To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environment...To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.展开更多
The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane‐rich biogas. However, digested sludge, the residue produced in that process...The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane‐rich biogas. However, digested sludge, the residue produced in that process, still contains high levels of heavy metals and other harmful substances that might make traditional disposal difficult. We have devised a facile method of converting digested sludge into a mesoporous material that acts as an effective and stable heterogeneous catalyst for the photo‐Fenton reaction. A comparison of the removal of rhodamine B under different conditions showed that FAS‐1‐350, which was synthesized by mixing the digested sludge with a 1 mol/L（NH4）2Fe（SO4）2 solution followed by calcination at 350 °C, exhibited the best catalytic activity owing to its faster reaction rate and lower degree of Fe leaching. The results indicate that Fe^（2＋）‐loaded catalysts have significant potential to act as stable and efficient heterogeneous promoters for the photo‐Fenton reaction, with better performance than Fe^3＋‐loaded catalysts because the Fe（II）/Fe（III）compounds formed in the calcination process are necessary to sustain the Fenton reaction. This protocol provides an alternative, environmentally friendly method of reusing digested sludge and demonstrates an easily synthesized mesoporous material that effectively degrades azo dyes.展开更多
Using cetyl-trimethyl-ammonium bromide （CTMAB） as the template agent and tetraethylorthosilicate （TEOS） as the silica source, the MCM-41 mesoporous materials were synthesized with La or Ce incorporated in the fram...Using cetyl-trimethyl-ammonium bromide （CTMAB） as the template agent and tetraethylorthosilicate （TEOS） as the silica source, the MCM-41 mesoporous materials were synthesized with La or Ce incorporated in the framework under hydrothermal conditions. The structure and the state of La or Ce were investigated through the analyses of XRD, nitrogen adsorption-desorption, FT-IR, and UV-Vis. XRD and N2 adsorption-desorption results showed that Ln-MCM-41 exhibited the loss of the lattice ordering of the MCM-41 construct, and larger unit cell parameter and pore diameter than pure silica MCM-41. The FT-IR and UV-Vis results indicated the presence of isolated tetra-coordinated La or Ce ions in the framework and other Ln species dispersed highly on the Ln-MCM-41 surface simultaneously. Furthermore, their catalytic behaviors in the oxidation of styrene were studied using H2O2 as the oxidant. The La-MCM-41 catalysts exhibited high reactivity and the reactivity increased with the increase of the La content in the La-MCM-41 samples. On the contrary, Ce-MCM-41 catalysts showed low reactivity in the oxidation of styrene and the conversion of styrene decreased with the increase of the Ce content in the Ce-MCM-41 samples.展开更多
La-doped and La-B-doped KIT-6 mesoporous materials were prepared by direct hydrothermal synthesis with pH-adjusting method and characterized by X-ray diffractometer(XRD),nitrogen sorption,FT-IR,UV-Vis,X-ray photoelect...La-doped and La-B-doped KIT-6 mesoporous materials were prepared by direct hydrothermal synthesis with pH-adjusting method and characterized by X-ray diffractometer(XRD),nitrogen sorption,FT-IR,UV-Vis,X-ray photoelectron spectroscopy(XPS) and ICP-AES.The catalytic performance for the oxidation of styrene by hydrogen peroxide,tert-butyl hydroperoxide or oxygen was investigated.The results showed that the introduction of heteroatoms did not destroy the mesostructure of KIT-6 with cubic Ia3d space group.La or ...展开更多
The mesoporous Al-SBA-15 zeolite was obtained via impregnation of pure silica-based SBA-15 zeolite with aluminum nitrate.The Al-SBA-15 sample was calcined in air at 800 ℃ for 6 h and hydrothermally treated at near 1...The mesoporous Al-SBA-15 zeolite was obtained via impregnation of pure silica-based SBA-15 zeolite with aluminum nitrate.The Al-SBA-15 sample was calcined in air at 800 ℃ for 6 h and hydrothermally treated at near 100 ℃ for 120 h,respectively,and then the thermal and hydrothermal stability of Al-SBA-15 sample was investigated by X-ray diffractometry (XRD),scanning electron microscopy (SEM),transmission electron microscopy (TEM) and nitrogen adsorption and desorption techniques.The Al-SBA-15 sample was also studied by 27 Al nuclear magnetic resonance (27 Al NMR) and ammonia temperature programmed desorption (NH 3-TPD) techniques.In addition,the catalytic activity of Al-SBA-15 zeolite was investigated by the Friedel-Crafts reactions of 2,4-di-tert-butylphenol with cinnamyl alcohol.The test results showed that the thermal and hydrothermal stability of Al-SBA-15 zeolite was better than that of SBA-15 zeo-lite.The Al-SBA-15 zeolite sample prepared by impregnation method exhibits more framework aluminum species and Al-O-Si units.Therefore,the number of the surface hydroxyl groups was reduced,resulting in the stabilization of framework structure ofAl-SBA-15 zeolite.The aluminum species can form weak and medium-strong acid sites with catalytic activity.展开更多
Although hydrotalcite, or layered double hydroxides （LDHs）, is not a common mineral, it is an important material that can be easily synthesized in laboratory. In this study, structural evolvement and BET surface are...Although hydrotalcite, or layered double hydroxides （LDHs）, is not a common mineral, it is an important material that can be easily synthesized in laboratory. In this study, structural evolvement and BET surface area changes of heat treated Mg/AI-LDH is evaluated by XRD, TEM and N2-BET analyses. The results indicate that the magnesium-aluminum LDH with carbonate as interlayer anion, periclase-like oxides was formed at temperatures of 400-800℃. Meanwhile, 2-3 nanometer mesoporous were formed during decomposition of LDH. However, the heat treated samples still preserve the morphology of the original LDH plates. Periclase-like formed from LDH heat treatment may re-hydrolyze and recover the structure of LDH. However, crystallinity of the recovered LDH is lower than that of the original LDH. This heat treatment will result in formation of （Mg, Al）-oxide nano-crystals and nanopores among the nano-crystals. When heating temperature exceeds 1000, the periclase-like （Mg, Al）-oxide is transformed into a composite with periclase （MgO） and spinel phases. The periclase can be re-hydrolyzed and dissolved in HCl solution. After acid treatment, the sample with a high surface area is composed of spinel nano-crystals and nanopores among them. Our results will provide a new and economic way to synthesize mesoporous materials through pathways of phase transformation of precursor materials with different composition.展开更多
