Preparation of CoMo/γ-Al2O3 catalyst for hydrodesulfurization by impregnation with pulsed electromagnetic fields
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摘要: 利用脉冲电磁场（PEMF）辅助浸渍法和常规等体积浸渍法制备了一系列CoMo/γ-Al2O3加氢脱硫催化剂样品。以噻吩、2-甲基噻吩或苯并噻吩为模型化合物，在微反装置上评价了催化剂的加氢脱硫活性，经200 V脉冲电磁场处理的催化剂上各硫化物的转化率均比常规催化剂明显提高。采用XRD、BET、H2-TPR和TEM等方法表征了催化剂样品的表面状态和物化性质。结果表明，适当强度的脉冲电磁场与制备体系内带电粒子的交互作用有助于催化剂活性组分的分散，使活性组分在γ-Al2O3载体表面分布更为均匀，同时削弱了活性组分MoO3同载体间的较强相互作用，降低了催化剂表面钼物种的还原温度，促进了CoMoS活性相的形成。
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关键词:
- 脉冲电磁场 /
- CoMo/γ-Al2O3 /
- 负载型催化剂 /
- 浸渍法 /
- 加氢脱硫
Abstract: CoMo/γ-Al2O3 catalyst for hydrodesulfurization (HDS) were prepared by equal volume impregnation method with and without the presence of pulsed electronmagnetic field (PEMF). Experimental results revealed that the catalyst prepared by PEMF with a voltage of 200 V exhibited higher catalytic activity for hydrodesulfurization of thiophene, 2-methythiophene and benzothiophene than the catalyst prepared by conventional impregnation. The surface morphology and physico-chemical properties were characterized by using BET, XRD, H2-TPR and TEM techniques, respectively. The results showed that appropriate PEMF treatment promotes the active component dispersion on the γ-Al2O3 surface by interacting with the charged particles in reaction system. The interaction between the support and the active species MoO3 is weakened and thus facilitates the reduction of the catalyst and the formation of CoMoS active phase.-
Key words:
- pulsed electronmagnetic field /
- CoMo/γ-Al2O3 /
- supported catalyst /
- impregnation /
- hydrodesulfurization
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图 2 γ-Al2O3载体及不同催化剂样品的N2吸附-脱附等温线及其孔结构参数
Figure 2 N2 adsorption-desorption isotherms and pore structural parameters of γ-Al2O3 and the catalyst samples
图 4 催化剂样品的TEM照片
Figure 4 TEM images of the catalyst samples
(a) and (b): CON-Cat; (c) and (d): Cat 200 V
表 1 不同催化剂样品对噻吩、2-甲基噻吩和苯并噻吩加氢脱硫的催化活性
Table 1 Catalytic activity for hydrodesulfurization (HDS) of thiophene, 2-methythiophene and benzothiophene
Catalyst Thiophene conversion x /% 2-methythiophene conversion x /% Benzothiophene conversion x /% 60 min 90 min 120 min 60 min 90 min 120 min 60 min 90 min 120 min CON-Cat 82.97 54.79 39.43 75.68 50.73 35.82 69.52 51.64 32.86 Cat 100 V 83.36 65.38 41.94 73.58 48.96 37.63 71.35 53.48 33.62 Cat 200 V 91.50 74.09 51.59 86.25 71.59 48.26 80.67 71.95 43.55 Cat 400 V 83.78 72.65 43.79 71.45 46.65 32.79 70.12 48.85 36.78 Cat 600 V 78. 82 63.18 35.68 68.95 43.26 31.54 68.56 43.98 33.59 T203 78.34 57.84 47.62 78.63 56.26 46.65 65.25 52.31 42.96 
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表 2 噻吩、2-甲基噻吩和苯并噻吩的非氢原子净电荷
Table 2 Non-hydrogen atom charges for thiophene, 2-methythiophene and benzothiophene
Atom Thiophene 2-methythiophene Benzothiophene C1 -0.0951 -0.0991 -0.052 C2 -0.0747 -0.0776 -0.0503 C3 -0.0747 -0.0825 -0.0174 C4 -0.0951 -0.0321 -0.0267 S 0.0786 0.0690 0.0738 C6 - -0.0965 -0.0574 C7 - - -0.0533 C8 - - -0.0704 C9 - - -0.0813 Molecular structure 
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