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2023


Carboxylate functionalized NaDy(MoO4)(2) nanoparticles with tunable size and shape as high magnetic field MRI contrast agents


Gomez-Gonzalez, E; Nuñez, NO; Caro, C; Garcia-Martin, ML; Ocaña, M
Journal of Colloid and Interface Science, 629 (2022) 310-321
Materiales Coloidales

ABSTRACT ▼

Uniform sodium-dysprosium double molybdate (NaDy(MoO4)(2)) nanoparticles having different morphologies (spheres and ellipsoids) and tunable size have been synthesized for the first time in literature. The procedure is based on a homogeneous precipitation process at moderated temperatures (<= 220 ?) from solutions containing appropriated precursors dissolved in ethylene glycol-water mixtures, in the absence (spheres) or the presence (ellipsoids) of tartrate anions. The effects of the morphological characteristics (size and shape) of the nanoparticles on the magnetic relaxivity at high field (9.4 T) have been evaluated finding that the latter magnitude was higher for the spheres than for the ellipsoids, indicating their better suitability as contrast agents for high-field magnetic resonance imaging. Such nanoparticles have been successfully coated with polymers bearing carboxylate functional groups through a layer-by -layer process, which improves the colloidal stability of the nanoparticles in physiological media. It has been also found that the coating layer had no significant effects on the nanoparticles relaxivity and that such coated nanoparticles exhibited a high biocompatibility and a high chemical stability. In summary, we have developed NaDy(MoO4)(2 )based bioprobes which meet the required criteria for their use as contrast agents for high-field magnetic resonance imaging. 


Enero, 2023 | DOI: 10.1016/j.jcis.2022.08.130



2022


Analysis of Dry Reforming as direct route for gas phase CO2 conversion. The past, the present and future of catalytic DRM technologies


le Sache, E; Reina, TR
Progress in Energy and Combustion Science, 89 (2022) 100970
Química de Superficies y Catálisis

ABSTRACT ▼

Transition to low carbon societies requires advanced catalysis and reaction engineering to pursue green routes for fuels and chemicals production as well as CO2 conversion. This comprehensive review provides a fresh perspective on the dry reforming of methane reaction (DRM) which constitutes a straightforward approach for effective CO2 conversion to added value syngas. The bottleneck for the implementation of this process at industrial scale is the development of highly active and robust heterogeneous catalysts able to overcome the CO2 activation barrier and deliver sufficient amount of the upgrading products at the desired operation conditions. Also, its high energy demand due to the endothermic nature of the reaction imposes extra difficulties. This review critically discusses the recent progresses on catalysts design ranging from traditional metal-supported catalysts to advanced structured and nanostructured systems with promising performance. The main advantages and culprits of the different catalytic systems are introduced aiming to inspire the catalysis community to further refine these formulations towards the development of "supercatalysts" for DRM. Besides the design of increasingly complex catalyst morphologies as well as other promising alternatives aiming at reducing the energy consumption of the process or tackle deactivation through reactor design are introduced.


Marzo, 2022 | DOI: 10.1016/j.pecs.2021.100970

Highly Anisotropic Organometal Halide Perovskite Nanowalls Grown by Glancing-Angle Deposition


Castillo-Seoane, J; Contreras-Bernal, L; Obrero-Perez, JM; Garcia-Casas, X; Lorenzo-Lazaro, F; Aparicio, FJ; Lopez-Santos, C; Rojas, TC; Anta, JA; Borras, A; Barranco, A; Sanchez-Valencia, JR
Advanced Materials (2022) 2107739
Nanotecnología en Superficies y Plasma - Materiales Nanoestructurados y Microestructura

