钛硅分子筛/地聚物复合微球的制备及其催化性能

摘要/Abstract

摘要： 以经过聚乙烯亚胺（PEI）修饰后的地聚物微球（GQ）作为载体，采用原位生长的方法，制备了钛硅分子筛/地聚物复合微球（TS-1@GQ）。探讨了PEI浓度对TS-1@GQ催化性能的影响，并运用扫描电镜(SEM)、X射线衍射(XRD)、傅里叶变换红外光谱(FT-IR)、X射线光电子能谱(XPS)等方法对最佳TS-1@GQ进行表征，同时评价了其催化1-己烯制备1,2-环氧己烷的性能。结果表明，当PEI浓度达到0.003 mol/L时，TS-1@GQ表面的TS-1分子筛负载量(w)可达11.43%。在反应温度25 ℃下，当TS-1@GQ用量为0.02 g、n（1-己烯）：n（H₂O₂）为1：1时，TS-1@GQ对1-己烯的转化率可达13.19%，1,2-环氧己烷的选择性达到95.88%，优于商用TS-1的催化效果。此外，该催化剂还展现出了良好的可循环性。

关键词: 钛硅分子筛, 地聚物微球, 1-己烯, 1,2-环氧己烷

Abstract: Titanium-silicon molecular sieve/geopolymer composite microspheres (TS-1@GQ) were prepared by in situ growth method using geopolymer microspheres (GQ) modified with polyethyleneimine (PEI) as carriers. The effects of PEI concentration on the catalytic performance of TS-1@GQ were investigated, the optimal TS-1@GQ was characterized by scanning electron microscope (SEM), X-Ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS), and its catalytic performance for the preparation of 1,2-epoxyhexane from 1-hexene was also evaluated. The results showed that the loading of TS-1 molecular sieves on the surface of TS-1@GQ could reach 11.43% when the PEI concentration was 0.003 mol/L. At the reaction temperature of 25 ℃, when the dosage of TS-1@GQ was 0.02 g, and n(1- hexene): n(H₂O₂) was 1: 1, the conversion rate of 1-hexene could reach 13.19%, and the selectivity of 1,2-epoxyhexane could reach 95.88%. In addition, the catalyst also showed good recyclability.

Key words: titanium-silicon molecular sieve, geopolymer microspheres, 1-hexene, 1,2-epoxyhexane

陈锦泓王梦琦龙联真王扬扬苏文锋赖芳葛圆圆. 钛硅分子筛/地聚物复合微球的制备及其催化性能[J]. 石油炼制与化工, 2024, 55(12): 22-30.

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