Engineering Reaction Kinetics by Tailoring the Metal Tips of Metal Semiconductor Nanodumbbells

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Semiconductor-metal hybrid nanostructures are one of the best model catalysts for understanding photocatalytic hydrogen generation. To investigate the optimal structure of metal cocatalysts, metal-CdSe-metal nanodumbbells were synthesized with three distinct sets of metal tips, Pt-CdSe-Pt, Au-CdSe-Au, and Au-CdSe-Pt. Photoelectrochemical responses and transient absorption spectra showed that the competition between the charge recombination at the metal CdSe interface and the water reduction on the metal surface is a detrimental factor for the apparent hydrogen evolution rate. For instance, a large recombination rate (k(rec)) at the Pt CdSe interface limits the quantum yield of hydrogen generation despite a superior water reduction rate (k(WR)) on the Pt surface. To suppress the recombination process, Pt was selectively deposited onto the Au tips of Au-CdSe-Au nanodumbbells in which the krec was diminished at the Au-CdSe interface, and the large k(WR) was maintained on the Pt surface. As a result, the optimal structure of the Pt -coated Au-CdSe-Au nanodumbbells reached a quantum yield of 4.84%. These findings successfully demonstrate that the rational design of a metal cocatalyst and metal-semiconductor interface can additionally enhance the catalytic performance of the photochemical hydrogen generation reactions.
Publisher
AMER CHEMICAL SOC
Issue Date
2017-09
Language
English
Article Type
Article
Keywords

PHOTOCATALYTIC H-2 GENERATION; FERMI-LEVEL EQUILIBRATION; DECORATED CDS NANORODS; HYDROGEN-PRODUCTION; ELECTRON-TRANSFER; QUANTUM RODS; HETEROSTRUCTURES; WATER; NANOPARTICLES; NANOCRYSTALS

Citation

NANO LETTERS, v.17, no.9, pp.5688 - 5694

ISSN
1530-6984
DOI
10.1021/acs.nanolett.7b02582
URI
http://hdl.handle.net/10203/226413
Appears in Collection
CH-Journal Papers(저널논문)
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