Controlled surface properties of Au/ZSM5 catalysts and their effects in the selective oxidation of ethanol

Abstract

The catalytic activity of gold supported on ZSM5 (Au/ZSM5) was investigated for the selective oxidation of ethanol in the presence of excess oxygen. Au/ZSM5 catalyst pretreated by nonthermal O2 plasma method showed the best oxidative activity compared to low-temperature calcination in air and high-temperature reduction in hydrogen atmosphere. Results from microscopy and X-ray diffraction characterizations proved that plasma pretreatment afforded a small Au particle size and a uniform dispersion of Au nanoparticles on ZSM5 surfaces. Characterization results further demonstrated that the residual ammonia adsorbed on ZSM5 surfaces during the precipitation can be oxidized to nitrate ions by nonthermal O2 plasma treatment, while it converted to NO+ by low-temperature oxygen calcination and was completely removed by high-temperature hydrogen reduction. Dissimilar surface/interface properties caused the tremendously different interaction between gold nanoparticles and zeolite support, and consequently the catalytic performances in ethanol oxidation. In particular, under the nonthermal O2 plasma pretreatment, the formed NO3− species lowered the acidity of ZSM5 surfaces as well as anchored the Au nanoparticles, resulting in nearly 100% selectivity toward selective oxidation instead of acid-catalyzed reactions even under high reaction temperature.