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1.
镍基催化剂上积碳是甲烷干气重整反应急需解决的关键问题。实验采用TPSR、TPD、XPS和脉冲反应等方法系统研究了镍基催化剂表面积碳的形态和特点。热力学研究表明,在573 K到1273 K的温度范围内,催化剂的表面积碳是不可避免的。TPSR、XPS和TPD研究表明,甲烷在催化剂表面裂解将形成至少三种碳物种:Cα、Cβ和Cγ。这三种碳物种具有不同的表面迁移能力、热稳定性和反应活性。其中,Cα物种在甲烷干气重整反应中是一种非常活泼和重要的中间体;Cγ物种则可能是表面积碳的前驱物:部分脱氢的Cβ物种能够与H2或CO2反应生成CH4或CO。 相似文献
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甲烷/二氧化碳重整反应催化剂的制备及反应性能研究 总被引:10,自引:1,他引:9
采用浸渍法制备载镍CH4/CO2重整反应催化剂,应用ICP,BET,EPMA,SEM,TEM,XPS等手段考察了焙烧温度,浸渍液酸度,助剂等制备条件对催化剂结构及反应性能的影响。结果表明,低温热处理制备的Ni/γ-Al2O3催化剂具有较高的CH4/CO2重整反应活性.经酸或强碱溶液中制备的催化剂尽管活性分布及孔结构等均扔所不同,但二者的反应活性都很高; 相似文献
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报道了用脉冲反应研究Ni/Al2O3催化剂上CH4/CO2重整反应的结果。脉冲反应显示,在还原的Ni/Al2O3催化剂上,CH4在673K就开始发生分解,并有C2H6、C2H4生成,1023K下,CH4几乎完全分解,单纯的CO2则很难在还原的催化剂上发生反应,在973K以上的高温下才会有少量C胜成CO.CHCO2的脉冲反应表明,当CH4在较低温度下开始分解时,CO2也会发生分解,并生成CO。脉冲反 相似文献
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应用FTIR和脉冲反应技术研究了CO_2和O_2在Ag-Ba-Ca-K/α-Al2O3上的吸附及CO2对C2H4环氧化、完全氧化及环氧乙烷(EO)深度氧化反应的影响.研究结果表明,CO2和表面吸附氧在负载银催化剂表面存在竞争吸附,CO2对表面吸附氧有置换作用,该作用降低了银催化剂表面吸附氧的浓度,并且所形成的碳酸根物种改善了乙烯环氧化反应活住氧种的表面分布,对C_2H_4的环氧化反应有一定的抑制作用,但是对C2H4和EO的深度氧化反应的抑制作用更强,使得乙烯环氧化反应的选择性得到改善. 相似文献
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应用FTIR和脉冲反应技术研究了CO2和O2在Ag-Ba-Ca-K/α-Al2O3上的吸附及CO2对C2H4环氧化,完全氧化及环氧乙烷(EO)深度氧化反应的影响。研究结果表明,CO2和表面吸附氧在负载银催化剂表面存在竞争吸附,CO2对表面吸附氧有置换作用,该作用降低了银催化剂表面吸附氧的浓度,并且所形成的碳酸根物种改善了乙烯环氧化反应活性氧种的表面分布,对C2H4的环氧化反应有一定的抑制作用,但是 相似文献
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以乙烯、乙烷为探针反应分子,以混合不同锌含量的ZnO/SiO2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)下研究高温焙烧的催化剂对乙烯、乙烷芳构化反应的影响。考察了不同含量的Zn/HZSM-5上C2H4、C2H6的芳构化反应及NaHZSM-5与ZnO/SiO2和NaZnHZSM-5与ZnO/SiO2混合催化剂高温焙烧后的C2H4芳构化反应。发现Zn/HZSM-5是一种 相似文献
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对具有磁铅石结构的Sr1-xLaxNiAl11O19对甲烷和二氧化碳重整反应的催化活性,积炭量和稳定性进行了研究。不同还原温度下催化剂的XRD和催化剂活性的实验结果表明,金属镍是CH4+CO2重整反应的活性组分,金属镍含量越大,反应活性越高。反应后催化剂积炭量的分析结果说明,在相同镍含量和分散度的情况下,La62+离子对Sr^2+离子调变,可以降低催化剂的表面酸性,提高催化剂的抗积炭能力。 相似文献
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超细镍基催化剂上CH4-CO2重整反应的性能 Ⅱ.制备方法对催化性能及积碳性能的影响 总被引:5,自引:0,他引:5
采用溶胶-凝胶法和超临界干燥(SCD)技术制备了超细二元NiO-Al2O3和三元NiO-La2O3-Al2O3催化剂,并以浸渍超细氧化铝载体和普通氧化铝载体制得的二元和三元催化剂为对比,考察了不同制备方法对催化剂上CH4-CO2重整反应性能的影响。结果表明,超细催化剂表现出很高的高温催化活性、选择性和显著的抗积碳能力,即使不含助剂的超细二元催化剂也明显优于含镧助剂的负载三元催化剂,而含镧的超细三元 相似文献
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Toward new camptothecins. Part 6: Synthesis of crucial ketones and their use in Friedländer reaction
Laurent Gavara Thomas Boisse Jean-Pierre Hénichart Adam Daïch Philippe Gautret 《Tetrahedron》2010,66(38):7544-5571
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
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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
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N. A. Nedolya 《Chemistry of Heterocyclic Compounds》2008,44(10):1165-1219
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
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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
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Rebecca J. Burton Mandy L. CrowtherNeal J. Fazakerley Shaun M. FilleryBarry M. Hayter Jason G. KettleCaroline A. McMillan Paula PerkinsPeter Robins Peter M. SmithEmma J. Williams Gail L. Wrigley 《Tetrahedron letters》2013
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
16.
Uroš Grošelj Mojca Žorž Amalija Golobič Branko Stanovnik Jurij Svete 《Tetrahedron》2013,69(52):11092-11108
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
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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
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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.
Mohammed KajjoutChristian Rolando 《Tetrahedron》2011,67(25):4731-4741
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