TY - JOUR
T1 - Volcano-curves for dehydrogenation of 2-propanol and hydrogenation of nitrobenzene by SiO 2-supported metal nanoparticles catalysts as described in terms of a d-band model
AU - Tamura, Masazumi
AU - Kon, Kenichi
AU - Satsuma, Atsushi
AU - Shimizu, Ken Ichi
PY - 2012/9/7
Y1 - 2012/9/7
N2 - To confirm whether the activity trends in multistep organic reactions can be understood in terms of the Hammer-Nørskov d-band model in combination with the linear energy relations, we studied correlations between the reaction rates for dehydrogenation and hydrogenation reactions and the position of the d-band center (ε d) relative to the Fermi energy (E F), the ε d - E F value, of various metal catalysts. SiO 2-supported metal (M = Ag, Cu, Pt, Ir, Pd, Rh, Ru, Ni, and Co) catalysts with the same metal loading (5 wt %) and similar metal particle size (8.9-11.7 nm) were prepared. The dehydrogenation of adsorbed 2-propanol in a flow of He and the hydrogenation of adsorbed nitrobenzene in a flow of H 2 were tested as model reactions of organic reactions on the metal surface. As a test reaction of H 2 dissociation on the surface, SiOH/SiOD exchange on the M/SiO 2 catalysts in a flow of D 2 is carried out. The liquid phase hydrogenation of nitrobenzene under 3.0 MPa of H 2 is adopted as an organic reaction under realistic conditions. Generally, the activities show volcano-type dependences on the ε d - E F value, indicating that the ε d - E F value is useful as a qualitative activity descriptor in heterogeneous catalysis of metal nanoparticles for multistep organic reactions.
AB - To confirm whether the activity trends in multistep organic reactions can be understood in terms of the Hammer-Nørskov d-band model in combination with the linear energy relations, we studied correlations between the reaction rates for dehydrogenation and hydrogenation reactions and the position of the d-band center (ε d) relative to the Fermi energy (E F), the ε d - E F value, of various metal catalysts. SiO 2-supported metal (M = Ag, Cu, Pt, Ir, Pd, Rh, Ru, Ni, and Co) catalysts with the same metal loading (5 wt %) and similar metal particle size (8.9-11.7 nm) were prepared. The dehydrogenation of adsorbed 2-propanol in a flow of He and the hydrogenation of adsorbed nitrobenzene in a flow of H 2 were tested as model reactions of organic reactions on the metal surface. As a test reaction of H 2 dissociation on the surface, SiOH/SiOD exchange on the M/SiO 2 catalysts in a flow of D 2 is carried out. The liquid phase hydrogenation of nitrobenzene under 3.0 MPa of H 2 is adopted as an organic reaction under realistic conditions. Generally, the activities show volcano-type dependences on the ε d - E F value, indicating that the ε d - E F value is useful as a qualitative activity descriptor in heterogeneous catalysis of metal nanoparticles for multistep organic reactions.
KW - d-band center
KW - transition metals
KW - trend in catalytic activity
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U2 - 10.1021/cs300376u
DO - 10.1021/cs300376u
M3 - Article
AN - SCOPUS:84866071649
VL - 2
SP - 1904
EP - 1909
JO - ACS Catalysis
JF - ACS Catalysis
SN - 2155-5435
IS - 9
ER -