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Scientific Papers in SCI



2020


Química de Superficies y Catálisis

Evaluation of the Oxygen Mobility in CePO4-Supported Catalysts: Mechanistic Implications on the Water-Gas Shift Reaction

Navarro-Jaen, S; Bobadilla, LF; Romero-Sarria, F; Laguna, OH; Bion, N; Odriozola, JA
Journal of Physical Chemistry C, 124 (2020) 16391-16401

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The hexagonal and monoclinic phases of CePO4 have been demonstrated to be excellent catalytic supports for Pt-based water-gas shift (WGS) catalysts. Consequently, the elucidation of the WGS reaction mechanism in these materials constitutes a fundamental aspect in order to explain their catalytic behavior. Because the observed WGS reaction path is closely related to the absence or presence of oxygen vacancies in the support, the study of the oxygen mobility in these solids constitutes a key factor for the understanding of the structure of the materials and its influence on the reaction mechanism. In this study, the oxygen mobility in CePO4 supports and the corresponding Pt catalysts has been evaluated by means of isotopic exchange experiments using O-18(2) and (CO2)-O-18 as probe molecules. Results demonstrate that the evaluated solids present a low exchange activity when O-18(2) is used, indicating the absence of oxygen vacancies in these solids, thus suggesting a poor influence of the WGS redox mechanism. On the contrary, a high oxygen exchange activity is observed using (CO2)-O-18, demonstrating that the exchange in these materials takes place through the formation of carbonate-like intermediates, thus suggesting the associative mechanism of the WGS reaction as the preferred path in these solids. Operando diffuse reflectance infrared spectroscopy experiments under WGS reaction conditions confirm these results, proving that the WGS reaction in the studied materials takes place through a formate-mediated associative mechanism.


July, 2020 | DOI: 10.1021/acs.jpcc.0c03649

Química de Superficies y Catálisis

Metal catalysts supported on biochars: Part I synthesis and characterization

Santos, JL; Maki-Arvela, P; Monzon, A; Murzin, DY; Centeno, MA
Applied Catalysis B-Environmental, 268 (2020) 118423

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In the current study, synthesis and detailed characterization of cellulose biochars as a waste biomass model component and vine shoot biochars as a real waste biomass catalyst was performed. Although initially biochars exhibit poor textural properties, a simple activation process can make them much more suitable as a catalyst supports. A combination of physical (CO2) and chemical activation (ZnCl2) was evaluated. The characterization results indicated that the surface area and pore volume of the biochars have increased significantly by chemical activation treatment with ZnCl2. A series of metal catalysts (Pd, Au and Ru) supported on biochars was prepared and characterized. The prepared materials represent a set of noble metal catalysts supported on biochars with different textural and surface properties, which can be used to evaluate the catalytic role of the active phase and carbon support nature in catalytic reactions of interest, such as hydrodeoxygenation, described in the part II.


July, 2020 | DOI: 10.1016/j.apcatb.2019.118423

Química de Superficies y Catálisis

Hydrodeoxygenation of vanillin over noble metal catalyst supported on biochars: Part II: Catalytic behaviour

Santos, JL; Maki-Arvela, P; Warna, J; Monzon, A; Centeno, MA; Murzin, DY
Applied Catalysis B-Environmental, 268 (2020) 118425

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Vanillin hydrodeoxygenation was investigated using noble metal (Pd, Au, Ru) supported on active carbon prepared from waste derived biochars, which were produced via pyrolysis in CO2 atmosphere. Chemical activation with ZnCl2 and HNO3 was also used in the preparation of active carbon to enhance the specific surface area and demineralize material, respectively. Both fresh and spent catalysts were characterized with X-ray diffraction, DRIFTS, zeta potential measurement and HR-TEM. The highest selectivity to p-creosol, 92 % selectivity at complete vanillin conversion after 3 h was obtained in vanillin hydrodeoxygenation at 100 degrees C under 30 bar in hydrogen in water with Pd/C catalyst prepared via pyrolysis under CO2 from wine waste and using ZnCl2 as a chemical activation agent. Hydrodeoxygenation activity increased with increasing metal dispersion. A kinetic model including adsorption of vanillin described well the experimental data.


July, 2020 | DOI: 10.1016/j.apcatb.2019.118425

Materiales de Diseño para la Energía y Medioambiente

Performance trends in wall-flow diesel particulate filters: Comparative analysis of their filtration efficiency and pressure drop

Orihuela, MP; Chacartegui, R; Gomez-Martin, A; Ramirez-Rico, J; Villanueva, JAB
Journal of Cleaner Production, 60 (2020) 12063

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Soot and particulate emissions from the transport sector are a major concern worldwide, given their harmful effects on public health and the environment. On-road vehicles are the main contributing source to this kind of pollution. They are strictly regulated in many countries, with limitations on the number and concentration of released particles, and they must be equipped with particle abatement systems. Wall-flow particulate filters are the most popular and effective devices to reduce particulate emissions from diesel and gasoline vehicles. Diesel Particulate Filters (DPFs) have been a recurrent research topic since the last century. There are different research studies analysing different aspects of these systems, at different levels, using different methodologies and different approaches. Their results are not always comparable. This work analyses the latest advances and trends in this technology by comparing two relevant performance parameters: their filtration efficiency and pressure drop. The findings of this study suggest that, in order to be competitive, upcoming DPFs should have filtration efficiencies above 80%, and pressure drops below 10 kPa, for space velocities of 1.5.10(5) h(-1) or more at the clean state. They should reach similar to 100% efficiency after a short operation period, before the soot load reaches 0.2 g/L. Later, they should keep a low pressure drop for a longer time, with a reference of no more than 13 kPa for 6 g/L of soot load. Based on this analysis, this work proposes some test criteria and suggestions for the main parameters. 


July, 2020 | DOI: 10.1016/j.jclepro.2020.120863

Nanotecnología en Superficies y Plasma

Chemistry and Electrocatalytic Activity of Nanostructured Nickel Electrodes for Water Electrolysis

Lopez-Fernandez, E; Gil-Rostra, J; Espinos, JP; Gonzalez-Elipe, AR; Consuegra, AD; Yubero, F
ACS Catalysis, 10 (2020) 6159-6170

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Herein we have developed nanostructured nickel-based electrode films for anion exchange membrane water electrolysis (AEMWE). The electrodes were prepared by magnetron sputtering (MS) in an oblique angle configuration and under various conditions aimed at preparing metallic, oxide, or oxyhydroxide films. Their electrochemical analysis has been complemented with a thorough physicochemical characterization to determine the effect of microstructure, chemical state, bilayer structure, and film thickness on the oxygen evolution reaction (OER). The maximum electrocatalytic activity was found for the metallic electrode, where analysis by X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) demonstrated that the active catalytic phase at the surface after its electrochemical conditioning is a kind of oxidized nickel oxide/hydroxide layer with the thickness of a few nanometers. Electrochemical impedance spectroscopy analysis of these steady-state working electrodes supports that the enhanced performance of the metallic nickel anode vs other chemical states resides in the easier electron transfer through the electrode films and the various interlayers built up during their fabrication and activation. The long-term steady-state operation of the anodes and their efficiency for water splitting was proved in a full-cell AEMWE setup incorporating magnetron-sputtered metallic nickel as the cathode. This work proves that MS is a suitable technique to prepare active, stable, and low-cost electrodes for AEMWE and the capacity of this technique to control the chemical state of the electrocatalytically active layers involved in the OER.


June, 2020 | DOI: 10.1021/acscatal.0c00856

 

 

 

 

 

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