Organic Template Method Research Articles

The Role of ZSM‐5 Zeolite Paracrystalline on Compatibility of CMCh‐Based Composite Solid Electrolyte

AbstractAchieving compatibility of composite solid electrolytes among materials for fabricating lithium‐ion batteries presents a significant challenge. This work aimed to study the role of the ZSM‐5 zeolite paracrystalline on the compatibility of CMCh‐based CSE. The ZSM‐5 zeolite intermediates and products were synthesized using the free organic template method, while the CSE membranes were fabricated by combining CMCh, ZSM‐5, and lithium perchlorate (LiClO4) using the solution‐casting method. The result showed that the synthesis of ZSM‐5 zeolite has been successfully performed. FTIR spectrum at wavenumber ~950 cm−1 of ZSM‐5 zeolite indicates that secondary building unit (SBU) structures exist. The SBU structure of ZSM‐5 zeolite indicates the paracrystalline structure of ZSM‐5 zeolite, which is compatible with the CMCh structure. The characterizations in this work were conducted to study the interaction, morphology, crystallinity index, thermal stability, mechanical strength, and ionic conductivity through FTIR, SEM, XRD, TGA, tensile tester, and EIS, respectively. The CSE of CMCh/Z5AH‐LiClO4 was the optimum condition exhibiting ionic conductivity as high as 4.35 x 10−6 S cm−1 with a crystallinity index of 34.25 %, a tensile strength of 46.67 MPa and onset thermal degradation of 262.61 °C. These results suggest that CMCh/Z5AH‐LiClO4 holds promise as a solid electrolyte material for lithium‐ion batteries.

Erbium-ytterbium containing upconversion mesoporous bioactive glass microspheres for tissue engineering: luminescence monitoring of biomineralization and drug release.

The development of functional biomaterials with real-time monitoring of mineralization processes, drug release and biodistribution has potential applications but remains an unsolved challenge. Herein, erbium- and ytterbium- containing mesoporous bioactive glass microspheres (MBGs:Er/Yb) with blue and red emission at an excitation wavelength of 980nm were synthesized by a sol-gel combined with organic template method. As the concentration of Yb3+ ions gradually increases, the emission intensity of the MBGs:Er/Yb exhibits a clear concentration quenching effect. Combined with in vitro bioactivity tests, the optimal molar ratio of Er3+/Yb3+ was determined to be 4:3. Therefore, MBGs:4Er/3Yb was selected for in vitro biomineralization and drug release monitoring. The results of biomineralization monitoring show that the upconversion luminescence intensity is closely related to the degree of biomineralization. The upconversion luminescence intensity of MBGs:4Er/3Yb is quenched with the increase of the degree of biomineralization. The degree of luminescence quenching during biomineralization can be semiquantized. Drug release monitoring experiments showed that the anticancer drug doxorubicin hydrochloride (DOX) was successfully loaded into MBGs:4Er/3Yb and selectively quenched the green emission. When DOX was released, the green emission recovered stably, and It/I0 increased gradually. Moreover, there was a linear relationship between It/I0 and cumulative drug release, indicating that DOX-MBGs:4Er/3Yb is highly sensitive to DOX release, and monitoring the It/I0 values of DOX-MBGs:4Er/3Yb can achieve real-time tracking of the DOX release process to a certain extent. In conclusion, MBGs:4Er/3Yb has potential application as an upconversion luminescence biomonitoring material in the field of bone tissue engineering. STATEMENT OF SIGNIFICANCE: Mesoporous bioactive glasses have great potential for applications in bone tissue repair due to their excellent biological properties, but the effective information of the repair process cannot be grasped in a timely manner. Therefore, real-time monitoring of mineralization and drug release processes will be beneficial to obtain the degree of healing and optimize the amount and distribution of drugs to improve targeted therapeutic effects. For biomaterials, in vitro biological properties determine their biological properties in vivo, where the environment is more complex and diverse, and thus in vitro biomonitoring is particularly crucial. The organic combination of physical properties and biological properties will also provide a feasible idea for the development of biomaterials.

Effect of mesoporous bioactive glass on odontogenic differentiation of human dental pulp stem cells.

