{"paper_id":"36739b4b-8752-4338-9b81-5a65313fd190","body_text":"Flexible π-stacked organic frameworks with dynamic electronic interactions for highly efficient photocatalytic hydrogen evolution | 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 Flexible π-stacked organic frameworks with dynamic electronic interactions for highly efficient photocatalytic hydrogen evolution Shu Hu, Yang Yang, Dong Meng, Yuzhang Li, Philippe Sautet, Ran Zheng, and 22 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6890653/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 There is growing interest in using light-responsive soft matter with dynamic noncovalent bonding for solar-driven fuel production. Here, we report a supramolecular organic light absorber, the π-stacked organic framework (πOF-1), formed through the self-assembly of π-conjugated photoactive units via dynamic π-π interactions. Its building blocks incorporate flexible and nonfused organic rings with strong visible-light absorption, along with hydrophilic side groups that form high surface-area inner pores and uniformly distributed micropores (~1.8 nm in size). In aqueous surfactant dispersions, πOF-1 forms stable particles that anchor platinum clusters on both internal and external surfaces via photodeposition. Under 1-sun illumination at 70 °C, πOF-1 achieves a record-high hydrogen evolution rate of 618 mmol h-1 g-1, corresponding to an averaged internal quantum efficiency of 17.7% at 450-750 nm range. The performance at elevated temperatures is enabled by dynamic π-stacked networks, which facilitate efficient exciton dissociation and charge transfer via interactions between heterocyclic rings and platinum clusters. For energy conversion and photosynthesis, πOF-1 photocatalysts offer a compelling alternative to traditional soft-matter systems such as covalent organic frameworks, metal-ligand coordination frameworks, or densely packed crystalline semiconductors. Physical sciences/Chemistry/Supramolecular chemistry/Self-assembly Physical sciences/Chemistry/Catalysis/Photocatalysis Physical sciences/Chemistry/Photochemistry/Photocatalysis Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryinformationFinal.docx Supplementary Information file SupplementaryVideo1.mp4 Supplementary Video 1 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. 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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-6890653\",\"acceptedTermsAndConditions\":true,\"allowDirectSubmit\":true,\"archivedVersions\":[],\"articleType\":\"Article\",\"associatedPublications\":[],\"authors\":[{\"id\":476991462,\"identity\":\"25b6ba95-68e6-4758-9f0b-8fa881539e18\",\"order_by\":0,\"name\":\"Shu 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