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新型苯选择加氢制环己烯非晶态催化剂Ru-Fe-B/ZrO2的制备及其可调变性 总被引:1,自引:0,他引:1
采用化学还原法制备了一种新型高活性和高选择性苯选择加氢制环己烯的Ru-Fe-B/ZrO2纳米非晶态合金催化剂,并利用透射电镜、选区电子衍射、X射线衍射和N2物理吸附仪等手段对催化剂进行了表征.重点研究了Ru-Fe-B/ZrO2催化剂活性和选择性的可调变性,及还原剂NaBH4浓度和洗涤后滤液的pH值对其催化性能的影响.结果表明,在新型Ru-Fe-B/ZrO2催化剂上,当苯转化54%时,环己烯选择性高达80%,同时环己烯选择性随苯转化率升高而缓慢下降.向反应浆液中添加酸性或碱性物质可以调变催化剂的活性和选择性,同时催化剂制备工艺和性能具有很好的可重复性.Ru-Fe-B/ZrO2催化剂融合了纳米和非晶材料的特性,这是其对苯选择加氢制环己烯表现出高活性和高选择性的主要原因. 相似文献
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苯选择加氢制环己烯Ru-Co-B/ZrO2催化剂的研究 总被引:2,自引:0,他引:2
对苯选择加氢制环己烯催化剂的研究,关键是选择性,这方面已经有不少文献报道[1,2],但具有工业应用价值的甚少。此外,载体也是影响环己烯选择性的一个重要因素。本文用化学还原法制备了Ru Co B/ZrO2催化剂,研究了助剂Co和载体ZrO2含量及还原剂对苯选择加氢制环己烯催化性能的影响。1 实验部分1 1 催化剂制备分别用KBH4和甲醛作还原剂,采用化学还原法制备出Ru Co B/ZrO2和Ru Co/ZrO2催化剂。其中RuCl3·xH2O和过渡金属Co盐分别作为活性组分和助剂的前体,纳米级ZrO2作分散剂,所得催化剂为黑色固体粉末。1 2 催化剂性能测试F… 相似文献
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用水热合成法制备了纳米Zr O2和Y2O3掺杂的Zr O2(Zr O2-Y),并考察了它们作载体对苯选择加氢制环己烯催化剂Ru-La-B/Zr O2性能的影响。结果表明,2种Zr O2具有相同微晶尺寸、织构性质和粒度分布。但Zr O2仅含有单斜相Zr O2,而Zr O2-Y不但含有单斜相Zr O2,还含有一部分四方相Zr O2。Y2O3掺杂影响Zr O2的组成和物相,进而影响用其制备催化剂的组成和物相。掺杂的Y2O3可以占据一部分不适宜苯加氢生成环己烯的活性位。因此,Zr O2-Y负载Ru-La-B催化剂活性明显低于Zr O2负载的,在低苯转化率下环己烯选择性前者比后者高。由于四方相Zr O2表面羟基比单斜相少,Zr O2-Y负载Ru-La-B催化剂的亲水性比Zr O2负载的差。环己烯不易从Zr O2-Y负载的催化剂表面脱附。当苯转化率高于52%时,Zr O2-Y负载的催化剂的环己烯选择性低于单斜相Zr O2负载的。Zr O2负载的Ru-La-B催化剂上20 min的环己烯收率达到了52.1%,而Zr O2-Y负载的环己烯收率仅45.2%。纳米单斜相Zr O2较适宜作苯选择加氢制环己烯Ru催化剂的载体。 相似文献
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聚酰胺生产新技术—苯不完全加氢制环己烯的开发研究 总被引:11,自引:0,他引:11
本文介绍并评述了由苯不完全加氢制环已烯这一聚酰胺生产的全新技术路线.通过与现存的工艺进行对比分析,阐述了它在工业生产上的巨大应用前景.对其关键步聚苯不完全加氢生成环己烯,从反应工艺、催化剂制备、反应机理及环己烯的分离与应用等几个方面,综述了其历史、现状和未来发展趋势. 相似文献
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蜂窝陶瓷整体反应器内苯选择加氢制环己烯 总被引:2,自引:0,他引:2
研究了Ru/ZrO2蜂窝陶瓷整体催化剂对苯液相选择加氢制环己烯反应的催化性能,考察了催化剂载体、活性组分含量、预处理条件、反应温度、反应压力、水和硫酸锌水溶液等对该反应的影响. 结果表明,整体催化剂不经预还原就可以直接进行苯液相加氢反应; 反应物中不加水或其它无机添加剂时环己烯的选择性为0,水或硫酸锌水溶液的加入大大降低了反应活性,但环己烯的选择性显著提高,约达到20%; 反应物中水和苯有最优配比,以保证最佳的环己烯选择性和收率; 反应温度在413~443 K,反应压力为3~4 MPa,硫酸锌浓度为0.1 mol/L时,反应结果较好. 相似文献
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采用共沉淀法制备了水溶性聚合物修饰的苯选择加氢制环己烯Ru-Zn催化剂, 并用X射线衍射、 透射电镜、 X射线能量色散谱、 X射线光电子能谱和氮气物理吸附等对加氢后催化剂进行了表征. 结果表明, 水溶性聚合物的种类和聚乙二醇-20000(PEG-20000)的用量对Ru-Zn催化剂微晶尺寸有显著影响. 在ZnSO4存在下, 随着Ru-Zn催化剂Ru微晶尺寸增加, 苯转化率降低, 环己烯最高收率则呈火山型变化趋势. 用0.4 g PEG-20000修饰的Ru-Zn催化剂[m(PEG-20000)∶m(Ru)=0.2]Ru的微晶尺寸为4.8 nm, 环己烯最高收率为62.2%. Ru微晶尺寸影响催化剂表面的Zn/Ru原子比, 进而影响Ru-Zn催化剂性能. 相似文献
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纳米 ZrO2 作分散剂的 Ru-Zn 催化剂上苯选择加氢制环己烯 总被引:2,自引:0,他引:2
采用水热法合成了比表面积分别为 34 和 87 m2/g 的 ZrO2 样品 (分别记为 ZrO2-34 和 ZrO2-87), 并考察了它们作分散剂时 Ru-Zn 催化剂上苯选择加氢制环己烯反应的性能. 结果表明, 两个 ZrO2 样品具有相近的纯度和物相, 晶粒粒径分别为 21.6 和 11.4 nm. 其中 ZrO2-34 具有较小的比表面积、较大的孔径、较小的粒径、集中的粒度分布和较大的堆密度, 因而更适合用作苯选择加氢制环己烯 Ru-Zn 催化剂的分散剂, 且循环使用多次催化剂仍表现出较高的选择性和稳定性. 相似文献
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Solvent extraction studies have been made on some metals: In/III/-Tl/III/ and Hg/II/-Cd/II/-Co/II/, from ammonium thiocyanate solutions by dialkyl sulphoxides. Separation of these metals from one another can be achieved by suitable choice of the extracted conditions. The nature of the extractable metal species has been elucidated. 相似文献
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Synthesis of chlorobis/β-diketonato/oxotechnetium/V/ and tris/β-diketonato/technetium/III/ complexes
K. Hashimoto Y. Yamada T. Omori K. Yoshihara 《Journal of Radioanalytical and Nuclear Chemistry》1989,135(3):187-197
