Scientific Papers in SCI
2024
2024
Química de Superficies y Catálisis
Optimizing biogas methanation over nickel supported on ceria-alumina catalyst: Towards CO2-rich biomass utilization for a negative emissions society
González-Arias, J; Torres-Sempere, G; Arroyo-Torralvo, F; Reina, TR; Odriozola, JAEnrironmental Research, 242 (2024) 117735
Biogas methanation emerges as a prominent technology for converting biogas into biomethane in a single step. Furthermore, this technology can be implemented at biogas plant locations, supporting local economies and reducing dependence on large energy producers. However, there is a lack of comprehensive studies on biogas methanation, particularly regarding the technical optimization of operational parameters and the profitability analysis of the overall process. To address this gap, our study represents a seminal work on the technical optimization of biogas methanation obtaining an empirical model to predict the performance of biogas methanation. We investigate the influence of operational parameters, such as reaction temperature, H2/CO2 ratio, space velocity, and CO2 share in the biogas stream through an experimental design. Based on previous research we selected a nickel supported on ceria-alumina catalyst; being nickel a benchmark system for methanation process such selection permits a reliable data extrapolation to commercial units. We showcase the remarkable impact of studied key operation parameters, being the temperature, the most critical factor affecting the reaction performance (ca. 2 to 5 times higher than the second most influencing parameter). The impact of the H2/CO2 ratio is also noticeable. The response surfaces and contour maps suggest that a temperature between 350 and 450 degrees C and an H2/CO2 ratio between 2.5 and 3.2 optimize the reaction performance. Further experimental tests were performed for model validation and optimization leading to a reliable predictive model. Overall, this study provides validated equations for technology scaling-up and techno-economic analysis, thus representing a step ahead towards real-world applications for bio-methane production.
February, 2024 | DOI: 10.1016/j.envres.2023.117735
Fotocatálisis Heterogénea: Aplicaciones
Insights into the physicochemical properties of Sugar Scum as a sustainable biosorbent derived from sugar refinery waste for efficient cationic dye removal
F. Atmani, M.M. Kaci, N. Yeddou-Mezenner, A. Soukeur, I. Akkari, J.A. NavíoBiomass Conversion and Biorefinery, 14 (2024) 4843-4857
The objective of this study was to determine the ability of sugar scum (SS), an industrial waste, as a novel biosorbent for the removal of Basic Blue 41 (BB 41) from aqueous solutions. The biosorbent was characterized by SEM/EDS, BET, FTIR, and pHpzc measurements, respectively. To reach a maximum adsorption capacity of 26.45 mg.g–1, impacting operational factors such as pH, biosorbent dose, contact duration, starting dye concentration, and temperature were adjusted, when the removal efficiency reached 84% during 60 min at pH 10, 1.5 g.L–1 of biosorbent and Co = 10 mg.L–1. The experimental data were modeled by various isotherm models, whereas the best fit was found for Freundlich with a high correlation coefficient (R2 = 0.991). Other kinetic models including pseudo-first, pseudo-second order, and intra-particle diffusion models were tested to fit the kinetic data. The biosorption of BB 41 onto SS was spontaneous (∆G° < 0) and exothermic (∆H° < 0), while the biosoprtion mechanism of BB41 over SS was proposed with repeated reuse showing that SS could be regenerated after four successive runs. Furthermore, this study revealed that sugar scum is an underutilized bioresource in Algeria, with the potential to provide low-cost environmental removal of additional contaminants in the wastewater treatment domain.
