The Importance of Catalytic Effects in Hot-Electron-Driven Chemical Reactions
Journal
ACS Nano
Journal Volume
18
Journal Issue
50
Start Page
34332
End Page
34340
ISSN
1936-0851
1936-086X
Date Issued
2024-12-04
Author(s)
Farheen Khurshid
Jeyavelan Muthu
Yen-Yu Wang
Yao-Wei Wang
Mu-Chen Shih
Ding-Rui Chen
Yu-Jung Lu
Drake Austin
Nicholas Glavin
Jan Plšek
Martin Kalbáč
Ya-Ping Hsieh
Abstract
Hot electrons (HEs) represent out-of-equilibrium carriers that are capable of facilitating reactions which are inaccessible under conventional conditions. Despite the similarity of the HE process to catalysis, optimization strategies such as orbital alignment and adsorption kinetics have not received significant attention in enhancing the HE-driven reaction yield. Here, we investigate catalytic effects in HE-driven reactions using a compositional catalyst modification (CCM) approach. Through a top-down alloying process and systematic characterization, using electrochemical, photodegradation, and ultrafast spectroscopy, we are able to disentangle chemical effects from competing electronic phenomena. Correlation between reactant energetics and the HE reaction yield demonstrates the crucial role of orbital alignment in HE catalytic efficiency. Optimization of this parameter was found to enhance HE reaction efficiency 5-fold, paving the way for tailored design of HE-based catalysts for sustainable chemistry applications. Finally, our study unveils an emergent ordering effect in photocatalytic HE processes that imparts the catalyst with an unexpected polarization dependence.
Subjects
Bimetallic Alloy
Compositional Catalyst Modification
Gradient
Hot-Electron
Photocatalysis
SDGs
Publisher
American Chemical Society (ACS)
Type
journal article