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1.
低碳烷烃合成芳烃的研究   总被引:2,自引:0,他引:2  
对ZSM-5型高硅沸石进行了锌改性,制备了不同锌含量的Zn/HZSM-5催化剂。以丙烷为原料,在反应温度470~550℃,空速1~7h ̄(-1)条件下反应,并考察了催化剂的稳定性。结果表明,Zn/HZSM-5较HZSM-5在原料转化率变化不大的情况下,芳烃选择性有较大提高,液体产物收率明显增加。氨TPD和吡啶陡吸附红外光谱表明,Zn/HZSM-5较HZSM-5总酸量低,L酸量多,B酸量少。丙烷在线热重分析表明,Zn/HZSM-5积炭初速度较HZSM-5低一半,H_2化学吸附表明,Zn/HZSM-5的吸氢量是0.45mmolH2/gZn,相当于每mg锌可吸附2.71×10 ̄(17)个氢分子。  相似文献   

2.
对ZSM-5型高硅沸石进行了锌改性,制备了不同锌含量的Zn/HZSM-5催化剂。以丙烯为原料,在反应温度470 ̄550℃,空速1 ̄7h^-1条件下反应,并考察了催化剂的稳定性。结果表明,Zn/HZSM-5较HZSM-5在原料转化率变化不大的情况下,芳烃选择性有较大提高,液体产物收率明显增加。氨TPD和吡啶吸附红外光谱表明,Zn/HZSM-5较HZSM-5总酸量低,L酸量多,B酸量少。丙烷在线热重分  相似文献   

3.
采用等量浸渍法制得一系列不同担载量的Mo/HZSM-5催化剂,运用XRD和FTIR方法考察了Mo物种在催化剂表面的分散状态,首次采用微分吸一热技术对Mo/HzSM-5催化剂的表面酸性进行表征。同时研究了催化剂对丙烷芳构化的反应活性。结果表明:对于担载Mo的HZSM-5分子筛催化剂,Mo物种在HZSM-5分子筛表面上顺序为HZSM-5〉1%Mo/HZSM-5〉2%Mo/HZSM-5分子筛本身表面的酸  相似文献   

4.
利用ZSM-5型沸石可将轻烃选择性地转化为苯,甲苯和二甲苯。HZSM-5催化剂上丙烷转化率和芳烃选择性都很低,但在HZSM-5上添加Ga或Pt-Ga(双金属改性)后丙烷转化率和芳烃选择性都有很大提高。实验结果表明,Ga/HZSM-5催化剂经氢气高温预处理后,其上的Bro..nsted酸中心数目减少。铂的加入促进了镓物种的还原,而还原的镓物种可以中和相当一部分催化剂表面Br.nsted酸中心,然后形成高度不饱和的催化活性中心。这些中心可以作为Lewis中心,从丙烷和反应中间产物中拔除H-,使丙烷高选择性地生成芳烃  相似文献   

5.
低碳烃芳构化过程中HZSM—5催化剂结炭规律的研究   总被引:1,自引:0,他引:1  
用GC、TPO-GC、NH3-TPD和TEM等方面,测定了丙烷在HZSM-5沸石上芳构化过程中,催化剂的活性、结炭量、结炭C/H比、酸密度等,考察了催化剂的结炭量与其它参数之间的关系。结果表明,在反应温度为873K,进料空速WHSV=5h^-1时,丙烷在HZSM-5上的结炭首先发生在沸石晶体的外表面的活性中心上;结炭量为1.8-3.4%时,主要在孔道交叉点结炭;结炭量在3.4-5.7%时,孔道已有  相似文献   

6.
Mo系改性HZSM—5分子筛催化剂上丙烷的芳构化反应   总被引:1,自引:1,他引:0  
采用Mo及稀土元素对HZSM-5分子筛进行改性并用于丙烷的芳构化反应。考察了Mo含量、引入方法及反应条件对催化活性的影响。在La、Ce、Nd、Sm、Dy等五种稀土元素中,以La的改性效果最佳,在550℃、600h-1的反应条件下,Mo-LaHZSM-5分子筛催化剂上丙烷转化率及芳烃选择性分别达到8843%、6847%,催化剂活性稳定性也得到提高  相似文献   

7.
Pt-Ga/HZSM-5催化剂上丙烷芳构化   总被引:4,自引:0,他引:4  
考察了Pt/HZSM-5,Ga/HZSM-5和Pt-Ga/HZSM-5上的丙烷芳构化反应,其中Pt-Ga/HZSM-5双组份催化剂上有较高的丙烷反应活性和芳烃选择性,用程序升温还原(TPR)和H2化学吸附法表征催化剂,发现Pt与Ga的协同相互作用促进了Ga^3+的还原,使其峰温向低温移动的70℃,且双组分催化剂中Pt的H2吸附性能大大降低,使催化剂表成乙烯加氢能力降低,从而提高了产物芳烃的选择性,  相似文献   

8.
以乙烯、乙烷为探针反应分子,以混合不同锌含量的ZnO/SiO_2,与HZSM-5为催化剂,在不同处理条件与不同混合方式(直接混合或机械研磨)下研究高温焙烧的俗化剂对乙烯、乙烷芳构化反应的影响。考察了不同含量的Zn/HZSM-5上C_2H_4、C_2H_6的芳构化反应及NaHZSM-5与ZnO/SiO_2和NaZnHZSM-5与ZnO/SiO_2混合催化剂高温焙烧后的C_2H_4芳构化反应。发现Zn/HZSM-5是一种双功能催化剂,乙烯、乙烷芳构化反应的活性和选择性均与Zn/HZSM-5的双中心Zn ̄(2+)和B酸的相互匹配有密切关系,B酸和Zn ̄(2+)存在最合适匹配。而NZSM-5与ZnO/SiO_2合催化剂高温焙烧后具有Zn/HZSM-5的双功能性,HZSM-5与ZnO/SiO_2在高温下发生了固相反应。  相似文献   

9.
根据实验结果,从理论上分析了Al2O3无机膜反应器对HZSM-5,0.4%Ga/HZSM-5和0.5%Pt-0.4%Ga/HZSM-5催化剂上丙烷芳构化反应历程的影响。结果表明,氢气在烷烃活化、环烃形成芳烃和低碳烯烃加氢过程中担当着重要角色,膜反应器通过影响这些步骤,进而影响整个芳构化反应的选择性。  相似文献   

10.
水热处理Zn/HZSM-5催化剂对丙烷芳构化反应的影响   总被引:7,自引:0,他引:7  
解红娟  王军威 《分子催化》2000,14(4):289-293
考察了水热处理对Zn/HZSM-5催化剂丙烷芳构化反应的影响,并采用FT-IR手段,研究了处理温度对催化剂表面酸性的影响,结果表明,随着水热处理温度的升高,单位晶胞中的B酸中心数减少,而上酸中心数增加,丙烷的转化率和芳烃选择性升高,水热处理温度为400℃时达到最大值,此时催化剂的脱氢中心Zn^2+与聚合,环化的B酸中心为最佳匹配状态,随着处理温度的进一步升高、B酸中心数显著下降,丙烷的转化率和芳烃  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.
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   

14.
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   

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.
N-Heterocyclic carbene-palladacyclic complexes 3 were successfully achieved in a one-pot procedure under mild conditions. The structure of 3a was unambiguously confirmed by X-ray single crystal diffraction and it was an active catalyst in the Buchwald-Hartwig amination and α-arylation of ketones even at very low catalyst loadings (0.01?mol%).  相似文献   

20.
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   

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