Healthy pulp tissue plays an important role in normal function and long-term retention of teeth. Mesoporous bioactive glass (MBG) as a kind of regenerative biomaterials shows the potential in preserving the vital pulp. In this study, MBG prepared by organic template method combined with sol-gel method were used in human dental pulp cell culture and ectopic mineralization experiment. Real-Time PCR was used to explore its ability to induce odontogenic differentiation of dental pulp cells. MBG and rat crowns were implanted under the skin of nude mice for 4 weeks to observe the formation of pulp dentin complex. We found that MBG can release Si and Ca ions and has a strong mineralization activity in vitro. The co-culture of MBG with human dental pulp cells promoted the expression of DMP-1 (dentin matrix protein-1) and ALP (alkalinephosphatase) without affecting cell proliferation. After 4 weeks of subcutaneous implantation in nude mice, the formation of hard tissue with regular structure under the material could be seen, and the structure was similar to dentin tubules. These results indicate that MBG can induce the differentiation of dental pulp cells and the formation of dental pulp-dentin complex and has the potential to promote the repair and regeneration of dental pulp injuries.

Silver-phosphate glass matrix for iodine conditioning: From sorbent design to vitrification

A new route for the synthesis of silver-phosphate based sorbent beads as precursors of final iodine waste form is proposed here. This sorbent is used to entrap gaseous iodine produced during the reprocessing of spent nuclear fuels and to be directly transformed into materials composed of a silver phosphate glass phase considered as high efficient iodine containment matrix for long-term storage in deep geological repository. Using sacrificial organic template method (alginate) and well controlled calcination of the obtained silver phosphate grains materials, this innovative synthesis makes in-situ formation of metallic silver inside them. Ag0 then can easily entrap iodine when in contact with gaseous iodine. The obtained sorbent were tested for iodine trapping in static conditions. They showed great performances with a catch rate of 480 mg.g−1. The iodine-loaded sorbent were finally heat treated at 650 °C with an iodine loss lower than 3% wt. The resulted materials shows the presence of the expected silver phosphate glass matrix with a great iodine incorporation of 9% mol.

Preparation of a Spherical MnO2 Intermediate by an Organic Template Method and Its Effect on the Electrochemical Performance of Lithium-Rich Manganese-Based Materials

Polyvinylpyrrolidone (PVP) and ethylene glycol (EG) are used as the template agents to prepare an assisted spherical MnO2 intermediate, which is used to prepare lithium-rich manganese-based materia...

Al2O3–FSM16-supported cobalt catalyst: a promising novel Fischer–Tropsch synthesis catalyst

High specific surface area ordered meso-porous solid (FSM16) was synthesized by using the organic template method. The surface acidity of solid (FSM16) was modified significantly with the addition of alumina content by impregnation of alumina nitrate aqueous solution with Si/Al molar ratios of 10. Al2O3–FSM16 and conventional γ-alumina-supported cobalt catalysts were introduced for Fischer–Tropsch synthesis (FTS). The catalysts were prepared using wet impregnation with a cobalt loading of 15.0 wt% and characterized by ICP, TPR, BET, XRD, TEM, NH3-TPD, TGA and H2 chemisorptions. Finally, the activity, selectivity and stability of the catalysts were assessed in FTS. The characterizations clearly confirmed that morphology of the Al2O3–FSM16 support (surface area, pore volume, pore size distribution and crystallite phase) can affect the catalyst performances. The proposed 15 wt% Co/Al2O3–FSM16 catalyst has shown surprising stability during 120 h continuous of FTS reaction and also at first 24 h of test run, increased the FTS rate from 0.15 to 0.34 g HC/gcat./h, CO conversion by about 68%; also the C5+ hydrocarbons increased, compared to that prepared by conventional γ-alumina support (Conndea Vista Catalox B g-alumina).

Fe2P@mesoporous carbon nanosheets synthesized via an organic template method as a cathode electrocatalyst for Zn–air batteries

Organic layers were formed using a melamine crystal template, which transformed carbon nanosheets with Fe2P into a mesoporous structure after carbonization.

