镶嵌式钌炭催化剂的制备及芳环加氢性能

发布时间：2018-01-07 04:02

  本文关键词：镶嵌式钌炭催化剂的制备及芳环加氢性能　出处：《浙江工业大学》2016年硕士论文　论文类型：学位论文

  更多相关文章： 镶嵌式催化剂 钌炭催化剂 芳环加氢 固相碾磨法

【摘要】：新型镶嵌式钌炭催化剂具有载体与活性组分之间的相互作用力强、抗烧结、抗流失性好等特征,在加氢反应中具有较好的活性及稳定性。通过浸渍/模板法和固相研磨/模板法制备了新型镶嵌式的介孔钌炭催化剂。用氮气物理吸附、CO化学吸附、TPR-MS、XRD、TEM、SEM等技术对催化剂进行了表征,研究了其在甲苯、苯甲酸、对苯二甲酸二甲酯等芳环加氢反应中的性能,取得了以下结果:1.制备了系列不同方法改性的活性炭负载的Ru/AC催化剂和浸渍模板法制备了镶嵌式Ru-MC催化剂,考察了上述催化剂在甲苯、对苯二甲酸二甲酯及苯甲酸等不同取代基的芳环加氢反应中的性能。在所有的芳环加氢反应中,随着活性炭表面含氧基团的增加,Ru/AC催化活性增加;镶嵌式Ru-MC催化剂的芳环加氢性能远高于负载型Ru/MC催化剂;对不同取代基的芳环加氢反应,底物的取代基位阻越大,芳环加氢越困难,催化剂的活性越低。2.用固相研磨模板法和浸渍模板法制备了镶嵌式钌炭催化剂,和负载型的Ru/MC,Ru/AC催化剂的加氢性能做了对比。固相碾磨法模板法制备的Ru-MC-g和浸渍模板法制得Ru-MC的苯甲酸苯环加氢性能相当,但因前者制备的催化剂钌纳米粒子的镶嵌度稍高,表面暴露的钌原子比例较低,所以其TOF值最高,在120 ℃,和4.0 MPa氢气压力条件下,Ru-MC-g催化剂的TOF达到了2415 h~(-1),较负载型催化剂的活性提高了约6倍。3.利用固相研磨模板法,采用尿素作为氮源,制备了N掺杂的介孔炭材料,用其作载体制备了负载型Ru/MC-N催化剂。随着制备过程中尿素添加量的增加,其载体中的N含量也增加,其负载催化剂的活性先增高后降低。
[Abstract]:The new type of inlaid ruthenium carbon catalyst has the characteristics of strong interaction between the support and active components, anti-sintering, good anti-loss, and so on. A new type of mesoporous ruthenium carbon catalyst was prepared by impregnation / template method and solid phase grinding / template method. The catalyst was characterized by TPR-MSXRDX Tem SEM and its performance in the hydrogenation of toluene, benzoic acid and dimethyl terephthalate was studied. The following results were obtained: 1. A series of modified activated carbon supported Ru/AC catalysts and impregnated Ru-MC catalysts were prepared. The above catalysts were investigated in toluene. The properties of aromatic ring hydrogenation of dimethyl terephthalate and benzoic acid were studied. The catalytic activity of Ru-r-AC increased with the increase of oxygen-containing groups on the surface of activated carbon. The hydrogenation performance of the embedded Ru-MC catalyst is much higher than that of the supported Ru/MC catalyst. For the hydrogenation of aromatic rings with different substituents, the larger the substituent resistance of the substrates is, the more difficult the hydrogenation of aromatic rings is, and the lower the activity of the catalysts is. 2. The inlaid ruthenium carbon catalysts are prepared by solid phase grinding template method and impregnation template method. And load type Ru/MC. The hydrogenation performance of Ru/AC catalyst was compared. The hydrogenation performance of Ru-MC-g prepared by solid phase milling method was comparable to that of Ru-MC prepared by impregnation template method. However, the TOF value of ruthenium nanoparticles prepared by the former was the highest at 120 鈩，

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