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Electrochemical synthesis of Au@semiconductor core-shell nanocrystals guided by single particle plasmonic imaging.

ABSTRACT: Plasmonic photocatalysts have opened up a new direction in utilization of visible light and promoting photocatalytic efficiency. An electrochemical deposition method is reported to synthesise metal@semiconductor (M@SC) core-shell nanocrystals. Due to the strong affinity of Au atoms to S2- and Se2- reduced at negative potential, CdS, CdSe and ZnS were selectively deposited on the surface of the Au core to form a uniform shell with a clear metal/semiconductor interface, which conquered the barrier caused by the large lattice mismatch between the two components. Plasmonic effects increased the photocatalytic performance, as well as provided a chance to in situ monitor the surface nucleation and growth. The structure formation process could be observed under dark-field microscopy (DFM) in real-time and precisely controlled via the scattering color, intensity and wavelength. The proof-of-concept strategy combines the electrochemical deposition and plasmonic imaging, which provides a universal approach in controllable synthesis of core-shell heterostructures, and leads to the improvement of plasmonic photocatalysts.

SUBMITTER: Wang H

PROVIDER: S-EPMC7006628 | biostudies-literature | 2019 Oct

REPOSITORIES: biostudies-literature

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Electrochemical synthesis of Au@semiconductor core-shell nanocrystals guided by single particle plasmonic imaging.

Wang Hui H Zhao Wei W Xu Cong-Hui CH Chen Hong-Yuan HY Xu Jing-Juan JJ

Chemical science 20190813 40

Plasmonic photocatalysts have opened up a new direction in utilization of visible light and promoting photocatalytic efficiency. An electrochemical deposition method is reported to synthesise metal@semiconductor (M@SC) core-shell nanocrystals. Due to the strong affinity of Au atoms to S<sup>2-</sup> and Se<sup>2-</sup> reduced at negative potential, CdS, CdSe and ZnS were selectively deposited on the surface of the Au core to form a uniform shell with a clear metal/semiconductor interface, which ...[more]

PMID: 32110293

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Project description:Integration of plasmonic nanoantennas with catalytically active reactors in deliberately designed hybrid supra-nanostructures creates a dual-functional materials platform, based upon which precise modulation of catalytic reaction kinetics becomes accomplishable through optical excitations of plasmon resonances. Here, we have developed a multistep synthetic approach that enables us to assemble colloidal Au@C/Pt core@shell/satellite supra-nanostructures, in which the Au core functions as a light-harvesting plasmonic nanoantenna, the Pt satellites act as catalytically active reactors, and the C shell serves as a nanoscale dielectric spacer separating the reactors from the antenna, respectively. By adjusting several synthetic parameters, the size of the Au core, the thickness of the C shell, and the surface coverage of Pt satellites can all be tuned independently. Choosing Pt-catalyzed cascade oxidation of 3,3',5,5'-tetramethylbenzidine in an aerobic aqueous environment as a model reaction, we have systematically studied the detailed kinetic features of the catalytic reactions both in the dark and under visible light illumination over a broad range of reaction conditions, which sheds light on the interplay between plasmonic and catalytic effects in these antenna-reactor nanohybrids. The plasmonic antenna effect can be effectively harnessed to kinetically modulate multiple crucial steps during the cascade reactions, benefiting from plasmon-enhanced interband electronic transitions in the Pt satellites and plasmon-enhanced intramolecular electronic excitations in chromogenic intermediate species. In addition to the plasmonic antenna effect, photothermal transduction derived from plasmonic excitations can also provide significant contributions to the kinetic enhancements under visible light illumination. The knowledge gained from this work serves as important guiding principles for rational design and structural optimization of plasmonic antenna-reactor hybrid nanomaterials, endowing us with enhanced capabilities to kinetically modulate targeted catalytic/photocatalytic molecule-transforming processes through light illumination.

Dataset Information

Electrochemical synthesis of Au@semiconductor core-shell nanocrystals guided by single particle plasmonic imaging.

Publications

Electrochemical synthesis of Au@semiconductor core-shell nanocrystals guided by single particle plasmonic imaging.

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