Recycling of construction and demolition waste generated by building infrastructure for the production of glassy materials

The use of waste materials generated by construction and demolition industry to yield valuable glassy materials, i.e. enamel for glazed ceramic tiles and cellular glasses is presented in this study. Both types of materials are produced by one-step treatment at moderate temperatures after simple waste chemical composition adjust. The enamels are manufactured directly from the initial waste powder by melting, while the expanded materials result from mixing of the vitreous material obtained after waste vitrification with an adequate foaming agent and posterior thermal treatment. Through the manuscript the feasibility of one step production of second generation profit materials is discussed in order to help achieving sustainable development and environmental protectio

CO oxidation at low temperature on Au/CePO4: Mechanistic aspects

This work reports the synthesis and characterization of a cerium phosphate supported gold catalyst as well as its catalytic activity for the oxidation of CO. A precipitation method in the presence of an organic modifier followed by a hydrothermal treatment was used for the support synthesis, resulting in high surface area nanometric particles. Gold/cerium phosphate catalyst with a 1% (w/w) nominal gold content was characterized using XRF, XRD, N2 adsorption-desorption measurements, TEM and DRIFTS-MS. The catalyst shows good catalytic activity at low temperature. The activity is related to the generation of oxygen vacancies in the support caused by the elimination of structural oxygen. In situ studies revealed that the reaction of the oxygen vacancies with gaseous oxygen resulted in the formation of peroxo species. These species are responsible for the activity detected at room temperature in both the catalyst and the support. Moreover, the presence of carbonate and hydrogen carbonate acting as reaction intermediates have been observed

Intensifying glycerol steam reforming on a monolith catalyst: a reaction kinetic model

In this work, a structured monolithic catalyst has been tested under a wide range of conditions (partial pressure, residence time, temperature and time-on-stream), with the aim of modeling its kinetic behavior and assessing its economic and upscaling potential. We have developed a sequential model to help us interpret both main trends and salient features. Unexpected behavior was found for certain parameter values, which led us to consider kinetic parasitic effects such as mass or heat transfer limitations. By independently invoking these effects, a conciliatory view of the results observed could not be reached. A combined explanation may prove successful, although overfitting could not be ruled out at this point. More importantly, however, the observed salient features of this stable and selective monolith catalyst may hold potential for process intensification of glycerol steam reforming, thus contributing to a more sustainable industry.Ministerio de Economía y Competitividad ENE2013-47880-C3-2-R, ENE2015-66975-C3-2-

CO oxidation: effect of Ce and Au addition on MnOx catalysts

The effect of cerium and/or gold addition to a manganese oxide which was greatly active in CO oxidation was studied. The catalysts obtained by this way were characterized by N2 adsorption, XRF, XRD and TPR, and their catalytic activity was measured in the CO oxidation reaction. The pure MnOx catalyst was active in the CO oxidation but the addition of 5 wt % cerium decreased their catalytic activity. Adding 2 wt % gold improved the activity of MnOx and Ce/MnOx and caused a slight decrease of the catalyst specific area and of the average oxidation state of manganese in catalysts, which was found between 3.3 and 3.6. The order of activity found on the basis of T50 for the four catalysts was: Au/MnOx > Au/Ce/MnOx > MnOx > Ce/MnOx, with T50 of 89, 95, 99 and 139 ºC, respectively. The solids Au/MnOx and Au/Ce/MnOx presented a T10 of 30 and 49 ºC, indicating that gold favored the conversion at room temperature. The effect of water vapor on the reaction was also analyzed, finding a decrease in the catalytic activity of all catalysts, due to the blocking of active sites in the catalyst surfaceUnión Europea AlBan UE E06D101739C

Au/CeO2 metallic monolith catalysts: Influence of the metallic substrate

Ceria-based gold catalysts were successfully deposited on ferritic stainless steel (Fecralloy) and aluminium monoliths. The prepared monolithic and reference powder catalysts were characterized by means of S BET, X-ray diffraction, glow discharge optical emission spectroscopy and scanning electron microscopy-energy dispersive X-ray analysis techniques and tested in the CO oxidation reaction. Characterization results put in evidence the diffusion of cations from the catalytic layer on the surface of the monoliths to the metallic oxide scale and inversely, from the oxide scale to the catalysts, thus altering the catalytic formulation and affecting the CO oxidation properties of the catalytic device. The extension and nature of the modifications produced depend on the nature of the catalysts and the metallic substrate, as well as the reaction conditions applied. These facts must be considered when gold catalysts are supported on metallic-structured devices.Ministerio de Economía y Competitividad ENE2012- 37431-C03-03Junta de Andalucía TEP-819

Hydrogen production by methanol steam reforming on NiSn/MgO-Al 2O3 catalysts: The role of MgO addition

