A comparative study on the selective hydrogenation of α,β unsaturated aldehyde and ketone to unsaturated alcohols on Au supported catalysts
A comparative study on the selective hydrogenation of α,β unsaturated aldehyde and ketone to unsaturated alcohols on Au supported catalysts
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DOI：
10.1016/j.cattod.2007.01.011
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发表时间：
2007-04
期刊：
影响因子：
5.3
通讯作者：
C. Milone;C. Crisafulli;R. Ingoglia;L. Schipilliti;S. Galvagno
中科院分区：
文献类型：
--
作者：
C. Milone;C. Crisafulli;R. Ingoglia;L. Schipilliti;S. Galvagno
以铁氧化物为载体的Au为催化剂，对反式，4-苯基，3-丁烯，2-酮（苄叉丙酮）和反式，3-苯基，丙烯醛（肉桂醛）进行了加氢反应。以商品针铁矿（FeOOH）、磁赤铁矿（γ Fe 2 O3）和赤铁矿（α Fe 2 O3）为载体，研究了它们对催化剂性能的影响。考察了世界黄金理事会提供的Au/Fe 2 O 3参比催化剂的催化活性。采用BET、XRD、TPR、NH3-TPD和高分辨透射电镜（HRTEM）等手段对金催化剂和载体进行了表征。在所研究的催化剂中，以FeOOH为载体的Au对不饱和羰基化合物的加氢反应具有最高的活性和选择性，而以α-Fe 2 O3为载体的Au的活性和选择性较差。在苯甲醛丙酮和肉桂醛的加氢反应中，金粒子的形貌对催化剂的活性和不饱和醇（UA）的选择性影响较小，而主要受载体性质的影响。发现催化剂还原度与UA的活性和选择性有一定的相关性，催化剂还原度越大，UA的活性和选择性越高。这些结果让我们认为，活性和选择性的网站是由负的金粒子通过电子从还原载体转移到金属形成的。
The hydrogenation of trans,4-phenyl,3-buten,2-one (benzalacetone) and trans,3-phenyl, propenal (cinnamaldehyde) was carried out on Au supported on iron oxides catalysts. Commercial goethite (FeOOH), maghemite (γFe2O3) and hematite (αFe2O3) were used as supports. The catalytic activity of Au/Fe2O3reference catalyst, supplied by the World Gold Council, was also investigated. Gold catalysts and the parent supports were characterized by BET, X-ray diffraction (XRD), temperature programmed reduction (TPR), temperature programmed desorption of ammonia (NH3-TPD) and high resolution transmission electron microscopy (HRTEM). Among the catalysts investigated Au supported on FeOOH shows the highest activity and selectivity to UA in the hydrogenation of unsaturated carbonyl compounds whereas Au supported on αFe2O3are the less active and selective catalysts. The catalytic activity and selectivity to unsaturated alcohols (UA) in the hydrogenation of benzalacetone and cinnamaldehyde are less influenced by the morphology of gold particles and are mainly influenced by the nature of the support. A correlation between the reducibility of the catalysts and the activity and selectivity to UA has been found. Increasing the reducibility of the catalysts both the activity and selectivity to UA increase. These results let us to argue that active and selective sites are formed by negative gold particles formed through the electron transfer from the reduced support to the metal.