Sulfhydryl MCM-41(SH-MCM-41) mesoporous materials were prepared via a hydrothermal method,and-SH was successfully imported by a post-grafting method.The structure and surface properties of the materials were character...Sulfhydryl MCM-41(SH-MCM-41) mesoporous materials were prepared via a hydrothermal method,and-SH was successfully imported by a post-grafting method.The structure and surface properties of the materials were characterized using Fourier Transform infrared spectroscopy,X-ray diffraction and Transmission Electron Microscopy analysis.The low concentrations of La^3+,Gd^3+ and Yb^3+ adsorption on the material were investigated.This paper discusses the effects of system factors,such as pH and the solid-liquid ratio,on the performance of the adsorption process.The adsorption thermodynamics and kinetics were also explored.Experimental results indicated that the materials were in good order and had high specific surface area(956 m^2/g) with an average pore diameter of 2.1 nm;the mercapto groups were successfully grafted onto a molecular sieve,and the best grafted amount was 1.46×10^-3 mol/g.The materials showed preferable adsorption of La^3+,Gd^3+ and Yb^3+ with maximum adsorption capacities of560.56 mg/g,467.60 mg/g and 540.68 mg/g,respectively.The adsorption process can be described by the Freundlich isotherm model,and the adsorption data fits pseudo-second-order kinetics.After repeating the elution-regeneration cycle four times,the adsorption capacity of rare earth ions was mostly maintained,indicating that the adsorbent can be regenerated well and recycled to save costs.It has potential in practical application.展开更多
Titanium-containing mesoporous molecular sieves are of great significance in selective catalytic oxidation processes with bulky molecules. Recent researches and developments on the designing and synthesis of Ti-contai...Titanium-containing mesoporous molecular sieves are of great significance in selective catalytic oxidation processes with bulky molecules. Recent researches and developments on the designing and synthesis of Ti-containing mesoporous materials have been reviewed. Various strategies for the preparation of Ti-containing mesoporous materials, such as direct synthesis and post-synthesis, are described. Modifications of Ti-containing mesoporous materials by surface-grafting and atom-planting are also discussed. All approaches aimed mainly at the improving of the stability, the hydrophobicity, and mostly the catalytic activity. Structural and mechanistic features of various synthetic systems are discussed. Ticontaining mesoporous materials in liquid phase catalytic oxidation of organic compounds with H2O2 as an oxidant is briefly summarized, showing their broad utilities for green synthesis of fine chemicals by catalytic oxidative reactions.展开更多
We describe the sol-gel synthesis of a new family of organic-inorganic hybrid materials, in which various vinyl polymers are covalently bonded to and uniformly distributed in inorganic oxide matrices. The materials ca...We describe the sol-gel synthesis of a new family of organic-inorganic hybrid materials, in which various vinyl polymers are covalently bonded to and uniformly distributed in inorganic oxide matrices. The materials can be tailored to have both good toughness and hardness while maintaining excellent optical transparency. Doping the sol-gel metal oxides with optically active compounds such as D-glucose results in new optical rotatory composite materials. Removal of the dopant compounds from the composites affords mesoporous oxide materials; which represents a new, nonsurfactant-templated route to mesoporous molecular sieves. We have successfully immobilized a series of enzymes and other bioactive agents in mesoporous materials. Catalytical activities of the enzyme encapsulated in mesoporous materials were found to be much higher than those encapsulated in microporous materials.展开更多
Using cetyl-trimethyl-ammonium bromide （CTMAB） as template and tetraethylortho-silicate （TEOS） as silica source, the MCM-41 mesoporous materials incorporated in framework by Y, Nd and Sm were synthesized by hydrot...Using cetyl-trimethyl-ammonium bromide （CTMAB） as template and tetraethylortho-silicate （TEOS） as silica source, the MCM-41 mesoporous materials incorporated in framework by Y, Nd and Sm were synthesized by hydrothermal synthesis method. The structure, morphology of materials and the state of Y, Nd, Sm in materials were investigated by means of XRD, nitrogen adsorption-desorption, SEM, IR spectrometry, TG-DTA. The XRD results indicate that the samples possess the mesoporous MCM-41 structures with ordered hexagonal arrangements. Y, Nd and Sm ions can get into the framework of mesoporous materials. Nitrogen adsorption desorption isotherms show that the samples have typical mesopores characteristics. SEM micrographs reveal that incorporated sampies show a spherical morphology and the diameters are averagely 0. l0 to 0.15 μm. In IR spectrum of samples, there are the feature adsorption peaks about Si-O-Ln（Ln=Y, Sm, Nd）at 960-985 cm^-1, which affirm that Y, Nd, Sm ions locate in the framework of several mesoporous materials. Results from TG-DTA analysis suggest that two different template sorption sites exist in the framework of YMCM-41, SmMCM-41, NdMCM-41, which powerfully proves that the presence of Y, Nd and Sm in Si framework of the materials.展开更多
