Controlling Reaction Selectivity over Hybrid Plasmonic Nanocatalysts

Area of Science:

• Nanotechnology
• Catalysis
• Physical Chemistry

Background:

• Localized surface plasmon resonance (LSPR) in plasmonic nanoparticles accelerates visible-light-driven catalysis.
• Multimetallic nanoparticles combining plasmonic and catalytic components offer synergistic effects for enhanced catalytic activity.
• Controlling reaction selectivity in plasmonic catalysis remains a significant challenge.

Purpose of the Study:

• To demonstrate control over reaction selectivity in sequential reactions using multimetallic nanoparticles under visible light illumination.
• To investigate the role of nanoparticle architecture in dictating catalytic selectivity.
• To explore the potential of plasmonic catalysis for selective molecular transformations.

Main Methods:

• Synthesis of multimetallic nanoparticles with Au, Ag, and Pt in core-shell (Au@Ag@Pt) and nanorattle (Au@AgPt) architectures.
• Utilizing phenylacetylene hydrogenation as a model reaction for sequential transformation.
• Employing visible-light irradiation to drive the catalytic process.
• Conducting atomistic calculations to elucidate reaction mechanisms and selectivity drivers.

Main Results:

• Achieved controlled reaction selectivity in a sequential reaction under visible light using Au@Ag@Pt and Au@AgPt nanoparticles.
• Demonstrated selective hydrogenation of phenylacetylene's triple bond to styrene over further hydrogenation.
• Identified localized interaction between phenylacetylene and Pt surface as key to selectivity.
• Atomistic calculations revealed distinct adsorption configurations and charge delocalization driving selectivity.

Conclusions:

• Multimetallic nanoparticle architecture and localized interactions are crucial for controlling selectivity in plasmonic catalysis.
• Plasmonic catalysis can be harnessed to drive selective molecular transformations under visible light.
• This work contributes to the development of ecofriendly catalytic processes using visible light.