In Situ Monitoring of Individual Plasmonic Nanoparticles
Resolves Multistep Nanoscale Sulfidation Reactions Hidden by Ensemble
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Posted on 2019-09-10 - 14:56
The generation of
complex nanostructures to obtain novel characteristics
and improved performance has been achieved by coupling multiple nanoscale
reactions. Because reactions at the nanometer scale directly govern
the morphology of nanostructures, understanding the reaction mechanism
is critical to precisely control the morphology and, eventually, the
physicochemical properties of the materials. However, because of the
ensemble-average effect, investigating the reaction mechanism at the
bulk level does not provide sufficient information. In this study,
we investigated the overall sulfidation reaction mechanism that occurred
on individual silver nanocubes in real time at high temperature. Using
the single-particle dark-field imaging technique, three discrete steps
of the sulfidation reaction were clearly resolved in the profiles
of the plasmon peak shift and the intensity change of individual particles
according to time progress: (I) reactant diffusion to the silver surface
by passing through a ligand barrier, (II) silver sulfide formation
by C–S bond cleavage of cysteine molecules, and (III) diffusion
of silver atoms in the silver sulfide layer until the complete formation
of silver sulfide. By a combination of simulation and control experiments,
physical constants were derived for each step, which is completely
hidden in the ensemble measurements. Each individual nanoparticle
exhibited a large variation of physical values, such as the reaction
rate constant and diffusivity, mainly resulting from the intrinsic
structural heterogeneity. Dark-field microscopy image processing based
on surface plasmon scattering would be helpful to analyze the reaction
kinetics and understand the reaction mechanisms of the numerous multistep
nanoscale reactions in real time with high spatial and temporal resolutions
under actual reaction conditions.
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Park, Youngchan; Oh, Hyuncheol; Park, Jiseong; Choi, Woong; Ryu, Hyein; Seo, Daeha; et al. (2019). In Situ Monitoring of Individual Plasmonic Nanoparticles
Resolves Multistep Nanoscale Sulfidation Reactions Hidden by Ensemble
Average. ACS Publications. Collection. https://doi.org/10.1021/acs.jpcc.9b05630
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AUTHORS (7)
YP
Youngchan Park
HO
Hyuncheol Oh
JP
Jiseong Park
WC
Woong Choi
HR
Hyein Ryu
DS
Daeha Seo
HS
Hyunjoon Song
KEYWORDS
multistep nanoscale reactionssulfidation reaction mechanismsilver sulfide formationIndividual Plasmonic Nanoparticles Resolves Multistep Nanoscale Sulfidation Reactionsplasmon peak shiftreaction mechanismsilver sulfide layerDark-field microscopy image processingsingle-particle dark-field imaging techniqueIIIII