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SELECTIVE PHENOL HYDROGENATION IN AQUEOUS PHASE ON PD-BASED CATALYSTS SUPPORTED ON HYBRID TiO2-CARBON MATERIALS

机译:在杂交TiO2-碳材料上负载的Pd基催化剂的水相中选择性酚氢化

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A reaction in where the interplay between support and metal active phase becomes determinant, is the catalytic hydrogenation of phenol to cyclohexanone. This ketone is of industrial interest for the production of caprolactam and adipic acid [1]. The phenol hydrogenation route is undertaken through either two-step or one-step processes. In the two-step procedure, phenol is first hydrogenated to cyclohexanol, which is in turn dehydrogenated to cyclohexanone. The one-step selective hydrogenation of phenol to cyclohexanone is advantageous from an efficiency standpoint [2], and the reaction can be conducted in gas or liquid phase. The gas-phase phenol hydrogenation is usually performed at high temperatures over supported Pd catalysts and different supports [3]. However, liquid-phase phenol hydrogenation can be of interest since the reaction can be performed at relatively low temperatures [4]. The attainment of high selectivity (>95%) at high phenol conversion (>80%) is a challenge [2] because cyclohexanone can be further hydrogenated to cyclohexanol under the reaction conditions [5]. From the different commercial catalytic support we thought that TiO2-carbon composites could be suitable supports of an active metal (Pd) to catalyze the hydrogenation of phenol to cyclohexanone [6]. Thus, a series of TiO2-carbon composites have been prepared in where the carbon was generated through different routes changing the polarity of the surface [7]. When Pd is supported on TiO2-carbon composites, it is possible to achieve close to 100% yield to cyclohexanone or to cyclohexanol depending on the surface properties of the support.
机译:在载体和金属活性相之间的相互作用变为决定因素的情况下,是苯酚至环己酮的催化氢化。这种酮是生产己内酰胺和己二酸的产业利益[1]。通过两步或一步方法进行酚氢化途径。在两步方法中,将苯酚首先氢化至环己醇,其反向脱氢至环己酮。苯酚对环己酮的一步选择性氢化是有利的,效率观点[2]是有利的,并且反应可在气体或液相中进行。气相酚氢化通常在负载的Pd催化剂上的高温下进行,并不同支持[3]。然而,液相酚氢化可以是有益的,因为反应可以在相对低的温度下进行[4]。在高酚转化率(> 80%)的高选择性(> 95%)的培养是一种挑战[2],因为环己酮可以在反应条件下进一步氢化至环己醇[5]。从不同的商业催化载体中,我们认为TiO2-碳复合材料可以是有效金属(Pd)的合适支撑,以催化苯酚的氢化至环己酮[6]。因此,已经制备了一系列TiO2-碳复合材料,其中通过不同的路线产生碳的碳改变表面的极性[7]。当Pd支撑在TiO 2 - 碳复合材料上时,可以根据载体的表面性质达到环己酮或环己醇的接近100%的产率。

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