Mesoporous silica SBA-15 sheet with perpendicular nanochannels

Free-standing thin sheet form of mesoporous silica materials with perpendicular orientation is a much desired materials for its possible applications in catalysis, mask, and separation. A three component amphiphile system of sodium dodecyl sulfate/hexadecyltrimethylammonium bromide/pluronic-123(C(16)TMAB/SDS/P123) was employed to template the condensation of sodium silicates for the formation of SBA(⊥), a thin sheet of SBA-15 with perpendicular nanochannels. SBA(⊥) can be synthesized at SDS/C(16)TMAB=1.5 and T≥40°C and shows pH-dependent morphology. It has uniform pore size ～9 nm, homogeneous sheet thickness in the range of 60-300 nm and dimension of several microns. We studied in details the structure and morphology of the SBA(⊥) with variation of three experimental parameters: the SDS/C(16)TMAB ratio, the temperature, and the pH condition in the synthetic gel. It is proposed that the mixed surfactants of SDS and C(16)TMAB form catanionic vesicle in which the P123 and silicates are condensed. The balanced interaction of P123/silicate with the narrow confinement under surfactant bi-layers of C(16)TMAB/SDS promoted the formation of perpendicular nanochannels. Low temperature and pH conditions favor stronger segregation of the PPO and PEO-oligosilicate segments in the SBA(⊥) structure which gives the basis of thickness control of the sheet. The control of structure and morphology are discussed with modern theory of microphase separation in block copolymers under confinement.     

Controlling the shape and alignment of mesopores by confinement in colloidal crystals: designer pathways to silica monoliths with hierarchical porosity

Monolithic pieces of hierarchically structured silica, containing both periodic macropores and mesopores with well-controlled architecture, are synthesized by dual templating methods. Colloidal crystal templating with close-packed arrays of poly(methyl methacrylate) spheres yields regular, highly interconnected macropores a few hundred nanometers in diameter, and templating with nonionic surfactants produces mesoporosity (2.5-5.1 nm pore diameters) in the macropore walls. Several distinct mesostructures can be achieved within the silica skeleton, depending on the choice of surfactant, co-surfactant, and processing conditions. In the three-dimensional (3D) confinement of the colloidal crystal template, wormlike channels, cubic (Pm3n), or two-dimensional (2D) hexagonal (P6mm) mesostructures are produced with the surfactant Brij 56 (C16H33(OCH2CH2)nOH (n approximately 10) and dodecane as cosurfactant. In the 2D hexagonal structure, channels are oriented perpendicular to the polymer spheres, thereby connecting adjacent macropores through the silica walls. This orientation contrasts with channel alignment parallel to latex spheres when the polymeric surfactant Pluronic P123 (EO20PO70EO20) is used. On the basis of high-resolution 3D transmission electron microscopy, scanning electron microscopy, small-angle X-ray scattering, and nitrogen sorption measurements, structural and textural properties of the monoliths are described in detail as a function of the synthesis parameters. The control over the mesoarchitecture of these silica-surfactant systems in 3D confinement is explained by considering the relative dimensions of the mesostructures with respect to the interstitial space in the latex template, interfacial interactions, entropic effects, and structural frustration.     

Tuning the mesostructures of vinyl silica by adjusting the micellar curvature

In our previous study (Wang, Y. Q.; Yang, C.-M.; Zibrowius, B.; Spliethoff, B.; Lindén, M.; Schüth, F. Chem. Mater. 2003, 15, 5029), mesoporous vinyl-functionalized silica (vinyl silica) with hexagonal P6mm and cubic Ia3d structures has been synthesized at different loadings of vinyl groups and at different concentrations of sodium chloride when triblock copolymer P123 was used as a template. Our further investigations presented in this article reveal that at a loading of 10% vinyl groups, well-ordered cubic Ia3d structure was obtained at a low concentration of Na2SO4 (0.5 M) and the hexagonal structure was produced at 1.0 M NaCl. When NaNO3 was used as the inorganic salt, the hexagonal structure was still maintained even at a salt concentration of 2.0 M. The result is in accordance with the Hofmeister series order (salting-out effect): SO4(2-) > Cl- > NO3(-). The lowering of the acidity also induced the formation of the cubic Ia3d structure. At 20% loading, hexagonal structure can be obtained by adding the more hydrophilic Pluronic F127 (EO106PO70EO106) to the acidic solutions of P123, but the hexagonal structure cannot be produced with pure P123 under the synthesis conditions investigated. All of these results can be rationalized through hydrophilic-hydrophobic balance and the change in micellar curvature. Furthermore, 10% mercaptopropyl-functionalized mesoporous silica with cubic Ia3d structure was designed and synthesized successfully with the assistance of an inorganic salt (NaCl) in an acidic solution of P123, which is the first example of mercaptopropyl-functionalized large-pore mesoporous silica with high loadings.     

