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1.
《Comptes Rendus Chimie》2015,18(3):293-301
Dry reforming of methane has been carried out on SBA-15 catalysts containing 5 wt% Ni and 6 wt% Ce. The effect of the order of Ni and Ce impregnation on the catalytic activity has been studied. Both metals were added using the “two-solvent” method that favors metal dispersion inside the pores. Characterizations by XRD (low and high angles), N2 sorption, SEM and TEM of the materials after metal addition and calcination indicate good preservation of the porosities and high NiO and CeO2 dispersion inside the porous channels. Reduction was carried out before the catalytic tests and followed by TPR measurements. The most active reduced catalyst was the Ni–Ce/SBA-15 sample prepared by impregnating cerium first, then nickel. All catalysts were highly active and selective towards H2 and CO at atmospheric pressure. Full CH4 conversion was obtained below 650 °C. The higher performances compared to those reported in the literature for mesoporous silica with supported Ni and Ce catalysts are discussed. 相似文献
2.
As a typical volatile organic compound, toluene is a hazardous material for human health and the environment, and currently, the development of catalysts for its oxidation into CO2 and water is crucial. The series of Ag-CeO2/SBA-15 catalysts is synthesized by wetness impregnation techniques and characterized by a number of physical-chemical methods (nitrogen [N2] physisorption, small angle X-ray scattering [SAXS], transmission electron microscopy [TEM], and temperature-programmed reduction [TPR]). The toluene sorption and catalytic properties in toluene oxidation are studied. Small silver [Ag] and cerium oxide [ceria, CeO2] particles with sizes below 3 nm are predominantly formed in the ordered structure of Santa Barbara Amorphous-15 [SBA-15]. The interactions between the Ag and CeO2 nanoparticles are established. Temperature-programmed desorption of toluene [TPD-C7H8] analysis shows that physical adsorption of toluene occurs on pristine SBA-15 material, while the introduction of either silver or ceria to SBA-15 leads to the appearance of additional strongly bound chemisorbed toluene on such sites. When both Ag and CeO2 are introduced, only chemisorbed toluene is formed over the Ag-CeO2/SBA-15 catalyst, and the highest catalytic activity in toluene oxidation is observed over this catalyst (T98% = 233 °C, 0.2% C6H5CH3) that is attributed to the synergistic effect of ceria [CeO2] and silver [Ag]. 相似文献
3.
以SBA-15为载体,采用浸渍法制备了不同Ag含量的Ag/SBA-15,通过N2吸附-脱附、X射线衍射、扫描电子显微镜、高分辨透射电子显微镜、X射线光电子能谱和电感耦合等离子体质谱对催化剂进行了表征。将Ag/SBA-15用于苯甲醇气相选择性催化氧化合成苯甲醛,研究了反应条件对转化率和选择性的影响。结果表明,Ag/SBA-15具有均一的一维孔道结构、较厚的孔壁(3-5 nm)及较大的比表面积(411-541 m2/g),其规整纳米空间的限域作用使一定负载量的Ag以纳米尺寸均匀分散于介孔SBA-15孔道内,增加了活性组分的比表面积。亲核性氧物种从Ag到SBA-15表面的氧溢流,提高了低温下Ag/SBA-15对苯甲醇气相选择性氧化合成苯甲醛的催化性能。5.3% Ag/SBA-15中的Ag粒径为5-6 nm,且均匀分散于载体孔道中,反应温度为220℃时,苯甲醇转化率为87%,苯甲醛选择性为95%;240℃时,苯甲醇转化率和苯甲醛选择性分别高达94%和97%;并在240-300℃范围内,其催化活性和选择性保持不变,表现出了良好的温度耐受能力。催化剂经活化再生可以连续使用40 h,选择性基本保持不变。 相似文献
4.
