P改性β沸石的制备及其催化C_(9)芳烃与丙烯的烷基化反应性能研究  

Preparation of modifiedβzeolite with phosphorus for catalytic alkylation of C_(9) aromatics with propylene

作　　者：陈强强[1] 郭宇[1] 吴红梅[1] CHEN Qiang-qiang;GUO Yu;WU Hong-mei(School of Chemical and Environmental Engineering,Liaoning University of Technology,Jinzhou 121001,China)

机构地区：[1]辽宁工业大学化学与环境工程学院,辽宁锦州121001

出　　处：《燃料化学学报》2022年第1期98-108,共11页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21601075);辽宁省高校基本科研项目(JZL201715403);辽宁省“百千万人才工程”项目(辽人社函〔2020〕78号);辽宁省“兴辽英才计划”项目(XLYC2007171)资助。

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、N_(2)吸附-脱附和NH_(3)-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C_(9)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C_(9)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C_(12+)重芳烃的比例达到17%,m_(1,3,5-TMB)/mC_(9)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。To investigate the catalytic properties ofβzeolite for catalytic alkylation of C_(9) aromatics with propylene,βzeolites modified with phosphorus were prepared by using impregnation method.The modifiedβcatalysts with different loading amount of phosphorus were characterized by XRD,SEM,EDX,MAS NMR,Py-IR,N_(2) adsorptiondesorption,and NH_(3)-TPD.The results showed that the morphology and crystal structure of theβzeolite catalysts did not change obviously after modification with phosphorus.However,the specific surface area and the surface Si/Al mass ratio of theβzeolite decreased with the increase of amount of phosphorus.It was proved that the interaction between the phosphorus andβzeolite could affect the acid strength distribution of βzeolite and the catalytic performance of alkylation of C_(9)aromatics.In comparison withβzeolite,theβzeolite modified with 0.5%phosphorus(β-0.5P)had good catalytic performance in alkylation reaction of C_(9)aromatics.The ratio of C_(12+)aromatics in the alkylation products was up to 17%,and the value of m1,3,5-TMB/mC_(9)was increased by 5.3%.Theβ-0.5P catalytic activity showed stable after reaction for 10 h.However,when the loading amount of phosphorus onβzeolite was too high,the alkylation activity of the catalyst decreased and the isomerization and disproportionation performance of the catalyst increased.

关 键 词：Β沸石 改性 C_(9)芳烃 丙烯 烷基化 

分 类 号：TE624[石油与天然气工程—油气加工工程]