Ru, Os and Ru-Os supported on mesoporous silica doped with zirconium as mild thio-tolerant catalysts in the hydrogenation and hydrogenolysis/hydrocracking of tetralin
Ru, Os and Ru-Os supported on mesoporous silica doped with zirconium as mild thio-tolerant catalysts in the hydrogenation and hydrogenolysis/hydrocracking of tetralin
复制标题
锆掺杂介孔二氧化硅负载的 Ru、Os 和 Ru-Os 作为温和耐硫催化剂用于四氢化萘的加氢和氢解/加氢裂化
DOI：
10.1016/j.apcata.2004.10.031
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发表时间：
2005
影响因子：
5.5
通讯作者：
A. Jiménez
中科院分区：
文献类型：
--
作者：
D. Eliche;J. Mérida;E. Rodriguez;A. Jiménez
将摩尔比为8：1、4：1和1：1的MonoRu和Os催化剂和MonoRu-Os催化剂负载在掺杂有锆（摩尔比Si/Zr=5）的介孔二氧化硅上，总金属负载量为5 wt.%通过湿初始浸渍法制备，然后在120°C下干燥，最后在400°C下用氢气还原。通过XRD、XPS、N2吸附-脱附容量法、H2-TPR和NH3-TPD等手段对催化剂进行了表征，并在高氢压下进行了四氢萘加氢开环反应。具有高Ru含量的催化剂即使在低反应温度（200-295°C）下也显示出优异的氢化性能。然而，具有高Os含量的催化剂显示出弱的加氢活性，但具有非常好的氢解/加氢裂化活性（裂化化合物的30-40%）。这种高水平的活性是由酸中心的强度解释的。具有高Ru含量的催化剂在320°C下在进料中存在600 ppm二苯并噻吩的情况下保持其催化性能，但所有其它催化剂部分或完全失活。所有催化剂都被含有1000 ppm二苯并噻吩的进料不可逆地毒化。
Monometallic Ru and Os catalysts and bimetallic Ru–Os catalysts with molar ratios (8:1, 4:1 and 1:1) supported on a mesoporous silica doped with zirconium (molar ratio Si/Zr=5) with a total metal loading of 5wt.% were prepared by the wet incipient impregnation method, then dried at 120°C and finally reduced with hydrogen at 400°C. After a complete characterisation with XRD, XPS, N2adsorption–desorption volumetry, H2-TPR and NH3-TPD, the catalysts were tested in the hydrogenation and ring opening of tetralin at high hydrogen pressure. Catalysts with a high Ru content display excellent hydrogenation properties even at low reaction temperatures (200–295°C). However, catalysts with a high Os content display weak hydrogenation activity but a very good hydrogenolysis/hydrocracking activity (30–40% of cracking compounds). This high level of activity is explained by the strength of the acid centres. Catalysts with a high Ru content maintain their catalytic performance in the presence of 600ppm of dibenzopthiophene in the feed at 320°C, but all other catalysts are partially or totally deactivated. All catalysts are irreversibly poisoned with a feed containing 1000ppm of dibenzothiophene.