The ordered bimodal mesoporous silica MCM-48 spheres were facile synthesized by mild- temperature post-synthesis H2O2 hydrothermal treatment of as-synthesized MCM-48. The results showed that H2O2 is indispensable for ...The ordered bimodal mesoporous silica MCM-48 spheres were facile synthesized by mild- temperature post-synthesis H2O2 hydrothermal treatment of as-synthesized MCM-48. The results showed that H2O2 is indispensable for simultaneously removing organic templates and forming ordered bimodal mesoporous silica MCM-48 spheres. The bimodal mesoporous MCM-48 was characterized by X-ray diffraction, transmission electron micrographs, FT-IR, and N2 adsorption-desorption, and a possible mechanism was proposed for the formation of bimodal mesoporous MCM-48.展开更多
By using the bimodal mesoporous silica(BMMS) as the carrier and butyl titanate as the titanium source, the TiO_2/BMMS catalyst was prepared. The samples were characterized by XRD, XRF, N_2 adsorption and desorption, F...By using the bimodal mesoporous silica(BMMS) as the carrier and butyl titanate as the titanium source, the TiO_2/BMMS catalyst was prepared. The samples were characterized by XRD, XRF, N_2 adsorption and desorption, FTIR, UVvis,SEM, EDS, and TEM techniques. The test results showed that TiO_2 was amorphous, the TiO_2/BMMS catalyst had an ordered bimodal mesoporous structure, and the chemical interaction existed between BMMS and TiO_2. Since the TiO_2/BMMS had a lower band gap, its photocatalytic activity was better than TiO_2. Under UV irradiation a one-pot PODS system was set up, using TiO_2/BMMS as the catalyst, H_2O_2 as the oxidant, and methanol as the solvent. The TiO_2/BMMS catalyst showed better photocatalytic activity than the mono-modal mesoporous TiO_2/SBA-15 catalyst, and the desulfurization rate of dibenzothiophene(DBT) over TiO_2/BMMS catalyst could reach 99._2%. The TiO_2/BMMS catalyst also had so good stability that the desulfurization rate of DBT did not drop apparently after 8 cycles of reusing, and could still be close to 90%.展开更多
Cobalt oxide catalysts supported on mesoporous silica （Co3O4/MPS） were prepared, characterized and applied for catalytic oxidation of NO. Effects of catalyst supports, calcination temperatures, H2O and SO2 on NO con...Cobalt oxide catalysts supported on mesoporous silica （Co3O4/MPS） were prepared, characterized and applied for catalytic oxidation of NO. Effects of catalyst supports, calcination temperatures, H2O and SO2 on NO conversion were investigated. The samples were also characterized by BET, XRD, FTIR and TG/DTG. The results suggested that Co3O4/MPS catalyst calcined at 573 K had the smallest crystal particles and the best surface dispersion. This catalyst had the highest activity and yielded 82% NO conversion at 573 K, at a space velocity of 12000 h^-1. Although the conversion of NO decreased with the introduction of H2O, it could be restored completely after removing residual H2O from Co3O4/MPS catalyst by heating at 573 K. In the presence of SO2, the oxidation activity decreased and COSO4 was detected on the catalyst. The NO conversion decreased to 30.2% in the presence of SO2 and H2O. It could not be restored completely after cutting off H2O and SO2. The deactivation of the catalyst in the presence of SO2 and H2O was attributed to the formation of cobalt sulfate species.展开更多
A rational integration of multiple reactive centers into a combined unit to facilitate their cooperative effects is a smart approach for accelerating the catalytic activity.Here,to achieve this goal,linear imidazolium...A rational integration of multiple reactive centers into a combined unit to facilitate their cooperative effects is a smart approach for accelerating the catalytic activity.Here,to achieve this goal,linear imidazolium-based ionic polymers were confined into the nanopores of mesoporous silica nanospheres anchored with homogeneously distributed zinc salts.Owing to the flexible character and the reinforced cooperative effects of the ionic liquid(nucleophile)and zinc species(Lewis acid)in the confined mesoporous structure,the resultant composite exhibited dramatically improved catalytic performance in the cycloaddition of CO2 with epoxides to form cyclic carbonates.This was in contrast to that observed for the individual catalytic components.Moreover,such a solid catalyst could be easily recovered and reused four times without a significant loss of activity.展开更多
