The immobilization of acetylcholinesterase （ACHE） on amino functionalized SBA-15 mesoporous sieves （NH2-SBA-15） was explored for detection of organophosphorus and carhamate pesticides. Several methods have been st...The immobilization of acetylcholinesterase （ACHE） on amino functionalized SBA-15 mesoporous sieves （NH2-SBA-15） was explored for detection of organophosphorus and carhamate pesticides. Several methods have been studied and the ＂adsorption-crosslinking＂ is found to be the best one. Firstly, AChE and bovine serum albumin （BSA） were adsorbed in turn on the surface of NH2-SBA-15 by electrostatic adsorption, and then glutaraldehyde was added for cross-linking the amino group of AChE. The NH2-SBA- 15 showed around 95% immobilization efficiency and the specific activity of immobilized AChE （ACHE- NH2-SBA-15） reached 130% relative to free AChE under optimal immobilization conditions. It was found AChE-NH2-SBA-15 retained 94.0% and 82.8% of its initial activity after 60days at 4℃ and 25℃, respectively. It remained 55.0% of its initial activity after 6 times recycling. During the detection of pesticide, the AChE-NH2-SBA-15 showed wider linear range and much lower limit of detection compared with free ACHE. The current method showed good recovery （93.8%-109.3%） and low RSD （〈5%） for both standard solution and real vegetable samples of Carbaryl and Trichlorfon. It was believed that AChE-NH2- SBA- 15 could be exploited as a fast, sensitive and low-cost biocatalyst towards the detection of pesticides residues which could be stored at room temperature for a long time.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
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
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
Preparation of dispersed transition metal oxides catalyst with low oxidation state still remains a challenging task in heterogeneous catalysis.In this study,vanadium oxides supported on zeolite SBA-15 have been prepar...Preparation of dispersed transition metal oxides catalyst with low oxidation state still remains a challenging task in heterogeneous catalysis.In this study,vanadium oxides supported on zeolite SBA-15 have been prepared under hydrothermal condition using V 2 O 5 and oxalic acid as sources of vanadium and reductant,respectively.The structures of samples,especially the oxidation state of vanadium,and the surface distribution of vanadium oxide species,have been thoroughly characterized using various techniques,including N 2-physisorption,X-ray diffraction（XRD）,transmission electron microscopy（TEM）,X-ray photoelectron spectroscopy（XPS）,UV-visible spectra（UV-Vis） and UV-visible-near infrared spectra（UV-Vis-NIR）.It is found that the majority of supported vanadium was in the form of vanadium（IV） oxide species with the low valence of vanadium.By adjusting hydrothermal treatment time,the surface distribution of vanadium（IV） oxide species can be tuned from vanadium（IV） oxide cluster to crystallites.These materials have been tested in the hydroxylation of benzene to phenol in liquid-phase with molecular oxygen in the absence of reductant.The catalyst exhibits high selectivity for phenol（61%） at benzene conversion of 4.6%,which is a relatively good result in comparison with other studies employing molecular oxygen as the oxidant.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
基金supported by the National Natural Science Foundation of China (No.21303105)Shanghai Committee of Science and Technology (No.13430503400)
文摘The immobilization of acetylcholinesterase （ACHE） on amino functionalized SBA-15 mesoporous sieves （NH2-SBA-15） was explored for detection of organophosphorus and carhamate pesticides. Several methods have been studied and the ＂adsorption-crosslinking＂ is found to be the best one. Firstly, AChE and bovine serum albumin （BSA） were adsorbed in turn on the surface of NH2-SBA-15 by electrostatic adsorption, and then glutaraldehyde was added for cross-linking the amino group of AChE. The NH2-SBA- 15 showed around 95% immobilization efficiency and the specific activity of immobilized AChE （ACHE- NH2-SBA-15） reached 130% relative to free AChE under optimal immobilization conditions. It was found AChE-NH2-SBA-15 retained 94.0% and 82.8% of its initial activity after 60days at 4℃ and 25℃, respectively. It remained 55.0% of its initial activity after 6 times recycling. During the detection of pesticide, the AChE-NH2-SBA-15 showed wider linear range and much lower limit of detection compared with free ACHE. The current method showed good recovery （93.8%-109.3%） and low RSD （〈5%） for both standard solution and real vegetable samples of Carbaryl and Trichlorfon. It was believed that AChE-NH2- SBA- 15 could be exploited as a fast, sensitive and low-cost biocatalyst towards the detection of pesticides residues which could be stored at room temperature for a long time.
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.
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supported by the National Nature Science Foundation of China (21073184 and 21103175)One Hundred Person Project of the Chinese Academy of Sciences
文摘Preparation of dispersed transition metal oxides catalyst with low oxidation state still remains a challenging task in heterogeneous catalysis.In this study,vanadium oxides supported on zeolite SBA-15 have been prepared under hydrothermal condition using V 2 O 5 and oxalic acid as sources of vanadium and reductant,respectively.The structures of samples,especially the oxidation state of vanadium,and the surface distribution of vanadium oxide species,have been thoroughly characterized using various techniques,including N 2-physisorption,X-ray diffraction（XRD）,transmission electron microscopy（TEM）,X-ray photoelectron spectroscopy（XPS）,UV-visible spectra（UV-Vis） and UV-visible-near infrared spectra（UV-Vis-NIR）.It is found that the majority of supported vanadium was in the form of vanadium（IV） oxide species with the low valence of vanadium.By adjusting hydrothermal treatment time,the surface distribution of vanadium（IV） oxide species can be tuned from vanadium（IV） oxide cluster to crystallites.These materials have been tested in the hydroxylation of benzene to phenol in liquid-phase with molecular oxygen in the absence of reductant.The catalyst exhibits high selectivity for phenol（61%） at benzene conversion of 4.6%,which is a relatively good result in comparison with other studies employing molecular oxygen as the oxidant.
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.