《Comptes Rendus Chimie》2014,17(9):913-919
Different cobalt loadings (3, 6, 12, 24 wt%) were impregnated using the double-solvent technique on SBA-15 calcined at 500 °C presenting a high specific surface area. The impregnated solids were stabilized at 450 °C in the air. The impregnation of cobalt led to the incorporation of cobalt oxide nanoparticles in the mesoporosity of the SBA-15. The cobalt nanoparticles were easily reducible compared to similar solids prepared by different methods. The presence of these nanoparticles enhanced significantly the reactivity of the catalysts in the considered reaction. The addition of more than 12 wt% of cobalt did not enhance the catalytic reactivity due to the deposition of cobalt oxide species on the surface of the support. The cobalt-impregnated solids are efficient in decreasing the oxidation temperature of different probe molecules and are totally selective towards the formation of CO2 and H2O. 相似文献
5.
《Tetrahedron: Asymmetry》2005,16(21):3562-3569
Two immobilized chiral MnIII(salen) complexes covalently anchored on modified MCM-41 (50 Å) and SBA-15 (75 Å) were prepared using 3-aminopropyltriethoxysilane as a reactive surface modifier to afford comparable or even higher enantioselectivity than homogeneous catalysts for the enantioselective epoxidation of a series of smaller to bulkier alkenes. The catalyst immobilized in silica with larger pore diameters was found to be more active. Compared to homogeneous catalysts, the heterogenized catalysts are more stable and can be recycled four times with retention of enantioselectivity. 相似文献
6.
《Comptes Rendus Chimie》2015,18(3):358-367
Fe/SBA-15 catalysts containing iron oxide nanoparticles confined inside silica pores (replicated, internal, poorly crystalline) and grown outside silica grains (external, mainly crystalline hematite) in different proportions are prepared using a single silica support. Fe-species are deposited by the two-solvent technique with two iron salts precursors (Fe(NO3)3·9H2O, FeCl3·6H2O) and two solvents (cyclohexane, hexane) for 11 wt% of iron. Calcination is performed in reproducible conditions (700 °C, 2 °C/min, thin bed, in air). SAXS measurements are used to show that the 2D hexagonal structure of the used silica is maintained after Fe-loading and calcination. Ar sorption measurements show that the pores are partially plugged. The oxidation of pure methanol is used as a test reaction to compare photocatalytic properties. H2O2 and visible light both activate the reaction. More active catalysts are formed with hexane associated with FeCl3·6H2O than with Fe(NO3)3·9H2O. A reversed situation is observed with cyclohexane. Iron leaching (after 1 h 30 of test, up to 3 mg of Fe by mL) is important. These results are expected to be of interest in the exploration of size and shape “nanocatalysis” and to provide a further understanding for the reactions that take place when porous silicas are used as supports. 相似文献
7.
《Solid State Sciences》2012,14(2):250-257
CO2 adsorption properties on Mg modified silica mesoporous materials were investigated. By using the methods of co-condensation, dispersion and ion-exchange, Mg2+ was introduced into SBA-15 and MCM-41, and transformed into MgO in the calcination process. The basic MgO can provide active sites to enhance the acidic CO2 adsorption capacity. To improve the amount and the dispersion state of the loading MgO, the optimized modification conditions were also investigated. The XRD and TEM characteristic results, as well as the CO2 adsorption performance showed that the CO2 adsorption capacity not only depended on the pore structures of MCM-41 and SBA-15, but also on the improvement of the dispersion state of MgO by modification. Among various Mg modified silica mesoporous materials, the CO2 adsorption capacity increased from 0.42 mmol g−1 of pure silica SBA-15 to 1.35 mmol g−1 of Mg–Al–SBA-15-I1 by the ion-exchange method enhanced with Al3+ synergism. Moreover, it also increased from 0.67 mmol g−1 of pure silica MCM-41 to 1.32 mmol g−1 of Mg–EDA–MCM-41-D10 by the dispersion method enhanced with the incorporation of ethane diamine. The stability test by 10 CO2 adsorption/desorption cycles showed Mg–urea–MCM-41-D10 possessed quite good recyclability. 相似文献
8.
