多级孔道沸石分子筛的合成、表征及催化应用
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摘要
多级孔道沸石分子筛同时具有沸石分子筛及介孔材料的优点,具有很高的酸性、水热稳定性及多级孔道结构,同时具有很好的择形性能和传质能力,被认为是潜在的下一代催化材料,有望在重油裂化、大分子催化等领域中发挥重要作用。它的合成、表征及催化应用已经得到了广泛的研究。但是多级孔道沸石分子筛合成中的诸多关键问题仍未解决:如沸石分子筛的晶化、介孔形成机理及第二模板的作用等。而且目前多级孔道沸石分子筛的合成路线大部分是基于纳米复制技术开发的,合成工艺相对复杂,合成成本较高。所合成的介孔沸石中介孔孔道的有序程度也有待于进一步改善。本文通过吸收纳米技术、无机合成化学及沸石分子筛机理的最新研究结果,致力于这些关键问题的解决,形成更经济的多级孔道沸石分子筛合成方法,制备具有优良结构特征的多级孔道沸石分子筛。论文中详细研究了沸石分子筛在硬模板,软模板及无第二模板存在条件的晶化过程,开发了硬模板,软模板及无第二模板存在条件的多级孔道沸石分子筛的合成路线,认识不同合成路线所蕴含的共同点,并对所合成的多级孔道沸石分子筛样品进行详细的表征,同时考察了典型材料的催化性能。
不同结构炭材料为模板制备沸石分子筛的研究表明炭材料模板的结构特征对沸石分子筛的晶化过程有着很大的影响,通过控制炭材料的结构可以在很大程度上控制沸石分子筛的晶化过程。采用炭气凝胶为模板时不需要控制晶化条件即可合成含有晶体内介孔的沸石分子筛,所得介孔沸石的孔结构与炭材料模板具有良好的对应关系。在炭材料为模板的条件下更容易生成含无序介孔的纳米沸石团聚体,对比炭材料模板及沸石产物的结构发现某些条件下炭材料模板并没有起到占据孔道造孔的功能,因而在合成这一类沸石材料的过程中,介孔模板可能不是必须的。
采用具有不同初始炭纳米颗粒大小的炭气凝胶可以合成具有可调控介孔结构(尺寸10-100 nm)的介孔沸石。炭材料纳米复制法表征结果表明不同炭气凝胶合成的沸石样品具有不同的介孔连接性。
采用原位生成的CMK-5或常规表面活性剂及硅烷化类似物的混合物为模板可以实现均有序介孔沸石的合成。所得的有序介孔沸石具有很好的水热稳定性,产品经过120小时沸水处理及在水蒸气条件下850℃焙烧4小时后仍能保持所有的结构特征。两种合成路线中有序介孔沸石分子筛的形成均经历了无定形有序介孔二氧化硅的生成、初始二氧化硅相的溶解、沸石的成核及晶化等过程。在合成过程中对沸石的生长进行一定的限制是实现成功合成的关键因素,但限制作用并非越强越好,而需要控制在一个合适的范围,使得沸石分子筛的成核、生长能够与介孔相的生长、保持实现最优的匹配。
具有介孔的纳米沸石团聚体确实在较大分子尺寸化合物的催化反应中体现出比常规沸石分子筛更好的催化性能。采用CMK-3为模板合成的介孔TS-1纳米沸石团聚体在噻吩类含硫模型化合物的催化氧化反应中体现出比常规TS-1更好的催化性能,而且二苯并噻吩比噻吩更容易被氧化脱除。具有介孔的纳米ZSM-12沸石团聚体及ZSM-5团聚体可在没有第二模板存在的条件下通过纳米沸石分子筛的原位自组装成功合成。
多级孔沸石分子筛的合成通常是经历了基于颗粒团聚的沸石生长机理,多级孔道沸石分子筛的形成是沸石的晶化过程在特定的条件下终止而生成的动力学控制产物,而多级孔道的形成并不一定需要介孔形成模板的参与。
在2,6-二甲基萘选择合成的催化反应中,量子化学计算的结果表明目标产物2,6-二甲基萘的分子尺寸要略大于主要的副产物2,7-二甲基萘,但从本征的化学反应性上看2,6-二甲基萘比2,7-二甲基萘更有利于生成。基于这些计算结果,开发了Zr同晶取代的ZSM-5作为这一催化体系的催化剂。基于有序介孔沸石(OMZ-1)的催化剂在2-甲基萘选择甲基化反应中具有比常规ZSM-5更好的催化性能。在反应条件为反应温度为400℃,当2-MN的质量空速为0.5 h~(-1)和2-MN/甲醇/均三甲苯摩尔比为1:1:3时,经过8小时反应,2-甲基萘的转化率、β,β选择性、2,6-/2,7-DMN比、2,6-DMN的选择性及收率分别可达到44%、78%、2.7、49%和17%。
Hierarchical zeolite has advantages of zeolites (high thermal, hydrothermal stability and ordered microposity) and ordered mesoporous materials (large mesopore structure) simultaneity, is a proven strategy to combine shape selectivity with efficient mass transport. These features make it highly desirable in catalysis and adsorption, especially in bulk molecule processes. Its synthesis, characterization and performance in catalytic reaction have gathered a lot of research interests. However, some fundamental questions in hierarchical zeolite synthesis such as the zeolite crystallization and mesopore formation mechanism are still unresolved. Also, recently mesoporous zeolites are generally synthesized based on a nanocasting route with carbon materials as secondary template. This nanocasting route, though very effective, is industrially unfavorable because of its high cost and complex process. Moreover, the structure order in mesopore scale is need further improve. In the doctor thesis, with the recently development in nanotechnology, inorganic synthesis chemistry and zeolite crystallization mechanism, we hope to overcome above motioned question in hierarchical zeolite synthesis, develop cost effective mesoporous zeolite synthesis method, improve the properties of zeolite products and test typical zeolites in model catalytic reaction.
