Hydrogen Peroxide to Propylene Oxide (HPPO) reaction is an attractive process exploiting Titanium Silicalite-1 (TS-1) as catalyst in combination with aqueous hydrogen peroxide as oxidizing agent. Beyond the industrial interest, TS-1 represents one of the most widely characterized catalyst due to its unique properties. However, a unified description on the speciation of the different Ti species and their correlation to catalytic performances is missing in the literature. This work aims to exploit spectroscopic techniques (namely Diffuse Reflectance UV-VIS, Raman, FT-IR and Ti K-edge XANES) in a qualitative and quantitative way to thoroughly characterize Ti sites in a selected set of industrially relevant TS-1 samples, each one owning a peculiar Ti speciation. The outcomes of this study have been then related to the activity of each catalyst in HPPO reaction, showing its linear correlation with the content of perfect Ti sites (i.e. isomorphously substituting Si in the zeolitic framework). Other Ti species, such as amorphous TiOx and bulk titania, are instead not involved in the peroxide conversion (neither in a detrimental way).

Effect of Ti Speciation on Catalytic Performance of TS-1 in the Hydrogen Peroxide to Propylene Oxide Reaction

Signorile, Matteo;Crocellà, Valentina;Damin, Alessandro;Lamberti, Carlo;Bonino, Francesca;Bordiga, Silvia
2018-01-01

Abstract

Hydrogen Peroxide to Propylene Oxide (HPPO) reaction is an attractive process exploiting Titanium Silicalite-1 (TS-1) as catalyst in combination with aqueous hydrogen peroxide as oxidizing agent. Beyond the industrial interest, TS-1 represents one of the most widely characterized catalyst due to its unique properties. However, a unified description on the speciation of the different Ti species and their correlation to catalytic performances is missing in the literature. This work aims to exploit spectroscopic techniques (namely Diffuse Reflectance UV-VIS, Raman, FT-IR and Ti K-edge XANES) in a qualitative and quantitative way to thoroughly characterize Ti sites in a selected set of industrially relevant TS-1 samples, each one owning a peculiar Ti speciation. The outcomes of this study have been then related to the activity of each catalyst in HPPO reaction, showing its linear correlation with the content of perfect Ti sites (i.e. isomorphously substituting Si in the zeolitic framework). Other Ti species, such as amorphous TiOx and bulk titania, are instead not involved in the peroxide conversion (neither in a detrimental way).
2018
122
16
9021
9034
https://pubs.acs.org/doi/abs/10.1021/acs.jpcc.8b01401
Electronic, Optical and Magnetic Materials; Energy (all); Physical and Theoretical Chemistry; Surfaces, Coatings and Films
Signorile, Matteo; Crocellà, Valentina; Damin, Alessandro; Rossi, Barbara; Lamberti, Carlo; Bonino, Francesca*; Bordiga, Silvia
File in questo prodotto:
File Dimensione Formato  
signorile_jpcc_postprint.pdf

Open Access dal 12/04/2019

Descrizione: Articolo principale
Tipo di file: POSTPRINT (VERSIONE FINALE DELL’AUTORE)
Dimensione 11.83 MB
Formato Adobe PDF
11.83 MB Adobe PDF Visualizza/Apri
signorile_jpcc_SI.pdf

Open Access dal 12/04/2019

Descrizione: Supporting Information
Tipo di file: POSTPRINT (VERSIONE FINALE DELL’AUTORE)
Dimensione 6.05 MB
Formato Adobe PDF
6.05 MB Adobe PDF Visualizza/Apri
acs.jpcc.8b01401.pdf

Accesso riservato

Descrizione: PDF editoriale articolo principale
Tipo di file: PDF EDITORIALE
Dimensione 2.47 MB
Formato Adobe PDF
2.47 MB Adobe PDF   Visualizza/Apri   Richiedi una copia

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2318/1668934
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 73
  • ???jsp.display-item.citation.isi??? 70
social impact