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杂多酸的固载化─关于制备负载型酸催化剂的一般原理 总被引:10,自引:0,他引:10
杂多酸同时具有酸和氧化-还原的催化特性,有着很广泛的应用前景.这类化合物在一系列精细合成中取代硫酸作为催化剂以满足环保的要求,显示出了很大的潜力.杂多酸固载化后,不仅能在液相氧化和酸催化反应中把催化剂从反应介质中很方便地分离出来,而且还为这类均相催化反应的多相化,甚至利用催化蒸馏新工艺等创造了应有的条件,可以使生产工艺大大简化,获得更广泛的应用.本文以很好表征过的多种孔性材料,包括氧化物,如Al_2O_3、SiO_2、TiO_2、硅藻土、膨润土和来源不同的活性炭为载体,考察了负载杂多酸催化剂的催化活性.在大量前期工作的基础上,通过总结载体对固载杂多酸催化活性的影响等,探讨载体的内在性质在杂多酸固载、吸附和催化反应中的作用本质,为由吸附法制备各种负载型固体酸催化剂在液相中的应用提供可资参考的模型. 相似文献
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含钼四元杂多磷钨酸盐的电化学研究 总被引:3,自引:0,他引:3
含钼四元杂多磷钨酸盐的电化学研究张恒彬,齐兴义,郑军伟,李树家(吉林大学化学系,长春,130023)关键词磷钨杂多酸,氧化还原,电催化,循环伏安Keggin结构钼或钨的杂多酸有良好的氧化还原性质和电催化作用[1~3].其中钼或钨被其它过渡金属元素取代... 相似文献
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基于杂多酸的固体高质子导体* 总被引:1,自引:0,他引:1
杂多酸固体高质子导体在燃料电池、传感器和电显色装置等方面具有潜在的应用前景。本文概述了杂多酸的质子导电性,归纳了其质子导电性的一些规律,以表格形式列举了各类杂多酸的电导率。将不同质量分数的杂多酸固载在各类固体基质上,可以对杂多酸质子导电材料改性以便于工业中实际应用。这些杂化材料兼有杂多酸的高质子导电性以及基质的稳定性与机械延展性。本文综述了近几年来新型杂多酸,杂多酸-无机基质复合材料,杂多酸-有机基质复合材料,杂多酸-多元基复合材料的质子电导率、稳定性、结构形态等等方面的研究进展,详细介绍了杂多酸在质子交换膜燃料电池中的应用,并对杂多酸固体高质子导体的应用前景进行了展望。 相似文献
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在氢离子浓度均为3mol/L的硫酸,盐酸,磷酸,醋酸水溶液中和冰醋酸中研究了具有Keggin结构的硅钨杂多酸(SiW12)在不同来源活性炭上的吸附作用,各活性炭对SiW12吸附等温线的形式是不相同的,吸附剂载体的微孔结构以及杂多酸的溶剂化起着重要的,工且在无机酸介质中,杂多酸的吸附量比在水溶液中成规律地增加,且与酸强度正比关系,在有机酸介质中,吸附作用比较复杂,根据所得结果,提出了在酸性中杂多酸在 相似文献
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Villabrille P Vázquez P Blanco M Cáceres C 《Journal of colloid and interface science》2002,251(1):151-159
Molybdosilicic acid solutions acidified with HCl were impregnated on carbon and silica by the equilibrium adsorption technique. From the equilibrium adsorption isotherms performed at 20 degrees C, it was established that the heteropolyacid amount adsorbed on carbon is higher than that on silica. Differences in shape and initial slope of the isotherm were observed. The interaction of the molybdosilicate anion was higher with carbon surface groups than with silanol groups. The physicochemical characterization of the solids has shown that the molybdosilicic acid presents an undegraded Keggin structure in the supported samples up to 250 degrees C. The surface acidity, mainly related to heteropolyacid adsorbed amount, was higher for samples on carbon. However, the silica-supported acid showed a bulk acidity higher than that on carbon, due to its lower interaction degree. 相似文献
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L.F. Chen J.A. Wang J. Aguilar P. Salas P. Del Ángel 《Journal of solid state chemistry》2007,180(10):2958-2972
For the first time, modifications of the surface and framework of Si-MCM-41 by depositing a heteropolyacid on the surface and by introducing foreign Zr4+ ions into the framework are investigated. The Zr-modified Si-MCM-41 mesoporous materials (hereafter referred as WSZn, n=Si/Zr=25, 15, 8, 4) were synthesized through a surfactant-templated preparation approach, using low-cost fumed silica as the Si precursor. After impregnation with 25 wt% of H3PW12O40, the surface Brönsted acidity of the Pt/H3PW12O40/WSZn catalysts was greatly enhanced by 2-10 times relative to the bare WSZn support. Two kinds of supported heteropolyacids were formed: (i) bulk-like heteropolyacid crystals with unchanged Keggin structures, and (ii) highly dispersed heteropolyacid with distorted Keggin units. The formation of various kinds of heteropolyacid structures is closely related to the interaction between the heteropolyanions and the hydroxyl groups in the host support. 相似文献
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Nathalie Laronze Jean-François Moisan Catherine Roch-Marchal Feng-Xian Liu Gilbert Hervé 《Journal of Cluster Science》2002,13(3):355-368
Transition metal salts of heteropolyacids have been prepared taking into account the strong acidic and cation exchanging properties of the solid heteropolyacids. The exchange between protons and the transition metal cation is carried out by stirring a suspension of the hydrated heteropolyacid in a solution of the metal acetylacetonate complex in toluene. The exchange occurs on the surface of the solid particles and diffusion of protons and metal cations into the hydrated lattice leads to the substitution of all the protons. The method can be utilized in order to prepare supported vanadyl and copper molybdophosphates from supported heteropolyacids and they have been studied in the catalysis of the oxidative dehydrogenation of isobutyric acid. The effect of vanadyl counter-ions on the catalytic behavior is the same as observed with bulk catalysts but, on the contrary, copper supported molybdophosphate shows an acid catalytic activity not observed with bulk catalysts. 相似文献
