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运用XRD、TPR、H2-TPD等表征手段考察了Cu-Mn催化剂的物相结构、氢气的还原性能及H2的吸附性能;在高压微反色谱系统中进行了CO加氢合成二甲醚的研究并和表征结果相关联。评价结果表明,Cu-Mn双组分催化剂对一氧化碳具有很高的活性及二甲醇的选择性; XRD测定结果表明, Mn的存在使得CuO的分散度提高:TPR结果表明,锰的存在阻碍了CuO的还原,CuO存在能够促进MnOx的还原,双组分催化剂的还原并不是单组分催化剂的简单叠加,说明在催化剂的制备过程中CuO和MnOx之间发生了一定的相互作用。H2的脱附实验表明,Mn的添加增强了催化剂对H2的吸附能力。 相似文献
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锰基催化剂上CO2加氢反应性能的研究 总被引:1,自引:0,他引:1
研究了Mn基催化上CO2的加氢反应性能,结果表明:CO2活化吸附量的增加有利于CO2转化率的提高。Mn具有较好的CO2加氢生成CO的催化活性,CuO,Fe2O3的ZnO的加入使催化剂活性得到进一步的提高;NiO的加入增加了催化剂的H2活化吸附量,从而使催化剂对CH4的选择性得到提高,同时使CO2的转化率与Ni/γ-Al2O3相比略有下降。 相似文献
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Cu对Cu—Mn—Ce—O和Cu—Mn—Ce—Pd—O催化剂三效性能的影响 总被引:1,自引:0,他引:1
利用火焰脉冲-微反装置考察了Cu-Mn-Ce-O和Cu-Mn-Ce-Pd-O两类催化剂的三效活性。结果表明Cu的加入有利Cu-Mn-Ce-O的NOx和CO的转化,而不利于Cu-Mn-Ce-Pd-O的NOx和HC的转化。XRD分析结果表明在Cu-Mn-Ce-O中加入Pd,原来的CuMn2O3消失,生成新相MnAl2O4;TPR分析结果表明Cu使Mn-Ce-O样品表面氧量增加,表面易于还原,而使Mn- 相似文献
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Cu对Cu-Mn-Ce-O和Cu-Mn-Ce-Pd-O催化剂三效性能的影响 总被引:1,自引:0,他引:1
利用火焰脉冲-微反装置考察了Cu-Mn-Ce-O和Cu-Mn-Ce-Pd-O两类催化剂的三效活性。结果表明Cu的加入有利于Cu-Mn-Ce-O的NOx和CO的转化,而不利于Cu-Mn-Ce-pd-O的NOx和HC的转化。XRD分析结果表明在Cu-Mn-Ce-O中加入Pd,原来的CuMn_2O_3消失,生成新相MnAl_2O_4;TPR分析结果表明Cu使Mn-Ce-O样品表面氧量增加,表面易于还原,而使Mn-Ce-pd-O样品表面难于还原。实验结果还表明Mn-Ce-pd-O催化剂的三效性能远远优于Cu-Mn-Ce-O催化剂。 相似文献
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主要用第四周期金属元素的氧化物与Al2O3的复合氧化物催化剂上甲烷氧化的结果证实了催化剂设计中的预测:(1)催化剂首先应能解离活化甲烷,(2)催化剂要能较快地活化O2分子.只有同时满足这两个条件,催化剂才可能有较好的甲烷部分氧化活性.第四周期元素中只有镍具有这样的性质.Cu,Mn,Cr,La,Ca,Zn等氧化物的添加可明显提高Ni-Al2O3催化剂的甲烷部分氧化性能,其中Cu的助催化性能最好.催化剂NiO-CuO-Al2O3,NiO-MnO-Al2O3,NiO-Cr2O3-Al2O3的反应活性和选择性顺序,与金属Cu,Mn,Cr上CO和H2脱附的顺序是一致的 相似文献
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在低温低压和浆态反应条件下,考察了空速、反应时间、杂质及Cu-Cr摩尔比对铜基催化剂催化合成气一步合成甲醇和甲酸甲酯反应的影响。实验结果表明,空速对催化剂活性有较显著的影响;CO转化率与反应时间无关,但H2的转化率与反应时间有关。在15小时之内H2的转化率随反应时间增加而缓慢增加,此后与反应时间无关。此外,高浓度的杂质使催化剂的活性和寿命下降,而且Cu/Cr摩尔比和热处理气氛对催化剂的物相和活性也有显著的影响。 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