Novel layered silinaite has been synthesized using an aqueous mixture of water glass, LiOH and NaOH under hydrothermal crystallization. Subsequently transformation of silinaite into mesoporous materials （SDM） was ac...Novel layered silinaite has been synthesized using an aqueous mixture of water glass, LiOH and NaOH under hydrothermal crystallization. Subsequently transformation of silinaite into mesoporous materials （SDM） was achieved at mild condition using cetyltfimethylammonium bromide as structure-directing agents. The resulting samples were characterized by XRD, SEM, FTIR nitrogen adsorption-desorption isotherms and catalytic performance in bulky molecular involved reaction. The results revealed that synthesized mesoporous materials derived from the silinaite exhibited an ordered hexagonal crystal structure with average pore diameter 2.7 nm and BET surface area 817m^2/g. The SDM-supported ZnCl2 catalyst, prepared by impregnationevaporation method, retained the mesoporous structure and showed high selectivity in alkylation of benzene with benzyl chloride.展开更多
The lanthanum aluminum mesoporous materials were synthesized using sodium dodecyl sulfate as a template agent by ultrasonic hydrothermal method.The resulting samples were characterized by low angle X-ray diffraction（...The lanthanum aluminum mesoporous materials were synthesized using sodium dodecyl sulfate as a template agent by ultrasonic hydrothermal method.The resulting samples were characterized by low angle X-ray diffraction（XRD）,N2 adsorption-desorption studies,transmission electron microscopy（TEM）and surface morphology analysis（SEM）,surface acid（NH3-TPD）,reducibility properties（TPR）,X-ray energy dispersive spectrometer（EDS）and thermogravimetric analysis（TG/DTG）.A l/La composite mesoporous material were synthesized with n（Al）︰n（La）=70︰1.0,80°C of reaction temperature,20 h of reaction time,12 h of crystallization time,650°C of calcination temperature.The specific surface area of the sample is 273.90 m 2 ·g ？1 ,with the average diameter 5.642 nm and pore volume 0.2354 cm 3 ·g ？1 .The samples have mesoporous structure and its particles are similar to a worm-shaped tubular structure.The influence of calcination temperature on the surface physical and chemical properties of Al/La composited mesoporous materials was examined,and the results showed that the acid strength was increased but the amount of acidic sites is decreased as the calcination temperature increased.It was found that the sample calcined at 650°C had appropriate acid content,acid strength and better reducibility.展开更多
Mesoporous materials with the highest surface area were synthesized by hydrothermal treatment from coal-measure kaolin using cetyltrimethylammonium bromide（CTAB）as template.The effect of several factors on surface a...Mesoporous materials with the highest surface area were synthesized by hydrothermal treatment from coal-measure kaolin using cetyltrimethylammonium bromide（CTAB）as template.The effect of several factors on surface area of products also had been discussed.The products were characterized by FT- IR,HRTEM and N 2 adsorption and desorption isotherm plot methods.There was typical structure as Si-O,Si- OH and Si-O-Si of mesoporous materials in the framework of synthesized materials;the pore size distributions of the products showed a sharp peak at 3.82 nm.The effect of hydrothermal treatment time and the amount of template on the specific surface area of mesoporous materials was important,when the Surf/Si=0.135,and hydrothermal time=12 h,and the surface area of the product reached up to 1 070 m2/g,which was higher than other products.展开更多
Using cetyl-trimethyl-ammonium bromide （CTMAB） as template agent and tetraethylorthosilicate （TEOS） as silica Source, the MCM-41 mesoporous materials were synthesized with Y, Nd and Sm incorporated in the framewor...Using cetyl-trimethyl-ammonium bromide （CTMAB） as template agent and tetraethylorthosilicate （TEOS） as silica Source, the MCM-41 mesoporous materials were synthesized with Y, Nd and Sm incorporated in the framework under hydrothermal conditions. The structure and the micro-morphology of the materials and the state of Y, Nd and Sm were investigated through the analyses of XRD, nitrogen adsorption-desorption isotherm, SEM, IR and TG-DTA. The XRD resuits indicate that the synthetic samples are of typical structure of mesoporous MCM-41 with ordered hexagonal arrangements, and Y, Nd and Sm can be incorporated into the framework of these mesoporous materials. Nitrogen adsorption-desorption isotherms show that the samples possess the typical mesopores character. SEM micrographs reveal that the incorporated samples show a well-defined spherical morphology with the diameter ranging 0.10 - 0.15μm. The occurrence of two different template sorption sites in the framework as revealed by TG-DTA analysis further suggests the presence of Y, Nd and Sm in siliceous framework.展开更多
To efficiently address the current high cost associated with preparing pseudo-boehmite from organic aluminum,a low-cost alternative,AlCl_(3),is employed as the raw material.The sol-gel method is utilized,and H_(2)O_(2...To efficiently address the current high cost associated with preparing pseudo-boehmite from organic aluminum,a low-cost alternative,AlCl_(3),is employed as the raw material.The sol-gel method is utilized,and H_(2)O_(2)is incorporated for the modification of pseudo-boehmite.The modification mechanism is thoroughly investigated through the use of X-ray powder diffractometer,scanning electron microscope,and BET data analysis,as well as molecular dynamics simulations.Under specific conditions(temperature at 80°C,pH=7,and H_(2)O_(2)volume ratios of 0.5:1,1:1,and 2:1),mesoporous pseudo-boehmite is synthesized with a specific surface area of 227 m^(2)/g,a pore volume of 0.281 cm^(3)/g,a pore size of 6.78 nm,and a peptizing index of 99.47%.A novel and innovative methodology for the cost-effective production of high-performance alumina is offered through the approach.展开更多
A series of lanthanum doped meosoporous MCM-41 （LaxM41, x is Si/La molar ratio） was prepared by sol-gel method. The surface structure of the materials was investigated with X-ray diffraction and N2 adsorption/desorp...A series of lanthanum doped meosoporous MCM-41 （LaxM41, x is Si/La molar ratio） was prepared by sol-gel method. The surface structure of the materials was investigated with X-ray diffraction and N2 adsorption/desorption technique. The content of La in the materials was determined by ICE It was found that the La content of La25M41, La50M41 and La100M41 was 7.53%, 3.89% and 2.32%, respectively. The phosphate adsorption capacities increased with increasing amount of La incorporation. With 0.40 g La25M41 99.7% phosphate could be removed. The effects of Si/La molar ratio, LaxM41 dose, pH, initial concentration of phosphate solution, co-ions on phosphate adsorption were also evaluated. The phosphate adsorption kinetics of LaxM41 could be well-described by the pseudo second-order model, and Langmuir isotherm fit equilibrium data much better than the Freundlich isotherm.展开更多
