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Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles / Andrés T. Aguayo in Industrial & engineering chemistry research, Vol. 51 N° 40 (Octobre 2012) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 51 N° 40 (Octobre 2012) . - pp. 13073–13084 Titre : Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles Type de document : texte imprimé Auteurs : Andrés T. Aguayo, Auteur ; Ana G. Gayubo, Auteur ; Ainara Ateka, Auteur Année de publication : 2012 Article en page(s) : pp. 13073–13084 Note générale : Industrial chemistry Langues : Anglais (eng) Mots-clés : Methanol  Zeolite  Catalys Résumé : The joint transformation of methanol and n-butane has been studied under energy-neutral conditions (methanol/n-butane molar ratio of 3/1) on an HZSM-5 zeolite catalyst in order to determine the reactivation kinetics and optimize the process conditions for maximizing the light olefin production rate. The methodology for determining the reactivation kinetics combines the kinetic models for the main reaction and deactivation (determined in previous studies), as well as the experimental reactivation results obtained for a reaction step (at 500 and 550 °C) subsequent to regeneration by coke combustion with air (at 550 °C, up to 120 min). By simulation of the operation in reaction–regeneration cycles, an optimum average olefin production rate of 22 mol/(gcatalyst h) is obtained for a reaction temperature of 500 °C, space time of 0.37 gcatalyst h mol–1, time on stream of 40 min, and partial reactivation by coke combustion for 15 min. ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie301142k [article] Joint Transformation of Methanol and n-Butane into Olefins on an HZSM-5 Zeolite Catalyst in Reaction–Regeneration Cycles [texte imprimé] / Andrés T. Aguayo, Auteur ; Ana G. Gayubo, Auteur ; Ainara Ateka, Auteur . - 2012 . - pp. 13073–13084. Industrial chemistry Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 51 N° 40 (Octobre 2012) . - pp. 13073–13084 Mots-clés : Methanol  Zeolite  Catalys Résumé : The joint transformation of methanol and n-butane has been studied under energy-neutral conditions (methanol/n-butane molar ratio of 3/1) on an HZSM-5 zeolite catalyst in order to determine the reactivation kinetics and optimize the process conditions for maximizing the light olefin production rate. The methodology for determining the reactivation kinetics combines the kinetic models for the main reaction and deactivation (determined in previous studies), as well as the experimental reactivation results obtained for a reaction step (at 500 and 550 °C) subsequent to regeneration by coke combustion with air (at 550 °C, up to 120 min). By simulation of the operation in reaction–regeneration cycles, an optimum average olefin production rate of 22 mol/(gcatalyst h) is obtained for a reaction temperature of 500 °C, space time of 0.37 gcatalyst h mol–1, time on stream of 40 min, and partial reactivation by coke combustion for 15 min. ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie301142k

Kinetic Model for the Transformation of Bioethanol into Olefins over a HZSM-5 Zeolite Treated with Alkali / Ana G. Gayubo in Industrial & engineering chemistry research, Vol. 49 N° 21 (Novembre 2010) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 49 N° 21 (Novembre 2010) . - pp. 10836–10844 Titre : Kinetic Model for the Transformation of Bioethanol into Olefins over a HZSM-5 Zeolite Treated with Alkali Type de document : texte imprimé Auteurs : Ana G. Gayubo, Auteur ; Ainhoa Alonso, Auteur ; Beatriz Valle, Auteur Année de publication : 2011 Article en page(s) : pp. 10836–10844 Note générale : Chimie industrielle Langues : Anglais (eng) Mots-clés : Kinetic  Bioethanol  Zeolite Résumé : A kinetic model for the transformation of bioethanol (aqueous ethanol into hydrocarbons) has been established for a catalyst with slow deactivation by coke (prepared from a HZSM-5 zeolite treated with alkali in order to moderate its acid strength and generate mesopores in the zeolite structure). The kinetic model allows quantifying the distribution of the lumps of products (ethylene, C3−C4 olefins, gasoline or C5−C10, and C1−C3 paraffins) and is particularly interesting for quantifying the production of C3−C4 olefin lump, which is the one of greater commercial interest. The experimental data have been obtained in an isothermal fixed-bed reactor in a wide range of operating conditions (temperature of 300−400 °C, space time and water content in the feed). The remarkable features of the kinetic model are (i) consideration of the autocatalytic formation of C3−C4 olefin lump following their reaction with ethylene, (ii) consideration of the combined involvement of ethylene and the light olefin lump in the formation of heavier hydrocarbons; and (i) quantification of the effect of water in the reaction medium, which attenuates the rate of each one of the steps in the kinetic scheme, except the dehydration of ethanol which is instantaneous under these conditions. ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie100407d [article] Kinetic Model for the Transformation of Bioethanol into Olefins over a HZSM-5 Zeolite Treated with Alkali [texte imprimé] / Ana G. Gayubo, Auteur ; Ainhoa Alonso, Auteur ; Beatriz Valle, Auteur . - 2011 . - pp. 10836–10844. Chimie industrielle Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 49 N° 21 (Novembre 2010) . - pp. 10836–10844 Mots-clés : Kinetic  Bioethanol  Zeolite Résumé : A kinetic model for the transformation of bioethanol (aqueous ethanol into hydrocarbons) has been established for a catalyst with slow deactivation by coke (prepared from a HZSM-5 zeolite treated with alkali in order to moderate its acid strength and generate mesopores in the zeolite structure). The kinetic model allows quantifying the distribution of the lumps of products (ethylene, C3−C4 olefins, gasoline or C5−C10, and C1−C3 paraffins) and is particularly interesting for quantifying the production of C3−C4 olefin lump, which is the one of greater commercial interest. The experimental data have been obtained in an isothermal fixed-bed reactor in a wide range of operating conditions (temperature of 300−400 °C, space time and water content in the feed). The remarkable features of the kinetic model are (i) consideration of the autocatalytic formation of C3−C4 olefin lump following their reaction with ethylene, (ii) consideration of the combined involvement of ethylene and the light olefin lump in the formation of heavier hydrocarbons; and (i) quantification of the effect of water in the reaction medium, which attenuates the rate of each one of the steps in the kinetic scheme, except the dehydration of ethanol which is instantaneous under these conditions. ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie100407d

Kinetics of methanol transformation into hydrocarbons on a HZSM - 5 zeolite catalyst at high temperature (400 - 550 °C) / Andrés T. Aguayo in Industrial & engineering chemistry research, Vol. 49 N° 24 (Décembre 2010) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 49 N° 24 (Décembre 2010) . - pp. 12371–12378 Titre : Kinetics of methanol transformation into hydrocarbons on a HZSM - 5 zeolite catalyst at high temperature (400 - 550 °C) Type de document : texte imprimé Auteurs : Andrés T. Aguayo, Auteur ; Diana Mier, Auteur ; Ana G. Gayubo, Auteur Année de publication : 2011 Article en page(s) : pp. 12371–12378 Note générale : Chimie industrielle Langues : Anglais (eng) Mots-clés : Kinetics  Zeolite  catalyst Résumé : A kinetic model of seven lumps has been established which allows the quantification of the product distribution (oxygenates, n-butane, C2−C4 olefins, C2−C4 paraffins (without n-butane), C5−C10 fraction, methane) in the transformation of methanol into hydrocarbons at high temperature (400−550 °C) on a HZSM-5 zeolite catalyst (SiO2/Al2O3 = 30) with high acidic strength (>120 kJ (mol of NH3)−1) and agglomerated with bentonite and alumina. The kinetic model fits well the experimental data obtained in a fixed bed reactor, from small values of space time in which the formation of hydrocarbons is incipient, to a space time of 2.4 (g of catalyst) h (mol CH2) −1 for a complete conversion of methanol. The rise in temperature increases the yield of C2−C4 olefins, so that the maximum value (50%) is obtained at the ceiling temperature for the hydrothermal stability of the HZSM-5 (550 °C) and space times between 0.6 and 1 (g of catalyst) h (mol CH2)−1. DEWEY : 660 ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie101047f [article] Kinetics of methanol transformation into hydrocarbons on a HZSM - 5 zeolite catalyst at high temperature (400 - 550 °C) [texte imprimé] / Andrés T. Aguayo, Auteur ; Diana Mier, Auteur ; Ana G. Gayubo, Auteur . - 2011 . - pp. 12371–12378. Chimie industrielle Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 49 N° 24 (Décembre 2010) . - pp. 12371–12378 Mots-clés : Kinetics  Zeolite  catalyst Résumé : A kinetic model of seven lumps has been established which allows the quantification of the product distribution (oxygenates, n-butane, C2−C4 olefins, C2−C4 paraffins (without n-butane), C5−C10 fraction, methane) in the transformation of methanol into hydrocarbons at high temperature (400−550 °C) on a HZSM-5 zeolite catalyst (SiO2/Al2O3 = 30) with high acidic strength (>120 kJ (mol of NH3)−1) and agglomerated with bentonite and alumina. The kinetic model fits well the experimental data obtained in a fixed bed reactor, from small values of space time in which the formation of hydrocarbons is incipient, to a space time of 2.4 (g of catalyst) h (mol CH2) −1 for a complete conversion of methanol. The rise in temperature increases the yield of C2−C4 olefins, so that the maximum value (50%) is obtained at the ceiling temperature for the hydrothermal stability of the HZSM-5 (550 °C) and space times between 0.6 and 1 (g of catalyst) h (mol CH2)−1. DEWEY : 660 ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie101047f

