Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2022-07-28 , DOI: 10.1016/j.apcatb.2022.121801 Shuisen He, Tingting Huang, Yu Fan
Novel alumina-supported Ni-Mo hydrodesulfurization (HDS) catalysts were prepared via assembly of Mo and Al precursors induced by tetradecylamine (TDA). Compared with conventional impregnation, this assembly method improves Mo dispersion, weakens metal-support interactions, enhances Ni modification at MoS2 edge sites, and produces more NiMoS phases on Al2O3. The optimal NiMoS microstructure was obtained by modulating the TDA/Mo ratio in the assembly. A microstructure-activity correlation indicated that the S vacancies at the NiMoS corner sites favored σ-adsorption and direct desulfurization of 4,6-dimethylbenzothiophene (4,6-DMDBT), and those at the NiMoS edge sites promoted C-S breaking in hydrogenated derivatives of 4,6-DMDBT. Among these catalysts, NiTMo-2.0/Al2O3, which had the most corner and edge S vacancies, exhibited the highest reaction rate constant of 5.89 × 10−7 mol·g−1·s−1 and the highest desulfurization ratio of 99.5% in HDS of 4,6-DMDBT.
中文翻译:
十四烷胺诱导Mo和Al前驱体组装制备高效NiMoS/Al2O3超深加氢脱硫催化剂
新型氧化铝负载的 Ni-Mo 加氢脱硫 (HDS) 催化剂是通过由十四胺 (TDA) 诱导的 Mo 和 Al 前驱体的组装制备的。与常规浸渍相比,这种组装方法改善了 Mo 的分散,减弱了金属-载体的相互作用,增强了 MoS 2边缘位点的 Ni 改性,并在 Al 2 O 3上产生了更多的 NiMoS 相. 通过调节组件中的 TDA/Mo 比获得最佳的 NiMoS 微观结构。微观结构-活性相关性表明,NiMoS 角位的 S 空位有利于 4,6-二甲基苯并噻吩 (4,6-DMDBT) 的 σ 吸附和直接脱硫,而 NiMoS 边缘位的 S 空位促进 CS 的氢化衍生物的断裂。 4,6-DMDBT。在这些催化剂中,角和边缘S空位最多的NiTMo-2.0/Al 2 O 3的反应速率常数最高,为5.89×10 -7 mol·g -1 ·s -1,脱硫率最高99.5% 在 4,6-DMDBT 的 HDS 中。