WxC/SBA-16催化剂的制备、表征及催化加氢脱硫性能

以正硅酸乙酯为硅源, 仲钨酸铵为钨源, P123和F127为混合模板剂,采用水热晶化法一步合成了不同钨含量(以n(Si):n(W)表示)的WO3/SBA-16, 然后经甲烷/氢气(V(CH4)/V(H2)=1/4)混和气体程序升温还原碳化(TPC), 制备出了WxC/SBA-16(x=1, 2)催化剂. 采用XRD、N2-吸附/脱附、TEM和FTIR等分析测试技术对样品的结构进行了表征, 并以噻吩作为模型化合物, 对WxC/SBA-16催化剂的加氢脱硫催化活性进行了评价. 结果表明, 在一定钨含量的条件下, WO3/SBA-16和WxC/SBA-16样品仍然保持立方笼状介孔结构, 当n(Si):n(W)为30-10时, 碳化钨的物相为W2C; n(Si):n(W)为7.5时, 碳化钨的物相为W2C和WC. WxC/SBA-16催化剂表现出了良好的加氢脱硫催化性能.     

介孔二氧化硅的扩孔及其氨基功能化

利用嵌段共聚物聚环氧乙烷-聚环氧丙烷-聚环氧乙烷(P123)作为胶束模板,均三甲苯(TMB)为扩孔剂,在强酸条件下制备出了一系列大孔径的介孔二氧化硅材料,获得了一种泡状新型结构的硅材料;通过N2吸附-脱附、高分辨透射电镜(HTEM)等手段对这种新型结构的材料进行了表征,综合考察了扩孔剂的用量、酸的浓度以及水热处理温度对...     

Morphological and structural evolution of mesoporous silicas in a mild buffer solution and lysozyme adsorption

Mesoporous silicas with various morphologies and structures were synthesized with the aid of 2,2,4-trimethylpentane (TMP) in the presence of nonionic surfactant P123 [(EO)20(PO)70(EO)20] as a structure-directing agent under mild reaction conditions (HAc-NaAc buffer solution, pH 4.4). The ropelike particles formed by end-to-end interconnected nanorods were obtained at a TMP/P123 weight ratio of 0.5. It is noteworthy to mention that the mesoporous nanorods have channels running parallel to the short axis. The silica hollow spheres can be obtained at a higher TMP/P123 weight ratio because of the fusion of the primary nanorods around the interface of the O/W emulsion. Initial synthesis temperatures of 15, 25, and 40 degrees C can lead to mesoporous silicas with highly ordered 2D hexagonal mesostructure, vesicular mesostructure, and mesostructured cellular foams (MCF), respectively. The mesoporous silicas exhibit high adsorption capacity (up to 536 mg g(-1)) and very rapid (<5 min to reach equilibrium) lysozyme immobilization. More importantly, it is revealed that mesoporous silica hollow spheres with rugged surfaces can greatly accelerate the adsorption rate of the enzyme during the adsorption process.     

Intercalation of poly(oxyethylene) alkyl ether into a layered silicate kanemite

Poly(oxyethylene) alkyl ether (CnEOm) is intercalated into the interlayer space of a layered silicate kanemite by using layered hexadecyltrimethylammonium (C16TMA) intercalated kanemite (C16TMA-kanemite) as the intermediate. C16TMA-kanemite was treated with an aqueous solution of C16EO10, and the intercalation of C16EO10 was confirmed by the slight increase in the basal spacing (from 2.92 to 3.34 nm) with the increase in the carbon content, yielding C16EO10-C16TMA-kanemite. The product was dispersed again in a C16EO10 aqueous solution, and then 1.0 M HCl was added to the suspension to remove C16TMA ions completely. The basal spacing was further increased (from 3.34 to 5.52 nm) and the content of nitrogen was virtually zero, indicating further intercalation of C16EO10 molecules and complete elimination of C16TMA ions simultaneously. Though C16EO10 molecules are not directly intercalated into kanemite, the mutual interactions among C16TMA ions, C16EO10 molecules, and the interlayer silicate surfaces effectively induce the intercalation of C16EO10. C16EO10-kanemite shows a reversible adsorption of n-decane and water owing to the hydrophobicity and hydrophilicity of C16EO10, respectively, in the interlayer space. Layered CnEO10-kanemites (n = 12 and 18) were also synthesized in a manner similar to layered C16EO10-kanemite.     

