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The low temperature oxidation of propane using H2O2 and Fe/ZSM-5 catalysts; insights into the active site and enhancement of catalytic turnover frequencies

Peneau, Virginie, Armstrong, Robert, Shaw, Greg, Xu, Jun, Jenkins, Robert, Morgan, David John, Dimitratos, Nikolaos, Taylor, Stuart Hamilton, Zanthoff, Horst, Pietz, Stefan, Stochniol, Guido, He, Qian, Kiely, Christopher and Hutchings, Graham John 2017. The low temperature oxidation of propane using H2O2 and Fe/ZSM-5 catalysts; insights into the active site and enhancement of catalytic turnover frequencies. ChemCatChem 9 (4) , pp. 642-650. 10.1002/cctc.201601241

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Abstract

Fe- containing ZSM-5 catalysts are reported to be efficient catalysts for the partial oxidation of propane to oxygenated products at reaction temperatures as low as 50 oC in an aqueous phase reaction using the green oxidant H2O2. It was previously proposed that extra framework Fe species at the zeolite's exchange sites are responsible for activation of both the alkane and hydrogen peroxide. Through a systematic study of the influence of framework topology and exchange properties it is now shown that this high catalytic activity is specific to the MFI-type Brønsted acidic zeolite ZSM-5. Furthermore, through a simple aqueous acid washing treatment, leaching ca. 77 % of iron present within a Fe/ZSM-5 catalyst only caused the relative propane conversion to decrease by 17 %; implying that most of the initially loaded Fe does not actually contribute to the catalytic activity. This small change in conversion after 'excess' Fe removal, amounts to a three-fold increase in TOF (Fe) from 66 h-1to 232 h-1 compared with the parent Fe/ZSM-5 catalyst. By comparing these samples, it is shown by NH3-TPD, 27Al MAS NMR, XPS and TEM analysis, that surface iron oxide species are effectively spectators in the oxidation of propane with H2O2. This provides further insight as to the location and true nature of the catalytically active Fe species.

Item Type: Article
Date Type: Publication
Status: Published
Schools: Cardiff Catalysis Institute (CCI)
Chemistry
Subjects: Q Science > QD Chemistry
Uncontrolled Keywords: propane oxidation hydrogen peroxide ZSM-5
Publisher: Wiley
ISSN: 1867-3880
Funders: Evonik
Date of First Compliant Deposit: 9 January 2017
Date of Acceptance: 22 November 2016
Last Modified: 27 Jun 2019 10:23
URI: http://orca.cf.ac.uk/id/eprint/97284

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