期刊
CATALYSIS TODAY
卷 187, 期 1, 页码 122-128出版社
ELSEVIER
DOI: 10.1016/j.cattod.2011.10.037
关键词
Glycerol; Hydrogenolysis; Pretreatment; DRIFT-CO; Cu species
资金
- Spanish Ministry of Science and Innovation [ENE2009-12743-C04-01, BIOSOCAT, RYC-2010-06067]
- Autonomous Government of Madrid [S2009/ENE-1660]
- FSE funds
We have used Cu/gamma-Al2O3 catalysts submitted to different activation protocols (calcination, reduction in H-2/Ar, and reoxidation in N2O/N-2) in order to investigate the role of the different copper surface species and acid properties in glycerol hydrogenolysis to 1,2-propanediol (1,2-PDO) under mild reaction conditions (493 K, 2.4 MPa H-2). The activated catalysts have been characterized by temperature-programmed reduction (TPR), temperature-programmed desorption of NH3 (TPD-NH3), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and diffuse reflectance infrared Fourier transform spectroscopy of adsorbed CO (DRIFT-CO). The significant different catalytic performance obtained with the Cu/gamma-Al2O3 solids is not integrally related to their acid properties, surface Cu species also participate in the glycerol conversion. Partially reduced copper species (Cu+) promotes glycerol conversion rates. Activated catalysts follow the sequence: reoxidation > reduction > calcination, when glycerol conversion is compared. Moreover. Cu species are mostly responsible for the observed 1,2-PDO selectivity values. It is strongly dependent on the Cu-0/Cu+ atomic ratio and on the surface concentration of both Cu-0 and Cu+ species. Accordingly, 10CuAl-c-r catalyst showed the best behavior in glycerol hydrogenolysis to 1,2-PDO. (C) 2011 Elsevier B.V. All rights reserved.
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