Carley, Albert Frederick, Davies, Philip Rosser  ORCID: https://orcid.org/0000-0003-4394-766X, Roberts, Meirion Wyn and Thomas, Kevin K.
2010.
Transient Oxygen States in Catalysis: Ammonia Oxidation at Ag(111).
Langmuir
26
(21)
, pp. 16221-16225.
10.1021/la100953m
|
Abstract
Although the reactive sticking probability of oxygen at Ag(111) is of the order of 10-6 at 295 K, ammonia oxidation is a facile process at low temperatures. A combination of quantitative analysis of photoelectron spectra together with high resolution electron energy loss spectroscopy provides kinetic and spectroscopic evidence for an ammonia-dioxygen complex, stable at 100 K, as the key intermediate. The reactive oxygen O2(s) is a transient dioxygen precursor of the unreactive peroxo state O2-(a). It is present as a complex when ammonia and dioxygen are coadsorbed at low temperature (100 K) with evidence from both O(1s) and energy loss spectra. Hydroxyl and amide/imide species are formed, followed by dehydroxylation and oxide formation at 260 K. This is a further example (zinc was the first) of how an sp-metal, where dioxygen bond cleavage is slow, provides an alternative pathway via a transient dioxygen state to catalytic oxidation through precursor assisted dioxygen bond cleavage. Whether it is a general characteristic of sp-metals remains to be established. Comparisons are made with the homogeneously catalyzed Gif reaction, the selective oxidation of hydrocarbons by dioxygen.
| Item Type: | Article |
|---|---|
| Date Type: | Publication |
| Status: | Published |
| Schools: | Schools > Chemistry Research Institutes & Centres > Cardiff Catalysis Institute (CCI) Research Institutes & Centres > Neuroscience and Mental Health Research Institute (NMHII) |
| Subjects: | Q Science > QD Chemistry |
| Publisher: | American Chemical Society |
| ISSN: | 0743-7463 |
| Last Modified: | 18 Oct 2022 12:34 |
| URI: | https://orca.cardiff.ac.uk/id/eprint/10328 |
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