An Au/ceria(0.44%, mass fraction) catalyst containing gold ions was prepared by a modified deposition precipitation method, and the evolution of gold ions in the catalyst and its influence on the catalysis of CO oxidation were investigated. It was found that the as-prepared catalyst containing gold ions with high valence could fully oxidize CO at –10 °C initially but was deactivated gradually at low temperatures during the reaction with CO or treatment by unpurified air. The deactivation of the catalyst during CO oxidation or treatment of it by unpurified air was independent and progressive at low temperatures while the activity of the catalyst at relatively high temperatures was maintained well. During the reaction with CO or treatment by unpurified air, the XPS results indicate that gold species evolved from high valence to low valence and the diffuse reflectance UV-Vis spectra show that high valence gold was reduced to charged gold clusters, gold clusters grew to small gold crystals and small gold crystals grew to large gold particles. Accordingly, the high valence gold corresponded to the activity at low temperatures and the metallic gold was active and relatively stable at high temperatures. The turnover frequencies(TOF) of the catalysts treated by different methods at 273 K decreased with the evolution of gold species from high valence to low valence, no maximum of TOF was observed although gold particles in the catalyst attained to about 2―3 nm during the treatment. An Au/ceria catalyst with a gold load of 0.87% (mass fraction) maintained a good activity for CO oxidation within 18 h at room temperature. The catalysts were characterized via transmitted electronic microscopy(TEM), inductively coupled plasma optical emission spectrometry(ICP-OES), X-ray diffraction(XRD) and BET specific surface area and UV-Vis DRS as well.
Aqueous precipitation and deposition-precipitation method were used to prepare CeO2 supports and Au/CeO2 catalysts, respectively. The effect of preparation condition of support on the catalyst activity was investigated. The catalytic combustion of HCHO was considered as the probe reaction for comparing the catalyst activity. The BET, X-ray diffraction, X-ray photoelectron spectroscopy (XPS), and Temperature-programmed reduction (TPR) were carried out to analyze the influence factor on the catalysts activity. The results showed that the addition of dispersant and use of microwave in the support preparation procedure could be beneficial for enhancing the interaction of supports and gold species and thus improved the catalytic activity. The total conversion temperature for HCHO was 146 °C over AC400. With the modification during supports preparation process, the catalytic activity increased with total conversion temperature decreasing to 98 °C. The results of XPS indicated that Au0 and Au+1 species coexisted in these catalysts and the activity of catalyst correlated with Au+1/Au0 ratio. Temperature-programmed reduction results demonstrated that the reduction peak appeared between 100–170 °C with the inducing of gold. The dependence of activity on the reduction peak temperature implied that ionic gold was catalytic activity component for HCHO oxidation.