Amine-functionalized mesoporous silica was prepared by using lauric acid and N-stearoyl-l-glutamic acid as structure directing agents via the S-N+-I- mechanism and applied to CO2 adsorption at room temperature. With ...Amine-functionalized mesoporous silica was prepared by using lauric acid and N-stearoyl-l-glutamic acid as structure directing agents via the S-N+-I- mechanism and applied to CO2 adsorption at room temperature. With γ-aminopropyltriethoxysilane as co-structure directing agent and due to the direct electrostatic interaction with anionic surfactant, most of the amino groups were uniformly distributed at the inner surface of pores and the per- formance was stable. The amine-functionalized mesoporous silica was characterized by Fourier transform infrared spectrometer, X-ray diffraction, nitrogen physisorption and thermogravimetric analysis. The CO2 adsorption capacity was measured by digital recording balance. At the room temperature and under the atmospheric pressure, the adsorption capacity of LAA-AMS-0.2 for CO2 and N2 is 1.40 mmol·g-1 and 0.03 mmol·g-1, respectively, indicating high separation coefficient of CO2/N2.展开更多
Supported nanocrystalline TiO2 with a diameter of 15–30 nm was prepared from previously synthesized radial mesoporous silica（RMS） by a post-synthesis method. In addition, their adsorption-photocatalytic activity to...Supported nanocrystalline TiO2 with a diameter of 15–30 nm was prepared from previously synthesized radial mesoporous silica（RMS） by a post-synthesis method. In addition, their adsorption-photocatalytic activity toward the degradation of methylene blue（MB） was determined. RMS was tailor-made with the main template of CTAB and the SiO2 precursor of TEOS through a facile self-assembly process. The structural, morphological and textural properties of the well-designed TiO2/RMS samples were characterized.The RMS structure was retained after loading TiO2, but its surface area and pore diameter decreased as a result of partial pore blocking. The removal activity of MB for TiO2/RMS was significantly higher than that of commercial TiO2 nanoparticles. The optimal TiO2 loading（20 wt%） on the support could achieve the complete removal of MB within 70 min. The prepared TiO2/RMS particles can be easily separated and display good durability after six reaction cycles.展开更多
Chemical modification/ambient drying method and freeze drying method were introduced to research the synthesis of mesoporous silica aerogels. By analyzing N2 gas adsorption/desorption isotherms, the fractal geometric ...Chemical modification/ambient drying method and freeze drying method were introduced to research the synthesis of mesoporous silica aerogels. By analyzing N2 gas adsorption/desorption isotherms, the fractal geometric characteristics of gels were focused. The overall surface fractal dimensions were determined by analyzing N2 gas adsorption branch and a Frenkel-Halsey-Hill （FHH） equation was empolyed to determine surface fractal dimension Df It is found that, during ambient drying process, VTMCS/VWetgel ratio plays a crucial role in the changes of geometric feature, the key point is 50%, when the ratio is lower, and surface roughness increases with the ratio, when it exceeds 50%, the surface is almost unaffected by the modification. While freeze drying always tends to get larger Df freeze drying process could cause a rough surface of the gels. Compared with traditional porosity and specific surface area analyses, fractal geometry may be expected to be favorable for mesoporous structural analyses of materials.展开更多
The mesoporous silica modifed with magnesium ox- ide （MgO） was syntbesized by one step method and impregnating method, respectively. The samples were characterized by small angle X-Ray diffraction （XRD）, N2 adsorp...The mesoporous silica modifed with magnesium ox- ide （MgO） was syntbesized by one step method and impregnating method, respectively. The samples were characterized by small angle X-Ray diffraction （XRD）, N2 adsorption-desorption and transmission electron microscopy （TEM）, and the carbon dioxide adsorption capacity was analyzed by thermal gravimetric analysis （TGA）. Compared with the original mesoporous silica （20.7 mg/g）, the CO2 adsorption capacity of MgO-modified mesoporous silica processed by one step method increases to 32.9 mg/g. Although its surface area greatly decreases compared with that of the original mesoporous silica, the MgO-modified mesoporous silica prepared by impregnating reaches an adsorptive value of 31.1 mg/g because the number of basic sites increases on the surface of the mesoporous silica.展开更多
