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高硅MCM-22分子筛的合成与催化性能

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以六亚甲基亚胺(HMI)和N,N,N-三甲基-1-金刚烷基氢氧化铵(TMAdaOH)为复合有机结构导向剂合成高硅MCM-22分子筛,并负载钼制备不同SiO2/Al2O3摩尔比的MCM-22催化剂,采用XRD、FT-IR、UV-Raman、SEM、NH3-TPD等手段对分子筛产品进行表征,并对负载型MCM-22催化剂进行重芳烃轻质化反应性能评价.结果表明:HMI和TMAdaOH复合协同作用能有效促进硅原子进入MCM-22分子筛骨架,抑制麦羟硅钠石的出现,提升分子筛的骨架结晶性和结构稳定性,其中SiO2/Al2O3摩尔比80合成的MCM-22分子筛(S80)具有最高的微孔结晶度和丰富的中强酸分布;在反应温度为360 ℃、H2/重芳烃原料摩尔比为3.0、反应压力为3.0 MPa、MHSV为3.0 h-1的条件下,Mo/H-S8 0催化剂作用下碳九芳烃和碳十芳烃转化率分别为64.9％和62.7％,产物苯、甲苯和二甲苯的总选择性达到87.6％;对反应后Mo/H-S80催化剂的积炭分析结果表明,高硅MCM-22分子筛S80更易于扩散并转化重组分、控制副反应的发生,是高效轻质化的理想催化材料.
Synthesis and Catalytic Performance of High-Silicon MCM-22 Zeolite
High-silicon MCM-22 zeolite was synthesized using hexamethylene imine(HMI)and N,N,N-trimethyl-l-ammonium adamantine(TMAdaOH)as composite organic structure directing agents.MCM-22 catalysts with different SiO2/Al2O3 molar ratios were prepared by loading molybdenum.The MCM-22 zeolites were characterized by XRD,FT-IR,UV-Raman,SEM,and NH3-TPD,and the performance of the supported MCM-22 catalyst for heavy aromatics lightweight reaction was evaluated.The results show that the composite synergism of HMI and TMAdaOH can effectively promote the entry of Si atoms into the framework of MCM-22 zeolite,inhibit the emergence of magadiite,and thus improve the crystallinity and structural stability of the framework of molecular sieves.The MCM-22 zeolite(S80)with a SiO2/Al2O3 molar ratio of 80 boasts the highest microporous crystallinity and rich distribution of moderate-strong acid sites.When using Mo/H-S80 catalyst at the reaction temperature of 360 ℃,H2/heavy aromatic molar ratio of 3.0,reaction pressure of 3.0 MPa,and MHSV of 3.0 h-1,the conversion rates of C9 and C10 aromatics can reach 64.9％and 62.7％,respectively,and the total selectivity of the products benzene,toluene,and xylene(BTX)is 87.6％.The analysis of carbon deposition on the Mo/H-S80 catalyst after reaction shows that the high silicon MCM-22 zeolite S80 is more suitable for the diffusion and conversion of heavy components,and controlling the occurrence of side reactions.Thus,it is an ideal catalytic material for the efficient lightweight transformation.

SiO2/Al2O3 molar ratioMCM-22 zeoliteorganic structure directing agentheavy aromaticslightweight reactioncarbon deposit

童伟益、刘闯、张俊玲、侯敏

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中石化(上海)石油化工研究院有限公司绿色化工与工业催化全国重点实验室,上海 201208

华东理工大学化工学院,上海 200237

SiO2/Al2O3摩尔比 MCM-22分子筛 有机结构导向剂 重芳烃 轻质化反应 积炭

中国石油化工股份有限公司项目中国石油化工股份有限公司项目中国石油化工股份有限公司项目中国石油化工股份有限公司化工事业部课题

21/Y2S23-B5-00121/Y2S23-B1-00222/Y2S24-L1-00322/Y2S23-Y1-05

2024

10.3969/j.issn.1001-8719.2024.01.007

石油学报(石油加工)
中国石油学会

石油学报(石油加工)

CSTPCD北大核心
影响因子：0.764
ISSN：1001-8719
年,卷(期)：2024.40(1)
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