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微波场中甲烷部分氧化制合成气 Ⅱ.Co/ZrO_2催化剂在微波场中的升温行为及催化活性 总被引:4,自引:0,他引:4
近年来,甲烷部分氧化制合成气(POM)的研究一直十分活跃[1,2].前文报道了用于甲烷部分氧化制合成气的镍基催化剂(Ni/La2O3)在微波场中的升温行为和催化活性[3],发现在达到相同的CH4转化率时,微波活化方式下的催化剂床层温度比常规加热低得多... 相似文献
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近年来,对甲烷部分氧化制合成气(POM)的研究,一直十分活跃[1~8].该反应常用的催化剂是负载型贵金属(Rh)和过渡金属(Ni和Co).由于贵金属的价格昂贵,因而Ni和Co受到人们的极大重视,但Ni和Co在反应温度较高时,易发生催化剂的挥发流失和烧... 相似文献
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在甲烷氧化偶联制C2烃的研究中,人们发现碱土金属与稀土金属组成的复合氧化物催化剂具有高的催化活性[1,2].稀土化合物作为有希望的工业催化剂之一,已受到广泛的关注.一般认为,它们含有的氧空位对活化甲烷的有效氧物种有利.Debey等在1%Sr/La2O... 相似文献
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Ni/Al2O3催化剂上甲烷部分氧化制合成气 总被引:19,自引:2,他引:19
研究了Ni/Al2O3催化剂对甲烷部分氧化制合成气的反应性能.结果表明,催化剂在其活性组份Ni为10%时反应性能最好.条件实验表明,在600~900℃范围内,甲烷转化率和CO、H2的选择性随温度升高而增加;转化率和选择性在甲烷空速≤1.5×105h-1时基本不变,空速>1.5×105h-1时,转化率和选择性有所下降.随着压力的增加(0.05~0.40MPa),转化率和选择性下降.SEM和化学分析结果证明在反应过程中,Ni组份存在烧结和流失现象. 相似文献
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Rh/SiO2催化剂上甲烷部分氧化制合成气反应 总被引:4,自引:0,他引:4
利用程序升温脱附、程序升温还原、程序升温表面反应、程序升温反应和化学捕获反应等手段,对Rh/SiO2催化剂上甲烷部分氧化制合成气反应进行了研究.结果表明,Rh/SiO2催化剂上甲烷部分氧化制合成气机理属于热解-氧化反应机理.甲烷首先在催化剂上发生解离吸附,产生具有不同H/C比的化学吸附物种CHx(x=1~3).其中,具有较高H/C比的CHx可能是甲烷部分氧化反应的活性物种,而具有较低H/C比的CHx可能是催化剂上积碳并导致催化剂失活的来源.活性物种CHx在活性氧物种的作用下,生成含氧中间体物种CHxO或继续脱氢.含氧中间体物种进一步分解,即生成CO和H2;CO2也可由CHx或CHxO物种进一步氧
化生成. 相似文献
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用晶格氧为氧源的甲烷部分氧化制合成气 总被引:16,自引:0,他引:16
采用热重分析技术在甲烷气氛下考察了储氧材料Fe2O3提供晶格氧的过程,用甲烷/氧切换反应和在线质谱检测方法研究了以Fe2O3晶格氧代替气相氧用于甲烷部分氧化制合成气的可能性.结果表明,Fe2O3在甲烷气氛下的还原过程包括Fe2O3→Fe3O4和Fe3O4→FeO→Fe,甲烷被氧化为CO2和H2O.在750℃下进行的CH4/O2切换反应结果表明,首先,约25%的CH4与Fe2O3中的晶格氧反应,生成CO2和H2O,然后,生成的CO2和H2O与剩余的约75%的CH4在Ni/Al2O3催化剂上进行蒸汽重整和C\r\nO2重整,从而按燃烧-重整机理实现甲烷部分氧化制合成气.选择合适的CH4/O2切换条件,可使甲烷高转化率、高选择性地生成合成气. 相似文献
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用溶胶-凝胶法以磷钼酸(MPA)的镍盐溶液水解钛酸四丁酯制备了NiPMo/TiO2催化剂.使用ICP、 XRD、 TG-DTA、 IR、 TPD-MS和微反应技术研究了催化剂的化学组成、热稳定性、化学吸附性质和催化反应性能.杂多钼酸盐与TiO2通过O2-在TiO2表面发生了键合.在623 K下,杂多阴离子仍保持原有的Keggin结构.CO2在Lewis酸位Ni(Ⅱ)和Lewis碱位Ni-O-Mo的桥氧协同作用下生成CO2卧式吸附态Ni(Ⅱ)←O-(CO)←(O--Ni).丙烯有多种吸附态在催化剂上吸附.在563 K、 1 MPa和空速1500 h-1的反应条件下,丙烯的摩尔转化率为3.2%,产物MAA选择性为95%. 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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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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The Langevin paramagnetic theory can’t describe the relation between magnetization of ferrofluids and applied magnetic field. The structuralization of ferrofluids, which is considered the main influence factor of the magnetization, is regarded. The part of magnetization works is deposited when the structure is forming. This action influences the magnetization of ferrofluids directly or indirectly. On the base of the “compressing” model, the Langevin function that usually describes the magnetization of ferrofluid is modified, and a well-fitted curve is obtained. An equation of the relation between the equivalent volume fraction after being “compressed” and the intensity of magnetic field is discovered, which approximately describes the process of magnetization. The relation between the approximate initial susceptibility and the volume fraction can be obtained from modified formula. 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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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
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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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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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Shashikant U. Dighe Surya K. Samanta Shivalinga Kolle Sanjay Batra 《Tetrahedron》2017,73(17):2455-2467
An efficient iodine-mediated oxidative Pictet-Spengler reaction in dimethyl sulphoxide (DMSO) using terminal alkynes as the 2-oxoaldehyde surrogate for the synthesis of aryl (9H-pyrido[3,4-b]indol-1-yl)methanones is described. The scope of the protocol includes the total synthesis of Fascaplysin, Eudistomins Y1 and Y2. The methodology is extended for preparing pyrrolo[1,2-a]-quinoxaline and indolo[1,5-a]quinoxaline derivatives. The utility of 1-aroyl-β-carbolines was demonstrated by performing palladium-catalyzed β-carboline directed ortho-C(sp2)-H functionalization of the phenyl ring with thiomethyl (SMe) group using DMSO as source and for accessing 4-aryl-canthin-6-ones. 相似文献