Chlorobis/-diketonato/ oxotechnetium/V/ complexes [TcOCl/-dik/2, -diketone=acetylacetone, benzoylacetone and dibenzoylmethane] were newly synthesized using macroamount of99Tc. These complexes were further separated into geometrical isomers. Furthermore, an improvement of the yields for the syntheses of tris/-dike-tonato/technetium/III/ complexes [Tc/-dik/3, -diketone=acetylacetone, benzoylacetone and 2-thenoyltrifluoroacetone] was examined using Tc/III/-thiourea complexes as a starting material. 相似文献
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The crystal structure of trisodium monophosphate hemihydrate was determined. The space group is and a unit cell contains eight formula units. The unit cell dimensions of are a = 9.631(3), b = 5.416(2), c = 16.938(8) Å, β = 102.60(5)°. The final R value is 0.027 for a set of 1430 independent reflections. This atomic arrangement is mainly a three-dimensional network of distorted NaO6 octahedra. The hydrogen bonding scheme is given. 相似文献
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Summary Single reverse water-gas shift (RWGS) and dehydrogenation of propane with CO2(DH-CO2) reactions in the presence and absence of the CrOx/SiO2 catalyst have been studied between 673 and 873 K. It was found that the CrOx/SiO2 catalyst is active both in the dehydrogenation of propane and in the RWGS reactions. The obtained results suggest that the
dehydrogenation of propane to propene in the presence of CO2on CrOx/SiO2can be facilitated by the RWGS reaction.</o:p> 相似文献
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Summary CexTi1-xO2 and H3PW12O40/CexTi1-xO2 catalysts were prepared using a sol-gel method, and applied to the direct synthesis of dimethyl carbonate from methanol and
carbon dioxide. H3PW12O40/CexTi1-xO2 showed a better catalytic performance than the corresponding CexTi1-xO2, due to the bifunctional catalysis of Br?nsted acid sites (provided by H3PW12O40) and base sites (provided by CexTi1-xO2). H3PW12O40/Ce0.1Ti0.9O2 showed the highest catalytic performance among the H3PW12O40/CexTi1-xO2 catalysts. 相似文献
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Ninh Nguyen Jacques Choisnet Maryvonne Hervieu Bernard Raveau 《Journal of solid state chemistry》1981,39(1):120-127
Oxygen defect K2NiF4-type oxides have been synthesized for a wide composition range: 0 ≤ x ≤ 1.34. From the X-ray and electron diffraction study three domains have been characterized: orthorhombic compounds with La2CuO4 structure for 0 ≤ x < 0.10, tetragonal oxides similar to LaSrCuO4 for 0.10 ≤ x < 1 and several superstructures derived from the tetragonal cell ( with n = 3, 4, 4.5, 5, 6) for 1 ≤ x ≤ 1.34. The compounds corresponding to 0 < x < 1 differ from the other oxides in that they are characterized by the presence of copper with two oxidation states: + 2 and + 3. A model structure for La0.8Sr1.2CuλO3.4, in which copper has only the + 2 oxidation state, and for which the actual cell is tegragonal—a = 18.804 Å and c = 12.94 Å—has been established. The particular structural evolution of these compounds is discussed in terms of a competition between the capability of Cu(II) to be oxidized to Cu(III) and the ordering of oxygen vacancies. 相似文献
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Grisel Corro Odilón Vázquez-Cuchillo Fortino Ba?uelos 《Reaction Kinetics and Catalysis Letters》2005,87(1):171-175
