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Al₂O₃在促进CuZnAl催化剂中的作用的新见解:一项模型研究。 (注:原文中Al O表述有误,推测为Al₂O₃)

New Insights into the Role of Al O in the Promotion of CuZnAl Catalysts: A Model Study.

作者信息

Hu Jun, Song Yanying, Huang Junjie, Li Yangyang, Chen Mingshu, Wan Huilin

机构信息

State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, Fujian, P. R. China.

出版信息

Chemistry. 2017 Aug 4;23(44):10632-10637. doi: 10.1002/chem.201701697. Epub 2017 Jul 11.

Abstract

The Cu/Al O /ZnO(0001)-Zn ternary model catalysts and their binary analogues were prepared and characterized. It was found that Al O grew on the ZnO(0001)-Zn surface by a layer-by-layer model, whereas Cu grew on the ZnO(0001)-Zn surface as two-dimensional clusters up to 0.2 monolayers (ML), and thereafter formed three-dimensional clusters. Because of the layer-by-layer growth of Al O on the ZnO(0001)-Zn, Cu/Al O can be considered without the effect of ZnO. Ternary model catalyst Cu/Al O /ZnO(0001)-Zn, which has all three parts on the surface, was prepared by deposition of Cu on the surface of Al O /ZnO(0001)-Zn. Low-energy ion scattering spectra showed that Cu preferred to locate at the Al O /ZnO interfaces. Compared with Cu/ZnO, the addition of Al O obviously suppressed the reduction of copper oxides and led to a higher concentration of Cu . The Cu clusters were found to be covered by thin ZnO overlayers after reduction of Cu/Al O /ZnO(0001)-Zn by using H . Therefore, the high activity of industrial Cu/ZnO/Al O catalysts may origin from Cu -rich clusters at the Al O /ZnO interface that are covered by thin ZnO overlayers.

摘要

制备并表征了Cu/Al₂O₃/ZnO(0001)-Zn三元模型催化剂及其二元类似物。发现Al₂O₃通过逐层模型生长在ZnO(0001)-Zn表面,而Cu在ZnO(0001)-Zn表面生长为二维簇,直至0.2单层(ML),此后形成三维簇。由于Al₂O₃在ZnO(0001)-Zn上的逐层生长,Cu/Al₂O₃可以在不考虑ZnO影响的情况下进行研究。通过在Al₂O₃/ZnO(0001)-Zn表面沉积Cu制备了表面具有所有三个部分的三元模型催化剂Cu/Al₂O₃/ZnO(0001)-Zn。低能离子散射光谱表明,Cu优先位于Al₂O₃/ZnO界面处。与Cu/ZnO相比,Al₂O₃的加入明显抑制了氧化铜的还原,并导致更高浓度的Cu⁺。通过用H₂还原Cu/Al₂O₃/ZnO(0001)-Zn后发现,Cu簇被薄的ZnO覆盖层覆盖。因此,工业Cu/ZnO/Al₂O₃催化剂的高活性可能源于Al₂O₃/ZnO界面处富Cu簇被薄的ZnO覆盖层覆盖。

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