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PUBLICATIONS
2020
Raso, Raquel; García, Lucia; Ruiz, Joaquín; Oliva, Miriam; Arauzo, Jesús
Study of Ni/Al-Fe Catalyst Stability in the Aqueous Phase Hydrogenolysis of Glycerol Journal Article
In: Catalysts 2020, Vol. 10, Page 1482, vol. 10, no. 12, pp. 1482, 2020, ISSN: 2073-4344.
@article{Raso2020,
title = {Study of Ni/Al-Fe Catalyst Stability in the Aqueous Phase Hydrogenolysis of Glycerol},
author = {Raquel Raso and Lucia García and Joaquín Ruiz and Miriam Oliva and Jesús Arauzo},
url = {https://www.mdpi.com/2073-4344/10/12/1482/htm https://www.mdpi.com/2073-4344/10/12/1482},
doi = {10.3390/CATAL10121482},
issn = {2073-4344},
year = {2020},
date = {2020-12-01},
journal = {Catalysts 2020, Vol. 10, Page 1482},
volume = {10},
number = {12},
pages = {1482},
publisher = {Multidisciplinary Digital Publishing Institute},
abstract = {The present work studied the stability and reusability of Ni/Al-Fe catalyst in the aqueous phase hydrogenolysis of glycerol without external hydrogen addition. The catalyst based on 28 molar % of Ni with 3/1 molar ratio of Al/Fe was prepared through co-precipitation. This catalyst presented the best performance in our last study which compares several Ni/Al-Fe catalysts with different molar ratios of Al/Fe. To see the influence of the pressurized water on the physicochemical characteristics of Ni/Al-Fe catalyst, a test of up to 9 h has been carried out. Fresh and used catalysts were characterized by various techniques: X-ray Diffraction (XRD), N2-physisorption, field emission scanning electron microscopy (FESEM) and STEM. Glycerol conversion and carbon yield to gases and liquids did not vary significantly when compared at 3 h and 9 h. Furthermore, the morphology of the catalyst remains stable after continuous recycling under severe hydrothermal conditions. The nickel rich phase of the catalyst, which was determined by XRD and scanning transmission electron microscopy (STEM) techniques, showed a stable size after 9 h under reaction.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
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}
}
Remón, Javier; Arcelus-Arrillaga, P; García, Lucía; Arauzo, Jesús
Simultaneous production of gaseous and liquid biofuels from the synergetic co-valorisation of bio-oil and crude glycerol in supercritical water Journal Article
In: Applied Energy, vol. 228, pp. 2275–2287, 2018, ISSN: 03062619.
@article{Remon2018,
title = {Simultaneous production of gaseous and liquid biofuels from the synergetic co-valorisation of bio-oil and crude glycerol in supercritical water},
author = {Javier Remón and P Arcelus-Arrillaga and Lucía García and Jesús Arauzo},
doi = {10.1016/j.apenergy.2018.07.093},
issn = {03062619},
year = {2018},
date = {2018-10-01},
journal = {Applied Energy},
volume = {228},
pages = {2275--2287},
publisher = {Elsevier Ltd},
abstract = {This work addresses the co-valorisation in supercritical water of bio-oil obtained from the fast pyrolysis of wood and crude glycerol yielded as a by-product during biodiesel production. The experiments were conducted at 380 °C and 230 bar for 30 min with a Ni-Co/Al-Mg catalyst, analysing the effects on the process of the catalyst loading (0–0.25 g catalyst/g organics) and feed composition (each material alone and all possible binary mixtures). The yields to gas, upgraded bio-oil (liquid) and solid varied as follows: 4–87%, 0–46% and 0–18%, respectively. A synergistic interaction between crude glycerol and bio-oil took place during the upgrading process, which allowed the complete and simultaneous transformation of both materials into gas and liquid bio-fuels with a negligible solid formation. The compositions of the gas and the upgraded liquid can be easy tailored by adjusting the catalyst amount and the composition of the feed. The gas phase was made up of H2 (7–49 vol.%), CO2 (31–56 vol.), CO (0–7 vol.%) and CH4 (6–57 vol.%) and had a Lower Heating Value (LHV) ranging from 8 to 22 MJ/m3 STP. The upgraded bio-oil consisted of a mixture of carboxylic acids (0–73%), furans (0–7%), phenols (0–85%), ketones (0–22%) and cyclic compounds (0–53%). The proportions of C, H and O in the liquid shifted between 66–77 wt.%, 7–11 wt.% and 15–25 wt.%, respectively, while its Higher Heating Value (HHV) ranged from 29 to 34 MJ/kg. An optimum for the simultaneous production of gas and liquid bio-fuels was achieved with a solution having equal amounts of each material and employing a catalyst amount of 0.25 g catalyst/g organics. Under such conditions, 37% of the bio-oil was transformed into an upgraded liquid having a HHV (32 MJ/kg) two times higher than the original material (16 MJ/kg) with a negligible solid formation; the rest of the bio-oil and all the crude glycerol being converted into a rich CH4 (55 vol.%) biogas with a high LHV (21 MJ/m3 STP). This represents a step-change in future energy production and can help to establish the basis for a more efficient and sustainable biomass valorisation.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
2017
Remón, Javier; Jarauta-Córdoba, C; García, Lucía; Arauzo, Jesús
Effect of acid (CH3COOH, H2SO4 and H3PO4) and basic (KOH and NaOH) impurities on glycerol valorisation by aqueous phase reforming Journal Article
In: Applied Catalysis B: Environmental, vol. 219, pp. 362–371, 2017, ISSN: 09263373.
