Cardiff University | Prifysgol Caerdydd ORCA
Online Research @ Cardiff 
WelshClear Cookie - decide language by browser settings

Light alkane oxidation using catalysts prepared by chemical vapour impregnation: tuning alcohol selectivity through catalyst pre-treatment

Forde, Michael, Armstrong, Robert, McVicker, Rebecca, Wells, Peter P., Dimitratos, Nikolaos ORCID: https://orcid.org/0000-0002-6620-4335, He, Qian ORCID: https://orcid.org/0000-0003-4891-3581, Lu, Li, Jenkins, Robert Leyshon, Hammond, Ceri ORCID: https://orcid.org/0000-0002-9168-7674, Lopez-Sanchez, Jose Antonio, Kiely, Christopher ORCID: https://orcid.org/0000-0001-5412-0970 and Hutchings, Graham John ORCID: https://orcid.org/0000-0001-8885-1560 2014. Light alkane oxidation using catalysts prepared by chemical vapour impregnation: tuning alcohol selectivity through catalyst pre-treatment. Chemical Science 5 (9) , pp. 3603-3616. 10.1039/C4SC00545G

[thumbnail of Forde 2014.pdf]
Preview
PDF - Published Version
Available under License Creative Commons Attribution.

Download (901kB) | Preview

Abstract

Fe/ZSM-5(30) catalysts have been prepared by chemical vapour impregnation (CVI) using iron(III) acetylacetonate as the precursor. These materials have been used for the oxidation of methane and ethane using aqueous hydrogen peroxide as oxidant. Heating in air leads to materials that exhibit high catalytic activity and give formic and acetic acid with high selectivity from methane and ethane respectively. Heat treatment of the uncalcined materials under a reducing atmosphere results in partial reduction of iron from the FeIII to FeII oxidation state with the majority of the iron being present as isolated octahedral extra-framework species having oxygen neighbours and showing no evidence of a coordination shell containing Al or Fe, as evidenced from studies using X-ray absorption and UV-Vis spectroscopies. These hydrogen treated catalysts show the same catalytic activity as their analogues formed by heating in air, but in contrast exhibit higher alcohol selectivities for both methane and ethane conversion to oxygenates and are reusable. Our findings for both the oxidation of methane and ethane indicate that the selectivity to the oxidation products, i.e. acids or alcohols, can be controlled by tuning the active site structure and/or oxidation state of the Fe species in Fe/ZSM-5.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Publisher: Royal Society of Chemistry
ISSN: 2041-6520
Funders: EPSRC
Date of First Compliant Deposit: 30 March 2016
Last Modified: 11 Oct 2023 21:41
URI: https://orca.cardiff.ac.uk/id/eprint/65717

Citation Data

Cited 37 times in Scopus. View in Scopus. Powered By Scopus® Data

Actions (repository staff only)

Edit Item Edit Item

Downloads

Downloads per month over past year

View more statistics