Synthesis of CuO/SBA-15 adsorbents for SOx removal applications,using different impregnation methods
《Comptes Rendus Chimie》2015,18(10):1013-1029
In this paper, SBA-15 mesoporous silica based adsorbents were synthesized for the desulfurization of flue gas streams, by several methods (wet impregnation, incipient wetness impregnation and ion exchange). The influence of the drying and calcination conditions on the porous texture and the dispersion of the active phase (CuO), as well as the efficiency of the adsorbents for SOx trapping, were studied. Depending on the synthesis conditions, copper species are present as large CuO particles (1 μm) and/or as homogeneously dispersed species, undetectable by XRD/TEM. The SOx adsorption efficiency seems to be closely related to the undetected copper species. 相似文献
9.
Miroslav Stanković Margarita Gabrovska Jugoslav Krstić Peter Tzvetkov Maya Shopska Tsenka Tsacheva Predrag Banković Rumeana Edreva-Kardjieva Dušan Jovanović 《Journal of molecular catalysis. A, Chemical》2009,297(1):54-62
Silver modified Mg-Ni/diatomite materials with ratios of SiO2/Ni = 1.07 and Mg/Ni = 0.1, differing in Ag content (Ag/Ni = 0.025 and 0.1) were prepared by the precipitation–deposition method. The effects of silver presence and content on the structure, morphology, texture and H2-adsorption capacity of the obtained precursors were studied by X-ray diffraction, scanning electron microscopy, Hg-porosimetry and H2-chemisorption techniques. The catalytic performance of the corresponding catalysts in the soybean oil hydrogenation was investigated. The increase of the silver loading resulted in the development of macroporosity and increase in the total sample porosity. The decrease of both H2-adsorption capacity and hydrogenation activity are related to the metallic silver covering and blocking effects on the Ni2+ species, thus hampering the access of hydrogen. The decrease of hydrogenation activity and favorable limiting of cis–trans isomerization on the silver modified catalyst are explained by Horiuti–Polanyi mechanism based on the assumption that hydrogenation and isomerization proceed at the same active metallic nickel sites via half-hydrogenated intermediates.It was shown that the adjustment of the catalyst composition by changing the content of silver modifier offers the possibility to control the total amount of solid fat content, stearic acid and detrimental trans fatty acids in the hydrogenated derivatives. The catalyst with higher silver content is proposed as a promising candidate for selective edible oil hydrogenation catalyst. 相似文献
10.
G. V. Mamontov V. V. Dutov V. I. Sobolev O. V. Vodyankina 《Kinetics and Catalysis》2013,54(4):487-491
The catalysts of silver supported on mesoporous silica modified with Co3O4, CeO2, and ZrO2 were prepared by an impregnation method; characterized by X-ray diffraction analysis, temperature-programmed reduction, and low-temperature nitrogen adsorption; and studied in a model reaction of CO oxidation. It was found that the Ag/SiO2 system exhibited high activity in the reaction of CO oxidation, and the addition of transition metal oxides led to reduction of the temperature of 50% CO conversion by 40°C. The modification of Ag/SiO2 with cerium dioxide was found most effective because of the interaction of silver particles and CeO2 on the surface of silica gel. 相似文献
11.