Phosphate removal from aqueous waste streams is an important approach to control the eutrophication downstream bodies of water. A Fe（Ⅲ） coordinated amino-functionalized silicate adsorbent for phosphate adsorption w...Phosphate removal from aqueous waste streams is an important approach to control the eutrophication downstream bodies of water. A Fe（Ⅲ） coordinated amino-functionalized silicate adsorbent for phosphate adsorption was synthesized by a post-grafting and metal cation incorporation process. The surface structure of the adsorbent was characterized by X-ray diffraction, N2 adsoropion/desoprotion technique, and Fourier transform infrared spectroscopy. The experimental results showed that the adsorption equilibrium data were well fitted to the Langmuir equation. The maximum adsorption capacity of the modified silicate material was 51.8 mg/g. The kinetic data from the adsorption of phosphate were fitted to pseudo second-order model. The phosphate adsorption was highly pH dependent and the relatively high removal of phosphate fell within the pH range 3.0-6.0. The coexistence of other anions in solutions has an adverse effect on phosphate adsorption; a decrease in adsorption capacity followed the order of exogenous anions： F^- 〉 SO4^2- 〉 NO3^- 〉 Cl^-. In addition, the adsorbed phosphate could be desorbed by NaOH solutions. This silicate adsorbent with a large adsorption capacity and relatively high selectivity could be utilized for the removal of phosphate from aqueous waste streams or in aquatic environment.展开更多
A series of mesoporous Cu-Mn-Al2O3（CMA） materials was synthesized at moderate temperature and their structures were characterized by XRD, N2 physical adsorption and TPR techniques. It was found that using metal comp...A series of mesoporous Cu-Mn-Al2O3（CMA） materials was synthesized at moderate temperature and their structures were characterized by XRD, N2 physical adsorption and TPR techniques. It was found that using metal complex ion[Cu（NH3） 4^2＋-Mn（NH3）6^2＋] as raw materials is easier to form good-structure mesoporous Cu-Mn-Al2O3 materials than using its nitrate salt [Cu（NO3）2-Mn（NO3）2]. The TPR tests results indicate that CuO and MnOx were homogeneously dispersed in the mesoporous materials. Their catalytic application to preferential catalytic oxidation of CO in a hydrogen-rich stream was studied. The activity varies in the order of CMA（1：1, molar ratio）〉 CMA（1：2）〉CMA（2：1）〉CMA（CP）〉CMA（1：0）≈CMA（0：1）. The CMA（1：0） and CMA（0：1） have lower activity compared to other samples, implying that there existed coordination effect between Cu-Mn in the samples. The selectivity varied in the order of CMA（0：1）≥CMA（1：2）〉CMA（1：1）〉CMA（2：1）〉CMA（1：0） at higher temperature （≥ 120 ℃）, indicating that increasing the Cu content enhanced the conversion of H2. The sample CMA（CP） made by coprecipitation method has a lower CO oxidation activity and selectivity than its counter-parts of mesoporous Cu-Mn-Al2O3 materials[CMA（1：2）], this attributed to the lower surface area of the former and poor interaction of CuO with MnOx.展开更多
H2S can cause multiple diseases and poses a great threat to human health.However,the precise detection of extremely toxic H2S at room temperature is still a great challenge.Here,a facile solvent evaporation induced ag...H2S can cause multiple diseases and poses a great threat to human health.However,the precise detection of extremely toxic H2S at room temperature is still a great challenge.Here,a facile solvent evaporation induced aggregating assembly(EIAA)method has been applied for the production of ordered mesoporous carbon(OMCs)in an acidic THF/H2 O solution with high-molecular-weight poly(ethylene oxide)-b-polystyrene(PEO-b-PS)copolymers as the structure-directing agent,formaldehyde and resorcinol as carbon precursors.Along with the continuous evaporation of THF from the mixed solution,cylindrical micelles are formed in the solution and further assemble into highly ordered mesostructure.The obtained OMCs possesses a two-dimensional(2 D)hexagonal mesostructure with uniform and large pore diameter(~19.2 nm),high surface area(599 m2/g),and large pore volume(0.92 cm3/g).When being used as the resonant cantilever gas sensor for room-temperature H2S detection,the OMCs has delivered not only a superior gas sensing performance with ultrafast re s ponse(14 s)and recovery(21 s)even at low concentration(2 ppm)but also an excellent selectivity toward H2S among various common interfering gases.Moreover,the limit of detection is better than 0.2 ppm,indicating its potential application in environmental monitoring and health protection.展开更多
Protein phosphorylation as one of the most important post-translational modifications in mammalian cells regulates numerous biological processes. Here we propose a novel strategy for the selective isolation and sensit...Protein phosphorylation as one of the most important post-translational modifications in mammalian cells regulates numerous biological processes. Here we propose a novel strategy for the selective isolation and sensitive analysis of mul- ti-phosphopeptides based on TiO2-gratfed mesoporous materials, in which MCM-41 and SBA-15 were chosen as the hard templates. The commercialized IMAC and TiO2 nanopartices were further investigated in the phosphopeptide analysis for comparison. The enrichment efficiency was evaluated and measured by MALDI-TOF mass spectrometry. The results indicated that both TiO2-SBA-15 and TiO2-MCM-41 exhibited the preferential affinity to multi-phosphopeptides compared with the other two widely used strategies. The mesoporous TiO2 based protocol showed highly selective and sensitive properties, where phosphopepddes could be identified at femtomole.展开更多
基金supported by the National Natural Science Foundation of China(52370041)National Natural Science Foundation of China(21976134 and 21707104)State Key Laboratory of Pollution treatment and Resource Reuse Foundation(NO.PCRRK21001).
