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Article Dans Une Revue Applied Catalysis B: Environmental Année : 2023

Unravelling the critical role of silanol in Pt/SiO2 for room temperature HCHO oxidation: An experimental and DFT study

Résumé

In the present work, Pt/SiO2 catalysts have been prepared by impregnating as-prepared Pt NPs NPs onto commercial SiO2 of tailored silanol density (2.3, 3.1 and 4.5 OH nm-2) produced through hexamethyldisilazane passivation. The resulting Pt/SiO2 catalysts were then tested for formaldehyde (HCHO) total oxidation. The catalytic tests showed that high surface silanol density led to lower apparent activation energy (from 40.7 kJ⸱mol-1 at 2.3 OH nm-2 to 21.9 kJ⸱mol-1 at 4.5 OH nm-2)), allowing formaldehyde total oxidation in dry and wet conditions (100% conversion into CO2 over Pt/SiO2 (4.5 OH nm-2) at room temperature in dry condition, among the best catalytic performances reported). DFT calculations described the different interaction behaviours of HCHO, H2O, CO and CO2 on pure SiO2 and Pt/SiO2 (1.1-7.2 OH nm-2) surface, showing the critical role of silanols in the total oxidation of formaldehyde over Pt/SiO2 in different humid conditions.

Domaines

Catalyse
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Dates et versions

hal-04249843 , version 1 (19-10-2023)

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Shuo Chen, Saber Gueddida, Michael Badawi, Sébastien Lebègue, Jean-Marc Giraudon, et al.. Unravelling the critical role of silanol in Pt/SiO2 for room temperature HCHO oxidation: An experimental and DFT study. Applied Catalysis B: Environmental, 2023, Applied Catalysis B: Environmental, 331, pp.122672. ⟨10.1016/j.apcatb.2023.122672⟩. ⟨hal-04249843⟩
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