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1.
This review covers the results obtained in carbon nanotube synthesis by chemical vapor deposition. Parameters such as catalysts, supports, carbon precursors, reaction time, temperature and gas flow rates that are used in the production of carbon nanotubes are discussed throughout the text. Purification of the synthesized carbon nanotubes and methods utilized for cost reduction were also explored.  相似文献   

2.
Since the 1970s, palladium-catalysed carbon–carbon (C–C) bond formation has made a critical impact in organic synthesis. In early studies, homogeneous palladium catalysts were extensively used for this reaction with limitations such as difficulty in separation and recycling ability. Lately, heterogeneous palladium-based catalysts have shown promise as surrogates for conventional homogeneous catalysts in C–C coupling reactions, since the product is easy to isolate, while the catalyst is reusable and hence sustainable. Recently, a better part of these heterogeneous palladium catalysts are supported on carbon nanotubes (Pd/CNTs), that have shown superior catalytic performance and better recyclability since the CNT support imparts stability to the palladium catalyst. This review discusses the wide variety of surface functionalization techniques for CNTs that improve their properties as catalyst supports, as well as the methods available for loading the catalyst nanoparticles onto the CNTs. It will survey the literature where Pd/CNTs catalysts have been utilized for C–C coupling reactions, with particular emphasis on Suzuki–Miyaura and Mizoroki–Heck coupling reactions. It will also highlight some of the important parameters that affect these reactions.  相似文献   

3.
Taguchi's robust design method is for the first time employed to optimize many aspects of the production of nanohybrids based on C nanotubes by iron-catalyzed chemical vapor deposition in i-C4H10 + H2 atmosphere. By analyzing the outcomes of the catalytic process in terms of selectivity, carbon yield, purity and crystalline arrangement of the hybrid-forming nanotubes, the influence is ranked of the following parameters: synthesis temperature (500-700 degrees C), support material (alumina, magnesia or sodium-exchanged montmorillonite), calcination- (450-750 degrees C) and reduction-(500-700 degrees C) temperatures of the 15 wt% Fe-catalyst. In the experiments initially performed for this purpose, the growth process had, on average, scarce selectivity (2 in a scale 1-5) and poor yield (130 wt%); carbonaceous deposits exhibited unsatisfactory graphitization degree (Raman D/G intensity ratio > 1.5) and contained large amounts of metal impurities (14 wt%) and amorphous carbon (5 wt%). The indications emerging from Taguchi approach to the process optimization are critically examined. The experimental conditions chosen for carrying out test experiments allow achieving excellent selectivity (5) or large yield (760 wt%), hybrids with well-graphitized nanotubes (D/G intensity ratio < 0.6), nearly free of metallic (0.3 wt%) or amorphous (0.4 wt%) inclusions, with consequent possibility of satisfying the different requisites that the specific application to be addressed may require.  相似文献   

4.
This work reports on the syntheses of one-dimensional (1D) H2Ti3O7 materials (nanotubes, nanowires and their mixtures) by autoclaving anatase titania (Raw-TiO2) in NaOH-containing ethanol-water solutions, followed by washing with acid solution. The synthesized nanosized materials were characterized using XRD, TEM/HRTEM, BET and TG techniques. The autoclaving temperature (120-180 degrees C) and ethanol-to-water ratio (V(EtOH)/V(H2O) = 0/60 approximately 30/30) were shown to be critical to the morphology of H2Ti3O7 product. The obtained H2Ti3O7 nanostructures were calcined at 400-900 degrees C to prepare 1D-TiO2 nanomaterials. H2Ti3O7 nanotubes were converted to anatase nanorods while H2Ti3O7 nanowires to TiO2(B) nanowires after the calcination at 400 degrees C. The calcination at higher temperatures led to gradual decomposition of the wires to rods and phase transformation from TiO2(B) to anatase then to rutile. Photocatalytic degradation of methyl orange was conducted to compare the photocatalytic activity of these 1D materials. These 1D materials were used as new support to prepare Au/TiO2 catalysts for CO oxidation at 0 degrees C and 1,3-butadiene hydrogenation at 120 degrees C. For the CO oxidation reaction, Au particles supported on anatase nanorods derived from the H2Ti3O7 nanotubes (Au/W-180-400) were 1.6 times active that in Au/P25-TiO2, 4 times that in Au/Raw-TiO2, and 8 times that on TiO2(B) nanowires derived from the H2Ti3O7 nanotubes (Au/M-180-400). For the hydrogenation of 1,3-butadiene, however, the activity of Au particles in Au/M-180-400 was 3 times higher than those in Au/W-180-400 but similar to those in Au/P25-TiO2. These results demonstrate that the potential of 1D-TiO2 nanomaterials in catalysis is versatile.  相似文献   

