自模板法制备大孔-微孔等级孔TS-1分子筛及其1-己烯环氧化性能  

Synthesis of Hierarchical Macro-Microporous TS-1 Zeolite by Self-Template Method for Efficient Catalytic Epoxidation of 1-Hexene

作　　者：时浩峰 孙明慧[1] 余申 刘湛 吕佳敏 朱绍林 陈丽华[1] 苏宝连[1,2] SHI Haofeng;SUN Minghui;YU Shen;LIU Zhan;L Jiamin;ZHU Shaolin;CHEN Lihua;SU Baolian(State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China;Laboratory of Inorganic Materials Chemistry,University of Namur,Namur B-5000,Belgium)

机构地区：[1]武汉理工大学材料复合新技术国家重点实验室,武汉430070 [2]那慕尔大学无机材料化学实验室,比利时那慕尔B-5000

出　　处：《石油学报（石油加工）》2024年第6期1485-1496,共12页Acta Petrolei Sinica(Petroleum Processing Section)

基　　金：国家重点研发计划项目(2022YFB3504000)基金资助。

摘　　要：针对等级孔钛硅分子筛TS-1合成方法存在步骤复杂及成本高等难题,使用二氧化硅纳米球同时作为硅源和大孔模板,结合蒸汽辅助结晶方法,通过“硅源溶解-分子筛结晶”过程形成大孔结构,得到大孔-微孔TS-1分子筛。通过调控二氧化硅纳米球的尺寸,可以系统调变大孔直径(100~500 nm)。此外,合成的大孔-微孔TS-1分子筛硅/钛摩尔比可调(30、50、100)。HTS-1-200-30分子筛样品在1-己烯催化环氧化反应中,温度343 K、反应时间6 h条件下1-己烯转化率可达41%,高于微孔TS-1分子筛的催化性能。研究所采用的自模板法使用低成本St9ber法制备二氧化硅纳米球,相较于高成本介孔二氧化硅纳米球,降低了等级孔钛硅分子筛的合成成本,适用于工业大规模生产。In response to the challenges such as complex procedure and high costs for the current synthesis method of the hierarchically porous titanosilicate zeolite TS-1,silica nanospheres were used as both silicon source and macroporous template in this work.Combined with the steam-assisted crystallization method,macroporous TS-1 zeolites were obtained by dissolution-crystallization process.The macropore size were systematically adjusted to be 100—500 nm by changing the diameters of silica dioxide nanospheres.In addition,the silica/titanium molar ratio of the synthesized macro-microporous TS-1 zeolites can be adjusted to be 30,50,100.At the temperature of 343 K and reaction time of 6 h,the conversion rate of 1-hexene in the catalytic epoxidation reaction over HTS-1-200-30 zeolite can reach 41%,demonstrating its higher catalytic performance than the microporous TS-1 zeolite.The self-template technique adopted by the research institute uses a low-cost St ber method to prepare silica nanospheres.Compared with high cost mesoporous silica nanospheres,the method reduces the synthesis cost of hierarchically porous titanosilicate zeolites,and is suitable for large-scale industrial production.

关 键 词：二氧化硅纳米球 自模板 蒸汽辅助晶化 大孔-微孔分子筛 TS-1分子筛 1-己烯环氧化 

分 类 号：O643.36[理学—物理化学]