摘要
肉桂醛选择性加氢在香精香料、医药等制造过程中具有重要作用。在这部分工作中,我们制备了一系列Pt/TiO_2-SiO_2有序介孔催化剂,并且Pt/TiO_2-SiO_2-介孔混相催化剂在转化率近100%时,肉桂醇的选择性高达90.9%以上。我们探讨了催化剂表面缺陷和金属-载体间强相互作用在肉桂醛加氢中的影响,同时也揭示了催化剂表面Ti~(2+)对肉桂醛选择性加氢的促进作用。此外,肉桂醛分子在Pt/有序介孔TiO_2-SiO_2催化剂上的吸附方式,倾向于通过C=O立式吸附在富电子的Pt表面,促进C=O键加氢,提高了不饱和醇的选择性。
Selective hydrogenation of cinnamaldehyde(CAL) is crucial in the manufacture of parfumes,pharmaceuticals,etc~1.In this work,a series of Pt/TiO_2-SiO_2 ordered mesoporous catalysts were prepared and the Pt/TiO_2-SiO_2-mixed catalyst showed a high selectivity of 90.9% to COL at nearly complete conversion.Meanwhile,the influences of surface defects,SMSI~2 and the promoting role of Ti~(2+) in selective hydrogenation of CAL over the catalysts were discussed.In addition,the adsorption mode of CAL over the Pt/TiO_2-SiO_2 catalysts preferred to adsorb vertically through the terminal C=O groups anchored onto the electron-enriched Pt surface,thus promoted the hydrogenation of C=O bond,and enhanced the reaction rate and selectivity of COL.
引文
[1]Kahsar,K.R.;Schwartz,D.K.;Medlin,J.W.;J.Am.Chem.Soc.2014,136:520-526.
[2]Ohyama,J.;Yamamoto,A.;Teramura,K.;ACS Catal.2011,1:187-192.
[3]Wu,Q.F.;Zhang,C.;Zhang,B.;Zhao,F.Y.;J.Colloid Interface Sci.2016,463:75–82.
