
A. Bueno-LópezUniversity of Alicante | UA · Inorganic Chemistry
A. Bueno-López
PhD Chemistry
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October 2016 - present
September 2006 - October 2016
September 2003 - August 2005
Publications
Publications (195)
7‐Azaindole has been integrated as building block with complementary N−H⋅⋅⋅N hydrogen bonding sites for the synthesis of a tetrahedral molecular tecton, namely tetra(α‐carbolin‐6‐yl)methane, TACM. The self‐assembly of this molecule results in a 3D hydrogen‐bonded organic framework (HOF). This supramolecular structure constitutes a crystalline micro...
7‐Azaindole has been integrated as building block with complementary N‐H···N hydrogen bonding sites for the synthesis of a tetrahedral molecular tecton, namely tetra(α‐carbolin‐6‐yl)methane, TACM. The self‐assembly of this molecule results in a 3D hydrogen‐bonded organic framework (HOF). This supramolecular structure constitutes a crystalline micro...
The present research exploits an innovative methodology for producing auto‐pressurized carbon microreactors with a precise and controlled structure analyzing the influence of their design on the fluid dynamics and their catalytic performance. Carbon monoliths with Tesla‐valve shape channels (Tesla, T, and modified Tesla, Tm) are synthesized through...
In this study, the effect of the cell density of monolithic catalysts was investigated and further mathematically modeled on cordierite supports used in CO2 methanation. Commercial cordierite monoliths with 200, 400, and 500 cpsi cell densities were coated by immersion into an ethanolic suspension of Ni/CeO2 active phase. SEM–EDS analysis confirmed...
Carbon sorbents have been tested in this study to improve the retention of microplastics thermodecomposition compounds in Thermoextraction-Desorption Gas Chromatography-Mass Spectrometry (TED-GC-MS) technique and has been demonstrated an optimal behavior for this application, highlighting two main advantages with regard to conventional PDMS sorbent...
Thermal Extraction-Desorption (TED) using a thermobalance coupled to a gas chromatograph (GC) with mass spectrometer (MS) detector is an extended method for polymers identification in complex matrixes. A new TED-GC/MS method for microplastics identification is developed in this study, where the whole filter with solids collected from water is therm...
Ni/CeO2 catalysts are very active and selective for total hydrogenation of CO2 to methane, but the nature of the active sites is still unclear. The surface of a Ni/CeO2 catalyst has been monitored under CO2 methanation conditions by Near Ambient Pressure-XPS (NAP-XPS) using synchrotron radiation, and has been concluded that the species involved in...
The preparation and use of Guefoams as heterogeneous catalyst is reported. The Guefoam catalyst consists of an open-pore Al-Si foam that accommodates a freely mobile guest phase (Ni/CeO2/Al2O3 particles) in its cavities, with neither a physical nor a chemical matrix-guest bond. A eutectic Al-12Si alloy was used as a low-melting matrix precursor to...
The mechanism and kinetic of CO2 methanation reaction of 9.5 % Ni/Al2O3 catalyst is analysed under a wide range of operating conditions. Once the catalyst activity is stabilized, the influence of temperature, total pressure and space velocity is studied for kinetic characterisation. A data set comprising of 153 experimental runs has been used to de...
A Ce0.5Pr0.5Ox soot combustion catalyst has been shaped combining this material prepared in two different structures (nanoparticles and MS-macroporous) in a single active phase. Nanoparticles, prepared by reversed microemulsion method, provide high activity to the hybrid material, and the MS structure, obtained by a hard template synthesis method,...
The preferential CO oxidation (so-called CO-PROX) is the selective CO oxidation amid H2-rich atmospheres, a process where ceria-based materials are consolidated catalysts. This article aims to disentangle the potential CO–H2 synergism under CO-PROX conditions on the low-index ceria surfaces (111), (110) and (100). Polycrystalline ceria, nanorods an...
Sponge-like carbon monoliths with tailored channel architecture and porosity were prepared by combining sol-gel polymerization and 3D printing technology. The pore size distribution (PSD) and macropore volume were controlled by varying the water concentration used in the synthesis. The size and interconnection degree of primary particles, and conse...
This study addresses the yet unresolved CO2 methanation mechanism on a Ru/CeO2 catalyst by means of near-ambient-pressure X-ray photoelectron spectroscopy (NAP–XPS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) complemented with periodic density functional theory (DFT) calculations. NAP–XPS results show that the switch fr...
