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1.
改变硅源和晶化时间合成了系列SAPO5分子筛.用原位红外光谱和NH3TPD研究了不同样品的酸碱性,用TGDTA和MASNMR考察了硅源及晶化时间对分子筛模板剂的影响,评价了不同样品对正己烷裂解的催化活性.结果表明,SAPO5分子筛孔道不仅与模板剂的胺基有作用,而且与其甲基也有作用.以硅凝胶为硅源时,在48h内,延长晶化时间可使分子筛中硅含量和强酸中心数目增加,低温下正己烷裂解活性提高;晶化72h时,分子筛的酸性减弱,正己烷裂解活性降低.以正硅酸乙酯为硅源时,延长晶化时间可使SAPO5的酸性增强,正己烷裂解性能提高.  相似文献   

2.
SAPO-34分子筛晶化机理的研究   总被引:5,自引:1,他引:5  
采用XRD,SEM,IR和CP/MAS及MASNMR等手段,对快速水热合成SAPO34分子筛的全过程进行了监测,研究了由原始凝胶到SAPO34结晶体过程中固相物质的组成结构随晶化时间的变化规律.结果表明,SAPO34晶核的形成过程既是一个硅氧、磷氧和铝氧四面体由无序排列的胶团到有序排列的晶格骨架的重排过程,同时又是羟基缔合脱水环化的过程.晶化分为晶化前期和晶化后期两个阶段.晶化前期,硅原子直接参与晶核的形成和晶粒的长大过程,生成Si(4Al)结构;晶化后期,少量硅以同时取代一对磷铝原子的方式进入分子筛骨架形成Si(3Al),Si(2Al),Si(1Al),Si(0Al)等多种硅结构.但在整个晶化过程中Si(4Al)结构的生成并不排除硅单独取代磷机理的共同作用.  相似文献   

3.
SAPO-34分子筛晶化过程中硅进入骨架的方式和机理   总被引:5,自引:0,他引:5  
采用 X R D, S E M, I R 和 N M R 等手段考察了 S A P O34 分子 筛的晶化过 程,深入研 究了晶化过程中硅进入 S A P O34 晶格 骨架的方式和机理. 结果表明 ,在 S A P O34 分子筛的整个晶化过程中没有 Al P O34 分 子筛晶相生成. 在 初始 凝 胶的 制备 过 程中, 模板 剂 的添 加和 混 合凝 胶的 老 化处 理对 S A P O34 晶化过程的进行起着关键性的作用. 晶化前 期( < 25 h) , 硅原子直接参与晶核的形成和晶粒的长大过程,形成 Si(4 Al) 结构,此阶段基本上 可以排除硅取代磷机理的作用; 晶化后期( > 25 h) ,少量硅以取代方式进入分子 筛骨架形成 Si( n Al)( n = 0 ~4) 多种硅结构  相似文献   

4.
本文首次在非水体系Na2OSiO2N2O3Fe2O3H2N(CH2)6NH2C2H5)3N中合成了FeZsM48杂原子分子筛。X衍射和扫描电镜测试表明产物具有ZSM48沸石结构。红外光谱和热重差热分析结果表明Fe(II)进入了分子筛骨架,ESR光谱中较强的信号g=4.3有力地证明了分子筛骨架中存在四面体配位的Fe(II)离子。通过对碱度影响的考察发现反应混合物中适当的碱度有利于产物的生成。产物表面富铁富铝。  相似文献   

5.
肖天存  安立敦 《催化学报》1998,19(2):144-148
改变硅源和晶化时间合成了系列SAPO-5分子筛,用原位红外光谱和NH3-TPD研究了不同样品的酸碱性,用TG-DTA和MAS NMR考察了硅源及晶化时间对分子筛模板剂的影响,评价了不同样品对正己烷裂解的催化活性。结果表明,SAPO-5分子筛孔道不仅与模板剂的胺基有作用,而且与其甲基也有作用。以硅凝胶为硅源时,在48h内,延长晶化时间可使分子筛中硅含量和强酸中心数目增加,低温下正己烷裂解活性提高;晶  相似文献   

