Laboratoire de Réactivité de Surface, CNRS and UPMC Université Paris 06, UMR CNRS 7197, Paris, France.
Phys Chem Chem Phys. 2013 Mar 14;15(10):3473-9. doi: 10.1039/c2cp44157h. Epub 2013 Jan 29.
Gold catalysts supported on titania (Au-TiO(2)) and alumina (Au-Al(2)O(3)) were prepared by deposition-precipitation with urea and then activated before characterisation and reaction in CO oxidation, either by calcination in air at 500 °C or reduction under H(2) at 300 °C. Gold nanoparticles with average size in the range 2-4 nm were obtained, with calcination leading to larger gold nanoparticles than reduction. For Au-TiO(2), high activity was observed in CO oxidation at room temperature, independent of the activation treatment. This high activity could not be correlated to the presence of sub-nanometer gold clusters as reported in the literature, since they could not be detected by atomic-resolution high-angle annular dark-field scanning-transmission electron microscopy (HAADF-STEM). In the case of Au-Al(2)O(3), the performance in CO oxidation was found to strongly depend on the water content in the reaction gas feed and on the activation conditions, with calcination resulting in a poorly active catalyst whereas reduction gave activity of the same order as Au-TiO(2). A comparative study of Au-TiO(2) and Au-Al(2)O(3) by electron microscopy did not reveal distinct differences in the shapes of the Au nanoparticles, which are mostly flattened through interaction with the substrate in both samples, with side profile shapes varying from rounded hemispherical to well faceted truncated cubo-octahedra. More faceting is found for the samples calcined at 500 °C than reduced at 300 °C. Various possible parameters affecting the catalytic properties of gold in CO oxidation are discussed in the context of the relevant literature.
金催化剂负载在二氧化钛(Au-TiO(2))和氧化铝(Au-Al(2)O(3))上,通过尿素沉淀法制备,然后在 CO 氧化反应中进行特征化和反应之前进行活化,活化方法是在空气中 500°C 煅烧或在 300°C 下氢气还原。得到了平均粒径在 2-4nm 范围内的金纳米粒子,煅烧导致金纳米粒子比还原得到的更大。对于 Au-TiO(2),在室温下的 CO 氧化中表现出高活性,与活化处理无关。这种高活性不能与文献中报道的亚纳米金簇的存在相关联,因为它们不能通过原子分辨率高角度环形暗场扫描透射电子显微镜(HAADF-STEM)检测到。对于 Au-Al(2)O(3),发现 CO 氧化的性能强烈依赖于反应气体进料中的含水量和活化条件,煅烧导致催化剂活性差,而还原得到的活性与 Au-TiO(2)相当。通过电子显微镜对 Au-TiO(2)和 Au-Al(2)O(3)进行的比较研究没有显示出金纳米粒子形状的明显差异,在这两种样品中,金纳米粒子主要通过与基底相互作用而被扁平化,侧轮廓形状从圆形半球形到具有良好面的截角八面体变化。在 500°C 煅烧的样品中发现更多的面,而在 300°C 还原的样品中则较少。在相关文献的背景下,讨论了影响 CO 氧化中金催化性能的各种可能参数。