Highly Efficient and Robust Au/MgCuCr2O4 Catalyst for Gas-Phase Oxidation of Ethanol to Acetaldehyde
Highly Efficient and Robust Au/MgCuCr2O4 Catalyst for Gas-Phase Oxidation of Ethanol to Acetaldehyde
复制标题
DOI：
10.1021/ja406820f
复制
发表时间：
2013-09-25
影响因子：
15
通讯作者：
Hensen, Emiel J. M.
中科院分区：
文献类型：
--
作者：
Liu, Peng;Hensen, Emiel J. M.
负载在 MgCuCr2O4-尖晶石上的金纳米颗粒 (AuNP) 对于乙醇有氧氧化为乙醛具有高活性和选择性（转化率 100%；产率接近 95%）。催化剂稳定至少500小时。前所未有的催化性能归因于金属 AuNP 和表面 Cu+ 物质之间的强大协同作用。 X 射线光电子能谱表明，Cu+ 在催化剂制备过程中已经形成，并且在乙醇氧化过程中在表面变得更加占主导地位。这些 Cu+ 物质稳定在三元 MgCuCr2O4-尖晶石载体的表面。进一步的动力学测量表明 Cu+ 物质充当 O-2 活化位点。
Gold nanoparticles (AuNPs) supported on MgCuCr2O4-spinel are highly active and selective for the aerobic oxidation of ethanol to acetaldehyde (conversion 100%; yield similar to 95%). The catalyst is stable for at least 500 h. The unprecedented catalytic performance is due to strong synergy between metallic AuNPs and surface Cu+ species. X-ray photoelectron spectroscopy shows that Cu+ is already formed during catalyst preparation and becomes more dominant at the surface during ethanol oxidation. These Cu+ species are stabilized at the surface of the ternary MgCuCr2O4-spinel support. Further kinetic measurements indicate that the Cu+ species act as sites for O-2 activation.