P改性β沸石的制备及其催化C9芳烃与丙烯的烷基化反应性能研究

Preparation of modified β zeolite with phosphorus for catalytic alkylation of C9 aromatics with propylene

  • 摘要: 利用浸渍法对β沸石进行磷改性,制备了不同磷负载量的改性β沸石催化剂。采用XRD、SEM、EDX、MAS NMR、Py-FTIR、N2吸附-脱附和NH3-TPD手段对催化剂样品进行了表征,并且研究了改性β沸石在催化C9芳烃与丙烯烷基化反应中的性能。结果表明,β沸石经磷改性后,其形貌和晶体结构没有发生明显变化。然而,随着磷添加量的增加,β沸石的比表面积和表面硅铝质量比逐渐减小;磷与β沸石相互作用,改变了催化剂酸强度分布。β沸石上磷的负载量显著影响C9芳烃烷基化反应结果。与未改性的β沸石相比,β-0.5P催化剂烷基化反应活性明显提高,烷基化反应产物中C12+重芳烃的比例达到17%,m1,3,5-TMB/mC9值增加了5.3%,连续反应10 h,活性稳定;然而,当磷负载量过高,催化剂烷基化活性降低,异构化和歧化反应性能增强。

     

    Abstract: To investigate the catalytic properties of β zeolite for catalytic alkylation of C9 aromatics with propylene, β zeolites modified with phosphorus were prepared by using impregnation method. The modified β catalysts with different loading amount of phosphorus were characterized by XRD, SEM, EDX, MAS NMR, Py-IR, N2 adsorption-desorption, and NH3-TPD. The results showed that the morphology and crystal structure of the β zeolite catalysts did not change obviously after modification with phosphorus. However, the specific surface area and the surface Si/Al mass ratio of the β zeolite decreased with the increase of amount of phosphorus. It was proved that the interaction between the phosphorus and β zeolite could affect the acid strength distribution of β zeolite and the catalytic performance of alkylation of C9 aromatics. In comparison with β zeolite, the β zeolite modified with 0.5% phosphorus (β-0.5P) had good catalytic performance in alkylation reaction of C9 aromatics. The ratio of C12+ aromatics in the alkylation products was up to 17%, and the value of m1,3,5-TMB/mC9 was increased by 5.3%. The β-0.5P catalytic activity showed stable after reaction for 10 h. However, when the loading amount of phosphorus on β zeolite was too high, the alkylation activity of the catalyst decreased and the isomerization and disproportionation performance of the catalyst increased.

     

/

返回文章
返回