TY - JOUR
T1 - Structure and composition of Au-Cu and Pd-Cu bimetallic catalysts affecting acetylene reactivity
AU - Murugadoss, Arumugam
AU - Sorek, Elishama
AU - Asscher, Micha
PY - 2014/6
Y1 - 2014/6
N2 - Au-Cu and Pd-Cu bimetallic model catalysts were prepared on native SiO 2/Si(100) substrate under ultra high vacuum (UHV) by employing buffer layer assisted growth procedure with amorphous solid water as the buffer material. The effect of the bimetallic nanoclusters (NCs) surface composition and morphology on their chemical reactivity has been studied with acetylene decomposition and conversion to ethylene and benzene as the chemical probe. It was found that among the Au-Cu NCs compositions, Au0.5Cu3 NCs revealed outstanding catalytic selectivity towards ethylene formation. These NCs were further characterized by employing TEM, XPS and HAADF-STEM coupled EDX analysis. With CO molecule as a probe, CO temperature programmed desorption has been used to investigate the distribution of gold on the top-most surface of the supported clusters. Surface segregation at high relative elemental fraction of gold leads to a decreased activity of the Au-Cu NCs towards ethylene formation. In contrast to the Au-Cu NCs, the Pd-Cu bimetallic system reveals reduced sensitivity to the relative elemental composition with respect to selectivity of the acetylene transformation toward ethylene formation. On the other hand, remarkable activity towards benzene formation has been observed at elemental composition of Cu3Pd, at comparable rates to those for ethylene formation on clean Pd NCs.
AB - Au-Cu and Pd-Cu bimetallic model catalysts were prepared on native SiO 2/Si(100) substrate under ultra high vacuum (UHV) by employing buffer layer assisted growth procedure with amorphous solid water as the buffer material. The effect of the bimetallic nanoclusters (NCs) surface composition and morphology on their chemical reactivity has been studied with acetylene decomposition and conversion to ethylene and benzene as the chemical probe. It was found that among the Au-Cu NCs compositions, Au0.5Cu3 NCs revealed outstanding catalytic selectivity towards ethylene formation. These NCs were further characterized by employing TEM, XPS and HAADF-STEM coupled EDX analysis. With CO molecule as a probe, CO temperature programmed desorption has been used to investigate the distribution of gold on the top-most surface of the supported clusters. Surface segregation at high relative elemental fraction of gold leads to a decreased activity of the Au-Cu NCs towards ethylene formation. In contrast to the Au-Cu NCs, the Pd-Cu bimetallic system reveals reduced sensitivity to the relative elemental composition with respect to selectivity of the acetylene transformation toward ethylene formation. On the other hand, remarkable activity towards benzene formation has been observed at elemental composition of Cu3Pd, at comparable rates to those for ethylene formation on clean Pd NCs.
KW - Acetylene
KW - Amorphous solid water
KW - Bimetallic nano-clusters
KW - Catalysis
KW - Hydrogenation
UR - http://www.scopus.com/inward/record.url?scp=84902665866&partnerID=8YFLogxK
U2 - 10.1007/s11244-014-0264-x
DO - 10.1007/s11244-014-0264-x
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AN - SCOPUS:84902665866
SN - 1022-5528
VL - 57
SP - 1007
EP - 1014
JO - Topics in Catalysis
JF - Topics in Catalysis
IS - 10-13
ER -