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1.
Ni-Cu和MgO-SiO_2间的相互作用及其对催化性能的影响   总被引:2,自引:0,他引:2  
本文用TPR,IR,TPD和TPSR等技术研究了以表面改性法制备的MgO-SiO2(MSO)表面复合物担载的Ni-CU合金间的相互作用及其对CO加氢反应催化性能的影响.结果表明,NiO-CuO与MSO间的相互作用导致部分MO与MSO形成表面物种从而使金属组分氧化物还原温度明显升高;还原后的Ni-Cu/MSO表面上存在着两类活性中心,即合金相中的Ni与载体相中的Mg2+(或Mg2+-O);在两类活性中心的协同作用下,CO吸附除有孪生、线式和桥式吸附态物种外,还有一种新的卧式吸附态(Ni...C=O→Mg2+).这种吸附态的活化程度较高,易在表面上发生裂解形成Ni-C和Mg2+-O,其中Ni-C是加氢反应的碳源;H2在催化剂表面上发生解离吸附形成Ni-H和Mg2+-OH,前者比较活泼,是加氢反应的氢原.CO加氢生成烃类的反应在Ni中心上按"表面碳"机理进行,其生成CZH4的选择性高于80%;H2O的生成反应按2(Mg2+-OH)-→Mg2++(Mg2+-O)+H2O方式进行.  相似文献   

2.
许峥  李玉敏  张继炎  张鎏  何菲 《催化学报》1997,18(5):364-367
考察了碱性助剂K2O,Li2O,MgO,La2O3与CeO2对Ni/γ-Al2O3催化剂上CH4-CO2重整反应活性和抗积炭能力等方面的影响,结果表明,这些助剂对催化剂的抗积炭能力都有明显的改善作用,CH4-CO2重整活性不同温度范围内也有不同程度的提高,其中,MgO,La2O3和CeO2助剂的作用明显,但与添加顺序有关,先浸Ni后浸Mg制备的催化剂有较高的CH4转化率,但抗积炭能力远不如先浸Mg  相似文献   

3.
对镍铜甲烷部分氧化催化剂的制备化学研究表明,在Al2O3、SiO2、MgO、TiO2、Y型分子筛等载体中,具有较好氢溢流功能的Al2O3所担载的镍铜催化剂,有最佳的反应性能,载体的产物溢流功能对反应中合成气的生成是有利的.对于NiO-CuO-Al2O3催化剂,组分Cu的最佳含量是Cu/Al=0.2/4(原子比),Ni/Al(原子比)在1/4-1.5/4范围内催化剂均保持最佳的反应性能,此时,甲烷转化率为98.1%,对CO、H2的选择性分别达97%、100%.制备方法对催化性能影响的结果显示,以(NH4)2CO3为沉淀剂的共沉淀法,是制备NiO-CuO-Al2O3催化剂的最佳方法.NiO-CuO-Al2O3催化剂的甲烷部分氧化性能在400-500℃间有一突跃,并在700℃时达到最佳值;过高的反应气空速对CO、H2的选择性是不利的  相似文献   

4.
载体对镍基催化剂CH4/CO2重整制合成气性能的影响   总被引:10,自引:3,他引:7  
李基涛  陈明旦 《分子催化》1999,13(4):277-281
在Ni/MgO、Ni/CaO和Ni/CeO催化剂上,CH4/CO2重整制事成的活性测试表明MgO是一种较好的载体,TPR实验显示,Ni-MgO之间的相互作用比Ni-CaO和Ni-CeO2强,现场CO岐化和CH4解离实验表明, 经剂表面吸附的氢会促进CO歧化和CH4解离积炭。  相似文献   

