Article ID | Journal | Published Year | Pages | File Type |
---|---|---|---|---|
61141 | Journal of Catalysis | 2013 | 17 Pages |
•Cu catalysts supported on am-, m-, and t-ZrO2 for selective ethanol conversion.•Cu/m-ZrO2 catalyst shows a high selectivity to ethyl acetate.•The high rate of ethyl acetate is defined by oxygen mobility from bulk ZrO2 to Cu.•A high rate for acetaldehyde formation is observed for Cu/t-ZrO2 catalyst.
The effect of amorphous (am-), monoclinic (m-), and tetragonal (t-) ZrO2 phase on the physicochemical and catalytic properties of supported Cu catalysts for ethanol conversion was studied. The electronic parameters of Cu/ZrO2 were determined by in situ XAS, and the surface properties of Cu/ZrO2 were defined by XPS and DRIFTS of CO-adsorbed. The results demonstrated that the kind of ZrO2 phase plays a key role in the determination of structure and catalytic properties of Cu/ZrO2 catalysts predetermined by the interface at Cu/ZrO2. The electron transfer between support and Cu surface, caused by the oxygen vacancies at m-ZrO2 and am-ZrO2, is responsible for the active sites for acetaldehyde and ethyl acetate formation. The highest selectivity to ethyl acetate for Cu/m-ZrO2 catalyst up to 513 K was caused by the optimal ratio of Cu0/Cu+ species and the high density of basic sites (O2−) associated with the oxygen mobility from the bulk m-ZrO2.
Graphical abstractEffect of ZrO2 phases on the formation of acetaldehyde and ethyl acetate from ethanol over Cu/ZrO2 catalysts.Figure optionsDownload full-size imageDownload high-quality image (98 K)Download as PowerPoint slide