February, 2024 | DOI: 10.1007/s13399-022-02646-3
Tribología y Protección de Superficies
Synthesis and Characterization of Multilayered CrAlN/Al2O3 Tandem Coating Using HiPIMS for Solar Selective Applications at High Temperature
Sánchez-Pérez, M; Rojas, TR; Reyes, DF; Ferrer, FJ; Farchado, M; Morales, A; Escobar-Galindo, R; Sánchez-López, JCACS Applied Energy Materials, 7 (2024) 438-449
The effect of applying a negative bias during deposition of a previously designed multilayer solar selective absorber coating was studied on two types of substrates (316L stainless steel and Inconel 625). The solar selective coating is composed of different chromium aluminum nitride layers deposited using a combination of radiofrequency (RF), direct current (DC), and high-power impulse magnetron sputtering (HiPIMS) technologies. The chemical composition is varied to generate an infrared reflective/absorber layer (with low Al addition and N vacancies) and two CrAlN intermediate layers with medium and high aluminum content (Al/Cr = 0.6 and 1.2). A top aluminum oxide layer (Al2O3) is deposited as an antireflective layer. In this work, a simultaneous DC-pulsed bias (−100 V, 250 kHz) was applied to the substrates in order to increase the film density. The optical performance, thermal stability, and oxidation resistance was evaluated and compared with the performance obtained with similar unbiased coating and a commercial Pyromark paint reference at 600, 700, and 800 °C. The coating remained stable after 200 h of annealing at 600 °C, with solar absorptance (α) values of 93% and 92% for samples deposited on stainless steel and Inconel, respectively, and a thermal emittance ε25°C of 18%. The introduction of additional ion bombardment during film growth through bias assistance resulted in increased durability, thermal stability, and working temperature limits compared with unbiased coatings. The solar-to-mechanical energy conversion efficiency at 800 °C was found to be up to 2 times higher than Pyromark at C = 100 and comparable at C = 1000.
February, 2024 | DOI: 10.1021/acsaem.3c02310
Química de Superficies y Catálisis
Synthetic natural gas production using CO2-rich waste stream from hydrothermal carbonization of biomass: Effect of impurities on the catalytic activity
González-Arias, J; Torres-Sempere, G; Villora-Picó, JJ; Reina, TR; Odriozola, JAJournal of CO2 Utilization, 79 (2024) 102653
The utilization of biomass and bio-waste, particularly through hydrothermal processes, has shown promise as a technology for converting these materials into valuable products. While most research has traditionally focused on the solid and liquid byproducts of these hydrothermal treatments, the gaseous phase has often been over-looked. This study specifically investigates the conversion of off-gases produced during hydrothermal carbonation (HTC) into synthetic natural gas, offering a readily marketable product with economic potential. Although the methanation of conventional flue gases has been extensively studied, dealing with non-standard off-gases from processes like HTC presents challenges due to the presence of minor impurities like CO and CH4. This novel research seeks to experimentally evaluate the methanation of HTC off-gases using nickel-based catalysts and analyze how these impurities affect the catalytic performance. The studied catalysts include nickel supported by ceria and alumina, as well as alumina supported nickel-cobalt systems. The results demonstrate that these catalysts exhibit high CO2 conversion and CH4 selectivity under ideal gas conditions. However, when real gas compositions with impurities are considered, CO2 conversion decreases at lower temperatures (ca. 20% lower conversion for real gas vs. ideal), probably due to side reactions such as CH4 cracking. This difference becomes less pronounced at higher temperatures. Nevertheless, the catalysts perform satisfactorily, especially at temperatures exceeding 350 degrees C. In conclusion, this study sheds light on the methanation of HTC off-gases and underscores the significance of understanding how impurities in real gases impact the process, providing potential directions for future research.
January, 2024 | DOI: 10.1016/j.jcou.2023.102653
Química de Superficies y Catálisis
Boosting Low-Temperature CO2 Hydrogenation over Ni-based Catalysts by Tuning Strong Metal-Support Interactions
Ye, RP; Ma, LX; Hong, XL; Reina, TR; Luo, WH; Kang, LQ; Feng, G; Zhang, RB; Fan, MH, Zhang, RGAngewandte Chemie-International Edition, 63 (2024) e202317669
Rational design of low-cost and efficient transition-metal catalysts for low-temperature CO2 activation is significant and poses great challenges. Herein, a strategy via regulating the local electron density of active sites is developed to boost CO2 methanation that normally requires >350 °C for commercial Ni catalysts. An optimal Ni/ZrO2 catalyst affords an excellent low-temperature performance hitherto, with a CO2 conversion of 84.0 %, CH4 selectivity of 98.6 % even at 230 °C and GHSV of 12,000 mL g−1 h−1 for 106 h, reflecting one of the best CO2 methanation performance to date on Ni-based catalysts. Combined a series of in situ spectroscopic characterization studies reveal that re-constructing monoclinic-ZrO2 supported Ni species with abundant oxygen vacancies can facilitate CO2 activation, owing to the enhanced local electron density of Ni induced by the strong metal-support interactions. These findings might be of great aid for construction of robust catalysts with an enhanced performance for CO2 emission abatement and beyond.