5.
The catalytic oxidation of toluene was studied over an iron-based spent and regenerated catalysts. Air, hydrogen, or four different acid solutions (oxalic acid (C2H2O4), citric acid (C6H8O7), acetic acid (CH3COOH), and nitric acid (HNO3)) were employed to regenerate the spent catalyst. The properties of pretreated spent catalyst were characterized by the Brunauer Emmett Teller (BET), inductively coupled plasma (ICP), temperature programmed reduction (TPR), and X-ray diffraction (XRD) analyses. The air pretreatment significantly enhanced the catalytic activity of the spent catalyst in the pretreatment temperature range of 200-400 degrees C, but its catalytic activity diminished at the pretreatment temperature of 600 degrees C. The catalytic activity sequence with respect to the air pretreatment temperatures was 400 degrees C>200 degrees C>parent>600 degrees C. The TPR results indicated that the catalytic activity was correlated with both the oxygen mobility and the amount of available oxygen on the catalyst. In contrast, the hydrogen pretreatment had a negative effect on the catalytic activity, and toluene conversion decreased with increasing pretreatment temperatures (200-600 degrees C). The XRD and TPR results confirmed the formation of metallic iron which had a negative effect on the catalytic activity with increasing pretreatment temperature. The acid pretreatment improved the catalytic activity of the spent catalyst. The catalytic activity sequence with respect to different acids pretreatment was found to be oxalic acid>citric acid>acetic acid>or=nitric acid>parent. The TPR results of acid pretreated samples showed an increased amount of available oxygen which gave a positive effect on the catalytic activity. Accordingly, air or acid pretreatments were more promising methods of regenerating the iron-based spent catalyst. In particular, the oxalic acid pretreatment was found to be most effective in the formation of FeC2O4 species which contributed highly to the catalytic combustion of toluene.  相似文献   

6.
Nanocomposites containing FeCo alloy nanoparticles dispersed in a highly ordered 3D cubic Im3m mesoporous silica (SBA-16) matrix were prepared by a novel, single-step templated-assisted sol-gel technique. Two different approaches were used in the synthesis of nanocomposites; a pure SBA-16 sample was also prepared for comparison. Low-angle X-ray diffraction, transmission electron microscopy and N2 physisorption at 77 K show that after metal loading, calcination at 500 degrees C and reduction in H2 flux at 800 degrees C the nanocomposites retain the cubic mesoporous structure with pore size not very different from the pure matrix. X-ray absorption fine structure (EXAFS) analysis at Fe and Co K-edges demonstrates that the FeCo nanoparticles have the typical bcc structure. The final nanocomposites were tested as catalysts for the production of carbon nanotubes by catalytic chemical vapour deposition and high-resolution TEM shows that good quality multi-walled carbon nanotubes are obtained.  相似文献   

7.
Highly ordered carbon nanotubes (CNTs) are wildly pursued due to their unique properties. Anodic aluminum oxide (AAO) exhibits great possibility for this purpose. Here, CNTs based on AAO template were produced using acetylene or ethylene as the hydrocarbon sources with or without the presence of Co catalysts. CNTs grown on the Co-embedded AAO samples were normally confined within the nanopores of the AAO template. It was found that C2H4 normally requires 100 degrees C higher pyrolysis temperature than C2H2 under otherwise identical conditions. The pyrolysis temperature is greatly reduced with the presence of Co catalysts. CNTs can grow out of the nanopores, if Co particles are present at the bottom of the nanopores and if the nanopores are short in length or large in diameter. The graphitization of AAO template grown CNTs was studied by Raman spectroscopy. The CNTs produced from ethylene are generally better in graphitization than those from acetylene, and the CNTs grown with the presence of Co catalysts deposited at the bottom of nanopores are better than those without Co catalysts or with Co catalysts coated on the entire inner wall of nanopores. The growth temperature is found not to play a critical role in graphitization.  相似文献   

8.
An effective method of growth by catalytic chemical vapor deposition (CCVD) to get a large-scale yield of carbon nanotubes is reported. In this method, acetylene is decomposed catalytically over well-dispersed metal particles (Co-Fe and Co-Ni) embedded in commercially available zeolite at a lower temperature (600-700 degrees C). The two binary-metal catalysts (Co-Fe and Co-Ni) used are compared by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Crucial reaction parameters, such as reaction time, temperature, and the effect of purity of gas to obtain optimum production of the nanotubes, both qualitatively and quantitatively, are also reported.  相似文献   

