摘要：By using density functional theory (DFT) calculation and dispersion corrections of DFT-D method, the stacking effect of unsupported multilayer NiMoS nanocluster on hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene (4,6-DMDBT) via direct desulfurization (DDS) route is investigated. We establish multilayer NiMoS nanocluster by stacking the monolayer active phase according to former characterization. The results show that the activation energy of C-S bond cleavage on dilayer is about 60 kJ∙mol⁻¹ than that of monolayer in case I and near 160 kJ∙mol⁻¹ higher in case II, moreover, it is about 300 kJ∙mol⁻¹ higher on trilayer model. It seems DDS of 4,6-DMDBT could only occur at the corner sites of the top or bottom layer of regular multilayer NiMoS. Besides, the hydrogen transfer from the adjacent layer is also investigated in case IV and V of dilayer and trilayer, respectively. However, the activation energies of case IV and V are both over 400 kJ∙mol⁻¹, which makes the reactions unlikely to happen. Overall, the stacking effects of unsupported multilayer NiMoS cause severe steric hindrance in the process of C-S bond cleavage, hydrogen transfer and C[sbnd]H bond formation. Therefore, only the monolayer model is the most efficient surface in catalyzing DDS of 4,6-DMDBT and usage of active metals, the dilayer model is barely acceptable and the multilayer model (layer ≥ 3) is unnecessary.
© 2020 Elsevier Ltd

ISSN号：0016-2361

卷、期、页：v 280,

发表日期：2020-01-01

影响因子：5.578500

期刊分区（SCI为中科院分区）：二区

收录情况：SCIE（科学引文索引网络版）,EI（工程索引）

发表期刊名称：Fuel

通讯作者：刘晓东,黄文斌,张鹏飞,徐朱松

第一作者：魏强,周亚松

论文类型：期刊论文

论文概要：刘晓东,魏强,黄文斌,周亚松,张鹏飞,徐朱松，DFT insights into the stacking effects on HDS of 4,6-DMDBT on Ni-Mo-S corner sites，Fuel，2020，v 280,

论文题目：DFT insights into the stacking effects on HDS of 4,6-DMDBT on Ni-Mo-S corner sites