The catalytic performance of mesoporous cerium oxides prepared through a nanocasting route for the total oxidation of naphthalene

Cerium oxides have been prepared by nanocasting of a mesoporous siliceous KIT-6. Through this synthesis method a partially ordered mesoporous structure, as demonstrated by several characterization techniques (N2 adsorption, XRD and HRTEM) has been obtained. Accordingly, very high surface areas have been achieved (up to 163 m2/g), despite using high calcination temperatures (550 °C). We have demonstrated that the aging temperature of the siliceous template is of outstanding importance, as this parameter is directly responsible for both the pore size and the surface area of the catalysts. In addition, whilst a low preparation temperature (40 °C) makes the further removal of the silica templat…

Total oxidation of VOCs on mesoporous iron oxide catalysts: Soft chemistry route versus hard template method

9 figures, 3 tables.-- Supplemantary information available

Promoting Deoxygenation of Bio-Oil by Metal-Loaded Hierarchical ZSM-5 Zeolites

3 Figuras.- 5 tablas.-1 Esquema.- This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Sustainable Chemistry & Engineering, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acssuschemeng.5b01606 ”

Insights into the catalytic production of hydrogen from propane in the presence of oxygen: Cooperative presence of vanadium and gold catalysts

7 figures.-- © 2015. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

The key role of nanocasting in gold-based Fe2 O3 nanocasted catalysts for oxygen activation at the metal-support interface

5 Tablas.- 10 Figuras.- This is the peer reviewed version of the following article: The key role of nanocasting in gold‐based Fe2O3 nanocasted catalysts for oxygen activation at the metal‐support interface, ChemCatChem 11: 1915-1927 (2019), which has been published in final form at http://dx.doi.org/10.1002/cctc.201900210. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions.

Size-activity relationship of iridium particles supported on silica for the total oxidation of volatile organic compounds (VOCs)

12 Figures, 2 Tables.-- Datos suplementarios disponibles en línea en la página web del editor.-- © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

Low temperature conversion of levulinic acid into γ-valerolactone using Zn to generate hydrogen from water and nickel catalysts supported on sepiolite

1 scheme, 2 tables, 7 figures.-- Supplementary material available.

Deep oxidation of volatile organic compounds using ordered cobalt oxides prepared by a nanocasting route

Ordered Co3O4 with high surface area (until 173 m2/g) has been successfully obtained through a nanocasting route using mesoporous KIT-6 silica as a hard template and tested in the deep oxidation of a series of representative volatile organic compounds (VOCs): propane as a model of short chain alkane and toluene as a model of monoaromatic hydrocarbon. It has been demonstrated that the catalytic activity for VOC deep oxidation is very elevated and its catalytic stability at moderate temperatures very good. However, the role of the ordered structure in the catalytic performance does not seem to be beneficial. The enhanced catalytic activity has been explained in terms of both the high surface …

Promoting the activity and selectivity of high surface area Ni–Ce–O mixed oxides by gold deposition for VOC catalytic combustion

Gold supported on nickel cerium oxide catalysts (Ni–Ce–O) have been studied for the total oxidation of propane, as a model for hydrocarbon volatile organic compound emission control. High surface area Ni–Ce–O catalysts were synthesized using a very simple evaporation method, where cerium and nickel salts were evaporated in the presence of a mixture of methanol and oxalic acid. Gold catalysts were prepared following a deposition–precipitation method. A very efficient catalyst for the oxidation of propane, in terms of both activity and selectivity, was obtained. This high activity has been related to the high surface area of the catalyst (and therefore to the presence of more active sites ava…

The effect of gold addition on the catalytic performance of copper manganese oxide catalysts for the total oxidation of propane

Mixed copper manganese oxide catalysts (Hopcalite) have been studied for the total oxidation of propane, as a model for hydrocarbon volatile organic compound emission control. Catalysts were prepared using coprecipitation with and without gold. Calcination temperature influenced the catalyst activity and those prepared at 300 °C were the most active. Characterization showed that the catalysts had a nanowire-type morphology, and for those containing gold it was present as metallic particles occluded within the nanowires. The incorporation of gold into the catalyst enhanced the activity for propane conversion, but the presence of gold did not noticeably enhance the light-off activity. Althou…

Oxygen defects: The key parameter controlling the activity and selectivity of mesoporous copper-doped ceria for the total oxidation of naphthalene