ABSTRACT ▼

Polarizers are ubiquitous components in current optoelectronic devices as displays or photographic cameras. Yet, control over light polarization is an unsolved challenge, since the main drawback of the existing display technologies is the significant optical losses. In such a context, organometal halide perovskites (OMHP) can play a decisive role given their flexible synthesis with tunable optical properties such as bandgap and photoluminescence, and excellent light emission with a low non-radiative recombination rate. Therefore, along with their outstanding electrical properties have elevated hybrid perovskites as the material of choice in photovoltaics and optoelectronics. Among the different OMHP nanostructures, nanowires and nanorods have lately arisen as key players in the control of light polarization for lighting or detector applications. Herein, the fabrication of highly aligned and anisotropic methylammonium lead iodide perovskite nanowalls by glancing-angle deposition, which is compatible with most substrates, is presented. Their high alignment degree provides the samples with anisotropic optical properties such as light absorption and photoluminescence. Furthermore, their implementation in photovoltaic devices provides them with a polarization-sensitive response. This facile vacuum-based approach embodies a milestone in the development of last-generation polarization-sensitive perovskite-based optoelectronic devices such as lighting appliances or self-powered photodetectors.


Marzo, 2022 | DOI: 10.1002/adma.202107739

Ultrathin Plasma Polymer Passivation of Perovskite Solar Cells for Improved Stability and Reproducibility


Obrero-Perez, JM; Contreras-Bernal, L; Nuñez-Galvez, F; Castillo-Seoane, J; Valadez-Villalobos, K; Aparicio, FJ; Anta, JA; Borras, A; Sanchez-Valencia, JR; Barranco, A
Advanced Energy Materials, (2022) 2200812
Materiales Nanoestructurados y Microestructura

ABSTRACT ▼

Despite the youthfulness of hybrid halide perovskite solar cells, their efficiencies are currently comparable to commercial silicon and have surpassed quantum-dots solar cells. Yet, the scalability of these devices is a challenge due to their low reproducibility and stability under environmental conditions. However, the techniques reported to date to tackle such issues recurrently involve the use of solvent methods that would further complicate their transfer to industry. Herein a reliable alternative relaying in the implementation of an ultrathin plasma polymer as a passivation interface between the electron transport layer and the hybrid perovskite layer is presented. Such a nanoengineered interface provides solar devices with increased long-term stability under ambient conditions. Thus, without involving any additional encapsulation step, the cells retain more than 80% of their efficiency after being exposed to the ambient atmosphere for more than 1000 h. Moreover, this plasma polymer passivation strategy significantly improves the coverage of the mesoporous scaffold by the perovskite layer, providing the solar cells with enhanced performance, with a champion efficiency of 19.2%, a remarkable value for Li-free standard mesoporous n-i-p architectures, as well as significantly improved reproducibility.


Julio, 2022 | DOI: 10.1002/aenm.202200812

Unraveling the Mo/HZSM-5 reduction pre-treatment effect on methane dehydroaromatization reaction


Lopez-Martin, A; Caballero, A; Colon, G
Applied Catalysis B-Environmental, 312 (2022) 121382
Materiales y Procesos Catalíticos de Interés Ambiental y Energético

ABSTRACT ▼

Reduction pre-treatment at different temperatures were performed over Mo/HZSM-5 system before methane dehydroaromatiztion reaction. We have shown the crucial effect of reduction temperature on the final catalytic performance. Outstanding improvement in the aromatics conversion has been attained. Thus, H-2 formation form methane cracking reaction seems to be hindered for pre-treated catalysts. As a consequence, the deposition of coke in these samples appeared also notably suppressed. The optimum performance has been achieved for reduction pre-treatment at 550 degrees C. For this temperature, we have observed that the fraction of reduced Mo species is higher.


Septiembre, 2022 | DOI: 10.1016/j.apcatb.2022.121382

Characterization of Re-Mo/ZSM-5 catalysts: How Re improves the performance of Mo in the methane dehydroaromatization reaction


Lopez-Martin, A; Sini, MF; Cutrufello, MG; Caballero, A; Colon, G
Applied Catalysis B-Environmental, 304 (2022) 120960
Materiales y Procesos Catalíticos de Interés Ambiental y Energético