Reverse water gas shift(RWGS)reaction is a crucial process in CO_(2)utilization.Herein,Ni-and NiCe-containing hexagonal mesoporous silica(Ni-HMS and NiCe-HMS)catalysts were synthesized using an insitu one-pot method a...Reverse water gas shift(RWGS)reaction is a crucial process in CO_(2)utilization.Herein,Ni-and NiCe-containing hexagonal mesoporous silica(Ni-HMS and NiCe-HMS)catalysts were synthesized using an insitu one-pot method and applied for RWGS reaction.At certain reaction temperatures 500-750℃,Ni-HMS samples displayed a higher selectivity to the preferable CO than that of conventionally impregnated Ni/HMS catalyst.This could be originated from the smaller NiO nanoparticles over Ni-HMS catalyst.NiCe-HMS exhibited higher activity compared to Ni-HMS.The catalysts were characterized by means of TEM,XPS,XRD,H_(2)-TPR,CO_(2)-TPD,EPR and N_(2) adsorption-desortion technology.It was found that introduction of Ce created high concentration of oxygen vacancies,served as the active site for activating CO_(2).Also,this work analyzed the effect of the H_(2)/CO_(2)molar ratio on the best NiCe-HMS.When reaction gas H_(2)/CO_(2)molar ratio was 4 significantly decreased the selectivity to CO at low temperature,but triggered a higher CO_(2)conversion which is close to the equilibrium.展开更多
Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially acces...Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar vip species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.展开更多
A CO2 solid sorbent based on polyethyleneimine 10k (PEI-10k) impregnated into mesoporous silica (MPS) foam was synthesized and utilized to capture CO2 at temperatures ranged from 65°C to 95°C. The calculated...A CO2 solid sorbent based on polyethyleneimine 10k (PEI-10k) impregnated into mesoporous silica (MPS) foam was synthesized and utilized to capture CO2 at temperatures ranged from 65°C to 95°C. The calculated nitrogen and carbon contents in the bulk of the PEI-10k/MPS sorbent were similar to the XPS results measured on the surface of the foam, suggesting that the PEI was homo-geneously distributed throughout the MPS support. After CO2 adsorptionthe N 1s peak was broadened and could be resolved into two components: a high binding energy component (~401 eV) and a lower binding energy one (396 eV), respectively. The former nitrogen states are consistent with a protonated amine, presumably, due to carbamate formation. The lower binding energy component (~396 eV) could possibly be due to strongly chemisorbed CO2. The maximum sorption capacity was about 4 mmole CO2/g sorbent at 85°C and 1 bar. This capacity was doubled by raising the CO2 pressure to 24.95 bars. The adsorption results can be described by a Langmuir adsorption isotherm.展开更多
KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these cat...KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these catalysts and the effect of pore sizes on ethanol catalytic oxidation were investigated.Mn‐40,Mn‐100,and Mn‐150 have triple,double,and single pore systems,respectively.On decreasing the aging temperature of KIT‐6,the pore sizes of KIT‐6 decrease and that of mesoporous MnO2 catalysts increase.The pore sizes and catalytic activities increase in the order:Mn‐40>Mn‐100>Mn‐150.Mn‐40 catalyst has a higher TOF(0.11 s–1 at 120°C)and the best catalytic activity for ethanol oxidation because of a bigger pore size with three pore systems with maximum distribution at 1.9,3.4,and 6.6 nm,decrease in symmetry and degree of order,more surface lattice oxygen species,oxygen vacancies resulting from more Mn3+ions,and better low‐temperature reducibility.展开更多
A series of Z-schemeβ-Bi_(2)O_(3)/ZrO_(2)hetero-junction composites containing three-dimensional(3D)mesoporous silica nanospheres(MSNs)were synthesized as efficient catalysts for antibiotic remediation.The obtained M...A series of Z-schemeβ-Bi_(2)O_(3)/ZrO_(2)hetero-junction composites containing three-dimensional(3D)mesoporous silica nanospheres(MSNs)were synthesized as efficient catalysts for antibiotic remediation.The obtained MSN/β-Bi_(2)O_(3)/ZrO_(2)ternary composites possess novel lamellar cross structure,which is well constructed byβ-Bi_(2)O_(3)nanosheets,3D MSNs,and ZrO_(2)nanoparticles.The optimal sample BZS-2(Bi∶Zr∶Si=1∶0.4∶0.33)shows an adsorptive-photocatalytic removal efficiency of 92.7%towards