FTIR INVESTIGATION OF SURFACE INTERMEDIATES FORMED DURING THE AMMOXIDATION OF TOLUENE OVER VANADYL PYROPHOSPHATE

Citation
Y. Zhang et al., FTIR INVESTIGATION OF SURFACE INTERMEDIATES FORMED DURING THE AMMOXIDATION OF TOLUENE OVER VANADYL PYROPHOSPHATE, Journal of molecular catalysis. A, Chemical, 118(2), 1997, pp. 205-214
Citations number
33
Categorie Soggetti
Chemistry Physical
ISSN journal
13811169
Volume
118
Issue
2
Year of publication
1997
Pages
205 - 214
Database
ISI
SICI code
1381-1169(1997)118:2<205:FIOSIF>2.0.ZU;2-P
Abstract
The mechanism of formation of surface intermediates, appearing during the interaction of vanadyl pyrophosphate (VO)(2)P2O7 with feed compone nts of the toluene ammoxidation was studied by FTIR spectroscopy. The investigation of ammonia adsorption at elevated temperature showed pro tonated and coordinated ammonia as expected as well as the generation of amido species; all could be so called 'nitrogen insertion species' or a source of these at least. The interaction of toluene and possible reaction intermediates such as benzaldehyde and benzylamine with (VO) (2)P2O7 was studied. The investigations revealed that the ammoxidation of toluene probably proceeds via the formation of a benzaldehyde inte rmediate. Afterwards, benzylimine surface species were probably formed by a N-insertion, using NH4+ surface species followed by the formatio n of benzonitrile by subsequent oxidative dehydrogenation. However, no benzamide species were observed. The surface species generated upon a dsorption of benzaldehyde were similar to those formed from toluene, i ndicating the role of the former as intermediate in the nitrile format ion path. Otherwise, the adsorption of benzylamine in the presence of oxygen did not lead to the formation of benzonitrile. Therefore, an am moxidation mechanism of toluene via a benzaldehyde intermediate is pre ferred and reaction pathways via benzamide or benzylamine as intermedi ates seem to be improbable.