文摘To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
基金supported by the National Key Technology Research&Development Program of China(2014BAL02B02)the National Natural Science Foundation of China(51578397)~~
文摘The anaerobic digestion of sludge has recently received increased interest because of the potential to transform organic matter into methane‐rich biogas. However, digested sludge, the residue produced in that process, still contains high levels of heavy metals and other harmful substances that might make traditional disposal difficult. We have devised a facile method of converting digested sludge into a mesoporous material that acts as an effective and stable heterogeneous catalyst for the photo‐Fenton reaction. A comparison of the removal of rhodamine B under different conditions showed that FAS‐1‐350, which was synthesized by mixing the digested sludge with a 1 mol/L（NH4）2Fe（SO4）2 solution followed by calcination at 350 °C, exhibited the best catalytic activity owing to its faster reaction rate and lower degree of Fe leaching. The results indicate that Fe^（2＋）‐loaded catalysts have significant potential to act as stable and efficient heterogeneous promoters for the photo‐Fenton reaction, with better performance than Fe^3＋‐loaded catalysts because the Fe（II）/Fe（III）compounds formed in the calcination process are necessary to sustain the Fenton reaction. This protocol provides an alternative, environmentally friendly method of reusing digested sludge and demonstrates an easily synthesized mesoporous material that effectively degrades azo dyes.
基金Project supported by the National Basic Research Program of China (2004CB719500)the Commission of Science and Technology of Shanghai Municipality (03DJ14006)
文摘Using cetyl-trimethyl-ammonium bromide （CTMAB） as the template agent and tetraethylorthosilicate （TEOS） as the silica source, the MCM-41 mesoporous materials were synthesized with La or Ce incorporated in the framework under hydrothermal conditions. The structure and the state of La or Ce were investigated through the analyses of XRD, nitrogen adsorption-desorption, FT-IR, and UV-Vis. XRD and N2 adsorption-desorption results showed that Ln-MCM-41 exhibited the loss of the lattice ordering of the MCM-41 construct, and larger unit cell parameter and pore diameter than pure silica MCM-41. The FT-IR and UV-Vis results indicated the presence of isolated tetra-coordinated La or Ce ions in the framework and other Ln species dispersed highly on the Ln-MCM-41 surface simultaneously. Furthermore, their catalytic behaviors in the oxidation of styrene were studied using H2O2 as the oxidant. The La-MCM-41 catalysts exhibited high reactivity and the reactivity increased with the increase of the La content in the La-MCM-41 samples. On the contrary, Ce-MCM-41 catalysts showed low reactivity in the oxidation of styrene and the conversion of styrene decreased with the increase of the Ce content in the Ce-MCM-41 samples.
基金supported by the National Basic Research Program of China (2010CB732300)Education Commission of Shanghai Municipality (2008CG35)Science and Technology Commission of Shanghai Municipality (09ZR1408200)
文摘La-doped and La-B-doped KIT-6 mesoporous materials were prepared by direct hydrothermal synthesis with pH-adjusting method and characterized by X-ray diffractometer(XRD),nitrogen sorption,FT-IR,UV-Vis,X-ray photoelectron spectroscopy(XPS) and ICP-AES.The catalytic performance for the oxidation of styrene by hydrogen peroxide,tert-butyl hydroperoxide or oxygen was investigated.The results showed that the introduction of heteroatoms did not destroy the mesostructure of KIT-6 with cubic Ia3d space group.La or ...
文摘The mesoporous Al-SBA-15 zeolite was obtained via impregnation of pure silica-based SBA-15 zeolite with aluminum nitrate.The Al-SBA-15 sample was calcined in air at 800 ℃ for 6 h and hydrothermally treated at near 100 ℃ for 120 h,respectively,and then the thermal and hydrothermal stability of Al-SBA-15 sample was investigated by X-ray diffractometry (XRD),scanning electron microscopy (SEM),transmission electron microscopy (TEM) and nitrogen adsorption and desorption techniques.The Al-SBA-15 sample was also studied by 27 Al nuclear magnetic resonance (27 Al NMR) and ammonia temperature programmed desorption (NH 3-TPD) techniques.In addition,the catalytic activity of Al-SBA-15 zeolite was investigated by the Friedel-Crafts reactions of 2,4-di-tert-butylphenol with cinnamyl alcohol.The test results showed that the thermal and hydrothermal stability of Al-SBA-15 zeolite was better than that of SBA-15 zeo-lite.The Al-SBA-15 zeolite sample prepared by impregnation method exhibits more framework aluminum species and Al-O-Si units.Therefore,the number of the surface hydroxyl groups was reduced,resulting in the stabilization of framework structure ofAl-SBA-15 zeolite.The aluminum species can form weak and medium-strong acid sites with catalytic activity.
基金the National Natural Science Foundation of China （No. 40472026） the 0utstanding 0verseas Chinese Scholars Fund of Chinese Academy of Sciences （2003-1-7）.
