我室周剑章副教授和吴德印教授在 J. Am. Chem. Soc. 上发表论文：Plasmonic Hot Electron-Mediated Hydrodehalogenation Kinetics on Nanostructured Ag Electrodes

文章链接：https://pubs.acs.org/doi/10.1021/jacs.0c07027

摘要：An attractive field of plasmon-mediated chemical reaction (PMCR) is developing rapidly, but there is still incomplete under-standing of how to control the kinetics of such a reaction related to hot carriers. Here, we chose 8-bromoadenine (8BrAd) as a probe molecule of hot electrons to investigate the influence of the electrode potential, laser wavelength and power on the PMCR kinetics on silver nanoparticle-modified silver electrodes (Ag NPs@Ag). Plasmonic hot electron-mediated cleavage of the C-Br bond in 8BrAd has been investigated by combining in situ electrochemical surface-enhanced Raman spectroscopy (EC-SERS) and density functional theory (DFT) calculations. The experimental and theoretical results reveal that the energy position of plasmon relaxation-generated hot electrons can be modulated conveniently by applied potentials and laser light. This allows proposal of a mechanism of modulating the matching energy of the hot electron of plasmon relaxation to pro-mote the efficiency of PMCR in electrochemical interfaces. Our work will be helpful to design surface plasmon resonance (SPR) photoelectrochemical reactions on metal electrode surfaces of nanostructures with higher efficiency.