共查询到20条相似文献,搜索用时 10 毫秒
1.
Dr. Wenwen Zi Xianshu Cai Feng Jiao Prof. Hongbin Du 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(71):17143-17148
Pure silica zeolites possessing uniform micropores, large surface area and high thermal and chemical stability have been widely studied and used in the fields of fine chemicals and oil industry. The incorporation of aluminium into the framework of silica zeolites changes their properties, making them more industrially useful as adsorbents and catalysts. Herein, we report the synthesis and characterization of an extra-large-pore aluminosilicate zeolite NUD-6 with a 16-membered-ring pore channel. Aluminium was directly incorporated into the zeolite NUD-6 framework, as confirmed by 27Al MAS NMR studies and ammonia temperature-programmed desorption probes. Al-NUD-6 was not stable when heated at 550 °C to remove the organic templates. However, the organic templates in Al-NUD-6 could be removed by oxidation in nitric acid at room temperature. The obtained Al-NUD-6H retained the crystalline structure and possessed both micropores and mesopores despite the occurrence of severe structural distortions due to the presence of the corner-sharing Q3 Si2O7 units. The incorporation of aluminium resulted in both medium and strong acid sites in Al-NUD-6H, and could facilitate its use in adsorption and catalysis. 相似文献
2.
Dr. Mariya V. Shamzhy Dr. Pavla Eliašová Dr. Dana Vitvarová Dr. Maksym V. Opanasenko Daniel S. Firth Prof. Russell E. Morris 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(48):17377-17386
Germanosilicate zeolites often suffer from low hydrothermal stability due to the high content of Ge. Herein, we investigated the post‐synthesis introduction of Al accompanied by stabilization of selected germanosilicates by degermanation/alumination treatments. The influence of chemical composition and topology of parent germanosilicate zeolites ( ITH , IWW , and UTL ) on the post‐synthesis incorporation of Al was studied. Alumination of ITH (Si/Ge=2–13) and IWW (Si/Ge=3–7) zeolites resulted in the partial substitution of Ge for Al (up to 80 %), which was enhanced with a decrease of Ge content in the parent zeolite. In contrast, in extra‐large pore zeolite UTL (Si/Ge=4–6) the hydrolysis of the interlayer Ge?O bonds dominated over substitution. The stabilization of zeolite UTL was achieved using a novel two‐step degermanation/alumination procedure by the partial post‐synthesis substitution of Ge for Si followed by alumination. This new method of stabilization and incorporation of strong acid sites may extend the utilization of germanosilicate zeolites, which has been until now been limited. 相似文献
3.
Vicente J. Margarit Marta E. Martínez‐Armero Dr. M. Teresa Navarro Dr. Cristina Martínez Prof. Avelino Corma 《Angewandte Chemie (International ed. in English)》2015,54(46):13724-13728
A two‐dimensional zeolite with the topology of MWW sheets has been obtained by direct synthesis with a combination of two organic structure‐directing agents. The resultant material consists of approximately 70 % single and double layers and displays a well‐structured external surface area of about 300 m2 g?1. The delaminated zeolite prepared by means of this single‐step synthetic route has a high delamination degree, and the structural integrity of the MWW layers is well preserved. The new zeolite material displayed excellent activity, selectivity, and stability when used as a catalyst for the alkylation of benzene with propylene and found to be superior to the catalysts that are currently used for producing cumene. 相似文献
4.
5.
研究了旋转烘箱中无模板剂条件下,预晶化液添加对合成ZSM-5分子筛的影响。系统研究了预晶化液加入量对合成分子筛晶化速率及颗粒大小的影响。采用X射线衍射,扫描电镜,N2吸附-脱附,和激光粒度分布等分析方法对合成的ZSM-5分子筛样品的物化性能进行了表征。结果表明,预晶化液的添加可以明显加快分子筛的晶化速率,预晶化液添加量为33.3wt%时达到最大结晶度的合成时间由未添加时的48 h减少到24 h。添加预晶化液的母液在150℃晶化24 h时所得ZSM-5分子筛团聚体的颗粒大小随着预晶化液加入量的增大而增大,由5.5μm增大到26.3μm。团聚体颗粒的比表面积比未添加预晶化液得到的分子筛(292 m2.g-1)有了不同程度的提高,如添加量为33.3wt%时为394 m2.g-1。对预晶化液添加法合成ZSM-5分子筛团聚体颗粒的生长机理进行了讨论。 相似文献
6.
7.
8.
