A functionalized material, PW/SBA-15m, was prepared successfully in diluted H_2SO_4 aqueous solutions by immobilizing 12-tungstophosphates on chemically modified mesoporous silica SBA-15 and characterized by elemental...A functionalized material, PW/SBA-15m, was prepared successfully in diluted H_2SO_4 aqueous solutions by immobilizing 12-tungstophosphates on chemically modified mesoporous silica SBA-15 and characterized by elemental analysis, FTIR, ~ ~31 P MAS NMR, XRD and TEM. The results indicate that the framework of SBA-15 and the Keggin structure of PW_~12 O^3- _~40 were retained, and that 23%-33%(mass fraction) of ~PW_~12 O^3- _~40 was immobilized; the PW_~12 O^3- _~40 anions were finely dispersed on the pore wall of SBA-15. Having been leached in ethanol at 60 ℃ for 7 h, the loss of PW_~12 O^3- _~40 anions was not found.展开更多
Mesoporous silica SBA-15 consists of uniform hexagonal, unconnected cylindrical channels with diameters that can be tuned within a range of 1.5 nm-30 nm, and is thought to have a special thermal conductivity. The theo...Mesoporous silica SBA-15 consists of uniform hexagonal, unconnected cylindrical channels with diameters that can be tuned within a range of 1.5 nm-30 nm, and is thought to have a special thermal conductivity. The theoretical investigation of the shell thermal conductivity of the mesoporous silica is performed in the relaxation time approximation in this paper and an available one-dimensional heat transfer model is used to predict the effective thermal conductivity （ETC） of the mesoporous silica. The experimental result of the ETC is also presented for comparison. The shell thermal conductivity of the mesoporous silica decreases with mesochannel radius increasing or wall thickness decreasing, but does not strictly decrease with porosity increasing. The thermal radiation possibly plays a primary role in heat transfer at the large porosity scale. The predicted ETC of SBA-15 with only conduction considered is quite low at the large porosity, even lower than the thermal conductivity of the silica aerogels. To realize it, doping carbon or other matters which can strongly absorb infrared light into SBA-15 is a possible way.展开更多
Mesoporous silicas have a very attractive ability of sorption and enrichment of metal ions due to their huge surface area and facile functionalization by organic ligands. In this work, phosphonate-amino hifunctionaliz...Mesoporous silicas have a very attractive ability of sorption and enrichment of metal ions due to their huge surface area and facile functionalization by organic ligands. In this work, phosphonate-amino hifunctionalized mesoporous silica SBA-15 （PA-SBA-15） as U（VI） sorbent was fabricated through post-grafting method. The obtained mesoporous silica was character- ized by SEM, XRD, NMR and nitrogen sorption/desorption experiments, which revealed the existence of ordered mesoporous structure with uniform pore diameter and large surface area. The adsorptivity of PA-SBA-15 for U（VI） from aqueous solution was investigated using batch sorption technique under different experimental conditions. The preliminary results show that the U（VI） sorption by PA-SBA-15 is very quick with equilibrium time of less than 1 h, and the U（VI） uptake is as large as 373 mg/g at pH 5.5 under 95℃. The sorption isotherm has been successfully modeled by the Langmuir isotherm, suggesting a monolayer homogeneous sorption of U（VI） in PA-SBA-15. The sorption is pH-dependent due to the pH-dependent charge of sorbent in the aqueous solution. The thermodynamics research shows that the sorption is a feasible and endothermic process. Based on these results, PA-SBA-15 could be a promising solid phase sorbent for highly-efficient removal of U（VI） ions from waste water and enrichment of U（VI） from a solution at a very low level.展开更多
In this paper,the effects of pore-size of SBA-15 on the adsorption kinetics and equilibrium of large protein molecules Bovine serum albumin(BSA)and lysozyme(LYS)have been investigated.The mesoporous molecular sieve SB...In this paper,the effects of pore-size of SBA-15 on the adsorption kinetics and equilibrium of large protein molecules Bovine serum albumin(BSA)and lysozyme(LYS)have been investigated.The mesoporous molecular sieve SBA-15 with six different pore sizes were synthesized with P123 triblock copolymer as the template agent,and 1,3,5-trimethylbenzene(TMB)and isopropyl alcohol as the pore-expanding agent.The samples were characterized by N2 adsorption/desorption,Scanning Electron Microscopy(SEM),Transmission Electron Microscopy(TEM)and X-Ray Diffraction(XRD).It