Improved micellar hydration and gelation characteristics of PEO-PPO-PEO triblock copolymer solutions in the presence of LiCl

LiCl-induced changes in the micellar hydration and gelation characteristics of aqueous solutions of the two triblock copolymers F127 (EO(100)PO(70)EO(100)) and P123 (EO(20)PO(70)EO(20)) (where EO represents the ethylene oxide block and PO represents the propylene oxide block) have been studied by small-angle neutron scattering (SANS) and viscometry. The effect of LiCl was found to be significantly different from those observed for other alkali metal chloride salts such as NaCl and KCl. This can be explained on the basis of the complexation of hydrated Li(+) ions with the PEO chains in the micellar corona region. The interaction between the chains and the ions is more significant in the case F127 because of its larger PEO block size, and therefore, micelles of this copolymer show an enhanced degree of hydration in the presence of LiCl. The presence of the hydrated Li(+) ions in the micellar corona increases the amount of mechanically trapped water there and compensates more than the water molecules lost through the dehydration of the PEO chains in the presence of the Cl(-) ions. The enhancement in micellar hydration leads to a decrease in the minimum concentration required for the F127 solution to form a room-temperature cubic gel phase from 18% to 14%. Moreover, for both copolymers, the temperature range of stability of the cubic gel phase also increases with increasing LiCl concentration, presumably because of the ability of the Li(+) ions to reduce micellar dehydration with increasing temperature. Viscosity studies on a poly(ethylene glycol) (PEG) homopolymer with a size equivalent to that of the PEO block in F127 (4000 g/mol) also suggest that the dehydrating effect of the Cl(-) ion on the PEG chain is compensated by its interaction with the hydrated Li(+) ions.     

Aggregation of alkyltrimethylammonium ions at the cleaved muscovite mica-water interface: a Monte Carlo study

The precise molecular structure of organically modified mineral surfaces is still not well understood. To establish a relation between experimental observations and underlying molecular structure, we performed Monte Carlo simulations of the aggregation behavior of alkyltrimethylammonium surfactants (C(n)TMA(+)) at the interface between C(n)TMACl solution and cleaved K(+)-muscovite. The structures were examined with regard to the influence of varying alkyl chain length n (n = 8, 12, 16) and surface coverage of C(n)TMA(+) ions. The simulation results indicate that the water film structure at the muscovite surface is considerably influenced by the adsorption of C(n)TMA(+). A fraction of the C(n)TMA(+) ions forms inner-sphere and outer-sphere adsorption complexes with nitrogen-surface distances of 3.3-3.8 and 5.5-8.4 ?, respectively. The simulated monolayer aggregates exhibit thicknesses of 31-35, 22-27, and ～18 ? for C(16)TMA(+), C(12)TMA(+), and C(8)TMA(+), respectively. C(16)TMA(+) and C(12)TMA(+) ions form bilayer aggregates, which show a strong interdigitation of the two opposing layers composing them. The aggregate thicknesses equal 35-39 and 30-35 ?, respectively, and are in agreement with available experimental data. In contrast, the short-chained C(8)TMA(+) ions do not form bilayer aggregates. In agreement with previous experimental studies, the alkyl chains of the aggregated ions show high conformational order markedly decreasing with decreasing chain length. We suggest that the simulated structures represent C(n)TMA(+) aggregates, which are formed on muscovite during the experimentally observed initial equilibration phase characterized by the presence of inorganic ions within the aggregates.     

Investigation of the morphology of the mesoporous SBA-16 and SBA-15 materials

Mesoporous SBA-16 and SBA-15 were studied in order to control their possible morphologies. SBA-16 is synthesized using a silicon source (tetraethoxysilane, TEOS) and a ternary system consisting of surfactant F127 (EO106PO70EO106), water, and butanol. The same ternary system, with higher butanol concentration, is used to form SBA-15 material as well. An increase of the TEOS concentration results in a morphology shift of SBA-16 from micron-sized spheres, over randomly shaped aggregated particles, to macrospheres with a size of 15 mm. An identical increase in TEOS concentration also results in the formation of SBA-15 macrospheres, which can be controlled in size. Micron-sized spheres of SBA-15 were formed using a quaternary system of surfactant P123 (EO20PO70EO20), cetyltrimethylammonium bromide (CTAB), ethanol, and water. All mesoporous silica materials were characterized using SEM, XRD, and N2 sorption techniques.     

