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1.
A variety of barium sulfate （BaSO4） carriers with or without mesopore structure were synthesized via precipitation reaction in aqueous solution of barium hydroxide and sulfuric acid with ethylene glycol as a modifying agent, and then calcined at various temperatures. The obtained BaSO4 was used as catalyst carriers for polystyrene （PS） hydrogenation, and BaSO4 supported palladium （Pd） catalysts with Pd content of 5wt% were prepared by using impregnation method. N2 physisorption, transmission electron microscopy, X-ray diffraction and kinetics studies were used to investigate the effect of carrier structure on the dispersion and geometric location of active metal and their catalytic activities in PS hydrogenation. It was found that the pore structure of carrier played an important role in the dispersion and location of Pd grains. The activation energy values for all the Pd/BaSO4 catalysts were around 49.1 kJ/mol, while the pre-exponential factor for Pd/BSC-6H was much higher than others. The Pd/BSC-6H without mesopores had Pd grains deposited on the external surface of the carrier, and exhibited better activity than the mesoporous catalysts. It is indicated that the utilization of Pd/BSC-6H can reduce the pore diffusion of PS coils and enabled more active sites to participate in the PS hydrogenation.  相似文献   

2.
The synthesis of methanol and dimethyl ether (DME) from CO hydrogenation has been investigated on Cu-based catalysts. A series of Cu/ZnO/Al2O3 catalysts were prepared using a solvent-free routine which involved a direct blend of copper/zinc/aluminum salts and citric acid, followed by calcination at 450 °C. The calcination processes were monitored using thermogravimetry differential scanning calorimetry (TG-DSC). Catalysts were further characterized using N2 adsorption, scanning electronic microscopy (SEM), X-ray diffraction (XRD), N2O oxidation followed by H2 titration, and temperature-programmed reduction with H2 (H2-TPR). The reduction processes were also monitored with in-situ XRD. The physicochemical properties of catalysts depended strongly on the types of precursor salts, and catalysts prepared using Al acetate and Cu nitrate as starting materials had a larger surface area, larger exposed metallic copper surface area, and lower reduction temperature. The CO hydrogenation performances of these catalysts were compared and discussed in terms of their structures. Catalysts prepared with copper nitrate, zinc and aluminum acetates exhibited the highest catalytic activity.  相似文献   

3.
The thermolysis of urea-water solution and its product, HNCO hydrolysis is investigated in a dual-reactor system. For the thermal decomposition below about 1073 K, the main products are ammonia (NH3) and isocyanic acid (HNCO) whereas at higher temperatures the oxidation processes take effect and the products include a low concentration of nitric oxide (NO) and nitrous oxide (N2O). The gas HNCO is quite stable and a high yield of HNCO is observed. The ratio of NH3 to HNCO increases from approximately 1.2 to 1.7 with the temperature. The chemical analysis shows that H radical is in favor of HNCO hydrolysis by instigating the reaction HNCO+H·→·NH2+CO and high temperature has positive effect on H radical. The hydrolysis of HNCO over an alumina catalyst made using a sol-gel process (designated as γ-Al2O3) is investigated. The conversion of HNCO is high even at the high space velocities (6×105 h-1) and low temperatures (393–673 K) in the tests with catalysts, which enhances HNCO hydrolysis and raises the ratio of NH3 to HNCO to approximately 100. The pure γ-Al2O3 shows a better catalytic performance than CuO/γ-Al2O3. The addition of CuO not only reduces the surface area but also decreases the Lewis acid sites which are recognized to have a positive effect on the catalytic activity. The apparent activation energy of the hydrolysis reaction amounts to about 25 kJ/mol in 393–473 K while 13 kJ/mol over 473 K. The overall hydrolysis reaction rate on catalysts is mainly determined by external and internal mass-transfer limitations.  相似文献   

4.
Ultrafine γ-Al2O3 particles are synthesized in Triton X-100/n-hexanol/cyclohexane/water water in oil(w/o) microemulsion by mixing two separately prepared microemulsions containing Al(NO)3 and (NH4)2CO3 respectively. The ultrafine Al2O3 particles are characterized by transmission electron microscopy (TEM) and X-ray diffraction (XRD) and their size and distribution are measured. The effects of water, surfactant and reactant concentrations on the particle size and distribution are studied. The results show that the particle size and distribution can be changed by varying the preparation conditions, and the size of the microemulsion droplets has a controlling effect on the size of the particles. A possible mechanism of ultrafine particles (UFPs) prepared by microemulsions is proposed.  相似文献   

