摘要
铜基催化剂(Cu/Zn O/Al_2O_3)是甲醇合成反应中常用的工业催化剂,但目前对于该反应的活性位点及机理的争论还比较多[1]。使用结构明确均一的模型催化剂能够有效理解催化结构与性能之间的关系。目前有关铜基模型催化剂的研究,主要集中在Cu/Zn O二元组分,缺乏对Al_2O_3的深入认识。在此研究中,我们分别制备了Cu/Al_2O_3/Zn O(0001)-Zn、Al_2O_3/Zn O(0001)-Zn、Cu/Zn O(0001)-Zn三种模型催化剂,并对其氧化还原性能进行了XPS及LEIS的分析。结果显示,在实验条件下,Al_2O_3在Zn O(0001)-Zn的表面以层层生长的模式进行生长,Cu在Zn O(0001)-Zn的表面先以二维岛状的模式生长,再三维岛状生长。氧化还原的过程显示,相对于二元模型催化剂Cu/Zn O(0001)-Zn,一定量的Al_2O_3的加入能够有效延缓Cu2+的还原过程,稳定Cu+。
The Cu/Al_2O_3/ZnO(0001)-Zn ternary model catalysts were prepared and characterized,as well as the growth models of binary model catalysts:Al_2O_3/ZnO(0001)-Zn and Cu/Zn O(0001)-Zn.It was found that Al_2O_3 grew on the ZnO(0001)-Zn surface by a layer-by-layer model,while Cu formed two-dimensional islands only at low coverage and three dimensional clusters at high coverage.Comparing to the Cu/Zn O binary model catalyst,the addition of Al_2O_3 obviously slowed down the reduction of Cu/Al_2O_3/ZnO by H_2,which may help to stabilize the surface Cu+.
引文
[1]Kasatkin,I.;Kurr,P.;Kniep,B.;Trunschke,A.;Schl?gl,R.Angew.Chem.2007,119(38):7465.