The potential of thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC) to identify, distinguish among the most relevant microplastics, and quantification, has been studied, including semicrystalline polymers (polypropylene (PP), polyamide (PA), high density polyethylene (HDPE), low density polyethylene (LDPE) and polyethylene...
The conversion of CO2 towards added valuable products is considered as a potential alternative to achieve the increase of the petrochemical industry while reducing the CO2 emissions. In the present work, the effect of Ru loading on CeO2 supports has been studied for the CO2 methanation reaction, and catalysts with different Ru loading in the 1–5 wt...
Honeycomb monoliths are the preferred supports in many industrial heterogeneous catalysis reactions, but current extrusion synthesis only allows obtaining parallel channels. Here, we demonstrate that 3D printing opens new design possibilities that outperform conventional catalysts. High performance carbon integral monoliths have been prepared with...
Cryptomelane is an abundant mineral manganese oxide with unique physicochemical features. This work investigates the real capabilities of cryptomelane as an oxidation catalyst. In particular, the preferential CO oxidation (CO-PROX), has been studied as a simple reaction model. When doped with copper, the cryptomelane-based material has revealed a g...
PrOx nanoparticles (10nm; 81m²/g) were synthesized and analysed as soot combustion catalyst in comparation with other reference materials including CeO2 nanoparticles and PrOx and CeO2 catalysts with three dimensionally ordered (3DOM) and without controlled structure. PrOx nanoparticles reached the highest activity; T50 decreases from 603 °C (uncat...
CO2 hydrogenation to CH4 (or methanation) has been proposed to diminish CO2 emissions producing a valuable fuel. A catalyst consisting of NiO-CeO2 mixed oxide 6–7 nm nanoparticles with enhanced properties has been prepared, and compared with other NiO-CeO2 reference catalysts including a mixed oxide with the same composition but without control of...
This work investigates the viability of 10-50% LaNiO 3 /CeO 2 formulations, prepared by combined citric acid and impregnated methods, as precursor of highly active and stable materials for CO 2 methanation. The prepared...
A new method to synthesize integral carbon monoliths with a controlled channel morphology has been developed in this work by combining 3D-printing technology and sol–gel polymerization.
Three-dimensional (3D)-printed catalysts are being increasingly studied; however, most of these studies focus on the obtention of catalytically active monoliths, and thus traditional channeled monolithic catalysts are usually obtained and tested, losing sight of the advantages that 3D-printing could entail. This work goes one step further, and an a...
The individual and simultaneous removal of NOx by Storage and Reduction with H2 (H2‐NSR) and combustion of soot have been studied for La and CuLa catalysts. The NOx storage capacity of pure lanthanum oxide is improved either by copper addition or by using a colloidal crystal hard template for the synthesis of a macroporous structure. Although the N...
A new NiO-CeO2 dry methane reforming catalyst (DRM) is presented (8.7 wt% Ni), which consist of high surface area mixed oxide nanoparticles (122 m²/g; 6–7 nm). These nanoparticles showed catalytic stability under the severe conditions of DRM (700 ºC), and improved carbon resistance with regard to conventional NiO-CeO2 catalysts prepared without con...
The role of different active sites on Ni/CeO2 catalysts in the CO2 methanation has been studied. Two types of active sites have been identified: CO2 chemisorption and dissociation sites at the NiO-ceria interface and H2 dissociation sites on Ni⁰ entities. Additionally, the proportion of these active sites has been optimized to maximize the activity...
The preferential CO oxidation (CO-PROX) reaction is paramount for the purification of reformate H2-rich streams, where CuO/CeO2 catalysts show promising opportunities. This work sheds light on the lattice oxygen recovery mechanism on CuO/CeO2 catalysts during CO-PROX reaction, which is critical to guarantee both good activity and selectivity, but t...
Soot oxidation process over La0.7Ag0.3MnOδ≤3 (LAM) and LaMnO3 (LM) catalysts was studied through ¹⁸O2 isotopic labelling experiments in the presence and absence of NO, using catalyst-soot mixtures under loose contact conditions. Isotopic exchange experiments evidenced that silver-particles enhanced oxygen exchange capacity, explained by the increas...
A new concept, referred to as key‐lock catalyst, is presented in this article. Soot combustion ceria catalysts were prepared combining hard (polymethylmethacrylate colloidal crystals) and soft (Pluronic F127) templates, tuning the porosity of ceria in different size ranges to match the morphology of soot aggregates. The catalysts porosity was chara...