5.
在固定床反应器中研究了二甲基二硫醚对Ni/Al2O3上模拟裂解汽油原料油中主要化合物芳烃、单烯烃和共轭烯烃的加氢活性的影响。结果显示,二甲基二硫醚对以上化合物加氢抑制的顺序为:芳香环单烯烃共轭烯烃。通过XRD和XPS表征分析,推测了Ni/Al2O3催化剂失活的可能原因。  相似文献   

6.
In this article, we illustrated the preparation method of γ-Al2O3 ultrafine particles. The particle size and morphology were decided by a transmission electron microscopy (TEM) and crystal patterns were determined by an X-ray diffractometer (XRD). γ-Al2O3 ultrafine particles have ultra characters in physics and chemistry, and the hydrogen peroxide biosensors based on it display not only fast response and high sensitivity, but also good stability.  相似文献   

7.
Novel homo-dinuclear silicon bridged cyanoethyl cyclopentadienyl complexes of titanium and zirconium (CH3)2Si((η5 ? C5H3CH2CH2CN)(C5H5)MCl2)2(M = Ti(1), Zr(2)) were synthesized and developed for the polymerization of ethylene. Compared with their corresponding mononuclear complexes (η5 ? C5H4CH2CH2CN)(C5H5)MCl2(M = Ti(3), Zr(4)), the dinuclear complexes had higher catalytic activity. And the polyethylene produced had a higher molecular weight than that obtained with mononuclear catalysts. Effects of conditions on the ethylene polymerization catalyzed by (2)/MAO (methylaluminoxane) were studied in detail. The catalyst showed a very high activity (> 106 g PE/mol Zr·h) under low catalyst concentration and high molar ratio of Al/Zr.  相似文献   

8.
Activities of FeO in CaO-SiO2-Al2O3-MgO-FeO slags were determined at 1673 K by electrochemical of the solid electrolyte cell： Mo [Mo＋MoOu[ZrO2（MgO）[Fe＋（CaO-SiO2-Al2O3-MgO-FeO）＋Ag[Fe. The influences of slag compositions and basicity on FeO activities were analyzed. The results reveal that, for slags of fixed （%CaO）/（%SiO2） ratio, MgO and Al2O3 content, there was an increase of FeO activities with increase of FeO content. For slags with constant {（%CaO）＋ （%MgO）}/（%SiO2） ratio, fixed FeO and A1203 content, FeO activities decreased when MgO content increased from 5% to 10%, and increased with the increase of MgO content when it was over 10%. The FeO activities increased when （%CaO）/（%SiO2） ratio changed from 1.03 to 1.30 in the slags of constant MgO, FeO and Al2O3 content.  相似文献   

9.
The pure γ-Ca2SiO4 （]t-C2S） phase was prepared at 1623 K of calcining temperature, 10 h of holding time and furnace cooling. The 13-C2S phase was obtained through γ-C2S conversion with the following calcination system which was adopted at 1473 K of calcining temperature, 1 h of holding time and then water-cooling. The conversion rate of γ-C2S was studied by the Rietveld quantitative laboratory X-ray powder diffraction supported by synchrotron X-ray diffraction images. The refinement results show that the final conversion rate of γ-C2S is higher than 92%. The absolute error of the γ-C2S conversion rate between two Rietveld refinements （sample with or without α-Al2O3） is 3.6%, which shows that the Rietveld quantitative X-ray diffraction analysis is an appropriate and accurate method to quantify the γ-C2S conversion rate.  相似文献   

10.
An ecofriendly heterogeneous polyoxometalate (POM)-gold catalyst Au/BW11/Al2O3 was synthesized and used for solvent-free epoxidation of cyclooctene under mild reaction conditions using molecular oxygen as an oxidant and t-butyl hydroperoxide (TBHP) as an initiator. The catalyst was characterized by Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), energy dispersive X-ray analysis (EDX), X-ray diffraction (XRD), induced coupled plasma optical emission spectrometry (ICP-OES), and Brunauer-Emmett-Teller (BET). The catalyst showed good conversion and high selectivity without use of solvents or environmentally harmful oxidants. Moreover, the catalyst is recyclable up to three cycles with no significant loss in selectivity towards epoxide.  相似文献   