ABSTRACT ▼

In this study, the promoting effect of rhenium addition as a co-dopant on Mo/ZSM-5 catalysts system has been analysed. Hence, bimetallic (Re-Mo/ZSM-5) catalysts have been synthesized using a sequential impregnation methodology. The catalytic performance for direct aromatization of methane reaction has been determined and correlated with their physical and chemical state combining multiple characterization techniques. An important synergy between Mo and Re, affected by the sequential impregnation, has been observed. Thus, Re1-Mo4/ZSM-5 in which Re has been incorporated first shows notably higher aromatic yields and stability against deactivation. Characterization results suggest that catalytic enhancement is due to the important effect of Re presence in close interaction with Mo. Improved evolution of ethane through C-C coupling would be correlated to this catalytic performance. As we discuss, Mo nature and location in the bimetallic systems are strongly conditioned by Re and the impregnation sequence and favours such intermediate step.


Mayo, 2022 | DOI: 10.1016/j.apcatb.2021.120960

Evidence of new Ni-O-K catalytic sites with superior stability for methane dry reforming


Azancot, L; Blay, V; Blay-Roger, R; Bobadilla, LF; Penkova, A; Centeno, MA; Odriozola, JA
Applied Catalysis B-Environmental, 307 (2022) 121148
Química de Superficies y Catálisis

ABSTRACT ▼

Liquid fuels produced via Fischer-Tropsch synthesis from biomass-derived syngas constitute an attractive and sustainable energy vector for the transportation sector. This study focuses on the role of potassium as a promoter in Ni-based catalysts for reducing coke deposition during catalytic dry reforming. The study provides a new structural link between catalytic performance and physicochemical properties. We identify new Ni-O-K chemical states associated with high stability in the reforming process, evidenced by different characterization techniques. The nickel particles form a core surrounded by a Ni-O-K phase layer (Ni@Ni-O-K) during the reduction of the catalyst. This phase likely presents an alkali-nickelate-type structure, in which nickel is stabilized in oxidation state + 3. The Ni-O-K formation induces essential changes in the electronic, physical, structural, and morphological properties of the catalysts, notably enhancing their long-term stability in dry reforming. This work thus provides new directions for designing more efficient catalysts for sustainable gas-to-liquids processes.


Junio, 2022 | DOI: 10.1016/j.apcatb.2022.121148

Plasma engineering of microstructured piezo-Triboelectric hybrid nanogenerators for wide bandwidth vibration energy harvesting


Garcia-Casas, X; Ghaffarinehad, A; Aparicio, FJ; Castillo-Seoane, J; Lopez-Santos, C; Espinos, JP; Cotrino, J; Sanchez-Valencia, JR; Barranco, A; Borras, A
Nano Energy, 91 (2022) 106673
Nanotecnología en Superficies y Plasma

ABSTRACT ▼

We introduce herein the advanced application of low-pressure plasma procedures for the development of piezo and triboelectric mode I hybrid nanogenerators. Thus, plasma assisted deposition and functionalization methods are presented as key enabling technologies for the nanoscale design of ZnO polycrystalline shells, the formation of conducting metallic cores in core@shell nanowires, and for the solventless surface modification of polymeric coatings and matrixes. We show how the perfluorinated chains grafting of polydimethylsiloxane (PDMS) provides a reliable approach to increase the hydrophobicity and surface charges at the same time that keeping the PDMS mechanical properties. In this way, we produce efficient Ag/ZnO convoluted piezoelectric nanogenerators supported on flexible substrates and embedded in PDMS compatible with a contact-separation triboelectric architecture. Factors like crystalline texture, ZnO thickness, nanowires aspect ratio, and surface chemical modification of the PDMS are explored to optimize the power output of the nanogenerators aimed for harvesting from low-frequency vibrations. Just by manual triggering, the hybrid device can charge a capacitor to switch on an array of color LEDs. Outstandingly, this simple three-layer architecture allows for harvesting vibration energy in a wide bandwidth, thus, we show the performance characteristics for frequencies between 1 Hz and 50 Hz and demonstrate the successful activation of the system up to ca. 800 Hz.


