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See detailNi-doped γ-Al2O3 as secondary catalyst for bio-syngas purification: influence of Ni loading, catalyst preparation and gas composition on catalytic activity
Claude, Vincent; Mahy, Julien ULiege; Geens, Jérémy ULiege et al

in Materials Today Chemistry (2019), 13

In this work, Ni/γ-Al2O3 catalysts were prepared by sol-gel methods with different Ni loadings (10 to 50 wt.%) and used as secondary catalyst for the steam reforming of toluene. A sample prepared by wet ... [more ▼]

In this work, Ni/γ-Al2O3 catalysts were prepared by sol-gel methods with different Ni loadings (10 to 50 wt.%) and used as secondary catalyst for the steam reforming of toluene. A sample prepared by wet impregnation with 10 wt.% of Ni was also synthesized and compared to the corresponding sol-gel sample. This study was divided in three main parts: the comparison of catalysts prepared by sol-gel process and impregnation, the influence of the gas composition on the catalytic performance of the sol-gel 10 wt.% Ni/γ-Al2O3 catalyst and the influence of Ni loading on the catalytic activity. When sol-gel and impregnated samples are compared, the impregnated catalyst showed a high initial toluene conversion followed by a consequent and progressive deactivation. Contrarily, the sol-gel catalyst showed a stable catalytic activity and relatively low carbon deposit. Indeed, before the steam reforming of toluene at 650 °C, the sol-gel catalyst was only calcined and no reduction step was realized to reduce nickel oxide. So this sample was reduced during the catalytic test at 650 °C. Moreover, it was observed that, if toluene was withdrawn from the syngas mixture during the catalytic test, the sol-gel sample was progressively re-oxidized by CO2 and H2O, leading to higher deactivation. As the Ni loading increased, the nickel oxide with strong interactions (NiAl2O4) was progressively joined by nickel oxide with low interactions (NiO/Al2O3) and bulk nickel oxide (NiO). This led to a high initial conversion of toluene, but also to a progressive loss of the catalytic activity throughout the catalytic test. It was shown that the sol-gel method developed throughout this work allowed preparing micro/mesoporous Ni/γ-Al2O3 catalysts with a high dispersion of Ni nanoparticles. [less ▲]

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See detailSynthesis of Ni/γ-Al2O3-SiO2 catalysts with different silicon precursors for the steam toluene reforming
Claude, Vincent; Mahy, Julien ULiege; Geens, Jérémy ULiege et al

in Microporous and Mesoporous Materials (2019), 284

This work investigated the intrinsic properties and performances of Ni/γ-Al2O3-SiO2 modified with different silicon precursors for the steam reforming of toluene in biomass gasifier exit conditions (8000 ... [more ▼]

This work investigated the intrinsic properties and performances of Ni/γ-Al2O3-SiO2 modified with different silicon precursors for the steam reforming of toluene in biomass gasifier exit conditions (8000 ppmv of toluene, 650 °C). Samples were synthesized by an aqueous sol-gel process in presence of aluminum nitrate, nickel nitrate and the use of either tetramethoxysilane (TMOS, Si-(OCH3)4) or tetraethoxysilane (TEOS, Si-(OC2H5)4) in order to understand the influence of the reactivity of the silicon precursor. Furthermore, the use of N-[3-(trimethoxysilyl)propyl]ethylenediamine (EDAS, (OCH3)3-Si-(CH2)3-NH-(CH2)2-NH2) is also investigated in order to understand the influence of a silicon precursor containing an ethylenediamine group, able to complex Ni2+ ions. By the chelation of Ni2+ ions by ethylenediamine groups during the synthesis, Ni/γ-Al2O3-SiO2 samples modified with EDAS showed higher dispersion of the metallic Ni nanoparticles and the higher resistance against the sintering of Ni particles. This was also attributed to the high microporous volume and the narrow mesoporous distribution of the support, which could also prevent the migration of the metallic Ni nanoparticles. The catalytic tests revealed that the reactivity of the silicon precursor played a major role on the conversion of toluene. For alumina supports modified with a silicon precursor with a low reactivity such as TEOS, the low integration of the Si atoms inside the bulk alumina lead to a slightly higher catalytic activity, but also to a high formation of structured carbon. The opposite effect was observed for the samples modified with a highly reactive silicon precursor, such as TMOS or EDAS, which showed a slightly lower catalytic activity, but a higher resistance against coking compared to pure Ni/γ-Al2O3 catalysts. [less ▲]

