Monitoring Reaction Intermediates in Plasma-Driven SO2, NO, and NO2Remediation Chemistry Using in Situ SERS Spectroscopy

Shujin Li, Bofan Zhao, Alejo Aguirre, Yu Wang, Ruoxi Li, Sisi Yang, Indu Aravind, Zhi Cai, Ran Chen, Lasse Jensen, Stephen B. Cronin

Research output: Contribution to journalArticlepeer-review

Abstract

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. Density functional theory (DFT) calculations are used to confirm the experimental observations by calculating the vibrational modes of the surface-bound intermediate species. 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. 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. 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. 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.

Original languageEnglish (US)
Pages (from-to)6421-6427
Number of pages7
JournalAnalytical Chemistry
Volume93
Issue number16
DOIs
StatePublished - Apr 27 2021

All Science Journal Classification (ASJC) codes

  • Analytical Chemistry

Fingerprint

Dive into the research topics of 'Monitoring Reaction Intermediates in Plasma-Driven SO<sub>2</sub>, NO, and NO<sub>2</sub>Remediation Chemistry Using in Situ SERS Spectroscopy'. Together they form a unique fingerprint.

Cite this