levofloxacin(LVF)and a total organic carbon(TOC)removal efficiency of 60.0%under simu-lated solar light irradiation for 100 min.BZS-2 can also remove 90.1%and 91.2%of tetracycline hydrochloride(TC)and oxytetracycline hydrochloride(OTC),respectively,and themaximum adsorptioncapacityof TCover BZS-2is almost 10 times that of-BiO.Theimprovement ofphotocatalytic activitycan bemainly attributed to the enhanced visible-light adsorption capacity and more efficientseparationof photogenerated electron-hole pairs.A possible Z-scheme photocatalytic mechanism of p BiO/ZrOheterojunctions based on valence band offset(AEvBo)andconduction band offset(EcBo)isproposed.This study provides an efficient way to construct novel mesoporous ternary photocatalyst with increased accessible surface area and active sites for treatment of antibiotics by synergistic adsorption and photocatalysis.展开更多
Enzymes,as highly efficient biocatalysts,play a crucial role in diverse biotechnological applications.However,enzyme(re)purification and recovery challenges pose substantial obstacles,rendering them costly for industr...Enzymes,as highly efficient biocatalysts,play a crucial role in diverse biotechnological applications.However,enzyme(re)purification and recovery challenges pose substantial obstacles,rendering them costly for industrial utilization.Addressing this,our study developed mesoporous zinc ferrite nanoparticles coated with amine-functionalized mesoporous silica structure(ZnFe_(2)O_(4)@MS)through the solvothermal method.These nano-particles are an effective nano-support for immobilizing Candida rugosa Lipase(CRL),ensuring easy separability and recoverability through a magnetic field and providing a significant surface area for high mass transference capacity.Immobilizing the lipase on the nano-support(ZnFe_(2)O_(4)@MS/CRL)through covalent bonds on the surface and within the pores led to a notable increase in enzyme activity from 324 U/mg for free enzyme to 689 U/mg for immobilized enzyme.This indicates unchanged active sites post-immobilization,accompanied by enhanced catalytic activity.The immobilized lipases demonstrated prolonged stability at elevated temperatures,maintaining over 59%of initial catalytic activity through five cycles.Furthermore,ZnFe_(2)O_(4)@MS/CRL exhibited substantial antibacterial activity against Staphylococcus aureus,more than that observed in Gram-negative bac-teria.The immobilized lipase was also effective in synthesizing banana flavor(isoamyl acetate)in n-hexane,achieving 64%esterification at 45℃ after 4 h.Overall,the study underscores the industrial promise of this immobilized enzyme system,emphasizing its potential for sustainable and cost-effective biotechnological processes.展开更多
Here,we introduce a new p H-responsive optical nanosensor designed for precise detection and selective uptake of Pd^(2+)ions from wastewater and urban mining sites.Our approach focuses on creating silica nano-sphere m...Here,we introduce a new p H-responsive optical nanosensor designed for precise detection and selective uptake of Pd^(2+)ions from wastewater and urban mining sites.Our approach focuses on creating silica nano-sphere mesostructure-based nanosensor(MSNS-OYS)through a simple and reproducible synthesis method by directly immobilizing disodium 6-hydroxy-5-[(4-sulfonatophenyl)diazenyl]naphthalene-2-sulfonate(orange yellow S;OYS)chelate onto mesoporous silica nano-spheres(MSNS)carriers.We exploited the inherent surface properties and active acid sites of silica to facilitate stable interactions with the OYS chelate[OYS-Pd]^(n+),ensuring the integrity of the sensor during Pd^(2+)sensing assays as evidenced by N_(2)adsorption/desorption,FT-IR,SEM,HR-TEM,XPS,and elemental analyses.The nano-sized MSNS-OYS has large surface-tovolume ratios with a surface area of 686 m^(2)/g and a pore volume of 0.0925 cm^(3)/g.Adsorption capacity reaches 70.8 mg/g at pH 2.Fast mass transfer properties allow the equilibrium to be reached within 30 min.This method yields a sensitive sensor capable of detecting Pd^(2+)ions down to a limit of detection(LOD)of 11.6μg/L and a limit of quantification(LOQ)of 38.6μg/L,off ering stability,selectivity,and sensitivity.Additionally,the sensor can be easily regenerated by treatment with thiourea acidifi ed with 0.05 M HNO3.展开更多
基金ACKNOWLEDGMENTS This work was supported by the National Natural Science Foundation of China （No.20872135） and the China National Tobacco Corporation （No.110200701007）.