January, 2024 | DOI: 10.1002/anie.202317669
Materiales y Procesos Catalíticos de Interés Ambiental y Energético
CuO-TiO2 pilot-plant system performance for solar photocatalytic hydrogen production
Villachica-Llamosas, JG; Ruiz-Aguirre, A; Colón, G; Peral, J; Malato, SInternational Journal of Hydrogen Energy, 51 (2024) 1069-1077
The main goal of the present study was to explore photocatalytic performance of the TiO2 -CuO mixture, for solar to hydrogen conversion at pilot plant scale under two different irradiation conditions (sunny and partly cloudy), focusing on high-temperature pretreat-ment of the catalyst mixture to try to improve TiO2 doping with copper. P25-TiO2 and commercial CuO were used with different amounts of Cu (2 wt% or 7 wt% Cu) calcined at 200-400 degrees C during several hours. Catalysts were tested at pilot plant scale using solar compound parabolic collectors, with glycerol as the sacrificial agent. The photocatalyst prepared after heating at 200 degrees C for 3 h and with 7 wt% Cu, resulted in higher hydrogen production than under the other heating conditions, and results were slightly better (5 -10%) than the reference values with the untreated catalysts. Photocatalytic efficiency was slightly lower at the higher calcination temperature (400 degrees C). CO2 production and formation of formate and glycolate clearly demonstrated glycerol photoreforming. The Cu from the calcined catalyst remaining on the solid was significantly less (2.5%) than on the non -calcined catalyst (4.2%), with an important fraction of lixiviated copper and copper deposition on the reactor walls. This is a critical drawback that must be considered for large-scale applications.
January, 2024 | DOI: 10.1016/j.ijhydene.2023.07.149
Química de Superficies y Catálisis
Switchable catalysis for methanol and synthetic natural gas synthesis from CO2: A techno-economic investigation
Merkouri, LP; Mathew, J; Jacob, J; Reina, TR; Duyar, MSJournal of CO2 Utilization, 79 (2024) 102652
The oil and gas sector produces a considerable volume of greenhouse gas emissions, mainly generated from flaring and venting natural gas. Herein, a techno-economic analysis has been performed of a switchable catalytic process to convert the CH4 and CO2 in flared/vented natural gas into syngas or methanol. Specifically, it was shown that depending on greenhouse gas composition, dry methane reforming (DRM), reverse water-gas shift (RWGS), and CO2 methanation could be chosen to valorise emissions in an overall profitable and flexible operation scenario. The switchable process produced methanol and synthetic natural gas as its products, resulting in an annual income of €687m and annual operating expenses of €452m. The pre-tax profit was calculated at €234m, and at the end of the project, the net present value was calculated as €1.9b with a profitability index of 4.7€/€. The expected payback time of this process was ca. 4 years, and with a 35% internal rate of return (IRR). Most importantly, this process consumed 42.8m tonnes of CO2 annually. The sensitivity analysis revealed that variations in operation time, green hydrogen price, and products' prices significantly impacted the profitability of the process. Overall, this techno-economic analysis demonstrated that switchable catalysis in greenhouse gas utilisation processes is profitable, and thus it could play an important role in achieving net zero emissions.
