摘要
以氟化铵(NH4F)为结构导向剂,采用晶种诱导法合成方糖状全硅分子筛(Cubic Sugarshaped Silicon-1,缩写为CSS)。在pH值为9.5的碱性条件下,利用聚合物电解质PDDA对方糖状全硅分子筛进行表面电荷修饰,在钛溶胶体系当中静止吸附4 h后,借助水蒸气静态晶化24 h,得到全硅分子筛表面包裹钛硅结构的方糖状CSS@n-TS-1分子筛,并采用SEM、 TEM、 XRD、 FT-IR、UV-vis、XPS和N2气吸脱附等手段对CSS@n-TS-1分子筛进行表征分析。结果表明,CSS@n-TS-1分子筛颗粒尺寸为100 nm左右,具有多级介孔结构,表相中Ti的含量在9.0%以上。在以含500 mg/L的二苯并噻吩(DBT)或4,6-二甲基二苯并噻吩(4,6-DMDBT)的正辛烷作为模拟油的催化氧化脱硫反应体系中,表面富钛的方糖状的CSS@n-TS-1分子筛对大分子有机硫化合物显示出优异的催化氧化脱硫性能,在150 min内,DBT或4,6-DMDBT转化率均可达到100%。
Cubic sugar-shaped silicon-1(CSS)was synthesized by using the seed induction method with ammonium fluoride(NH4F)as the structure directing agent.The surface charge of CSS was then modified using the polymer electrolyte PDDA under alkaline conditions with a pH value of 9.5.After static adsorption in a titanium sol system for 4 h,the PDDA-modified CSS was further crystallized statically with water vapor for 24 h,to obtain the cubic sugar-shaped CSS@n-TS-1 zeolites where a titanium-silicon structure was coated on the surface of the all-silica zeolites.The CSS@n-TS-1 zeolites were characterized by means of SEM,TEM,XRD,FT-IR,UV-vis spectroscopy,XPS and N2 sorption.The results indicate that the CSS@n-TS-1 zeolites display a hierarchical mesoporous structure,with a particle size of about 100 nm;in addition,the content of Ti in the surface phase is over 9.0%.When used in the oxidative desulfurization of a model oil,viz.,n-octane containing 500 mg/L dibenzothiophene(DBT)or 4,6-dimethyldibenzothiophene(4,6-DMDBT),the cubic sugar-shaped CSS@n-TS-1 zeolites with a titanium-rich surface exhibit excellent catalytic performance in the oxidative desulfurization towards large molecular organic sulfur compounds;the conversion of both DBT and 4,6-DMDBT reach 100% within 150 min.
作者
张玉妹
任铁强
王钰佳
孙悦
耿忠兴
武宏大
刘宇彤
王海彦
ZHANG Yumei;REN Tieqiang;WANG Yujia;SUN Yue;GENG Zhongxing;WU Hongda;LIU Yutong;WANG Haiyan(School of Petrochemical Engineering,Liaoning Petrochemical University,Fushun 113001,China)
出处
《燃料化学学报(中英文)》
北大核心
2025年第11期1617-1627,共11页
Journal of Fuel Chemistry and Technology
基金
辽宁省教育厅基本科研基金(JYTMS20231433)资助。
关键词
钛硅分子筛
表面富钛
方糖状
氧化脱硫
titanium silicate zeolite
titanium-enriched silicon surface
cubic-sugar shaped
oxidative desulfurization
