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 oxi...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 ℃ 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.展开更多
基金Supported by the National Natural Science Foundation of China(No.20563003)the Inner Mongolia Education Depart-ment Fund(No.NJZY07013)
文摘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 ℃ 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.
