共查询到19条相似文献,搜索用时 187 毫秒
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介孔MCM-41分子筛载钯配合物催化Heck反应的性能 总被引:11,自引:0,他引:11
以MCM 41分子筛作为固载材料 ,经氨基功能化后与各种钯化合物形成MCM 41载钯配合物。采用XRD、XPS等技术对其结构及表面性能进行了表征 ,并研究了催化剂的制备条件等因素对催化Heck芳基化反应性能的影响 ;同时 ,以共轭烯烃和各种芳基碘的Heck芳基化反应考察了MCM NH2 ·Pd(0 ,Ⅱ )配合物的催化性能。结果表明 ,MCM NH2 固载钯配合物具有高的催化活性和立体选择性 ,高得率地生成了一系列取代的反式产物。 相似文献
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MCM-41分子筛固载腈钯配合物的合成及其催化Heck偶联反应的性能 总被引:1,自引:0,他引:1
合成了MCM-41分子筛固载腈钯(0,Ⅱ)配合物催化剂,并利用XPS、FT-Raman等技术对催化剂进行了表征.研究表明,MCM-41分子筛载体上的-CN基可通过叁键上的π电子对与Pd发生弱配位.MCM-(CH2)3CN·Pd(O)具有良好的催化性能和稳定性,在反应温度70℃、DMF-Et3N的存在下,对催化各种碘代芳烃与共轭烯烃的Heck偶联反应均较有效,高产率且高立体选择地生成了一系列取代的反式产物,产物分离收率达到84%以上. 相似文献
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聚-ω-(甲硒基)十一烷基硅氧烷钯(0)配合物的合成与催化性能 总被引:1,自引:0,他引:1
ω-氯代十一烷基三乙氧基硅烷依次用气相法二氧化硅固载、与甲硒基钠和氯化钯作用, 再用水合肼还原, 合成了气相法二氧化硅负载的聚-ω-(甲硒基)十一烷基硅氧烷钯(0)配合物. 该钯(0)配合物对丙烯腈和丙烯酸与芳基碘的Heck芳基化反应具有很高的催化活性, 为各种肉桂腈和肉桂酸的立体选择合成提供了方便实用的新途径. 相似文献
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合成了MCM-41负载的双(全氟烷基磺酰亚胺)催化剂 (HN(SO2Rf)2,Rf为全氟烷基),并用XRD, FTIR, SEM, TG-DTA and N2-吸附技术等对它们的结构进行了表征。将这些负载催化剂(HN(SO2Rf)2/MCM–41)用作对苯二酚和叔丁醇的烷基化反应的催化剂,研究了各种反应条件对该反应的影响。在优化反应条件下,仅用5 mol% HN(SO2C4F9)2/MCM-41催化该反应,可以得到高产率(52.0%)的2-叔丁基对苯二酚。研究结果表明,该新型负载催化剂可以至少重复使用6次,而其催化活性基本不变。 相似文献
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首先通过两步后合成处理,在MCM-41上接枝苄基磺酸;然后,以苄基磺酸为过渡产物,用手性Mn(salen)配合物修饰处理,得到了苄基磺酸轴向负载手性Mn(salen)配合物的MCM-41;实现了在廉价且温和条件下均相手性Mn(salen)催化剂的非均相化。采用X射线衍射(XRD)、低温N2吸附-脱附、红外光谱、热重-差示扫描量热(TG-DSC)分析、电感耦合等离子体发射光谱(ICP)和酸度滴定等对样品进行了表征。结果表明,手性Mn(salen)配合物成功固载在MCM-41上,且MCM-41的介孔结构和Mn(salen)配合物的手性特征仍然保留。以间氯过氧苯甲酸为氧化剂,考察了所得固载型催化剂对α-甲基苯乙烯的不对称环氧化催化性能,结果表明在0 ℃反应2 h,催化剂用量为0.02 mmol,无需加入轴向配体N-甲基吗啉氮氧化物(NMO)的条件下对映体过量(enantiomeric excess,e.e.)值可达99%以上,转化率为77%。归因于苄基磺酸基起到了很好的轴向配体作用。经适当处理,固载型催化剂在循环使用5次后e.e.值依然有71%,表现出较好的活性和重复使用性能。 相似文献
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Jianmin Zhou Yulin Yang Lan Zhao Xiaokun Li Renxian Zhou Xiaoming Zheng 《Frontiers of Chemistry in China》2009,4(2):142-148
Using MCM-41 as the supporter, a series of MCM-41 supported amino-palladium complexes has been prepared and characterized
by XRD (X-ray diffraction) and XPS (X-ray photoelectron spectroscopy), etc. The XRD and XPS results indicate that the Pd coordinates
with the -NH2 groups on the MCM-41 surface, and the structure of MCM-41 has been not damaged. Its catalytic performance for Heck arylation
of alkene with aryl iodide shows that the catalysts have high activity and stereoselectivity in 70–90°C. The product of Heck
reaction is in E form. And the effect of the preparation condition of catalyst on the catalytic performance was examined.