Yuanyuan Guo Limin Chen Ding Ma Daiqi Ye Bichun Huang 《Journal of Energy Chemistry》2013,22(4):591-598
Activated carbon (AC) supported silver catalysts were prepared by incipient wetness impregnation method and their catalytic performance for CO preferential oxidation (PROX) in excess H2 was evaluated. Ag/AC catalysts, after reduction in H2 at low temperatures (≤200 °C) following heat treatment in He at 200 °C (He200H200), exhibited the best catalytic properties. Temperature-programmed desorption (TPD), X-ray diffraction (XRD) and temperature-programmed reduction (TPR) results indicated that silver oxides were produced during heat treatment in He at 200 °C which were reduced to metal silver nanoparticles in H2 at low temperatures (≤200 °C), simultaneously generating the adsorbed water/OH. CO conversion was enhanced 40% after water treatment following heat treatment in He at 600 °C. These results imply that the metal silver nanoparticles are the active species and the adsorbed water/OH has noticeable promotion effects on CO oxidation. However, the promotion effect is still limited compared to gold catalysts under the similar conditions, which may be the reason of low selectivity to CO oxidation in PROX over silver catalysts. The reported Ag/AC-S-He catalyst after He200H200 treatment displayed similar PROX of CO reaction properties to Ag/SiO2. This means that Ag/AC catalyst is also an efficient low-temperature CO oxidation catalyst. 相似文献
12.
Seong-Eun Kim Ji Hyun Park Byung cheol Lee Jong-Chan Lee Yong Ku Kwon 《Radiation Physics and Chemistry》2012,81(8):978-981
Size-controlled large scale synthesis of silver nanoparticles was performed using Ag(I)–S12 inorganic-organic hybrid polymer with supramolecular structures though electron beam irradiation. The Ag(I)–S12 polymer was simply prepared by mixing dodecanethiol with the solution of silver salts. The silver nanoparticles with various sizes were prepared from Ag(I)–S12 polymer with an electron beam voltage from 0.3 MeV to 2 MeV, current from 0.06 mA to 0.48 mA, and/or irradiation time from 1 to 10 min. The morphology and chemical composition of the irradiated samples were characterized by transmission electron microscopy (TEM), and Fourier transform infrared spectroscopy (FT-IR). 相似文献
13.
Ag nanocubes that are 45 nm in size are synthesized and successfully used as catalysts in oxygen electroreduction. Electrochemical surface areas (ESAs) are considered to determine the effect on HO2− production, which is found to be in the following order: nanocubes < nanoparticles. Comparative data generated using Tafel analyses in 0.1 M NaOH electrolyte without and with methanol show that unchanged slopes on the prepared cubic catalysts can indicate high resistance of Ag nanocubes for methanol oxidation during oxygen reduction reaction. Among these Ag catalysts, nanocubes exhibit 9.29 × 10− 2 mA cm− 2 (at − 0.15 V vs. Ag/AgCl), the better activity in the oxygen reduction reaction. 相似文献
14.
Daniela Aiello Rosario Aiello Flaviano Testa Tonino Martino Iolinda Aiello Massimo La Deda Mauro Ghedini 《Journal of photochemistry and photobiology. A, Chemistry》2009,201(2-3):81-86
New luminescent inorganic–organic hybrid materials incorporating the luminescent zinc(II) complex ZnL2 (λem = 457 nm and Φem = 4.4% reference values for ZnL2; HL = chelating ligand resulting from the reaction between salicylaldehyde and 3-aminopropyltriethoxysilane), covalently bonded to different types of mesoporous silica hosts (namely MCM-41, MCM-48 and SBA-15), were prepared via both the methods of grafting post-synthesis (GPS) and one-pot synthesis (OPS). The products obtained, which form the GPS [(GPS)(Zn/MCM-41), (GPS)(Zn/MCM-48), (GPS)(Zn/SBA-15)] and the OPS [(OPS)(Zn/MCM-41), (OPS)(Zn/MCM-48), (OPS)(Zn/SBA-15)] series, contain the ZnL2 guest covalently bonded to the silica framework through silicon–oxygen bonds formed when the silane group is placed at the periphery of the Zn(II) coordination sphere. GPS and OPS materials were characterized by powder X-ray diffraction, N2 adsorption/desorption, thermogravimetric analysis (TGA) and UV/vis spectroscopy. For the new mesoporous materials the emission quantum yield (EQY) was measured by means of an integrating sphere combined with a spectrofluorimeter. The ZnL2 loading (measured by the ZnL2/SiO2 ratio calculated from TGA data) for MCM-41 appears to be independent of the synthesis procedure, whereas, for both MCM-48 and SBA-15, the ZnL2/SiO2 ratio of the materials obtained via OPS is about four times higher than products obtained from GPS. The ZnL2 loaded GPS and OPS series show λem maxima at about 485 and 455 nm, respectively. Moreover, with reference to EQY (GPS)(Zn/SBA-15) and (OPS)(Zn/SBA-15), although featuring ZnL2/SiO2 ratios of 0.13 and 0.45, respectively, they showed similar EQY values: 2% and 5%. On the contrary, (GPS)(Zn/MCM-41) and (OPS)(Zn/MCM-41) which give similar ZnL2/SiO2 ratios (0.09 and 0.14) exhibit very different EQY, i.e. 2% and 22%, respectively. 相似文献
15.