Mesoporous CeO2 modified by the addition of copper has shown high efficiency for the total oxidation of naphthalene. High activity and 100% selectivity to carbon dioxide throughout the whole range of temperatures studied were achieved for copper loadings of 3.6% and lower. The catalytic behaviour has been related to the concentration of surface oxygen defects. A clear correlation between the concentration of surface oxygen defects (determined by XPS and DRIFTS) and the catalytic performance has been identified. Catalytic activity increased as copper was incorporated into the ceria up to 3.6%. In this range of copper content the copper was incorporated into the cubic fluorite lattice of CeO2…

Au deposited on CeO2 prepared by a nanocasting route: A high activity catalyst for CO oxidation

Abstract A set of catalysts comprised of gold on different CeO 2 supports has been prepared by a nanocasting route and characterized by several physicochemical techniques. These catalysts have been tested for CO oxidation and show outstanding catalytic activity. Higher calcination temperatures of the hard template, producing a poorly ordered silica template, have led to a higher amount of oxygen vacancies on the surface of CeO 2 . The presence of surface oxygen defects in the support combined with the deposition of Au nanoparticles ( ca. 3 nm) homogeneously dispersed on the CeO 2 support may explain the excellent behaviour for low temperature CO oxidation. Surprisingly, it has been observed…

The influence of cerium to urea preparation ratio of nanocrystalline ceria catalysts for the total oxidation of naphthalene

The influence of cerium salt/urea ratio on the activity of nanocrystalline ceria catalysts prepared by homogeneous precipitation with urea for the complete oxidation of naphthalene has been evaluated. Ceria catalysts were prepared from five different cerium salt/urea ratios (2:1, 1:1, 1:2, 1:3 and 1:4). Catalyst characterization (by BET, XRD and TPR) only revealed subtle differences in the characteristics of these catalysts with cerium salt to urea ratio. However, Raman and scanning electron microscopy (SEM) results indicated differences in the oxygen defect concentration (FWHM of Raman band) and morphology of the catalysts with variation of the preparation ratio. Catalysts prepared with 2:…

Understanding the role of Ti-rich domains in the stabilization of gold nanoparticles on mesoporous silica-based catalysts

3 Tablae, 14 Figures.-- Supplementary material.-- © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

Highly dispersed encapsulated AuPd nanoparticles on ordered mesoporous carbons for the direct synthesis of H2O2 from molecular oxygen and hydrogen

AuPd nanoparticles (<3 nm) have been encapsulated on the pores of a nanostructured CMK-3 carbon prepared by a nanocasting procedure. This material has been shown to be an excellent catalyst for the direct synthesis of hydrogen peroxide from molecular hydrogen and oxygen.

Total oxidation of naphthalene using bulk manganese oxide catalysts

Several Mn2O3 catalysts have been synthesized using different preparation methods and tested for the total oxidation of naphthalene, a model polycyclic aromatic compound. The catalysts have been characterized by several physico-chemical techniques such as XRD, TPR, XPS, EDX and TEM. The surface area of the catalyst seems to be of paramount importance, since the mass normalized activity of catalysts increases as the surface area of the Mn2O3 catalysts increases. Consequently, a high surface area ordered mesoporous Mn2O3 catalyst, obtained through a nanocasting route using mesoporous KIT-6 silica as a hard template, was the most efficient catalyst for the deep oxidation of naphthalene. In add…

High activity mesoporous copper doped cerium oxide catalysts for the total oxidation of polyaromatic hydrocarbon pollutants

The doping of mesoporous ceria with copper significantly enhances activity for naphthalene total oxidation, the enhanced performance is controlled by the increased concentration of surface oxygen defects.

Supported iridium catalysts for the total oxidation of short chain alkanes and their mixtures: Influence of the support

13 figures, 3 tables.-- Supplementary information available.-- © 2020. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

The prevalence of surface oxygen vacancies over the mobility of bulk oxygen in nanostructured ceria for the total toluene oxidation

12 figures, 2 tables

Gamma-valerolactone from levulinic acid and its esters: Substrate and reaction media determine the optimal catalyst

13 figures, 7 tables.-- © 2021. This manuscript version is made available under the CC-BY-NC-ND 4.0 license https://creativecommons.org/licenses/by-nc-nd/4.0

Deep oxidation of pollutants using gold deposited on a high surface area cobalt oxide prepared by a nanocasting route.