is found that BSA and LYS were adsorbed rapidly on SBA-15 materials with large pores.The BSA adsorption capacity of sieve with the pore diameter of 21.4 nm reached 500 mg·g-1 within 25 minutes.However,if the pore diameter was smaller than 14 nm,the BSA adsorption capacity of the sieve was only about 220 mg·g-1.The adsorption equilibrium data fits in the Langmuir model,where the coefficient of effective use of specific area of mesoporous molecular sieve was found to be 0.03,0.18,0.37 and 0.48,corresponding to the pore diameter of 10.1 nm,13.2 nm,15.4 nm and 21.4 nm,respectively.The equilibrium loading amount of LYS on SBA-15 materials with pore size of 15.4 nm could be up to 1000 mg·g-1.The coefficient of effective use of surface area of mesoporous molecular sieve with diameter of 3.9 nm,7.4 nm,10.1 nm,13.2 nm and 15.4 nm was 0.10,0.47,0.56,0.71 and 0.79,respectively.It is also noted that greater pore size of mesoporous molecular sieve would lead to a higher coefficient of effective use of surface area.展开更多
Photocatalysis is one of the most promising methods owing to its great potential to relieve environmental issue. To construct efficient photocatalyst with low energy consumption, mild catalytic conditions, and stable ...Photocatalysis is one of the most promising methods owing to its great potential to relieve environmental issue. To construct efficient photocatalyst with low energy consumption, mild catalytic conditions, and stable chemical properties are highly desired. In this work, a novel, highly active and environmental friendly mesoporous photocatalyst Bi4O5Br2/SBA-15 was synthesized by hydrothermal method, and its characteristics and visible-light catalytic activity were investigated. The synthesized photocatalyst consisted of Langmuir type IV hysteresis loops, which was confirmed to be a composite material with mesoporous structure. It exhibited a high visible-light absorption intensity and a low recombination rate of photo-generated electrons and holes. When the mass ratio of Bi/SiO2 was 30/100 during the synthesis, the obtained photocatalyst (Bi30/SBA-15) reflected the fastest Rhodamine B (RhB) removal rate and achieved 100% decolorization of RhB by both adsorption and degradation process. This high decolorization efficiency can also be maintained and realized by recycling the used composite in practice. The enhanced visible-light photocatalytic activity of novel Bi4O5Br2/SBA-15 photocatalyst can be ascribed to the existing active sites both inside and outside SBA-15 which enhanced the separation of photo-generated electrons and holes.展开更多
A Cr/SBA-16 catalyst was prepared using Cr（NO3）3 as a precursor and mesoporous silica SBA-16 as a support via a simple impregnation method. The catalyst was characterized using wide-angle X-ray diffraction （XRD）, ...A Cr/SBA-16 catalyst was prepared using Cr（NO3）3 as a precursor and mesoporous silica SBA-16 as a support via a simple impregnation method. The catalyst was characterized using wide-angle X-ray diffraction （XRD）, low-angle XRD, N2 adsorption-desorption, transmission electron microscopy, and ultraviolet-visible spectroscopy. The catalyst activity was investigated in the direct bydroxylation of benzene to phenol using H2O2 as the oxidant. Various operating variables, namely reaction temperature, reaction time, amount of H2O2, and catalyst dosage, were optimized using central composite design combined with response surface methodology （RSM）. The results showed that the correla- tion between the independent parameters and phenol yield was represented by a second-order polynomial model. The high correlation coefficient （R2）, i.e., 0.985, showed that the data predicted using RSM were in good agreement with the experimental results. The optimization results also showed that high selectivity for phenol was achieved at the optimized values of the operating variables： reaction temperature 324 K, reaction time 8 h, H2O2 content 3.28 mL, and catalyst dosage 0.09 g. This study showed that RSM was a reliable method for optimizing process variables for benzene hydroxylation to phenol.展开更多
Chromium-incorporated mesoporous silica materials （MCrS） have been successfully prepared in strong acidic media by assembly of preformed CrSI precursors with triblock copolymer of the Pluronic type （P123） by a two...Chromium-incorporated mesoporous silica materials （MCrS） have been successfully prepared in strong acidic media by assembly of preformed CrSI precursors with triblock copolymer of the Pluronic type （P123） by a two steps procedure. Various techniques including XRD, N2 adsorption, FT-IR spectroscopy, diffuse reflectance UV-vis （DRUV-vis） and EPR were employed for the materials characterization. MCrS materials have a hexagonal structure with uniform mesopores and contain Cr（V） and Cr（VI） under low and high Cr content and that the mesoporous walls contain the MFI structure building units.展开更多
