Persona: Pérez Mayoral, María Elena
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Pérez Mayoral
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Publicación Developing strategies for the preparation of Co-carbon catalysts involved in the free solvent selective synthesis of aza-heterocycles(Elsevier, 2018-02) Godino Ojer, Marina; Pérez Cadenas, Agustín Francisco; Pérez Mayoral, María Elena; Martín Aranda, Rosa MaríaWe report herein different series of new zero valent Cobalt nanocarbons, as doped and supported aerogels, able to efficiently catalyze the reaction of 2-amino-5-chlorobenzaldehyde and -ketoesters, via Friedländer reaction. The reaction works under solvent-free and mild conditions affording yields over 80% in only 30 min of reaction time. The catalysts could be reused almost during two consecutive cycles without almost any activity loss. A comparative study between supported and doped-carbon aerogels, as catalysts highly efficient in the reaction, has allowed to stablish the relationship between the catalyst structure and the catalytic performance. At this regard, different parameters such as carbonization temperature and surface chemistry on the aerogels under study have been also explored. As a result, although the carbon matrix is involved in the reaction, the Co(0) nanoparticles on the carbon surface are the predominant active catalytic species. Oxygen functionalities on the oxidized samples in the surroundings of Co(0) nanoparticles probably prevent the access of the reagents, notably decreasing their catalytic performance.Publicación Metal-free synthesis of quinolines catalyzed by carbon aerogels: Influence of the porous texture and surface chemistry(Elsevier, 2017-04-17) Godino Ojer, Marina; Soriano, Eva; Calvino Casilda, Vanesa; Maldonado-Hódar, Francisco J.; Pérez Mayoral, María ElenaWe report herein an experimental and theoretical study of the Friedländer reaction, from 2-amino-5-chlorobenzaldehyde and ethyl acetoacetate, catalyzed by free-metal nanocatalysts based on carbon aerogels, to afford quinoline 3a. The developed methodology implies the combined use of carbon aerogels with solvent-free technologies under MW irradiation yielding the corresponding quinoline with moderated yield (66%) in only 5 min of reaction time. Our results demonstrated that the reactivity of the samples upon MW irradiation is strongly dependent on the porosity and surface chemistry of the carbon aerogels, the most active catalytic species being the most acidic oxygenated functional groups, –CO2H groups originated by oxidant treatment, or even in situ by hydrolysis of –CO–O–CO–, over the carbon surface. The theoretical investigation of the reaction mechanism, by using computational methods, demonstrated that the synthesis of quinoline 3a in the absence or in the presence of carbon aerogels takes place by aldolization, subsequent heterocyclization and finally double dehydration. Relatively strong π-π stacking interactions between carbon support and reagents could be behind of the observed catalytic performance also extended for the oxygenated models. Furthermore, the concentration of –CO2H groups over the carbon surface is a key factor favoring each step of the reaction but acting as individual catalytic sites.Publicación Tantalum vs Niobium MCF nanocatalysts in the green synthesis of chromene derivatives(Elsevier, 2019-03-15) Smuszkiewicz, Agata; López Sanz, Jesús; Sobczakb, Izabela; Ziolek, María; Martín Aranda, Rosa María; Pérez Mayoral, María ElenaTaMCF silicas modified with alkaline metals can be considered a novel family of highly efficient bifunctional catalysts involved in the synthesis of chromene derivatives, from salicylaldehyde 2 and acetonitrile compounds, under mild conditions, showing enhanced catalytic performance than their NbMCF analogues. The observed reactivity was mainly attributed to the higher basicity of the Me/TaMCF but also the texture of the samples. The Me/TaMCF silicas showed higher Brønsted basicity than the Nb ones as indicated by the stronger interaction between alkali metals and Ta in the UV–vis and the test reaction experiments. On the other hand, the basicity of Me/TaMCF together the reactivity degree and steric hindrance of the starting acetonitriles are key factors influencing the reaction selectivity. In conclusion, the basicity of the samples plays an important role initiating the reaction by activation of nucleophile but also a compromise between alkaline cation size and basicity is required.Publicación Cobalt oxide-Carbon nanocatalysts with highly enhanced catalytic performance for the green synthesis of nitrogen heterocycles through Friedländer condensation(Royal Society of Chemistry, 2019-03-19) Godino Ojer, Marina; López Peinado, Antonio José; Maldonado Hódar, Francisco J.; Bailón García, Esther; Pérez Mayoral, María ElenaA novel series of eco-sustainable catalysts developed by supporting CoO nanoparticles on different carbon supports, highly efficient in the synthesis of quinolines and naphthyridines, through the Friedländer condensation, are reported for the first time. Textural properties, dispersion and location of the Co-phase are influenced by the nature of the carbon support, Co-precursor salt and metal loading, having a significant impact on the catalytic performance. Thus, the presence of the mesopores and macropores in carbon aerogels together with the homogeneous distribution of the active phase favours the formation of product 3a as a function of the metal loading. However, an increase in the metal content when using CNTs indicates the formation of CoO aggregates and an optimal concentration of 3 wt% CoO was observed, providing the highest conversion values. The carbon-based catalysts herein reported can be considered to be a sustainable alternative having advantages such as easy preparation, superior stability and notably enhanced catalytic performance, operating at lower temperature and under solvent-free conditions.Publicación Eco-friendly catalytic systems based on MgO- Supporting carbon materials for the Friedländer condensation(Wiley, 2014-12) Godino Ojer, Marina; López Peinado, Antonio José; Przepiórski, J.; Pérez Mayoral, María Elena; Soriano, E.; Martín Aranda, Rosa MaríaCarbon-supported MgO materials are excellent and sustainable catalysts for the synthesis of N-containing heterocyclic compounds by the Friedländer condensation under mild, solvent-free conditions. The results reported herein indicate that MgO is the most active catalytic species that accelerates the reaction compared with the catalytic behavior observed for the carbon material Norit RX3. On the basis of DFT calculations, a reaction mechanism that involves dual activation of the reacting structures by the catalyst is proposed. Oxide, outside: MgO supported on carbon is able to catalyze the synthesis of interesting N-containing heterocyclic compounds efficiently under mild conditions. MgO on the carbon surface is responsible for the catalytic behavior. These carbon materials are environmentally friendly catalysts for the Friedländer reaction.