January, 2024 | DOI: 10.1016/j.jcou.2023.102652
Química de Superficies y Catálisis
A review on high-pressure heterogeneous catalytic processes for gas-phase CO2 valorization
Villora-Picó, J.J; González-Arias, J; Pastor-Pérez, L; Odriozola, JA; Reina, TREnvironmental Research, 240 (2024) 117520
This review discusses the importance of mitigating CO2 emissions by valorizing CO2 through high-pressure catalytic processes. It focuses on various key processes, including CO2 methanation, reverse water-gas shift, methane dry reforming, methanol, and dimethyl ether synthesis, emphasizing pros and cons of high-pressure operation. CO2 methanation, methanol synthesis, and dimethyl ether synthesis reactions are thermodynami-cally favored under high-pressure conditions. However, in the case of methane dry reforming and reverse water -gas shift, applying high pressure, results in decreased selectivity toward desired products and an increase in coke production, which can be detrimental to both the catalyst and the reaction system. Nevertheless, high-pressure utilization proves industrially advantageous for cost reduction when these processes are integrated with Fischer-Tropsch or methanol synthesis units. This review also compiles recent advances in heterogeneous catalysts design for high-pressure applications. By examining the impact of pressure on CO2 valorization and the state of the art, this work contributes to improving scientific understanding and optimizing these processes for sustainable CO2 management, as well as addressing challenges in high-pressure CO2 valorization that are crucial for industrial scaling-up. This includes the development of cost-effective and robust reactor materials and the development of low-cost catalysts that yield improved selectivity and long-term stability under realistic working environments.
January, 2024 | DOI: 10.1016/j.envres.2023.117520
Nanotecnología en Superficies y Plasma
Green hydrogen production using doped Fe2O3 foams
Damizia, M; Lloreda-Jurado, PJ; De Filippis, P; de Caprariis, B; Chicardi, E; Sepúlveda, RInternational Journal of Hydrogen Energy, 51 (2024) 834-845
Hydrogen is the ideal energy vector to reduce our fossil-fuels dependency and diminish the climate change consequence. However, current production is still methane based. It is possible to produce hydrogen using bioethanol from the alcoholic fermentation of organic waste by chemical looping processes, but unfortunately current redox systems generate hydrogen with significant traces of CO. In the case of proton exchange membrane fuel cells (PEMFC), hydrogen must be highly purified to produce electricity. Here, high porosity inter-connected Fe2O3 foams doped with 2 wt% Al2O3 were manufactured by the freeze-casting method, obtaining around 5.1 mmol H2$g?1 sample of highly pure hydrogen (<10 ppm of CO) consuming only 3.42 mmol of ethanol on each redox cycles, with no deactivation. This result shows the possibility of using an abundant and inexpensive raw material as the iron oxide to scale-up the direct pure H2 production and facilitates its use in the automotive sector.
January, 2024 | DOI: 10.1016/j.ijhydene.2023.09.008
Química de Superficies y Catálisis
Natural hydrogen in the energy transition: Fundamentals, promise, and enigmas
Blay-Roger, R; Bach, W; Bobadilla, LF; Reina, TR; Odriozola, JA; Amils, R; Blay, VRenewable & Sustainable Energy Reviews, 189 (2024) 113888
Beyond its role as an energy vector, a growing number of natural hydrogen sources and reservoirs are being discovered all over the globe, which could represent a clean energy source. Although the hydrogen amounts in reservoirs are uncertain, they could be vast, and they could help decarbonize energy-intensive economic sectors and facilitate the energy transition. Natural hydrogen is mainly produced through a geochemical process known as serpentinization, which involves the reaction of water with low-silica, ferrous minerals. In favorable locations, the hydrogen produced can become trapped by impermeable rocks on its way to the atmosphere, forming a reservoir. The safe exploitation of numerous natural hydrogen reservoirs seems feasible with current technology, and several demonstration plants are being commissioned. Natural hydrogen may show variable composition and require custom separation, purification, storage, and distribution facilities, depending on the location and intended use. By investing in research, in the mid-term, more hydrogen sources could become exploitable and geochemical processes could be artificially stimulated in new locations. In the long term, it may be possible to leverage or engineer the interplay between microorganisms and geological substrates to obtain hydrogen and other chemicals in a sustainable manner.
January, 2024 | DOI: 10.1016/j.rser.2023.113888
- ‹ previous
- 11 of 214
- next ›