《化学:亚洲杂志》2017,12(5):530-542
The seed‐assisted synthesis of zeolites without using organic structure‐directing agents (OSDAs) has enabled alternative routes to the simple, environmentally friendly and low‐cost production of industrially important zeolites. In this study, the successful seed‐assisted synthesis of MCM‐22 (MWW‐type) zeolite with an OSDA‐free gel is reported for the first time. MWW‐type zeolites are obtained by the addition of as‐synthesized MCM‐22 seeds prepared with hexamethyleneimine (HMI) into OSDA‐free Na‐aluminosilicate gels. Based on the results of XRD, ICP‐AES, NMR, N2 physisorption and NH3‐TPD, the product exhibited different features compared to those of the seeds. The H‐form product can serve as a catalyst in Friedel–Crafts alkylation reaction of anisole with 1‐phenylethanol, and its catalytic activity is comparable to the seeds. Furthermore, XRD, FE‐SEM, TG‐DTA, CHN, FT‐IR and NMR analyses of products and intermediates provide insights into the role of seeds and occluded HMI, the crystallization process, and key factors for achieving seed‐assisted synthesis of MWW‐type zeolites with an OSDA‐free gel system. The present results provide a new perspective for the economical and environmentally friendly production of MWW‐type zeolites. 相似文献
9.
10.
Dr. Veronika Pashkova Dr. Kinga Mlekodaj Dr. Petr Klein Dr. Libor Brabec Dr. Radek Zouzelka Dr. Jiri Rathousky Dr. Venceslava Tokarova Dr. Jiri Dedecek 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(52):12068-12073
The economical and environmentally benign synthesis of SSZ-13 zeolite was possible due to the mechanochemical activation of dry reagents by planetary mill. Contrary to manual grinding in a mortar, the proposed automatized approach is scalable and reproducible. This solvent-free process provided a huge gain in product/gel ratios, significantly minimized reaction space and organic structure-directing agent use, and allowed for the elimination of agitation. Obtained materials were comparable to the product of “classical” syntheses. The use of different silica sources resulted in SSZ-13 zeolites with various characteristics: different Si/Al ratio and crystal size. 相似文献
11.
Yuki Shinno Dr. Kenta Iyoki Dr. Koji Ohara Yutaka Yanaba Dr. Yusuke Naraki Prof. Dr. Tatsuya Okubo Prof. Dr. Toru Wakihara 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(45):20274-20278
The STW-type zeolite is attractive for developing novel enantioselective syntheses/separation of chiral compounds because it is the only chiral zeolitic microporous material whose enantioenriched synthesis has been achieved. In addition to the conventional industries in which zeolites are used, STW should have diverse industrial applications in the pharmaceutical and food industries. However, the toxic and caustic fluoride required for synthesizing STW severely hinders its commercialization by mass production. Herein, we report the first example of fluoride-free STW synthesis, in which the two roles of fluoride—formation of a zeolitic framework rich in tetravalent T-atoms and promotion of double 4-membered ring unit formation—were substituted by dry gel conversion and Ge addition, respectively. The STW obtained was highly crystalline, with a similar micropore volume and thermal stability as those of original fluoride-based STW. Our approach is promising not only for the fluoride-free synthesis of enantiomeric STW but also for general fluoride-free syntheses. 相似文献
12.
Lijun Gu Ding Ma Prof. Dr. Songdong Yao Xiumei Liu Xiuwen Han Prof. Wenjie Shen Prof. Dr. Xinhe Bao Prof. Dr. 《Chemistry (Weinheim an der Bergstrasse, Germany)》2009,15(48):13449-13455
A facile method has been developed for the fabrication of porous silicon carbide (SiC) by means of sintering a mixture of SiC powder and carbon pellets at a relatively lower temperature, that is, 1450 °C, in air. The pore density and the total pore volume of the resulting porous SiC could be tuned by changing the initial SiC/C weight ratio. The structure evolution and the associated property changes during the preparation were examined through X‐ray diffraction, scanning electron microscopy, thermogravimetric analysis, 29Si magic‐angle spinning (MAS) NMR spectroscopy, and mercury‐intrusion porosimetry analyses. Silica and SiOxCy ceramics formed in situ during the calcination process acted as binders of the porous SiC grains. The porous SiC can be used as a host for the growth of ZSM‐5 zeolite crystals to form the ZSM‐5/porous‐SiC composite material. After loading another catalytic active component of molybdenum, a novel catalytic material, Mo‐ZSM‐5/porous‐SiC, was obtained, which exhibited improved catalytic activity in the methane dehydroaromatization reaction. 相似文献
13.
Prof. Satoshi Inagaki Yasuyuki Tsuboi Yuji Nishita Tuan Syahylah Prof. Toru Wakihara Prof. Yoshihiro Kubota 《Chemistry (Weinheim an der Bergstrasse, Germany)》2013,19(24):7780-7786
An aluminum‐rich MSE‐type zeolite (Si/Al is as small as 7) has been successfully synthesized in a remarkably short crystallization period of only 3 days by the hydrothermal conversion of an FAU‐type zeolite, presumably by the assembly of four‐membered‐ring (4‐R) aluminosilicate oligomers supplied by the double 6‐R (D6R) components of the FAU framework with the aid of the structure‐directing agents and seed crystals. The dealuminated version of the aluminum‐rich MSE‐type zeolite showed a high level of coke durability in addition to a significant yield of propylene, which indicates that this novel zeolitic material is suitable for industrial applications as a highly selective and long‐lived catalyst. 相似文献
14.