Translated form Chinese Journal of Organic Chemistry, 2008, 28(5) (in Chinese) 相似文献
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一种无机-有机高分子杂化催化剂Pd(0)-CS/MCM-41的制备及其性能研究 总被引:1,自引:0,他引:1
将天然高分子聚合物壳聚糖负载到MCM-41介孔分子筛上,再在室温与氯化钯乙醇溶液作用,制得了一种无机-有机天然高分子杂化催化剂Pd(0)-CS/MCM-41,并利用XPS、FTIR、XRD、热重等手段对其进行了表征。以碘代苯与丙烯酸的Heck芳基化反应考察了所得催化剂的催化性能。结果表明,催化剂具有较高的催化活性和良好的重复使用性能,催化剂在氮气保护下能有效地催化碘代苯与丙烯酸的Heck反应,高产率地得到反式肉桂酸。经8次重复使用后,肉桂酸的产率仍达80%以上。 相似文献
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Shuwei Chen Zheqi Xu Dongchen Tan Dahai Pan Xingyu Cui Yan Qiao Ruifeng Li 《应用有机金属化学》2020,34(2):e5396
Catalytic performance of Al-MCM-41-supported vanadia catalysts (V/Al-MCM-41) with different V loading was investigated for oxidative dehydrogenation of ethylbenzene to styrene (ST) with CO2 (CO2-ODEB). For comparison, pure silica MCM-41 was also used as support for vanadia catalyst. The catalysts were characterized by N2 adsorption, X-ray diffraction (XRD) pyridine-Fourier-transform infrared spectroscopy, H2-temperature-programmed reduction, thermogravimetric analysis (TGA), UV-Raman, and diffuse reflectance (DR) UV–vis spectroscopy. The results indicate that the catalytic behavior and the nature of V species depend strongly on the V loading and the support properties. Compared with the MCM-41-supported catalyst, the Al-MCM-41-supported vanadia catalyst exhibits much higher catalytic activity and stability along with a high ST selectivity (>98%). The superior catalytic performance of the present V/Al-MCM-41 catalyst can be attributed to the Al-MCM-41 support being more favorable for the high dispersion of V species and the stabilization of active V5+ species. Together with the characterization results of XRD, TGA, and DR UV–Vis spectroscopy, the deep reduction of V5+ into V3+ during CO2-ODEB is the main reason for the deactivation of the supported vanadia catalyst, while the coke deposition has a less important impact on the catalyst stability. 相似文献
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Palladium chloride was grafted to amino‐functionalized MCM‐41 to prepare heterogeneous catalysts. XRD, N2 adsorption–desorption isotherms, IR, 13C and 29Si cross‐polarization magic‐angle spinning NMR spectroscopy and XPS techniques were employed to characterize the catalytic materials. The heterogeneous palladium catalyst exhibited excellent catalytic activity for the Heck vinylation of iodobenzene with methyl acrylate, giving 92% yield of methyl cinnamate in the presence of N‐methylpyrrolidone (NMP) and triethylamine (Et3N). The stability of the heterogeneous catalyst was also studied in detail. The catalytic tests showed that the palladium leaching correlated to solvent, base and palladium loading. The heterogeneous catalyst exhibited excellent stability towards loss of activity and palladium leaching was not observed during six recycles in the presence of toluene and Na2CO3. Copyright © 2007 John Wiley & Sons, Ltd. 相似文献
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Hengquan Yang Gaoyong Zhang Xinlin Hong YinyanZhu 《Journal of molecular catalysis. A, Chemical》2004,210(1-2):143-148
Palladium(II,0) complexes were anchored on dicyano-functionalized MCM-41, producing new heterogeneous catalysts of the Heck reaction, which were synthesized via two-step surface modification of mesoporous molecular sieve MCM-41. The developed catalysts demonstrated easy separation after reaction, and reusability. BET, XRD, FT-IR, ICP-AES, H2 chemisorption as well as XPS techniques were employed to characterize the catalytic materials. 相似文献