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See detailCatalytic reforming of biomass gasification tars with bimetallic catalysts
Claude, Vincent; Solis Garcia, Hugo Fernando ULiege; Geens, Jérémy ULiege et al

Poster (2018, July 11)

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 ... [more ▼]

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. The objectives of this project is to synthesize, characterize and evaluate the catalytic performances of Ni/γ-Al2O3 catalysts doped with different metals (Cu, Co, Mo, Mn, Fe). [less ▲]

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See detailCatalytic reforming of biomass gasification tars with bimetallic catalysts
Wolfs, Cédric ULiege; Claude, Vincent; Lambert, Stéphanie ULiege

Poster (2017, September 07)

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 ... [more ▼]

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 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. Reforming catalysts present the following properties : a tailored mesoporous texture for the support and the high dispersion of active sites like metallic nanoparticles (Ni, Pd, Fe,…) [1]. In this work, Ni based alumina catalysts and doped with a second metal (Co, Cu, Fe, Mn, Mo) are synthesized by an aqueous sol-gel process. [less ▲]

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See detailCorrection to overview and essentials of biomass gasification technologies and their catalytic cleaning methods
Claude, Vincent; Courson, Claire; Kölher, Martina et al

in Energy & Fuels (2017), 31

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See detailElaboration of an Easy Aqueous Sol-Gel Method for the Synthesis of Micro- and Mesoporous γ-Al2O3 Supports
Claude, Vincent; Solis Garcia, Hugo Fernando ULiege; Wolfs, Cédric ULiege et al

in Advances in Materials Physics and Chemistry (2017), 7

An aqueous sol-gel method for the synthesis of γ-Al2O3 supports has been developed for the use in tar reforming applications. It was determined the influences of two different aluminum precursors ... [more ▼]

An aqueous sol-gel method for the synthesis of γ-Al2O3 supports has been developed for the use in tar reforming applications. It was determined the influences of two different aluminum precursors (aluminum sec -butoxide (Al[OCH(CH3)CH2CH3]3) and aluminum nitrate (Al(NO3)3)) on the textural and crystallographic properties of Al2O3 supports. Only the formation of γ- Al2O3 is aimed in order to use these alumina materials as catalytic supports, because it presents high specific surface area and pore volume values. Additionally, the synthesis of γ-Al2O3 was realized with the use of a functionalized silicon precursor, [3-(2-aminoethylamino)propyl]trimethoxysilane, called EDAS. By the presence of an ethylenediamine group in this molecule, it is possible to chelate metallic ions and to highly increase their dispersion at a molecular level during the synthesis of metallic catalysts supported on alumina, which is an asset for catalytic applications. So it was developed a synthesis sol-gel procedure for the cogelation between the functionalized silicon alkoxide EDAS and alumina precursor. The alumina supports synthesized with Al(NO3)3 as precursor presented higher porous values than the ones obtained with aluminium sec-butoxide precursor. Since nitrate salts are much easier to handle than alkoxides, these observations allowed validating Al(NO3)3 as aluminum source for the future synthesis procedures for metallic catalysts supported on alumina. [less ▲]

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See detailReforming of toluene with bimetallic catalysts supported on alumina and synthesized by an aqueous sol-gel process
Wolfs, Cédric ULiege; Claude, Vincent; Courson, Claire et al

in Journal of Advanced Chemical Engineering (2017), 7

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 ... [more ▼]

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 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. [less ▲]

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