多级孔道TS-1干胶法制备及其催化性能研究
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摘要
TS-1的成功开发被视为沸石及多相催化领域的里程碑。然而由于其孔道狭窄,限制了它在石油化工及精细化工等领域的应用。因此,合成具有介孔/大孔的多级孔道TS-1非常有意义。目前,多级孔道沸石多采用模板法水热晶化制备；然而大部分模板剂制备过程繁琐,价格昂贵,而且在晶化的过程中也经常会发生钛硅物种与介孔/大孔模板剂相分离的现象。为了解决上述问题,本文研究采用干胶法,以廉价的糖类为介孔/大孔模板剂制备多级孔道TS-1。论文的主要内容如下：
在TPABr为微孔模板剂的合成体系中,采用干胶法制备了TS-1,并对其合成条件及催化性能进行了研究。随着釜底液相中n(EDA)/n(H2O)摩尔比的降低,TS-1的结晶度、骨架钛的含量以及其在噻吩氧化反应中的催化活性均呈现出升高的趋势。当n(TPABr)/n(SiO2)摩尔比超过0.12后,所得TS-1的结晶度及骨架钛含量变化不大。
采用硅碳复合物合成路线,制备了多级孔道TS-1,其介孔/大孔分布主要集中于5-200nm之间。晶化时间为7d时,所得分子筛样品的结晶度最高。随着干胶碳化温度的降低,多级孔道TS-1的亲水性逐渐增强,介孔/大空的孔径也随之增大。多级孔道TS-1在噻吩氧化中的催化活性明显高于TS-1,而且能够催化较大分子硫化物苯并噻吩的氧化反应。当以H2O2为氧化剂时,亲水性较弱的多级孔道TS-1在苯并噻吩的氧化反应中显示了较高的催化活性。
以焦糖为介孔/大孔模板剂,制备了多级孔道TS-1。焦糖可由葡萄糖的氨水溶液在145℃下反应0.5h而制得。在沸石胶液烘干的同时,焦糖能够部分碳化而直接转化为硬模板,避免了硅碳复合物合成路线所需的惰性气体保护下的碳化过程。随着n(氨)/n(葡萄糖)摩尔比的增加,焦糖Zeta电位逐渐由正值变为负值；但不影响其作为模板剂应用于多级孔道TS-1的制备。分别采用N2物理吸附法和压汞法对所得多级孔道TS-1进行了表征,结果表明多级孔道TS-1具有相互连通且可延伸至表面的介孔/大孔孔道。与TS-1相比,多级孔道TS-1在硫化物噻吩、苯并噻吩及4,6-二甲基二苯并噻吩的氧化反应中均表现出良好的催化活性。
直接采用农产品蔗糖(成品)为模板剂,同样能够制备出含有介孔及大孔孔道的多级孔道TS-1。N2物理吸附法和压汞法的表征结果表明这些介孔/大孔并不是封闭的孔道。n(蔗糖)/n(SiO2)摩尔比在0.25-0.52的范围内,增加蔗糖的用量,多级孔道TS-1的结晶度变化不大,但样品中非骨架钛含量有所增加。此外,还将由甘蔗直接榨取(成品蔗糖生产的第一道工序)得到的蔗糖汁用于多级孔道TS-1的制备,这明显简化了模板剂的生产工艺。多级孔道TS-1在噻吩、苯并噻吩及4,6-二甲基二苯并噻吩的氧化反应中催化活性明显高于TS-1。
The discovery of TS-1is a milestone in zeolite and heterogeneous catalysis research fields. But the pore size of TS-1is small, which limites its application in the area of petrochemical industry and fine chemicals. Hence, it is important to synthesize the hierarchical TS-1with meso/macropores. Currently, the templating method for the preparation of hierarchical zeolites is always used in the system of conventional hydrothermal crystallization. However, the preparation processes of many templates are complicated, and some other templates are costly. Moreover, the titanium and silicalite species are often separated with the meso/macroporous templates during the hydrothermal crystallization. To solve the problems mentioned above, we adopted the dry gel conversion method to synthesize hierarchical TS-1with the carbohydrates as the meso/macropore templates. The main contents of this paper are as follows.