In chapter 1, detailed literature review on hierarchical zeolite synthesis, characterization and catalytic application is given. The detailed experimental methods are given in chapter 2. In chapter 3 with the purpose to understand the influence of carbon template structure on zeolite crystallization, typical carbon materials with difference structure properties was used as template for zeolite synthesis. The final product and materials obtained with different crystallization time were carefully characterized. The results show that the structure of carbon materials has large influence on the zeolite crystallization and the structure of zeolite product can be controlled by varying structure of carbon template. Mesoporous zeolite single crystal can be synthesized with ambient drying carbon aerogel as template without any control on crystallization conditions. The structure of so called mesoporous zeolite single crystal successfully cast the nanostructure of carbon aerogel template. With carbon materials as template, mesoporous aggregate of zeolite nanocrystals is often formed as product or intermediate phase for mesoporous zeolite single crystal synthesis, determining on the structure of carbon template, the structure of zeolite nanocrystals have no obvious relationship with carbon template thus the carbon template is not strictly needed in the synthesis of this type mesoporous zeolite. In chapter 4, we show by changing the structure of carbon aerogel through controlling the catalyst concentration during synthesis, zeolite with tunable intracrystal nanoporsity over larger range (10 nm-100 nm) can be synthesized. A method based on nanocasting concept for test the interconnectivity of mesopore channel in mesoporous zeolite single crystal was developed in this chapter. The result indicate that mesoporous zeolite synthesized with different carbon template have different mesopore interconnectivity. In chapter 5, ordered mesoporous zeolite was synthesized with hard or soft template. It was found that the pore wall of SBA-15 can be recrystallized into ZSM-5 zeolite with in-situ formed carbon material (CMK-5) as template. Zeolite with intracrystal wormhole like mesopore channel can be synthesized with mixture of common cationic surfactant and its silylated analogue as template. Ordered mesoporous