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Steering S-scheme charge transfer via interfacial dipoles induced by amine-containing polyelectrolytes

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Abstract

The lack of a robust interfacial driving source over multicomponent photocatalysts is an essential contributor to the sluggish spatial charge transfer across the heterointerface and severe carrier recombination, thereby rendering maneuvering charge transfer of composite materials a thorny issue. Herein, we demonstrate an electric dipole moment-driven charge transfer photosystem utilizing amine-containing polyfluorene polyelectrolyte (i.e., PFN) and inorganic semiconductor matrices (i.e., WO3) as the building blocks to direct the interfacial charge transfer, effectively targeting the photoexcited charge carriers to the active sites. Experimental results and theoretical simulations reveal that the electronic coupling interaction between the pendant electron-rich amine groups along the PFN backbone and WO3 surface enables the nonuniform charge distribution at the interface over the WO3@PFN heterojunction, which ultimately fosters the formation of interfacial dipoles oriented from conjugated macromolecular backbone of PFN to the surface of WO3 matrices. The interfacial dipoles with excellent charge transfer kinetics spontaneously activate the unidirectional and accelerated S-scheme charge motion from the WO3 framework to the conjugated chain of PFN due to the suitable band offsets at the interface, thus endowing WO3@PFN heterostructures with a significantly enhanced net efficiency of photoactivity. These findings would provide some insights into the design of advanced heterojunction photocatalysts for solar energy conversion as well as the study of the working mechanism of polyelectrolyte interlayers in optoelectronic devices.

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Acknowledgements

The authors are grateful to the financial support from the Guangdong International Science and Technology Cooperation Foundation (2020A0505100002), the 111 Project (BP0618009), the China Scholarship Council, Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials (2019B121205002), the RGC Senior Research Fellowship Scheme (SRFS2021-5S01), the Hong Kong Research Grants Council (PolyU 15307321), Research Institute for Smart Energy (CDAQ) and Miss Clarea Au for the Endowed Professorship in Energy (847S). The authors would like to thank Miss Hanbo Yang from Imperial College London for wealthy discussion and helpful advice for the paper.

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Authors and Affiliations

  1. Institute of Polymer Optoelectronic Materials and Devices, State Key Laboratory of Luminescent Materials and Devices, School of Material Science and Engineering, South China University of Technology, Guangzhou, 510640, China

    Tao Li, Chuang Feng, Xuhui Zhu & Zhicai He

  2. Department of Applied Biology & Chemical Technology and Research Institute for Smart Energy, The Hong Kong Polytechnic University, Hung Hom, Hong Kong, China

    Biquan Xiong & Wai-Yeung Wong

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  1. Tao Li
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  2. Chuang Feng
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  3. Biquan Xiong
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  4. Xuhui Zhu
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  5. Zhicai He
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  6. Wai-Yeung Wong
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Correspondence to Zhicai He or Wai-Yeung Wong.

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The supporting information is available online at https://chem.scichina.com and https://link.springer.com/journal/11426. The supporting materials are published as submitted, without typesetting or editing. The responsibility for scientific accuracy and content remains entirely with the authors.

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Li, T., Feng, C., Xiong, B. et al. Steering S-scheme charge transfer via interfacial dipoles induced by amine-containing polyelectrolytes. Sci. China Chem. 66, 2098–2108 (2023). https://doi.org/10.1007/s11426-023-1652-7

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  • DOI: https://doi.org/10.1007/s11426-023-1652-7

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