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标题化合物(Me2SiSiMe2)〔η^5-(3-Me3SiC5H3)Fe(CO)2〕2/(μ-CO)2(A)分子中的Fe-Fe键被钠汞齐还原断裂,生成相应的双铁负离子,分别与MeCOCl、PhCOCl、PhCH2Cl、ClCH2COOC2H5和Ph3SnCl进行亲核取代反应,生成在铁原子上引入相应取代基的产物(Me2SiSiMe2)〔η^5-(3-Me3SiC5H3)Fe(CO)2R〕2(R:M 相似文献
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TiO2,La2O3和ZrO2以单层形式分布在SiO2上制得了Pd催化剂。经473K(LTR)及773K(HTR)H2处理后,进行H2-O2滴定反应,测定催化剂对H2的吸附能力。结果表明,Pd/TiO2/SiO2,Pd/La2O3/SiO2及Pd/ZrO2/SiO2的吸氢能力高于单一载体Pd催化剂的吸能力,说明SiO2骨架经涂层氧化物的改性,Pd得到较好的分散。Pd与载体之间相互作用为:Pd/Ti 相似文献
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本文应用碱性气体吸附的红外光谱和TPD技术研究了FeZSM-5(F4)的酸性,酸性为:H-F4〉Fe2O3/F4〉F4原粉〉水热处理的K-F4〉Li-F4〉Na-F4〉K-F4〉NaOH/F4。比较了酸强度和积炭对乙苯氧化脱氢性能的影响,以及催化剂酸碱性质与积炭的关系。结果表明,乙苯氧化脱氢反应是在酸碱协同作用下进行的,积炭也参与了氧化脱氢反应,催化剂表面上L酸中心产生的具有一定C、H、O比的积炭 相似文献
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本文用化学吸附、原位IR、和XPS考察了钒助剂对Rh2/SiO2催化剂的H2和CO化学吸附的影响.结果表明,1)CO吸附在RhI、RhⅡ和RhⅢ中心上分别产生孪生、线式和桥式CO表面吸附物种.2)H2主要解离吸附在RhⅡ和RhⅢ中心上,但CO能优先吸附;RhI中心对H2的化学吸附能力弱,但H2和CO能共吸附在RhI中心上形成表面羰基氢化物.3)Rh2-V/SiO2催化剂在573K还原后,铑与钒助剂的强相互作用主要发生在RhⅡ和RhⅢ与钒助剂之间,H2吸附比CO吸附受到更强烈的抑制.用覆盖模型可以较好地解释钒助剂对Rh2/SiO2催化剂的H2和CO化学吸附的影响. 相似文献
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丙炔醇聚合股对铁在酸性溶液中的缓蚀作用 总被引:1,自引:0,他引:1
应用电化学交流阻抗谱技术研究了Fe/H_2SO_4与Fe/H_2SO_4+H_2S体系中丙炔醇(PA)聚合膜的形成及其缓蚀作用,同时利用SEM、AFM及EDX对PA聚合不同时期铁表面腐蚀形貌进行观测与成分分析.结果表明,Fe/H_2SO_4与 Fe/H_2SO_4+ H_2S体系中 PA可逐渐聚合成膜,从而有效抑制基体的腐蚀,使电极表面较为平整,微米尺度下呈现规则的块状结构;但Fe/H_2SO_4体系中宏观上PA并未形成连续的保护膜,导致电极表面局部发生腐蚀;而Fe/H_2SO_4+H_2S体系中,H_2S、HS-在电极表面的吸附减缓了PA聚合成膜,但长时间腐蚀后,由于硫化物的生成覆盖在PA聚合膜上,使其具有长期缓蚀效能. 相似文献
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镍盐和氧化镍在NaY沸石中存在状态研究 总被引:1,自引:0,他引:1
用XRD、EXAFS和TPR方法研究了Ni(NO3)2/NaY和NiO/NaY分散体系。在沸石上,Ni(NO3)2的分散比NiO容易得多。XRD相定量方法测定的NiO在NaY沸石上的分散阈值很低,仅为密置单层容量的2%左右。在分散阈值关NiO在沸石上处于分散相和笼外小晶粒两种状态。分散相NiO比笼外NiO小晶粒难还原。样品中NiO含量超过阈值时,笼外小晶粒长大成XRD可检测的较大晶粒。 相似文献
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以H2S和CS2作硫化剂,用PPS和TPDS方法研究了水煤气变换催化剂CoMoK/γ-Al2O3的硫化及反硫化过程。用H2S/H2硫化时,只发现H2S的消耗和H2O的生成,用CS2/H2硫化时,只发现H2S的消耗和H2O的生成。用CS2/H2硫化时,首先生成CO2,然后是CH4,H2O和H2S,TPG实验表明催化剂表面上积炭,造成催化剂和活性降低,但积炭在水煤变换反应进行了逐渐除法。TPDS实验表 相似文献
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CO2和CH3OH直接合成碳酸二甲酯Cu-Ni/V2O5-SiO2催化剂 总被引:11,自引:0,他引:11
采用表面反应改性法制备了V2O5-SiO2(VSiO)表面复合物,用等体积浸渍法制备了VSiO担载的Cu-Ni双金属催化剂,用IR,TPD,TPSR和微反技术研究了CO2和CH3OH在催化剂表面上的化学吸附与反应性能。结果表明,在Cu-Ni/VSiO催化剂上存在着金属位Cu-Ni合金,Lewis酸位V^n+和Lewis碱位V=O三类活性中心;CO2在金属位和Lewis酸位协同作用下可生成CO2卧式 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