文摘The ordered bimodal mesoporous silica MCM-48 spheres were facile synthesized by mild- temperature post-synthesis H2O2 hydrothermal treatment of as-synthesized MCM-48. The results showed that H2O2 is indispensable for simultaneously removing organic templates and forming ordered bimodal mesoporous silica MCM-48 spheres. The bimodal mesoporous MCM-48 was characterized by X-ray diffraction, transmission electron micrographs, FT-IR, and N2 adsorption-desorption, and a possible mechanism was proposed for the formation of bimodal mesoporous MCM-48.
基金financially supported by the Program for Liaoning Excellent Talents in University,abbreviated as“LNET”(LJQ2015062)Program for Science and Technology Agency of Liaoning Province(20170540585)+1 种基金General Scientific Research Project of Liaoning Provincial Department of Education(L2015296,L2016018)Science and Technology Planning project of Fushun(FSKJHT201376)
文摘By using the bimodal mesoporous silica(BMMS) as the carrier and butyl titanate as the titanium source, the TiO_2/BMMS catalyst was prepared. The samples were characterized by XRD, XRF, N_2 adsorption and desorption, FTIR, UVvis,SEM, EDS, and TEM techniques. The test results showed that TiO_2 was amorphous, the TiO_2/BMMS catalyst had an ordered bimodal mesoporous structure, and the chemical interaction existed between BMMS and TiO_2. Since the TiO_2/BMMS had a lower band gap, its photocatalytic activity was better than TiO_2. Under UV irradiation a one-pot PODS system was set up, using TiO_2/BMMS as the catalyst, H_2O_2 as the oxidant, and methanol as the solvent. The TiO_2/BMMS catalyst showed better photocatalytic activity than the mono-modal mesoporous TiO_2/SBA-15 catalyst, and the desulfurization rate of dibenzothiophene(DBT) over TiO_2/BMMS catalyst could reach 99._2%. The TiO_2/BMMS catalyst also had so good stability that the desulfurization rate of DBT did not drop apparently after 8 cycles of reusing, and could still be close to 90%.
文摘Cobalt oxide catalysts supported on mesoporous silica （Co3O4/MPS） were prepared, characterized and applied for catalytic oxidation of NO. Effects of catalyst supports, calcination temperatures, H2O and SO2 on NO conversion were investigated. The samples were also characterized by BET, XRD, FTIR and TG/DTG. The results suggested that Co3O4/MPS catalyst calcined at 573 K had the smallest crystal particles and the best surface dispersion. This catalyst had the highest activity and yielded 82% NO conversion at 573 K, at a space velocity of 12000 h^-1. Although the conversion of NO decreased with the introduction of H2O, it could be restored completely after removing residual H2O from Co3O4/MPS catalyst by heating at 573 K. In the presence of SO2, the oxidation activity decreased and COSO4 was detected on the catalyst. The NO conversion decreased to 30.2% in the presence of SO2 and H2O. It could not be restored completely after cutting off H2O and SO2. The deactivation of the catalyst in the presence of SO2 and H2O was attributed to the formation of cobalt sulfate species.
基金supported by the National Natural Science Foundation of China(201573136,21603128,U1510105)the Natural Science Foundation for Young Scientists of Shanxi Province(2016021034)the Scientific Research Start-up Funds of Shanxi University(RSC723)~~
文摘A rational integration of multiple reactive centers into a combined unit to facilitate their cooperative effects is a smart approach for accelerating the catalytic activity.Here,to achieve this goal,linear imidazolium-based ionic polymers were confined into the nanopores of mesoporous silica nanospheres anchored with homogeneously distributed zinc salts.Owing to the flexible character and the reinforced cooperative effects of the ionic liquid(nucleophile)and zinc species(Lewis acid)in the confined mesoporous structure,the resultant composite exhibited dramatically improved catalytic performance in the cycloaddition of CO2 with epoxides to form cyclic carbonates.This was in contrast to that observed for the individual catalytic components.Moreover,such a solid catalyst could be easily recovered and reused four times without a significant loss of activity.