Template‐Free Synthesis of High‐Content Vanadium‐Doped ZSM‐5 with Enhanced Catalytic Performance

AbstractThe high cost of preparation of transition metal doped ZSM‐5 zeolite is limited to the use of organic template such as tetrapropylammonium hydroxide or tetrapropylammonium bromide. In this work, vanadium atom was successfully incorporated into the framework of ZSM‐5 zeolite without using any organic template. Moreover, the method not only decreases the preparation cost of vanadium doped ZSM‐5, but also greatly enhances the utilization ratio of vanadium atom. Vanadium atom mainly exists as tetrahedral coordination in the framework of ZSM‐5 which was demonstrated by the ultraviolet visible and X‐ray photoelectron spectrum. Furthermore, vanadium doped ZSM‐5 performs high and stability catalytic activity in the oxidation of styrene compared to that of the catalyst prepared by the traditional organic template method ascribe to the greatly increase of tetrahedral vanadium species.

Synthesis, characterization and catalytic properties of NiMoP/MCM41-γAl2O3 catalysts for DBT hydrodesulfurization

NiMoP/MCM41-γAl2O3 (NiMoP/AMx) supported catalysts have been investigated as a modification of MCM41 by using the sol–gel alumina incorporation method. Different catalysts were synthesized varying the Si/Al molar ratio (5, 10, 25 and 50). The aqueous solution method was used to impregnate the metallic species (NiMoP) on the AMx supports. A surface area high mesoporous solid was synthesized by using an organic template method. The incorporation of sol–gel alumina did modified the hexagonal array of the mesoporous material MCM41 when the preparation of AMx supports was carried out. The XRD patterns of the catalytic supports show that phases, MCM-41 and γ-Al2O3 exist, indicating the presence of the two materials in the synthesized solids. Raman spectroscopy also indicates the formation of NiMoO4 and MoO3 which are more difficult to sulfide and produce MoS2 and Ni3S2 as separated sulfides instead of the NiMoS phase. The symmetries of the materials were determined through UV–vis where octahedral NiO as well as tetrahedral and octahedral Mo were found. The main reaction products were biphenyl (BP), cyclohexylbenzene (CHB) and bicyclohexyl (BCH) when the materials were tested in the HDS of DBT.

Synthesis of composites SBA-15 mesoporous particles carrying oxytocin and evaluation of their properties, functions, and in vitro biological activities.

Using the organic template method, we have synthesized mesoporous SBA-15 particles and characterized them by scanning electron microscopy and transmission electron microscopy. The bone metabolism regulating hormone oxytocin (OT) was selected as a model for preparation of drug/SBA-15 complexes. The process of drug loading was studied using X-ray diffraction and nitrogen absorption methods. Optimal drug loading parameters were experimentally investigated. The kinetics of drug release from the carrier was evaluated. Finally, the extractions of SBA-15 particles were tested for cytotoxicity, in vitro hemolysis, and the direct attachment toxicity. Our findings suggest that SBA-15 materials have good biocompatibility. Moreover, we demonstrated that OT/SBA-15 complex can stimulate alkaline phosphatase activity in osteoblast cells. The study provides fundamental information for further in vivo drug-carrier testing.

Alginate encapsulated mesoporous silica nanospheres as a sustained drug delivery system for the poorly water-soluble drug indomethacin

We applied a combination of inorganic mesoporous silica material, frequently used as drug carriers, and a natural organic polymer alginate (ALG), to establish a sustained drug delivery system for the poorly water-soluble drug Indomethacin (IND). Mesoporous silica nanospheres (MSNs) were synthesized using an organic template method and then functionalized with aminopropyl groups through postsynthesis. After drug loading into the pores of aninopropyl functionalized MSNs (AP-MSNs), IND loaded AP-MSNs (IND-AP-MSNs) were encapsulated by ALG through the ionic interaction. The effects of surface chemical groups and ALG layer on IND release were systematically studied using scanning electron microscopy (SEM), transmission electron microscopy (TEM), nitrogen adsorption, zeta-potential analysis and TGA analysis. The surface structure and surface charge changes of the ALG encapsulated AP-MSNs (ALG-AP-MSNs) were also investigated. The results showed that sustained release of IND from the designed drug delivery system was mainly due to the blockage effect from the coated ALG. We believe that this combination will help designing oral sustained drug delivery systems for poorly water-soluble drugs.