《Arabian Journal of Chemistry》2014,7(6):1192-1198
Nano-gold and silver particles supported on manganese oxide were synthesized by the co-precipitation method. The catalytic properties of these materials were investigated for the oxidation of benzyl alcohol using molecular oxygen as a source of oxygen. The catalyst was calcined at 300, 400 and 500 °C. They were characterized by electron microscopy, powder X-ray diffraction (XRD) and surface area. It was observed that the calcination temperature affects the size of the nanoparticle, which plays a significant role in the catalytic process. The catalyst calcined at 400 °C, gave a 100% conversion and >99% selectivity, whereas catalysts calcined at 300 and 500 °C gave a conversion of 69.51% and 19.90% respectively, although the selectivity remains >99%. 相似文献
16.
Min Su Jang Tuan Ngoc Phan Im Sik Chung In-Gu Lee Young-Kwon Park Chang Hyun Ko 《Research on Chemical Intermediates》2018,44(6):3723-3735
Catalytic hydrodeoxygenation (HDO) of anisole, a methoxy-rich lignin-derived bio-oil model compound, was carried out over a series of Ni-containing (5, 10, 20, and 30 wt%) catalysts with commercial silica and ordered mesoporous silica SBA-15 as support. Both supports and catalysts were characterized by N2 adsorption–desorption isotherms, X-ray diffraction, CO chemisorption, and transmission electron microscopy (TEM). Catalytic reaction was performed at 250 °C and 10 bar H2 pressure. Depending on the catalyst support used and the content of active metal, the catalytic activity and product distribution changed drastically. Increase of the nickel loading resulted in increased anisole conversion and C6 hydrocarbon (benzene and cyclohexane) yield. However, loading more Ni than 20 wt% resulted in a decrease of both conversion and C6 yield due to agglomeration of Ni particles. In addition, Ni/SBA-15 samples exhibited much stronger catalytic activity and selectivity toward C6 hydrocarbon products compared with Ni/silica catalysts. The differences in catalytic activity among these catalysts can be attributed to the effect of the pore size and pore structure of mesoporous SBA-15. SBA-15 can accommodate more Ni species inside channels than conventional silica due to its high pore volume with uniform pore structure, leading to high HDO catalytic activity. 相似文献
17.
Nanostructured PtRu material has been successively synthesized via chemical co-reduction of hexachloroplatinic acid and ruthenium trichloride using three-dimensional (3D) hexagonal mesoporous SBA-12 silica as a solid template, and has been studied as an electrocatalyst toward methanol electro-oxidation. The ordered nanostructure of the PtRu particles has been disclosed by transmission electron micrographs and is characterized by regular pores of ca. 3.0 ± 0.3 nm in diameter separated by walls of ca. 3.0 ± 0.3 nm thick. X-ray diffraction and energy dispersive X-ray spectroscope studies indicate that the PtRu material comprises of complicated phases rather than a single alloy phase of Pt and Ru. The specific electrochemical surface area of the nanostructured powder measured using both CO and underpotential deposited Cu stripping techniques is 74–78 m2 g–1, higher than that of unsupported precious metal catalysts prepared using standard techniques. The combination of high surface area and periodic nanostructure of the templated PtRu makes it an interesting promising fuel cell electrocatalyst. This has been demonstrated by the high activity of the templated PtRu towards the methanol electrooxidation. Therefore the solid template route based on 3D mesoporous silica with controlled pore size and high pore interconnectivity provides an interesting alternative to produce promising high-surface-area electrode materials. 相似文献
18.
