当前位置: X-MOL 学术Catal. Today › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Effect of Pd- precursor and support acid properties on the Pd electronic state and the hydrodesulfurization activity of Pd-zeolite catalysts
Catalysis Today ( IF 5.3 ) Pub Date : 2018-08-02 , DOI: 10.1016/j.cattod.2018.07.058
Svetlana A. Yashnik , Gleb A. Urzhuntsev , Andrei I. Stadnichenko , Dmitry A. Svintsitskiy , Arcady V. Ishchenko , Andrei I. Boronin , Zinfer R. Ismagilov

We studied on the function of Pd species located in mesopores and inside zeolite channels (micropores) of the montmorillonite-modified zeolite catalyst for the hydrodesulfurization of diesel fraction with 350 ppm of sulfur as DBT, 4-MDBT, and 4,6-DMDBT. It was shown that the ex-dihydrogentetrachloropalladate impregnated catalyst as well as the ex-tetraamminepalladium(II) chloride ion-exchanged catalyst have high efficiency of sulfur removal from the diesel fuel in temperature range 280–300 оC.

The sulfur tolerance of catalyst depended on the method of Pd adding. The catalyst prepared by ion-exchange with tetraamminepalladium chloride solution exhibited the highest sulfur tolerance. According to FTIR of adsorbed CO, this catalyst contains a small Pd metal atoms or cluster in electron-deficient state inside zeolite channels. They probably ensure sulfur tolerance due to hydrogen spillover.

The montmorillonite addivite significantly modifies performance of the Pd-Zeolite catalyst in hydrotreating of diesel fraction. It leads to a decrease of cracking function, while those of hydrogenolysis of sulfurorganic molecules and hydrogenation of aromatic molecules are strengthened in comparison with the unmodified catalyst. This effect is explained by the change of acidic properties of the catalyst, limitations of diffusion of various molecules into the zeolite channels, and diffusion of Pd from the zeolite channels.



中文翻译:

钯前驱体和载体酸性质对钯电子态和钯沸石催化剂加氢脱硫活性的影响

我们研究了蒙脱石改性沸石催化剂的介孔和沸石通道(微孔)内部的Pd物种对以350 ppm的硫作为DBT,4-MDBT和4,6-DMDBT的柴油馏分进行加氢脱硫的功能。结果表明,该前dihydrogentetrachloropalladate浸渍的催化剂以及该前四氨(II)氯化物离子交换催化剂具有在温度范围280-300从柴油燃料硫去除的高效率 о C.

催化剂的耐硫性取决于Pd的添加方法。通过用四氨合氯化钯溶液进行离子交换而制备的催化剂表现出最高的耐硫性。根据吸附的CO的FTIR,该催化剂在沸石通道内包含小的Pd金属原子或电子缺乏状态的簇。由于氢的溢出,它们可能确保对硫的耐受性。

蒙脱土加成剂显着改变了钯-沸石催化剂在柴油馏分的加氢处理中的性能。与未改性的催化剂相比,它导致了裂化功能的降低,而硫有机分子的氢解和芳族分子的氢化得到了增强。可以通过改变催化剂的酸性性质,限制各种分子向沸石通道中扩散以及Pd从沸石通道中扩散来解释这种影响。

更新日期:2018-08-02
down
wechat
bug