Citral hydrogenation on high surface area mesoporous TiO2-SiO2 supported Pt nanocomposites: Effect of titanium loading and reduction temperature on the catalytic performances

被引:23
作者
Bidaoui, Mourad [1 ,2 ]
Especel, Catherine [1 ]
Bouchenafa-Saib, Naima [2 ]
Duprez, Daniel [1 ]
Mohammedi, Ourida [2 ]
Royer, Sebastien [1 ]
机构
[1] Univ Poitiers, CNRS UMR 7285, Inst Chim Milieux & Mat Poitiers IC2MP, F-86022 Poitiers, France
[2] LCPMM, Blida, Algeria
关键词
Titania; Silica; Platinum; Mesoporous materials; Citral hydrogenation; Nanocomposites; LIQUID-PHASE HYDROGENATION; BIMETALLIC RH-GE; SELECTIVE HYDROGENATION; MOLECULAR-SIEVES; ALPHA; BETA-UNSATURATED ALDEHYDES; CROTONALDEHYDE HYDROGENATION; SILICA; DEHYDROGENATION; CYCLOHEXANE; COPOLYMER;
D O I
10.1016/j.apcata.2012.07.023
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070305 [高分子化学与物理];
摘要
Platinum-based catalysts supported on TiO2-modified mesostructured silica were prepared using the direct co-condensation of silica and titania precursors to synthesize the mixed-oxide support. The physico-chemical properties of the Pt/xTi-SBA15 samples with various xTi contents (in mol%) were further evaluated using several techniques, including elemental analysis, X-ray diffraction, N-2-physisorption, H-2-chemisorption, transmission electronic microscopy and the probe reaction of cyclohexane dehydrogenation to evaluate the metal-support interaction (SMSI effect). All the Pt/xTi-SBA15 samples display high specific surface areas (650-820 m(2) g(-1)) and high mesopore volumes (0.44-0.68 cm(3) g(-1)), with the formation of TiO2 anatase nanoparticles since the low titanium content, i.e. 2 mol%. The hexagonal organized pore structure of SBA silica is also strongly altered by the titanium adding, but mixed oxides so obtained present very particular morphology with maintaining of high surface areas. The catalytic performances of the Pt/xTi-SBA15 catalysts were estimated for the citral hydrogenation performed at 70 degrees C under hydrogen pressure (7 MPa), and discussed in terms of activity and unsaturated alcohols (UA: nerol and geraniol) selectivity. A synergetic effect on the UA selectivity was obtained on the Pt/xTi-SBA15 catalysts, compared to both Pt/SBA15 and Pt/TiO2 P25 reference samples (reduction temperature = 300 degrees C), and was explained by the specific role of the reducible TiO2 species, which under the nano-anatase form generate a strong metal-support interaction (SMSI effect) with platinum after reduction at 300 degrees C. The formation of partially reduced support species was finally modulated by varying the reduction temperature of the catalysts. It is then possible to achieve high selectivity after reduction at 350 degrees C, while maintaining high conversions. (C) 2012 Elsevier B.V. All rights reserved.
引用
收藏
页码:14 / 25
页数:12
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