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Preparation of Silver-Palladium Alloyed Nanoparticles for Plasmonic Catalysis under Visible-Light Illumination
Published on: August 18, 2020
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Isotope Effects in Plasmonic Photosynthesis.
Sungju Yu1,2, Prashant K Jain1,3,4,5
1Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois, 61801, USA.
Angewandte Chemie (International Ed. in English)
|September 8, 2020
Summary
Identifying the initial step in plasmon-driven chemistry is crucial. This study reveals that the O-H bond scission in water is a key limiting step in plasmonic photosynthesis, using kinetic isotope effects.
Area of Science:
- Photochemistry
- Nanotechnology
- Catalysis
Background:
- Plasmonic nanoparticles enable complex chemical reactions upon light excitation.
- Understanding the initial photoinitiation step is vital for precise modeling of plasmon-driven chemistry.
- Applications include converting carbon dioxide (CO2) into hydrocarbons.
Purpose of the Study:
- To identify the critical photoinitiation step in plasmonic photosynthesis.
- To elucidate the mechanism of light-driven chemical reactions on plasmonic nanoparticles.
Main Methods:
- Measurement of H/D and 12C/13C kinetic isotope effects (KIEs).
- Analysis of hydrocarbon production rates under varying isotopic conditions (H2O vs. D2O).
Main Results:
- A significant primary H/D kinetic isotope effect was observed, slowing hydrocarbon production by a factor of 5-8 when using D2O instead of H2O.
- This indicates that the scission of the O-H bond in water is a rate-limiting step.
Conclusions:
- The hole-driven scission of the O-H bond in water is identified as a critical, limiting step in plasmonic photosynthesis.
- This finding advances the mechanistic understanding of light-driven chemical reactions facilitated by plasmonic nanoparticles.
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