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Laser illumination-induced dramatic catalytic activity change on Au nanospheres.

ABSTRACT: Understanding morphology dependent catalytic kinetics from a single nanoparticle plays a significant role in the development of robust nano-catalysts with high efficiency. Unfortunately, detailed knowledge of the morphology dependent catalytic properties of single nanoparticles after shape transitions is lacking. In this work, the distinct catalytic properties of a single gold nanoparticle (GNP) after symmetry breaking were disclosed at the single-particle level for the first time. The morphology of the spherical GNP was elongated into a rod shape (i.e., gold nanorod, GNR) with a tightly focused Gaussian laser beam based on the photothermal effect. By using the fluorogenic oxidation reaction (i.e., amplex red to resorufin) as a model reaction, noticeable variation in catalytic efficiency after the shape modulation process was found at the single-particle level. The GNP displays noticeably higher catalytic efficiency which might be ascribed to the heterogeneous lattice structure on the particle surface as confirmed by transmission electron microscopy (TEM) characterization. Rearrangement of surface atoms after shape modulation normally generates a more ordered crystal structure, resulting in a lower surface energy for catalytic reaction. However, both of these nanoparticles still exhibit dynamic activity fluctuation in a temporal dependent route, indicating a distinct spontaneous dynamic surface restructuring process. These kinetic evidences might facilitate the development nanoparticle-based heterogeneous catalysts, particularly based on the morphology effect.

SUBMITTER: Ye Z

PROVIDER: S-EPMC6568046 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Laser illumination-induced dramatic catalytic activity change on Au nanospheres.

Ye Zhongju Z Wei Lin L Xiao Lehui L Wang Jianfang J

Chemical science 20190429 22

Understanding morphology dependent catalytic kinetics from a single nanoparticle plays a significant role in the development of robust nano-catalysts with high efficiency. Unfortunately, detailed knowledge of the morphology dependent catalytic properties of single nanoparticles after shape transitions is lacking. In this work, the distinct catalytic properties of a single gold nanoparticle (GNP) after symmetry breaking were disclosed at the single-particle level for the first time. The morpholog ...[more]

PMID: 31293767

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Project description:In this work we investigated methods of modifying gold nanospheres bound to a silicon surface by depositing palladium onto the surfaces of single nanoparticles. Bimetallic Au-Pd nanoparticles can thus be gained for use in catalysis or sensor technology. For Pd deposition, two methods were chosen. The first method was the reduction of palladium acetate by ascorbic acid, in which the amounts of palladium acetate and ascorbic acid were varied. In the second method we utilized light-induced metal deposition by making use of the plasmonic effect. Through this method, the surface bond nanoparticles were irradiated with light of wavelengths capable of inducing plasmon resonance. The generation of hot electrons on the particle surface then reduced the palladium acetate in the vicinity of the gold nanoparticle, resulting in palladium-covered gold nanospheres. In our studies we demonstrated the effect of both enhancement methods by monitoring the particle heights over enhancement time by atomic force microscopy (AFM), and investigated the influence of ascorbic acid/Pd acetate concentration as well as the impact of the irradiated wavelengths on the enhancement effect. It could thus be proven that both methods were valid for obtaining a deposition of Pd on the surface of the gold nanoparticles. Deposition of Pd on the gold particles using the light-assisted method could be observed, indicating the impact of the plasmonic effect and hot electron for Pd acetate reduction on the gold particle surface. In the case of the reduction method with ascorbic acid, in addition to Pd deposition on the gold nanoparticle surface, larger pure Pd particles and extended clusters were also generated. The reduction with ascorbic acid however led to a considerably thicker Pd layer of up to 54 nm in comparison to up to 11 nm for the light-induced metal deposition with light resonant to the particle absorption wavelength. Likewise, it could be demonstrated that light of non-resonant wavelengths was not capable of initiating Pd deposition, since a growth of only 1.6 nm (maximum) was observed for the Pd layer.

Dataset Information

Laser illumination-induced dramatic catalytic activity change on Au nanospheres.

Publications

Laser illumination-induced dramatic catalytic activity change on Au nanospheres.

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