Synthesis and characterization of hollow glass–ceramics microspheres

Hollow glass–ceramics microspheres (HGCMs), with the diameter from 10 to 60μm and the shell thickness less than 2μm, were successfully fabricated by a simple technique using polyacrylamide microspheres (PAMs) as template. The corresponding HGCM were obtained after a thermal treatment of the core–shell microspheres, which were synthesized with organic template method. The size, morphology and phase composition of synthesized products were determined via XRD, SEM, TGA. The effects of the amount of glass powder, the Hydrophile–Lipophile Balance (HLB) value, the sintering temperature, and the ratio of pre-adsorbed water to the water in the slurry on the morphologies of HGCM have been investigated. The results showed that the agglomeration of HGCM can be reduced by adjusting the HLB value. In addition, the amount of solid beads decreases obviously by reducing ratios and adjusting the HLB value. As the sintering temperature increases, the surface of the HGCM becomes smooth and compact. Meanwhile, computational investigations are carried out to better understand the strengthen effect of taking glass–ceramics materials in the system MgO–Al2O3–SiO2 (MAS) as shell materials.

Synthesis and characterization of hollow glass–ceramics microspheres

Hollow glass–ceramics microspheres (HGCM), with the diameter from 10 μm to 60 μm and the shell thickness less than 2 μm, were successfully fabricated by a simple technique using polyacrylamide microspheres (PAM) as template. The corresponding HGCM were obtained by a thermal treatment of the core–shell microspheres, which were synthesized with organic template method. The size, morphology and phase composition of synthesized products were determined via XRD, SEM, TGA. The effects of the amount of glass powder, the Hydrophile–Lipophile Balance (HLB) value, the sintering temperature, and the ratios of pre-adsorbed water and the water in the slurry on the morphologies of HGCM have been investigated. The results showed that the agglomeration of HGCM can be reduced by adjusting the HLB value. In addition, the amount of solid beads decreases obviously by reducing ratios and adjusting the HLB value. As the sintering temperature increases, the surface of the HGCM becomes smooth and compact.

Research of Activated Carbon for Supercapacitor Prepared by Organic Template Method

Activated carbon was fabricated by using phenolic resin as carbon source, PEG as organic template, KOH as activator. The samples were analyzed by N2 adsorption, scanning electron microscopy (SEM). Cyclic voltammetry and galvanostatic charge-discharge were used to characterize the electrochemical performance of the samples. The results showed that the specific surface area of the prepared sample (AC1) was 2469 m2/g, the pore size was mainly in the range of 1.0～4.0 nm. At a current density of 7.5 mA/cm2, a specific capacitance of 327F/g was achieved, the equivalent series resistance (ESR) was 0.8Ω. Supercapacitors based on the sample have low ESR and excellent power property. For comparison, commercial AC (AC2) was also studied.

Synthesis of hollow glass-ceramics microspheres via template method

Hollow glass-ceramics microspheres (HGCM) were successfully fabricated by a simple technique using polyacrylamide microspheres (PAM) as template. The corresponding HGCM were obtained by a thermal treatment of the core–shell microspheres, which were synthesized with organic template method. The effects of the concentration of glass powder, the Hydrophile–Lipophile Balance (HLB) value, and the amount of pre-adsorbed water on the morphologies of the core–shell microspheres and HGCM have been investigated. The size, morphology, core–shell structure and crystalline phase of HGCM and core–shell microspheres were determined via XRD, SEM and TGA. The influences of initiator and surfactant on the monodispersity and average diameter of PAM were investigated via SEM. The results showed that: (a) the average diameter and monodispersity of PAM can be controlled by varying the amount of initiator and surfactant, and (b) the agglomeration of core–shell microspheres and HGCM can be reduced using PAM with pre-adsorbed water and adjusting the HLB value. In addition, the amount of solid beads decreases obviously by reducing the concentration of glass powder and adjusting the HLB value.

