Active Intermediates in Plasmon-Induced Water Oxidation
at Au Nanodimer Structures on a Single Crystal of TiO2
Posted on 2020-03-24 - 16:10
The
photoinduced water-splitting reaction is a promising approach
for converting sustainable sunlight into chemical energy. However,
the high overpotential for traditional metal catalysts to drive oxygen
evolution limits the conversion efficiency. Plasmonic metal–semiconductor
systems can potentially overcome this problem, as hot electrons generated
by localized surface plasmon resonance are rapidly injected into the
semiconductor and hot holes are concentrated to oxidize water. The
intermediates and pathways of such plasmon-induced water oxidation
are currently unknown. Herein, taking Au-nanostructured TiO2 as a prototype, we investigated distinct spectral characteristics
of water oxidation intermediates at electrochemical potentials close
to the flat-band potential of TiO2 using in situ electrochemical surface-enhanced Raman spectroscopy. Au–O
stretching vibrations are attributed to the initial oxidized-state
intermediate Au(OH)3 at pH 0 or 13 and the highest-energy
intermediate AuOOH at pH 7. The existence of AuOOH provides the first
robust experimental evidence for the accelerated four-electron multistep
reaction via plasmon-assisted water oxidation.
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Suzuki, Kentaro; Li, Xiaowei; Wang, Yuchun; Nagasawa, Fumika; Murakoshi, Kei (2020). Active Intermediates in Plasmon-Induced Water Oxidation
at Au Nanodimer Structures on a Single Crystal of TiO2. ACS Publications. Collection. https://doi.org/10.1021/acsenergylett.0c00478