Gold deposited on a cobalt oxide with high surface area (138 m2 g−1), obtained through a nanocasting route using a siliceous KIT-6 mesoporous material as a hard template, has demonstrated high activity for the total oxidation of propane and toluene, and ambient temperature CO oxidation. The addition of gold promotes the activity when compared to a gold-free Co3O4 catalyst prepared using the same nanocasting technique. The enhanced catalytic activity when gold is present has been explained for the deep oxidation of propane and toluene in terms of the improved reducibility of cobalt oxide when gold is added, rather than to the intrinsic activity of metallic gold particles. The improved behavi…

The promoter effect of Nb species on the catalytic performance of Ir-based catalysts for VOCs total oxidation

12 figures, 2 tables.-- Supporting information available.

TAP reactor study of the deep oxidation of propane using cobalt oxide and gold-containing cobalt oxide catalysts

Abstract A transient reactor study of the oxidation of propane to CO 2 on gold-free and gold-doped CoO x catalysts has been carried out. It has been demonstrated that the presence of gold markedly promotes the catalytic reactivity of cobalt oxide in the total oxidation of propane. Both catalysts oxidised propane directly to CO 2 via a Mars–Van Krevelen mechanism, and this was confirmed using isotopically labelled oxygen experiments. The increased activity of the gold catalyst is related to the faster reoxidation of the cobalt oxide when gold is present in the catalyst, since the reaction step in which the catalyst is reduced, due to propane oxidation, is similar for both catalysts. The fast…

Eco-friendly cavity-containing iron oxides prepared by mild routes as very efficient catalysts for the total oxidation of VOCs

Iron oxides (FeOx) are non-toxic, non-expensive and environmentally friendly compounds, which makes them good candidates for many industrial applications, among them catalysis. In the present article five catalysts based on FeOx were synthesized by mild routes: hydrothermal in subcritical and supercritical conditions (Fe-HT, Few200, Few450) and solvothermal (Fe-ST1 and Fe-ST2). The catalytic activity of these catalysts was studied for the total oxidation of toluene using very demanding conditions with high space velocities and including water and CO2 in the feed. The samples were characterized by X-ray diffraction (XRD), scanning and high-resolution transmission electron microscopy (SEM and…

Total oxidation of propane using nanocrystalline cobalt oxide and supported cobalt oxide catalysts

Abstract Supported and unsupported nanocrystalline cobalt oxides have been shown to be extremely efficient catalysts for the total oxidation of propane. Total conversion with a high stability has been achieved at reaction temperatures as low as 250 °C. In the present work, a comparison between the catalytic performance of bulk and alumina-supported nanocrystalline cobalt oxide catalysts has been made. The influence of crystallite size, nature of the support (alpha, gamma and mesoporous alumina) and cobalt loading, has been probed. Unsupported cobalt oxide catalysts were more active than any supported cobalt oxide catalysts. The catalytic activity was mainly dependent on the crystallite size…

Easy Method for the Transformation of Levulinic Acid into Gamma-Valerolactone Using a Nickel Catalyst Derived from Nanocasted Nickel Oxide

Different nickel catalysts have been tested for the transformation of levulinic acid into &gamma

The significance of the order of impregnation on the activity of vanadia promoted palladium-alumina catalysts for propane total oxidation

The increased activity of alumina-supported palladium catalysts promoted with vanadium oxide has been investigated. Three different vanadium promoted Pd/Al2O3 catalysts with the same composition but synthesized employing sequential and co-impregnation were tested for the total oxidation of propane. The order of impregnation was critical to produce high activity catalysts. Vanadium and palladium co-impregnation on the Al2O3 support led to the most active catalyst, whereas the step-wise impregnated catalysts show a catalytic performance similar to or slightly better than unpromoted palladium catalysts. The high activity of the co-impregnated catalysts is related to the particle size and oxida…

Stable anchoring of dispersed gold nanoparticles on hierarchic porous silica-based materials

The nanometric organization of MOx (M = Co, Zn, Ni) domains partially embedded inside the mesoporous silica walls but accessible to the pore voids, which is achieved through a simple one-pot surfactant-assisted procedure, define optimal anchors for the nucleation and growth of gold nanoparticles, which in turn favours an exceptional thermal stability for the final Au-supported materials. As silica support we have selected a UVM-7 silica having a highly accessible architecture defined by two hierarchic pore systems. The combination of nanometric pore length, tortuous mesopores and MOx inorganic anchors favours the stability of the final Au/CoOx-UVM-7 nanocomposites.

