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1.
Nanomaterials (Basel) ; 12(20)2022 Oct 21.
Artículo en Inglés | MEDLINE | ID: mdl-36296893

RESUMEN

Among various iron carbide phases, χ-Fe5C2, a highly active phase in Fischer-Tropsch synthesis, was directly synthesized using a wet-chemical route, which makes a pre-activation step unnecessary. In addition, χ-Fe5C2 nanoparticles were encapsulated with mesoporous silica for protection from deactivation. Further structural analysis showed that the protective silica shell had a partially ordered mesoporous structure with a short range. According to the XRD result, the sintering of χ-Fe5C2 crystals did not seem to be significant, which was believed to be the beneficial effect of the protective shell providing restrictive geometrical space for nanoparticles. More interestingly, the protective silica shell was also found to be effective in maintaining the phase of χ-Fe5C2 against re-oxidation and transformation to other iron carbide phases. Fischer-Tropsch activity of χ-Fe5C2 in this study was comparable to or higher than those from previous reports. In addition, CO2 selectivity was found to be very low after stabilization.

2.
J Nanosci Nanotechnol ; 16(2): 2004-9, 2016 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-27433718

RESUMEN

Uniform rhodium nanoparticles (NP) with three different particle sizes (1.9, 2.4, and 3.6 nm) were prepared via a polyol method with rhodium (III) acetylacetonate, poly(vinylpyrrolidone) with different concentrations of sodium citrate. The prepared Rh nanoparticles were impregnated into the ordered mesoporous carbon supports with two different pore structures (2D hexagonal and 3D cubic). The prepared Rh nanoparticle-supported ordered mesoporous carbons (OMCs) were introduced as catalysts for the CO hydrogenation of syngas to produce C2 higher alcohols. The characteristics of the Rh nanoparticle-supported ordered mesoporous carbons catalysts were analyzed through transmission electron microscopy, powder X-ray diffraction, and N2 physisorption analysis. The catalytic tests of the catalyst were performed using a fixed-bed reactor. The results revealed that the catalysts exhibited the different catalytic activity and selectivity of higher alcohols, which could be attributed to the different OMC structures, the nanoparticle size of Rh, and aggregation of Rh nanoparticles during the reaction.


Asunto(s)
Alcoholes/síntesis química , Carbono/química , Rodio/química , Alcoholes/química , Catálisis , Porosidad
3.
Prep Biochem Biotechnol ; 46(4): 410-9, 2016 May 18.
Artículo en Inglés | MEDLINE | ID: mdl-26176425

RESUMEN

Klebsiella pneumoniae is known to produce 2,3-butanediol (2,3-BDO), a valuable chemical. In K. pneumoniae, the 2,3-BDO operon (budBAC) is involved in the production of 2,3-BDO. To observe the physiological role of the 2,3-BDO operon in a mixed acid fermentation, we constructed a budBAC-deleted strain (SGSB109). The production of extracellular metabolites, CO2 emission, carbon distribution, and NADH/NAD(+) balance of SGSB109 were compared with the parent strain (SGSB100). When comparing the carbon distribution at 15 hr, four significant differences were observed: in 2,3-BDO biosynthesis, lactate and acetate production (lactate and acetate production increased 2.3-fold and 4.1-fold in SGSB109 compared to SGSB100), CO2 emission (higher in SGSB100), and carbon substrate uptake (higher in SGSB100). Previous studies on the inactivation of the 2,3-BDO operon were focused on the increase of 1,3-propanediol production. Few studies have been done observing the role of 2,3-BDO biosynthesis. This study provides a prime insight into the role of 2,3-BDO biosynthesis of K. pneumoniae.


Asunto(s)
Butileno Glicoles/metabolismo , Klebsiella pneumoniae/genética , Operón , Genes Bacterianos
4.
J Biomed Nanotechnol ; 11(7): 1183-92, 2015 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-26307841

RESUMEN

The functionality of ultrasound in early cancer detection is limited because of its relatively low contrast resolution. Because it has a high degree of echogenicity, a microbubble contrast agent is often used to overcome this intrinsic limitation of imaging at low-contrast resolution. A targeted and drug-loaded microbubble contrast agent for simultaneous diagnosis and therapy has recently been investigated. However, no optimized theragnosis ultrasound microbubbles have been developed. Paclitaxel (PTX)-encapsulating human serum albumin nanoparticles (PTX-HSA-NPs) were conjugated onto an ultrasound microbubbles (PTX-HSA-NPs-MBs) fabricated in the laboratory to result in a narrow size distribution (1.7 ± 0.7 µm) and an optimal resonance frequency of 3 MHz. After intravenous injection of HSA-NPs-MBs, echogenicity in the tumor xenografted with breast cancer MCF-7 cells was significantly enhanced, showing the possibility of early cancer diagnosis. Mice injected with PTX-HSA-NPs-MBs showed higher survival rates in comparison with control groups, demonstrating the possibility of theragnosis. In the present study, the conjugation of PTX-HSA-NPs onto the ultrasound microbubbles simultaneously provided (1) enhanced ultrasound signal generation, (2) sufficient drug-loading capacity, (3) ability to deliver drugs to a preferred tumor site, and (4) increased stability in blood circulation.


