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In situ synthesis of MoS2 nanoflakes within a 3D mesoporous carbon framework for hydrodesulfurization of DBT
Journal of Catalysis ( IF 6.5 ) Pub Date : 2022-10-13 , DOI: 10.1016/j.jcat.2022.10.006
Jilei Liang , Mengwei Fan , Mengmeng Wu , Jiawei Hua , Wangshui Cai , Tingting Huang , Yunqi Liu , Chenguang Liu

Two new mesoporous carbon-supported Co-Mo hydrodesulfurization catalysts with different Co contents have been successfully prepared by one-step vacuum freeze-drying, followed by calcination under a nitrogen atmosphere and washing. Evans-Showell polyoxometalate (NH4)6[Co2Mo10O38H4]·7H2O was used as the Co-Mo precursor instead of the conventional precursors, and the obtained catalysts were structurally characterized by various technologies, including X-ray diffraction, thermogravimetric analysis, scanning electron microscopy, high-resolution transmission electron microscopy, X-ray photoelectron spectroscopy, H2 temperature programmed reduction, CO temperature programmed desorption and low temperature N2 adsorption-desorption isotherm. The results show that MoS2 particles (4.6 nm and 4.5 slabs) are homogeneously dispersed in the mesoporous carbon framework with a narrow pore size distribution centered at 3.7 nm. The catalysts were evaluated by the hydrodesulfurization of dibenzothiophene, and the results show that the dibenzothiophene conversion, overall pseudo-first order rate constant and turnover frequency can reach 95 %, 5.4 × 10−6 mol g1 s−1 and 6.1 × 10−3 s−1 at 300 °C, respectively, indicating higher catalytic activity than previously reported catalysts. The higher proportion of the CoMoS active phase can account for the higher catalytic activity. By using in situ-produced sodium chloride crystals and thiourea as hard templates and sulfidizing agents respectively, this study opens a new avenue for the simple and environmentally friendly preparation of hydrodesulfurization catalysts with the synchronization and riveting of MoS2 nanoflakes and 3D mesoporous carbon frameworks.



中文翻译:

在 3D 介孔碳框架内原位合成 MoS2 纳米薄片用于 DBT 的加氢脱硫

通过一步真空冷冻干燥、氮气气氛下煅烧和洗涤,成功制备了两种不同Co含量的新型介孔碳负载Co-Mo加氢脱硫催化剂。Evans-Showell多金属氧酸盐(NH 4 ) 6 [Co 2 Mo 10 O 38 H 4 ]·7H 2 O作为Co-Mo前驱体代替了传统的前驱体,得到的催化剂通过多种技术进行了结构表征,包括X射线衍射、热重分析、扫描电子显微镜、高分辨率透射电子显微镜、X射线光电子能谱、H 2程序升温还原、CO程序升温脱附和低温N 2吸附-脱附等温线。结果表明,MoS 2颗粒(4.6 nm 和 4.5 板)均匀分散在介孔碳骨架中,孔径分布窄,中心为 3.7 nm。通过二苯并噻吩的加氢脱硫对催化剂进行了评价,结果表明二苯并噻吩的转化率、总准一级速率常数和周转频率可达到95%、5.4 × 10 -6 mol g - 1 s -1和6.1 × 10 -3-1分别在 300°C 下,表明催化活性高于先前报道的催化剂。较高比例的 CoMoS 活性相可以解释较高的催化活性。本研究利用原位制备的氯化钠晶体和硫脲分别作为硬模板和硫化剂,为同步铆接MoS 2纳米片和3D介孔碳骨架的加氢脱硫催化剂的简单、环保制备开辟了新途径。

更新日期:2022-10-15
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