基金Supported by Tianjin Hi-tech Support Program Key Projects, China (2009F3-0005)
文摘Amine-functionalized mesoporous silica was prepared by using lauric acid and N-stearoyl-l-glutamic acid as structure directing agents via the S-N+-I- mechanism and applied to CO2 adsorption at room temperature. With γ-aminopropyltriethoxysilane as co-structure directing agent and due to the direct electrostatic interaction with anionic surfactant, most of the amino groups were uniformly distributed at the inner surface of pores and the per- formance was stable. The amine-functionalized mesoporous silica was characterized by Fourier transform infrared spectrometer, X-ray diffraction, nitrogen physisorption and thermogravimetric analysis. The CO2 adsorption capacity was measured by digital recording balance. At the room temperature and under the atmospheric pressure, the adsorption capacity of LAA-AMS-0.2 for CO2 and N2 is 1.40 mmol·g-1 and 0.03 mmol·g-1, respectively, indicating high separation coefficient of CO2/N2.
基金supported by the Fundamental Research Funds for the Central Universities (Grant No. 2652015011)
文摘Supported nanocrystalline TiO2 with a diameter of 15–30 nm was prepared from previously synthesized radial mesoporous silica（RMS） by a post-synthesis method. In addition, their adsorption-photocatalytic activity toward the degradation of methylene blue（MB） was determined. RMS was tailor-made with the main template of CTAB and the SiO2 precursor of TEOS through a facile self-assembly process. The structural, morphological and textural properties of the well-designed TiO2/RMS samples were characterized.The RMS structure was retained after loading TiO2, but its surface area and pore diameter decreased as a result of partial pore blocking. The removal activity of MB for TiO2/RMS was significantly higher than that of commercial TiO2 nanoparticles. The optimal TiO2 loading（20 wt%） on the support could achieve the complete removal of MB within 70 min. The prepared TiO2/RMS particles can be easily separated and display good durability after six reaction cycles.
基金Funded by the National Mega-Project of Scientific&Technical Supporting Programs,Ministry of Science&Technology of China(No.2006BAJ04A04)Science Foundation of Liaoning Province,China(No.2008S190)
文摘Chemical modification/ambient drying method and freeze drying method were introduced to research the synthesis of mesoporous silica aerogels. By analyzing N2 gas adsorption/desorption isotherms, the fractal geometric characteristics of gels were focused. The overall surface fractal dimensions were determined by analyzing N2 gas adsorption branch and a Frenkel-Halsey-Hill （FHH） equation was empolyed to determine surface fractal dimension Df It is found that, during ambient drying process, VTMCS/VWetgel ratio plays a crucial role in the changes of geometric feature, the key point is 50%, when the ratio is lower, and surface roughness increases with the ratio, when it exceeds 50%, the surface is almost unaffected by the modification. While freeze drying always tends to get larger Df freeze drying process could cause a rough surface of the gels. Compared with traditional porosity and specific surface area analyses, fractal geometry may be expected to be favorable for mesoporous structural analyses of materials.
基金Supported by the National Natural Science Foundation of China(51272183)the Program for Discipline Leader in Wtthan(201051730563)the self-determined and innovative research funds of Wuhan University
文摘The mesoporous silica modifed with magnesium ox- ide （MgO） was syntbesized by one step method and impregnating method, respectively. The samples were characterized by small angle X-Ray diffraction （XRD）, N2 adsorption-desorption and transmission electron microscopy （TEM）, and the carbon dioxide adsorption capacity was analyzed by thermal gravimetric analysis （TGA）. Compared with the original mesoporous silica （20.7 mg/g）, the CO2 adsorption capacity of MgO-modified mesoporous silica processed by one step method increases to 32.9 mg/g. Although its surface area greatly decreases compared with that of the original mesoporous silica, the MgO-modified mesoporous silica prepared by impregnating reaches an adsorptive value of 31.1 mg/g because the number of basic sites increases on the surface of the mesoporous silica.