Enero, 2022 | DOI: 10.1016/j.nanoen.2021.106673

Electrocatalytic CO2 conversion to C-2 products: Catalysts design, market perspectives and techno-economic aspects


Ruiz-López, E; Gandara-Loe, J; Baena-Moreno, F; Reina, TR; Odriozola, JA
Renewable & Sustainable Energy Reviews, 161 (2022) 112329
Química de Superficies y Catálisis

ABSTRACT ▼

The energy crisis caused by the incessant growth in global energy demand joint to its associated greenhouse emissions motivates the urgent need to control and mitigate atmospheric CO2 levels. Leveraging CO2 as carbon pool to produce value-added products represents a cornerstone of the circular economy. Among the CO2 utilization strategies, electrochemical reduction of CO2 conversion to produce fuels and chemicals is booming due to its versatility and end-product flexibility. Herein most of the studies focused on C-1 products although C-2 and C2+ compounds are chemically and economically more appealing targets requiring advanced catalytic materials. Still, despite the complex pathways for C2+ products formation, their multiple and assorted applications have motivated the search of suitable electrocatalysts. In this review, we gather and analyse in a comprehensive manner the progress made regarding C2+ products considering not only the catalyst design and the electrochemistry features but also techno-economic aspects in order to envisage the most profitable scenarios. This state-of-the-art analysis showcases that electrochemical reduction of CO2 to C-2 products will play a key role in the decarbonisation of the chemical industry paving the way towards a low-carbon future.


Junio, 2022 | DOI: 10.1016/j.rser.2022.112329

Ionomer-Free Nickel-Iron bimetallic electrodes for efficient anion exchange membrane water electrolysis


Lopez-Fernandez, E; Gomez-Sacedon, C; Gil-Rostra, J; Espinos, JP; Gonzalez-Elipe, AR; Yubero, F; De Lucas-Consuegra, A
Chemical Engineering Journal, 433 (2022) 133774
Nanotecnología en Superficies y Plasma

ABSTRACT ▼

A bottleneck for the deployment of the Anion Exchange Membrane Water Electrolysis (AEMWE) is the manufacturing of efficient and long lasting anodes and cathodes for the cells. Highly performant bimetallic Ni/Fe catalyst films with various atomic ratios have been prepared by magnetron sputtering in an oblique angle configuration (MS-OAD) and used as anodes for AEMWE. Electrocatalytic experiments in a small three-electrode cell and a thorough analysis of the electrode properties with various physico-chemical characterization tech-niques have been used to select the nanostructured anode catalyst which, depicting an optimized Ni/Fe ratio, presents the maximum activity for the oxygen evolution reaction. These anode layers are then scale-up for their integration in an AEMWE cell where the influence of assembly conditions and the effect of adding an ionomer to the anodes have been studied. The obtained results have demonstrated the outstanding properties of the fabri-cated bimetallic films in terms of activity, stability, and operation under ionomer-free conditions. Current density values around 400 and 600 mA cm(-2) at 40??& nbsp;and 60 C (2.0 V), respectively, much higher than those obtained with pure Ni, were obtained with an optimized membrane electrode assembly. The high yield obtained with these electrodes gains further relevance when considering that the current yield per unit mass of the anodic active phase catalyst (i.e., 1086 mA mg(-1) at 2.0 V and 40??) is the highest among equivalent values reported in literature. The possibilities and prospects of the use of bimetallic catalyst films prepared by MS-OAD for AEMWE are discussed.


Abril, 2022 | DOI: 10.1016/j.cej.2021.133774

Plasma assisted CO2 dissociation in pure and gas mixture streams with a ferroelectric packed-bed reactor in ambient conditions


Navascues, P; Cotrino, J; Gonzalez-Elipe, AR; Gomez-Ramirez, A
Chemical Engineering Journal, 430 (2022) 133066
Nanotecnología en Superficies y Plasma

