Direct encapsulation of graphene
shells on noble metal nanoparticles
via chemical vapor deposition (CVD) has been recently reported as
a unique way to design and fabricate new plasmonic heterostructures.
But currently, the fundamental nature of the growth mechanism of graphene
layers on metal nanostructures is still unknown. Herein, we report
a systematic investigation on the CVD growth of graphene-encapsulated
Au nanoparticles (Au@G) by combining an experimental parameter study
and theoretical modeling. We studied the effect of growth temperature,
duration, hydrocarbon precursor concentration, and extent of reducing
(H2) environment on the morphology of the products. In
addition, the influence of plasma oxidation conditions for the surface
oxidation of gold nanoparticles on the graphene shell growth is evaluated
in combination with thermodynamic calculations. We find that these
parameters critically aid in the evolution of graphene shells around
gold nanoparticles and allow for controlling shell thickness, graphene
shell quality and morphology, and hybrid nanoparticle diameter. An
optimized condition including the growth temperature of ∼675
°C, duration of 30 min, and xylene feed rate of ∼10 mL/h
with 10% H2/Ar carrier gas was finally obtained for the
best morphology evolution. We further performed finite-element analysis
(FEA) simulations to understand the equivalent von Mises stress distribution
and discrete dipolar approximation (DDA) calculation to reveal the
optical properties of such new core–shell heterostructures.
This study brings new insight to the nature of CVD mechanism of Au@G
and might help guiding their controlled growth and future design and
application in plasmonic applications.