基金the Chengdu University of Technology Teachers Development Research Fund (No. 10912-2019KYQD07266)National Natural Science Foundation of China (No. 21806015) for financial support
文摘Reverse water gas shift(RWGS)reaction is a crucial process in CO_(2)utilization.Herein,Ni-and NiCe-containing hexagonal mesoporous silica(Ni-HMS and NiCe-HMS)catalysts were synthesized using an insitu one-pot method and applied for RWGS reaction.At certain reaction temperatures 500-750℃,Ni-HMS samples displayed a higher selectivity to the preferable CO than that of conventionally impregnated Ni/HMS catalyst.This could be originated from the smaller NiO nanoparticles over Ni-HMS catalyst.NiCe-HMS exhibited higher activity compared to Ni-HMS.The catalysts were characterized by means of TEM,XPS,XRD,H_(2)-TPR,CO_(2)-TPD,EPR and N_(2) adsorption-desortion technology.It was found that introduction of Ce created high concentration of oxygen vacancies,served as the active site for activating CO_(2).Also,this work analyzed the effect of the H_(2)/CO_(2)molar ratio on the best NiCe-HMS.When reaction gas H_(2)/CO_(2)molar ratio was 4 significantly decreased the selectivity to CO at low temperature,but triggered a higher CO_(2)conversion which is close to the equilibrium.
基金supported by the National Key R&D program of China(2019YFA0706802)National Natural Science Foundation of China(52063029)+2 种基金Natural Science Basic Research Program of Shaanxi(2022JM-200,2021JQ-716)China Postdoctoral Science Foundation(2020M672269)Doctoral Research Program of Yan’an University(YDBK2019-02)
文摘Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar vip species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.
文摘A CO2 solid sorbent based on polyethyleneimine 10k (PEI-10k) impregnated into mesoporous silica (MPS) foam was synthesized and utilized to capture CO2 at temperatures ranged from 65°C to 95°C. The calculated nitrogen and carbon contents in the bulk of the PEI-10k/MPS sorbent were similar to the XPS results measured on the surface of the foam, suggesting that the PEI was homo-geneously distributed throughout the MPS support. After CO2 adsorptionthe N 1s peak was broadened and could be resolved into two components: a high binding energy component (~401 eV) and a lower binding energy one (396 eV), respectively. The former nitrogen states are consistent with a protonated amine, presumably, due to carbamate formation. The lower binding energy component (~396 eV) could possibly be due to strongly chemisorbed CO2. The maximum sorption capacity was about 4 mmole CO2/g sorbent at 85°C and 1 bar. This capacity was doubled by raising the CO2 pressure to 24.95 bars. The adsorption results can be described by a Langmuir adsorption isotherm.
基金supported by the National Key Research and Development Program Foundation of China(2016YFC0209203)the National Natural Science Foundation of China(21707130,21325731)~~
文摘KIT‐6 mesoporous silica aged at 40,100,and 150°C were used as hard templates to prepare different mesoporous MnO2 catalysts,marked as Mn‐40,Mn‐100,and Mn‐150,respectively.The catalytic activities of these catalysts and the effect of pore sizes on ethanol catalytic oxidation were investigated.Mn‐40,Mn‐100,and Mn‐150 have triple,double,and single pore systems,respectively.On decreasing the aging temperature of KIT‐6,the pore sizes of KIT‐6 decrease and that of mesoporous MnO2 catalysts increase.The pore sizes and catalytic activities increase in the order:Mn‐40>Mn‐100>Mn‐150.Mn‐40 catalyst has a higher TOF(0.11 s–1 at 120°C)and the best catalytic activity for ethanol oxidation because of a bigger pore size with three pore systems with maximum distribution at 1.9,3.4,and 6.6 nm,decrease in symmetry and degree of order,more surface lattice oxygen species,oxygen vacancies resulting from more Mn3+ions,and better low‐temperature reducibility.
