Lamellar Aromatic Polyimine with Strong Self-Trapped Excitons for Efficient Capacitive Energy Storage

Lamellar Aromatic Polyimine with Strong Self-Trapped Excitons for Efficient Capacitive Energy Storage | 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 Lamellar Aromatic Polyimine with Strong Self-Trapped Excitons for Efficient Capacitive Energy Storage Lichuan Jia, Xiquan Xiao, Yilin Zhang, Guoli Ding, Chenyu Wang, and 12 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6303672/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 Solid film capacitors play a crucial role in the modern electrical and electronic industry, with organic polymer materials dominating the market owing to their cost-effectiveness and exceptional processability. However, the low dielectric constants of current polymers gradually fail to meet the increasing demands for high energy density of capacitors. Improving the energy storage capacity of polymer films is imperative yet very challenging. This work synthesizes an aromatic polyimine (API) with high crystallinity and unique electronic structures, which experimentally demonstrate outstanding charge storage capacity. The simple synthesis procedures of APIs allow for large-scale production at a low cost. The obtained API exhibits a typical layered crystal structure, which can be further exfoliated into quasi-two-dimensional lamellar nanoflakes via direct sonication. Notably, API undergoes a self-trapped transition band state due to the strong electron-phonon coupling at room temperature, imparting reliable charge capture ability under high electric field strength. As a result, incorporating a small amount of lamellar API into biaxially oriented polypropylene film can significantly enhance their energy storage density. This work introduces a novel crystalline polymer with exceptional charge capture and storage capabilities, providing a new avenue for the development of next-generation polymer film capacitors. Polymer Science Dielectric polymer Film capacitors Figures Figure 1 Figure 2 Figure 3 Figure 4 Full Text Additional Declarations The authors declare no competing interests. Supplementary Files SupportingInformationPreprint.pdf 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-6303672","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":433752214,"identity":"5b0efe69-f220-4eb7-ae14-2df7b88e7912","order_by":0,"name":"Lichuan Jia","email":"","orcid":"","institution":"","correspondingAuthor":false,"prefix":"","firstName":"Lichuan","middleName":"","lastName":"Jia","suffix":""},{"id":433752690,"identity":"dd55062d-c852-4b51-8452-4ae08a938cde","order_by":1,"name":"Xiquan 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Li","email":"","orcid":"","institution":"","correspondingAuthor":false,"prefix":"","firstName":"Zhongming","middleName":"","lastName":"Li","suffix":""}],"badges":[],"createdAt":"2025-03-25 12:20:55","currentVersionCode":1,"declarations":{"humanSubjects":false,"vertebrateSubjects":false,"conflictsOfInterestStatement":false,"humanSubjectEthicalGuidelines":false,"humanSubjectConsent":false,"humanSubjectClinicalTrial":false,"humanSubjectCaseReport":false,"vertebrateSubjectEthicalGuidelines":false},"doi":"10.21203/rs.3.rs-6303672/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-6303672/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":79235606,"identity":"f32a0591-ad8d-46aa-bbe6-eb3d4462e8b9","added_by":"auto","created_at":"2025-03-26 03:58:21","extension":"jpg","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":536044,"visible":true,"origin":"","legend":"\u003cp\u003eSynthesis and structural characterization of lamellar aromatic polyimine (API). (\u003cstrong\u003ea\u003c/strong\u003e) one-step chemical synthesis and (\u003cstrong\u003eb\u003c/strong\u003e) X-ray diffraction pattern of API. (\u003cstrong\u003ec\u003c/strong\u003e) FTIR spectra of API and their two monomers. (\u003cstrong\u003ed\u003c/strong\u003e) TGA curve of API. (\u003cstrong\u003ee\u003c/strong\u003e) SEM, (\u003cstrong\u003ef\u003c/strong\u003e) POM, (\u003cstrong\u003eg\u003c/strong\u003e) AFM, (\u003cstrong\u003eh\u003c/strong\u003e) TEM, (\u003cstrong\u003ei\u003c/strong\u003e) HRTEM images and (\u003cstrong\u003ej\u003c/strong\u003e) FFT pattern of API.