Immobilized enzymes have an advantage over enzymes free in solution in that they are easily recovered after completed reaction. In addition, immobilization often gives enhanced stability. Entrapment of an enzyme in the pores of a mesoporous material is an attractive procedure since the enzyme is immobilized without any covalent bonding to a support which may be detrimental to the catalytic performance. The objective of this work is to compare the encapsulation and catalytic performance of lipase from Mucor miehei and trypsin from bovine pancreas, two hydrolases with rather dissimilar properties and structures. We also demonstrate the importance of the pore dimensions and the pH for proper function of the encapsulated enzyme. Mesoporous silica particles (SBA-15) with three different pore sizes (50 Å, 60 Å and 89 Å) were synthesized and hexagonal structures with narrow pore size distributions were confirmed with TEM, SAXS and N2-adsorption. Lipase and trypsin were encapsulated separately in the silica particles and the results indicate distinct differences between the two enzymes, both in loading capacity and catalytic activity. For trypsin the encapsulation rate and the loading capacity were large with a maximum reached at pH 7.6. The largest product yield was obtained with the particles with 60 Å pores, however, the yield was significantly lower than with free trypsin. For lipase optimal encapsulation rate and loading capacity were reached with the particles with 89 Å pores at pH 6.0 but were low compared to trypsin. However, the catalytic activity of the encapsulated lipase was more than twice as large as for free lipase, which can be explained by an interfacial activation of lipase at the silica surface. 相似文献
19.
采用共浸渍、不同分步浸渍的方法制备了8 wt% Ag/CeO2-SiO2催化剂,运用XRD、UV-Vis、BET等多种手段对催化剂的结构进行表征,考察了其对CO氧化的活性,并初步探讨了助剂CeO2对催化剂结构及活性物种的影响。实验结果表明,添加1 wt% CeO2的8 wt% Ag/SiO2催化剂表现出较好的低温CO催化活性,随后氢气预处理明显提高了催化剂的反应活性。XRD和UV-Vis谱图表明少量的CeO2(1 wt%)有利于金属银物种的形成,并且能够提高Ag粒子的稳定性,高温处理不易聚集。高CeO2负载量下的催化剂中银物种主要以银簇( )形式存在。 相似文献
20.
Aiping Zhang Yi Zhang Puguang Wang Jun Li Ying Lv Shuang Gao 《Research on Chemical Intermediates》2011,37(8):975-984
Five catalysts containing PW or W active species that anchored onto aminosilylated mesoporous silica SBA-15 by a post-grafting
route were prepared and the resulting PW or W/APTES/SBA-15 hybrid materials were characterized by XRD, N2 adsorption/desorption, surface area analysis, TEM, FT-IR, and ICP (inductively coupled plasma atomic emission spectroscopy).
The names of these catalysts have been abbreviated as SBA-15m-a, SBA-15m-b, SBA-15m-c, SBA-15m-d, and SBA-15m-e according
to the different active species. The PW or W active species were highly dispersed in the channels of the modified mesoporous
materials. The interaction between PW or W species and amino groups grafted on the channel surface of SBA-15 led to the immobilization
of PW or W species. Their catalytic activity in the epoxidation of cyclooctene with H2O2 as oxidant was investigated. Among them, SBA-15m-a showed the best performance, with 98.9% conversion and 98.4% selectivity.
The catalyst could be reused for six times with a little decrease in activity. 相似文献