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Artículos SCI



2023


Química de Superficies y Catálisis

Impact of topology framework of microporous solids on methanol carbonylation: An operando DRIFTS-MS study

Luque-Alvarez, LA; Serrano-Cruz, M; Gonzalez-Castano, M; Bobadilla, LF; Odriozola, JA
Microporous and mesoporous materials, 360 (2023) 112725

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Methanol carbonylation was evaluated over heterogeneous catalysts based on Cu-exchanged zeolitic materials with different topology: Cu@MOR, Cu@FER, and Cu@ZSM-5. Despite the similar Si/Al ratios, it is crucial to acknowledge that the acid strength is influenced by the framework topology, as supported by the NH3-TPD results. This, along with other characterization techniques allowed us to estimate the impact of pore size and pore distribution in these microporous materials on catalytic performance. The channel structure influenced catalytic parameters such as conversion and selectivity. The higher methanol conversion achieved on Cu@FER shows the importance of Bronsted acid sites and redox centres location regarding the topology of the material. Concerning the selectivity, the production of acetic acid was endorsed by the 12-MR (MOR) channels, methyl acetate's production by the 10-MR (FER) channels. Finally, the presence of 6-MR (ZSM-5) channels led to a complete selectivity towards DME production. The reaction mechanism was elucidated via operando DRIFTS-MS and results revealed a bifunctional mechanism in which methanol adsorbs and dehydrates on acidic Bronsted sites and CO is activated over Cu+ species.


Octubre, 2023 | DOI: 10.1016/j.micromeso.2023.112725

Química de Superficies y Catálisis

Water-assisted HDO of biomass model compounds enabled by Ru-based catalysts

Carrasco-Ruiz, S; Parrilla-Lahoz, S; Santos, JL; Penkova, A; Odriozola, JA; Reina, TR; Pastor-Pérez, L
Fuel Processing Technology, 249 (2023) 107860

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Biofuels upgrading gathering momentum in view of the gradual depletion of fossil fuels and the pursuit of renewable energy sources to mitigate global warming. Hydrodeoxygenation (HDO) is a key reaction in the upgrading of bio-oil to produce hydrocarbon fuels or high-value chemicals. Oxygen removal in bio-oil increases its calorific value, improve thermal and chemical stability, reduce corrosiveness, etc., making the upgraded biooil suitable as a fuel or blending fuel. However, the dependence on high-pressure hydrogen is a serious disadvantage, as it is an expensive resource whose use also poses safety concerns. In this scenario, we propose a pioneering route for model biomass compounds upgrading via H2-free HDO. Herein we have developed multifunctional catalysts based on Ru and ceria supported on carbon able conduct the hydrodeoxygenation reaction using water as hydrogen source. We found that cerium oxide improves ruthenium metallic dispersion and the overall redox properties of the multicomponent system leading to enhanced catalytic performance. Along with the successful catalytic formulation we identify 300 degrees C as an optimal temperature validating the H2-free HDO route for bio-compounds upgrading.


Octubre, 2023 | DOI: 10.1016/j.fuproc.2023.107860

Química de Superficies y Catálisis

Enroute to the Carbon-Neutrality Goals via the Targeted Development of Ammonia as a Potential Nitrogen-Based Energy Carrier

Nawaz, MA; Blay-Roger, R; Saif, M; Meng, FH; González-Arias, J; Miao, BJ; Bobadilla, LF; Ramírez-Reina, T; Odriozola, J.A.
ACS Catalysis, 13 (2023) 14415-14453

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The reliance of a future carbon-free horizon is strongly aligned with the long-term energy storage avenues which are completely derived from renewable energy resources. Ammonia with its high energy content and density can perform as a decent candidate for buffering the short-term storage options. However, the current NH3 production majorly feeding the current huge desire for ammonia is dominated by the conventional nonrenewable Haber–Bosch (H–B) process route, thus continuously damaging the target of carbon neutrality goals. High-purity hydrogen (H2) gas is an essential precursor for the H–B process; however, it is a significant energy consumer (about 2% of the global energy supply) and contributes over 420 million tons of CO2/annum. Therefore, the research on the renewable synthesis of nitrogen-based energy carriers (such as ammonia) from the direct electrochemical, photocatalytic, or plasma catalytic processes; its conversion; and utilization to the potential derivatives has been a hot topic in the past few decades. A prospective analysis of the highly appealing processes has been summarized in this study, which could facilitate the adaption of renewable alternatives as an effective approach for zero carbon emission, paving the excellent pathways along the road to the development of nitrogen-based energy technologies, especially the targeted development of ammonia. Further, this Review covers the current and future impacts of the H–B process, the development of aspiring ammonia synthesis routes (via electro, photo, bio, chemical loop, or plasma catalysis), and its conversion and utilization to the renewable derivatives in terms of fabrication of model catalysts, advanced characterization technology, and efficient device design.


Octubre, 2023 | DOI: 10.1021/acscatal.3c02410

Materiales de Diseño para la Energía y Medioambiente

Mechanical treatments on design powder ceramic materials: Insight into the textural and structural changes

Osuna, FJ; Fernández, M; Pavón, E; Sánchez, RMT; Alba, MD
Advanced Powder Technology, 34 (2023) 104189

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Mechanical treatment of porous ceramics, such as porous clay minerals, is a crucial step in ceramic processing. Among clay minerals, design swelling brittle micas have shown exceptional properties for further applications, although they exhibit low surface area and porosity. But, their mechanical activation could improve their textural properties and deserves to be investigated. Thus, the aim of this work was to evaluate the effects of gradual grinding in their surface and framework. At short grinding times, the surface area increases and mesoporous and microporous are generated. Long grinding time provokes particle agglomeration with the consequent change in their colloidal stability. At bulk level, framework defects are observed in both tetrahedral and octahedral sheets and increase with the total layer charge.


Octubre, 2023 | DOI: 10.1016/j.apt.2023.104189

Nanotecnología en Superficies y Plasma

Cobalt Stabilization through Mesopore Confinement on TiO2 Support for Fischer-Tropsch Reaction

Platero, F; Todorova, S; Aoudjera, L; Michelin, L; Lebeau, B; Blin, JL; Holgado, JP; Caballero, A; Colón, G
ACS Applied Energy Materials, 6 (2023) 9475-9486

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Cobalt supported on mesostructured TiO2 catalysts has been prepared by a wet-impregnation method. The Co/TiO2 catalytic system showed better catalytic performance after support calcination at 380 °C. Co nanoparticles appeared well distributed along the mesopore channels of TiO2. After reduction pretreatment and reaction, a drastic structural change leads to mesopore structure collapse and the dispersion of the Co nanoparticles on the external surface. Along this complex process, Co species first form discrete nanoparticles inside the pore and then diffuse out as the pore collapses. Through this confinement, a strong metal–support interaction effect is hindered, and highly stable metal active sites lead to better performance for Fischer–Tropsch synthesis reaction toward C5+ products.


Septiembre, 2023 | DOI: 10.1021/acsaem.3c01432

 

 

 

 

 

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