Abstract
Different gold nanoparticle catalysts on titania, silica, and titanosilicate supports
are compared in the hydro-epoxidation of propene. All catalysts tested
were active in the propene epoxidation, with Au/TiO2 showing the highest
activity at low temperature, but also a high rate of deactivation. It is shown
that the deactivation of the catalysts is directly related to a side reaction of a
bidentate propoxy reaction intermediate. This species can react to produce
propene oxide, but as a side reaction it can also produce very strongly
adsorbed species, most likely carbonates, which cause a reversible deactivation.
There are no indications that the catalyst deactivation is caused by
changes in the size or the state of the gold nanoparticles. Catalysts containing
a lower amount of titania dispersed in or on a silica support are more stable, but require a higher reaction temperature for a similar activity. Ti-SBA-15 is
the most promising support material, but the gold deposition inside the
structure requires further optimization. A key factor, that needs to be solved
for all gold catalysts, is the efficiency in which hydrogen is used as a coreactant.
The currently obtained hydrogen efficiencies of up to 10% are
insufficient to run a process profitably.
Original language | Undefined/Unknown |
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Title of host publication | Mechanisms in homogeneous and heterogeneous epoxidation catalysis |
Editors | S. Ted Oyama |
Place of Publication | Amsterdam [etc.] |
Publisher | Elsevier |
Pages | 340-353 |
Number of pages | 501 |
ISBN (Print) | 978-0-444-53188-9 |
Publication status | Published - 2008 |