@article{Remon2017a,
title = {Effect of acid (CH3COOH, H2SO4 and H3PO4) and basic (KOH and NaOH) impurities on glycerol valorisation by aqueous phase reforming},
author = {Javier Remón and C Jarauta-Córdoba and Lucía García and Jesús Arauzo},
doi = {10.1016/j.apcatb.2017.07.068},
issn = {09263373},
year = {2017},
date = {2017-12-01},
journal = {Applied Catalysis B: Environmental},
volume = {219},
pages = {362--371},
publisher = {Elsevier B.V.},
abstract = {This work analyses and compares, under the same operating conditions (220 °C and 44 bar with a Ni-La/Al2O3 catalyst), the effects of some of the most common acid (CH3COOH, H2SO4, H3PO4) and basic (KOH and NaOH) biodiesel-derived impurities on the aqueous phase reforming (APR) of a 30 wt.% glycerol solution. The statistical analysis of the results revealed that the impurities did not greatly influence the initial reforming results. Conversely, they significantly influenced the catalyst deactivation, which resulted in different evolutions over time for the glycerol conversion, liquid production and the composition of the gas and liquid phases. Significant decreases over time in the glycerol conversion and liquid production were detected, the severity of the decay being as follows: H3PO4 (KOH = NaOH) > H2SO4 (KOH < NaOH) > CH3COOH (KOH < NaOH). The characterisation of the spent catalyst and the liquid phases revealed that poisoning/fouling, and catalyst active phase or support modification (leaching and crystalline phases alteration), were the major deactivation mechanisms. The proportions of metals (K or Na) deposited on the catalysts with the different acids was as follows: H3PO4 > H2SO4 > CH3COOH. In addition, S and P were also deposited on the catalyst, while boehmite and other new crystalline phases were detected in the spent catalyst after the APR reaction.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}
Bimbela, Fernando; Ábrego, Javier; Puerta, R; García, Lucía; Arauzo, Jesús
Catalytic steam reforming of the aqueous fraction of bio-oil using Ni-Ce/Mg-Al catalysts Journal Article
In: Applied Catalysis B: Environmental, vol. 209, pp. 346–357, 2017, ISSN: 09263373.
@article{Bimbela2017,
title = {Catalytic steam reforming of the aqueous fraction of bio-oil using Ni-Ce/Mg-Al catalysts},
author = {Fernando Bimbela and Javier Ábrego and R Puerta and Lucía García and Jesús Arauzo},
doi = {10.1016/j.apcatb.2017.03.009},
issn = {09263373},
year = {2017},
date = {2017-07-01},
journal = {Applied Catalysis B: Environmental},
volume = {209},
pages = {346--357},
publisher = {Elsevier B.V.},
abstract = {The performance of different Ni/Mg-Al catalysts modified with Ce was evaluated in the catalytic steam reforming of aqueous fractions of bio-oil from biomass pyrolysis. The effects of several preparation methods for incorporating Ce as a modifier (co-precipitation, impregnation and direct thermal decomposition of the salt precursors), the Ce content (0–5 wt.%) and the feed streams (three different aqueous fractions from bio-oil) on the catalyst performance were examined, and it was found that the stability and activity of the catalysts were significantly influenced by all these factors. In general, the addition of Ce to a reference Ni/Mg-Al catalyst improved the overall carbon conversion to gas and the yield to H2 as well as enhancing the catalyst stability in the steam reforming of aqueous fractions of bio-oils. The best preparation method was impregnation and the optimal Ce content was found to be 0.5 wt.%. Much higher initial carbon conversion to gas and initial H2 yields was obtained using bio-oils derived from pine than those derived from poplar. A very low coke formation, 103 mg C/(g of catalyst textperiodcentered g of organics in the aqueous fraction reacted), was achieved using the optimized catalyst, 0.5 wt.% Ce prepared by impregnation.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}