Novel in-situ reduction approach was applied for the synthesis of palladium nanoparticles in the pores of mesoporous silica materials with grafted siliconhydride groups. Matrices possessing different structural proper...Novel in-situ reduction approach was applied for the synthesis of palladium nanoparticles in the pores of mesoporous silica materials with grafted siliconhydride groups. Matrices possessing different structural properties (MCM-41, SBA-15 and Silochrom) were used. Samples were studied by nitrogen adsorption-desorption method, low-angle X-ray diffraction, transmission electron microscopy (TEM) and FT-IR/PAS spectroscopy. The temperature-programmed oxidation (TPO) and reduction (TPR) methods were applied to examine reducibility of palladium species. Palladium containing catalysts were tested in methane oxidation reaction. It was demonstrated that relatively large pores in SBA-15 type silica facilitated formation of well-dispersed palladium nanoparticles confined in the pores channels. In the case of MCM-41 support, metallic palladium nanoparticles were formed on the external surface. The obtained materials showed high catalytic activity. Lower activity of the samples containing small crystallites located in the pore volume at high temperatures was related to worse accessibility of active sites to the reation mixture.展开更多
The hexagonal silica mesoporous material SBA-15 with ordered 2-dimensional channel structure was used as a suppport to the immobilization of emzyme. α-Chymotrypsin, an enzyme, was assembled in the channel of SBA-15 b...The hexagonal silica mesoporous material SBA-15 with ordered 2-dimensional channel structure was used as a suppport to the immobilization of emzyme. α-Chymotrypsin, an enzyme, was assembled in the channel of SBA-15 by immersion method. The absorbed amount of enzyme in SBA-15 and the activity of the immobilized enzyme were studied. It was found that there was more absorbed enzyme in SBA-15 than in other carrier and the activity of the immobilized α-chymotrypsin was increased compared with the free enzyme. It suggests that silica mesoporous material SBA-15 is a good support for immobilization of enzyme.展开更多
文摘A functionalized material, PW/SBA-15m, was prepared successfully in diluted H_2SO_4 aqueous solutions by immobilizing 12-tungstophosphates on chemically modified mesoporous silica SBA-15 and characterized by elemental analysis, FTIR, ~ ~31 P MAS NMR, XRD and TEM. The results indicate that the framework of SBA-15 and the Keggin structure of PW_~12 O^3- _~40 were retained, and that 23%-33%(mass fraction) of ~PW_~12 O^3- _~40 was immobilized; the PW_~12 O^3- _~40 anions were finely dispersed on the pore wall of SBA-15. Having been leached in ethanol at 60 ℃ for 7 h, the loss of PW_~12 O^3- _~40 anions was not found.
基金supported by the National Basic Research Program of China (973 Program) (Grant No. 2012CB720404)the National Natural Science Foundation of China (Grant No. 50836001)+1 种基金the FOK Ying Tong Education Foundation,China (Grant No. 121055)the Fundamental Research Funds for the Central Universities,China (Grant Nos. FRF-AS-12-002 and FRF-TP-11-001B)
文摘Mesoporous silica SBA-15 consists of uniform hexagonal, unconnected cylindrical channels with diameters that can be tuned within a range of 1.5 nm-30 nm, and is thought to have a special thermal conductivity. The theoretical investigation of the shell thermal conductivity of the mesoporous silica is performed in the relaxation time approximation in this paper and an available one-dimensional heat transfer model is used to predict the effective thermal conductivity （ETC） of the mesoporous silica. The experimental result of the ETC is also presented for comparison. The shell thermal conductivity of the mesoporous silica decreases with mesochannel radius increasing or wall thickness decreasing, but does not strictly decrease with porosity increasing. The thermal radiation possibly plays a primary role in heat transfer at the large porosity scale. The predicted ETC of SBA-15 with only conduction considered is quite low at the large porosity, even lower than the thermal conductivity of the silica aerogels. To realize it, doping carbon or other matters which can strongly absorb infrared light into SBA-15 is a possible way.
