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1.
铜、锰氧化物的表面过剩氧及其甲苯催化燃烧活性   总被引:9,自引:0,他引:9  
研究了负载型Cu-Mn-O催化剂对烃类深度氧化的活性,并将XRD分析、电子探针考察和表面过剩氧浓度的分布测定等结果与催化剂活性进行了关联.以甲苯催化燃烧为模型反应,除用常规的微反考察其动力学性质外,还用脉冲反应技术研究了表面过剩氧的氧化功能和甲苯的吸附等.Mn/Cu原子比为0.88~0.9时,催化剂活性最好.这是由CuO和CuMn2O4的功能匹配决定的,后者提供与催化作用有关的表面过剩氧,前者促进甲苯的吸附.对催化剂的作用机理也进行了初步的探讨.  相似文献   

2.
铜,锰氧化物的表面过剩氧及其甲苯催化燃烧活性   总被引:6,自引:0,他引:6  
王幸宜  卢冠忠 《催化学报》1994,15(2):103-108
研究了负载型Cu-Mn-O催化剂对烃类深度氧化的活性,并将XRD分析、电子探针考察和表面过剩氧浓度的分布测定等结果与催化剂活性进行了关联。以甲苯催化燃烧为模型反应,除用常规的微反考察其动力学性质外,还用脉冲反应技术研究了表面过剩氧的氧化功能和甲苯的吸附等。Mn/Cu原子比为0.88~0.9时,催化剂活性最好。这是由CuO和CuMn2O4的功能匹配决定的,后者提供与催化作用有关的表面过剩氧,前者促进  相似文献   

3.
对硅胶负载钒磷氧化物(VPO) 催化剂( n(V)/ n(P) = 1) 催化2 ,6二氯甲苯(DCT) 氨氧化反应进行了研究. 考察了反应温度、空气/DCT 比和氨/DCT 比等因素对反应的影响. 反应温度对氨氧化反应影响较大,空气/DCT比和氨/DCT 比对反应的影响不很大. 最佳反应条件为: T= 673 K, n(air)/n(DCT) = 30 , n(NH3)/n(DCT)= 6 . 在此条件下,DCT转化率为90 % , 产率为57 % . 与使用(NH4)2[(VO)3(P2O7)2] 催化剂的文献报道值相比,反应温度降低40 K, 产率提高34 % .XRD分析结果表明, VPO/SiO2 催化剂中的活性组分以均匀分散的无定形状态存在,而未负载的VPO催化剂中存在αVOPO4 和βVOPO4 晶相.  相似文献   

4.
Pt/NM,Pd/NM催化剂上甲苯深度氧化反应动力学   总被引:4,自引:0,他引:4  
在氧气过量的条件下,考察了Pt/NM、Pd/NM催化剂上甲苯深度氧化反应动力学及反应活性。Pt/NM催化剂对甲苯的氢化活性高于Pd/NM,深度氧化反应服从反应物强吸附双分子反应Ltangmuir-Hinshelwood机理,其动力学方程为:相应的动力学参数,Pt/NM为:活化能△E=49.9kJ/mol,吸附热Q=-29.6kJ/mol;Pd/NM为:△E=94.2kJ/mol,Q=-19.1kJ/mol.  相似文献   

5.
采用固定床流动反应装置、CO吸附、TG、TPO、XPS和XRD等手段考察了NiO/Al2O3和LiNiLaO/Al2O3催化剂上的甲烷部分氧化反应。实验结果表明,LiNiLaO/Al2O3对甲烷部分氧化反应具有较高的反应活性。锂和镧的添加不仅改善了活性组分镍的分散度,而且提高了NiO/Al2O3的抗积碳能力和热稳定性  相似文献   

6.
采用脉冲色谱技术、XRD、TPR和XPS等方法研究了在天然气二氧化碳转化制合成气反应中催化剂的抗积炭性能。实验结果表明,在N Al2O3催化剂中添加CeO2和MgO助剂(催化剂记为Ni/ARM)能有效抑制甲烷脱氢反应,提高二氧化碳消炭能力,增加催化剂的抗积炭性能。其主要原因是,添加CeO2和MgO助剂增加了活性组分镍的分散度,加强了活性组分和载体的相互作用。改性后的Ni/ARM催化剂在1023K、二氧化碳/天然气/氧气比为2.4/0.1以及1123K、二氧化碳/天然气/氧气比为1.4/1/0.05的条件下反应800小时后活性不降低,产物中合成气(CO+H2)摩尔百分含量始终保持在94-96%左右。说明该催化剂具有较高的活性、选择性和抗积炭性。  相似文献   

7.
水相中金属铜表面生成亚铜—邻菲罗啉配合物的反应   总被引:1,自引:0,他引:1  
本文研究了零价铜在邻菲罗啉水溶液中的反应。当溶液敞露于空气并存在有机阴离子X-时,例如苯甲酸盐(Bz)、对甲基苯磺酸盐(Ts)等,铜的表面生成了致密的反应产物的薄层,经IR、UV/VIS、MS和元素分析证明了该薄层为相当纯的亚铜的邻菲罗啉配位化合物,结构为[Cu(phen)2]+X-。在乙醇/甲苯混合溶剂中得到了表面反应产物的晶体[Cu(phen)2](CH3C4H6SO3)C2H5OH,并用X-ray测得了结构。本工作表明溶液中的CuⅡ离子抑制Cu0氧化成CuⅠ而影响反应层的形成,同时又促进CuⅠ氧化成CuⅡ的过程  相似文献   

8.
研究了稀土金属氧化物(La2O3,CeO2,Pr6O11和Nd2O3)对Ni/α-Al2O3催化剂上甲烷部分氧化制合成气反应的影响.X光粉末衍射和活性考察结果表明,稀土氧化物使Ni/α-Al2O3催化剂的稳定性有显著提高.稀土氧化物与活性组份Ni之间的相互作用抑制了催化剂表面Ni晶粒的生长和迁移,由于这种作用也抑制了催化剂表面积炭的生成.在实验中还发现CeO2容易进行Ce3+Ce4+氧化还原反应而对反应具有催化活性.  相似文献   

9.
制备了一系列负载型V-Ti-Al-O催化剂并用于甲苯的气相选择性氧化制苯甲醛,考察了接触时间、氧浓度、V2O5负载量以及催化剂焙烧温度对反应性能的影响。用TPR、XRD和BET等测试手段,对催化剂进行了表征。研究发现,催化剂在773K时活化,接触时间1.2秒,氧浓度21%时,可获得较好的反应结果,V2O5负载量为6(wt)%的催化剂,在593K时反应,得到了转化率20.5%,苯甲醛产率8.3%的最好结果。  相似文献   

10.
黄驰  郑穹 《分子催化》1999,13(6):467-470
研究P/V=1的SiO2负载钒磷氧化物催化剂催化2,4-二氯甲苯氨氧化反应,考察了反应温度,氨气比,空气比和空间速度等工艺条件的影响,在673K,二氯甲苯:氨气:空气:7:15,空间速度250h^-1的条件下,2,4-二氯甲苯的转化率为97%,2,4-二氯苯腈的摩尔产率为70.2%,远高于文献所报道的使用未负载VPO催化剂的结果,且反应温度降低40K。  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.
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   

19.
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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