Performance of C24N24 Single Atom Catalysts for Methane Oxidation: A Combined QTAIM, IBO and DIAS Analysis

Performance of C24N24 Single Atom Catalysts for Methane Oxidation: A Combined QTAIM, IBO and DIAS Analysis | 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 Research Article Performance of C 24 N 24 Single Atom Catalysts for Methane Oxidation: A Combined QTAIM, IBO and DIAS Analysis Kwanele C. Ngubane, Mafereka F.T. Moabisane, Adedapo S. Adeyinka This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9436195/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 4 You are reading this latest preprint version Abstract The direct, efficient and selective oxidation of methane to methanol remains a major challenge in catalysis due to the strength of the C–H bond and the tendency for overoxidation. This study investigates the catalytic potential of first-row (Mn, Fe, Co, Ni, Cu) and second-row (Ru, Rh, Pd) transition metals as single-atom catalysts (SACs) supported on nitrogen-doped fullerene (C 24 N 24 ) for methane oxidation to methanol. The aim of the work is to determine whether the catalytic performance of first-row transition metals matches that of second-row transition metals and to understand the factors responsible for their catalytic activity in order to propose rational design principles for TM-doped C 24 N 24 SACs. The results reveal that Ni and Cu SACs have the lowest activation barriers due to negligible structural distortion and more negative interaction energies at the transition state. QTAIM analysis revealed significant differences in bond critical point features of various TM-O interactions, whereas IBO analysis demonstrated that more efficient catalysts promote smoother and more delocalized electron rearrangements during C-H activation. Metals, such as Ru and Mn, exhibit increased electron localization and structural reorganization, which corresponds to higher energy barriers. This emphasises the importance of structural, electrostatic, and orbital parameters in determining the catalytic performance of SACs for methane oxidation. The findings help rationalize the design of effective methane valorisation C 24 N 24 supported SACs and provide useful methodologies for modifying their selectivity and activity using atomic-level changes. Methane Oxidation Transition metal Single-atom catalyst Fullerene Activation Energy Full Text Additional Declarations No competing interests reported. Supplementary Files SupportingInformation.docx Cite Share Download PDF Status: Under Review Version 1 posted Editorial decision: Revision requested 24 Apr, 2026 Editor assigned by journal 24 Apr, 2026 Submission checks completed at journal 24 Apr, 2026 First submitted to journal 16 Apr, 2026 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-9436195","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":628903854,"identity":"743d38a5-dee5-4d42-99f6-21bb6bf2c39e","order_by":0,"name":"Kwanele C. Ngubane","email":"","orcid":"","institution":"University of Johannesburg","correspondingAuthor":false,"prefix":"","firstName":"Kwanele","middleName":"C.","lastName":"Ngubane","suffix":""},{"id":628903855,"identity":"d330957a-4759-43d9-b6c5-2f038772ebb7","order_by":1,"name":"Mafereka F.T. 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This study investigates the catalytic potential of first-row (Mn, Fe, Co, Ni, Cu) and second-row (Ru, Rh, Pd) transition metals as single-atom catalysts (SACs) supported on nitrogen-doped fullerene (C\u003csub\u003e24\u003c/sub\u003eN\u003csub\u003e24\u003c/sub\u003e) for methane oxidation to methanol. The aim of the work is to determine whether the catalytic performance of first-row transition metals matches that of second-row transition metals and to understand the factors responsible for their catalytic activity in order to propose rational design principles for TM-doped C\u003csub\u003e24\u003c/sub\u003eN\u003csub\u003e24\u003c/sub\u003e SACs. The results reveal that Ni and Cu SACs have the lowest activation barriers due to negligible structural distortion and more negative interaction energies at the transition state. QTAIM analysis revealed significant differences in bond critical point features of various TM-O interactions, whereas IBO analysis demonstrated that more efficient catalysts promote smoother and more delocalized electron rearrangements during C-H activation. Metals, such as Ru and Mn, exhibit increased electron localization and structural reorganization, which corresponds to higher energy barriers. This emphasises the importance of structural, electrostatic, and orbital parameters in determining the catalytic performance of SACs for methane oxidation. The findings help rationalize the design of effective methane valorisation C\u003csub\u003e24\u003c/sub\u003eN\u003csub\u003e24\u003c/sub\u003e supported SACs and provide useful methodologies for modifying their selectivity and activity using atomic-level changes.\u003c/p\u003e","manuscriptTitle":"Performance of C24N24 Single Atom Catalysts for Methane Oxidation: A Combined QTAIM, IBO and DIAS Analysis","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-05-12 17:57:37","doi":"10.21203/rs.3.rs-9436195/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2026-04-24T10:00:23+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2026-04-24T08:20:21+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2026-04-24T08:20:01+00:00","index":"","fulltext":""},{"type":"submitted","content":"Journal of Molecular Modeling","date":"2026-04-16T09:22:55+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"journal-of-molecular-modeling","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"jmmo","sideBox":"Learn more about [Journal of Molecular Modeling](https://www.springer.com/journal/894)","snPcode":"894","submissionUrl":"https://submission.nature.com/new-submission/894/3","title":"Journal of Molecular Modeling","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"em","reportingPortfolio":"Springer Hybrid","inReviewEnabled":true,"inReviewRevisionsEnabled":false}}],"origin":"","ownerIdentity":"ced03018-da95-46b4-934e-e73662b579e6","owner":[],"postedDate":"May 12th, 2026","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2026-05-12T17:57:37+00:00","versionOfRecord":[],"versionCreatedAt":"2026-05-12 17:57:37","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-9436195","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-9436195","identity":"rs-9436195","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}