Affiliation:
1. Department of Materials Science and Technology, University of Crete, 70013 Heraklion, Greece
Abstract
The development of functional catalysts for the photogeneration of hydrogen (H2) via water-splitting is crucial in the pursuit of sustainable energy solutions. To that end, metal-sulfide semiconductors, such as CdS and ZnS, can play a significant role in the process due to their interesting optoelectronic and catalytic properties. However, inefficient charge-carrier dissociation and poor photochemical stability remain significant limitations to photocatalytic efficiency. Herein, dual-semiconductor nanocomposites of ZnS/CdS nanocrystal assemblies (NCAs) are developed as efficient visible light photocatalysts for H2 generation. The resultant materials, synthesized via a polymer-templated self-polymerization method, comprise a unique combination of ~5–7 nm-sized metal-sulfide nanoparticles that are interlinked to form a 3D open-pore structure with large internal surface area (up to 285 m2 g−1) and uniform pores (circa 6–7 nm). By adjusting the ratio of constituent nanoparticles, the optimized ZnS/CdS catalyst with 50 wt.% ZnS content demonstrates a remarkable stability and visible light H2-evolution activity (~29 mmol g−1 h−1 mass activity) with an apparent quantum yield (AQY) of 60% at 420 nm. Photocatalytic evaluation experiments combined with electrochemical and spectroscopic studies suggest that the superior photocatalytic performance of these materials stems from the accessible 3D open-pore structure and the efficient defect-mediated charge transfer mechanism at the ZnS/CdS nanointerfaces. Overall, this work provides a new perspective for designing functional and stable photocatalytic materials for sustainable H2 production.
Funder
Hellenic Foundation for Research and Innovation
Special Account for Research Funds of University of Crete
Subject
General Materials Science,General Chemical Engineering
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