TY - JOUR
T1 - Enhancement of biphenyl hydrogenation over gold catalysts supported on Fe-, Ce- and Ti-modified mesoporous silica (HMS)
AU - Castaño, Pedro
AU - Zepeda, T. A.
AU - Pawelec, B.
AU - Makkee, Michiel
AU - Fierro, J. L.G.
N1 - Generated from Scopus record by KAUST IRTS on 2019-08-08
PY - 2009/10/1
Y1 - 2009/10/1
N2 - Mesoporous metallosilicates (HMS-M; M = Ce, Fe, Ti) were used as supports for the preparation of Au catalysts, and were tested in the liquid-phase hydrogenation of biphenyl at 5 MPa and 488 K. Irrespective of the support, uniformly dispersed Au nanoparticles in range 3.2-6.5 nm were obtained. The highest turn over frequency (TOF), expressed per surface Au atom, was achieved on the Au/HMS-Fe, furthermore this catalyst gave the highest selectivity to the most saturated compound (bicyclohexyl with the highest cetane number) by means of enhancing the second aromatic-ring hydrogenation. From the catalyst activity-structure correlation, the highest activity of the Au/HMS-Fe catalyst is linked with: (i) the higher ratio of positively charged metallic gold Auδ+/Si (XPS), and (ii) the higher stability of Au nanoparticles (HRTEM). A linear correlation between the activity (per gram of metal) of the catalysts and their ratio Auδ+/Si is observed; however, Au/HMS-Ce catalyst displays a different behaviour in terms of activity per gram of metal exposed caused by the fact that ceria is not incorporated in the framework. © 2009 Elsevier Inc. All rights reserved.
AB - Mesoporous metallosilicates (HMS-M; M = Ce, Fe, Ti) were used as supports for the preparation of Au catalysts, and were tested in the liquid-phase hydrogenation of biphenyl at 5 MPa and 488 K. Irrespective of the support, uniformly dispersed Au nanoparticles in range 3.2-6.5 nm were obtained. The highest turn over frequency (TOF), expressed per surface Au atom, was achieved on the Au/HMS-Fe, furthermore this catalyst gave the highest selectivity to the most saturated compound (bicyclohexyl with the highest cetane number) by means of enhancing the second aromatic-ring hydrogenation. From the catalyst activity-structure correlation, the highest activity of the Au/HMS-Fe catalyst is linked with: (i) the higher ratio of positively charged metallic gold Auδ+/Si (XPS), and (ii) the higher stability of Au nanoparticles (HRTEM). A linear correlation between the activity (per gram of metal) of the catalysts and their ratio Auδ+/Si is observed; however, Au/HMS-Ce catalyst displays a different behaviour in terms of activity per gram of metal exposed caused by the fact that ceria is not incorporated in the framework. © 2009 Elsevier Inc. All rights reserved.
UR - https://linkinghub.elsevier.com/retrieve/pii/S0021951709002449
U2 - 10.1016/j.jcat.2009.07.011
DO - 10.1016/j.jcat.2009.07.011
M3 - Article
SN - 0021-9517
VL - 267
JO - Journal of Catalysis
JF - Journal of Catalysis
IS - 1
ER -