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PUBLICATIONS
2018
García, Lucía; Valiente, Ana; Oliva, Miriam; Ruiz, Joaquín; Arauzo, Jesús
Influence of operating variables on the aqueous-phase reforming of glycerol over a Ni/Al coprecipitated catalyst Journal Article
In: International Journal of Hydrogen Energy, vol. 43, no. 45, pp. 20392–20407, 2018, ISSN: 03603199.
@article{Garcia2018,
title = {Influence of operating variables on the aqueous-phase reforming of glycerol over a Ni/Al coprecipitated catalyst},
author = {Lucía García and Ana Valiente and Miriam Oliva and Joaquín Ruiz and Jesús Arauzo},
doi = {10.1016/j.ijhydene.2018.09.119},
issn = {03603199},
year = {2018},
date = {2018-11-01},
journal = {International Journal of Hydrogen Energy},
volume = {43},
number = {45},
pages = {20392--20407},
publisher = {Elsevier Ltd},
abstract = {A systematic study focused on the aqueous-phase reforming of glycerol has been carried out in order to analyze the influence of several operating variables (system pressure, reaction temperature, glycerol content in feed, liquid feeding rate and catalyst weight/glycerol flow rate ratio) on the gas and liquid products. A continuous flow bench scale installation and a Ni/Al coprecipitated catalyst were employed. The system pressure was varied from 28 to 40 absolute bar, the reaction temperature was analyzed from 495 to 510 K, the glycerol content in the feed was studied from 2 to 10 wt%, the liquid feeding rate was changed from 0.5 to 3.0 mL/min and the catalyst weight/glycerol flow rate ratio varied from 10 to 40 g catalyst min/g glycerol. The main gas products obtained were H2, CO2 and CH4, while the main liquid products were 1,2-propanediol, ethylene glycol, acetol and ethanol. A W/mglycerol ratio of 40 g catalyst min/g glycerol, 34 bar, 500 K, 5 wt% glycerol and 1 mL/min, resulted in a high yield to H2 (6.8%), the highest yield to alkanes (10.7%), the highest 1,2-propanediol yield (0.20 g/g glycerol) and the highest ethylene glycol yield (0.11 g/g glycerol). The highest acetol yield (0.06 g/g glycerol) was obtained at 34 bar, 500 K, 5 wt% glycerol, 20 g catalyst min/g glycerol and 3 mL/min.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
A systematic study focused on the aqueous-phase reforming of glycerol has been carried out in order to analyze the influence of several operating variables (system pressure, reaction temperature, glycerol content in feed, liquid feeding rate and catalyst weight/glycerol flow rate ratio) on the gas and liquid products. A continuous flow bench scale installation and a Ni/Al coprecipitated catalyst were employed. The system pressure was varied from 28 to 40 absolute bar, the reaction temperature was analyzed from 495 to 510 K, the glycerol content in the feed was studied from 2 to 10 wt%, the liquid feeding rate was changed from 0.5 to 3.0 mL/min and the catalyst weight/glycerol flow rate ratio varied from 10 to 40 g catalyst min/g glycerol. The main gas products obtained were H2, CO2 and CH4, while the main liquid products were 1,2-propanediol, ethylene glycol, acetol and ethanol. A W/mglycerol ratio of 40 g catalyst min/g glycerol, 34 bar, 500 K, 5 wt% glycerol and 1 mL/min, resulted in a high yield to H2 (6.8%), the highest yield to alkanes (10.7%), the highest 1,2-propanediol yield (0.20 g/g glycerol) and the highest ethylene glycol yield (0.11 g/g glycerol). The highest acetol yield (0.06 g/g glycerol) was obtained at 34 bar, 500 K, 5 wt% glycerol, 20 g catalyst min/g glycerol and 3 mL/min.
2016
Remón, Javier; Ruiz, Joaquín; Oliva, Miriam; García, Lucía; Arauzo, Jesús
Effect of biodiesel-derived impurities (acetic acid, methanol and potassium hydroxide) on the aqueous phase reforming of glycerol Journal Article
In: Chemical Engineering Journal, vol. 299, pp. 431–448, 2016, ISSN: 13858947.
