Deactivation Behavior of Supported Gold Palladium Nanoalloy Catalysts during the Selective Oxidation of Benzyl Alcohol in a Micropacked Bed Reactor

Highly active, supported Au−Pd catalysts have been tested for catalyzing benzyl alcohol oxidation in a siliconglass 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.