Plasmon-Mediated Photoelectrochemical Hot-Hole Oxidation Coupling Reactions of Adenine on Nanostructured Silver Electrodes

Su, Yaqiong; Liu, Jia; Huang, Rao; Yang, Hongtao; Li, Mingxue; Pang, Ran; Zhang, Meng; Yang, Ming; Su, Hai‐Feng; Devasenathipathy, Rajkumar; Wu, Yuan‐Fei; Zhou, Jian-Zhang; Wu, De‐Yin; Xie, Su‐Yuan; Mao, Bing‐Wei; Zhang, Tian

doi:10.1021/acs.jpclett.3c00619

Cited by 10 publications

(4 citation statements)

References 72 publications

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“…Many kinds of chemical reactions caused by hot-electron transfer have been reported, following pioneering studies, including azo-bond formation, , epoxidation, and H 2 dissociation . In recent years, the generation and utilization of hot holes for chemical reactions have also attracted increasing attention. − Recent studies have revealed that hot holes can enhance or induce various chemical reactions such as the oxidative dissolution of Au nanorods, azo coupling reaction of adenine, and oxidative scission of the CC bond, and so on.…”

Section: Diverse Excitation Sourcesmentioning

confidence: 99%

Key Factors for Controlling Plasmon-Induced Chemical Reactions on Metal Surfaces

Kazuma

2023

J. Phys. Chem. Lett.

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including the dielectric function, electronic states, and surface properties. Further investigations of plasmonic metal catalysts, both macroscopically and microscopically, provide more detailed fundamental knowledge on controlling plasmoninduced chemical reactions. In addition, the development of a theory to handle the entangled key factors, as well as a precise and large amount of experimental data for various materials and reactions, is required to establish a strategy for designing and customizing plasmonic metal catalysts.

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Section: Diverse Excitation Sourcesmentioning

confidence: 99%

Key Factors for Controlling Plasmon-Induced Chemical Reactions on Metal Surfaces

Kazuma

2023

J. Phys. Chem. Lett.

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“…The energy of harmonic oscillations was calculated for each final geometry [127][128][129], together with the respective theoretical IR intensities and Raman activities. The obtained vibrational energies were not scaled, although in general, it can improve the agreement between calculated and experimental bands [130]. The transformation from Raman activities to excitation-dependent Raman intensities was conducted according to the method described in our earlier studies [131,132].…”

Section: Dft Calculationsmentioning

confidence: 99%

The Structural Characterisation and DFT-Aided Interpretation of Vibrational Spectra for Cyclo(l-Cys-d-Cys) Cyclic Dipeptide in a Solid State

Witkowski,

Trzybiński,

Pawlędzio

et al. 2023

Molecules

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Cyclic dipeptides with two intramolecular peptide bonds forming a six-membered 2,5-diketopiperazine ring are gaining significant attention due to their biological and chemical properties. Small changes in the local geometry of such molecules (from cis to trans) can lead to significant structural differences. This work presents the results of a study of cyclo(l-Cys-d-Cys), a dipeptide comprising two cysteine molecules in opposite chiral configurations, with the functional groups situated at both sides of the diketopiperazine ring. X-ray diffraction (XRD) experiment revealed that the molecule crystallises in the P-1 space group, which includes the centre of inversion. The IR and Raman vibrational spectra of the molecule were acquired and interpreted in terms of the potential energy distribution (PED) according to the results of density functional theory (DFT) calculations. The DFT-assisted analysis of energy frameworks for the hydrogen bond network within molecular crystals was performed to support the interpretation of X-ray structural data. The optimisation of the computational model based on three-molecule geometry sections from the crystallographic structure, selected to appropriately reflect the intermolecular interactions responsible for the formation of 1D molecular tapes in cyclo(l-Cys-d-Cys) crystal, allowed for better correspondence between theoretical and experimental vibrational spectra. This work can be considered the first complete structural characterisation of cyclo(l-Cys-d-Cys), complemented via vibrational spectroscopy results with full band assignment aided with the use of the DFT method.

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“…have been well-proven in several studies. [5][6][7][8][9][10][11][12][13] This has been extended further to study the reactivity of a range of biomolecules like peptides in a plasmonic hot spot by tipenhanced Raman scattering (TERS). 14 A common explanation of plasmon-induced processes is based on the well-developed models for reactions induced by electronic transitions namely desorption induced by electronic transition (DIET), and desorption induced by multiple electronic transitions (DIMET).…”

Section: Introductionmentioning

confidence: 99%

Plasmon-Driven Chemical Transformation of a Secondary Amide Probed by Surface Enhanced Raman Scattering

Bald,

Dutta,

Ončák

et al. 2024

Preprint

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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 the nanocavities of gold and silver nanoparticle aggregates under plasmonic excitation to gain an understanding of the reaction mechanism. NMSB is a secondary amide, which is a frequent binding motive found in peptides and common coupling products of organic 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 analyse 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. Importantly, the reaction rate showed negligible dependence on the external temperature excluding the dominant role of heat in the chemical transformation at the plasmonic interface. This is also reflected by the lack of superlinear dependence of the reaction rate constant on the laser power density. Although DEA studies and the nature of power dependence on the reaction rate reflect the hot-electron mediated pathway, the overall reaction rate is limited by the electron transfer probability to the NMSB molecule generating the reaction products.

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Plasmon-Mediated Photoelectrochemical Hot-Hole Oxidation Coupling Reactions of Adenine on Nanostructured Silver Electrodes

Cited by 10 publications

References 72 publications

Key Factors for Controlling Plasmon-Induced Chemical Reactions on Metal Surfaces

Key Factors for Controlling Plasmon-Induced Chemical Reactions on Metal Surfaces

The Structural Characterisation and DFT-Aided Interpretation of Vibrational Spectra for Cyclo(l-Cys-d-Cys) Cyclic Dipeptide in a Solid State

Plasmon-Driven Chemical Transformation of a Secondary Amide Probed by Surface Enhanced Raman Scattering

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