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Photoelectrochemical (PEC) nanomaterials are critical to producing clean oxygenation or value-added chemical production by utilizing sustainable solar energy, but are always limited by simultaneous integration of architectural engineering and electronic regulation in one structure. Directed by density functional theory (DFT) calculations and finite element analysis (FEA), the bio-inspired ivy-like Fe2O3 heterostructures with enriched oxygen defects on TiO2 nanofibers are designed for boosting PEC performances. Ivy-like Fe2O3 photo-sheets remarkably enhanced the light harvesting by multiple light–mater interactions. The oxygen vacancies on Fe2O3 photo-sheets could aid the photons catching and promote the reactivity at active sites. More importantly, demonstrated by a well-designed dynamic observation, the abundant tip-edges within ivy-like Fe2O3 photo-sheets enabled the surface of heterostructure with hydrophilic and aerophobic properties. The functionalized surface allowed the rapid desorption of produced bubbles and thus ensured a high density of unoccupied active sites for electrolyte accessing. Featured by these attributes, the Fe2O3@TiO2 nanofibers delivered an excellent photocurrent of 40.8 mA/mg, high donor density (1.2 × 1018 cm−3), and rapid oxygen production rate (1 mmol/(L∙h)). This work demonstrates a new strategy on nano-structural design for enhancing light-harvesting and making a hydrophilic/aerophobic surface on low-dimensional oxide nanomaterial, holding great potential on designing high-performance PEC devices for producing survival source gas, carbon-neutral fuel, and valued-chemicals.


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Aligning Fe2O3 photo-sheets on TiO2 nanofibers with hydrophilic and aerophobic surface for boosting photoelectrochemical performance

Show Author's information Xiangyu Meng1,§Qi Zhan1,§Yanan Wu1,§Mengmeng Zhu1Ken Liu1Na Wang2Kuibo Yin3Yueming Sun1Shuai Dong2Yunqian Dai1( )
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, China
School of Physics, Southeast University, Nanjing 211189, China
SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of Ministry of Education, Southeast University, Nanjing 210096, China

§ Xiangyu Meng, Qi Zhan, and Yanan Wu contributed equally to this work.

Abstract

Photoelectrochemical (PEC) nanomaterials are critical to producing clean oxygenation or value-added chemical production by utilizing sustainable solar energy, but are always limited by simultaneous integration of architectural engineering and electronic regulation in one structure. Directed by density functional theory (DFT) calculations and finite element analysis (FEA), the bio-inspired ivy-like Fe2O3 heterostructures with enriched oxygen defects on TiO2 nanofibers are designed for boosting PEC performances. Ivy-like Fe2O3 photo-sheets remarkably enhanced the light harvesting by multiple light–mater interactions. The oxygen vacancies on Fe2O3 photo-sheets could aid the photons catching and promote the reactivity at active sites. More importantly, demonstrated by a well-designed dynamic observation, the abundant tip-edges within ivy-like Fe2O3 photo-sheets enabled the surface of heterostructure with hydrophilic and aerophobic properties. The functionalized surface allowed the rapid desorption of produced bubbles and thus ensured a high density of unoccupied active sites for electrolyte accessing. Featured by these attributes, the Fe2O3@TiO2 nanofibers delivered an excellent photocurrent of 40.8 mA/mg, high donor density (1.2 × 1018 cm−3), and rapid oxygen production rate (1 mmol/(L∙h)). This work demonstrates a new strategy on nano-structural design for enhancing light-harvesting and making a hydrophilic/aerophobic surface on low-dimensional oxide nanomaterial, holding great potential on designing high-performance PEC devices for producing survival source gas, carbon-neutral fuel, and valued-chemicals.

Keywords: electrospinning, nanofibers, TiO2, photoelectrochemical, light harvesting, Fe2O3

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Publication history
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Acknowledgements

Publication history

Received: 06 July 2022
Revised: 08 August 2022
Accepted: 09 August 2022
Published: 13 September 2022
Issue date: March 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 21975042), the Project of Six Talents Climax Foundation of Jiangsu (No. XCL-082), the Innovation Platform Project Supported by Jiangsu Province (No. 6907041203), and the Priority Academic Program Development of Jiangsu Higher Education Institutions.

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