zeolite synthesized with both two method have very high thermal and hydrothermal stability, which is stable after treatment in steam at 850℃for 4 h or refluxing in boiling water for 120 h. The formation process of ordered mesoporous zeolite in the two synthesis methods is similar, which is, the formation and dissolve of initial mesopore phase, zeolite nucleation and the formation of ordered mesoporous zeolite. In both synthesis routes, the confine effect of secondary template on zeolite growth is needed and should be controlled in a certain degree. Ordered mesoporous zeolite can only be synthesized when a good match between zeolite growth kinetic and ordered mesopore structure formation is reached. In our synthesis method, ordered mesoporous zeolite can only be synthesized with CMK-5 have moderate thickness or mixture of common cationic surfactant and its silylated analogue as template. In chapter 6, we test the catalytic performance of mesoporous aggregate of zeolite nanocrystals in bulk molecular containing reaction and the possibility to synthesis of mesoporous aggregate of zeolite nanocrystals without secondary template. It was found that mesoporous zeolite aggregate actually show better performance in bulky molecular containing reaction, for instance, catalytic oxidative desulfurization. Hierarchical TS-1 synthesized with CMK-3 as template show improved catalytic performance for thiophene removing compare with common TS-1 and is able to catalytic oxidation remove of large sulfur containing molecular such as DBT. Mesoporous aggregate of ZSM-12 nanocrystals and ZSM-5 nanocrystals was successfully synthesized without secondary through in-situ assembly of zeolite nanocrystals into mesoporous aggregate of zeolite nanocrystals with single crystal like morphology. We further compare the synthesis method and formation process of mesoporous zeolite in different route and found that the hierarchical zeolite generally crystallization through a nanoparticles based aggregation formation mechanism. Stabilize of zeolite nanoparticles with different size and its further assembly leading to the formation of different type of mesoporous zeolite. Hence the hierarchical zeolite is generally kinetically favored product at the given condition. A general crystallization map of hierarchical was given in this chapter. In chapter 7, we test the performance of OMZ-1 in methylation of 2-methylnaphthalene. In 2,6-dimethylnaphthalene synthesis, based on quantum chemical calculation, 2,6-DMN is slightly bulkier and chemical reactivity more favored product than 2,7-DMN. OMZ-1 show better catalytic performance on this reaction than ZSM-5. With Zr/OMZ-1 as catalyst, after 8 h reaction at 400℃, the conversion of 2-methylnaphthalene, selectivity ofβ,β-DMN, ratio of 2,6- and 2,7-DMN and selectivity of 2,6-DMN is 44%, 78%, 2.7,49% and17%, respectively.
