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Marta Díaz,Eva Epelde,Andrés T. Aguayo,Javier Bilbao 한국공업화학회 2020 Journal of Industrial and Engineering Chemistry Vol.87 No.-
The capacity of HZSM-5 zeolite (SiO2/Al2O3 ratio = 30–280) based catalysts with a hierarchical porousstructure has been explored for the oligomerization of 1-butene at low pressure. Catalysts werecharacterized (structural, physical and acid properties) and tested in afixed bed reactor under thefollowing conditions: 1.5 bar; 175–325 C; space time, 0.5–10 gcatalyst h (molC) 1; butene partial pressure,0.375–1.5 bar; time on stream, 10 h. Results were evaluated with the aim of boosting naphtha (C5-C12=)fraction. A good compromise between conversion (62% in C units contained) and naphtha yield (42%) wasachieved by using a HZSM-5 zeolite with SiO2/Al2O3 = 30 at 275 C and 6 gcatalyst h (molC) 1, where 23%corresponds to C8-C12= and 19% to C5-C7=, respectively. Furthermore, the hierarchical porous structurefacilitated catalysts to tend to a pseudo-stationary deactivation state after 2–3 h time on stream, whichcould be interesting for process scale up.
Catalytic steam reforming of biomass fast pyrolysis volatiles over Ni–Co bimetallic catalysts
Laura Santamaria,Gartzen Lopez,Aitor Arregi,Maite Artetxe,Maider Amutio,Javier Bilbao,Martin Olazar 한국공업화학회 2020 Journal of Industrial and Engineering Chemistry Vol.91 No.-
The influence of the metal selected as catalytic active phase in the two-step biomass pyrolysis-catalyticreforming strategy has been analyzed. The pyrolysis step was carried out in a conical spouted bed reactorat 500 C, whereas steam reforming was performed in afluidized bed reactor at 600 C. Ni/Al2O3,Co/Al2O3 and two bimetallic Ni-Co/Al2O3 catalysts with different metal loadings were synthesized by wetimpregnation method, and fresh and deactivated catalysts were characterized by N2 adsorption/desorption, X-ray Fluorescence (XRF), Temperature Programmed Reduction (TPR), X-Ray powderDiffraction (XRD), Temperature Programmed Oxidation (TPO), Scanning Electron Microscopy (SEM) andTransmission Electron Microscopy (TEM). Although Ni/Al2O3 and both bimetallic catalysts had similarinitial activity in terms of oxygenate conversion, (higher than 98%), the poorer metal dispersion observedin both bimetallic catalysts led to a fast decrease in conversion due to the promotion of coke formation onlarge particles. This occurred even though Ni–Co alloy formation has a positive influence by hindering theoxidation of Co0 species. The main cause for the deactivation of these catalysts is the formation of a cokewith amorphous structure. The poor initial performance of Co/Al2O3 catalyst is related to changes in theCo0 oxidation state induced by the presence of steam, which led to a fast deactivation of this catalyst.
Reaction network of the chloromethane conversion into light olefins using a HZSM-5 zeolite catalyst
Monica Gamero,Beatriz Valle,Pedro Castaño,Andrés T. Aguayo,Javier Bilbao 한국공업화학회 2018 Journal of Industrial and Engineering Chemistry Vol.61 No.-
The second step of chlorine-mediated methane valorization into hydrocarbons has been investigated using a HZSM-5 zeolite catalyst. A parametric study has enabled to set the reaction network, which is dominated by the dual cycle mechanism and secondary reactions of light olefins. This network explains the formation of methane, light olefins, C5+ aliphatics, paraffins, aromatics and coke. Under the optimal conditions, the light olefin selectivity is >70%, of which >40% corresponds to propylene. Coke is originated in the zeolite micropores and then grows within the matrix meso- and macropores.