Shape-dependency activity of nanostructured CeO2 in the total oxidation of polycyclic aromatic hydrocarbons

11 figures, 2 tables.-- © 2012. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

High-Temperature Stable Gold Nanoparticle Catalysts for Application under Severe Conditions: The Role of TiO2 Nanodomains in Structure and Activity

Metal nanoparticles with precisely controlled size are highly attractive for heterogeneous catalysis. However, their poor thermal stability remains a major concern in their application at realistic operating conditions. This paper demonstrates the possibility of synthesizing gold nanoparticles with exceptional thermal stability. This has been achieved by using a simple conventional deposition–precipitation technique. The material employed as catalyst consists of gold supported on a TiO2-impregnated SiO2 bimodal mesoporous support. The resulting material shows gold nanoparticles with a narrow size distribution around 3.0 nm, homogeneously dispersed over the TiO2/SiO2 material. Most interesti…

Glycerol selective oxidation to lactic acid over AuPt nanoparticles; Enhancing reaction selectivity and understanding by support modification

2 Schemes, 3 Tables, 5 Figures.

Highly Active Co3O4-Based Catalysts for Total Oxidation of Light C1&ndash;C3 Alkanes Prepared by a Simple Soft Chemistry Method: Effect of the Heat-Treatment Temperature and Mixture of Alkanes

9 figures, 2 tables.

Green synthesis of cavity-containing manganese oxides with superior catalytic performance in toluene oxidation

10 Figuras.- 2 Tablas.- Datos suplementarios disponibles en línea en la página web del editor.-- © 2019. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

Synergy between tungsten and palladium supported on titania for the catalytic total oxidation of propane

Titania-supported palladium catalysts modified by tungsten have been tested for the total oxidation of propane. The addition of tungsten significantly enhanced the catalytic activity. Highly active catalysts were prepared containing a low loading of 0.5 wt.% palladium, and activity increased as the tungsten loading was increased up to 6 wt.%. Catalysts were characterised using a variety of techniques, including powder X-ray diffraction, laser Raman spectroscopy, X-ray photoelectron spectroscopy, temperature-programmed reduction and aberration-corrected scanning transmission electron microscopy. Highly dispersed palladium nanoparticles were present on the catalyst with and without the additi…

The different catalytic behaviour in the propane total oxidation of cobalt and manganese oxides prepared by a wet combustion procedure

Abstract Cobalt oxide and manganese oxide catalysts have been prepared through aqueous synthesis using a wet combustion procedure. These materials have been tested as catalysts for the total oxidation of propane. It has been observed a different catalytic behaviour between cobalt and manganese oxides although for both oxides a very high catalytic activity has been obtained. Cobalt oxides prepared by the wet combustion procedure are less reactive than a simple cobalt oxide prepared without the addition of organic acids. However, in the case of manganese oxide the use of organic acids highly increases the catalytic activity. The different catalytic behaviour has been related to the variation …

Low temperature total oxidation of toluene by bimetallic Au–Ir catalysts

9 Figuras.- 3 Tablas.- Información suplementaria disponible en la página web del editor

Performance of an automated human immunodeficiency virus (HIV) antigen/antibody combined assay for prenatal screening for HIV infection in pregnant women

Influence of the preparation method on the activity of ceria zirconia mixed oxides for naphthalene total oxidation

Cerium/zirconium mixed oxides, with different Ce/Zr ratios, have been synthesised by a co-precipitation method using two different precipitating agents (sodium carbonate and urea) and tested for the total oxidation of naphthalene. Catalysts were characterized by N2 adsorption, XRD, Raman, TPR, XPS and DRIFTS. Ceria prepared by carbonate precipitation had low activity and this is likely to be related to the high concentration of residual surface carbonate that covers catalytic sites and inhibits reaction. For carbonate precipitation, increasing the Zr content to 1% resulted in a significant increase of activity, which is related to the decrease of surface carbonate. Increasing the Zr content…

Total oxidation of naphthalene with high selectivity using a ceria catalyst prepared by a combustion method employing ethylene glycol.

