共查询到20条相似文献,搜索用时 0 毫秒
1.
Highly active, hierarchical zeolite ZSM-5 aggregates have been prepared in a one-step synthesis using alkanolamine as single template. The effects of SiO2/Al2O3, pH and H2O/SiO2 on the aggregate morphology of the ZSM-5 nanocrystals were investigated. The obtained aggregate zeolites characterized by SEM, TEM and BET possessed significant textual porosity (up to 0.22 cm3/g), which could be tuned by the number of substituents in the alkanolamine molecules and the amount of aluminum in the synthetic mixtures. These zeolite aggregates showed high activities for Friedel–Crafts alkylations and may curtail the filtration difficulties during the synthesis and applications to some extent. 相似文献
2.
Lifeng Wang Chengyang Yin Zhichao Shan Sen Liu Yunchen Du Feng-Shou Xiao 《Colloids and surfaces. A, Physicochemical and engineering aspects》2009,340(1-3):126-130
A hierarchical mesoporous ZSM-5 zeolite has been synthesized by using starch-derived bread as a meso-template. The obtained mesoporous ZSM-5 was characterized with X-ray diffraction (XRD), nitrogen sorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM) and thermogravimetric (TG)/differential thermal analysis (DTA) techniques. Hydrothermal treatments revealed that the mesoporosity in hierarchical mesoporous ZSM-5 exhibited excellent hydrothermal stability. Catalytic tests showed that hierarchical mesoporous ZSM-5 was more active than conventional zeolite of ZSM-5 in catalytic cracking of 1,3,5-tri-isopropylbenzene. Hydrogen adsorption measurements showed hierarchical mesoporous ZSM-5 had a higher storage capacity than the conventional ZSM-5. 相似文献
3.
以碳黑为第二模板剂在氟离子体系中一步水热合成了多级结构MCM-22分子筛组装体(简称为MCM-22-FC)。考察了碳黑和氟离子对MCM-22分子筛形貌和催化性能的影响。MCM-22-FC分子筛是由大量片状晶体交错生长形成的组装体结构,其中MCM-22的片层结构更薄,在其固有的微孔中存在的晶间孔呈现大孔和介孔的特征。MCM-22-FC负载Mo后得到的Mo/MCM-22-FC催化剂在甲烷无氧芳构化反应(MDA)中提高了苯收率和芳烃选择性,并且提高了催化剂的寿命。通过氨气程序升温脱附(NH3-TPD)表征,吡啶红外(Py-IR)表征,结合热重(TG)分析,得出的结论是Mo/MCM-22-FC在MDA中优越的催化性能是由于氟离子进入到分子筛骨架当中,形成具有拉电子效应的结构单元,从而提高了分子筛的Brönsted酸量,较多的Brönsted酸性位将更多的Mo物种迁移至分子筛孔道内部,形成更多的MoCx或MoOxCy活性物种以及更有利于大分子产物扩散的MCM-22薄片层的结构。少量过剩的Brönsted酸性位在成型后保留在Mo/HMCM-22-FC催化剂活性中心抑制了积碳的形成,也有助于改善芳烃的选择性。 相似文献
4.
In this paper,we present a simple method by combining surface wrinkling and template replication to create a series of hierarchical structures on polydimethylsiloxane(PDMS) elastomer.The primary stable lined patterns are formed by duplicating commercialized compact disk and digital versatile disk with PDMS.The secondary microscale patterns are from surface wrinkling,which is elicited by oxygen plasma(OP) treatment of the prestrained PDMS stamp followed with the prestrain release.By systematically varying the OP exposure duration,the prestrain,and the angle(θ) between the primary pattern orientation and the prestrain direction,we obtain highly ordered well-organized composite patterns from different patterning techniques and with different length scales and mechanical stabilities. 相似文献
5.
清液体系中T型分子筛膜的高重复性合成与渗透汽化性能 总被引:1,自引:0,他引:1
以自制微米级分子筛为晶种,在清液体系中成功合成出高性能的T型分子筛膜,考察了硅铝比、水硅比、碱度及合成温度与时间等条件对膜的生长和渗透汽化性能的影响.结果表明,在摩尔组成为1SiO2:0.015Al2O3:0.41(Na2O+K2O):30H2O的清液体系中,于423K晶化6h的条件下可较快地形成一层厚度为5μm的连续致密纯相T型分子筛膜,较大缩短了膜合成时间且提高了膜致密性.在优化条件下所合成的膜具有优良的分离性能和高重复性.348K时,在10wt%水-90wt%异丙醇混合物体系中膜的渗透通量和分离因子分别高达4.20kg/(m2·h)和7800. 相似文献
6.
