The Nature of Active Sites in Pt–ReOX/TiO2 Catalysts for Selective Hydrogenation of Carboxylic Acids to Alcohols
Full article
Общее |
Language:
Английский,
Genre:
Full article,
Status:
Published,
Source type:
Original
|
Journal |
Journal of Energy Chemistry
ISSN: 2095-4956
|
Output data |
Year: 2015,
Volume: 24,
Number: 5,
Pages: 646-654
Pages count
: 9
DOI:
10.1016/j.jechem.2015.09.003
|
Tags |
Hexanoic acid, Hexanol, Nanoparticles, Platinum, Rhenium, Selective hydrogenation |
Authors |
Suknev Alexey
1
,
Zaikovskii Vladimir
1,2
,
Kaichev Vasily
1,2
,
Paukshtis Eugenii
1,2
,
Sadovskaya Ekaterina
1,2
,
Balʹzhinimaev Bair
1
|
Affiliations |
1 |
Boreskov Institute of Catalysis SB RAS, Lavrentieva Ave., 5, 630090, Novosibirsk, Russia
|
2 |
Novosibirsk State University, Pirogova Str., 2, 630090, Novosibirsk, Russia
|
|
The highly dispersed Pt-ReOX (x 1) sites ca. 0.5 nm in size were formed via a successive and strong interaction of the
Re precursor with titania and then of the Pt complex with deposited low-valent rhenium oxide clusters. The size, charge and chemical composition were characterized by means of HRTEM/STEM with EDX mapping, XPS, and FTIRS. These sites with Re/Pt = 2 were shown to be highly active and selective in the hydrogenation of carboxylic acid to alcohol under very mild conditions (T = 130 °C, P = 50 bar). The reaction rate constant for the hydrogenation of hexanoic acid increased linearly with the Pt content. As for the homogeneous pincer-type Ru-organic complexes, the active Pt-ReO sites can dissociate heterolytically the molecular hydrogen with the formation of hydroxyl groups and Pt hydride for hydrogenation of the carboxylic group. Indeed, TOF of 20 h-1 and selectivity of 98%-99% are approaching the values typical of homogeneous catalysts. The first order kinetics described well the experimental data obtained in a wide range of reaction conditions. © 2015 Science Press and Dalian Institute of Chemical Physics.