The effect of the 3DOM structure and the Ni-doping of CeO2 on the physicochemical properties and catalytic activity for the soot combustion was studied. Moreover, the way in which Ni is introduced to the ceria support was also investigated. For that, CeO2 supports were synthesised with uncontrolled (Ref) and 3DOM structured morphology and their res...
The CO2 methanation mechanism was studied for Ni/CeO2 and Ni/Al2O3 catalysts. The higher methanation activity and selectivity of Ni/CeO2 is attributed to: i) Ni/CeO2 combines two types of active sites efficient for CO2 dissociation at the NiO-Ceria interface and for H2 dissociation on Ni⁰ particles; ii) water desorption is the slowest mechanism ste...
The effect of Ce/Pr ratio on ceria-praseodymia on structural and surface properties is studied. The catalytic activity towards soot combustion under NOx/O2 and O2/N2 atmospheres is also evaluated, together with the NO oxidation activity to NO2. CexPr1-xO2-δ compositions (x = 0.8, 0.5 and 0.2) have been prepared along with ceria and praseodymia. Cat...
Nominally different Cu contents have been loaded on synthetic Cryptomelane oxide and the resulting CuO/Cryptomelane catalysts have been tested in the CO-PROX reaction. Catalytic activity was assessed in terms of the tunable synergistic interaction between copper and cryptomelane. This work entails the use of conventional characterization techniques...
The microwave-synthesized-LaAgMnO3-catalyst can eliminate soot and NOx simultaneously below 400 °C. To get some insight about the chemical species formed on catalyst and soot surfaces, in situ diffuse reflectanced infrared Fourier transform (DRIFT) spectroscopy under NO, O2, and NO/O2 atmospheres was performed. The DRIFTS results indicated that ove...
Honeycomb-shaped cordierite monoliths are widely used as supports for a great number of industrial applications. However, the high manufacturing costs of cordierite monoliths only justifies its use for high temperatures and aggressive chemical environments, demanding applications where the economic benefit obtained exceeds the manufacturing costs....
A series of α-alumina supported cobalt spinel catalysts of various exposition of the (100), (111) and (110) planes was synthetized and tested in CO-PROX reaction. Successful control of the polyhedral shape of the nano-spinel active phase was achieved via glycerol and/or Zn additions to the impregnation solution. This allowed for the application of...
The hydrogenation of CO2 into CH4 from H2 produced by renewable energy is considered an interesting alternative in order to promote the development of such green energies. In the present work, the effect of Ni and Ru loadings on the catalytic performance of alumina-supported catalysts is studied for CO2 methanation reaction. All catalysts were prep...
An improved honeycomb-like monolith with asymmetrical channels, where the channels section decrease along the monolith, was fabricated using a template prepared by 3D printing. A reference honeycomb monolith was also prepared in the same way but with conventional straight channels. Cu/Ceria active phase was loaded on these supports, and SEM-EDX, Ra...
PrOx and CuO/PrOx catalysts have been prepared with conventional (Ref) and three dimensionally order macroporous (3DOM) structures, and the effect of the structure on the soot combustion has been studied. It has been demonstrated that the 3DOM structure significantly improves the catalytic combustion of soot with O2. The activity follows the trend...
One of the key objectives in fuel cell technology is to improve the alcohol oxidation efficiency of Pt-based catalysts. A series of carbon-supported PtRu nanowires with different concentrations of Pt and Ru were prepared for application in methanol oxidation in acid media. The physicochemical properties and electrocatalytic activity of these cataly...
The effect of the LnOx support has been studied for Ni‐based CO2 methanation catalysts. 10 wt.% nickel catalysts with LaOx, CeO2 and PrOx supports have been prepared, characterized by N2 adsorption, XRD, XRF, TG‐MS (N2‐TPD and H2‐TPR) and XPS, and have been tested for CO2 methanation. The catalytic activity follows the trend Ni/CeO2>Ni/PrOx≫Ni/LaOx...
The synthesis and use for soot combustion of praseodymium oxide with three-dimensionally ordered macroporous (3DOM) structure is described. This novel PrOx-3DOM catalyst is presented as an improved novel metal-free alternative to CeO2 as soot combustion catalyst. The PrOx-3DOM catalyst presents a well-defined 3DOM structure with high macropores vol...
