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Plasmon-driven chemical transformation of a secondary amide probed by surface enhanced Raman scattering

Chemistry

Plasmon-driven chemical transformation of a secondary amide probed by surface enhanced Raman scattering

A. Dutta, M. Ončák, et al.

This cutting-edge study explores the fascinating reactivity of N-methyl-4-sulfanylbenzamide (NMSB) at gold and silver nanoparticle aggregates under plasmonic excitation. By employing surface-enhanced Raman scattering (SERS), the authors reveal a hot electron-mediated transformation of NMSB into p-mercaptobenzamide and p-mercaptobenzonitrile, showcasing an unexpected non-thermal reaction pathway. Discover the exciting findings from this collaborative research by Anushree Dutta, Milan Ončák, Farhad Izadi, Eugene Arthur-Baidoo, João Ameixa, Stephan Denifl, and Ilko Bald.

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Abstract
Plasmon-driven chemical conversion is gaining burgeoning interest in the field of heterogeneous catalysis. Herein, we study the reactivity of N-methyl-4-sulfanylbenzamide (NMSB) at nanocavities of gold and silver nanoparticle aggregates under plasmonic excitation to gain understanding of the respective reaction mechanism. NMSB is a secondary amide, which is a frequent binding motive found in peptides and a common coupling product of organic molecules and biomolecules. Surface-enhanced Raman scattering (SERS) is used as a two-in-one in-situ spectroscopic tool to initiate the molecular transformation process and simultaneously monitor and analyze the reaction products. Supported by dissociative electron attachment (DEA) studies with the gas phase molecule, a hot electron-mediated conversion of NMSB to p-mercaptobenzamide and p-mercaptobenzonitrile is proposed at the plasmonic nanocavities. The reaction rate showed negligible dependence on the external temperature, ruling out the dominant role of heat in the chemical transformation at the plasmonic interface. This is reflected in the absence of a superlinear relationship between the reaction rate constant and the laser power density, and DEA and SERS studies indicate a hot-electron mediated pathway. We conclude that the overall reaction rate is limited by the availability of energetic hot electrons to the NMSB molecule.
Publisher
Communications Chemistry
Published On
Aug 27, 2024
Authors
Anushree Dutta, Milan Ončák, Farhad Izadi, Eugene Arthur-Baidoo, João Ameixa, Stephan Denifl, Ilko Bald
Tags
N-methyl-4-sulfanylbenzamide
gold nanoparticles
silver nanoparticles
surface-enhanced Raman scattering
molecular transformation
hot electron-mediated reaction
non-thermal pathway
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