Synthesis of Silicate Zeolite Analogues Using Organic Sulfonium Compounds as Structure‐Directing Agents 下载免费PDF全文
Dr. Changbum Jo Sungjune Lee Prof. Sung June Cho Prof. Ryong Ryoo 《Angewandte Chemie (International ed. in English)》2015,54(43):12805-12808
A microporous crystalline silica zeolite of the MEL structure type and three other zeolite analogues composed of germanosilicate frameworks were synthesized using tributylsulfonium, triphenylsulfonium, or tri(para‐tolyl)sulfonium as the structure‐directing agent. The germanosilicates thus obtained had ISV, ITT, or a new zeolite structure depending on the synthesis conditions. The structure of the new germanosilicate was solved using X‐ray powder diffraction data with the aid of a charge‐flipping method. The solution indicated a crystal structure belonging to the P63/mmc space group with cell parameters of a=16.2003 Å and c=21.8579 Å. After calcination, the new germanosilicate material exhibited two types of accessible micropores with diameters of 0.61 and 0.78 nm. 相似文献
15.
16.
以环己胺为模板剂的ZSM-35分子筛的合成及其催化性能 总被引:5,自引:0,他引:5
采用环己胺为有机模板剂成功地合成出ZSM-35分子筛.反应釜的转速对ZSM-35的晶化过程有明显的影响.NH3-TPD结果显示ZSM-35的酸性分布与ZSM-5分子筛类似,但ZSM-35具有强于ZSM-5的酸性中心.酸碱浸泡试验及热分析结果表明ZSM-35具有良好的耐酸碱性和热稳定性.在连续流动的固定床反应装置上,将担载少量镍的ZSM-35分子筛催化剂用于催化裂化汽油的加氢异构化反应,结果表明,Ni/ZSM-35催化剂可降低汽油中的烯烃含量,增加异构烷烃和芳烃的含量,从而提高汽油的质量. 相似文献
17.
本文简要介绍了2005年至今有机合成领域的进展,第一部份有机合成方法学的一些新进展中突出介绍了金属参与的有机合成反应、自由基介导的合成反应、"一个反应瓶"内的多步反应以及不对称反应四个方面;第二部份复杂天然产物全合成则以10个分子的为例介绍这方面的进展。 相似文献
18.
无导向剂直接水热合成小粒径的NaY分子筛 总被引:2,自引:0,他引:2
以铝酸钠和硅溶胶作为主要原料,在没有引入晶种或有机添加剂的情况下,通过控制合成体系的水含量以及水热合成条件(凝胶摩尔组成:5.1 Na2O.Al2O3.10 SiO2.(140~220)H2O,室温陈化1~3 d及100℃晶化9 h),可获得粒径为0.30~0.35μm的小晶粒NaY分子筛.借助于XRD,SEM,XRF和DLS等分析手段对分子筛进行了表征,表明所合成的小晶粒NaY分子筛具有粒度均匀、分散性好的特点.对比了两种不同粒径的La/Y催化剂对1-丁烯脉冲芳构化反应的催化性能和反应过程中催化剂的积炭行为,表明粒径较小的催化剂具有较好的稳定性,其容炭能力和抗积炭能力较强. 相似文献
19.
20.
Hollow aluminosilicate zeolite beta was successfully synthesized by adding CIT‐6, that is, zincosilicate zeolite, which has the same topology as beta, as seeds to the Na‐aluminosilicate gel without the need for organic structure‐directing agents. One important factor in the successful organic structure‐directing agent (OSDA)‐free synthesis of hollow beta crystals is the solubility of the seed crystals in alkaline media. CIT‐6 was less stable than aluminosilicate zeolite beta in alkaline media and the solubility changed depending on whether the crystals were calcined or not. The hollow beta could be obtained by using the uncalcined CIT‐6 seed crystals. The volumes of intra‐crystalline voids were tuned by changing the reaction time and the initial gel compositions, such as the SiO2/Al2O3 and Na2O/SiO2 ratios. We estimated that the intra‐crystalline voids were formed through the dissolution of the seed crystals, just after the crystal growth of new beta on the outer surface of the seeds. In addition, new crystal growth toward inside of the void was also observed by TEM. On the basis of the characterization data, such as chemical analysis, N2‐adsorption/desorption measurements, and TEM observation, a formation mechanism of the intra‐crystalline voids is proposed and discussed. 相似文献