9.
Highly ordered carbon nanotubes (CNTs) are widely pursued due to their unique properties. Anodic aluminum oxide (AAO) exhibits great possibility for this purpose. Here, CNTs based on AAO templates were produced using acetylene or ethylene as the hydrocarbon sources with or without the presence of Co catalysts. CNTs grown on the Co-embedded AAO samples were normally confined within the nanopores of the AAO template. It was found that C2H4 normally requires 100 degrees C higher pyrolysis temperature than C2H2 under otherwise identical conditions. The pyrolysis temperature is greatly reduced with the presence of Co catalysts. CNTs can grow out of the nanopores if Co particles are present at the bottom of the nanopores, and if the nanopores are short in length or large in diameter. The graphitization of AAO-template grown CNTs was studied by Raman spectroscopy. CNTs produced from ethylene are generally better in graphitization than those from acetylene, and CNTs grown with the presence of Co catalysts deposited at the bottom of nanopores are better than those without Co catalysts or with Co catalysts coated on the entire inner wall of nanopores. The growth temperature is found not to play a critical role in graphitization.  相似文献   

10.
So far carbon nanotubes grown from the method most common method at present, that is, pyrolysis of ferrocene, invariably contains Fe inclusion. In addition, they are generally grown in random configurations. In the present investigations CNTs without Fe inclusion and in aligned configurations have been prepared by the pyrolysis of ferrocene (C10H10Fe) as well as pyrolysis of ferrocene in the presence of ethylene (C2H4). This has been achieved through optimization of growth parameters, for example, heating rate of ferrocene, pyrolysis temperature, and flow rates of carrier gas argon (Ar) and ethylene (C2H4). The as-synthesized samples have been characterized by transmission and scanning electron microscopic techniques. The optimum results relating to synthesis of carbon nanotubes without Fe inclusion and in aligned configurations have been obtained at 1000 degrees C pyrolysis temperature under flow rates of Ar of approximately 1000 sccm and of C2H4 of approximately 100 sccm. These carbon nanotubes have been found to have an outer diameter between approximately 20 and 60 nm and lengths between approximately 15 and 20 microns.  相似文献   

11.
Vertically aligned carbon nanotubes are synthesized by Low Pressure Chemical Vapor Deposition (LPCVD) on Si substrate coated with Fe as a catalyst at a pressure of 20 Torr and at a growth temperature of 600 degrees C. The catalyst film is prepared by electro-chemical method which is very unique and a low cost method. Three precursor gases Acetylene (C2H2), Ammonia (NH3) and Hydrogen (H2) at the flow rate of 20 sccm, 100 sccm and 100 sccm respectively are allowed to flow through the Low Pressure Chemical Vapor Deposition reactor for 10 minutes. Scanning Electron Microscope (SEM) images show that synthesized CNTs are vertically aligned and uniformly distributed with a high density. Raman analysis shows G-band at 1574 cm(-1) and D-band at 1370 cm(-1). The G-band is higher than D-band, which indicates that CNTs are highly graphitized. The field emission measurement reveals good field emission properties of as-grown vertically aligned carbon nanotubes with turn-on field of 1.91 V/microm at the current density 10 mA/cm2. The field enhancement factor is calculated to be 7.82 x 10(3) for as-grown carbon nanotubes.  相似文献   

12.
Taguchi method, extensively applied for the optimization of multifactor processes in the most diverse fields, is for the first time applied to the synthesis of hybrids based on C nanotubes by iron-catalyzed chemical vapor deposition in 1:1 i-C4H10 + H2 atmosphere. For this purpose, assumed synthesis-temperature (500 °C, 600 °C or 700 °C), support-material (alumina, magnesia or Na+-exchanged K10 montmorillonite), calcination (450 °C, 600 °C or 750 °C) and reduction (500 °C, 600 °C or 700 °C) temperature of the iron catalysts as the four factors of importance in the process, nine suitably designed experiments are conducted and the influence is evaluated of the four three-level factors on the issue of the process in terms of selectivity toward nanotubes, catalytic yield and content of carbonaceous and metallic impurities in the C nanotubes. By this procedure, the configurations giving optimal results are predicted, and tested by carrying out new experiments.  相似文献   

