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1.
Environ Sci Technol ; 58(24): 10696-10705, 2024 Jun 18.
Artículo en Inglés | MEDLINE | ID: mdl-38845125

RESUMEN

Because ozone (O3) is a significant air pollutant, advanced O3 elimination technologies, particularly those under high-humidity conditions, have become an essential research focus. In this study, a nickel-iron layered double hydroxide (NiFe-LDH) was modified via intercalation with octanoate to develop an effective hydrophobic catalyst (NiFe-OAa-LDH) for O3 decomposition. The NiFe-OAa-LDH catalyst sustained its O3 decomposition rate of >98% for 48 h under conditions of 90% relative humidity, 840 L/(g·h) space velocity, and 100 ppm inlet O3 concentration. Moreover, it maintained a decomposition rate of 90% even when tested at a higher airflow rate of 2500 L/(g·h). Based on the changes induced by the Ni-OII to Ni-OIII bonds in NiFe-OAa-LDH during O3 treatment, catalytic O3 decomposition was proposed to occur in two stages. The first stage involved the reaction between the hydroxyl groups and O3, leading to the breakage of the O-H bonds, formation of NiOOH, and structural changes in the catalyst. This transformation resulted in the formation of abundant and stable hydrogen vacancies. According to density functional theory calculations, O3 can be effectively decomposed at the hydrogen vacancies with a low energy barrier during the second stage. This study provides new insights into O3 decomposition.


Asunto(s)
Hidróxidos , Ozono , Hidróxidos/química , Ozono/química , Níquel/química , Catálisis , Contaminantes Atmosféricos/química
2.
J Hazard Mater ; 465: 133429, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38232545

RESUMEN

TiO2/TiOF2 Z-scheme nanosheets have been successfully synthesized for photocatalytic antibacterial. The antibacterial efficiency of TiO2/TiOF2 against E. coli and S. aureus were 99.90 % and 81.89 % at low material concentration (110 µg/mL), respectively, which are higher than those of pure TiO2, TiOF2, and Degussa P25. In situ molecular spectroscopy results demonstrate that the microstructure of the synthesized material can be reconstructed and optimized to enhance the exposure of the active sites·H2O and O2 are effectively adsorbed on the catalyst surface and activated to form OH…Ti and O…Ti surface active species. Furthermore, the dense interface formed in TiO2/TiOF2 acts as an efficient transport path for photoexcited electrons from TiO2 to TiOF2, and thus accelerates the formation of reactive oxygen species. Finally, the mechanism of bacterial inactivation is systematically discussed considering the main active substances, cell morphological changes, and activity of antioxidant enzymes.


Asunto(s)
Escherichia coli , Staphylococcus aureus , Escherichia coli/efectos de la radiación , Titanio/química , Luz , Antibacterianos/química
3.
Environ Sci Technol ; 57(45): 17553-17565, 2023 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-37917662

RESUMEN

The hydrogenation of organic sulfur (CS2) present in industrial off-gases to produce sulfur-free hydrocarbons and H2S can be achieved by using noble-metal catalysts. However, there has been a lack of comprehensive investigation into the underlying reaction mechanisms associated with this process. In this study, we have conducted an in-depth examination of the activity and selectivity of Pt- and Pd-loaded alumina-based catalysts, revealing significant disparities between them. Notably, Pd/Al2O3 catalysts exhibit an enhanced performance at low temperatures. Furthermore, we have observed that CS2 displays a higher propensity for conversion to methane when employing Pt/Al2O3 catalysts, while Pd/Al2O3 catalysts demonstrate a greater tendency for coke deposition. By combining experimental observations with theoretical calculations, we revealed that the capability of H2 spillover along with the adsorption capacity of CS2, play pivotal roles in determining the observed differences. Moreover, the key intermediate species involved in the methanation and coke pathways were identified. The intermediate CH2S* is found to be crucial in the methanation pathway, while the intermediate CSH* is identified as significant in the coke pathway.


Asunto(s)
Coque , Adsorción , Óxido de Aluminio , Hidrogenación , Azufre
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