王亚权^1,2,3, 林永杰^1,2,3, 刘伟^1,2,3, 王书海^1,2,3, 叶家鑫^1,2,3, 李昊阳^1,2,3, 王守桂^1,2,3
AuthorsHTML:王亚权^1,2,3, 林永杰^1,2,3, 刘伟^1,2,3, 王书海^1,2,3, 叶家鑫^1,2,3, 李昊阳^1,2,3, 王守桂^1,2,3
AuthorsListE:Wang Yaquan ^1,2,3, Lin Yongjie^1,2,3, Liu Wei^1,2,3, Wang Shuhai^1,2,3, Ye Jiaxin^1,2,3, Li Haoyang^1,2,3, Wang Shougui^1,2,3
AuthorsHTMLE:Wang Yaquan ^1,2,3, Lin Yongjie^1,2,3, Liu Wei^1,2,3, Wang Shuhai^1,2,3, Ye Jiaxin^1,2,3, Li Haoyang^1,2,3, Wang Shougui^1,2,3
Unit:1. 绿色化学工艺教育部重点实验室，天津 300072；2. 天津大学化工学院，天津 300072；3.天津化学化工协同创新中心，天津 300072
Unit_EngLish:1．Key Laboratory for Green Chemical Technology of Ministry of Education, Tianjin 300072, China
2．School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
3．Collaborative Innovation Center of Chemical Science and Engineering(Tianjin), Tianjin 300072, China
Abstract_Chinese:用不同浓度的四丙基氢氧化铵(TPAOH)处理钛硅分子筛(TS-1), 处理后的钛硅分子筛作催化剂催化1-己烯发生环氧化反应．用X射线粉末衍射(XRD)、傅里叶变换红外光谱(FT-IR)、紫外漫反射(UV-Vis)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、N₂吸附-脱附曲线(BET)、氨气程序升温脱附(NH₃-TPD)和电感耦合等离子体发射光谱(ICP)对催化剂进行了表征．表征结果表明：样品的MFI结构没有被破坏; 当TPAOH碱处理钛硅分子筛时, 晶体内部部分硅溶解导致分子筛内部有介孔生成; 随着四丙基氢氧化铵浓度的增加, 分子筛中的骨架钛含量逐渐减少同时有非骨架钛生成．在催化1-己烯环氧化反应中, 介孔的生成使处理后的钛硅分子筛活性和选择性得到明显改善．但是当介孔体积大于0.219 cm³/g时, 由于骨架钛损失较多, 1-己烯转化率和1, 2-环氧己烷相对于1-己烯和过氧化氢的选择性都显著降低．
Abstract_English:Titanium silicalite-1(TS-1)was treated by tetrapropyl ammonium hydroxide(TPAOH)with different concentrations and used as catalyst in 1-hexene epoxidation. All the samples were characterized by X-ray powder diffraction(XRD)，Fourier-transform infrared spectrum(FT-IR)，ultraviolet-visible diffuse reflectance spectrum (UV-Vis)，scanning electron microscopy(SEM)，transmission electron microscopy(TEM)，nitrogen physical adsorption and desorption(BET)，NH₃-temperature programmed desorption(TPD)and inductively coupled plasma atomic emission spectrometry(ICP). The results show that the MFI structures of the samples are not destroyed and mesopores are formed in TS-1 crystals due to the dissolution of silica when TS-1 samples are treated by TPAOH. However，the framework Ti content decreases gradually，forming extraframework Ti. Due to the formation of mesopores，the catalytic activity and selectivity of the treated TS-1 are markedly improved in the reaction of 1-hexene epoxidation. However，when the volumes of the mesopores are larger than 0.219 cm³/g，the 1-hexene conversion and the selectivities of 1，2-epoxyhexane to 1-hexene and H₂O₂ sharply decrease as a result of the appreciable loss of the framework Ti in the TPAOH treatment.
Keyword_Chinese:钛硅分子筛; 四丙基氢氧化铵; 1-己烯环氧化; 介孔
Keywords_English:titanium silicalite-1(TS-1); tetrapropyl ammonium hydroxide(TPAOH); 1-hexene epoxidation; mesopores

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