13.
This study aimed to prepare and characterise titanium dioxide (TiO2) nanoparticles and titanate nanotubes produced from Ti-sat flocculated sludge with drinking water (DW) and seawater (SW). The Ti-salt flocculated sludge from DW and SW was incinerated at 600 degrees C to produce TiO2 nanoparticles. XRD results showed that the anatase TiO2 structure was predominant for TiO2 from DW (TiO2-DW) and TiO2 from SW (TiO2-SW), which were mainly doped with carbon atoms. Titanate nanotubes (tiNT) were obtained when TiO2-DW and TiO2-SW were hydrothermally treated with NaOH solution. Structure phase, shape, crystallisation and photocatalytic activity of tiNT were affected by the incineration temperature and the amount of sodium present in different tiNT. The tiNT doped with thiourea incinerated at 600 degrees C presented anatase phase, showing a high increase of the degree of crystallisation with nanotube-like structures. The photocatalytic activity of these photocatalysts was evaluated using photooxidation of gaseous acetaldehyde. Thiourea doped tiNT-DW and tiNT-SW showed similar photocatalytic activity compared to commercially available TiO2-P25 under UV light and indicated a photocatalytic activity under visible light.  相似文献   

14.
Gold catalysts supported on ceria and ceria-alumina were studied in NOx reduction by CO. Gold was loaded using deposition-precipitation method. The ceria-alumina (20 wt% alumina) support was synthesized by co-precipitation. The average size of gold and ceria nano-particles was bellow 10 nm. It was established that the type of pretreatment do not have a substantial effect on the catalytic activity. The presence of O2 in the feed leads to a high conversion of CO to CO2 but no NO conversion was registered. Both NO and CO conversion was increased adding H2 to the feed. The catalytic activity became higher upon adding higher amount of H2. Supplementary to the main reaction parallel reactions took place. Bellow 200 degrees C N2O formation and at 250 degrees C and above the NH3 formation was detected. At around 200 degrees C it was established 100% selectivity to N2. The addition of water to the feed influenced positively the CO conversion and did not influence negatively the conversion of NO. The selectivity to N2 at around 200 degrees C remained 100% independent of the presence of moisture. Alumina in the mixed support prevents the sintering of both gold and ceria nano-particles. The results obtained make the catalysts containing gold supported on ceria-alumina promising for practical application.  相似文献   

15.
We report the synthesis of composite nanoparticles by an integrated CVS/CVD process at atmospheric pressure. Iron oxide and silica support particles were generated by chemical vapour synthesis (CVS), using Fe(CO)5 and Si(OC2H5)4 and were directly coated in the aerosol state with molybdenum oxide by chemical vapour deposition of Mo(CO)6. Depending on the CVS temperature hematite (600 degrees C) or maghemite (1500 degrees C) iron oxide phases were determined by XRD and FTIR. Core-shell structures with a coating thickness in the lower nm range were obtained for CVD temperatures below 150 degrees C. Complete encapsulation of the core particles and uniform elemental distribution is shown by TEM and EELS measurements. Higher CVD temperatures lead to unwanted homogenous decomposition of the molybdenum precursor. Additional aerosol temperature treatment was used to reach further oxidation and the formation of a mixed oxide shell, indicated by FTIR measurements. The results show the potential of the process for the synthesis of structured core-shell nanoparticles.  相似文献   

16.
A series of potassium-promoted hydrotalcite-based CoMgAlO mixed oxide catalysts used for simultaneous soot combustion and nitrogen oxides storage were prepared by impregnation method. The techniques of TG/DTA, XRD, H2-TPR and in situ DRIFTS were employed for catalyst characterization. Over the catalyst containing 7.5% or 10% K, the soot ignition temperature (Ti=260 degrees C) and total removal temperature (Tf=390 degrees C) are decreased by 180 degrees C and 273 degrees C, respectively, as compared with the uncatalyzed reaction. The results of kinetic calculation show that the presence of K-promoted catalysts decreases the activation energy of soot combustion from 207kJ/mol to about 160kJ/mol. When 400ppm NO is introduced, lower characteristic temperatures or higher reaction rate for soot oxidation is achieved. Simultaneously, relatively larger nitrogen oxides storage capacity is obtained. It is revealed by H2-TPR that the addition of K increases the amount of active Co sites and the mobility of bulk lattice oxygen due to the low melting point of K-containing compounds, the low valence of K+ and the strong interaction between K and Mg(Al). For nitrogen oxides storage, different routes via chelating bidentate nitrates, monodentate nitrates and ionic nitrates are confirmed by in situ DRIFTS over the CoMgAlO catalysts with potassium loadings of 0, 1.5 and 7.5%, respectively.  相似文献   

