Journal
NANO LETTERS
Volume 17, Issue 9, Pages 5688-5694Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.7b02582
Keywords
Nanoparticles; photocatalyst; hydrogen generation; metal cocatalyst; charge recombination
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Funding
- Saudi-Aramco
- KAIST CO, management center
- Institute for Basic Science [IBS-R004-D1]
- National Research Foundation of Korea (NRF) - Korea Government (MSIP) [NRF-2015R1A2A2A01004196]
- NRF - Korea Government (MSIP) [NRF-2015R1A2A1A01004470]
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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.
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