With TPABr as the microporous template, the TS-1is prepared by dry gel conversion method. The synthetic conditions and catalytic performance of TS-1samples are investigated in details.With the decrease of the n(EDA)/n(H2O) molar ratio at the bottom of autoclave, TS-1samples present the trend of increase for the crystallinity, Ti content in framework and the catalytic activities in Th oxidation. The content of TPABr has no obvious effect on the crystallinity and the framework Ti content of TS-1as the n(TPABr)/n(H2O) molar ratio exceeds0.12.
The hierarchical TS-1has been prepared following the route of silicalite-carbon complex, and the meso/macropores size of the sample is mainly in the range of the5-200nm. As the crystallization time is7d, the crystallinity of the obtained hierarchical TS-1sample is high. With the carbonization temperature of dry gel decreasing, the hydrophilicity of hierarchical TS-1is strengthened and the meso/macropore size increases. The hierarchical TS-1exhibits better catalytic performance than TS-1in Th oxidation and could catalyze the oxidation of bulky molecule sulfur compounds BT. The catalytic activity of hierarchical TS-1with weak hydrophilicity is high in the oxidation of BT with the H2O2as oxidant.
The hierarchical TS-1is synthesized with the meso/macroporous template caramel that could be obtained through the heat-treatment of aqueous solution of glucose and ammonia at145℃for0.5h. The caramel could spontaneously convert to hard template due to partial carbonization during dryness of gel, which avoids high-temperature carbonization in inert atmosphere. With the n(ammonia)/n(glucose) molar ratio increasing, fhe Zeta potential of caramel changes from positive to negative. But the camarel with positive or negative Zeta potential could be used as meso/macroporous templates to synthesize the hierarchical TS-1. Both N2physical adsorption-desorption and mercury porosimetry are adopted to characterize the hierarchical TS-1, and the results show that the obtained samples possess the well connected network of meso/macropores that could be fully accessible from the external surface. Compared with TS-1, hierarchical TS-1exhibits improved catalytic performance in the oxidation of sulfur compounds Th, BT and4,6-DMDBT.
The hierarchical TS-1could be also synthesized by directly using agricultural product sucrose (finished product) as meso/macroporous templates. The characterization results of N2physical adsorption-desorption and mercury porosimetry indicate that these meso/macropores are not closed. The crystallinity of the hierarchical TS-1samples change little with the n(sucrose)/n(SiO2) molar ratio in the range of0.25～0.52, but the content of the extra-framework Ti increases as the amount of sucrose increasing. Moreover, the purely natural sugar juice directly squeezed from the sugarcane (the first procedure for sucrose pruduction) is also applied in the preparation of the hierarchical TS-1. The hierarchical TS-1shows better catalytic activities than TS-1in the oxidation of Th, BT and4,6-DMDBT.
在TPABr为微孔模板剂的合成体系中,采用干胶法制备了TS-1,并对其合成条件及催化性能进行了研究。随着釜底液相中n(EDA)/n(H2O)摩尔比的降低,TS-1的结晶度、骨架钛的含量以及其在噻吩氧化反应中的催化活性均呈现出升高的趋势。当n(TPABr)/n(SiO2)摩尔比超过0.12后,所得TS-1的结晶度及骨架钛含量变化不大。
采用硅碳复合物合成路线,制备了多级孔道TS-1,其介孔/大孔分布主要集中于5-200nm之间。晶化时间为7d时,所得分子筛样品的结晶度最高。随着干胶碳化温度的降低,多级孔道TS-1的亲水性逐渐增强,介孔/大空的孔径也随之增大。多级孔道TS-1在噻吩氧化中的催化活性明显高于TS-1,而且能够催化较大分子硫化物苯并噻吩的氧化反应。当以H2O2为氧化剂时,亲水性较弱的多级孔道TS-1在苯并噻吩的氧化反应中显示了较高的催化活性。
以焦糖为介孔/大孔模板剂,制备了多级孔道TS-1。焦糖可由葡萄糖的氨水溶液在145℃下反应0.5h而制得。在沸石胶液烘干的同时,焦糖能够部分碳化而直接转化为硬模板,避免了硅碳复合物合成路线所需的惰性气体保护下的碳化过程。随着n(氨)/n(葡萄糖)摩尔比的增加,焦糖Zeta电位逐渐由正值变为负值；但不影响其作为模板剂应用于多级孔道TS-1的制备。分别采用N2物理吸附法和压汞法对所得多级孔道TS-1进行了表征,结果表明多级孔道TS-1具有相互连通且可延伸至表面的介孔/大孔孔道。与TS-1相比,多级孔道TS-1在硫化物噻吩、苯并噻吩及4,6-二甲基二苯并噻吩的氧化反应中均表现出良好的催化活性。
直接采用农产品蔗糖(成品)为模板剂,同样能够制备出含有介孔及大孔孔道的多级孔道TS-1。N2物理吸附法和压汞法的表征结果表明这些介孔/大孔并不是封闭的孔道。n(蔗糖)/n(SiO2)摩尔比在0.25-0.52的范围内,增加蔗糖的用量,多级孔道TS-1的结晶度变化不大,但样品中非骨架钛含量有所增加。此外,还将由甘蔗直接榨取(成品蔗糖生产的第一道工序)得到的蔗糖汁用于多级孔道TS-1的制备,这明显简化了模板剂的生产工艺。多级孔道TS-1在噻吩、苯并噻吩及4,6-二甲基二苯并噻吩的氧化反应中催化活性明显高于TS-1。