6.
凝胶中硅含量对SAPO-5分子筛合成及其性能的影响   总被引:3,自引:0,他引:3  
通过改变反应物凝胶中的硅含量,用水热法合成了系列SAPO-5分子筛,并用XRD、SEM和MASNMR分别研究了不同硅含量的分子筛结构和形貌.以正己烷的催化裂解为模型反应,用微反色谱研究了不同硅含量的SAPO-5分子筛的催化性能.结果表明,分子筛骨架中的硅含量随反应物中硅含量的增加而增加;硅开始进入SAPO-5分子筛骨架时,是以取代单个磷原子而进行的;当反应物中硅含量较高时,硅进入分子筛骨架是通过两个硅原子取代一对铝和磷原子,从而在SAPO-5中形成富硅区.硅进入分子筛骨架,虽然未改变分子筛的晶体结构,但改变了分子筛的晶形晶貌.SAPO-5分子筛中存在3种酸中心,即弱酸、中强酸和强酸中心.在正己烷催化裂解中,较低温度时,催化活性中心主要是中强酸中心;当反应温度较高时,弱酸中心也可充当活性中心.在强酸中心上易发生结炭现象.  相似文献   

7.
模板剂种类、浓度、硅源对SAPO-5分子筛结构性质的影响   总被引:6,自引:1,他引:5  
研究了模板剂种类、浓度及硅源等因素对SAPO5分子筛结构、性质及酸催化性能的影响.结果表明,在合成SAPO5分子筛时,较合适的模板剂为三乙基胺或四乙基氢氧化铵.模板剂对分子筛结构的影响在于其空间效应,对酸性的影响在于其对硅反应性能和骨架硅含量的改变.不同硅源对分子筛骨架中的硅含量和酸性有较大的影响.得到较强酸性SAPO5分子筛催化剂的条件是:采用三乙胺模板剂和正硅酸乙酯.  相似文献   

8.
热及水热处理对SAPO-5分子筛结构的影响   总被引:1,自引:0,他引:1  
对合成的SAPO5分子筛进行了高温和水热处理,并用IR,XRD和MASNMR对处理过的分子筛进行了表征.结果表明,短时间的高温焙烧并不破坏分子筛的结构,而使分子筛中的骨架元素P,Al和Si发生重构;长时间的高温焙烧使分子筛的结晶度降低,主要是由于P和Al游离出分子筛的骨架而形成磷酸铝盐.水热处理使分子筛中的Si经历一个转晶和重构过程,在使SAPO5分子筛结构更加完整的同时,未完全结晶的杂质形成了少量的鳞英石颗粒.  相似文献   

9.
在水蒸气气氛中合成沸石分子筛及其特性   总被引:5,自引:0,他引:5  
无定型硅铝凝胶-Na2O-Al2O3-SiO2-H2O在水蒸气相中可以晶化合成出LTA,FAU和MOR沸石晶体。本文重点研究了MOR沸石的晶化条件和物理化学特性。  相似文献   

10.
氟氯有机化合物对HZSM-5分子筛改性过程中氟和氯的作用   总被引:2,自引:0,他引:2  
利用XRD,MAS,NMR,IR和XPS等手段研究了CF4-nCln改性的HZSM-5分子筛的体相和表面结构的变化。结果表明,改性过程中F和Cl均能使HZSM-5脱铝和脱硅。Cl可以使沸石骨架SiO2/Al2O3升高,而F除使沸石骨架脱铝外,还会极化其晶格。F比Cl更容易在沸石表面富集。F和Cl是通过取代O或OH与沸石表面Si或Al作用的。改性后的沸石表面有数种含氟表面物种存在。  相似文献   

11.
In the context of the preparation of camptothecin and luotonin A analogs, the synthesis of some key keto-precursors and their use in Friedländer condensation are described. This paper also focuses on the stability of these keto intermediates and emphasizes the major differences between indolizinones and pyrroloquinazolinones series. Noteworthy is also the report of some original structures isolated as by-products of some experiments.  相似文献   