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S. A. Popova A. L. Tarasov L. M. Kustov I. Yu. Chukicheva A. V. Kuchin 《Russian Journal of Physical Chemistry A, Focus on Chemistry》2013,87(2):342-344
Alkylation of phenol with camphene in the presence of supported heteropolyacids is studied. The main reaction products are found to be phenyl isobornyl ether, 2-isobornylphenol and 2-isocamphylphenol, the ratio between them being determined by the nature of heteropolyacid and carrier (ZrO2 or TiO2). 相似文献
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Amlie Thomas Cline Dablemont Jean-Marie Basset Frdric Lefebvre 《Comptes Rendus Chimie》2005,8(11-12):1969
The H3PW12O40 and H4SiW12O40 heteropolyacids supported on silica were studied by 1H MAS NMR as a function of both the coverage and the dehydroxylation temperature. The signal at ca. 8 ppm attributed to the highly acidic protons of the anhydrous form of the heteropolyacid was never observed in the case of the phosphotungstic polyanion supported on silica while it was clearly present in the case of the silicotungstic species. These results explain the different activities of the two supported heteropolyacids in acid reactions involving strong acid sites. To cite this article: A. Thomas et al., C. R. Chimie 8 (2005). 相似文献
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介绍了以活性炭为载体的负载型杂多酸催化剂的研究进展,包括制备方法、影响负载量的因素、负载催化剂的性质、吸附模型和脱附作用。总结了杂多酸在活性炭上的吸附形态研究以及杂多酸与活性炭表面含氧基团的化学键合作用的研究成果,展望了该催化剂未来的研究方向。 相似文献
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Esterification of phthalic anhydride with 1-butanol and 2-ethylhexanol catalyzed by heteropolyacids 总被引:5,自引:0,他引:5
M. Arabi M. Mohammadpour Amini M. Abedini A. Nemati M. Alizadeh 《Journal of molecular catalysis. A, Chemical》2003,200(1-2):105-110
Esterification of phthalic anhydride with 2-ethylhexanol and 1-butanol and ester decomposition of dioctyl phthalate (DOP) in presence of Keggin; H3PW12O40, H4SiW12O40, H4SiMo12O40, Wells–Dawson; H6P2W18O62, H6P2W17MoO62 and Preyssler; H14[NaP5W29MoO110], H14[NaP5W30O110], type heteropolyacids have been investigated. The heteropolyacids with Preyssler and Wells–Dawson structures and their molybdenum substituted derivatives show higher activity in esterification and ester decomposition reactions than Keggin type heteropolyacids. A complete conversion of phthalic anhydride to dioctyl phthalate and dibutyl phthalate are achieved in 2 h in presence of molybdenum substituted Preyssler heteropolyacid. In the decomposition of dioctyl phthalate in the presence of Preyssler heteropolyacid, 2-ethylhexene is formed in quantitative yield. 相似文献
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Angel G. Sathicq Valeria Palermo Patricia G. Vázquez Horacio J. Thomas 《Tetrahedron letters》2008,49(9):1441-1444
A range of sulfides can be selectively oxidized to the corresponding sulfoxides in good yields using catalytic quantities of heterocyclic amine salts (quinoline, cinchonine, and cinchonidine) of Keggin heteropolyacids with different green oxidants. The cinchonine heteropolyacid catalyst is easily recoverable and reusable without loss of its catalytic activity, and an enantiomeric excess can be obtained. 相似文献
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Tarlani A Abedini M Nemati A Khabaz M Amini MM 《Journal of colloid and interface science》2006,303(1):32-38
The Keggin and Preyssler tungsten heteropolyacids, H3PW12O40 and H15P5W30O110, have been immobilized on the inner surface of mesoporous MCM-41, fume silica and silica-gel by means of chemical bonding to aminosilane groups. The materials were characterized by FT-IR spectroscopy, low-angle XRD and BET surface area analysis. The tendencies of heteropolyacids adsorption in solution on functionalized silicas have been investigated by UV-vis. Among the functionalized silica materials, MCM-41 showed the largest amine to silica and the least heteropolyacid to silica ratios. The BET surface area revealed that in all three cases the surface area decreased after grafting amine group and anchoring of the HPAs clusters. Low-angle XRD analysis showed that by introducing HPA into functionalized MCM-41 the intensity of the main reflection decreased significantly. 相似文献