5.
用表面反应改性法制备了TiO2-SiO2(TSO)表面复合物载体.采用TPR,IR,TPDMS和TPSR-MS等技术研究了NI-Cu/TSO间的相互作用及其对CO加氢反应的催化性能.结果表明,NiO-CuO与TSO间的相互作用导致CuO的还原温度降低和NiO的还原温度升高,并有少量表面物种生成;还原后的Ni-Cu/TSO催化剂表面上存在着两类活性中心,即合金相中的Ni及载体相中的Tin+(或Tin+-O);CO在催化剂表面存在孪生、线式、桥式和卧式等4种吸附态;H2在催化剂表面上发生解离吸附形成Ni-H和Tin+-H,前者比较活泼,是加氢反应的主要H源;卧式吸附态极易在催化剂表面裂解形成Ni-C和Tin+-O,前者是加氢反应的C源,使CO加氢生成烃类的反应在Ni中心上按"表面碳"机理进行,其生成乙烯的选择性大于60%.H2O的生成反应在Tin+中心上按Tin+-O与Tin+-H或Ni-H反应的途径进行.  相似文献   

6.
助剂对负载型镍催化剂重整活性和抗积炭性能的影响   总被引:3,自引:0,他引:3  
邓存 《燃料化学学报》2000,28(2):124-128
应用XRD和催化活性评价手段,考察了助剂对C2重整制合成气的负勒型Ni催化剂的重整活性和其抗积炭性能的影响。实验结果表明,NiO在γ-Al2O3表面上最大分散量随MgO、La2O3助剂的添加没程度地增大,助剂能影响负载型Ni催化剂 论性能,MgO、La2O3的添加对改善Ni催化剂的重整活性和抗积炭性能有明显效果,并与助剂的种类添加次序有关。  相似文献   

7.
应用溶剂化金属原子浸渍(SMAI)法和普通浸渍(CI)法制备了三种不同摩尔比的γ-Al2O3负载Ni-Ag双金属催化剂。XRD和磁测定结果表明SMAI催化剂中Ni和Ag的粒度均小于金属含量相同的CI催化剂,SMAI催化剂中Ni和Ag未形成合金,而CI催化剂中Ni和Ag形成了合金。SMAI和CI催化剂都具有超顺磁性。XPS测定结果表明SMAI催化剂中零价Ni和Ag的含量均高于CI催化剂。SMAI催化剂Ni在表面含量高于体相,Ni在表面富集,而CI催化剂Ni在表面和体相的含量相同  相似文献   

8.
钟顺和  王杰慧 《催化学报》1995,16(4):257-262
用表面反应改性法制备了TiO2-SiO2(TSO)表面复合物载休,用TPR,IR,TPD-MS和TPSR-MS等技术研究了Ni-Cu/TSO间的相互作用及其对CO加氢反应的催化性能。结果表明,NiO-CuO与TSO间的相互作用导致CuO的还原温度降低和NiO的还原温度升高,并有少量表面物种生成;还原后的Ni-Cu/TSO催化剂表面上存在着两类活性中心,即合金相中的Ni及载体相中的Ti^n+(或Ti  相似文献   

9.
采用表面反应改性法制备了MoO3-SiO2(MoSiO)表面复合物,用等体积浸渍法制备了Mo-SiO担载的Cu-Ni双金属催化剂。利用IR和TPD研究了CO2在催化剂表面上的吸附性能,并讨论了CO2在Cu-Ni/MoSiO上的表面反应机理。结果表明,CO2在上述催化剂上有良好的化学吸附性能,形成线式吸附态、剪式吸附态和卧式吸附态;CO2卧式吸附态具有良好的表面反应活性,在一定温度下可解离为吸附的C  相似文献   

10.
CO_2在Cu-Ni-Mo O_3-SiO_2催化剂上的吸附与反应   总被引:3,自引:3,他引:0  
采用表面反应改性法制备了MoO3-SiO2(MoSiO)表面复合物,用等体积浸渍法制备了MoSiO担载的Cu-Ni双金属催化剂。利用IR和TPD研究了CO2在催化剂表面上的吸附性能,并讨论了CO2在Cu-NiMoSiO上的表面反应机理。结果表明,CO2在上述催化剂上有良好的化学吸附性能,形成线式吸附态、剪式吸附态和卧式吸附态;CO2卧式吸附态具有良好的表面反应活性,在一定温度下可解离为吸附的CO和O。这种新生态O具有良好的选择氧化性能  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.
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.
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   

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