Department of Chemical and Biological Engineering, Tufts University, 4 Colby Street, Medford, MA 02155, USA.
Phys Chem Chem Phys. 2011 Feb 21;13(7):2517-27. doi: 10.1039/c0cp02009e. Epub 2011 Jan 17.
We report the activity of shape-controlled metal oxide (CeO(2), ZnO and Fe(3)O(4)) supported gold catalysts for the steam reforming of methanol (SRM) and the water gas shift (WGS) reactions. Metal oxide nanoshapes, prepared by controlled hydrolysis and thermolysis methods, expose different crystal surfaces, and consequently disperse and stabilize gold differently. We observe that similar to gold supported on CeO(2) shapes exposing the {110} and {111} surfaces, gold supported on the oxygen-rich ZnO {0001} and Fe(3)O(4) {111} surfaces shows higher activity for the SRM and WGS reactions. While the reaction rates vary among the Au-CeO(2), Au-ZnO and Au-Fe(3)O(4) shapes, the apparent activation energies are similar, indicating a common active site. TPR data further indicate that the reaction lightoff coincides with the activation of Au-O-M species on the surface of all three oxide supports evaluated here. Different shapes contain a different number of binding sites for the gold, imparting different overall activity.
我们报告了形状控制的金属氧化物(CeO(2)、ZnO 和 Fe(3)O(4))负载金催化剂在甲醇蒸汽重整(SRM)和水汽变换(WGS)反应中的活性。通过控制水解和热解方法制备的金属氧化物纳米形状暴露了不同的晶体表面,因此金的分散和稳定方式也不同。我们观察到,与负载在暴露{110}和{111}表面的 CeO(2)形状上的金相似,负载在富氧 ZnO {0001}和 Fe(3)O(4) {111}表面上的金在 SRM 和 WGS 反应中表现出更高的活性。虽然 Au-CeO(2)、Au-ZnO 和 Au-Fe(3)O(4)形状之间的反应速率不同,但表观活化能相似,表明存在共同的活性位。TPR 数据进一步表明,反应的起始与三种氧化物载体上 Au-O-M 物种的活化同时发生。不同的形状包含不同数量的金结合位点,赋予了不同的整体活性。