Catalytic hydrogenation of pyrene over Mo-doped NiC/Al-MCM-41

doi:10.16085/j.issn.1000-6613.2024-0102

Abstract

Abstract:

Supported NiC/Al-MCM-41 and NiMoC/Al-MCM-41 catalysts were prepared by hydrothermal synthesis and utilized in pyrene hydrogenation. The catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), N₂ physical adsorption, NH₃ temperature-programmed desorption (NH₃-TPD), and thermogravimetric analysis (TG). The hydrogenation activity of the catalysts was evaluated in a batch high-pressure reactor. The effects of Mo doping on the physical-chemical structure and hydrogenation activity of NiC/Al-MCM-41 catalyst were investigated, and the structure-activity relationship between the physical and chemical properties of the catalyst and hydrogenation activity was explored. The results showed that the NiMoC/Al-MCM-41 catalyst exhibited the best hydrogenation activity and could be partially regenerated at a reaction temperature of 340℃, H₂ pressure of 6MPa, and continuous reaction for 2h. Compared with NiC/Al-MCM-41 catalyst, Mo doping increased the conversion of pyrene from 65.2% to 90.8% and deep hydrogenation selectivity from 58.9% to 76.2%, which effectively improved the hydrogenation performance of the catalyst. However, the stability of NiMoC/Al-MCM-41 catalyst was poor due to the carbon deposition caused by pore channel blocking of the catalyst, which hindered the diffusion and transfer of pyrene molecules in the pore channels. Therefore, the catalyst resistance to carbon deposition should be further improved in the future.

Key words: polycyclic aromatic hydrocarbons, pyrene, hydrogenation, catalyst, Mo doping

摘要：

通过水热合成法分别制备了负载型NiC/Al-MCM-41和NiMoC/Al-MCM-41催化剂，并将其应用于芘加氢反应。采用X射线衍射（XRD）、X射线光电子能谱（XPS）、傅里叶变换红外光谱（FTIR）、扫描电子显微镜（SEM）、透射电子显微镜（TEM）、N₂物理吸附、NH₃程序升温脱附（NH₃-TPD）和热重（TG）对催化剂进行表征，并通过间歇高压反应釜对催化剂的芘加氢活性进行评价。探究Mo掺杂改性对NiC/Al-MCM-41催化剂物理-化学结构及加氢反应活性的影响，揭示催化剂物理和化学性质与加氢活性之间的构效关系。结果表明，在反应温度为340℃、H₂压力为6MPa、连续反应2h时，NiMoC/Al-MCM-41催化剂表现出最佳的加氢活性，且具有一定的再生性能。相较于NiC/Al-MCM-41催化剂，Mo掺杂改性使得芘加氢转化率和深度加氢选择性分别从65.2%和58.9%提升至90.8%和76.2%，有效地提高了催化剂的加氢反应性能。但由于积炭堵塞催化剂孔道，阻碍了芘分子在催化剂孔道内的扩散转递，导致NiMoC/Al-MCM-41催化剂的稳定性较差，后续应进一步提高催化剂的抗积炭性能。

关键词: 多环芳烃, 芘, 加氢, 催化剂, Mo掺杂

CLC Number:

TQ536

GUI Xin, CHEN Huiyong, BAI Boyang, JIA Yongliang, MA Xiaoxun. Catalytic hydrogenation of pyrene over Mo-doped NiC/Al-MCM-41[J]. Chemical Industry and Engineering Progress, 2024, 43(5): 2386-2395.

桂鑫, 陈汇勇, 白柏杨, 贾永梁, 马晓迅. Mo掺杂改性NiC/Al-MCM-41的芘催化加氢性能[J]. 化工进展, 2024, 43(5): 2386-2395.

Figures/Tables 14

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