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Enhancing Catalytic Activity and Selectivity by Plasmon-Induced Hot Carriers
Xiao-Qing Liu1, Fei-Fei Meng1, Xing Chen2
1MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, The Key Lab of Low-carbon Chem & Energy Conservation of Guangdong Province, School of Chemistry, Sun Yat-Sen University, Guangzhou 510275, China.
Iscience
|May 15, 2020
Summary
Localized surface plasmon resonance (LSPR) enhances solar energy conversion by boosting nitrobenzene (NB) conversion to phenylhydroxylamine (PHA). This study reveals the underlying hot carrier mechanisms for improved reactivity and selectivity.
Area of Science:
- Photocatalysis
- Plasmonics
- Solar Energy Conversion
Background:
- Plasmon-assisted chemical transformations offer promise for solar energy applications.
- Achieving simultaneous enhancement in reactivity and selectivity remains a significant challenge.
- The underlying mechanisms of plasmon-enhanced reactions are not fully understood.
Purpose of the Study:
- To elucidate the principles of localized surface plasmon resonance (LSPR)-induced enhancement in photoelectrocatalytic redox of nitrobenzene (NB).
- To investigate the role of hot carriers in controlling reaction activity and selectivity.
- To understand the contribution of hot electrons and holes to selective chemical transformations.
Main Methods:
- Utilized gold nanoparticles for photoelectrocatalytic redox reactions.
- Employed in situ surface-enhanced Raman spectroscopy (SERS) for reaction monitoring.
- Conducted density functional theory (DFT) simulations to support experimental findings.
Main Results:
- Achieved a significant enhancement in overall activity (∼70%) and selectivity for NB conversion.
- Demonstrated selective acceleration of NB to phenylhydroxylamine (PHA) conversion by hot carriers (∼14%).
- Showed suppression of PHA to nitrosobenzene (NSB) transformation (∼13%), further enhanced by electron acceptors (up to 43%).
Conclusions:
- LSPR-induced hot carriers selectively control the rates of intermediate and final product formation.
- The observed selectivity arises from the interplay of accelerated hot electron transfer and residual hot holes.
- This work provides insights into directing chemical synthesis using renewable solar energy under mild conditions.