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M. J. Jia W. Y. Lin W. X. Zhang F. S. Xiao W. Q. Pang T. H. Wu 《Reaction Kinetics and Catalysis Letters》1999,67(2):353-358
Selective catalytic reduction of nitrogen monoxide with propene over two kinds of CuCl/MCM-41 catalysts prepared by a dispersion
method has been studied. It was found that CuCl/AlMCM-41 exhibits substantially higher activity over CuCl/SiMCM-41. Characterization
of these samples by H2-TPR, IR and XRD showed that the active copper species were mainly related to Cu2+ and Cu+ ions in CuCl/AlMCM-41 catalyst. 相似文献
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《Journal of Analytical and Applied Pyrolysis》2010,87(2):281-286
This paper investigates the catalytic activity of MCM-41 synthesized via silatrane route and Ru/MCM-41 in waste tire pyrolysis. The experimental results showed that the presence of catalysts strongly influenced the yield and nature of products. Namely, the gas yield increased at the expense of liquid yield. In addition, a considerable high yield of light olefins, 4 times higher than non-catalytic pyrolysis, can be achieved for Ru/MCM-41 catalyst. Furthermore, the uses of catalysts produced much lighter oil and there was a drastic increase in the concentration of single ring aromatics in accordance to a reduction in polycyclic aromatic compounds in the derived oils. Ru/MCM-41 produced the lightest oil and the oil has the highest concentration of mono-aromatics. The high activity of catalysts, particularly Ru/MCM-41 was discussed in relation with the catalyst characterization results obtained from various techniques including TPD-NH3, H2-chemisorption, XRD, N2-adsorption/desorption analysis, and TPO. 相似文献
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FT-IR study of NO and C3H6 adsorption, co-adsorption and interaction in the presence of oxygen were performed in order to estimate the catalytic behaviour
of Au and V-containing MCM-41 materials in NO-SCR with propene. MCM-41 were modified with gold, vanadium and niobium by their
introduction during the synthesis (co-precipitation) carried out with the use of HCl or H2SO4 as pH adjustment agent. The texture/structure properties of the prepared samples were investigated by N2 adsorption, XRD, XPS and TEM techniques. It has been found that the nature of acid used for the pH adjustment during the
synthesis determines the gold particles size and dispersion and influences the interaction of NO+O2+C3H6 with the catalyst surfaces. In both types of AuVMCM-41 catalysts, the SCR reaction route occurs via NO2 formation. In the case of AuVMCM-41(HCl) and AuVNbMCM-41(HCl) nitrites are formed and stored, and upon heating NO2 is released. These kinds of nitrites are not formed on AuVMCM-41(H2SO4) and AuVNbMCM-41(H2SO4). Instead of that NO2 is chemisorbed on metallic gold, niobium and vanadium species and reacts with propene and/or oxygenates. 相似文献
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The activities of a MnO/γ‐Al2O3 catalyst for the selective reduction of methyl benzoate to benzaldehyde have been studied in a continuous flow reactor. Characterization of the catalyst has been conducted by XRD, XPS, NH3‐TPD and TPD‐IR. XRD and XPS results revealed that the steady state catalyst is mainly MnO2/γ‐AlO3 before reduction and MnO/γ‐Al2O3 after reduction. Monolayer dispersion capacity obtained by XPS method is about w (Mn)11.3% TPD‐IR results revealed that there are only L acidic centers on the catalytic surface. NH3‐TPD determinations have verified that the catalyst with a certain number of moderate strength acidic sites is advantageous to hydrogenation of methyl benzoate to benzaldehyde. 相似文献