@article{Remon2016a,
title = {Effect of biodiesel-derived impurities (acetic acid, methanol and potassium hydroxide) on the aqueous phase reforming of glycerol},
author = {Javier Remón and Joaquín Ruiz and Miriam Oliva and Lucía García and Jesús Arauzo},
doi = {10.1016/j.cej.2016.05.018},
issn = {13858947},
year = {2016},
date = {2016-09-01},
journal = {Chemical Engineering Journal},
volume = {299},
pages = {431--448},
publisher = {Elsevier B.V.},
abstract = {This work analyses the influence of three biodiesel-derived impurities (CH3OH, CH3COOH and KOH) on the aqueous phase reforming of glycerol at 220 °C and 44 bar using a Ni-La/Al2O3 catalyst. The experiments were planed according to a factorial 2k design and analysed by means of an analysis of variance (ANOVA) test to identify the effect of each impurity and all possible binary and ternary combinations. The presence of CH3OH decreased the glycerol conversion, while CH3COOH and KOH decreased and increased the gas production, respectively. Catalyst deactivation took place under acidic conditions due to the loss of part of the active phase of the catalyst through leaching. The gas phase was made up of H2, CO2, CO and CH4. KOH exerted the greatest influence on the gas composition, increasing H2 production due to the greater gas production and the lower H2 consumption in the hydrogenation reactions. The liquid phase was made up of aldehydes, monohydric and polyhydric alcohols, C3 and C4 ketones and esters. CH3OH increased the proportion of monohydric alcohols, while CH3COOH promoted dehydration reactions, leading to an increase in the relative amount of C3-ketones.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
This work analyses the influence of three biodiesel-derived impurities (CH3OH, CH3COOH and KOH) on the aqueous phase reforming of glycerol at 220 °C and 44 bar using a Ni-La/Al2O3 catalyst. The experiments were planed according to a factorial 2k design and analysed by means of an analysis of variance (ANOVA) test to identify the effect of each impurity and all possible binary and ternary combinations. The presence of CH3OH decreased the glycerol conversion, while CH3COOH and KOH decreased and increased the gas production, respectively. Catalyst deactivation took place under acidic conditions due to the loss of part of the active phase of the catalyst through leaching. The gas phase was made up of H2, CO2, CO and CH4. KOH exerted the greatest influence on the gas composition, increasing H2 production due to the greater gas production and the lower H2 consumption in the hydrogenation reactions. The liquid phase was made up of aldehydes, monohydric and polyhydric alcohols, C3 and C4 ketones and esters. CH3OH increased the proportion of monohydric alcohols, while CH3COOH promoted dehydration reactions, leading to an increase in the relative amount of C3-ketones.
Remón, Javier; Ruiz, Joaquín; Oliva, Miriam; García, Lucía; Arauzo, Jesús
Cheese whey valorisation: Production of valuable gaseous and liquid chemicals from lactose by aqueous phase reforming Journal Article
In: Energy Conversion and Management, vol. 124, pp. 453–469, 2016, ISSN: 01968904.
@article{Remon2016h,
title = {Cheese whey valorisation: Production of valuable gaseous and liquid chemicals from lactose by aqueous phase reforming},
author = {Javier Remón and Joaquín Ruiz and Miriam Oliva and Lucía García and Jesús Arauzo},
doi = {10.1016/j.enconman.2016.07.044},
issn = {01968904},
year = {2016},
date = {2016-09-01},
journal = {Energy Conversion and Management},
volume = {124},
pages = {453--469},
publisher = {Elsevier Ltd},
abstract = {Cheese effluent management has become an important issue owing to its high biochemical oxygen demand and chemical oxygen demand values. Given this scenario, this work addresses the valorisation of lactose (the largest organic constituent of this waste) by aqueous phase reforming, analysing the influence of the most important operating variables (temperature, pressure, lactose concentration and mass of catalyst/lactose mass flow rate ratio) as well as optimising the process for the production of either gaseous or liquid value-added chemicals. The carbon converted into gas, liquid and solid products varied as follows: 5–41%, 33–97% and 0–59%, respectively. The gas phase was made up of a mixture of H2 (8–58 vol.%), CO2 (33–85 vol.%), CO (0–15 vol.%) and CH4 (0–14 vol.