In an attempt to convert the carcinogenic benzene which is almost restricted for its use in gasoline, alkylation reaction with olefin 1-hexene has been conducted on various zeolites. Four zeolites having different pore topology and pore size have been applied as solid acid catalysts for effective production of alkylate in a liquid phase, solvent-less low temperature reaction. The textural properties of all the four zeolites (ZSM-5, MOR, BEA, HY) have been characterized for crystal morphology by TEM, crystal structure by XRD and FTIR, BET for surface area, N2 sorption for porosity and TPD for acidity. Among the zeolite, BEA possessed high surface area (600.61 m2/g) and enhanced meso pores volume (0.3956 cm3/g) as compared to other zeolite samples. The performance of BEA was also observed to be superior in the liquid phase alkylation of benzene with 1-hexene in a batch reactor under autogenous pressure without using any solvent. At the optimum reaction conditions, the benzene conversion was 86.6 wt% and 3-Phenylhexane, 2-Phenylhexane yield were about 47.9 wt% and 38.7 wt% respectively on this catalyst. The BEA also exhibited longer time-on-stream and reusability performance, thus offers an attractive route for converting benzene into valuable (3-Phenylhexane, 2-Phenylhexane) alkylate product useful for the manufacturing of fine chemicals, dyestuff, detergents and scents. 相似文献
7.
β沸石中堆垛层错结构的研究 总被引:4,自引:0,他引:4
含TEA+离子的化合物作为模板剂会成的β沸石是由有序结构A、B、C到沿[001]方向堆积成堆垛层错结构.三种有序结构出现的几率分别为0.31、0.36和0.33;其数值不受样品中硅铝出的影响.几率值如此相近的原因是构成β沸石的结构单元Ⅰ的四种连接方式(见图2)能量相等.几率值之间的微小差别,是基于在晶体生长过程中支撑赶A、B和C型三维通道结构的TEA+离子以不同排列形成的难易程度不同所引起.B型对应的排列略易于C型、C型又略易于A型,因此使用此种模板剂时,A、B、C三种结构均可能出现,只能合成出具有堆垛层错结构的β沸石.由于三维通道的特点,合成β沸石对模板剂的用量必须大于具有二维通道或一维通道的分子筛合成时的用量.而且要求有机控离子不宜过大、反应温度相对较低、晶化时间相对较长,以利于有机按高子不同取向排列的形成 相似文献
8.
Pei Chen Xinbing Chen Xiangshu Chen Hidetoshi Kita 《Journal of membrane science》2009,330(1-2):369-378
The preparation of the supported titanium silicalite-1 (TS-1) zeolite membrane with inexpensive tetrapropylammonium bromide (TPABr)/weak base synthesis system was studied by three methods, and the catalytic activity of the obtained TS-1 zeolite membrane was evaluated with the oxidation of 2-propanol (IPA) under pervaporation condition. It was found that TS-1 zeolite membrane could be successfully prepared with “seeding” or “seeding in situ” method, but could not be achieved with “in situ” method. Adding a little amount of promoter ions of PO43− into the synthesis gel was of benefit to the catalytic activity of the prepared TS-1 zeolite membrane, but had no obvious effect on the membrane layer formation on the mullite porous support. For “seeding” method, the membrane prepared with the synthesis gel having molar composition of SiO2:0.1TPABr:0.9Et2NH:0.03TiO2:80H2O:0.06H3PO4 at 150 °C for 48 h showed the highest oxidation conversion of IPA of 72% accompanied by a flux of 0.35 kg/m2 h. Further more, much higher IPA oxidation conversion of 76% accompanied by a flux of 0.65 kg/m2 h was obtained for the TS-1 zeolite membrane prepared with the same synthesis gel by “seeding in situ” method at 150 °C for 72 h. 相似文献
9.
模板剂在沸石合成过程中的作用机理研究 总被引:5,自引:0,他引:5
通过分子模拟途径,对有机模板剂分子与沸石骨架间非成键互作用的能学分析 ,论证不同链长的双季铵盐[(CH3)3N(CH2)nN(CH3)3]2Br-在四种沸石(ZSM-50、ZSM-12、NU-87[HTK]和ZSM-23)合成中所起的模板作用。认为这种模板作用可用非成键互作用能定量表达;在一定程度上解释了Moini等人固定胶凝条件、实验考察以双季铵盐系列作为模板剂的合成结果。 相似文献
10.
