4.7 Article

A nano heterostructure with step-accelerated system toward optimized photocatalytic hydrogen evolution

Journal

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
Volume 47, Issue 3, Pages 1656-1668

Publisher

PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2021.10.143

Keywords

Nano heterostructure; Step-accelerated system; Quantum dots; Hollow spherical graphite carbon nitride; Photocatalytic hydrogen evolution

Funding

  1. National Natural Science Foundation of China [52173158, 32171725]
  2. Key Research and Development Program of Jiangsu Province [BE2021081]
  3. Postgraduate Research & Practice Innovation Program of Jiangsu Province [KYCX20_0125]
  4. Fund Project for Transformation of Sci-entific and Technological Achievements of Jiangsu Province of China [BA2019054, BA2021044]

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This study constructs a unique nano heterostructure for efficient photocatalytic hydrogen evolution, with significantly improved hydrogen evolution rate. Experimental results are supported by analysis of ultrafast TA spectroscopy, electrochemical measurements, and density functional theory calculations, revealing the crucial role of structure in electron transfer efficiency.
Adequate light absorption and high carrier separation/transfer efficiency are central to elevate the development of highly efficient photocatalytic hydrogen evolution. Herein, a unique nano heterostructure is constructed by translocating 0D CdSe@(Zn, Cd)Se@ZnS quantum dots (CSS QDs) into the 3D hollow spherical graphite carbon nitride (SCN). The ultrafast TA spectroscopy and electrochemical measurements were measured to reveal the enhanced surface dependent electron transfer efficiency. Besides, the density functional theory (DFT) calculations further explained the mechanism of electrons transfer between interfaces. As expected, benefiting from the structural advantages of SCN and the channel driven effectiveness produced by a step-accelerated system which is composed of (Zn, Cd)Se and ZnS double-shell layers of CSS QDs, the optimal hydrogen evolution rate of the prepared material in the photocatalytic hydrogen evolution reaction reached 132.5 mmol h(-1), which was 7.6 times higher than that of the pure SCN under visible light irradiation. This work provides a novel avenue into the construction of nano heterostructure for solar hydrogen evolution. (C) 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

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