11.
Mg2Ni0.8Cr0.2-x wt.% CoO/Al2O3 (x=0.5, 1, 2 and 3) composites were prepared by mechanically milling sintered Mg2Ni0.8Cr0.2 alloy and CoO/Al2O3 compound for 45 h. The addition of CoO/Al2O3 compound resulted in the good kinetics properties of hydriding/dehydriding reaction of the composites. The composite with 1.0 wt.% CoO/Al2O3 catalyst could reach the maximum hydrogen absorption capacity (2.9 wt.%) within 5 min at 393 K under H2 pressure of 4 MPa, and can desorb rapidly at 493 K. The decomposition and synthesis of hydrogen molecule on Mg2Ni0.8Cr0.2 alloy surface was promoted by addition of CoO/Al2O3 catalyst. In addition, the formation of metallic Ni particles, strain and defects during the ball milling process also resulted in the improved hydrogenation performance of Mg2Ni-based alloys.  相似文献   

12.
INTRODUCTION Mg-based alloys are considered as potentialcandidates for hydrogen storage materials because oftheir large hydrogen capacity (Reilly and Wiswall,1968; Pedersen and Larsen, 1993). However, asMg-based alloys desorb hydrogen at temperatureshigher than 600 K, they are not applicable to practicaluse. Many researches have studied to improve hy-driding/dehydriding kinetics and to lower the workingtemperature (Wang et al., 2002; Tsushio et al., 1998;Spassov and K?ster, 1998; Orim…  相似文献   

13.
Using SnxTi1-xO2 as carriers, CuO/Sn0.9Ti0.1O2 and CuO/Sn0.7Ti0.3O2 catalysts with different loading amounts of copper oxide (CuO) were prepared by an impregnation method. The catalytic properties of CuO/Sn0.9Ti0.1O2 and CuO/Sn0.7Ti0.3O2 were examined using a microreactor-gas chromatography (GC) NO CO reaction system and the methods of BET (Brun- auer-Emmett-Teller), TG-DTA (themogravimetric and differential thermal analysis), X-ray diffraction (XRD) and H2-temperature programmed reduction (TPR). The results showed that NO conversions of Sn0.9Ti0.1O2 and Sn0.7Ti0.3O2 were 47.2% and 43.6% respectively, which increased to 95.3% and 90.9% at 6 wt% CuO loading. However, further increase in CuO loading caused a decrease in the catalytic activity. The nitrogen adsorption-desorption isotherm and pore-size distribution curve of Sn0.9Ti0.1O2 and Sn0.7Ti0.3O2 represented type IV of the BDDT (Brunauer, Deming, Deming and Teller) system and a typical mesoporous sample. There were two CuO diffraction peaks (2θ 35.5° and 38.7°), and the diffraction peak areas increased with increasing CuO loading. TPR analysis also detected three peaks (α, β and γ) from the CuO-loaded catalysts, suggesting that the α peak was the reduction of the highly dispersed copper oxide, the β peak was the reduction of the isolated copper oxide, and the γ peak was the reduction of crystal phase copper oxide. In addition, a fourth peak (δ) of the catalysts meant that the SnxTi1-xO2 mixed oxides could be reductive.  相似文献   

14.
利用浸渍法制备了Pd/Al2O3催化剂,采用X射线衍射(XRD)、透射电子显微镜(TEM)和X射线光电子能谱(XPS)研究了Pd在载体Al2O3中的分布状态和价态.结果表明纳米尺寸的Pd颗粒主要以单质形式高度分散在载体Al2O3上,部分呈氧化态.  相似文献   

15.
The copolymerization of CO and styrene catalyzed by Pd/C toward the formation of polyketones(PK)was studied in the N-valeronitrile-N'-methylimidazolium hexafluorophosphate([C4CNmim]+PF-6) medium. The synthesized PK was characterized by Fourier transform infrared(FTIR), elemental analysis, 13C-nuclear magnetic resonance(13C-NMR), differential scanning calorimetry(DSC), thermogravimetric analysis(TGA) and gel permeation chromatography(GPC). The supported ionic liquid film on the surface of Pd/C catalyst can prevent the products from covering the hole of active carbon due to its chemical stability and weak coordination ability with metal ions, and thus efficiently improve the catalytic activity. The effects of different amounts of ionic liquid on the catalytic activity and reusability of the catalyst and the molecular weight of PK were discussed. When the usage of ionic liquid is 10wt%(0.1 g ionic liquid / 1 g active carbon carrier) and the theoretical content of Pd2+ is 5wt%(0.05 g Pd2+/ 1 g active carbon carrier), the highest catalytic activity 2 963.64 gSTCO/(gPd·h) is achieved with the molecular weight and polydispersity index of PK as Mn=9 684, Mw=13 452 and Mw /Mn=1.389.  相似文献   