Abstract During the catalytic combustion of naphthalene, compounds other than CO 2 are often obtained. These products, as polymerized polycyclic aromatic hydrocarbons, oxygenated aromatic compounds and benzene derivate compounds, are usually more toxic than naphthalene. At the present work it is shown a nanocrystalline cerium oxide prepared by a combustion method employing a proper ethylene glycol concentration that exhibits very high activity in the decomposition of naphthalene in the presence of air and, most importantly, a selectivity value towards CO 2 of 100% for any range of conversions and/or temperatures used. In addition, it has been demonstrated that the amount of ethylene glycol …

Enhanced H2O2 production over Au-rich bimetallic Au-Pd nanoparticles on ordered mesoporous carbons

1 figures, 3 tables.-- © 2014. This manuscript version is made available under the CC-BY-NC-ND 4.0 license http://creativecommons.org/licenses/by-nc-nd/4.0/

Influence of preparation conditions of nano-crystalline ceria catalysts on the total oxidation of naphthalene, a model polycyclic aromatic hydrocarbon

Abstract Nano-crystalline ceria catalysts prepared by homogeneous precipitation with urea were tested for the total oxidation of naphthalene, a model polycyclic aromatic hydrocarbon (PAH). Systematic variation of preparation conditions, including calcination temperature, calcination time and aging time, resulted in differences in surface area, reducibility, morphology and crystallite size of the CeO 2 catalyst and hence differences in catalytic performance. A combination of high surface area, small crystallite size and high oxygen defect concentration was found to favor the efficiency of the ceria catalysts for the total oxidation of naphthalene. Optimum preparation conditions for this stud…

Insights into the production of upgraded biofuels using Mg-loaded mesoporous ZSM-5 zeolites

9 figures, 6 tables.-- Supplementary information available.-- https://authorservices.wiley.com/author-resources/Journal-Authors/licensing/self-archiving.html

Total oxidation of VOCs on Au nanoparticles anchored on Co doped mesoporous UVM-7 silica

Abstract Gold deposited on a cobalt containing siliceous mesoporous structure, UVM-7, presents a good catalytic performance in the total oxidation of propane and toluene. The presence of both gold and cobalt is necessary as bimetallic Au/Co-UVM-7 catalysts are remarkably more active than monometallic Au/UVM-7 or Co-UVM-7 catalysts. The improved activity of the bimetallic AuCo-samples if compared to gold free cobalt catalysts can be explained on the basis of the enhanced reducibility of some cobalt species in the presence of gold, which facilitates the redox cycle. This high reducibility of cobalt species in the bimetallic samples is probably due to the formation of Co 3 O 4 domains at the g…

Deep oxidation of propane using palladium–titania catalysts modified by niobium

Abstract Pd/TiO 2 catalysts modified by niobium have been prepared and tested for the complete oxidation of propane. The catalysts have been characterised by BET, XRD, laser Raman spectroscopy, XPS, DRS and TPR. The incorporation of niobium into Pd/TiO 2 catalysts resulted in a marked increase in the catalytic activity compared to the Nb-free Pd/TiO 2 catalysts, and the activity increased as the niobium and/or palladium loading increased. The addition of Nb significantly modified the nature of the palladium and niobium species. There was a marked increase in the oxygen mobility after niobium addition. This could not only promote the presence of palladium species in a totally oxidized state …

Molybdenum–vanadium supported on mesoporous alumina catalysts for the oxidative dehydrogenation of ethane

Abstract Vanadium and/or molybdenum oxides supported on mesoporous alumina have been prepared by a “wet” impregnation method, characterized (by using several physico-chemical techniques TPR, DR-UV–vis, Raman spectroscopies) and tested in the oxidative dehydrogenation (ODH) of ethane. For comparison Mo–V-mixed oxides supported on γ-Al2O3 have also been studied. The characterization results indicate that the main vanadium species in both Mo-free and Mo-containing V-based samples present low aggregation and coordination, whereas molybdenum is present as monomeric or polymeric tetrahedral molybdenum species. Interestingly, no apparent interaction between molybdenum and vanadia takes place. The …

Total oxidation of propane in vanadia-promoted platinum-alumina catalysts: Influence of the order of impregnation

Differently prepared vanadium promoted Pt/alumina catalysts have been prepared, characterized and tested for propane total oxidation. V-promoted Pt/Al2O3 catalysts have shown remarkably higher catalytic activity than V-free Pt/Al2O3 catalyst. Among V-promoted Pt catalysts that prepared by coimpregnation gave the highest alkane conversions in the whole range of reaction temperatures studied. Factors such as Pt particle size or the oxidation state of platinum do not seem to be the responsible for the enhanced performance. Modification of the redox properties of the catalyst (i.e. high reducibility of vanadium species) likely provoked by the close contact between platinum particles and vanadiu…