Pd-promoted ternary oxides of the type Mn-Ce-Zr and Mn-Pr-Zr were characterized and evaluated for low temperature NOx storage applications such as diesel vehicle cold starts. While X-ray diffraction data were in all cases consistent with the formation of solid solutions, Mn/Zr and Mn/Ce(Pr) ratios found by XPS were consistently higher than the bulk...
CeO2 catalysts have been prepared with conventional (Ref) and three dimensionally order macroporous (3DOM) structures, and the effect of the structure on the soot combustion mechanism has been studied in detail. Isotopic exchange experiments showed that the CeO2-3DOM catalyst produces more active oxygen upon O2 chemisorption than the counterpart Ce...
In the present study, 20 wt % K2CO3 was added to coal and coal/biomass blends in 20:80 wt % ratio and subsequently were heating-treated at 600 °C using CO2 or N2 atmospheres. The reactivity under oxy-combustion conditions (21 % O2 + 79 % CO2) was studied by thermogravimetry, and characterization of chars was carried out by N2 adsorption, scanning e...
A Ce0.9Pr0.1O2 catalyst has been prepared using nitrates as metal precursors, which have been infiltrated into a polymethylmethacrylate colloidal crystal template and calcined at 500 °C. Its catalytic activity for CO oxidation (4.3 μmolCO s⁻¹ gcatalyst⁻¹ at 300 °C) is far superior compared to a reference catalyst prepared in the same way but withou...
A novel concept is presented, consisting of a macroporous carrier-free catalyst. As a proof of concept, a novel Cu-containing Sr-Ti NSR catalyst with a macroporous network has been synthesized, and its maximum NOx storage capacity (1500 μmolNOx/gcatalyst) significantly surpasses that of conventional Pt/Ba/Al2O3 formulations (∼600–800 μmolNOx/gcatal...
The catalytic activity of CuO/Cryptomelane for the preferential oxidation of CO in H2-rich streams has been studied in the absence and presence of H2O and CO2, paying special attention to the catalyst stability and to changes on its physical-chemical properties under CO-PROX reaction conditions.
For fresh CuO/cryptomelane catalyst, the presence of...
In the present study, wood biomass from Acacia mangium and its main components (hemicellulose (xylan), cellulose and lignin) were blended with a sub-bituminous coal in 20:80 wt% ratio and subsequently were heat-treated at 900 °C using CO2 or N2 atmospheres. The reactivity (ignition temperature and activation energy) under oxy-fuel conditions (21 %O...
Pt/CeO2-M2O3 and Pd/CeO2-M2O3 (M = La, Pr, Y, Sm, or Nd) were prepared by co-precipitation and impregnation and were investigated for potential passive NOx adsorber (PNA) use. During NOx storage at 120 °C, it was found that the amount of NOx stored as a function of time for Pt-promoted materials was higher than the Pd-promoted counterparts. For Pt/...
It is demonstrated that the synthesis procedure for preparing three-dimensionally ordered macroporous (3DOM) Pr-doped ceria catalysts using a polymethylmethacrylate (PMMA) template not only affects the porous structure, but also the chemistry of the ceria surface. The PMMA template does not affect the crystalline features (type of phases, crystalli...
En las prácticas experimentales de algunas asignaturas impartidas por el Dpto. de Química Inorgánica, en cursos anteriores, se han utilizado procedimientos de micro-escala para reducir el impacto de sus residuos. En esta Red GEQI se analizan las posibilidades adicionales para que una asignatura totalmente práctica del Grado en Química alcance un ni...
Novel methodology, referred to as rapid-scan operando, has been demonstrated to be a highly powerful tool for studying reaction mechanisms in heterogeneous catalysis, because it combines rapid scan for IR monitoring in the milliseconds time frame and operando methodology. As proof of concept, the NOx–CO and NOx–H2 reactions were studied as model ca...
The performance of noble metal-free copper-based NSR catalysts was studied by rapid-scan operando DRIFTS, using CeO2, BaO and BaO + CeO2 mixtures with different ratios as supports. The maximum temperature for CuO/CeO2 utilization as NSR catalyst was 400 °C, as the stored NOx species decomposed above this temperature. At 400 °C, CuO/CeO2 showed high...
5% copper catalysts with Ce0.8M0.2Oδ supports (M = Zr, La, Ce, Pr or Nd) have been studied by rapid-scan operando DRIFTS for NOx Storage and Reduction (NSR) with high frequency (30 seconds) CO, H2 and 50%CO + 50%H2 micropulses. In the absence of reductant pulses, below 200–250 °C NOx was stored on the catalysts as nitrite and nitro groups, and abov...
