Conjugating plasmonic metals with catalytically active materials with controlled configurations can harness their light energy harvesting ability in catalysis. Herein, we present a well-defined core−shell nanostructure composed of an octahedral Au nanocrystal core and a PdPt alloy shell as a bifunctional energy conversion platform for plasmon-enhanced electrocatalysis. The prepared Au@PdPt core−shell nanostructures exhibited significant enhancements in electrocatalytic activity for methanol oxidation and oxygen reduction reactions under visible-light irradiation. Our experimental and computational studies revealed that the electronic hybridization of Pd and Pt allows the alloy material to have a large imaginary dielectric function, which can efficiently induce the shellbiased distribution of plasmon energy upon illumination and, hence, its relaxation at the catalytically active region to promote electrocatalysis.
The rational design and synthesis
of multimetallic hollow nanostructures
(HNSs) have been attracting great attention due to their structural
and compositional advantages for application in electrocatalysis.
Herein, the one-pot synthesis of Pd–Pt–Ag ternary alloy
HNSs with controllable morphologies through a self-templating approach
without any pre-synthesized templates is reported. Simultaneous reduction
of multiple metal precursors by ascorbic acid in the presence of cetyltrimethylammonium
chloride (CTAC) yielded initially metastable Pd–Ag nanocrystals,
which can act as a self-template, and subsequent galvanic replacement
and reduction led to the formation of final Pd–Pt–Ag
HNSs. The size and hollowness (the ratio of inner cavity diameter
to outer diameter) of the HNSs could be tuned through control over
the concentration of CTAC. This can be attributed to the manipulated
reduction kinetics of multiple metal precursors with the change in
the CTAC concentration. The prepared Pd–Pt–Ag HNSs exhibited
improved catalytic performance for ethanol electro-oxidation due to
their large active surface areas and ternary alloy composition.
Regarding the design of high-performance solar energy conversion platforms, heteronanostructured photocatalysts consisting of plasmonic metals and semiconductors are of particular interest due to their capability for the conversion of solar...
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