Electron-Pump Engineering via CuO-Sm2CuO4 Heterojunction for Side-on N2O Activation and Efficient Catalytic Decomposition under O2-Rich Conditions

Electron-Pump Engineering via CuO-Sm2CuO4 Heterojunction for Side-on N2O Activation and Efficient Catalytic Decomposition under O2-Rich Conditions | 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 Electron-Pump Engineering via CuO-Sm2CuO4 Heterojunction for Side-on N2O Activation and Efficient Catalytic Decomposition under O2-Rich Conditions Junhua Li, Hao Liu, Xueqing Liu, Chuanzhi Sun, Yunpeng Long, Fang Huang, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9326059/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 Catalytic N2O decomposition on CuO-based catalysts is limited by poor N-O activation. Interfacial electron engineering can modulate active-site structure, yet its effect on N2O remains unclear. Here, we have developed a CuO-Sm2CuO4 heterostructure, which achieves over 90% N2O decomposition at 400 °C in 5% O2. In simulated NOx-N2O co-reduction, it retains 96% activity at 450 °C for 168 hours. This performance indicates significant application potential compared to reported catalyst systems. Our study demonstrates that Cu2+-O- sites on as-synthesized CuO-based catalysts drive N2O decomposition via the Mars-van-Krevelen mechanism, generating Cu+ species that complete the catalytic cycle through the Langmuir-Hinshelwood pathway. On pure CuO, Cu+ adsorbs N2O end-on and activates it via σ-backdonation. In contrast, the CuO-Sm2CuO4 heterojunction forms a dynamic electron-pumping interface where Sm2CuO4 donates electrons to stabilize Cu+, reverses N2O’s adsorption-configuration to side-on and enables π-backdonation-mediated activation. This work advances understanding of interfacial electron regulation in heterogeneous catalysis and provides a strategy for designing high-performance N2O decomposition catalysts. Physical sciences/Chemistry/Catalysis/Heterogeneous catalysis Physical sciences/Chemistry/Environmental chemistry/Pollution remediation N2O decomposition CuO-based catalyst Interfacial electron interaction Reaction mechanism Full Text Additional Declarations There is NO Competing Interest. 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. 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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-9326059","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Article","associatedPublications":[],"authors":[{"id":621053982,"identity":"fa71849b-19e5-4515-bd66-d6a98f11bca6","order_by":0,"name":"Junhua 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Interfacial electron engineering can modulate active-site structure, yet its effect on N2O remains unclear. Here, we have developed a CuO-Sm2CuO4 heterostructure, which achieves over 90% N2O decomposition at 400 °C in 5% O2. In simulated NOx-N2O co-reduction, it retains 96% activity at 450 °C for 168 hours. This performance indicates significant application potential compared to reported catalyst systems. Our study demonstrates that Cu2+-O- sites on as-synthesized CuO-based catalysts drive N2O decomposition via the Mars-van-Krevelen mechanism, generating Cu+ species that complete the catalytic cycle through the Langmuir-Hinshelwood pathway. On pure CuO, Cu+ adsorbs N2O end-on and activates it via σ-backdonation. In contrast, the CuO-Sm2CuO4 heterojunction forms a dynamic electron-pumping interface where Sm2CuO4 donates electrons to stabilize Cu+, reverses N2O’s adsorption-configuration to side-on and enables π-backdonation-mediated activation. This work advances understanding of interfacial electron regulation in heterogeneous catalysis and provides a strategy for designing high-performance N2O decomposition catalysts.","manuscriptTitle":"Electron-Pump Engineering via CuO-Sm2CuO4 Heterojunction for Side-on N2O Activation and Efficient Catalytic Decomposition under O2-Rich Conditions","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2026-04-14 18:23:34","doi":"10.21203/rs.3.rs-9326059/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":"d55c9f7e-fca5-44fa-b38e-27ce3bb84481","owner":[],"postedDate":"April 14th, 2026","published":true,"recentEditorialEvents":[{"type":"editorInvitedReview","content":"This content is not available.","date":"2026-05-13T11:12:47+00:00","index":3,"fulltext":"This content is not available."},{"type":"reviewerAgreed","content":"This content is not available.","date":"2026-05-02T10:16:39+00:00","index":3,"fulltext":"This content is not available."},{"type":"editorInvitedReview","content":"This content is not available.","date":"2026-05-02T08:49:15+00:00","index":2,"fulltext":"This content is not available."},{"type":"reviewerAgreed","content":"This content is not available.","date":"2026-05-02T00:21:06+00:00","index":2,"fulltext":"This content is not available."}],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[{"id":66098773,"name":"Physical sciences/Chemistry/Catalysis/Heterogeneous catalysis"},{"id":66098774,"name":"Physical sciences/Chemistry/Environmental chemistry/Pollution remediation"}],"tags":[],"updatedAt":"2026-04-14T18:23:34+00:00","versionOfRecord":[],"versionCreatedAt":"2026-04-14 18:23:34","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-9326059","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-9326059","identity":"rs-9326059","version":["v1"]},"buildId":"XKTyCvWXoU3ODBz1xrDgd","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}