Summary A strong promoting effect of the presence of C3H8or C3H6was determined for the combustion of CH4in excess oxygen, over pre-sulfated 1%Pt/g-Al2O3and pre-sulfated 1%Pt-2%Sn/g-Al2O3catalysts.</o:p> 相似文献
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P.P. Edwards R.G. Egdell I. Fragala J.B. Goodenough M.R. Harrison A.F. Orchard E.G. Scott 《Journal of solid state chemistry》1984,54(2):127-135
HeI-excited valence-band ultraviolet photoelectron spectra and MgKα-excited Ti-2p X-ray photoelectron spectra are reported for the spinel materials LiTi2O4 and . The presence of a Fermi edge in the ultraviolet photoelectron spectrum of LiTi2O4 confirms the metallic nature of this material, although the measured density of states at the Fermi energy is much lower than that expected from an independent-electron interpretation of the magnetic susceptibility. This difference is attributed to a strong interaction of the conduction electrons with the lattice vibrations. The localization of conduction electrons that occurs in the final state in the Ti-2p X-ray photoelectron spectrum of LiTi2O4 is attributed to a Coulomb interaction with a core hole. 相似文献
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A series of single-phase LixNi0.8-yCo0.2ZnyOp(0.96 ≤x≤ 1.10, 0 ≤y≤ 0.05, 2 ≤p≤ 2(1+y) ) (different in the y values) were synthesized by a two-step solid state reaction method, in which LiOH·H2O, Zn-doped spherical Ni(OH)2 and Co2O3 were used as the precursors. The ICP-AES analyses proved that the Zn-doped compounds synthesized had the nonstoichiometric form. The results of the XRD, SEM identified that the uniform particles of the as-prepared materials having a good layered structure were fine, narrowly distributed and well crystallized. The electrochemical performance test was carried out and the results showed that the as-prepared Zn-doped materials had not only a high capacity, but also a better cycling stability characterization than the un-doped one. The Li1.06Ni0.75Co0.22Zn0.03O2.03 material has an initial reversible capacity as high as 160.5mAh·g-1; and a first discharge efficiency 89.2%, and exhibits satisfactory cyclic stability with 90% retainable capacity after 50 cycles. 相似文献
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Mónica Martos Beatriz Julián Eloisa Cordoncillo 《Journal of solid state chemistry》2007,180(2):679-687
Doped-rutile has been traditionally used in ceramic pigments for its intense optical properties. In this paper, we compare the classical ceramic synthesis of Ti1−2xNbxNixO2−x/2 system with the sol-gel methodology, which allows a reduction of the anatase-rutile transformation temperature. The composition was optimised in order to obtain a unique rutile phase with the minimum amount of pollutant Ni(II) and enhanced chromatic coordinates. Incorporation of the doping ions in the rutile structure was corroborated by XRD and Rietveld refinements. The species responsible for the colour mechanism were studied by different techniques. UV-VIS spectroscopy showed the characteristic features of Ni2+ ions, whose existence was corroborated by EPR and magnetic measurements. From these results, (Ni,Nb)doped-TiO2 powder samples can be now shaped as thin films, monoliths, etc. by using sol-gel methodology without modifying their properties. This study introduces new possibilities of coloured TiO2-based solid solutions in new combined advanced applications (colouring agent and photocatalyst, etc.). 相似文献