Sulfur dioxide adsorption and photooxidation on isotopically-labeled titanium dioxide nanoparticle surfaces: roles of surface hydroxyl groups and adsorbed water in the formation and stability of adsorbed sulfite and sulfate
文献情報
Charith E. Nanayakkara
Transmission FTIR spectroscopy and X-ray photoelectron spectroscopy (XPS) are used to probe the details of sulfur dioxide adsorption and photooxidation on titanium dioxide nanoparticle surfaces. Adsorption sites, surface speciation and photooxidation chemistry have been determined from analysis of FTIR spectra in conjunction with isotope labeling experiments. These data show that surface hydroxyl groups are involved in the adsorption of sulfur dioxide, and in particularly, sulfur dioxide reacts with either one surface O–H group to yield adsorbed bisulfite or two surface O–H groups to yield adsorbed sulfite and water. Using 16O–H, 16O–D and 18O–H labeled surface O–H groups, additional insights into the adsorption mechanism as well as shifts in the vibrational modes of adsorbed sulfite have been determined. Upon irradiation, adsorbed sulfite/bisulfite converts to adsorbed sulfate. The relative stability of adsorbed sulfite to adsorbed sulfate on TiO2 nanoparticle surfaces was also examined in the presence of increasing relative humidity (RH). It is shown here that adsorbed water can more easily displace sulfite compared to sulfate by forming a stable sulfur dioxide water complex in the presence of adsorbed water. These differences in the RH-dependent stability of adsorbed species that form as a result of surface heterogeneous reactions on oxide particles surfaces has important implications in the heterogeneous chemistry of mineral dust aerosol in the atmosphere.
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掲載誌
Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.











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