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The diffusion, adsorption/desorption behaviors of water molecules and hydrogen molecules are of great importance in heterogeneous photocatalytic hydrogen production. In the study of structure–property–performance relationships, nanoconfined space provides an ideal platform to promote mass diffusion and transfer due to their extraordinary properties that are different from the bulk systems. Herein, we designed and prepared a nanoconfined CdS@SiO2-NH2 nanoreactor, whose shell is composed of amino-functionalized silica nanochannels, and encapsulates spherical CdS as a photocatalyst inside. Experimental and simulated results reveal that the amino-functionalized nanochannels promote water molecules’ and hydrogen molecules’ directional diffusion and transport. Water molecules are enriched in the nanocavity between the core and the shell, and promote the interfacial photocatalytic reaction. As a result, the maximized water enrichment and minimized hydrogen-occupied active sites enable photocatalyst with optimized mass transfer kinetics and localization electron distribution on the CdS surface, leading to superior hydrogen production performance with activity as high as 37.1 mmol·g−1·h−1.


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Nanoconfinement-induced water molecules and hydrogen molecules transport behaviors in ball-in-ball structure photocatalysts to improve hydrogen evolution

Show Author's information Ben ChongBaorong XuHe LiHonghui OuGuidong Yang( )
XJTU-Oxford Joint International Research Laboratory of Catalysis, School of Chemical Engineering and Technology, Xi’an Jiaotong University, Xi’an 710049, China

Abstract

The diffusion, adsorption/desorption behaviors of water molecules and hydrogen molecules are of great importance in heterogeneous photocatalytic hydrogen production. In the study of structure–property–performance relationships, nanoconfined space provides an ideal platform to promote mass diffusion and transfer due to their extraordinary properties that are different from the bulk systems. Herein, we designed and prepared a nanoconfined CdS@SiO2-NH2 nanoreactor, whose shell is composed of amino-functionalized silica nanochannels, and encapsulates spherical CdS as a photocatalyst inside. Experimental and simulated results reveal that the amino-functionalized nanochannels promote water molecules’ and hydrogen molecules’ directional diffusion and transport. Water molecules are enriched in the nanocavity between the core and the shell, and promote the interfacial photocatalytic reaction. As a result, the maximized water enrichment and minimized hydrogen-occupied active sites enable photocatalyst with optimized mass transfer kinetics and localization electron distribution on the CdS surface, leading to superior hydrogen production performance with activity as high as 37.1 mmol·g−1·h−1.

Keywords: mass transfer, photocatalytic hydrogen evolution, CdS, nanochannels, amino-functionalized

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Publication history
Copyright
Acknowledgements

Publication history

Received: 14 September 2023
Revised: 18 October 2023
Accepted: 30 October 2023
Published: 12 December 2023
Issue date: May 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 22108214) and Joint Funds of the National Natural Science Foundation of China (No. U22A20391).

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