Olefin production by catalytic transformation of crude bio-oil in a two-step process / Ana G. Gayubo in Industrial & engineering chemistry research, Vol. 49 N° 1 (Janvier 2010) 

Public ISBD [article]  in Industrial & engineering chemistry research > Vol. 49 N° 1 (Janvier 2010) . - pp. 123–131 Titre : Olefin production by catalytic transformation of crude bio-oil in a two-step process Type de document : texte imprimé Auteurs : Ana G. Gayubo, Auteur ; Beatriz Valle, Auteur ; Andrés T. Aguayo, Auteur Année de publication : 2010 Article en page(s) : pp. 123–131 Note générale : Industrail chemistry Langues : Anglais (eng) Mots-clés : Olefin--Production--Catalytic--Transformation--Crude--Bio-Oil----Two-Step  Process Résumé : The valorization of crude bio-oil by catalytic transformation into hydrocarbons has been carried out in an online two-step (thermal-catalytic) process. The deposition of pyrolytic lignin, formed by polymerization of biomass-derived products, is enhanced in the thermal step. Volatiles are processed in a fluidized bed reactor with a catalyst that is hydrothermally stable and selective for olefin production, which has been based on a HZSM-5 zeolite. A study has been made of the effect of operating conditions (methanol content in the feed of bio-oil/methanol, temperature, space time, and time on stream) on bio-oil conversion, product lump yields and the selectivity of each individual C2−C4 olefin. These conditions also have a significant effect on deactivation, which is attributed to coke deposited on the catalyst. The TPO curves of coke combustion identify two fractions: one of thermal origin (pyrolytic lignin) and the other of catalytic origin, whose formation depends on the concentration of oxygenates in the reaction medium. A feed with 50 wt % of methanol, at 500 °C, with space time of 0.371 (g of catalyst) h (g of methanol)−1 allows a 94 wt % conversion of the bio-oil in the feed, with a selectivity of C2−C4 olefins of 48 wt % (50 wt % is propene) and low yields of CO and CO2 (its formation is attenuated by cofeeding methanol). ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie901204n [article] Olefin production by catalytic transformation of crude bio-oil in a two-step process [texte imprimé] / Ana G. Gayubo, Auteur ; Beatriz Valle, Auteur ; Andrés T. Aguayo, Auteur . - 2010 . - pp. 123–131. Industrail chemistry Langues : Anglais (eng) in Industrial & engineering chemistry research > Vol. 49 N° 1 (Janvier 2010) . - pp. 123–131 Mots-clés : Olefin--Production--Catalytic--Transformation--Crude--Bio-Oil----Two-Step  Process Résumé : The valorization of crude bio-oil by catalytic transformation into hydrocarbons has been carried out in an online two-step (thermal-catalytic) process. The deposition of pyrolytic lignin, formed by polymerization of biomass-derived products, is enhanced in the thermal step. Volatiles are processed in a fluidized bed reactor with a catalyst that is hydrothermally stable and selective for olefin production, which has been based on a HZSM-5 zeolite. A study has been made of the effect of operating conditions (methanol content in the feed of bio-oil/methanol, temperature, space time, and time on stream) on bio-oil conversion, product lump yields and the selectivity of each individual C2−C4 olefin. These conditions also have a significant effect on deactivation, which is attributed to coke deposited on the catalyst. The TPO curves of coke combustion identify two fractions: one of thermal origin (pyrolytic lignin) and the other of catalytic origin, whose formation depends on the concentration of oxygenates in the reaction medium. A feed with 50 wt % of methanol, at 500 °C, with space time of 0.371 (g of catalyst) h (g of methanol)−1 allows a 94 wt % conversion of the bio-oil in the feed, with a selectivity of C2−C4 olefins of 48 wt % (50 wt % is propene) and low yields of CO and CO2 (its formation is attenuated by cofeeding methanol). ISSN : 0888-5885 En ligne : http://pubs.acs.org/doi/abs/10.1021/ie901204n