\u003c/p\u003e","description":"","filename":"Picture1.jpg","url":"https://assets-eu.researchsquare.com/files/rs-6303672/v1/76bf7d03fc1d2e63eb7f69f7.jpg"},{"id":79234941,"identity":"7255efb5-ca99-4a31-a649-cb473e839075","added_by":"auto","created_at":"2025-03-26 03:50:21","extension":"jpg","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":355872,"visible":true,"origin":"","legend":"\u003cp\u003eElectronic structure characterization of lamellar aromatic polyimine (API). (\u003cstrong\u003ea\u003c/strong\u003e) Diffuse reflectance UV-Visible spectrum, (\u003cstrong\u003eb\u003c/strong\u003e) ultraviolet photoelectron spectroscopy, (\u003cstrong\u003ec\u003c/strong\u003e) excitation spectra, (\u003cstrong\u003ed\u003c/strong\u003e) temperature-dependent fluorescence spectra of API. (\u003cstrong\u003ee\u003c/strong\u003e) The calculated full width at half maximum (FWHM) and (\u003cstrong\u003ef\u003c/strong\u003e) fluorescence peak intensity as a function of temperature derived from Gaussian peak fitting of temperature-dependent fluorescence spectra as shown in (\u003cstrong\u003ed\u003c/strong\u003e). (\u003cstrong\u003eg\u003c/strong\u003e) Schematic of the band structure and (\u003cstrong\u003eh\u003c/strong\u003e) charge transition process under electric fields of API in BOPP polymer matrix. (\u003cstrong\u003ei\u003c/strong\u003e) The measured thermal conductivity of API flakes under different temperatures.\u003c/p\u003e","description":"","filename":"Picture2.jpg","url":"https://assets-eu.researchsquare.com/files/rs-6303672/v1/21d03e442ef1184e34de05a1.jpg"},{"id":79234937,"identity":"57cad88a-da82-4120-ae7f-76934d5398f4","added_by":"auto","created_at":"2025-03-26 03:50:21","extension":"jpg","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":402301,"visible":true,"origin":"","legend":"\u003cp\u003eProcessing, structure, and physicochemical properties of BOPP and BOPP/0.1 wt% API films. (\u003cstrong\u003ea\u003c/strong\u003e) Photo of biaxial stretching process of BOPP/API film. (\u003cstrong\u003eb\u003c/strong\u003e) Cross-sectional SEM images and (\u003cstrong\u003ec\u003c/strong\u003e) 2D-WAXD patterns of BOPP and BOPP/API films, respectively. (d) Raman spectra of API, BOPP, and BOPP/API films. (\u003cstrong\u003ee\u003c/strong\u003e) DSC curves and (\u003cstrong\u003ef\u003c/strong\u003e) mechanical tensile stress-strain curves of BOPP and BOPP/API films. (\u003cstrong\u003eg\u003c/strong\u003e) Dielectric constant, (\u003cstrong\u003eh\u003c/strong\u003e) dielectric loss, and (\u003cstrong\u003ei\u003c/strong\u003e) thermal conductivity of BOPP and BOPP/API films, respectively.\u003c/p\u003e","description":"","filename":"Picture3.jpg","url":"https://assets-eu.researchsquare.com/files/rs-6303672/v1/244aafcf2245ee0db8fe1726.jpg"},{"id":79234939,"identity":"9f272915-86fc-4306-a18d-d13aa6050be2","added_by":"auto","created_at":"2025-03-26 03:50:21","extension":"jpg","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":423685,"visible":true,"origin":"","legend":"\u003cp\u003eEnergy storage performance of BOPP and BOPP/API films. (\u003cstrong\u003ea\u003c/strong\u003e) Dielectric breakdown strength. (\u003cstrong\u003eb\u003c/strong\u003e) Weibull breakdown strength versus filler content of BOPP composites. (\u003cstrong\u003ec\u003c/strong\u003e) Unipolar D-E loops at 600 MV m\u003csup\u003e-1\u003c/sup\u003e. Phase field simulation of (\u003cstrong\u003ed\u003c/strong\u003e) BOPP and (\u003cstrong\u003ee\u003c/strong\u003e) BOPP/0.1 wt% API composite films. (\u003cstrong\u003ef\u003c/strong\u003e) Discharge energy density and charge-discharge Coulomb efficiency of BOPP/API composite films with different contents under various electric fields. (\u003cstrong\u003eg\u003c/strong\u003e) Discharged energy density and efficiency versus charge-discharge cycle number for BOPP/0.1 wt% API films measured at 200 MV m\u003csup\u003e-1\u003c/sup\u003e.