene selectivity. By optimizing reaction conditions, an ethylene yield of 40% was achieved, surpassing the benchmarks of both plasma and thermal catalytic processes.\u003c/p\u003e","manuscriptTitle":"Overcoming the conversion-selectivity trade-off in plasma catalytic conversion of methane to ethylene","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-12-08 05:39:04","doi":"10.21203/rs.3.rs-8230494/v1","editorialEvents":[],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"nature-communications","isNatureJournal":true,"hasQc":false,"allowDirectSubmit":false,"externalIdentity":"NCOMMS","sideBox":"Learn more about [Nature Communications](http://www.nature.com/ncomms/)","snPcode":"","submissionUrl":"https://mts-ncomms.nature.com/","title":"Nature Communications","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"ejp","reportingPortfolio":"Nature Communications","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"1068a77f-1901-4f02-96c6-24582d0e1eb4","owner":[],"postedDate":"December 8th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":59165137,"name":"Physical sciences/Chemistry/Catalysis/Heterogeneous catalysis"},{"id":59165138,"name":"Physical sciences/Chemistry/Catalysis/Catalytic mechanisms"}],"tags":[],"updatedAt":"2026-04-06T13:36:38+00:00","versionOfRecord":[],"versionCreatedAt":"2025-12-08 05:39:04","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-8230494","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-8230494","identity":"rs-8230494","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}