文摘Although hydrotalcite, or layered double hydroxides （LDHs）, is not a common mineral, it is an important material that can be easily synthesized in laboratory. In this study, structural evolvement and BET surface area changes of heat treated Mg/AI-LDH is evaluated by XRD, TEM and N2-BET analyses. The results indicate that the magnesium-aluminum LDH with carbonate as interlayer anion, periclase-like oxides was formed at temperatures of 400-800℃. Meanwhile, 2-3 nanometer mesoporous were formed during decomposition of LDH. However, the heat treated samples still preserve the morphology of the original LDH plates. Periclase-like formed from LDH heat treatment may re-hydrolyze and recover the structure of LDH. However, crystallinity of the recovered LDH is lower than that of the original LDH. This heat treatment will result in formation of （Mg, Al）-oxide nano-crystals and nanopores among the nano-crystals. When heating temperature exceeds 1000, the periclase-like （Mg, Al）-oxide is transformed into a composite with periclase （MgO） and spinel phases. The periclase can be re-hydrolyzed and dissolved in HCl solution. After acid treatment, the sample with a high surface area is composed of spinel nano-crystals and nanopores among them. Our results will provide a new and economic way to synthesize mesoporous materials through pathways of phase transformation of precursor materials with different composition.
文摘Sulfhydryl MCM-41(SH-MCM-41) mesoporous materials were prepared via a hydrothermal method,and-SH was successfully imported by a post-grafting method.The structure and surface properties of the materials were characterized using Fourier Transform infrared spectroscopy,X-ray diffraction and Transmission Electron Microscopy analysis.The low concentrations of La^3+,Gd^3+ and Yb^3+ adsorption on the material were investigated.This paper discusses the effects of system factors,such as pH and the solid-liquid ratio,on the performance of the adsorption process.The adsorption thermodynamics and kinetics were also explored.Experimental results indicated that the materials were in good order and had high specific surface area(956 m^2/g) with an average pore diameter of 2.1 nm;the mercapto groups were successfully grafted onto a molecular sieve,and the best grafted amount was 1.46×10^-3 mol/g.The materials showed preferable adsorption of La^3+,Gd^3+ and Yb^3+ with maximum adsorption capacities of560.56 mg/g,467.60 mg/g and 540.68 mg/g,respectively.The adsorption process can be described by the Freundlich isotherm model,and the adsorption data fits pseudo-second-order kinetics.After repeating the elution-regeneration cycle four times,the adsorption capacity of rare earth ions was mostly maintained,indicating that the adsorbent can be regenerated well and recycled to save costs.It has potential in practical application.
基金the national natural science foundation of China (No.20541002)SINOPEC basic research foundation (X504034) Zhejiang provincial natural science foundation (No.Y405064)
文摘Titanium-containing mesoporous molecular sieves are of great significance in selective catalytic oxidation processes with bulky molecules. Recent researches and developments on the designing and synthesis of Ti-containing mesoporous materials have been reviewed. Various strategies for the preparation of Ti-containing mesoporous materials, such as direct synthesis and post-synthesis, are described. Modifications of Ti-containing mesoporous materials by surface-grafting and atom-planting are also discussed. All approaches aimed mainly at the improving of the stability, the hydrophobicity, and mostly the catalytic activity. Structural and mechanistic features of various synthetic systems are discussed. Ticontaining mesoporous materials in liquid phase catalytic oxidation of organic compounds with H2O2 as an oxidant is briefly summarized, showing their broad utilities for green synthesis of fine chemicals by catalytic oxidative reactions.
基金This work has been supported by the US National Institutes of Health (No. RO1-DE09848 to YW) and Natural Science Foundation of China (NSFC Nos. 29674001 and 19810760343 to KYQ and YW).
文摘We describe the sol-gel synthesis of a new family of organic-inorganic hybrid materials, in which various vinyl polymers are covalently bonded to and uniformly distributed in inorganic oxide matrices. The materials can be tailored to have both good toughness and hardness while maintaining excellent optical transparency. Doping the sol-gel metal oxides with optically active compounds such as D-glucose results in new optical rotatory composite materials. Removal of the dopant compounds from the composites affords mesoporous oxide materials; which represents a new, nonsurfactant-templated route to mesoporous molecular sieves. We have successfully immobilized a series of enzymes and other bioactive agents in mesoporous materials. Catalytical activities of the enzyme encapsulated in mesoporous materials were found to be much higher than those encapsulated in microporous materials.
文摘Using cetyl-trimethyl-ammonium bromide （CTMAB） as template and tetraethylortho-silicate （TEOS） as silica source, the MCM-41 mesoporous materials incorporated in framework by Y, Nd and Sm were synthesized by hydrothermal synthesis method. The structure, morphology of materials and the state of Y, Nd, Sm in materials were investigated by means of XRD, nitrogen adsorption-desorption, SEM, IR spectrometry, TG-DTA. The XRD results indicate that the samples possess the mesoporous MCM-41 structures with ordered hexagonal arrangements. Y, Nd and Sm ions can get into the framework of mesoporous materials. Nitrogen adsorption desorption isotherms show that the samples have typical mesopores characteristics. SEM micrographs reveal that incorporated sampies show a spherical morphology and the diameters are averagely 0. l0 to 0.15 μm. In IR spectrum of samples, there are the feature adsorption peaks about Si-O-Ln（Ln=Y, Sm, Nd）at 960-985 cm^-1, which affirm that Y, Nd, Sm ions locate in the framework of several mesoporous materials. Results from TG-DTA analysis suggest that two different template sorption sites exist in the framework of YMCM-41, SmMCM-41, NdMCM-41, which powerfully proves that the presence of Y, Nd and Sm in Si framework of the materials.
基金Fund supports by the National Natural Science Foundation of China （No,20541002）Zhejiang Provincial Natural Science Foundation （No.Y405064） are acknowledged.