\u003c/p\u003e","description":"","filename":"Picture4.jpg","url":"https://assets-eu.researchsquare.com/files/rs-6303672/v1/24897992ca864a1c6112fc8f.jpg"},{"id":79235861,"identity":"52950153-e913-47b7-8068-20de0ab539b6","added_by":"auto","created_at":"2025-03-26 04:06:25","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2136582,"visible":true,"origin":"","legend":"","description":"","filename":"ManuscriptPreprint.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6303672/v1_covered_3edf11a9-c3cb-47b3-b3a6-7f35e76068b2.pdf"},{"id":79234942,"identity":"ba7bfd23-36ae-43f7-91ab-b2afc7d573a2","added_by":"auto","created_at":"2025-03-26 03:50:22","extension":"pdf","order_by":1,"title":"","display":"","copyAsset":false,"role":"supplement","size":2739196,"visible":true,"origin":"","legend":"","description":"","filename":"SupportingInformationPreprint.pdf","url":"https://assets-eu.researchsquare.com/files/rs-6303672/v1/cab1f4699d0babd9ccca6d82.pdf"}],"financialInterests":"The authors declare no competing interests.","formattedTitle":"\u003cp\u003e\u003cstrong\u003eLamellar Aromatic Polyimine with Strong Self-Trapped Excitons for Efficient Capacitive Energy Storage\u003c/strong\u003e\u003c/p\u003e","fulltext":[],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":false,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":true,"hideJournal":true,"highlight":"","institution":"Sichuan University","isAcceptedByJournal":false,"isAuthorSuppliedPdf":true,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":true,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"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},"keywords":"Dielectric polymer, Film capacitors","lastPublishedDoi":"10.21203/rs.3.rs-6303672/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-6303672/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eSolid film capacitors play a crucial role in the modern electrical and electronic industry, with organic polymer materials dominating the market owing to their cost-effectiveness and exceptional processability. However, the low dielectric constants of current polymers gradually fail to meet the increasing demands for high energy density of capacitors. Improving the energy storage capacity of polymer films is imperative yet very challenging. This work synthesizes an aromatic polyimine (API) with high crystallinity and unique electronic structures, which experimentally demonstrate outstanding charge storage capacity. The simple synthesis procedures of APIs allow for large-scale production at a low cost. The obtained API exhibits a typical layered crystal structure, which can be further exfoliated into quasi-two-dimensional lamellar nanoflakes via direct sonication. Notably, API undergoes a self-trapped transition band state due to the strong electron-phonon coupling at room temperature, imparting reliable charge capture ability under high electric field strength. As a result, incorporating a small amount of lamellar API into biaxially oriented polypropylene film can significantly enhance their energy storage density. This work introduces a novel crystalline polymer with exceptional charge capture and storage capabilities, providing a new avenue for the development of next-generation polymer film capacitors.\u003c/p\u003e","manuscriptTitle":"Lamellar Aromatic Polyimine with Strong Self-Trapped Excitons for Efficient Capacitive Energy Storage","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-03-26 03:50:17","doi":"10.21203/rs.3.rs-6303672/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":"6a6504c7-c4b9-43bc-a7aa-7a4b4f5b26bc","owner":[],"postedDate":"March 26th, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[{"id":46186879,"name":"Polymer Science"}],"tags":[],"updatedAt":"2025-03-26T03:50:17+00:00","versionOfRecord":[],"versionCreatedAt":"2025-03-26 03:50:17","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-6303672","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-6303672","identity":"rs-6303672","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}