TY - JOUR
T1 - Deactivation Behavior of Supported Gold Palladium Nanoalloy Catalysts during the Selective Oxidation of Benzyl Alcohol in a Micropacked Bed Reactor
AU - Al-Rifai, Noor
AU - Miedziak, Peter J.
AU - Morad, Moataz
AU - Sankar, Meenakshisundaram
AU - Waldron, Conor
AU - Cattaneo, Stefano
AU - Cao, Enhong
AU - Pattisson, Samuel
AU - Morgan, David
AU - Bethell, Donald
AU - Hutchings, Graham J.
AU - Gavriilidis, Asterios
PY - 2017/11/15
Y1 - 2017/11/15
N2 - Highly active, supported Au-Pd catalysts have been tested for catalyzing benzyl alcohol oxidation in a silicon-glass micropacked bed reactor. The effects of Au-Pd composition and anion content during catalyst preparation on catalyst deactivation were studied, and a relationship between the deactivation rate and the amount of Cl- and Au used in the catalyst formulation was found. While Au AIDS in enhancing the selectivity to the desired product and the Cl- ions help the formation of uniform 1-2 nm nanoparticles, higher amounts of Au and Cl- become detrimental to the catalyst stability once a certain amount is exceeded. Loss of small (1-2 nm) metal nanoparticles was evident in all catalysts studied, accompanied by agglomeration and the formation of larger >10 nm particles. A secondary deactivation mechanism characterized by the formation of an amorphous surface film was observed via transmission electron microscopy in catalysts with high Cl- and Au and was associated with the detection of carbon species on the catalyst surface using Raman spectroscopy.
AB - Highly active, supported Au-Pd catalysts have been tested for catalyzing benzyl alcohol oxidation in a silicon-glass micropacked bed reactor. The effects of Au-Pd composition and anion content during catalyst preparation on catalyst deactivation were studied, and a relationship between the deactivation rate and the amount of Cl- and Au used in the catalyst formulation was found. While Au AIDS in enhancing the selectivity to the desired product and the Cl- ions help the formation of uniform 1-2 nm nanoparticles, higher amounts of Au and Cl- become detrimental to the catalyst stability once a certain amount is exceeded. Loss of small (1-2 nm) metal nanoparticles was evident in all catalysts studied, accompanied by agglomeration and the formation of larger >10 nm particles. A secondary deactivation mechanism characterized by the formation of an amorphous surface film was observed via transmission electron microscopy in catalysts with high Cl- and Au and was associated with the detection of carbon species on the catalyst surface using Raman spectroscopy.
U2 - 10.1021/acs.iecr.7b01159
DO - 10.1021/acs.iecr.7b01159
M3 - Article
AN - SCOPUS:85034250368
VL - 56
SP - 12984
EP - 12993
JO - Industrial and Engineering Chemistry Research
JF - Industrial and Engineering Chemistry Research
SN - 0888-5885
IS - 45
ER -