不同结构炭材料为模板制备沸石分子筛的研究表明炭材料模板的结构特征对沸石分子筛的晶化过程有着很大的影响,通过控制炭材料的结构可以在很大程度上控制沸石分子筛的晶化过程。采用炭气凝胶为模板时不需要控制晶化条件即可合成含有晶体内介孔的沸石分子筛,所得介孔沸石的孔结构与炭材料模板具有良好的对应关系。在炭材料为模板的条件下更容易生成含无序介孔的纳米沸石团聚体,对比炭材料模板及沸石产物的结构发现某些条件下炭材料模板并没有起到占据孔道造孔的功能,因而在合成这一类沸石材料的过程中,介孔模板可能不是必须的。
采用具有不同初始炭纳米颗粒大小的炭气凝胶可以合成具有可调控介孔结构(尺寸10-100 nm)的介孔沸石。炭材料纳米复制法表征结果表明不同炭气凝胶合成的沸石样品具有不同的介孔连接性。
采用原位生成的CMK-5或常规表面活性剂及硅烷化类似物的混合物为模板可以实现均有序介孔沸石的合成。所得的有序介孔沸石具有很好的水热稳定性,产品经过120小时沸水处理及在水蒸气条件下850℃焙烧4小时后仍能保持所有的结构特征。两种合成路线中有序介孔沸石分子筛的形成均经历了无定形有序介孔二氧化硅的生成、初始二氧化硅相的溶解、沸石的成核及晶化等过程。在合成过程中对沸石的生长进行一定的限制是实现成功合成的关键因素,但限制作用并非越强越好,而需要控制在一个合适的范围,使得沸石分子筛的成核、生长能够与介孔相的生长、保持实现最优的匹配。
具有介孔的纳米沸石团聚体确实在较大分子尺寸化合物的催化反应中体现出比常规沸石分子筛更好的催化性能。采用CMK-3为模板合成的介孔TS-1纳米沸石团聚体在噻吩类含硫模型化合物的催化氧化反应中体现出比常规TS-1更好的催化性能,而且二苯并噻吩比噻吩更容易被氧化脱除。具有介孔的纳米ZSM-12沸石团聚体及ZSM-5团聚体可在没有第二模板存在的条件下通过纳米沸石分子筛的原位自组装成功合成。
多级孔沸石分子筛的合成通常是经历了基于颗粒团聚的沸石生长机理,多级孔道沸石分子筛的形成是沸石的晶化过程在特定的条件下终止而生成的动力学控制产物,而多级孔道的形成并不一定需要介孔形成模板的参与。
在2,6-二甲基萘选择合成的催化反应中,量子化学计算的结果表明目标产物2,6-二甲基萘的分子尺寸要略大于主要的副产物2,7-二甲基萘,但从本征的化学反应性上看2,6-二甲基萘比2,7-二甲基萘更有利于生成。基于这些计算结果,开发了Zr同晶取代的ZSM-5作为这一催化体系的催化剂。基于有序介孔沸石(OMZ-1)的催化剂在2-甲基萘选择甲基化反应中具有比常规ZSM-5更好的催化性能。在反应条件为反应温度为400℃,当2-MN的质量空速为0.5 h~(-1)和2-MN/甲醇/均三甲苯摩尔比为1:1:3时,经过8小时反应,2-甲基萘的转化率、β,β选择性、2,6-/2,7-DMN比、2,6-DMN的选择性及收率分别可达到44%、78%、2.7、49%和17%。
Hierarchical zeolite has advantages of zeolites (high thermal, hydrothermal stability and ordered microposity) and ordered mesoporous materials (large mesopore structure) simultaneity, is a proven strategy to combine shape selectivity with efficient mass transport. These features make it highly desirable in catalysis and adsorption, especially in bulk molecule processes. Its synthesis, characterization and performance in catalytic reaction have gathered a lot of research interests. However, some fundamental questions in hierarchical zeolite synthesis such as the zeolite crystallization and mesopore formation mechanism are still unresolved. Also, recently mesoporous zeolites are generally synthesized based on a nanocasting route with carbon materials as secondary template. This nanocasting route, though very effective, is industrially unfavorable because of its high cost and complex process. Moreover, the structure order in mesopore scale is need further improve. In the doctor thesis, with the recently development in nanotechnology, inorganic synthesis chemistry and zeolite crystallization mechanism, we hope to overcome above motioned question in hierarchical zeolite synthesis, develop cost effective mesoporous zeolite synthesis method, improve the properties of zeolite products and test typical zeolites in model catalytic reaction.
