共查询到19条相似文献,搜索用时 203 毫秒
1.
利用介孔碳作硬模板合成出具有MFI骨架结构的介孔钛硅材料. 该样品复制了类似SBA-15的介孔结构, 同时骨架含有MFI微孔结构. 透射电镜表征结果表明, 样品表面还有部分大孔结构. 催化结果证明了该样品既具有介孔材料较大孔道结构, 又保持了微孔钛硅材料的高活性. 相似文献
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负载TS-1导向剂的介孔材料的合成、表征及催化性能研究 总被引:1,自引:0,他引:1
利用浸渍法将TS-1导向剂高度分散在介孔材料MCM-41和SBA-15的表面,制备出一系列在氧化反应中具有高活性的催化材料.对样品的表征显示催化剂保持了介孔的结构,同时具有四配位的钛物种均匀地分散于介孔催化剂的表面.催化结果显示,与钛硅分子筛(TS-1)相比,所制备的催化剂在小分子的氧化反应中表现出相似的活性,在大分子的氧化反应中展示了很高的活性,体现了介孔材料的优越性. 相似文献
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由沸石纳米粒子自组装制备具有高催化活性中心和水热稳定的新型介孔分子筛材料 总被引:18,自引:0,他引:18
人们合成了一系列介孔分子筛材料,并发现它们在催化、吸附与分离以及化学组装制备先进材料和分子器件等方面具有很大的潜在应用价值.但是,介孔分子筛材料相对于微孔沸石分子筛存在着两个致命弱点:较低的水热稳定性和较不活泼的催化活性中心.这两个弱点大大地影响了介孔分子筛在催化反应中的广泛应用.本文系统地综述了最近几年利用沸石纳米粒子自组装制备具有高催化活性中心和水热稳定的介孔分子筛材料的研究进展.这包括利用硅铝沸石纳米粒子自组装制备具有强酸性和水热稳定的新型介孔硅铝分子筛材料,利用钛硅沸石纳米粒子自组装制备具有高催化氧化活性中心和水热稳定的新型钛硅介孔分子筛材料,以及利用含有不同杂原子的沸石纳米粒子自组装制备一系列水热稳定的新型介孔分子筛催化材料. 相似文献
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通过对负载型Ti-MCM-41催化材料进行铁离子掺杂, 制备了双掺杂介孔催化剂Fe-Ti-MCM-41. 采用XRD, FTIR, HRTEM, BET和ICP等方法对材料的组成和结构进行了表征, 并研究了金属铁离子掺杂量和后处理温度等对介孔钛硅催化材料氧化催化性能的影响. 当掺杂量较低时, 铁离子主要是通过化学键键合在分子筛上, 呈分子级分散, 得到的催化剂对环辛烯、 环己烯、 苯乙烯和2-甲基苯乙烯等底物都表现出较好的催化活性. 当掺杂量较高时, 金属易形成聚集态, 导致催化剂比表面积下降, 使催化活性降低. 相似文献
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设计制备了一种新型微孔介孔复合核壳结构钛硅分子筛TS-1@Mesosilica(TS-l@Ms),核为MFI结构钛硅分子筛TS-1,壳层为以非离子表面活性剂P123为模板剂组装形成的介孔氧化硅.壳层氧化硅具有三维蠕虫状孔道结构,有利于微孔和介孔部分的连通及反应物和产物的扩散.通过沉积沉淀法将金纳米粒子负载在壳层介孔孔道,和TS-1中的钛活性中心协同,形成适合于C3H6和H2、O2直接气相环氧化制备环氧丙烷(PO)的双功能催化材料.实验结果表明,Au/TS-1@MS在空速8000mLg-h、温度473K条件下连续反应132h,活性和选择性没有明显下降,丙烯转化率保持在3.7%左右,PO选择性87%以上. 相似文献
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Titanium-Containing Mesoporous Materials:Synthesis and Application in Selective Catalytic Oxidation
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Jie Li Chunhui Zhou Huali Xie Zhonghua Ge Liangcai Yuan Xiaonian Li 《天然气化学杂志》2006,15(3):164-177
Titanium-containing mesoporous molecular sieves are of great significance in selective catalytic oxidation processes with bulky molecules. Recent researches and developments on the designing and synthesis of Ti-containing mesoporous materials have been reviewed. Various strategies for the preparation of Ti-containing rnesoporous materials, such as direct synthesis and post-synthesis, are described. Modifications of Ti-containing mesoporous materials by surface-grafting and atom-planting are also discussed. All approaches aimed mainly at the improving of the stability, the hydrophobicity, and mostly the catalytic activity. Structural and mechanistic features of various synthetic systems are discussed. Ti-containing mesoporous materials in liquid phase catalytic oxidation of organic compounds with H2O2 as an oxidant is briefly summarized, showing their broad utilities for green synthesis of fine chemicals by catalytic oxidative reactions. 相似文献
