Plasmonic
photocatalyst of Au nanoparticle-decorated hollow mesoporous
TiO2 with 0, 0.1, 0.25, 0.5, and 1% Au content was successfully
synthesized by a hydrothermal method. Controlling the particle size
of Au coated on TiO2 hollow microspheres (AuTHMSs) is expected
to improve the photocatalytic ability. Our results of X-ray absorption
spectroscopy (XAS) indicated that the coated Au ions are nulvalent
and cause a lattice distortion as well as a variation in Ti 3d orbital
orientation. It is also inferred that TiO6 octahedral symmetry
is significantly affected by the Au incorporation, giving rise to
an increase in the Ti 3d t2g unoccupied state. UV–visible
absorption spectra and I–V measurements were performed to examine localized surface plasmon
resonance (LSPR) effect and photoelectrocatalytic (PEC) ability. We
present the first in situ XAS measurements on AuTHMS system, which
enabled us to correlate the electronic structure and photocatalytic
property of the material. An analysis of the results showed an LSPR
effect triggered by the Au nanoparticles that provided a conductive
path to the excited charge carriers, resulting in an enhanced photocurrent
due to the charge transfer from Au 5d to Ti 3d orbitals under solar
illumination. The photocurrent density of AuTHMSs showed an increase
with Au content with a maximum for 0.5% Au, whereas in the case of
1% Au the photocurrent profile was similar to the 0% Au. Furthermore,
a comparison of the XAS and PEC performance implied that the lattice
distortion and the corresponding symmetry changes together with the
size of Au particle substantially influenced the rate of hot electron
charge transfer, resulting in the variation of PEC activity of AuTHMS
samples with a higher activity for 0.5% Au. Our studies are expected
to fabricate chemically stable innovative structures with enhanced
surface area that would boost the photocatalytic efficiency, which
is a vital factor for environmental and energy applications.
Ultrafine fluorescent gold nanoclusters (AuNC) have emerged as biocompatible nanoprobes of biomedical imaging in vivo and precision surface chemistry of AuNCs was the key for bridging their clinical application. Comparison...
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