Asunto(s)
Microburbujas/uso terapéutico , Nanocápsulas/uso terapéutico , Paclitaxel/administración & dosificación , Ultrasonografía/métodos , Animales , Antineoplásicos Fitogénicos/administración & dosificación , Antineoplásicos Fitogénicos/química , Apoptosis/efectos de los fármacos , Supervivencia Celular/efectos de los fármacos , Medios de Contraste , Humanos , Aumento de la Imagen/métodos , Células MCF-7 , Ratones , Ratones Endogámicos BALB C , Ratones Desnudos , Nanocápsulas/química , Resultado del Tratamiento
5.
ACS Nano ; 9(7): 7497-505, 2015 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-26095456

RESUMEN

Hybrid supercapacitors (battery-supercapacitor hybrid devices, HSCs) deliver high energy within seconds (excellent rate capability) with stable cyclability. One of the key limitations in developing high-performance HSCs is imbalance in power capability between the sluggish Faradaic lithium-intercalation anode and rapid non-Faradaic capacitive cathode. To solve this problem, we synthesize Nb2O5@carbon core-shell nanocyrstals (Nb2O5@C NCs) as high-power anode materials with controlled crystalline phases (orthorhombic (T) and pseudohexagonal (TT)) via a facile one-pot synthesis method based on a water-in-oil microemulsion system. The synthesis of ideal T-Nb2O5 for fast Li(+) diffusion is simply achieved by controlling the microemulsion parameter (e.g., pH control). The T-Nb2O5@C NCs shows a reversible specific capacity of ∼180 mA h g(-1) at 0.05 A g(-1) (1.1-3.0 V vs Li/Li(+)) with rapid rate capability compared to that of TT-Nb2O5@C and carbon shell-free Nb2O5 NCs, mainly due to synergistic effects of (i) the structural merit of T-Nb2O5 and (ii) the conductive carbon shell for high electron mobility. The highest energy (∼63 W h kg(-1)) and power (16 528 W kg(-1) achieved at ∼5 W h kg(-1)) densities within the voltage range of 1.0-3.5 V of the HSC using T-Nb2O5@C anode and MSP-20 cathode are remarkable.

6.
Environ Sci Technol ; 48(14): 8251-7, 2014 Jul 15.
Artículo en Inglés | MEDLINE | ID: mdl-24933030

RESUMEN

Two process models for carbon dioxide utilized gas-to-liquids (GTL) process (CUGP) mainly producing light olefins and Fischer-Tropsch (F-T) synthetic oils were developed by Aspen Plus software. Both models are mainly composed of a reforming unit, an F-T synthesis unit and a recycle unit, while the main difference is the feeding point of fresh CO2. In the reforming unit, CO2 reforming and steam reforming of methane are combined together to produce syngas in flexible composition. Meanwhile, CO2 hydrogenation is conducted via reverse water gas shift on the Fe-based catalysts in the F-T synthesis unit to produce hydrocarbons. After F-T synthesis, the unreacted syngas is recycled to F-T synthesis and reforming units to enhance process efficiency. From the simulation results, it was found that the carbon efficiencies of both CUGP options were successfully improved, and total CO2 emissions were significantly reduced, compared with the conventional GTL processes. The process efficiency was sensitive to recycle ratio and more recycle seemed to be beneficial for improving process efficiency and reducing CO2 emission. However, the process efficiency was rather insensitive to split ratio (recycle to reforming unit/total recycle), and the optimum split ratio was determined to be zero.


Asunto(s)
Dióxido de Carbono/química , Química Inorgánica/métodos , Efecto Invernadero , Hidrocarburos/síntesis química , Hierro/química , Vapor , Alquenos/síntesis química , Hidrógeno/química , Hidrogenación , Metano/síntesis química , Modelos Teóricos , Aceites/síntesis química , Reciclaje , Temperatura
7.
J Nanosci Nanotechnol ; 13(11): 7511-8, 2013 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-24245283

RESUMEN

A series of ordered mesoporous carbon materials (OMCs) possessing well-ordered nanoporosity with different mesopore structures were synthesized by the template-synthesis route. Two different pore strucutes (2-dimensional hexagonal and 3-dimensional cubic structures) and two different framework-configurations (rod-type and hollow-type carbon frameworks) are prepared by using the two different silica templates and synthetic conditions. The ordered mesoporous carbon supported promoted-rhodium catalysts were preparted by an incipient wetness method. The promoted Rh-OMC catalysts are tested by a fixed bed reactor for the catalytic conversion of syngas-to-alcohols. The characteristics of the promoted Rh-OMCs catalysts were scrutinized through a series of different techniques, including transmission electron microscopy (TEM), powder X-ray diffraction (XRD), and N2 sorption analysis, and the catalytic performance was tested in a fixed-bed reactor. It was found that the promoted Rh-OMC catalysts exhibited the different catalytic activity and selectivity of alcohols, which could be attributed to the size of metal nanoparticles being confined by the different mesostructure of OMCs.