The effect of the magnesia loading on the surface structure and catalytic properties of NiSn/MgO-Al2O3 catalysts for hydrogen production by methanol steam reforming has been investigated. The catalysts have been obtained by impregnation of γ-Al2O3 by the incipient wetness method, with variation of the MgO content. X-ray diffraction (XRD), BET surface area and H2-temperature programmed reduction (TPR) have been used to characterise the prepared catalysts. From this, it has been concluded that the incorporation of MgO results in the formation of MgAl 2O4 spinel, which modifies the acid-base properties of the catalysts. The formation of Ni-Sn alloys after the reductive pre-treatment has also been evidenced. The influence of the temperature of reaction and of the MgO loading on the hydrogen production by reforming of methanol has been established. Moreover, tests of catalytic stability have been carried out for more than 20 h. The carbonaceous deposits have been examined by temperature-programmed oxidation (TPO). The analysis of the catalysts after reaction has confirmed the low level of carbon formation on these catalysts. In no case, carbon nanotubes have been detected on the solids.Junta de Andalucía TEP106Ministerio de Ciencia e Innovación ENE2009-14522-C05-0

Gold Nanoparticles on Yttrium Modified Titania: Support Properties and Catalytic Activity

A series of titanium oxide catalysts modified with yttrium has been prepared by sol¿gel method and their structural properties have been studied. The incorporation of yttrium in the titania lattice favors the formation of oxygen vacancies while at low Y loadings the anatase structure is preserved. The catalytic activity of these solids for CO oxidation is found to be significantly dependent on their physical properties. In particular the amount of dopant controls the number of surface oxygen vacancies created as well as the gold particle size, which directly affects the catalytic activity. Also, a linear relationship between the catalytic activity and the band gap values, which depend on the Y loading, is observed. Density functional theory based calculations show that Y atoms are incorporated at the TiO2 surface at substitutional positions only, while the preferred oxygen vacancies arise by removing the bridge surface oxygen atoms. These O-vacancies are the preferential adsorption sites for Au atoms and nanoparticles, acting as nucleation centers that favor the dispersion of the catalyst active phase over the support surface. In agreement with experiment, Y doping is found to decrease the band gap of the support due to a destabilization of the valence band of the oxide.Ministerio de Ciencia e Innovación ENE2009-14522-C05-01, MAT2008-04918, CSD-00023Junta de Andalucía P08-FQM-0366

Carbon Supported Gold Nanoparticles for the Catalytic Reduction of 4-Nitrophenol

This work is a detailed study on how to optimize gold colloids preparation and their deposition to very different in nature carbon materials. The change of the continuous phase and its dielectric constant is used to assure the good dispersion of the hydrophilic/hydrophobic carbons and the successful transfer of the preformed small size colloids to their surface. The sintering behavior of the particles during the calcination step is also studied and the optimal conditions to reduce to a minimum the particle size increase during the protecting agent removal phase are found. The as prepared catalysts have been tested in a relevant reaction in the field of environmental catalysis such as the reduction of 4-nitrophenol leading to promising results. Overall, this work proposes an important methodology to follow when a carbonaceous material are selected as catalyst supports for green chemistry reactions.Ministerio de Ciencia, Innovación y Universidades ENE2017-82451-C3-3-RFEDE

Influence of the O2/CO ratio and the presence of H2O and CO2 in the feed-stream during the preferential oxidation of CO (PROX) over a CuOx/CeO2-coated microchannel reactor

The catalytic performance of a CuOx/CeO2 powder catalyst and that of a microchannel reactor or microreactor (MR) coated with the same solid was determined and compared. The catalytic activity measurements were carried out with varying O2/CO molar ratios in the feed-stream. In addition, the influence of the presence of CO2 and H2O in the reaction mixture was studied. Some discrepancies were observed between the performances of the powder catalyst and the MR depending on the O2/CO ratio. The MR presented a very good performance with a superior selectivity for CO conversion. This behaviour was due to a more efficient heat removal in the case of the MR that inhibited the H2 oxidation reaction and the r-WGS. The isothermicity of the microreactor during the process was demonstrated through the monitoring of the MR inlet and outlet temperatures. Concerning the presence of CO2 or H2O in the feed-stream, both compounds gave rise to a decrease of the CO conversion. The negative effect on the catalytic performance was more marked when both compounds were fed together, although the principal inhibitor effect was associated to the CO2. This seems to be related with the formation of stable carbonates at the catalyst surface.Ministerio de Ciencia e Innovación ENE2009-14522-C05-01Junta de Andalucía P09-TEP-545

Preferential oxidation of CO (CO-PROX) over CuOx/CeO2 coated microchannel reactor

The general aspects of the synthesis and characterization results of a CuOx/CeO2 catalyst were presented. In addition the principal steps for manufacturing a microchannel reactor and for the coating of the CuOx/CeO2 catalyst onto the microchannels walls, were also summarized. The catalytic activity of this microchannel reactor during the preferential oxidation of CO (CO-PROX) was evaluated employing a feed-stream that simulates a reformate off-gas after the WGS unit. Two activation atmospheres were studied (H2/N2 and O2/N 2). The reducing pretreatment improved the resistance to deactivation by formation of carbonaceous species over the catalyst surface at high temperatures. The presence of H2O and CO2 in the feed-stream was also analyzed indicating that the adsorption of CO2 inhibited the conversion of CO at lower temperatures because these compounds modified the active sites through the formation of carbonaceous species on the catalyst surface. Finally, the experimental results of the microreactor performance were compared with CFD simulations that were carried out using a kinetic for the CuOx/CeO2 powder catalyst. The experimental results were reasonably well described by the model, thus confirming its validity.Ministerio de Ciencia e Innovación ENE2009-14522-C05-01, ENE2009-14522-C05-03Junta de Andalucía P09-TEP-545