活性金属对含甲烷氛围稠环芳烃加氢转化性能的影响  

Influence of reactive metals on hydroconversion performance of polycyclic aromatic hydrocarbons with methane-containing atmosphere

作　　者：梁生荣[1,2,3] 张赏莉 申志兵 唐瑞源[1,2,3] 任朝阳 李乐园 LIANG Shengrong;ZHANG Shangli;SHEN Zhibing;TANG Ruiyuan;REN Zhaoyang;LI Leyuan(College of Chemistry and Chemical Engineering,Xi’an Shiyou University,Xi’an 710065,China;Xi’an Key Laboratory of Low-carbon Utilization of High Carbon Resources,Xi’an 710065,China;Shaanxi Green Low-Carbon Energy Materials and Process Engineering Technology Research Center,Xi’an 710065,China)

机构地区：[1]西安石油大学化学化工学院,陕西西安710065 [2]西安市高碳资源低碳化利用重点实验室,陕西西安710065 [3]陕西省绿色低碳能源材料与过程工程技术研究中心,陕西西安710065

出　　处：《石油化工》2023年第10期1361-1367,共7页Petrochemical Technology

基　　金：西安石油大学研究生创新与实践能力培养项目(YCS22213097);重质油国家重点实验室开放基金项目(SKLHOP201703);国家油页岩开采研发中心开放基金课题项目(33550000-22-ZC0613-0255);中国石油科技创新基金项目(2022DQ02-0402)。

摘　　要：在Hβ分子筛上负载不同活性金属制备了系列催化剂,利用GC、XRD、N2吸附-脱附、Py-IR、NH_(3)-TPD等方法对催化剂进行了表征,并以萘为模型化合物,考察了催化剂在CH_(4)-H_(2)混合气氛下对稠环芳烃加氢裂化反应过程的影响。实验结果表明,负载的活性金属均可以均匀分散在Hβ分子筛表面,促进萘加氢开环,萘转化率均达到80%以上。其中,Zn/Hβ,Cu/Hβ,Co/Hβ催化剂的主要产物为甲苯和二甲苯,表明CH_(4)被活化并参与了反应,提高了含甲基侧链芳烃的加氢裂化产物选择性。尤其是Zn/Hβ催化剂,在CH_(4)-H_(2)气氛下,表现出高液相收率和高苯-甲苯-二甲苯混合物选择性,分别为91.34%和56.78%。研究结果可为重质油和天然气资源的高效利用提供新的方向。A series of catalysts were prepared by loading different active metals on Hβmolecular sieves,and the catalysts were characterized by GC,XRD,N2 adsorption-desorption,Py-IR,and NH_(3)-TPD.The effects of the catalysts on the process of hydrocracking reaction of polycyclic aromatic hydrocarbons under the mixed atmosphere of CH_(4)-H_(2) were investigated using naphthalene as a model compound.The experimental results show that all loaded active metals can be uniformly dispersed on the surface of Hβmolecular sieves to promote naphthalene hydrogenation and ring opening,and the naphthalene conversions all reach more than 80%.The main products by Zn/Hβ,Cu/Hβ,and Co/Hβcatalysts are toluene and xylene,indicating that CH_(4) is activated and participates in the reaction,which improves the hydrocracking product selectivity of methyl-containing side-chain aromatics.In particular,Zn/Hβcatalyst exhibites high liquid phase yield and high benzene-toluene-xylene mixture selectivity of 91.34%and 56.78%respectively under CH_(4)-H_(2) atmosphere.The results may provide a new direction for the efficient utilization of heavy oil and natural gas resources.

关 键 词：稠环芳烃 加氢裂化 活性金属 选择性 

分 类 号：TQ426.8[化学工程]