Interfacial
Structure-Modulated Plasmon-Induced Water
Oxidation on Strontium Titanate
Posted on 2020-06-11 - 20:31
Plasmon-induced
carrier transfer at metallic nanoparticle/semiconductor
heterojunctions has received great attention because of its tremendous
potential in applications, such as photocatalysis and photoelectric
and energy conversion. The interfacial structure of the heterojunction
is known to play an important role in charge transfer as well as the
subsequent chemical reactions. Here, we studied the Au nanoparticle
(Au-NP)-loaded (100)-, (110)-, and (111)-oriented single-crystalline
strontium titanate (STO) as a model to investigate the effects of
interfacial structure on the plasmon-induced charge separation between
the metallic nanoparticles and semiconductors. Via photoelectrochemical characterizations, we found that the efficiency
of the plasmon-induced water oxidation reaction on STO(100) is more
than 1.4 times higher than that on the other two orientation facets.
This enhancement was demonstrated to stem from the high oxidation
ability of plasmon-induced holes captured in the surface states. Furthermore,
the molecular processes of water oxidation were investigated by monitoring
the surface oxidation status of Au-NP/STO as intermediates of plasmon-induced
water oxidation using in situ electrochemical surface-enhanced
Raman spectroscopy. The onset potential of Au–O vibrations
on Au-NP/STO(100) was determined to be 0.4 V more negative than that
of Au-NP/STO(110), further confirming the higher oxidation ability
of the plasmon-induced holes. Our observation provides an opportunity
to efficiently modulate plasmon-excited hot-carrier reaction processes
for photochemical applications through interfacial engineering.
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Shi, Xu; Li, Xiaowei; Toda, Takahiro; Oshikiri, Tomoya; Ueno, Kosei; Suzuki, Kentaro; et al. (2020). Interfacial
Structure-Modulated Plasmon-Induced Water
Oxidation on Strontium Titanate. ACS Publications. Collection. https://doi.org/10.1021/acsaem.0c00648