Effect of SDS on the self-assembly behavior of the PEO-PPO-PEO triblock copolymer (EO)20(PO)70(EO)20

The mixed micellar system comprising the poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide)-based triblock copolymer (EO)(20)(PO)(70)(EO)(20) (P123) and the anionic surfactant sodium dodecyl sulfate (SDS) has been investigated in aqueous media by small-angle neutron scattering (SANS) and viscosity measurements. The aggregation number of the copolymer in the micelles decreases upon addition of SDS, but a simultaneous enhancement in the degree of micellar hydration leads to a significant increase in the micellar volume fraction at a fixed copolymer concentration. This enhancement in the micellar hydration leads to a marked increase in the stability of the micellar gel phase until it is destroyed at very high SDS concentration. Mixed micellar systems with low and intermediate SDS concentrations form the micellar gel phase in much wider temperature and copolymer concentration ranges than the pure copolymer micellar solution. A comparison of the observed results with those for the copolymers (EO)(26)(PO)(40)(EO)(26) (P85) and (EO)(99)(PO)(70)(EO)(99) (F127) suggests that the composition of the copolymers plays a significant role in determining the influence of SDS on the gelation characteristics of the aqueous copolymer solutions. Copolymers with high PO/EO ratios show an enhancement in the stability of the gel phase, whereas copolymers with low PO/EO ratios show a deterioration of the same in the presence of SDS.     

Design of low-toxic and temperature-sensitive anionic microemulsions using short propyleneglycol alkyl ethers as cosurfactants

The phase behavior of anionic microemulsions composed of water, sodium dodecyl sulfate (SDS), dodecane, and short propyleneglycol monoalkyl ethers (C(n)()PO(m)(); n = 3, m = 1 and n = 4, m = 2, 3) is studied. From the pseudoternary phase diagrams, it is inferred that C(n)()PO(m)() compounds have cosurfactant behaviors comparable to those of 1-butanol and 1-pentanol, which are the most efficient and widely used cosurfactants. In contrast to these alcohols, the C(n)()PO(m)() cosurfactants induce high temperature dependences in the SDS microemulsion systems. Furthermore, SDS/C(n)()PO(m)() microemulsions can be formed with small SDS concentrations (SDS/C(4)PO(3) mass ratio of 1/6.26). These have a low toxicity in contrast to systems containing genotoxic short ethyleneglycol ethers (C(n)()EO(m)()) as the cosurfactant. The strong temperature dependence can be favorable in the recovery of reaction products when the microemulsion is used either as a reaction medium or in extraction processes.     

新型介孔二氧化硅囊泡结构的调变

本文采用水热合成法,利用非离子表面活性剂聚环氧乙烷-聚环氧丙烷-聚环氧乙烷(P123)对有机溶剂均三甲苯(TMB)的增容作用,合成了大孔径介孔二氧化硅囊泡材料,首次通过控制有机溶剂TMB与无机硅源正硅酸四乙酯(TEOS)的投料时间间隔t,实现对介孔二氧化硅囊泡材料结构的调变。通过小角X射线衍射和高分辨透射电镜(HTEM)检测技术对酸性P123模板体系中的材料结构转变过程进行了表征。结果表明,改变TMB与TEOS的投料时间间隔,能够实现介孔囊泡结构的调变,同时提出"协同囊泡模板"(cooperative vesicle templating,CVT)和"协同作用机制"(cooperative formation mechanism,FM)共存。通过简单合理的设计合成不同结构的介孔材料,以期开拓其在催化、分离以及医学等领域的潜在应用,也为合成其他介孔材料提供简单合理的设计思路。     

NMR investigations of self-aggregation characteristics of SDS in a model assembled tri-block copolymer solution

