1/8/2024 0 Comments Yu wang![]() ![]() ![]() View details for Web of Science ID 000645428400017 By closing the loop between the experimental and DFT-calculated spectra, we identified not only the adsorbed species associated with each peak in the SERS spectra but also their orientation and adsorption site, providing a detailed atomistic picture of the chemical reaction pathway and surface interaction chemistry. During the removal of NO in the dry and wet plasma, both NO2 and NO3 species were observed on the Ag surface however, the concentration of NO3 species was enhanced under wet-plasma conditions. We observed the formation of SO3 and SO4 species in the SO2 wet-plasma-driven remediation, while in the dry plasma, we only identified SO3 adsorbed on the Ag surface. Here, we provide spectroscopic evidence that the wet plasma increases the SO2 and the NOx removal through the formation of highly reactive OH radicals, driving the reactions to H2SO4 and HNO3, respectively. Density functional theory (DFT) calculations are used to confirm the experimental observations by calculating the vibrational modes of the surface-bound intermediate species. In situ surface-enhanced Raman scattering (SERS) spectroscopy is used to identify the key reaction intermediates during the plasma-based removal of NO and SO2 under dry and wet conditions on Ag nanoparticles. A., Wang, Y., Zhang, B., Weng, S., Cai, Z., Li, R., Baygi, A., Smith, A., Gundersen, M. CO2 Reduction to Higher Hydrocarbons by Plasma Discharge in Carbonated Water ACS ENERGY LETTERS Yang, S., Zhao, B., Aravind, I.View details for Web of Science ID 000773646200023 To our knowledge, this is the first work in which LSPR-induced hot electron-driven photochemistry and in situ photoexcited carrier dynamics are studied on the same plasmon resonance structure with and without adsorbates. Finite-difference time domain (FDTD) simulations show two resonant modes for both grating structures, corresponding to dipolar LSPR modes at the metal/fused silica and metal/water interfaces. The enhancement factor (i.e., reaction rate) is 15.6× between p-polarized and s-polarized light for the 300 nm linewidth grating and 4.4× for the 266 nm linewidth grating. Double peaks in the photocurrent measurement are observed when irradiating a 300 nm linewidth grating. Plateau-like photocurrent peaks appear when exciting a 266 nm linewidth grating with p-polarized (on resonance) light, accompanied by a similar profile in the measured absorptance. The LSPR TA signal is redshifted with delay time because of charge transfer and subsequent change in the dielectric constant of nearby solution. When the sample is immersed in solution under -1 V applied potential, the extracted electron-phonon interaction time decreases from 0.94 to 0.67 ps because of additional energy dissipation channels. In situ ultrafast transient absorption (TA) measurements show a depletion peak resulting from hot electrons. Here, we report a hot electron-driven hydrogen evolution reaction (HER) by exciting the localized surface plasmon resonance (LSPR) in Au grating photoelectrodes. While most studies have focused on hot carrier dynamics at metal/semiconductor interfaces, we study the in situ dynamics of direct hot electron injection from metal to adsorbates. Understanding the relaxation and injection dynamics of hot electrons is crucial to utilizing them in photocatalytic applications. Vice Provost for Undergraduate Education.Office of Vice President for Business Affairs and Chief Financial Officer.Office of VP for University Human Resources.Stanford Woods Institute for the Environment.Stanford Institute for Economic Policy Research (SIEPR).Institute for Stem Cell Biology and Regenerative Medicine.Institute for Human-Centered Artificial Intelligence (HAI). ![]() Institute for Computational and Mathematical Engineering (ICME).Freeman Spogli Institute for International Studies.Stanford Doerr School of Sustainability. ![]()
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