文献类型：期刊文献

中文题名：苯在Ru-Zn/ZrO_2表面部分加氢反应的理论和实验研究

英文题名：Theoretical and Experimental Study on the Partial Hydrogenation of Benzene over Ru-Zn/ZrO_2 Catalyst

作者：何惠民[1];袁佩青[1];马悦铭[1];程振民[1];袁渭康[1]

机构：[1]华东理工大学化学工程国家重点实验室,上海200237

年份：2009

卷号：30

期号：4

起止页码：312

中文期刊名：催化学报

收录：CSTPCD;;Scopus;北大核心:【北大核心2008】；CSCD:【CSCD2011_2012】；

语种：中文

中文关键词：钌锌合金;氧化锆;密度泛函;苯;部分加氢;环己烯

外文关键词：Ru-Zn alloy;zirconia;density functional theory;benzene;partial hydrogenation;cyclohexene

摘要：采用理论计算和实验方法研究了Ru-Zn/ZrO2催化剂上苯的部分加氢反应.在还原阶段于水相中引入Zn2+可使部分Zn以原子态进入Ru基催化剂.理论计算表明,Zn原子在Ru基催化剂中的存在同时抑制了苯和环己烯在催化剂表面的化学吸附,尤其是环己烯在整个催化剂表面的吸附处于一定钝化状态,这是环己烯选择性提高的重要原因.实验结果表明,Zn原子在催化剂中浓度的增加使得催化剂的加氢活性单调下降,而环己烯选择性则单调上升.实验和理论计算都证实了Ru基催化剂中最佳Zn含量的存在.
Partial hydrogenation of benzene over Ru-Zn/ZrO2 was investigated with the theoretical and experimental approaches.Atomic state of Zn was introduced into the Ru-based catalyst by loading ZnSO4 into the water phase during the reduction of the precursor.The DFT calculation showed that the presence of Zn atoms on the Ru-based catalyst has an unfavorable effect on the chemisorption of benzene and cyclohexene.Furthermore,the whole Zn atoms-modified catalyst surface is partly passivated for the chemisorption of cyclohexene,which is considered essential to the improvement of the cyclohexene yield on the Ru-Zn/ZrO2 catalyst.The experimental results showed that an increase in the Zn content in the Ru-based catalyst results in a monotonically decreased hydrogenation activity and an improved selectivity for cyclohexene.Both the theoretical and experimental investigation confirm the optimal Zn content in the Ru-based catalyst.