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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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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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An efficient tandem approach for the selective synthesis of 4,5-dihydroimidazo[1,5-a]quinoxalines 6a–g and imidazo[1,5-a]quinoxalines 7a–h by the reaction of 2-imidazolyl anilines 4a–c with aryl aldehydes 5a–k under mild reaction conditions is described. Introduction of electron releasing alkyl groups in substrates 4a–b was found to be instrumental for the success of the reaction. 相似文献
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The Diels-Alder reactivity of 1,2-heteroborines (H4C4B(H)X, X?=?NH, PH, AsH; O, S, Se) has been computationally explored by means of Density Functional Theory (DFT) calculations. The influence of the HB?=?X fragment on the reactivity of the system has been quantitatively analyzed in detail by means of the so-called Activation Strain Model (ASM) of reactivity. It is found that the interaction between these species and the dienophile is significantly stronger than that computed for their all-carbon isoelectronic counterpart, benzene. In addition, the strain energy plays a key role in the observed reactivity trends. The role of the aromaticity strength of these heteroarenes on the reactivity is also assessed. 相似文献
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Xi-Liu YunWen-Ying Bi Jian-Hui HuangYu Liu Daisy Zhang-NegrerieYun-Fei Du Kang Zhao 《Tetrahedron letters》2012,53(38):5076-5080
A variety of N-aryl and N-alkyl carbazolones were conveniently achieved in good to high yields via Pd2(dba)3-mediated intramolecular coupling of N-substituted α-iodo enaminones under microwave irradiation. The Pd(0)-catalyzed cyclization was found to proceed favorably with the more electron-deficient phenyl ring during the reactions involving unsymmetrical N,N-diaryl α-iodo enaminones. This unique property enables the construction of carbazolone skeleton containing nitro substituted benzenoid ring. 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
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Both substituted 2,4,5,6-tetrahydrocyclopenta[c]pyrazoles and 2,4,5,6-tetrahydropyrrolo[3,4-c]pyrazoles have been synthesized by the 3+2 intramolecular dipolar cycloaddition of nitrilimines to alkynes. This cyclization has been extended to more versatile 3-bromo derivatives by the use of alkynylbromides as dipolarophiles. 相似文献
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In this Letter, we described a facile method for constructing fused bicyclic 1-arylpyrazol-5-one ring system. We employed various methylene-containing carboxylic acids as the substrates and proved that the pyrazolone ring closure requires activated methylene group in intermediate II. Accordingly, a series of structurally diversified, fused bicyclic 1-arylpyrazol-5-ones was prepared in moderate to high yields using the requisite substrates. 相似文献