%). The liquid phase consisted of a mixture of aldehydes: 0–11%, carboxylic acids: 0–22%, monohydric alcohols: 0–23%, polyhydric-alcohols: 0–48%, C3-ketones: 4–100%, C4-ketones: 0–18%, cyclic-ketones: 0–15% and furans: 0–85%. H2 production is favoured at high pressure, elevated temperature, employing a high amount of catalyst and a concentrated lactose solution. Liquid production is preferential using diluted lactose solutions. At high pressure, the production of C3-ketones is preferential using a high temperature and a low amount of catalyst, while a medium temperature and a high amount of catalyst favours the production of furans. The production of alcohols is preferential using medium temperature and pressure and a low amount of catalyst.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Cheese effluent management has become an important issue owing to its high biochemical oxygen demand and chemical oxygen demand values. Given this scenario, this work addresses the valorisation of lactose (the largest organic constituent of this waste) by aqueous phase reforming, analysing the influence of the most important operating variables (temperature, pressure, lactose concentration and mass of catalyst/lactose mass flow rate ratio) as well as optimising the process for the production of either gaseous or liquid value-added chemicals. The carbon converted into gas, liquid and solid products varied as follows: 5–41%, 33–97% and 0–59%, respectively. The gas phase was made up of a mixture of H2 (8–58 vol.%), CO2 (33–85 vol.%), CO (0–15 vol.%) and CH4 (0–14 vol.%). The liquid phase consisted of a mixture of aldehydes: 0–11%, carboxylic acids: 0–22%, monohydric alcohols: 0–23%, polyhydric-alcohols: 0–48%, C3-ketones: 4–100%, C4-ketones: 0–18%, cyclic-ketones: 0–15% and furans: 0–85%. H2 production is favoured at high pressure, elevated temperature, employing a high amount of catalyst and a concentrated lactose solution. Liquid production is preferential using diluted lactose solutions. At high pressure, the production of C3-ketones is preferential using a high temperature and a low amount of catalyst, while a medium temperature and a high amount of catalyst favours the production of furans. The production of alcohols is preferential using medium temperature and pressure and a low amount of catalyst.
2013
Bimbela, Fernando; Oliva, Miriam; Ruiz, Joaquín; García, Lucía; Arauzo, Jesús
Hydrogen production via catalytic steam reforming of the aqueous fraction of bio-oil using nickel-based coprecipitated catalysts Journal Article
In: International Journal of Hydrogen Energy, vol. 38, no. 34, pp. 14476–14487, 2013, ISSN: 03603199.
@article{Bimbela2013,
title = {Hydrogen production via catalytic steam reforming of the aqueous fraction of bio-oil using nickel-based coprecipitated catalysts},
author = {Fernando Bimbela and Miriam Oliva and Joaquín Ruiz and Lucía García and Jesús Arauzo},
url = {http://www.sciencedirect.com/science/article/pii/S0360319913022295},
issn = {03603199},
year = {2013},
date = {2013-11-01},
journal = {International Journal of Hydrogen Energy},
volume = {38},
number = {34},
pages = {14476--14487},
abstract = {Hydrogen production was studied in the catalytic steam reforming of a synthetic and a real aqueous fraction of bio-oil. Ni/Al coprecipitated catalysts with varying nickel content (23, 28 and 33 relative atomic %) were prepared by an increasing pH technique and tested during 2 h under different experimental conditions in a small bench scale fixed bed setup. The 28% Ni catalyst yielded a more stable performance over time (steam-to-carbon molar ratio, S/C = 5.58) at 650 °C and a catalyst weight/organic flow rate (W/morg) ratio of 1.7 g catalyst min/g organic. Using the synthetic aqueous fraction as feed, almost complete overall carbon conversion to gas and hydrogen yields close to equilibrium could be obtained with the 28% Ni catalyst throughout. Up to 63% of overall carbon conversion to gas and an overall hydrogen yield of 0.09 g/g organic could be achieved when using the real aqueous fraction of bio-oil, but the catalyst performance showed a decay with time after 20 min of reaction due to severe coke deposition. Increasing the W/morg ratio up to 5 g catalyst min/g organic yielded a more stable catalyst performance throughout, but overall carbon conversion to gas did not surpass 83% and the overall hydrogen yield was only ca. 77% of the thermodynamic equilibrium. Increasing reaction temperatures (600–800 °C) up to 750 °C enhanced the overall carbon conversion to gas and the overall yield to hydrogen. However, at 800 °C the catalyst performance was slightly worse, as a result of an increase in thermal cracking reactions leading to an increased formation of carbon deposits.