基金supported by the National Natural Science Foundation of China (91026007)the "Strategic Priority Research program" of the Chinese Academy of Sciences (XDA03010401,XDA03010403)
文摘Mesoporous silicas have a very attractive ability of sorption and enrichment of metal ions due to their huge surface area and facile functionalization by organic ligands. In this work, phosphonate-amino hifunctionalized mesoporous silica SBA-15 （PA-SBA-15） as U（VI） sorbent was fabricated through post-grafting method. The obtained mesoporous silica was character- ized by SEM, XRD, NMR and nitrogen sorption/desorption experiments, which revealed the existence of ordered mesoporous structure with uniform pore diameter and large surface area. The adsorptivity of PA-SBA-15 for U（VI） from aqueous solution was investigated using batch sorption technique under different experimental conditions. The preliminary results show that the U（VI） sorption by PA-SBA-15 is very quick with equilibrium time of less than 1 h, and the U（VI） uptake is as large as 373 mg/g at pH 5.5 under 95℃. The sorption isotherm has been successfully modeled by the Langmuir isotherm, suggesting a monolayer homogeneous sorption of U（VI） in PA-SBA-15. The sorption is pH-dependent due to the pH-dependent charge of sorbent in the aqueous solution. The thermodynamics research shows that the sorption is a feasible and endothermic process. Based on these results, PA-SBA-15 could be a promising solid phase sorbent for highly-efficient removal of U（VI） ions from waste water and enrichment of U（VI） from a solution at a very low level.
基金Supported by the National Basic Research Program of China(2007CB714302)the Outstanding Young Teacher Visiting Scholar Program of Shandong Province
文摘In this paper,the effects of pore-size of SBA-15 on the adsorption kinetics and equilibrium of large protein molecules Bovine serum albumin(BSA)and lysozyme(LYS)have been investigated.The mesoporous molecular sieve SBA-15 with six different pore sizes were synthesized with P123 triblock copolymer as the template agent,and 1,3,5-trimethylbenzene(TMB)and isopropyl alcohol as the pore-expanding agent.The samples were characterized by N2 adsorption/desorption,Scanning Electron Microscopy(SEM),Transmission Electron Microscopy(TEM)and X-Ray Diffraction(XRD).It is found that BSA and LYS were adsorbed rapidly on SBA-15 materials with large pores.The BSA adsorption capacity of sieve with the pore diameter of 21.4 nm reached 500 mg·g-1 within 25 minutes.However,if the pore diameter was smaller than 14 nm,the BSA adsorption capacity of the sieve was only about 220 mg·g-1.The adsorption equilibrium data fits in the Langmuir model,where the coefficient of effective use of specific area of mesoporous molecular sieve was found to be 0.03,0.18,0.37 and 0.48,corresponding to the pore diameter of 10.1 nm,13.2 nm,15.4 nm and 21.4 nm,respectively.The equilibrium loading amount of LYS on SBA-15 materials with pore size of 15.4 nm could be up to 1000 mg·g-1.The coefficient of effective use of surface area of mesoporous molecular sieve with diameter of 3.9 nm,7.4 nm,10.1 nm,13.2 nm and 15.4 nm was 0.10,0.47,0.56,0.71 and 0.79,respectively.It is also noted that greater pore size of mesoporous molecular sieve would lead to a higher coefficient of effective use of surface area.