基金financially supported by National Natural Science Foundation of China (Nos.21962006, 21607064 and 21707055)the Youth Key Project of Natural Science Foundation of Jiangxi Province (Nos.20192ACBL20014 and 20192ACBL21011)+1 种基金the Natural Science Foundation of Jiangxi Province (Nos.20181BAB203018 and 20181BAB213010)Qingjiang Excellent Young Talents of Jiangxi University of Science and Technology
文摘A series of Z-schemeβ-Bi_(2)O_(3)/ZrO_(2)hetero-junction composites containing three-dimensional(3D)mesoporous silica nanospheres(MSNs)were synthesized as efficient catalysts for antibiotic remediation.The obtained MSN/β-Bi_(2)O_(3)/ZrO_(2)ternary composites possess novel lamellar cross structure,which is well constructed byβ-Bi_(2)O_(3)nanosheets,3D MSNs,and ZrO_(2)nanoparticles.The optimal sample BZS-2(Bi∶Zr∶Si=1∶0.4∶0.33)shows an adsorptive-photocatalytic removal efficiency of 92.7%towards levofloxacin(LVF)and a total organic carbon(TOC)removal efficiency of 60.0%under simu-lated solar light irradiation for 100 min.BZS-2 can also remove 90.1%and 91.2%of tetracycline hydrochloride(TC)and oxytetracycline hydrochloride(OTC),respectively,and themaximum adsorptioncapacityof TCover BZS-2is almost 10 times that of-BiO.Theimprovement ofphotocatalytic activitycan bemainly attributed to the enhanced visible-light adsorption capacity and more efficientseparationof photogenerated electron-hole pairs.A possible Z-scheme photocatalytic mechanism of p BiO/ZrOheterojunctions based on valence band offset(AEvBo)andconduction band offset(EcBo)isproposed.This study provides an efficient way to construct novel mesoporous ternary photocatalyst with increased accessible surface area and active sites for treatment of antibiotics by synergistic adsorption and photocatalysis.
文摘Enzymes,as highly efficient biocatalysts,play a crucial role in diverse biotechnological applications.However,enzyme(re)purification and recovery challenges pose substantial obstacles,rendering them costly for industrial utilization.Addressing this,our study developed mesoporous zinc ferrite nanoparticles coated with amine-functionalized mesoporous silica structure(ZnFe_(2)O_(4)@MS)through the solvothermal method.These nano-particles are an effective nano-support for immobilizing Candida rugosa Lipase(CRL),ensuring easy separability and recoverability through a magnetic field and providing a significant surface area for high mass transference capacity.Immobilizing the lipase on the nano-support(ZnFe_(2)O_(4)@MS/CRL)through covalent bonds on the surface and within the pores led to a notable increase in enzyme activity from 324 U/mg for free enzyme to 689 U/mg for immobilized enzyme.This indicates unchanged active sites post-immobilization,accompanied by enhanced catalytic activity.The immobilized lipases demonstrated prolonged stability at elevated temperatures,maintaining over 59%of initial catalytic activity through five cycles.Furthermore,ZnFe_(2)O_(4)@MS/CRL exhibited substantial antibacterial activity against Staphylococcus aureus,more than that observed in Gram-negative bac-teria.The immobilized lipase was also effective in synthesizing banana flavor(isoamyl acetate)in n-hexane,achieving 64%esterification at 45℃ after 4 h.Overall,the study underscores the industrial promise of this immobilized enzyme system,emphasizing its potential for sustainable and cost-effective biotechnological processes.
基金funded by the University of JeddahJeddah+2 种基金Saudi Arabiaunder grant No.UJ-23-DR-155the University of Jeddah for its technical and financial support。
文摘Here,we introduce a new p H-responsive optical nanosensor designed for precise detection and selective uptake of Pd^(2+)ions from wastewater and urban mining sites.Our approach focuses on creating silica nano-sphere mesostructure-based nanosensor(MSNS-OYS)through a simple and reproducible synthesis method by directly immobilizing disodium 6-hydroxy-5-[(4-sulfonatophenyl)diazenyl]naphthalene-2-sulfonate(orange yellow S;OYS)chelate onto mesoporous silica nano-spheres(MSNS)carriers.We exploited the inherent surface properties and active acid sites of silica to facilitate stable interactions with the OYS chelate[OYS-Pd]^(n+),ensuring the integrity of the sensor during Pd^(2+)sensing assays as evidenced by N_(2)adsorption/desorption,FT-IR,SEM,HR-TEM,XPS,and elemental analyses.The nano-sized MSNS-OYS has large surface-tovolume ratios with a surface area of 686 m^(2)/g and a pore volume of 0.0925 cm^(3)/g.Adsorption capacity reaches 70.8 mg/g at pH 2.Fast mass transfer properties allow the equilibrium to be reached within 30 min.This method yields a sensitive sensor capable of detecting Pd^(2+)ions down to a limit of detection(LOD)of 11.6μg/L and a limit of quantification(LOQ)of 38.6μg/L,off ering stability,selectivity,and sensitivity.Additionally,the sensor can be easily regenerated by treatment with thiourea acidifi ed with 0.05 M HNO3.