文摘Novel layered silinaite has been synthesized using an aqueous mixture of water glass, LiOH and NaOH under hydrothermal crystallization. Subsequently transformation of silinaite into mesoporous materials （SDM） was achieved at mild condition using cetyltfimethylammonium bromide as structure-directing agents. The resulting samples were characterized by XRD, SEM, FTIR nitrogen adsorption-desorption isotherms and catalytic performance in bulky molecular involved reaction. The results revealed that synthesized mesoporous materials derived from the silinaite exhibited an ordered hexagonal crystal structure with average pore diameter 2.7 nm and BET surface area 817m^2/g. The SDM-supported ZnCl2 catalyst, prepared by impregnationevaporation method, retained the mesoporous structure and showed high selectivity in alkylation of benzene with benzyl chloride.
文摘The lanthanum aluminum mesoporous materials were synthesized using sodium dodecyl sulfate as a template agent by ultrasonic hydrothermal method.The resulting samples were characterized by low angle X-ray diffraction（XRD）,N2 adsorption-desorption studies,transmission electron microscopy（TEM）and surface morphology analysis（SEM）,surface acid（NH3-TPD）,reducibility properties（TPR）,X-ray energy dispersive spectrometer（EDS）and thermogravimetric analysis（TG/DTG）.A l/La composite mesoporous material were synthesized with n（Al）︰n（La）=70︰1.0,80°C of reaction temperature,20 h of reaction time,12 h of crystallization time,650°C of calcination temperature.The specific surface area of the sample is 273.90 m 2 ·g ？1 ,with the average diameter 5.642 nm and pore volume 0.2354 cm 3 ·g ？1 .The samples have mesoporous structure and its particles are similar to a worm-shaped tubular structure.The influence of calcination temperature on the surface physical and chemical properties of Al/La composited mesoporous materials was examined,and the results showed that the acid strength was increased but the amount of acidic sites is decreased as the calcination temperature increased.It was found that the sample calcined at 650°C had appropriate acid content,acid strength and better reducibility.
基金Funded by Social Development Plan of Jiangsu Department of the Science and Technology,Jiangsu,China(No.BS2007038)
文摘Mesoporous materials with the highest surface area were synthesized by hydrothermal treatment from coal-measure kaolin using cetyltrimethylammonium bromide（CTAB）as template.The effect of several factors on surface area of products also had been discussed.The products were characterized by FT- IR,HRTEM and N 2 adsorption and desorption isotherm plot methods.There was typical structure as Si-O,Si- OH and Si-O-Si of mesoporous materials in the framework of synthesized materials;the pore size distributions of the products showed a sharp peak at 3.82 nm.The effect of hydrothermal treatment time and the amount of template on the specific surface area of mesoporous materials was important,when the Surf/Si=0.135,and hydrothermal time=12 h,and the surface area of the product reached up to 1 070 m2/g,which was higher than other products.
文摘Using cetyl-trimethyl-ammonium bromide （CTMAB） as template agent and tetraethylorthosilicate （TEOS） as silica Source, the MCM-41 mesoporous materials were synthesized with Y, Nd and Sm incorporated in the framework under hydrothermal conditions. The structure and the micro-morphology of the materials and the state of Y, Nd and Sm were investigated through the analyses of XRD, nitrogen adsorption-desorption isotherm, SEM, IR and TG-DTA. The XRD resuits indicate that the synthetic samples are of typical structure of mesoporous MCM-41 with ordered hexagonal arrangements, and Y, Nd and Sm can be incorporated into the framework of these mesoporous materials. Nitrogen adsorption-desorption isotherms show that the samples possess the typical mesopores character. SEM micrographs reveal that the incorporated samples show a well-defined spherical morphology with the diameter ranging 0.10 - 0.15μm. The occurrence of two different template sorption sites in the framework as revealed by TG-DTA analysis further suggests the presence of Y, Nd and Sm in siliceous framework.
基金Funded by the National Natural Science Foundation of China(Nos.22068021 and 52064030)the Yunnan Young and Middle-aged Academic and Technical Leaders Reserve Talent Program of China(No.202305AC160064)the Yunnan Major Scientific and Technological Program of China(Nos.202402AB080004,202202AG050011,and 202202AG050007)。
文摘To efficiently address the current high cost associated with preparing pseudo-boehmite from organic aluminum,a low-cost alternative,AlCl_(3),is employed as the raw material.The sol-gel method is utilized,and H_(2)O_(2)is incorporated for the modification of pseudo-boehmite.The modification mechanism is thoroughly investigated through the use of X-ray powder diffractometer,scanning electron microscope,and BET data analysis,as well as molecular dynamics simulations.Under specific conditions(temperature at 80°C,pH=7,and H_(2)O_(2)volume ratios of 0.5:1,1:1,and 2:1),mesoporous pseudo-boehmite is synthesized with a specific surface area of 227 m^(2)/g,a pore volume of 0.281 cm^(3)/g,a pore size of 6.78 nm,and a peptizing index of 99.47%.A novel and innovative methodology for the cost-effective production of high-performance alumina is offered through the approach.
基金supported by the National Major Research Plan for Water Pollution Control and Treatment of China (No.2008ZX07101-015)
文摘A series of lanthanum doped meosoporous MCM-41 （LaxM41, x is Si/La molar ratio） was prepared by sol-gel method. The surface structure of the materials was investigated with X-ray diffraction and N2 adsorption/desorption technique. The content of La in the materials was determined by ICE It was found that the La content of La25M41, La50M41 and La100M41 was 7.53%, 3.89% and 2.32%, respectively. The phosphate adsorption capacities increased with increasing amount of La incorporation. With 0.40 g La25M41 99.7% phosphate could be removed. The effects of Si/La molar ratio, LaxM41 dose, pH, initial concentration of phosphate solution, co-ions on phosphate adsorption were also evaluated. The phosphate adsorption kinetics of LaxM41 could be well-described by the pseudo second-order model, and Langmuir isotherm fit equilibrium data much better than the Freundlich isotherm.
