36 research outputs found

    Bi-Functional Catalyst/Sorbent for a H2-Rich Gas from Biomass Gasification

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    The aim of this work is to identify the effect of the CaO phase as a CO2 sorbent and mayenite (Ca12Al14O33) as a stabilizing phase in a bi-functional material for CO2 capture in biomass syngas conditioning and cleaning at high temperature. The effect of different CaO weight contents is studied (0, 56, 85, 100 wt%) in sorbents synthesized by the wet mixing method. These high temperature solid sorbents are upgraded to bi-functional compounds by the addition of 3 or 6 wt% of nickel chosen as the metal active phase. N2 adsorption, X-ray diffraction, scanning electronic microscopy, temperature-programmed reduction analyses and CO2 sorption study were performed to characterize structural, textural, reducibility and sorption properties of bi-functional materials. Finally, sorption-enhanced reforming of toluene (chosen as tar model), of methane then of methane and toluene with bi-functional compounds were performed to study the best material to improve H2 content in a syngas, provided by steam biomass gasification. If the catalytic activity on the sorption enhanced reforming of methane exhibits a fast fall-down after 10–15 min of experimental test, the reforming of toluene reaches a constant conversion of 99.9% by using bi-functional materials

    Síntesis sol-gel de catalizadores de hierro soportados sobre sílice y titania para la oxidación selectiva de metano hasta formaldehído

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    Materiales de hierro soportados sobre sílice y titania fueron obtenidos por el método sol-gel para evaluar su activi-dad catalítica en la reacción de oxidación selectiva de metano hasta formaldehído. Se prepararon cuatro (4) catali-zadores, uno del soporte de sílice (catalizador 1S), otro para el soporte de titania (catalizador 1T) y los dos (2) restantes con carga de hierro de 0,5% en peso, para el soportado en sílice (catalizador 2FS) y para el soportado so-bre titania (catalizador 2FT). Las mayores áreas superficiales BET se obtienen para los materiales de sílice, cataliza-dores 1S y 2FS con valores de 659 y 850 m2/g respectivamente, mientras que los catalizadores sobre titania 1T y 2FT presentaron áreas de 65 y 54 m2/g respectivamente. Los análisis de microscopia electrónica de barrido y trans-misión muestran estructuras amorfas en el caso del soporte de sílice, mientras que para el soporte de titania los materiales son densos con estructura definida. El análisis de difracción de rayos X confirma la estructura amorfa de los materiales preparados con sílice y presenta la estructura de la anatasa para los materiales de titania. Los experi-mentos de reducción a temperatura programada muestran para los catalizadores 1S y 2FS ausencia de especies potencialmente reducibles, y para el caso de los catalizadores 1T y 2FT se presentan picos de consumo de hidró-geno que para el caso del 2FT están relacionados con la reducción de Fe3O4 hasta α-Fe vía intermedio de FexO. La espectroscopia Fotoelectrónica de rayos X confirma la presencia de Fe(III) con el valor de la energía de enlace en 710,6 e.V tanto para el catalizador 2FS como para el 2FT. La actividad catalítica se realiza a presión atmosférica en reactor de cuarzo, mezcla de reacción CH4/O2/N2 =7,5/1/4, intervalo de temperatura 400-800°C. Los produc-tos de reacción se analizan por cromatografía de gases con columnas Hayesep R y T y tamiz molecular de 5Å. La mejor respuesta para la oxidación del metano hasta formaldehído la presenta el catalizador 2FS, con un porcentaje de conversión de metano de 3,4% mol a 650°C, selectividad al formaldehído de 11,9% mol y rendimiento de 0,021 g HCHO/Kg catalizador.Iron materials supported on silica were prepared by the sol-gel method for evaluating catalytic activity in selective o-xidation of methane to formaldehyde. Four catalysts were prepared, one corresponding to the silica support (catalyst 1S), another to the titanium support (catalyst 1T) and two more having 0.5% weight iron loads, one for the silica su-pport (catalyst 2FS) and the last one the titanium support (catalyst 2FT). The higher BET areas were 659 and 850 m2/g for catalysts 1S and 2FS, respectively while catalysts 1T and 2FT displayed areas of 65 and 54 m2/g, respec-tively. Scanning and transmission electronic microscopy displayed an amorphous structure in the silica-supported materials while titanium-supported materials displayed dense materials having defined structure. X-ray diffraction confirmed the silica’s amorphous structure in 1S and 2FS catalysts and displayed the 1T and 2FT catalysts’ anatase structure. The programmed temperature reduction for the 1S and 2FS catalysts did not display reducible species, while displaying hydrogen consumption peaks related to Fe3O4 reduction to α-Fe via FexO route for 1T and 2FT ca-talysts. The electronic spectroscopy X-ray photo confirmed the Fe(III) specie as having 710.6 e.V binding energy for both 2FS and 2FT catalysts. Catalytic activity was carried out at atmospheric pressure in a quartz reactor, reaction mixture as CH4/O2/N2 =7.5/1/4 at 400-800°C temperature range. The reaction products were analysed by gas chromatography on Hayesep R and T columns using 5Å molecular screening. The best response for selective oxida-tion of methane to formaldehyde was displayed by the 2FS catalyst with 3.4% mol methane conversion at 650°C, 11.9% mol formaldehyde selectivity and 0.0211 g HCHO/Kg catalyst yield