In chapter 1, detailed literature review on hierarchical zeolite synthesis, characterization and catalytic application is given. The detailed experimental methods are given in chapter 2. In chapter 3 with the purpose to understand the influence of carbon template structure on zeolite crystallization, typical carbon materials with difference structure properties was used as template for zeolite synthesis. The final product and materials obtained with different crystallization time were carefully characterized. The results show that the structure of carbon materials has large influence on the zeolite crystallization and the structure of zeolite product can be controlled by varying structure of carbon template. Mesoporous zeolite single crystal can be synthesized with ambient drying carbon aerogel as template without any control on crystallization conditions. The structure of so called mesoporous zeolite single crystal successfully cast the nanostructure of carbon aerogel template. With carbon materials as template, mesoporous aggregate of zeolite nanocrystals is often formed as product or intermediate phase for mesoporous zeolite single crystal synthesis, determining on the structure of carbon template, the structure of zeolite nanocrystals have no obvious relationship with carbon template thus the carbon template is not strictly needed in the synthesis of this type mesoporous zeolite. In chapter 4, we show by changing the structure of carbon aerogel through controlling the catalyst concentration during synthesis, zeolite with tunable intracrystal nanoporsity over larger range (10 nm-100 nm) can be synthesized. A method based on nanocasting concept for test the interconnectivity of mesopore channel in mesoporous zeolite single crystal was developed in this chapter. The result indicate that mesoporous zeolite synthesized with different carbon template have different mesopore interconnectivity. In chapter 5, ordered mesoporous zeolite was synthesized with hard or soft template. It was found that the pore wall of SBA-15 can be recrystallized into ZSM-5 zeolite with in-situ formed carbon material (CMK-5) as template. Zeolite with intracrystal wormhole like mesopore channel can be synthesized with mixture of common cationic surfactant and its silylated analogue as template. Ordered mesoporous zeolite synthesized with both two method have very high thermal and hydrothermal stability, which is stable after treatment in steam at 850℃for 4 h or refluxing in boiling water for 120 h. The formation process of ordered mesoporous zeolite in the two synthesis methods is similar, which is, the formation and dissolve of initial mesopore phase, zeolite nucleation and the formation of ordered mesoporous zeolite. In both synthesis routes, the confine effect of secondary template on zeolite growth is needed and should be controlled in a certain degree. Ordered mesoporous zeolite can only be synthesized when a good match between zeolite growth kinetic and ordered mesopore structure formation is reached. In our synthesis method, ordered mesoporous zeolite can only be synthesized with CMK-5 have moderate thickness or mixture of common cationic surfactant and its silylated analogue as template. In chapter 6, we test the catalytic performance of mesoporous aggregate of zeolite nanocrystals in bulk molecular containing reaction and the possibility to synthesis of mesoporous aggregate of zeolite nanocrystals without secondary template. It was found that mesoporous zeolite aggregate actually show better performance in bulky molecular containing reaction, for instance, catalytic oxidative desulfurization. Hierarchical TS-1 synthesized with CMK-3 as template show improved catalytic performance for thiophene removing compare with common TS-1 and is able to catalytic oxidation remove of large sulfur containing molecular such as DBT. Mesoporous aggregate of ZSM-12 nanocrystals and ZSM-5 nanocrystals was successfully synthesized without secondary through in-situ assembly of zeolite nanocrystals into mesoporous aggregate of zeolite nanocrystals with single crystal like morphology. We further compare the synthesis method and formation process of mesoporous zeolite in different route and found that the hierarchical zeolite generally crystallization through a nanoparticles based aggregation formation mechanism. Stabilize of zeolite nanoparticles with different size and its further assembly leading to the formation of different type of mesoporous zeolite. Hence the hierarchical zeolite is generally kinetically favored product at the given condition. A general crystallization map of hierarchical was given in this chapter. In chapter 7, we test the performance of OMZ-1 in methylation of 2-methylnaphthalene. In 2,6-dimethylnaphthalene synthesis, based on quantum chemical calculation, 2,6-DMN is slightly bulkier and chemical reactivity more favored product than 2,7-DMN. OMZ-1 show better catalytic performance on this reaction than ZSM-5. With Zr/OMZ-1 as catalyst, after 8 h reaction at 400℃, the conversion of 2-methylnaphthalene, selectivity ofβ,β-DMN, ratio of 2,6- and 2,7-DMN and selectivity of 2,6-DMN is 44%, 78%, 2.7,49% and17%, respectively.
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