Inhibiting effect of oxygenated model compounds on the HDS of dibenzothiophenes over CoMoP/Al2O3 catalyst
Inhibiting effect of oxygenated model compounds on the HDS of dibenzothiophenes over CoMoP/Al2O3 catalyst
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CoMoP/Al2O3 催化剂上含氧模型化合物对二苯并噻吩 HDS 的抑制作用
DOI：
10.1016/j.apcata.2010.04.055
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发表时间：
2010
影响因子：
5.5
通讯作者：
S. Brunet
中科院分区：
文献类型：
--
作者：
M. Philippe;F. Richard;D. Hudebine;S. Brunet
在硫化态CoMoP/Al_2O_3催化剂上，采用固定床微反装置（340 ℃，4.0MPa）研究了含氧化合物愈创木酚和苯酚对4，6-二甲基二苯并噻吩（46 DMDBT）和二苯并噻吩（DBT）加氢脱硫反应的影响。建立了在深度HDS操作条件下愈创木酚和苯酚（苯酚转化的主要中间体）转化的反应方案。苯酚的转化涉及两个主要途径：氢化途径（HYD），包括首先氢化芳环，然后C-O键断裂（导致形成苯）和直接脱氧（DDO）途径，仅涉及C-O键断裂（导致环己烷）。这两种方式是独立的，没有观察到苯转化为环己烷。这两种含氧化合物抑制硫化合物的加氢脱硫，由于氧气和含硫化合物之间的竞争吸附，愈创木酚的效果比苯酚的效果更强。对同一氧分子的46 DMDBT和DBT转化的抑制作用相似，表明参与HDS的两条主要途径（HYD和DDS）受到相同的影响。根据Langmuir-Hinshelwood模型，这对应于催化剂表面上所含的氧和硫化合物之间的竞争吸附。
The effect of oxygen compounds (guaiacol and phenol) on the hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene (46DMDBT) and dibenzothiophene (DBT) was studied on a sulfided CoMoP/Al2O3catalyst in a fixed bed microreactor (340°C, 4.0MPa). The reaction scheme of the transformation of guiaicol and of phenol (the main intermediate in the transformation of phenol) was established under deep HDS operating conditions. The transformation of phenol involved two main routes: a hydrogenation pathway (HYD) involving first the hydrogenation of the aromatic rings followed by C–O bond rupture (leading to the formation of benzene) and a direct deoxygenation (DDO) pathway involving only a C–O bond rupture (leading to cyclohexane). These two ways were independent, no transformation of benzene into cyclohexane was observed. Both oxygen compounds inhibited the hydrodesulfurization of sulfur compounds due to competitive adsorption between the oxygen and sulfur containing compounds, with the effect of guaiacol being stronger than the effect of phenol. The inhibition was similar in the transformation of 46DMDBT and DBT for the same oxygen molecule, showing that the two main routes (HYD and DDS) involved in the HDS were affected in the same way. This corresponds to a competitive adsorption between the oxygen and sulfur compounds containing on the catalyst surface according to a Langmuir–Hinshelwood model.