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催化新材料——钛硅分子筛合成及应用研究* 总被引:10,自引:0,他引:10
评述了钛硅分子筛新催化材料的合成及其催化应用的研究进展, 包括钛硅分子筛(TS21) 的水热合成方法、原料、模板剂、影响因素、TS21 同晶取代法合成、表征、活性中心、钛硅分子筛双氧水体系的应用研究及近年中孔钛硅分子筛的进展。对未来的研究提出了建议。 相似文献
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Feng-Shou Xiao 《Catalysis Surveys from Asia》2004,8(3):151-159
Microporous zeolites are widely used commercial catalysts, but their applications are intrinsically limited by their small channel diameters. Recent progress in solving this is used to ordered mesoporous materials such as MCM-41, HMS and SBA-15. These mesoporous materials have pore diameters of 30–60 Å and exhibit catalytic properties for the catalytic conversion of bulky reactants, but unfortunately, when compared with microporous zeolites, the catalytic activity and hydrothermal stability are relatively low, which severely hinders their practical applications. The relatively low catalytic activity and hydrothermal stability can be attributed to the amorphous nature of the mesoporous walls. We review here that the assembly of preformed zeolite precursors with surfactants can synthesize a series of ordered mesoporous materials, which include (1) strongly acidic and hydrothermally stable mesoporous aluminosilicates synthesized in alkaline media; (2) strongly acidic and hydrothermally stable mesoporous aluminosilicates synthesized in strongly acidic media; (3) hydrothermally stable mesoporous titanosilicates with catalytically active titanium species in oxidations; (4) hydrothermally stable mesoporous ferrisilicates. This work would open a door for the industrial application of mesoporous materials as catalysts for large molecules. 相似文献
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ChunHuiZHOU ZhongHuaGE XiaoNianLI HongQiangGUO JianSUN 《中国化学快报》2003,14(12):1285-1288
A mesoporous titanium/silicon -containing montmorillonite-based catalytic materials has been synthesized by novel gallery-templated techniques. XRD, SEM, framework IR, and N2 adsorption-desorption isotherms provided evidence of the formation of Si/Ti pillars. The synthetic materials show potential catalytic application for hydroxylation of phenol with peroxide. 相似文献
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Venkatathri Narayanan 《Reaction Kinetics and Catalysis Letters》2008,93(2):287-293
Two templates namely an inorganic template, CaCO3 and an organic template cetyltrimethylammonium bromide were used to synthesize a nanocrystalline Ti-containing mesoporous
molecular sieve. The results show that the material is mesoporous and titanium is present in tetrahedral and octahedral environment.