    Elaboration d'un système de dépollution adapté aux appareils de chauffage domestique au bois

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    Les contextes climatique et énergétique mondiaux encouragent les pays de l'Union Européenne à améliorer leurs impacts environnementaux. Un des objectifs consiste à diminuer les émissions de CO2 en développant les énergies renouvelables. En France, la filière bois énergie représente la première source d'énergie renouvelable avec une production s'élevant à 10 MTep par an. Toutefois, il est indispensable de ne pas se limiter aux émissions de CO2 pour déterminer l'impact global d'une source d'énergie. En effet, la combustion de bois dans les appareils de chauffage domestique tels que les poêles, les inserts, les foyers ouverts, est à l'origine d'une part non négligeable de certains polluants atmosphériques tels que le CO, les COV, les HAP et les particules fines. L'objectif de ce projet est de réaliser un système efficace de dépollution capable de traiter l'ensemble des polluants à la sortie de ces appareils de chauffage. Des technologies sont déjà disponibles pour la dépollution des fumées issues de différentes sources de combustion, néanmoins nous devons intégrer les problématiques liées au fonctionnement de ces appareils ainsi que des critères de coût, de fonctionnalité et de développement durable définis dans un cahier des charges réalisé avec le partenaire industriel. Le travail réalisé nous à permis de concevoir et de tester un système complet capable de traiter tant les composants gazeux à l'aide d'un catalyseur à base de fer imprégné sur de la cérine, que les particules grâce à un lit filtrant régénéré par microondes. Le système décrit dans ce manuscrit présente une réduction faible des émissions, mais a permis de mettre en lumière les contraintes et les espoirs d'un futur système de traitement efficient.The global energy and climate contexts encourage EU countries to improve their environmental impacts. One goal is to reduce CO2 emissions by developing the use of renewable energies. In France, wood is the first renewable energy source with an equivalent of 10 Mtoe produced each year. However, it is essential to study the global environment impact of on this energy source including CO2 emissions but also the different pollutants emitted. Indeed, the combustion of wood in small home heating units as stoves, open and closed fireplaces, is responsible for a significant part of typical air pollutants such as CO, VOCs, PAHs and fine particles. The objective of this project is to develop an effective system able to treat both pollutants emittedfrom those heaters. Few technologies are already available for smoke after treatment. However, we must incorporate in our study constraints related to the operation of these wood heating devices as well as criteria of cost, functionality and sustainability defined in the specifications set with the industrial partner of this project. The result of the work performed in this project was the conception of a complete prototype tested for emissions reduction. The system is composed of ceria impregnated iron catalyst for gaseous compounds oxidation and a microwave regenerated bed filter for particles elimination. The tests performed on the prototype showed weak emissions abatement. Nevertheless, this project highlighted constraints and hopes for a future efficient after treatment system.STRASBOURG-Bib.electronique 063 (674829902) / SudocSudocFranceF

    Reforming of toluene with bimetallic catalysts supported on alumina and synthesized by an aqueous sol-gel process

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    peer reviewedThe thermochemical method called “biomass gasification” is generating emphatic interest for the production of bio-Syngas (CO+H2) since this process presents the advantage of being renewable without emitting CO2. However, in practical applications, there are still some technical problems due to high concentration of tars in the outlet gas, which can condensate and clog the pipes. Previous studies have highlighted the fact that the tar elimination via catalytic reforming seem to be the more practical and economical solution. Catalysts were synthesized by an aqueous sol-gel process to develop γ-Al2O3 doped with 10wt.% of nickel and 2 wt.% of a second dopant (Co, Cu, Fe, Mn, Mo). Before their adding in AlOOH sol, metallic dopants were complexed with (OCH3)3-Si-(CH2)3-NH-(CH2)2-NH2 (EDAS) to increase their dispersion by cogelation between EDAS and AlOOH clusters. All the samples were tested for toluene reforming

    Catalytic reforming of biomass gasification tars with bi- or tri-doped catalysts optimized with organosilane precursors

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    The thermochemical method called “biomass gasification” is generating emphatic interest for the production of bio-Syngas (CO + H2) since this process presents the advantage of being renewable without emitting CO2. However, in practical applications, there are still some technical problems due to high tars concentration in the outlet gas which can condensate and clog the pipes. Many studies have highlighted the fact that the tar elimination via catalytic reforming seem to be the more practical and economical solution. The required properties of the catalysts are determined by its location: inside the reactor (primary catalyst) or outside of the reactor (secondary catalyst). Primary catalysts are generally robust, non-toxic, cheap and they are almost uniquely destined to fluidized bed reactors. Secondary catalysts can be used at the exit of both fluidized and fixed bed reactors. They are characterized by a tailored mesoporous shape, a controlled active site dispersion and an adapted elemental composition [1]. In this work , we decided to focus on designing materials for secondary catalytic applications, i.e. working at relatively low temperature (~650°C) with no mechanical stress. The supports were made of γ-Al2O3 synthesized via an easy Sol-Gel method. During their synthesis, these supports were doped with 10%wt of nickel and various combinations of metallic dopants (Co, Cu, Fe, Mn, Mo) in the aim of enhancing their catalytic activities and lifetime
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