Spherical mesoporous silica nanoparticles for loading and release of the poorly water-soluble drug telmisartan

The purpose of this study was to develop mesoporous silica nanoparticles (MSNs) loaded with a poorly water-soluble drug, intended to be orally administered, able to improve the dissolution rate and enhance the drug loading capacity. Spherical MSNs were synthesized using an organic template method in an oil/water phase, and large pore diameter MSNs were functionalized with aminopropyl groups through postsynthesis. MSNs as well as the resulting functionalized MSNs were investigated as matrices for loading and release of the model drug telmisartan (TEL). The effects of different pore sizes and surface chemical groups on TEL uptake and release were systematically studied using scanning electron microscopy (SEM), transmission electron microscopy (TEM), nitrogen adsorption, X-ray diffraction (XRD), Fourier transformation infrared spectroscopy (FT-IR), differential scanning calorimetry (DSC), thermogravimetric analysis (TGA) and HPLC. The total pore volume and the pore diameter of MSNs were the two main factors limiting the maximum drug load capacity. MSNs allow a very high drug loading of about 60% in weight. The release rate of TEL from MSNs with a pore diameter of 12.9 nm was found to be effectively increased and the release rate of TEL from the functionalized MSNs was effectively controlled compared with that from the unmodified MSNs. We believe that the present study will help in the design of oral drug delivery systems for the dissolution enhancement and/or sustained release of poorly water-soluble drugs.

Synthesis, characterization and catalytic properties of NiMo/Al 2O 3–MCM-41 catalyst for dibenzothiophene hydrodesulfurization

Ni–Mo/Al 2O 3–MCM-41 supported catalysts have been investigated for modification of MCM-41 by using sol–gel alumina incorporation method. Different catalysts were synthesized with variation of Si/Al molar ratios of 10, 50, 100 and 200. High specific surface area ordered meso-porous solid (MCM-41) was synthesized by using organic template method. In order to modify the low acidity of silica solid, the surface of MCM-41 was modified by incorporation of alumina. The surface acidity of solids modified significantly with variation of alumina content in the supports. The sol–gel method of alumina incorporation was used, which does not modify extensively the pore characteristics of MCM-41 material during the preparation of Al 2O 3–MCM-41. The X-ray diffraction intensities indicated that alumina as well as MCM-41 were present in the synthesized supports. Additionally, the hydrothermal stability of the Al 2O 3–MCM-41 materials was maintained up to 873 K using sever conditions like 100% water vapor stream. The catalytic activity of the catalysts was tested in the hydrodesulfurization (HDS) of dibenzothiophene (DBT). Selectivity was oriented mainly to the production of biphenyl (BP) and for high Si/Al ratios toward cyclohexylbenzene (CHB) and showed a higher conversion and better selectivity to hydrogenation (cyclohexylbenzene).

Biomorphic SiC Ceramics Prepared by Organic Template Method

Dense SiC/Si ceramics were prepared by a silicon melt infiltration method. Highly porous SiC ceramics with a wood-like microstructure were prepared by silica sol infiltration and carbothermal reduction reaction. Furthermore, laminated SiC/Si composites were also prepared by the carbonization and silicon melt infiltration of stacked papers. The microstructure and characteristics for this series of materials were determined and compared.

Template evaporation method for controlling anatase nanocrystal size in ordered macroporous TiO 2

The importance of pure-phase titanium oxide materials as catalysts, sensors, and photonic band-gap materials has been growing steadily. Recently, more attention has been focused on nanostructured titanium oxide showing controlled and periodic porosity on a nanometric scale. The nanocrystal size control of porous nanostructured titanium oxide in an anatase form is a crucial step for the organic template method. Simple template removal by evaporation in an inert atmosphere is reported in this article and compared with the calcination technique usually reported in the literature. The proposed method allows the formation of a double-porous (macro and meso) anatase phase. We demonstrate that it highly preserves the macropore order into a titanium oxide material and induces narrowly dispersed mesopores by controlling the nano-crystal size that is kept around 6 nm. For the proposed method, polystyrene beads are particularly suitable as templates, being evaporated in the temperature range of anatase existence. The final high surface area makes the materials appealing for applications as photocatalysts or sensors.