Compared to Ti-MCM-41, this catalyst shows higher conversion and selectivity. 相似文献
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By utilizing surfactant aggregates as supramolecular templates, mesoporous and mesostructured silicas with highly ordered structures became available. The resulting mesoporous silicas are promising candidates to host various photo- and electro-active species along with catalytically active species, due to their large and controllable pore sizes, highly ordered pore arrangements with low dimensional geometries, and reactive surfaces. We have developed the rapid solvent evaporation method, which is a modified sol-gel process, for synthesizing the mesostructured silica-surfactant films as well as the mesoporous silica films. Supported thin films, self-standing films and bubbles of mesoporous silicas have been synthesized by the rapid solvent evaporation method. The microstructures of the films have also been successfully controlled by changing the synthetic conditions. Taking advantage of the ease of synthetic operation and the transparency and homogeneity of the resulting materials, we have been interested in the introduction of functional units into the mesostructured materials. This paper reports the synthesis of transparent films of titanium- and aluminum-containing nanoporous silicas to modify the surface properties (such as adsorptive and catalytic) of nanoporous silicas. The incorporation of Al led to the formation of cation exchange or acidic sites on the mesopore surface, as revealed by the cationic dye adsorption experiments. The photocatalytic reactions of the Ti-containing nanoporous silica films were also examined. 相似文献
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C.N. Soekiman K. Miyake Y. Hayashi Y. Zhu M. Ota H. Al-Jabri R. Inoue Y. Hirota Y. Uchida S. Tanaka C.Y. Kong N. Nishiyama 《Materials Today Chemistry》2020
In this study, we have developed a new method to synthesize mesoporous titanium silicalite-1 (TS-1) with a higher content of active titanium in the framework (more than 5%) than that obtained from the conventional hydrothermal synthesis. The new method combines two methods as follows: (1) a sol-gel method in tetrahydrofuran for the synthesis of TiO2–SiO2 composite with highly dispersed Ti species and (2) a dry gel conversion method for the crystallization to TS-1. This investigation revealed that the dispersion of Ti in the starting materials was quite important to synthesize mesoporous TS-1 with high content of Ti besides dry conversion method. The obtained mesoporous TS-1 with a high content of titanium showed higher catalytic activity in 1-hexene epoxidation than conventional TS-1. This high activity is likely to originate from the high content of titanium in the framework. 相似文献
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水热一步法合成Ti-SBA-15分子筛及其催化性能研究 总被引:14,自引:1,他引:14
采用钛酸丁酯和乙酰丙酮作用后的产物作为钛的前驱体,水热法一步合成出了 Ti-SBA-15分子筛。通过X射线衍射、N2气吸附脱附、紫外—可见漫反射等表征手段 ,证明在Si/Ti=50,25,20时,钛原子成功地取代了SBA-15中的硅原子而没有改 变SBA-15高度有序的介孔二维六角结构,其中钛全部以四配位状态存在,而且高度 分散。当Si/Ti=12.5时,钛的分散度降低,部分钛聚集生成二氧化钛。与用两步 法合成的Ti-SBA-15比较,一步法合成的Ti-SBA-15中钛分散度好,添加量高,对催 化氧化环己烯有较高的催化活性。对一步法和两步法合成Ti-SBA-15的机理以及相 应产物在结构以及催化活性上的差异进行了探讨。 相似文献
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Titania sol-pillared clay (TiO(2) PILC) and silica-titania sol-pillared clay (SiO(2)-TiO(2) PILC) were synthesized by the sol-gel method. Supercritical drying (SCD) and treatment with quaternary ammonium surfactants were used to tailor the pore structure of the resulting clay. It was found that SCD approach increased the external surface area of the PILCs dramatically and that treatment with surfactants could be used to tailor pore size because the mesopore formation in the galleries between the clay layers follows the templating mechanism as observed in the synthesis of MCM-41 materials. Highly mesoporous solids were thus obtained. In calcined TiO(2) PILC, ultrafine crystallites in anatase phase, which are active for photocatalytic oxidation of organics, were observed. In SiO(2)-TiO(2) PILCs and their derivatives, titanium was highly dispersed in the matrix of silica and no crystal phase was observed. The highly dispersed titanium sites are good catalytic centers for selective oxidation of organic compounds. Copyright 2001 Academic Press. 相似文献