The present work was undertaken with a view to understand the influence of a model non-ionic tri-block copolymer PEO-PPO-PEO (poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide)) with molecular weight 5800 i.e., P123 [(EO)(20)-(PO)(70)-(EO)(20)] on the self-aggregation characteristics of the anionic surfactant sodium dodecylsulfate (SDS) in aqueous solution (D(2)O) using NMR chemical shift, self-diffusion and nuclear spin-relaxation as suitable experimental probes. In addition, polymer diffusion has been monitored as a function of SDS concentration. The concentration-dependent chemical shift, diffusion data and relaxation data indicated the significant interaction of polymeric micelles with SDS monomers and micelles at lower and intermediate concentrations of SDS, whereas the weak interaction of the polymer with SDS micelles at higher concentrations of SDS. It has been observed that SDS starts aggregating on the polymer at a lower concentration i.e., critical aggregation concentration (cac=1.94 mM) compared to polymer-free situation, and the onset of secondary micelle concentration (C(2)=27.16 mM) points out the saturation of the 0.2 wt% polymer or free SDS monomers/micelles at higher concentrations of SDS. It has also been observed that the parameter cac is almost independent in the polymer concentrations of study. The TMS (tetramethylsilane) has been used as a solubilizate to measure the bound diffusion coefficient of SDS-polymer mixed system. The self-diffusion data were analyzed using two-site exchange model and the obtained information on aggregation dynamics was commensurate with that inferred from chemical shift and relaxation data. The information on slow motions of polymer-SDS system was also extracted using spin-spin and spin-lattice relaxation rate measurements. The relaxation data points out the disintegration of polymer network at higher concentrations of SDS. The present NMR investigations have been well corroborated by surface tension and conductivity measurements.     

氨基功能化有序介孔Si02薄膜组装Au纳米粒子复合材料的可调色散性质

以聚环氧乙烷-聚环氧丙烷-聚环氧乙烷(P123)为模板剂,采用共溶胶的蒸发诱导自组装方法制备了氨基功能化介孔SO2薄膜,然后利用氯金酸(HAUCl4)与介孔SiO2薄膜孔道内壁的氨基之间的中和反应组装Au纳米粒子,制备得到Au/SiO2纳米复合材料.用TEM,XRD和UV-Vis光谱对材料进行了测试.结果表明,无水乙醇...     

Mixed micelles of a PEO-PPO-PEO triblock copolymer (P123) and a nonionic surfactant (C12EO6) in water. a dynamic and static light scattering study

The present article reports on static and dynamic light scattering (SLS and DLS) studies of aqueous solutions of the nonionic surfactant C12EO6 and the poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) triblock copolymer EO20PO68EO20 (P123) at temperatures between 25 and 45 degrees C. In water, P123 self-assembles into spherical micelles with a hydrodynamic radius of 10 nm, and at 40 degrees C, these micelles consist of 131 unimers. Addition of C12EO6 leads to an association of the surfactant molecules to the P123 micelles and mixed micelles are formed. The size and structure of the mixed micelles as well as interparticle interactions were studied by varying the surfactant-to-copolymer (C12EO6/P123) molar ratio. The novelty of this study consists of a composition-induced structural change of the mixed micelles at constant temperature. They gradually change from being spherical to polymer-like with increasing C12EO6 content. At low C12EO6/P123 molar ratios (below 12), the SLS measurements showed that the molar mass of the mixed micelles decreases with an increasing amount of C12EO6 in the micelles for all investigated temperatures. In this regime, the mixed micelles are spherical and the DLS measurements revealed a decrease in the hydrodynamic radius of the mixed micelles. An exception was found for C12EO6/P123 molar ratios between 2 and 3, where the mixed micelles become rodlike at 40 degrees C. This was the subject of a previous study and has hence not been investigated here. At high molar ratios (48 and above), the polymer-like micelles present a concentration-induced growth, similar to that observed in the pure C12EO6/water system.     

A calorimetry and light scattering study of the formation and shape transition of mixed micelles of EO20PO68EO20 triblock copolymer (P123) and nonionic surfactant (C12EO6)