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Hydrogen production was studied in the catalytic steam reforming of a synthetic and a real aqueous fraction of bio-oil. Ni/Al coprecipitated catalysts with varying nickel content (23, 28 and 33 relative atomic %) were prepared by an increasing pH technique and tested during 2 h under different experimental conditions in a small bench scale fixed bed setup. The 28% Ni catalyst yielded a more stable performance over time (steam-to-carbon molar ratio, S/C = 5.58) at 650 °C and a catalyst weight/organic flow rate (W/morg) ratio of 1.7 g catalyst min/g organic. Using the synthetic aqueous fraction as feed, almost complete overall carbon conversion to gas and hydrogen yields close to equilibrium could be obtained with the 28% Ni catalyst throughout. Up to 63% of overall carbon conversion to gas and an overall hydrogen yield of 0.09 g/g organic could be achieved when using the real aqueous fraction of bio-oil, but the catalyst performance showed a decay with time after 20 min of reaction due to severe coke deposition. Increasing the W/morg ratio up to 5 g catalyst min/g organic yielded a more stable catalyst performance throughout, but overall carbon conversion to gas did not surpass 83% and the overall hydrogen yield was only ca. 77% of the thermodynamic equilibrium. Increasing reaction temperatures (600–800 °C) up to 750 °C enhanced the overall carbon conversion to gas and the overall yield to hydrogen. However, at 800 °C the catalyst performance was slightly worse, as a result of an increase in thermal cracking reactions leading to an increased formation of carbon deposits.
2011
Bimbela, Fernando; Oliva, Miriam; Ruiz, Joaquín; García, Lucía; Arauzo, Jesús
Steam Reforming of Bio-Oil Aqueous Fractions for Syngas Production and Energy Journal Article
In: Environmental Engineering Science, vol. 28, no. 11, pp. 757–763, 2011, ISSN: 1092-8758.
@article{Bimbela2011,
title = {Steam Reforming of Bio-Oil Aqueous Fractions for Syngas Production and Energy},
author = {Fernando Bimbela and Miriam Oliva and Joaquín Ruiz and Lucía García and Jesús Arauzo},
url = {http://www.liebertpub.com/doi/10.1089/ees.2010.0367},
doi = {10.1089/ees.2010.0367},
issn = {1092-8758},
year = {2011},
date = {2011-11-01},
journal = {Environmental Engineering Science},
volume = {28},
number = {11},
pages = {757--763},
publisher = {Mary Ann Liebert, Inc. 140 Huguenot Street, 3rd Floor New Rochelle, NY 10801 USA},
abstract = {The biorefinery concept has been proposed as a route map to convert biomass into fuels and chemicals, maximizing economic and environmental benefits while minimizing pollution. A biorefinery strategy based on fast pyrolysis is proposed following a two-stage process, where biomass is first subjected to fast pyrolysis, optimized to collect up to 75% (per unit weight of biomass) of a liquid fraction called bio-oil. This bio-oil or its fractions can be upgraded in a second step to different chemicals, to a syngas and/or to energy. In particular, the catalytic steam reforming of the aqueous fraction of bio-oil obtained by fractionation with water is one of the most attractive possibilities for bio-oil upgrading, yielding a H2-rich syngas with low CO content. From the results obtained, it can be concluded that the best alternative for the catalytic steam reforming process is hydrogen production through further purification of the gas obtained. textcopyright 2011, Mary Ann Liebert, Inc.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
The biorefinery concept has been proposed as a route map to convert biomass into fuels and chemicals, maximizing economic and environmental benefits while minimizing pollution. A biorefinery strategy based on fast pyrolysis is proposed following a two-stage process, where biomass is first subjected to fast pyrolysis, optimized to collect up to 75% (per unit weight of biomass) of a liquid fraction called bio-oil. This bio-oil or its fractions can be upgraded in a second step to different chemicals, to a syngas and/or to energy. In particular, the catalytic steam reforming of the aqueous fraction of bio-oil obtained by fractionation with water is one of the most attractive possibilities for bio-oil upgrading, yielding a H2-rich syngas with low CO content. From the results obtained, it can be concluded that the best alternative for the catalytic steam reforming process is hydrogen production through further purification of the gas obtained. textcopyright 2011, Mary Ann Liebert, Inc.