Field-channel synergistic engineering in gradient-doped 2D overlayers for high-efficiency solar water splitting

Field-channel synergistic engineering in gradient-doped 2D overlayers for high-efficiency solar water splitting | 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 Field-channel synergistic engineering in gradient-doped 2D overlayers for high-efficiency solar water splitting Yang Cao, Xin Ding, Keng Chen, Hengjun Xie, Tongxin Tang, Wenhao Zou, and 6 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-9089829/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 Achieving high solar-to-hydrogen (STH) efficiency in photoelectrochemical (PEC) water splitting is fundamentally limited by the challenge of simultaneously optimizing light absorption and charge separation in photoanodes. Herein, we overcome this bottleneck by fabricating ~20 nm thick B:C3N5-x nanosheets featuring a macroscopic gradient of B dopants and N vacancies on Mo:BVO via a substrate-mediated stabilization strategy. This unique architecture not only broadens the visible-light absorption range of BiVO4 (BVO), but also establishes a robust macroscopic dipole field. Originating from the breaking of inversion symmetry and synergistically reinforced by localized interlayer B-N bonding, this dipole field provides a powerful internal driving force for ultrafast carrier separation. Consequently, achieving a record 2.89% ABPE, the Mo:BVO/B:C3N5-x/NiFeBi photoanode delivers an outstanding 8.52% STH efficiency in tandem with a perovskite solar cell. This work demonstrates that combining gradient engineering with interlayer coupling effectively reconciles the intrinsic trade-off between optical thickness and charge extraction. Furthermore, this strategy presents a versatile blueprint for rationally designing of complex 2D/3D heterostructures for next-generation solar energy conversion and related applications. Physical sciences/Energy science and technology/Renewable energy/Hydrogen energy Physical sciences/Materials science/Nanoscale materials/Two-dimensional materials Physical sciences/Chemistry/Photochemistry/Photocatalysis Full Text Additional Declarations There is NO Competing Interest. The authors declare no competing interests. Supplementary Files SourceData.xlsx Source Data ManuscriptSI.docx Supplementary information 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. 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