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| 金属改性对钛硅分子筛TS-1上油酸甲酯
环氧化性能的影响 |
| ffect of metal modification on titanium silicalite TS-1 for methyl oleate epoxidation |
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| DOI： |
| 中文关键词: 油酸甲酯 环氧化 钛硅分子筛 TS-1 金属改性 |
| 英文关键词:methyl oleate epoxidation titanium silicalite TS-1 metal modification |
| 基金项目:湖南省自然科学基金面上项目（2021JJ30289） |
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| 中文摘要: |
| 环氧植物油可广泛用作各种化工材料，为提高植物油环氧化催化剂钛硅分子筛TS-1的活性，采用沉淀沉积法制备了系列金属改性的TS-1催化剂（M/TS-1，M为Mn、Fe、Cu、Mg），对其进行了表征，并以油酸甲酯环氧化为探针反应，考察了金属改性对TS-1上油酸甲酯环氧化性能的影响。结果表明：Fe和Cu的引入提高了TS-1的催化活性，但Mg和Mn改性却抑制了油酸甲酯的环氧化，Cu/TS-1催化剂的催化活性最高；结合多种表征结果发现，Cu/TS-1催化剂的高活性归因于Cu的引入有效地改变了Ti活性中心的电子环境，并增加了新的中强酸性位点；Cu/TS-1催化油酸环氧化的最佳工艺条件为反应温度80 ℃、H2O2与油酸甲酯物质的量比3∶ 1、油酸甲酯与催化剂质量比10∶ 1~20∶ 1；Cu/TS-1重复使用5次后，油酸甲酯转化率和环氧油酸甲酯收率略有降低。综上，采用Cu改性TS-1可显著提高其催化活性，且Cu/TS-1具有良好的再生性能。 |
| 英文摘要: |
| Epoxy vegetable oil has widely utilized as various chemical material. To improve the activity of titanium silicalite TS-1, a vegetable oil epoxidation catalyst, a series titanium silicalite TS-1 supported various metals catalysts (M/TS-1, M=Mn, Fe, Cu, Mg) were prepared by a deposition-precipitation method and characterized. The effect of metal modification on the epoxidation performance of methyl oleate on TS-1 was investigated using the epoxidation of methyl oleate as a probe reaction.The results showed that the introduction of Fe and Cu into TS-1 promoted the catalytic activity but Mg and Mn modification inhibited the methyl oleate conversion, and Cu/TS-1 catalyst showed the highest catalytic activity. Combined with various characterization results, the high activity of Cu/TS-1 catalyst was attributed to the introduction of Cu, which effectively changed the electronic environment of Ti active center and added new medium and strong acidic sites. The optimal process conditions for Cu/TS-1 catalyzed epoxidation of methyl oleate were obtained as follows: reaction temperature 80 ℃, molar ratio of H2O2 to methyl oleate 3∶ 1, mass ratio of methyl oleate to catalyst 10∶ 1-20∶ 1. The conversion of methyl oleate and the yield of epoxy oleic methyl ester were slightly reduced after Cu/TS-1 was repeated for 5 times. In summary, TS-1 modified by Cu can significantly improve its catalytic activity and Cu/TS-1 has good regeneration performance. |
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