23 research outputs found

    Light-Promoted Hydrogenation of Carbon DioxideÂżAn Overview

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    [EN] Hydrogenation of carbon dioxide is considered as a viable strategy to generate fuels while closing the carbon cycle (heavily disrupted by the abuse in the exploitation of fossil resources) and reducing greenhouse gas emissions. The process can be performed by heat-powered catalytic processes, albeit conversion and selectivity tend to be reduced at increasing temperatures owing to thermodynamic constraints. Recent investigations, as summarised in this overview, have proven that light activation is a distinct possibility for the promotion of CO2 hydrogenation to fuels. This effect is particularly beneficial in methanation processes, which can be enhanced under simulated solar irradiation using materials based on metallic nanoparticles as catalysts. The use of nickel, ruthenium and rhodium has led to substantial efficiencies. Light-promoted processes entail performances on a par with (or even superior to) those of thermally-induced, industrially-relevant, commercial technologies.The author thanks the Spanish Government (Ministerio de Economía y Competitividad, MINECO) for financial support via a project for young researchers (CTQ2015-74138-JIN), and the ‘‘Severo Ochoa’’ programme (SEV 2012-0267). The European Union is also acknowledged for the SynCatMatch project (ERCAdG-2014-671093)Puga Vaca, A. (2016). Light-Promoted Hydrogenation of Carbon Dioxide¿An Overview. Topics in Catalysis. 59(15-16):1268-1278. https://doi.org/10.1007/s11244-016-0658-zS126812785915-16Centi G, Perathoner S (2009) Opportunities and prospects in the chemical recycling of carbon dioxide to fuels. Catal Today 148:191–205Aresta M, Dibenedetto A, Angelini A (2014) Catalysis for the valorization of exhaust carbon: from CO2 to chemicals, materials, and fuels. technological use of CO2. 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    Dealloying of Cobalt from CuCo Nanoparticles under Syngas Exposure

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    International audienceThe structure and composition of core−shell CuCo nanoparticles were found to change as a result of cleaning pretreatments and when exposed to syngas (CO + H 2) at atmospheric pressure. In situ X-ray absorption and photoelectron spectroscopies revealed the oxidation state of the particles as well as the presence of adsorbates under syngas. Transmission electron microscopy was used for ex situ analysis of the shape, elemental composition, and structure after reaction. The original core−shell structure was found to change to a hollow CuCo alloy after pretreatment by oxidation in pure O 2 and reduction in pure H 2. After 30 min of exposure to syngas, a significant fraction (5%) of the particles was strongly depleted in cobalt giving copper-rich nanoparticles. This fraction increased with duration of syngas exposure, a phenomenon that did not occur under pure CO or pure H 2. This study suggests that Co and Cu can each individually contribute to syngas conversion with CuCo catalysts

    Position-space representation of charged particles’ propagators in a constant magnetic field as an expansion over Landau levels

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    We have obtained propagators in the position space as an expansion over Landau levels for the charged scalar particle, fermion, and massive vector boson in a constant external magnetic field. The summation terms in the resulting expressions consisted of two factors, one being rotationally invariant in the 2-dimensional Euclidean space perpendicular to the direction of the field, and the other being Lorentz-invariant in the 1+1-dimensional space-time. The obtained representations are unique in the sense that they allow for the simultaneous study of the propagator from both space-time and energetic perspectives which are implicitly connected. These results contribute to the development of position-space techniques in QFT and are expected to be of use in the calculations of loop diagrams

    Nanostructured MnOxMnO_{x} as highly active catalyst for CO oxidation

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    Non-stoichiometric Mn-oxides (MnO x and MnO y) were prepared by temperature-programmed oxidation (TPO) of Mn-oxalates, MnC 2O 4·3H 2O and MnC 2O 4·2H 2O. Both oxides provide high specific surface areas (525 m 2 g -1 and 385 m 2 g -1, respectively) and identical CO oxidation reaction rates of 10 -2 molecules nm -2 s -1 (0.017 μmol CO m -2 s -1) at 298 K. A "spinodal" transformation of oxalates into oxides was observed by transmission electron microscopy (TEM). The quantitative evaluation of TPO and temperature-programmed reduction with CO allowed x-values of 1.61, ⋯, 1.67 to be determined for MnO x. The Mn oxidation state in MnO x was found to be 3.4 ± 0.1 by X-ray absorption near-edge structure analysis and X-ray photoelectron spectroscopy. In accordance with the high specific surface area and mixed-type I/IV adsorption isotherms of MnO x, high resolution TEM demonstrated the occurrence of nested micro-rod features along with nanocrystalline particles in the endings of the rods. After CO oxidation MnO and Mn 3O 4 phases were able to be identified in the regions between rods. © 2011 Elsevier Inc. All rights reserved.SCOPUS: ar.jinfo:eu-repo/semantics/publishe

    CO Oxidation Activity of Ag/TiO2 Catalysts Prepared via Oxalate Co-precipitation

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    Ag/TiO2 catalysts with different Ag loadings (2, 4, 7 and 10% (w/w)) have been prepared by means of co-precipitation of Ag- and TiO-oxalates followed by temperature programmed oxidation (TPO). The catalysts were subjected to CO oxidation in a flow reactor at atmospheric pressure and temperatures up to 573 K. Best conversion performance was obtained in a CO/O2 = 1:1 mixture over 10% Ag/TiO2 for which the temperature of 50% CO conversion was T50 = 333 K. The initial reaction rates were determined in a circulation reactor at low conversions and apparent activation energies between 13 and 25 kJ/mol were found for all catalysts. Transmission electron microscopy shows a broad range of nano-sized Ag particles on TiO2 (nearly pure anatase).info:eu-repo/semantics/publishe

    Evidence of Highly Active Cobalt Oxide Catalyst for the Fischer−Tropsch Synthesis and CO2 Hydrogenation

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    Hydrogenations of CO or CO2 are important catalytic reactions as they are interesting alternatives to produce fine chemical feedstock hence avoiding the use of fossil sources. Using monodisperse nanoparticle (NP) catalysts, we have studied the CO/H2 (i.e., Fischer-Tropsch synthesis) and CO2/H2 reactions. Exploiting synchrotron based in situ characterization techniques such as XANES and XPS, we were able to demonstrate that 10 nm Co NPs cannot be reduced at 250 C while supported on TiO2 or SiO2 and that the complete reduction of cobalt can only be achieved at 450 C. Interestingly, cobalt oxide performs better than fully reduced cobalt when supported on TiO2. In fact, the catalytic results indicate an enhancement of 10-fold for the CO2/H2 reaction rate and 2-fold for the CO/H2 reaction rate for the Co/TiO2 treated at 250 C in H2 versus Co/TiO2 treated at 450 C. Inversely, the activity of cobalt supported on SiO2 has a higher turnover frequency when cobalt is metallic. The product distributions could be tuned depending on the support and the oxidation state of cobalt. For oxidized cobalt on TiO2, we observed an increase of methane production for the CO2/H2 reaction whereas it is more selective to unsaturated products for the CO/H2 reaction. In situ investigation of the catalysts indicated wetting of the TiO2 support by CoOx and partial encapsulation of metallic Co by TiO 2-x. © 2014 American Chemical Society.close262
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