Asunto(s)
Alcoholes/síntesis química , Monóxido de Carbono/química , Carbono/química , Cristalización/métodos , Hidrógeno/química , Nanoestructuras/química , Nanoestructuras/ultraestructura , Adsorción , Hidrogenación , Sustancias Macromoleculares/química , Ensayo de Materiales , Conformación Molecular , Tamaño de la Partícula , Porosidad , Propiedades de Superficie
8.
Chem Commun (Camb) ; 49(45): 5141-3, 2013 Jun 07.
Artículo en Inglés | MEDLINE | ID: mdl-23482917

RESUMEN

A hexagonally ordered mesoporous carbon, CMK-3, was utilized as a support for a Fischer-Tropsch catalyst. Each array of elongated pore structures with Co nanoparticles can be regarded as a nanochannel reactor. Due to the pore confinement and the hydrophobic nature of the support, this catalyst demonstrated excellent catalytic performance.

9.
ChemSusChem ; 6(2): 299-307, 2013 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-23281317

RESUMEN

A disulfide/thiolate (T(2)/T(-)) redox-couple electrolyte, which is a promising iodine-free electrolyte owing to its transparent and noncorrosive properties, requires alternative counter-electrode materials because conventional Pt shows poor catalytic activity in such an electrolyte. Herein, ordered mesoporous tungsten suboxide (m-WO(3-x)), synthesized by using KIT-6 silica as a hard template followed by a partial reduction, is used as a catalyst for a counter electrode in T(2)/T(-)-electrolyte-based dye-sensitized solar cells (DSCs). The mesoporous tungsten suboxide, which possesses interconnected pores of 4 and 20 nm, provides a large surface area and efficient electrolyte penetration into the m-WO(3-x) pores. In addition to the advantages conferred by the mesoporous structure, partial reduction of tungsten oxide creates oxygen vacancies that can function as active catalytic sites, which causes a high electrical conductivity because of intervalence charge transfer between the W(5+) and W(6+) ions. m-WO(3-x) shows a superior photovoltaic performance (79 % improvement in the power conversion efficiency) over Pt in the T(2)/T(-) electrolyte. The superior catalytic activity of m-WO(3-x) is investigated by using cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and Tafel polarization curve analysis.


Asunto(s)
Colorantes/química , Disulfuros/química , Suministros de Energía Eléctrica , Óxidos/química , Energía Solar , Compuestos de Sulfhidrilo/química , Tungsteno/química , Electrodos , Platino (Metal)/química , Porosidad
10.
Environ Sci Technol ; 44(4): 1412-7, 2010 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-20078033

RESUMEN

A process model for a gas-to-liquids (GTL) process mainly producing Fischer-Tropsch (FT) synthetic oils has been developed to assess the effects of reforming methods, recycle ratio of unreacted syngas mixture on the process efficiency and the greenhouse gas (GHG) emission. The reforming unit of our study is composed of both steam reforming of methane (SRM) and carbon dioxide reforming of methane (CDR) to form syngas, which gives composition flexibility, reduction in GHG emission, and higher cost-competitiveness. With recycling, it is found that zero emission of CO(2) from the process can be realized and the required amount of natural gas (NG) can be significantly reduced. This GTL process model has been built by using Aspen Plus software, and it is mainly composed of a feeding unit, a reforming unit, an FT synthesis unit, several separation units and a recycling unit. The composition flexibility of the syngas mixture due to the two different types of reforming reactions raises an issue that in order to attain the optimized feed composition of FT synthesis the amount of flow rate of each component in the fresh feed mixture should be determined considering the effects of the recycle and its split ratio. In the FT synthesis unit, the 15 representative reactions for the chain growth and water gas shift on the cobalt-based catalyst are considered. After FT synthesis, the unreacted syngas mixture is recycled to the reforming unit or the FT synthesis unit or both to enhance process efficiency. The effect of the split ratio, the recycle flow rate to the FT reactor over the recycle flow rate to the reforming unit, on the efficiency of the process was also investigated. This work shows that greater recycle to the reforming unit is less effective than that to the FT synthesis unit from the standpoint of the net heat efficiency of the process, since the reforming reactions are greatly endothermic and greater recycle to the reformer requires more energy.


Asunto(s)
Dióxido de Carbono/química , Metano/química , Modelos Teóricos , Conservación de los Recursos Naturales
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