16.
In this study, we used a simple impregnation method to prepare Fe–Ce–O x catalysts and tested them regarding their low-temperature (200–300 °C) selective catalytic reduction (SCR) of NO using NH3. We investigated the effects of Fe/Ce molar ratio, the gas hourly space velocity (GHSV), the stability and SO2/H2O resistance of the catalysts. The results showed that the FeCe(1:6)O x (Ce/Fe molar ratio is 1:6) catalyst, which has some ordered parallel channels, exhibited good SCR performance. The FeCe(1:6)O x catalyst had the highest NO conversion with an activity of 94–99% at temperatures between 200 and 300 °C at a space velocity of 28,800 h?1. The NO conversion for the FeCe(1:6)O x catalyst also reached 80–98% between 200 and 300 °C at a space velocity of 204,000 h?1. In addition, the FeCe(1:6)O x catalyst demonstrated good stability in a 10-h SCR reaction at 200–300 °C. Even in the presence of SO2 and H2O, the FeCe(1:6)O x catalyst exhibited good SCR performance.  相似文献   

17.
The evolution of the surface oxide film along the depth direction of typical aluminum alloy under medium-temperature brazing was investigated by means of X-ray photoelectron spectroscopy （XPS）. For the alloy with Mg content below 2.0wt%, whether under cold rolling condition or during medium-temperature brazing process, the en-richment of Mg element on the surface was not detected and the oxide film was pure Al2O3. However, the oxide film grew obviously during medium-temperature brazing process, and the thickness was about 80 nm. For the alloy with Mg content above 2.0wt%, under cold rolling condition, the original surface oxide film was pure Al2O3. However, the Mg element was significantly enriched on the outermost surface during medium-temperature brazing process, and MgO-based oxide film mixed with small amount of MgAl2O4 was formed with a thickness of about 130 nm. The alloy-ing elements of Mn and Si were not enriched on the surface neither under cold rolling condition nor during medium-temperature brazing process for all the selected aluminum alloy, and the surface oxide film was similar to that of pure aluminum, which was almost entire Al2O3.  相似文献   

18.
采用溶胶凝胶法制备了Cu／SiO2催化荆,用浸渍法将Mg元素担载在Cu／SiO2催化荆制得Mg-Cu／SiO2催化荆,研究在NO＋CO反应中的催化活性．结果表明,Mg修饰的采用方法（c）制备的Cu／SiO2催化荆,当Cu的含量是载体SiO2质量的2％,Mg的含量是载体SiO2质量的3％时,Mg-Cu／SiO2催化荆活性最高,250℃时NO生成N2的转化率接近100％．  相似文献   

19.
Oxidative dehydrogenation (ODH) of mono and mixed-butenes to 1,3-butadiene (BD) was conducted using individual and dual bed catalyst systems, consisting of ZnFe2O4, Co9Fe3Bi1Mo12O51 or both. The dual bed catalyst system gave improved catalytic performance. A mechanism based on synergy between the catalysts is proposed to explain the improved overall butene conversion. The proportion of the reactants differed between the catalyst beds in the dual bed system, making better use of the catalytic activity of the second bed. The existence of all butene isomers inhibited isomerization, leading to a higher proportion of ODH reactions and thus improved the conversion of butene and the yield of BD. The packing sequences and the volume ratio of the catalysts in the bed were optimized. The results indicated that the sequence with ZnFe2O4 on top and a catalyst packing ratio of between 4:6 and 6:4 led to better activity.  相似文献   

20.
采用诱导法制备空心三元PdPtCu纳米材料,利用透射电镜(TEM)、扫描电镜(SEM)和X射线衍射(XRD)对其形貌、组成和结构进行表征,并在碱性条件下测试其对乙醇氧化的电催化性能。结果表明,以氧化铜为诱导剂制备的三元PdPtCu纳米材料主要呈空心结构,且其形貌和组成可控;Pd3Pt@Cu,PdPt@Cu和PdPt3@Cu三种材料的质量电流密度分别为8 510 A·g-1,9 270 A·g-1和5 490 A·g-1,无论是质量活性还是稳定性,均明显优于商业Pd/C和商业Pt/C催化剂。  相似文献   

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