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A study on the role of Ni atoms in the HDN activity of NiMoS2/Al2O3 catalyst
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2020-02-07 , DOI: 10.1016/j.apcata.2020.117458
Wei Han , Hong Nie , Xiangyun Long , Dadong Li

A monometallic catalyst MoS2/Al2O3 and a Ni-promoting catalyst NiMoS2/Al2O3 were prepared through using nano-sized MoS3 particles as the precursor. XPS analysis combined with a DBT probe test indicate that, compared with the conventional catalyst Ref-MoS2/Al2O3 derived from nano-sized MoO3 particles, the MoS3-derived catalyst MoS2/Al2O3 not only contains nearly fully-sulfided Mo species, but also holds much more coordination unsaturated sites (CUS) on its MoS2 nanoslabs, thus resulting in the successful preparation of a bimetallic catalyst NiMoS2/Al2O3 with much weaker Mo-Al2O3 interaction and higher decoration degree of Ni atoms onto MoS2 nanoslabs as compared with the conventional counterpart. These significant structural advantages of the bimetallic catalysts not only avoid the strong interference of γ-Al2O3 to the active phase, but also bring potential excellent Ni-promoting effects on the catalytic activity. Then, using quinolone (Q) as the reactant, the Ni-promoting effect on the hydrodenitrogenation (HDN) activity was discussed. It was found when MoS2 nanoslabs were decorated by Ni atoms, the HDN activity attains an essential improvement. Moreover, this Ni-promoting effect is much more beneficial to the Path II (Q→14THQ/58THQ→DHQ→PCHA→PCHE + PCH) than Path I (Q→14THQ→OPA→PB). The origin of Ni-promoting effects on HDN activity was finally suggested: Ni atoms one hand activate H2 to produce activated hydrogen which afterwards react with Mo-S2- species to form Mo-SH species, and on the other hand increase the basicity of the neighboring Mo-S2-, which together promote the cracking of C-N bonds and thereby remarkably enhance the HDN activity.



中文翻译:

Ni原子在NiMoS 2 / Al 2 O 3催化剂的HDN活性中的作用研究

以纳米级的MoS 3颗粒为前驱体,制备了单金属催化剂MoS 2 / Al 2 O 3和助镍催化剂NiMoS 2 / Al 2 O 3。XPS分析结合DBT探针测试表明,与源自纳米MoO 3颗粒的常规催化剂Ref-MoS 2 / Al 2 O 3相比,MoS 3衍生的催化剂MoS 2 / Al 2 O 3不仅包含几乎完全硫化的Mo物种,而且在其MoS 2纳米板上还具有更多的配位不饱和位点(CUS),从而成功制备了具有弱得多的Mo-Al的双金属催化剂NiMoS 2 / Al 2 O 3与传统方法相比,MoS 2纳米板上具有2 O 3相互作用和较高的Ni原子修饰度。该双金属催化剂的这些显著结构上的优点,不仅避免强干扰的γ-Al 2 ö 3到活性相,还带来潜在的极好的镍催化活性。然后,以喹诺酮(Q)为反应剂,探讨了镍对加氢脱氮(HDN)活性的促进作用。发现当用Ni原子修饰MoS 2纳米板时,HDN活性得到了本质的改善。而且,这种镍促进作用比路径I(Q→14THQ→OPA→PB)对路径II(Q→14THQ / 58THQ→DHQ→PCHA→PCHE + PCH)更有利。最终提出了促进HDN活性的Ni促进作用的起源:Ni原子一方面激活H 2以产生活化的氢,然后与Mo-S 2-物种反应形成Mo-SH物种,另一方面增加碱度。相邻的Mo-S 2-,它们一起促进CN键的断裂,从而显着增强HDN活性。

更新日期:2020-02-07
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