The interaction between the nonionic surfactant C12EO6 and the poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) triblock copolymer EO20PO68EO20 (P123) has been investigated by means of isothermal titration and differential scanning calorimetry (DSC) as well as static and dynamic light scattering (SLS and DLS). P123 self-assembles in water into spherical micelles at ambient temperatures. At raised temperatures, the DSC data revealed a sphere-to-rod transition of the P123 micelles around 60 degrees C. C12EO6 interacts strongly with P123 micelles in aqueous solution to give mixed micelles with a critical micelle concentration (cmc) well below the cmc for pure C12EO6. The presence of C12EO6 also lowers the critical micelle temperature of P123 so aggregation starts at significantly lower temperatures. A new phenomenon was observed in the P123-C12EO6 system, namely, a well-defined sphere-to-rod transition of the mixed micelles. A visual phase study of mixtures containing 1.00 wt % P123 showed that in a narrow concentration range of C12EO6 both the sphere-to-rod transition and the liquid-liquid phase separation temperature are strongly depressed compared to the pure P123-water system. The hydrodynamic radius of spherical mixed micelles at a C12EO6/P123 molar ratio of 2.2 was estimated from DLS to be 9.1 nm, whereas it is 24.1 nm for the rodlike micelles. Furthermore, the hydrodynamic length of the rods at a molar ratio of 2.2 is in the range of 100 nm. The retarded kinetics of the shape transition was detected in titration calorimetric experiments at 40 degrees C and further studied by using time-resolved DLS and SLS. The rate of growth, which was slow (>2000 s), was found to increase with the total concentration.     

Simplified synthesis of micropore-free mesoporous silica,SBA-15, under microwave-hydrothermal conditions

Synthesis of micropore-free hydrothermally stable mesoporous silica SBA-15 has been accomplished by templating a silica precursor (sodium silicate/tetraethylorthosilicate) with pluroni123 copolymer (EO20PO70EO20; M.W. 5,800) in the presence of cosolvent (ethanol) using a minimum salt (sodium chloride) content, under microwave-hydrothermal conditions at 373 K in 120 mins.     

General and simple approach for control cage and cylindrical mesopores, and thermal/hydrothermal stable frameworks

Highly ordered cage and cylindrical mesoporeous silica monoliths (HOM) with 2- and 3-dimensional (2D and 3D, respectively) structures, mesopore/micropore volumes, and thick-walled frameworks were successfully fabricated by instant direct templating of lyotropic phases of copolymer (EO(m)-PO(n)-EO(m)) surfactants. Large cage-like pores with uniform constriction sizes up to 10 nm and open cylindrical channel-like mesopores can be easily achieved by this simple and efficient synthesis design. Our results show that the cage-like pores could be fabricated at relatively lower copolymer concentrations used in the lyotropic phase domains at copolymer/TMOS ratios of 35 wt %. These ordered cage pore architectures underwent transition to open-cylindrical pores by increasing the copolymer concentration. High EO/PO block copolymers, in general, were crucially affected on the increase of the interior cavity sizes and on the stability of the cage mesopore characters. However, for F108 (EO(141)PO(44)EO(141)) systems, the fabrication of ordered and stable cage pore monoliths was achieved with significantly higher copolymer concentrations up to 90 wt %. Interestingly, the effective copolymer molecular nature was also observed in the ability to design various ordered mesophase geometries in large domain sizes. Our findings here show evidence that the synthetic strategy provides realistic control over a wide range of mesostructured phase geometries and their extended long-range ordering in the final replicas of the silica monolith frameworks. In addition, the HOM silica monoliths exhibited considerable structural stability against higher thermal temperature (up to 1000 degrees C) and longer hydrothermal treatment times under boiling water and steam. The remarkable structural findings of 3D frameworks, transparent monoliths, and micropores combined with large cage- and cylindrical-like mesopores are expected to find promising uses in materials chemistry.     

PW_(11)/SBA-15介孔杂化材料的直接合成与表征

采用三嵌段共聚物EO20PO70EO20(P123)为模板剂,正硅酸乙酯(TEOS)和缺位Keggin型多金属氧酸盐Na7PW11O39(PW11)为无机前驱体,由共缩合法一步合成了PW11/SBA-15介孔杂化材料.通过红外(IR)光谱、紫外-可见漫反射光谱(UV-Vis/DRS)、X射线衍射(XRD)、低温N2吸附、透射电子显微镜(TEM)等手段对杂化材料和合成过程进行了表征.结果表明:杂化材料中不仅多金属氧酸盐的Keggin单元保留完整,且共价键联于介孔孔道内部,而且样品基本具有规整有序的六方介孔结构.TEOS预水解时间的长短对有序结构的构筑有明显影响,随预水解时间延长,样品的介观有序性增加.这是因为多金属氧酸盐对模板剂P123有盐析作用,其作用大小与多金属氧酸盐前驱物的溶解度有关.