基金supported by the National Major Research Plan for Water Pollution Control and Treatment of China(No. 2009ZX07101-015,2009ZX07105-003)
文摘Phosphate removal from aqueous waste streams is an important approach to control the eutrophication downstream bodies of water. A Fe（Ⅲ） coordinated amino-functionalized silicate adsorbent for phosphate adsorption was synthesized by a post-grafting and metal cation incorporation process. The surface structure of the adsorbent was characterized by X-ray diffraction, N2 adsoropion/desoprotion technique, and Fourier transform infrared spectroscopy. The experimental results showed that the adsorption equilibrium data were well fitted to the Langmuir equation. The maximum adsorption capacity of the modified silicate material was 51.8 mg/g. The kinetic data from the adsorption of phosphate were fitted to pseudo second-order model. The phosphate adsorption was highly pH dependent and the relatively high removal of phosphate fell within the pH range 3.0-6.0. The coexistence of other anions in solutions has an adverse effect on phosphate adsorption; a decrease in adsorption capacity followed the order of exogenous anions： F^- 〉 SO4^2- 〉 NO3^- 〉 Cl^-. In addition, the adsorbed phosphate could be desorbed by NaOH solutions. This silicate adsorbent with a large adsorption capacity and relatively high selectivity could be utilized for the removal of phosphate from aqueous waste streams or in aquatic environment.
基金Supported by the Science and Technology Development Project of Shandong Province,China(No.2007GG3WZ03018)
文摘A series of mesoporous Cu-Mn-Al2O3（CMA） materials was synthesized at moderate temperature and their structures were characterized by XRD, N2 physical adsorption and TPR techniques. It was found that using metal complex ion[Cu（NH3） 4^2＋-Mn（NH3）6^2＋] as raw materials is easier to form good-structure mesoporous Cu-Mn-Al2O3 materials than using its nitrate salt [Cu（NO3）2-Mn（NO3）2]. The TPR tests results indicate that CuO and MnOx were homogeneously dispersed in the mesoporous materials. Their catalytic application to preferential catalytic oxidation of CO in a hydrogen-rich stream was studied. The activity varies in the order of CMA（1：1, molar ratio）〉 CMA（1：2）〉CMA（2：1）〉CMA（CP）〉CMA（1：0）≈CMA（0：1）. The CMA（1：0） and CMA（0：1） have lower activity compared to other samples, implying that there existed coordination effect between Cu-Mn in the samples. The selectivity varied in the order of CMA（0：1）≥CMA（1：2）〉CMA（1：1）〉CMA（2：1）〉CMA（1：0） at higher temperature （≥ 120 ℃）, indicating that increasing the Cu content enhanced the conversion of H2. The sample CMA（CP） made by coprecipitation method has a lower CO oxidation activity and selectivity than its counter-parts of mesoporous Cu-Mn-Al2O3 materials[CMA（1：2）], this attributed to the lower surface area of the former and poor interaction of CuO with MnOx.
基金supported by the National Natural Science Foundation of China(Nos.51822202 and 51772050)Shanghai Rising-Star Program(No.18QA1400100)+3 种基金Youth Top-notch Talent Support Program of Shanghai,the Shanghai Committee of Science and Technology,China(No.19520713200)Key Research Program of Frontier Sciences of Chinese Academy of Sciences(No.QYZDJSSW-JSC001)DHU Distinguished Young Professor Program and Fundamental Research Funds for the Central Universitiessupport of the Youth Innovation Promotion Association CAS(No.2016213)。
文摘H2S can cause multiple diseases and poses a great threat to human health.However,the precise detection of extremely toxic H2S at room temperature is still a great challenge.Here,a facile solvent evaporation induced aggregating assembly(EIAA)method has been applied for the production of ordered mesoporous carbon(OMCs)in an acidic THF/H2 O solution with high-molecular-weight poly(ethylene oxide)-b-polystyrene(PEO-b-PS)copolymers as the structure-directing agent,formaldehyde and resorcinol as carbon precursors.Along with the continuous evaporation of THF from the mixed solution,cylindrical micelles are formed in the solution and further assemble into highly ordered mesostructure.The obtained OMCs possesses a two-dimensional(2 D)hexagonal mesostructure with uniform and large pore diameter(~19.2 nm),high surface area(599 m2/g),and large pore volume(0.92 cm3/g).When being used as the resonant cantilever gas sensor for room-temperature H2S detection,the OMCs has delivered not only a superior gas sensing performance with ultrafast re s ponse(14 s)and recovery(21 s)even at low concentration(2 ppm)but also an excellent selectivity toward H2S among various common interfering gases.Moreover,the limit of detection is better than 0.2 ppm,indicating its potential application in environmental monitoring and health protection.
基金supported by the National Basic Research Program of Chi-na (2007CB714506)the National Natural Science Foundation of China (20735005 & 20925517)+1 种基金Science and Technology Committee of Shanghai (10XD1406000 & 09JC1402600)Shanghai Leading Academic Disci-pline B109
文摘Protein phosphorylation as one of the most important post-translational modifications in mammalian cells regulates numerous biological processes. Here we propose a novel strategy for the selective isolation and sensitive analysis of mul- ti-phosphopeptides based on TiO2-gratfed mesoporous materials, in which MCM-41 and SBA-15 were chosen as the hard templates. The commercialized IMAC and TiO2 nanopartices were further investigated in the phosphopeptide analysis for comparison. The enrichment efficiency was evaluated and measured by MALDI-TOF mass spectrometry. The results indicated that both TiO2-SBA-15 and TiO2-MCM-41 exhibited the preferential affinity to multi-phosphopeptides compared with the other two widely used strategies. The mesoporous TiO2 based protocol showed highly selective and sensitive properties, where phosphopepddes could be identified at femtomole.