17.
The raw materials, condition and the method of preparing the catalysts play an important role in the growth of high quality Carbon Nanotubes by Catalytic Chemical Vapor Deposition method. In this work, the efficiency of Carbon Nanotubes growth was increased by a simple controlled preheating of the catalyst in N2 atmosphere. Supports were prepared by mixing alumina powder with tetraethyl orthosilicate (TEOS) by a chemical method at low temperature. Afterwards, the supports were impregnated with iron. The dried and ground catalyst was heated in N2 atmosphere at 500 degrees C for 1 hour followed by cooling down to room temperature. Methane was passed over the prepared catalyst bed at 900 degrees C. Supports, supported catalysts and Carbon Nanotubes samples have been characterized by Transmission Electron Microscopy, Scanning Electron Microscopy, Gas Adsorption/Desorption Analysis, X-Ray Diffraction and Raman Spectroscopy. Scanning Electron Microscopy images of the nanotubes showed a drastic increase in the growth rate, length and straightness of the Nanotubes in comparison to the growth without preheating and even preheating in air atmosphere. Raman Spectroscopy of the samples and Transmission Electron Microscopy pictures showed bundles, mostly equi-diameter Single Wall Nanotubes. In fact, the growth rate, length, and purity of the Nanotubes, also the homogeneity of the tubes improved. The conclusion can be made with the help of proposed theory of nucleation and growth of Nanotubes based on comparative results of the characterizations with and without preheat-treatment. It seems that the preheat-treatment in N2 affected the catalyst structure and its interaction with support as well as distribution of the catalyst particles on the support. These changes in return affect the quality and quantity of final production.  相似文献   

18.
纳米碳管是一种性能优异的新型功能材料.利用循环失效后的AB5型贮氢合金电极材料作为反应催化剂、乙炔气体作为原料气体通过CVD法制备出多壁纳米碳管,研究了经过破碎、清洗、氧化处理后的失效AB5型贮氢合金电极材料在合成纳米碳管中的催化性能,讨论了不同氧化温度处理催化剂对纳米碳管产率、形貌和结构稳定性的影响.结果表明,氧化处理温度对催化剂的催化效能有明显的影响,600℃为最佳氧化处理温度.以氧化处理后的失效AB5型贮氢合金电极材料作为催化剂制备碳纳米管,方法简单易行,为废旧镍氢电池负极材料的回收再利用提供了一种新的思路.  相似文献   

19.
以硝酸镍和正硅酸乙酯为原料,制得Ni(OH)2/SiO2二元胶体,经水热晶化法和常压干燥法分别合成了纳米级氧化镍-二氧化硅复合粉体催化剂}用这两种催化剂在相同催化裂解条件下分别制得了多壁碳纳米管;采用XRD和TEM等测试手段对两种催化剂物相、形貌及由两种催化剂制得的碳纳米管形态、收率及纯度作了比较,结果表明:水热晶化法比常压干燥法合成的催化剂粉体颗粒粒径小(为10~20nm),分散性好,催化活性高,使得所制得的碳纳米管管径小(为10~16nm)、分布窄、纯度和收率都相对较高;同时对用不同水热反应温度合成的催化剂(物相不同)制备碳纳米管进行了研究。  相似文献   

20.
Carbon nanostructures were synthesized by decomposition of different carbon sources over an alumina supported palladium catalyst via Chemical Vapor Deposition (CVD). Several experimental conditions were varied to verify their influence in the synthesis products: temperature ramping rate, pre-annealing conditions, hydrogen pre-treatment, synthesis temperature and time, together with the use of different carbon sources. Depending on the experimental conditions carbon nanotubes and nanofibers with different shapes and structural characteristics were obtained. Straight, coiled and branched morphologies are the most common. Among our findings, the addition of hydrogen plays a significant role in the structure of the carbonaceous products. For example, the decomposition of acetylene on palladium catalysts at 800 degrees C in the absence of hydrogen produces only carbon micro- spheres as synthesis products. The incorporation of increasing amounts of hydrogen modifies the outcome, from thick fibers to carbon nanotubes. To verify the level of graphitization of the synthesis products we have used high resolution transmission electron microscopy (HRTEM) in addition to Raman spectroscopy. Our results, based on these complementary techniques, indicate the decomposition of acetylene on a palladium based catalyst, produces the best degree of graphitization in carbon nanotubes for a temperature of 800 degrees C and 100 cc/min of hydrogen flow. Similar hydrogen flows on the same catalyst, produced highly graphitized nanofibers by the decomposition of methane at 850 degrees C.  相似文献   

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