In this paper, the precise construction on the structure of silicalite-1 microcapsules (S1) was specifically described. The interior carbon modifications and the outside mesoporous functionalizations were successfully conducted and each sample was characterized in detail. It was found that the carbon networks could be formed inside the zeolite microcapsules via the pretreatment of sugar injections. The uniformity of the distinct microcapsule could be regulated by adjusting the sugar concentrations. With the encapsulated Pt species inside the MSSs, the nano-particles could be dispersed well within the carbon network. On the other hand, during the fabrication of the mesoporous materials outside the microcapsules, the template and the acidity of the system could play an important role in determining the morphology of S1. Besides, the PDDA modification on the shell of S1 could help the combination of the meso-layer and the shell of S1 at nano-scale. The thickness of the outside mesopore could be modulated through the controlling of the silica content. 相似文献
11.
12.
Rui Ma Rongming Ma Lingling Feng Liren Fan Yan Liu Bin Xing Yubang Hou Feng Bao 《Colloids and surfaces. A, Physicochemical and engineering aspects》2009,346(1-3):184-194
A series of block copolymers of styrene, maleic anhydride and acrylic acid were synthesized by the reverse addition–fragmentation chain transfer (RAFT) process. The structure, molecular weight and polydispersity index were determined by FTIR, 1H NMR, SEC&MALLS and DSC analysis. The results showed that the polymerization occurred in a living and controlled manner. Multiple self-assembled nanostructures of these block copolymers were investigated by transmission electron microscopy (TEM). Tetrahydrofuran (THF), N,N-dimethylformamide (DMF) and 1,4-dioxane were used as the common solvents and twice-distilled water as the selective solvent to clarify the effects of the solvent. The results revealed that with the increase of the extension degree of the core, non-spherical aggregates were easily formed, the composition of the copolymers influences the aggregation behavior, and other factors also influence the self-assembly, such as hydrolysis, temperature, annealing time, molecular architecture etc. A mechanism is proposed to illustrate the formation of the various aggregates of P(MAn-co-St)-b-PS-b-P(MAn-co-St) copolymer, which were confirmed by TEM results. 相似文献
13.
The successful application of zeolite A membranes in the industrial market has thus far been restricted to the pervaporative dehydration of solvent streams in the pharmaceutical and engineering industries. Their application in gas separation processes remains elusive, largely due to the existence of uncontrollable, intercrystalline diffusion pathways in the boundary regions of neighbouring crystals. 相似文献
14.
《Journal of Molecular Structure》2001,540(1-3):145-152
Unimolecular 1,2-methyl shift reaction and disproportionation of para-xylene is investigated by means of ab initio quantum chemical calculations. Isolated gas-phase models are used to estimate the optimum volume of the reaction complex. Space filling of the computed models is examined in zeolite Y, Beta and ZSM-5. It is suggested that the shape selectivity effect of zeolite molecular sieves on the disporportionation reaction can be associated with the steric conditions of the intrinsic rearrangement of the reaction complex in the course of the chemical transformation. 相似文献
15.
Miros?aw M?czka Maciej Ptak Leszek K?piński Jerzy Hanuza 《Journal of solid state chemistry》2011,184(9):2446-2457
Highly hierarchical barlike and flowerlike MnWO4 microcrystals have been synthesized for the first time by a hydrothermal method, where ethanolamine (EA) and cetyltrimethylamonnium bromide (CTAB) play important roles in directing growth and self-assembly of these structures. The possible formation process has been proposed. In addition, platelike nanosized MnWO4 was also synthesized by annealing of a precursor obtained by coprecipitation method. The obtained samples were characterized by XRD, SEM, TEM, Raman and IR methods. Raman spectra showed relatively weak dependence on particle size and morphology of the particles. In contrast to this behavior, IR-active bands showed pronounced shifts and changes in relative intensities on particle size and the morphology. Origin of this behavior is discussed. 相似文献
16.
Chuanqiang Zhou 《European Polymer Journal》2008,44(9):2850-2858
Nanosheet- or nanorod-based microspheres and nanorod-based microrods of polyaniline (PANI) with hierarchical structures were successfully prepared by oxidation polymerization of aniline in alkaline solution. Temperature was found to have important influence on the morphology of PANI hierarchical structures and their building blocks. The concentration of alkali (NaOH) could be used to guide the morphological evolution of PANI, from leaf-like structures to nanosheet-based particles, and to nanorod-based microspheres and nanorod-based microrods with increasing concentration of NaOH in synthesis. The chemical structures of product were characterized by FTIR, UV-vis spectra and XRD, and its solubility was also studied in this report. 相似文献
17.