The discovery of TS-1is a milestone in zeolite and heterogeneous catalysis research fields. But the pore size of TS-1is small, which limites its application in the area of petrochemical industry and fine chemicals. Hence, it is important to synthesize the hierarchical TS-1with meso/macropores. Currently, the templating method for the preparation of hierarchical zeolites is always used in the system of conventional hydrothermal crystallization. However, the preparation processes of many templates are complicated, and some other templates are costly. Moreover, the titanium and silicalite species are often separated with the meso/macroporous templates during the hydrothermal crystallization. To solve the problems mentioned above, we adopted the dry gel conversion method to synthesize hierarchical TS-1with the carbohydrates as the meso/macropore templates. The main contents of this paper are as follows.
With TPABr as the microporous template, the TS-1is prepared by dry gel conversion method. The synthetic conditions and catalytic performance of TS-1samples are investigated in details.With the decrease of the n(EDA)/n(H2O) molar ratio at the bottom of autoclave, TS-1samples present the trend of increase for the crystallinity, Ti content in framework and the catalytic activities in Th oxidation. The content of TPABr has no obvious effect on the crystallinity and the framework Ti content of TS-1as the n(TPABr)/n(H2O) molar ratio exceeds0.12.
The hierarchical TS-1has been prepared following the route of silicalite-carbon complex, and the meso/macropores size of the sample is mainly in the range of the5-200nm. As the crystallization time is7d, the crystallinity of the obtained hierarchical TS-1sample is high. With the carbonization temperature of dry gel decreasing, the hydrophilicity of hierarchical TS-1is strengthened and the meso/macropore size increases. The hierarchical TS-1exhibits better catalytic performance than TS-1in Th oxidation and could catalyze the oxidation of bulky molecule sulfur compounds BT. The catalytic activity of hierarchical TS-1with weak hydrophilicity is high in the oxidation of BT with the H2O2as oxidant.
The hierarchical TS-1is synthesized with the meso/macroporous template caramel that could be obtained through the heat-treatment of aqueous solution of glucose and ammonia at145℃for0.5h. The caramel could spontaneously convert to hard template due to partial carbonization during dryness of gel, which avoids high-temperature carbonization in inert atmosphere. With the n(ammonia)/n(glucose) molar ratio increasing, fhe Zeta potential of caramel changes from positive to negative. But the camarel with positive or negative Zeta potential could be used as meso/macroporous templates to synthesize the hierarchical TS-1. Both N2physical adsorption-desorption and mercury porosimetry are adopted to characterize the hierarchical TS-1, and the results show that the obtained samples possess the well connected network of meso/macropores that could be fully accessible from the external surface. Compared with TS-1, hierarchical TS-1exhibits improved catalytic performance in the oxidation of sulfur compounds Th, BT and4,6-DMDBT.
The hierarchical TS-1could be also synthesized by directly using agricultural product sucrose (finished product) as meso/macroporous templates. The characterization results of N2physical adsorption-desorption and mercury porosimetry indicate that these meso/macropores are not closed. The crystallinity of the hierarchical TS-1samples change little with the n(sucrose)/n(SiO2) molar ratio in the range of0.25～0.52, but the content of the extra-framework Ti increases as the amount of sucrose increasing. Moreover, the purely natural sugar juice directly squeezed from the sugarcane (the first procedure for sucrose pruduction) is also applied in the preparation of the hierarchical TS-1. The hierarchical TS-1shows better catalytic activities than TS-1in the oxidation of Th, BT and4,6-DMDBT.
引文
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