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The critical roles of hydrophobicity, surface Ru 0 and active O 2 - /O 2 2- sites on toluene combustion on Ru/ZSM-5 with varied Si/Al ratios.

Authors :
Liu J
Zeng L
Xu X
Xu J
Fang X
Bian Y
Wang X
Source :
Physical chemistry chemical physics : PCCP [Phys Chem Chem Phys] 2022 Jun 15; Vol. 24 (23), pp. 14209-14218. Date of Electronic Publication: 2022 Jun 15.
Publication Year :
2022

Abstract

By targeting more feasible catalysts for VOC combustion, 2%Ru/ZSM-5 catalysts were fabricated by supporting RuO <subscript>2</subscript> , a relatively cheaper noble metal, onto HZSM-5 supports with varied Si/Al ratios for toluene combustion. The valence state distribution of Ru and the Ru/RuO <subscript>2</subscript> -support interaction have been explored and elucidated. It has been revealed that the catalytic activity increases with the increase of the Si/Al ratio in the order 2%Ru/ZSM-5-18 < 2%Ru/ZSM-5-40 < 2%Ru/ZSM-5-72 < 2%Ru/ZSM-5-110 < 2%Ru/ZSM-5-255 < 2%Ru/SiO <subscript>2</subscript> -MFI. Interestingly, the hydrophobicity of the samples improves also with the increase in the Si/Al ratio, which impedes H <subscript>2</subscript> O adsorption effectively and its competition for the surface-active sites with the reactants. Both RuO <subscript>2</subscript> and Ru <superscript>0</superscript> are detected on all the catalysts, and the Ru <superscript>0</superscript> amount/ratio increases significantly with increasing the Si/Al ratio, which promotes the adsorption/activation of both toluene and O <subscript>2</subscript> molecules. Furthermore, the amount of surface-active O <subscript>2</subscript> <superscript>-</superscript> and O <subscript>2</subscript> <superscript>2-</superscript> is evidently improved. Therefore, the mixed interaction of higher hydrophobicity, more surface Ru <superscript>0</superscript> and active oxygen sites is the major reason for the enhancement in the activity of a Ru/ZSM-5 having a higher Si/Al ratio. It is concluded that the optimal catalyst can be designed by loading Ru/RuO <subscript>2</subscript> onto an MFI framework structure support with the highest Si content.

Details

Language :
English
ISSN :
1463-9084
Volume :
24
Issue :
23
Database :
MEDLINE
Journal :
Physical chemistry chemical physics : PCCP
Publication Type :
Academic Journal
Accession number :
35647687
Full Text :
https://doi.org/10.1039/d2cp01476a