5% copper catalysts with Ce0.8M0.2Oδ supports (M = Zr, La, Ce, Pr or Nd) were studied for the simultaneous combustion of soot and removal of NOx by the NSR method. The simultaneous chemisorption of NOx and combustion of soot could be carried out above 375 °C, and nitrates were formed upon NOx chemisorption above this temperature. The nature of the...
Cryptomelane and CuO/cryptomelane catalysts have been tested in the preferential oxidation of CO in the presence of H2 (CO-PROX reaction), paying special attention to deactivation and regeneration issues. Cryptomelane was stable during the CO-PROX reactions in ramp experiments until 200 °C and in a long-term isothermal experiment (10 h). Changes ne...
Model CuO/Ce0.8X0.2O catalysts (with X = Ce, Zr, La, Pr or Nd) have been prepared in order to obtain CuO/ceria materials with different chemical features, and have been characterized by XRD, Raman spectroscopy, N2 adsorption and H2-TPR. CO-PROX experiments have been performed in a fixed-bed reactor and in an operando DRIFTS cell coupled to a mass...
A series of 5%Cu/Ce0.5Pr0.5O2-δ and Ce0.5Pr0.5O2-δ mixed oxides have been prepared and combined in different ratios. The resulting catalysts have been characterized by N2 adsorption, XRD, Raman spectroscopy and H2-TPR and tested for soot combustion by means of temperature-programmed experiments. The optimum catalyst for soot combustion in NOx/O2/N2...
The literature available related to the utilization of perovskites as soot combustion catalysts has been reviewed in this chapter. The general formula of perovskites is ABO3, and soot combustion perovskite catalysts with many different cations have been reported for both A and B positions. The most studied formulations include transition metals tha...
Diesel Particulate Filters (DPFs) have been loaded with the same amount (0.6 wt.%) of either Pt or an optimized CePr active phase, and an experimental set-up has been designated and used to investigate the catalytic combustion of soot under realistic reaction conditions. Both active phases were stable under reaction conditions, with no evidences of...
Carbon-supported Ptx
–Rhy
–Snz
catalysts (x:y:z = 3:1:4, 6:2:4, 9:3:4) are prepared by Pt, Rh, and Sn precursors reduction in different addition order. The materials are characterized by X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy techniques and are evaluated for the electrooxidation of ethanol in acidi...
Carbon-supported Pt-Sn catalysts commonly contain Pt-Sn alloy and/or Pt-Sn bimetallic systems (Sn oxides). Nevertheless, the origin of the promotion effect due to the presence of Sn in the Pt-Sn/C catalyst towards ethanol oxidation in acid media is still under debate and some contradictions. Herein, a series of Ptx-Sny/C catalysts with different at...
A Ce0.5Pr0.5O2 mixed oxide has been prepared with the highest surface area and smallest particle size ever reported (125 m2/g and 7 nm, respectively), also being the most active diesel soot combustion catalyst ever tested under realistic conditions if catalysts forming highly volatile species are ruled out. This Ce–Pr mixed oxide is even more activ...
Ce0.64Zr0.27Nd0.09Oδ mixed oxides have been prepared by three different methods (nitrates calcination, coprecipitation and microemulsion), characterized by N2 adsorption, XRD, H2-TPR, Raman spectroscopy and XPS, and tested for soot combustion in NOx/O2. The catalyst prepared by microemulsion method is the most active one, which is related to its hi...
H– and Na–saponite supports have been prepared by several synthesis approaches. 5% Cu/saponite catalysts have been prepared and tested for soot combustion in a NOx + O2 + N2 gas flow and with soot and catalyst mixed in loose contact mode. XRD, FT-IR, N2 adsorption and TEM characterization results revealed that the use of either surfactant or microw...
Se plantea al alumnado el análisis de la huella de carbono que tiene, en la actualidad, la asignatura práctica Experimentación en Química Inorgánica, con el objetivo de que busquen las posibilidades de sustitución y/o reducción de reactivos tóxicos y peligrosos en las prácticas de laboratorio que se imparten.
CuO supported on CeO2 and Ce0.9X0.1O2, where X is Zr, La, Tb or Pr, were synthesized using
nitrate precursors, giving rise ceria based materials with a small particle size which interact with CuO
species generating a high amount of interfacial sites. The incorporation of cations to the ceria
framework modifies the CeO2 lattice parameter, improving...