Oil shale from the Kark region of Pakistan has been pyrolysed in a fixed bed batch reactor and the properties of the derived shale oil determined. The reactor system was then modified to incorporate a second reactor where the derived vapours from oil shale pyrolysis were passed directly to the second reactor containing zeolite ZSM-5 catalyst. The influence of the process parameters of vapour residence time (VRT) over the catalyst and the regeneration of the catalyst were examined. The yield and composition of the derived gases before and after catalysis were determined. In addition, the yield and composition of the derived oil in terms of total nitrogen and sulphur content and the content of aromatic hydrocarbons in the oils was investigated. The results showed that the yield of oil after catalysis was reduced with a consequent higher yield of gases and formation of coke on the catalyst. The main gases from the pyrolysis of oil shales were CO2, CO, H2, CH4, C2H4, C2H6 and C3H6, C3H8 and minor concentrations of other hydrocarbon gases. The main role of catalysis was to convert the long chain alkanes and alkenes in the oil to lower molecular weight, short chain, alkyl substituted and iso species and high concentrations of aromatic hydrocarbons. Total nitrogen and sulphur contents in the oils were markedly reduced after catalysis. This reduction was reflected in the reduced concentration of nitrogen and sulphur containing aromatic hydrocarbons. The influence of longer VRTs was to increase the formation of aromatic hydrocarbons, reduce the nitrogen, and sulphur compounds in the oils. The influence of catalyst regeneration, involving five regenerations was not significant on the yield and composition of the derived catalytically upgraded oils. 相似文献
18.
Ya-Jie Liu Hai-Feng Su Yi-Fan Sun San-Tai Wang Cheng-Yang Zhang Prof. Wei-Hui Fang Prof. Jian Zhang 《Angewandte Chemie (International ed. in English)》2023,62(49):e202309971
Clusters that can be experimentally precisely characterized and theoretically accurately calculated are essential to understanding the relationship between material structure and function. Here, we propose the concept of “supraclusters”, which aim to connect “supramolecules” and “suprananoparticles” as well as reveal the unique assembly behavior of “supraclusters” with nanoparticle size at the molecular level. The implementation of supraclusters is full of challenges due to the difficulty in satisfying the ordered connectivity of clusters due to their abundant and dispersed hydrogen bonding sites. By solvothermal synthesis under a high catechol (H2CATs) content, we successfully isolated a series of triangular {Al6M3} cluster compounds possessing brucite-like structural features. Interestingly, eight {Al6M3} clusters form 72-fold strong hydrogen bonding truncatedhexahedron Archimedean {Al6M3}8 supracluster cage (abbreviated as H-tcu ). Surprisingly, the solution stability of the H-tcu was further proved by electrospray ionization mass spectrometry (ESI-MS) characterization. Therefore, it is not difficult to explain the reason for assembly of H-tcu into edge-directed and vertex-directed isomers. These porous supraclusters can be obtained by scale-up synthesis and exhibit a noticeable catalysis effect towards the condensation of acetone and p-nitrobenzaldehyde. As an intermediate state of supramolecule and suprananoparticle, the supracluster assembly can enrich the cluster chemistry and bring new structural types. 相似文献
19.
钙黄绿素-藏红T与DNA作用机理的光谱研究 总被引:2,自引:0,他引:2
应用能量转移方法和光谱技术,研究了钙黄绿素-藏红T荧光能量转移体系与ctDNA的作用机理以及抑制作用的影响因素.在pH8.0和低离子强度条件下,ctDNA与Caleein-ST发生了静电电荷作用,降低了钙黄绿素-藏红T荧光体系的能量转移效率,对荧光体系的能量转移产生了明显的抑制作用. 相似文献
20.
The density functional theory and Hartree–Fock methods were used to investigate the proton transfer reaction for a series of model clusters of zeolite/(H2O)n; n=1,2,3, and 4. Without promoted water, the hydrogen-bonded dimer of the water/zeolite system exists as a simple hydrogen-bonded complex, ZOH.(H2O)2, and no proton transfer occurs from zeolite to water. The third promoted water, ZOH(H2O)2H2O, was found to induce a pathway for proton transfer, but at least addition two promoted molecules, ZO(H3O+)H2O(H2O)2, must be involved for complete proton transfer from zeolite to H2O. The results show that the hydronium ion in water cluster adsorbed on zeolite, ZO(H3O+)(H2O)3, can considerably affect the structure and bonding of the hydrogen-bonded dimer of water. The OO distance is contracted from 2.818 Å found in the neutral complex, ZOH(H2O)4, to 2.777 Å for ion-pair complex, ZO(H3O+)(H2O)3. The distance between the oxygen of the hydronium ion and the zeolitic acid site oxygen is predicted to be 2.480 Å which is in good agreement with the experimentally observed value of 2.510 Å. The corresponding density functional adsorption energy of the high coverages of adsorbing molecules on zeolite is calculated to be −9.14 kcal/mol per molecule at B3LYP/6-311+G(d,p) level of theory and compares well with the experimental observation of −8.20 kcal/mol. 相似文献