12.
KMnO4-mediated oxidative CN bond cleavage of tertiary amines producing secondary amine was introduced, which was trapped by electrophiles (acyl chloride and sulfonyl chloride) to form amides and sulfonamides. The reaction could take place at mild condition, tolerating a wide range of function groups and affording products in moderate to excellent yields.  相似文献   

13.
The review contains a concise historical account and information on the most significant researches undertaken by the staff at the A. E. Favorsky Irkutsk Institute of Chemistry, Siberian Branch of the Russian Academy of Sciences on the Chemistry of Heterocyclic Compounds. Dedicated to Academician of the Russian Academy of Sciences B. A. Trofimov on his 70th jubilee. Translated from Khimiya Geterotsiklicheskikh Soedinenii, No. 10, pp. 1443–1502, October, 2008.  相似文献   

14.
Different approaches for the synthesis of 1-benzyloxypyrazin-2(1H)-one derivatives from simple amino acids have been investigated. A library of 33 precursors for the preparation of N-hydroxy pyrazinones was obtained in moderate to good yields.  相似文献   

15.
A new and simple synthesis of novel N-protected methyl 5-substituted-4-hydroxypyrrole-3-carboxylates, which exist in equilibrium with their 4-oxo tautomers, has been developed in two steps starting from N-protected α-amino acids. The key intermediates are enaminones, which can also be isolated, characterized, and used for the construction of other functionalized heterocycles, before they spontaneously decompose to pyrrole products. 4-Hydroxypyrroles are prone to partial aerial oxidation but can be efficiently alkylated or reduced to stable polysubstituted pyrrolidine derivatives.  相似文献   

16.
The chemoselectivity in the intramolecular CH insertion of various diazosulfonamides has been experimentally studied. The results reveal that the aliphatic 1,4-, 1,5-, or 1,6-C(sp3)?H insertions of diazosulfonamides are not accessible, while the aromatic 1,5-C(sp2)?H insertion can be realized specifically by adjusting the diazo-adjacent group. In addition, the general chemoselectivities in the intramolecular CH insertions of diazosulfonyl compounds are summarized. Generally, diazosulfones undergo both aromatic 1,5-C(sp2)?H and aliphatic 1,5- and 1,6-C(sp3)?H insertions, while diazosulfonates undergo aliphatic 1,5- and 1,6-C(sp3)?H insertions. However, diazosulfonamides only undergo aromatic 1,5-C(sp2)?H insertion.  相似文献   

17.
The highly regioselective Buchwald–Hartwig amination at C-2 of the cheap and readily accessible reagent, 2,4-dichloropyridine with a range of anilines and heterocyclic amines is described. This new methodology is robust and provides a facile access to 4-chloro-N-phenylpyridin-2-amines on 0.25 mol scale. These intermediates undergo a further Buchwald–Hartwig amination at higher temperature to enable rapid exploration of the chemical space at C-4 and to provide a library of 2,4-bisaminopyridines.  相似文献   

18.
19.
An efficient approach to the synthesis of highly congested di, penta and hexacyclic pyrazoles as well as imidazole fragment containing novel heterocyclic molecule has been developed through a carbanion induced transformation of suitably functionalized 2H-pyran-2-ones, benzo[h]chromene and thiochromeno[4,3-b]pyrans. Due to the presence of fluorescence, we report their prime application metal sensor as off/on switching in ferric ions.  相似文献   

20.
Quercetin, the polyphenolic compound, which has the highest daily intake, is well known for its protective effects against aging diseases and has received a lot of attention for this reason. Both quercetin 3-O-β-d-glucuronide and quercetin 3′-O-β-d-glucuronide are human metabolites, which, together with their regioisomers, are required for biological as well as physical chemistry studies. We present here a novel synthetic route based on the sequential and selective protections of the hydroxyl functions of quercetin allowing selective glycosylation, followed by TEMPO-mediated oxidation to the glucuronide. This methodology enabled us to synthesize the five O-β-d-glucosides and four O-β-d-glucuronides of quercetin, including the major human metabolite, quercetin 3-O-β-d-glucuronide.  相似文献   

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