Catalytic cracking of raw bio-oil under FCC unit conditions over different zeolite-based catalysts
Alvaro Ibarra,Idoia Hita,Miren J. Azkoiti,Jose M. Arandes,Javier Bilbao 한국공업화학회 2019 Journal of Industrial and Engineering Chemistry Vol.78 No.-
The performance of different zeolite-based catalysts (HY, HZSM-5 and HBeta) on the catalytic cracking ofbio-oil has been explored, using a simulated riser reactor and resembling industrial FCC conditions. Theeffect of the C/O (catalyst/bio-oil) ratio and the zeolite types have been assessed. The level ofdeoxygenation is >61% (increasing with C/O ratio). Total hydrocarbon yield was higher for the HBetacatalyst (56 wt%), while the liquid hydrocarbons yields were relatively similar for all catalysts, obtaininghigher gasoline yields with the HY catalyst (46–55 wt%), and higher LPG yields with the HZSM-5 catalyst(12–14 wt%) due to its higher acidity. The HY zeolite produced more coke (4–7 wt%) given its capacity forretaining coke precursors within its micropores.
Lide Oar-Arteta,,Aingeru Remiro,Andre´ s T. Aguayo,Martin Olazar,Javier Bilbao,Ana G. Gayubo 한국공업화학회 2016 Journal of Industrial and Engineering Chemistry Vol.36 No.-
This study aims at optimizing the composition of the bifunctional catalyst with CuFe2O4 spinel metallicfunction for the steam reforming of DME (SRD). The g-Al2O3 obtained by calcination of boehmite at550 8C proves to be the most suitable acid function, given that it provides high activity for DMEhydrolysis and avoids hydrocarbon formation in the 300–400 8C range. Furthermore, the optimum massratio between CuFe2O4 and g-Al2O3 functions is 1/1 at 350 8C, since it allows obtaining the highest DMEconversion and H2 yield with suitable catalyst stability and mechanical resistance.
Regenerability of a Ni catalyst in the catalytic steam reforming of biomass pyrolysis volatiles
Aitor Arregi,Gartzen Lopez,Maider Amutio,Itsaso Barbarias,Laura Santamaria,Javier Bilbao,Martin Olazar 한국공업화학회 2018 Journal of Industrial and Engineering Chemistry Vol.68 No.-
A study has been carried out of the regenerability of a commercial Ni catalyst used in the steam reforming of the volatiles from biomass pyrolysis (gases and bio-oil), determining the evolution of the reaction indices (conversion, product yields and H2 production) in successive reaction–regeneration cycles. The causes of catalyst deactivation (coke deposition and Ni sintering) have been ascertained characterizing the deactivated and regenerated catalysts by TPO, TEM, TPR and XRD. Catalyst activity is not fully recovered by coke combustion in the first cycles due to the irreversible deactivation by Ni sintering, but the catalyst reaches a pseudo-stable state beyond the fourth cycle, reproducing its behaviour in subsequent cycles.
Hydrodeoxygenation of raw bio-oil towards platform chemicals over FeMoP/zeolite catalysts
Idoia Hita,Tomás Cordero-Lanzac,Giuseppe Bonura,Catia Cannilla,José M. Arandes,Francesco Frusteri,Javier Bilbao 한국공업화학회 2019 Journal of Industrial and Engineering Chemistry Vol.80 No.-
The hydrodeoxygenation of raw bio-oil was investigated in a continuousfixed bed reactor over a series ofFeMoP/zeolite catalysts, pursuing a maximized and stable production of phenolics and aromatics. After5 h of reaction, the catalysts reach a pseudosteady activity state. The FeMoP/HZSM-5 catalyst yields thehighest amount of carbon products (53.5 wt%) with the highest selectivity towards aromatics (13.6 wt%,dry basis) and phenolics (12.2 wt%), due to the synergy between the weak acidity of the FeMoP and themild acidity of the HZSM-5 zeolite, which minimizes dehydration and gasification. The MFI frameworkallows the sweeping of coke precursors.