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双功能钛硅分子筛的合成、表征及催化性能
Synthesis, characterization, and catalytic performance of bifunctional titanium silicalite-1
【摘要】 以四丙基溴化铵为模板剂,硅溶胶为硅源,正丁胺为碱源,采用水热合成的方法,将三价离子(Al3+,B3+或Fe3+)和Ti4+同时引入到MFI型分子筛的骨架,得到同时具有氧化和酸催化活性的双功能钛硅分子筛M-TS-1(M=Al,B或Fe).通过X射线粉末衍射、傅里叶变换红外光谱、紫外-可见漫反射光谱、氨程序升温脱附、电感耦合等离子体原子发射光谱和N2吸附-脱附等温线手段对样品进行了表征.结果表明,三价离子的引入,提高了TS-1的酸强度和酸量.采用乙烯选择氧化为探针反应考察了M-TS-1的催化性能.结果表明,Al-TS-1和B-TS-1在乙烯环氧化及后续的开环溶剂解反应中表现出较高的催化性能,H2O2的转化率在95%以上,H2O2的利用率大于90%,乙二醇和乙二醇单甲醚的总收率可达10%以上.
【Abstract】 A series of bifunctional Ti‐molecular sieves (M‐TS‐1, M=Al, B, or Fe) containing different trivalent ions (Al3+, B3+, or Fe3+), with MFI topology, were synthesized using tetrapropylammonium bromide, silica sol, and n‐butylamine as a template, base, and Si source, respectively. The simultaneous presence of Ti and trivalent ions in lattice positions provided catalysts with activity in both oxidation and acid‐catalyzed reactions. The samples were characterized using X‐ray diffraction, Fourier‐transform infrared spectroscopy, ultraviolet‐visible spectroscopy, NH3 temperature‐programmed desorption, inductively coupled plasma atomic emission spectroscopy, and N 2 adsorption‐desorption isotherms. The results showed that the numbers and strength of acid sites of TS‐1 were enhanced by the incorporation of trivalent ions. Using selective oxidation of ethylene as the probe reaction, the catalytic properties of M‐TS‐1 were investigated. The results showed that Al‐TS‐1 and B‐TS‐1 had better catalytic properties; conversion and utilization of H2O2 reached 95% and 90%, respectively, and the yield of ethylene glycol plus its monomethyl ether was greater than 10%.
- 【文献出处】 催化学报 ,Chinese Journal of Catalysis , 编辑部邮箱 ,2013年07期
- 【分类号】TQ424.25
- 【被引频次】18
- 【下载频次】501