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Converting water into hydrogen fuel and oxidizing benzyl alcohol to benzaldehyde simultaneously under visible light illumination is of great significance, but the fast recombination of photogenerated carriers in photocatalysts seriously decreases the conversion efficiency. Herein, a novel dual-functional 0D Cd0.5Zn0.5S/2D Ti3C2 hybrid was fabricated by a solvothermally in-situ generated assembling method. The Cd0.5Zn0.5S nano-spheres with a fluffy surface completely and uniformly covered the ultrathin Ti3C2 nanosheets, leading to the increased Schottky barrier (SB) sites due to a large contact area, which could accelerate the electron-hole separation and improve the light utilization. The optimized Cd0.5Zn0.5S/Ti3C2 hybrid simultaneously presents a hydrogen evolution rate of 5.3 mmol/(g·h) and a benzaldehyde production rate of 29.3 mmol/(g·h), which are ~3.2 and 2 times higher than those of pristine Cd0.5Zn0.5S, respectively. Both the multiple experimental measurements and the density functional theory (DFT) calculations further demonstrate the tight connection between Cd0.5Zn0.5S and Ti3C2, formation of Schottky junction, and efficient photogenerated electron-hole separation. This paper suggests a dual-functional composite catalyst for photocatalytic hydrogen evolution and benzaldehyde production, and provides a new strategy for preventing the photogenerated electrons and holes from recombining by constructing a 0D/2D heterojunction with increased SB sites.


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Efficient photocatalytic hydrogen evolution coupled with benzaldehyde production over 0D Cd0.5Zn0.5S/2D Ti3C2 Schottky heterojunction

Show Author's information Junnan TAOa,Mingyuan WANGb,Guiwu LIUa( )Qinqin LIUaLei LUaNeng WANbHua TANGc( )Guanjun QIAOa
School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, China
SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of Ministry of Education, School of Electrical Science and Engineering, Southeast University, Nanjing 210096, China
School of Environmental Science and Engineering, Qingdao University, Qingdao 266071, China

† Junnan Tao and Mingyuan Wang contributed equally to this work.

Abstract

Converting water into hydrogen fuel and oxidizing benzyl alcohol to benzaldehyde simultaneously under visible light illumination is of great significance, but the fast recombination of photogenerated carriers in photocatalysts seriously decreases the conversion efficiency. Herein, a novel dual-functional 0D Cd0.5Zn0.5S/2D Ti3C2 hybrid was fabricated by a solvothermally in-situ generated assembling method. The Cd0.5Zn0.5S nano-spheres with a fluffy surface completely and uniformly covered the ultrathin Ti3C2 nanosheets, leading to the increased Schottky barrier (SB) sites due to a large contact area, which could accelerate the electron-hole separation and improve the light utilization. The optimized Cd0.5Zn0.5S/Ti3C2 hybrid simultaneously presents a hydrogen evolution rate of 5.3 mmol/(g·h) and a benzaldehyde production rate of 29.3 mmol/(g·h), which are ~3.2 and 2 times higher than those of pristine Cd0.5Zn0.5S, respectively. Both the multiple experimental measurements and the density functional theory (DFT) calculations further demonstrate the tight connection between Cd0.5Zn0.5S and Ti3C2, formation of Schottky junction, and efficient photogenerated electron-hole separation. This paper suggests a dual-functional composite catalyst for photocatalytic hydrogen evolution and benzaldehyde production, and provides a new strategy for preventing the photogenerated electrons and holes from recombining by constructing a 0D/2D heterojunction with increased SB sites.

Keywords: photocatalysis, hydrogen, benzaldehyde, Schottky heterojunction, Cd0.5Zn0.5S, Ti3C2

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Publication history

Received: 21 January 2022
Revised: 30 March 2022
Accepted: 07 April 2022
Published: 04 June 2022
Issue date: July 2022

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© The Author(s) 2022.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant Nos. 51902137 and 51672113), the Key Research and Development Plan (Grant No. BE2019094), and the Qing Lan Project ([2016]15) of Jiangsu Province. The calculations were carried out by the Advanced Computing East China Sub-center and Big Data Center of Southeast University.

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