文摘Photocatalysis is one of the most promising methods owing to its great potential to relieve environmental issue. To construct efficient photocatalyst with low energy consumption, mild catalytic conditions, and stable chemical properties are highly desired. In this work, a novel, highly active and environmental friendly mesoporous photocatalyst Bi4O5Br2/SBA-15 was synthesized by hydrothermal method, and its characteristics and visible-light catalytic activity were investigated. The synthesized photocatalyst consisted of Langmuir type IV hysteresis loops, which was confirmed to be a composite material with mesoporous structure. It exhibited a high visible-light absorption intensity and a low recombination rate of photo-generated electrons and holes. When the mass ratio of Bi/SiO2 was 30/100 during the synthesis, the obtained photocatalyst (Bi30/SBA-15) reflected the fastest Rhodamine B (RhB) removal rate and achieved 100% decolorization of RhB by both adsorption and degradation process. This high decolorization efficiency can also be maintained and realized by recycling the used composite in practice. The enhanced visible-light photocatalytic activity of novel Bi4O5Br2/SBA-15 photocatalyst can be ascribed to the existing active sites both inside and outside SBA-15 which enhanced the separation of photo-generated electrons and holes.
基金the University of Tehran for financial support of this work
文摘A Cr/SBA-16 catalyst was prepared using Cr（NO3）3 as a precursor and mesoporous silica SBA-16 as a support via a simple impregnation method. The catalyst was characterized using wide-angle X-ray diffraction （XRD）, low-angle XRD, N2 adsorption-desorption, transmission electron microscopy, and ultraviolet-visible spectroscopy. The catalyst activity was investigated in the direct bydroxylation of benzene to phenol using H2O2 as the oxidant. Various operating variables, namely reaction temperature, reaction time, amount of H2O2, and catalyst dosage, were optimized using central composite design combined with response surface methodology （RSM）. The results showed that the correla- tion between the independent parameters and phenol yield was represented by a second-order polynomial model. The high correlation coefficient （R2）, i.e., 0.985, showed that the data predicted using RSM were in good agreement with the experimental results. The optimization results also showed that high selectivity for phenol was achieved at the optimized values of the operating variables： reaction temperature 324 K, reaction time 8 h, H2O2 content 3.28 mL, and catalyst dosage 0.09 g. This study showed that RSM was a reliable method for optimizing process variables for benzene hydroxylation to phenol.
文摘Chromium-incorporated mesoporous silica materials （MCrS） have been successfully prepared in strong acidic media by assembly of preformed CrSI precursors with triblock copolymer of the Pluronic type （P123） by a two steps procedure. Various techniques including XRD, N2 adsorption, FT-IR spectroscopy, diffuse reflectance UV-vis （DRUV-vis） and EPR were employed for the materials characterization. MCrS materials have a hexagonal structure with uniform mesopores and contain Cr（V） and Cr（VI） under low and high Cr content and that the mesoporous walls contain the MFI structure building units.
基金This work was supported by European Community,seventh Framework Programm(FP/2007-2013)Marie Curie International Research Staff Exchange Scheme(grant no.230790)project MEC 06 MAT2006 01997.
文摘Novel in-situ reduction approach was applied for the synthesis of palladium nanoparticles in the pores of mesoporous silica materials with grafted siliconhydride groups. Matrices possessing different structural properties (MCM-41, SBA-15 and Silochrom) were used. Samples were studied by nitrogen adsorption-desorption method, low-angle X-ray diffraction, transmission electron microscopy (TEM) and FT-IR/PAS spectroscopy. The temperature-programmed oxidation (TPO) and reduction (TPR) methods were applied to examine reducibility of palladium species. Palladium containing catalysts were tested in methane oxidation reaction. It was demonstrated that relatively large pores in SBA-15 type silica facilitated formation of well-dispersed palladium nanoparticles confined in the pores channels. In the case of MCM-41 support, metallic palladium nanoparticles were formed on the external surface. The obtained materials showed high catalytic activity. Lower activity of the samples containing small crystallites located in the pore volume at high temperatures was related to worse accessibility of active sites to the reation mixture.
文摘The hexagonal silica mesoporous material SBA-15 with ordered 2-dimensional channel structure was used as a suppport to the immobilization of emzyme. α-Chymotrypsin, an enzyme, was assembled in the channel of SBA-15 by immersion method. The absorbed amount of enzyme in SBA-15 and the activity of the immobilized enzyme were studied. It was found that there was more absorbed enzyme in SBA-15 than in other carrier and the activity of the immobilized α-chymotrypsin was increased compared with the free enzyme. It suggests that silica mesoporous material SBA-15 is a good support for immobilization of enzyme.