ABSTRACT ▼

Carbon dioxide decomposition is a challenging target to combat climate change. Nonthermal plasmas are advantageous for this purpose because they operate at ambient conditions and can be easily scaled-up. In this study, we attempt the CO2 splitting into CO and O-2 in a parallel plate packed-bed plasma reactor moderated with Lead Zirconate Titanate (PZT) as fermelectric component, achieving conversion rates and energy efficiencies higher than those obtained with BaTiO3 in our experimental device. The analysis of the reaction mechanisms with optical emission spectroscopy under various operating conditions has shown a direct correlation between energy efficiency and intensity of CO* emission bands. These results and those obtained with a LiNbO3 plate placed onto the active electrode suggest that high temperature electrons contribute to the splitting of CO2 through an enhancement in the formation of CO2+ intermediate species. Results obtained for CO2 + O-2 mixtures confirm this view and suggest that back recombination processes involving CO and O-2 may reduce the overall splitting efficiency. The study of mixtures of CO2 and dry air has proved the capacity of fermelectric packed-bed reactors to efficiently decompose CO2 with no formation of harmful NxOy subproducts in conditions close to those in real facilities. The found enhancement in energy efficiency with respect to that found for the pure gas decomposition supports that new reaction pathways involving nitrogen molecules are contributing to the dissociation reaction. We conclude that PZT moderated packed-bed plasma reactors is an optimum alternative for the decompositon of CO2 in real gas flows and ambient conditions.


Febrero, 2022 | DOI: 10.1016/j.cej.2021.133066

Shepherding reaction intermediates to optimize H-2 yield using composite-doped TiO2-based photocatalysts


Barba-Nieto, I.; Colon, G; Fernández-García, M; Kubacka, A
Chemical Engineering Journal, 442 (2022) 136333
Materiales y Procesos Catalíticos de Interés Ambiental y Energético

ABSTRACT ▼

Optimization of Pt-promoted TiO2-based is key to promote the photocatalytic production of hydrogen using sacrificial alcohol molecules. Combination of doping and surface decoration of the mentioned base photoactive material is here exploited to maximize hydrogen yield. Using the quantum efficiency parameter, it is shown that the resulting composite system can boost activity up to 7.3 times within the whole methanol:water mixture ratio, yielding quantum efficiencies in the ca. 13-16 % range. The key role of the different components in generating charge carrier species and their use to trigger the sacrificial molecule evolution and control reaction kinetics are examined through an in-situ spectroscopic study. The study unveils the complex reaction mechanism, with generation of C1 to C3 molecules from different carbon-containing radicals, and interprets the physical origin of the huge H2 production enhancement occurring in doped-composite titania-based catalysts.


Agosto, 2022 | DOI: 10.1016/j.cej.2022.136333

Albero: An alternative natural material for solar energy storage by the calcium-looping process


Moreno, V; Arcenegui-Troya, J; Sanchez-Jimenez, P; Perejon, A; Chacartegui, R; Valverde, JM; Perez-Maqueda, LA
Chemical Engineering Journal, 440 (2022) 135707
Reactividad de Sólidos

ABSTRACT ▼

Large-scale thermochemical energy storage (TCES) is gaining relevance as an alternative to current thermal energy storage systems in Concentrated Solar Power plants. Among the different systems, the reversible reaction between CaO and CO2 stands out due to the wide availability and low cost of the raw material: limestone. Direct solar absorption of the storage media would improve the efficiency of solar-to-thermal energy storage due to reduced thermal transfer barriers, but the solar optical absorption of CaCO3 is poor. In this work, we propose the use of a Ca-rich calcarenite sedimentary rock so-called albem as an alternative to limestone. We demonstrate that this reddish material exhibits an average solar absorptance that is approximately ten times larger than limestone. Moreover, the multicycle carbonation/calcination performance under different experimental conditions has been studied by thermogravimetry, and similar values to those exhibited for limestone have been obtained. Besides, the material is cheap (6 Elton), and simulations showed that the use of this material would significantly improve the overall CaL-CSP efficiency at the industrial level.


Julio, 2022 | DOI: 10.1016/j.cej.2022.135707

Au and Pt Remain Unoxidized on a CeO2-Based Catalyst during the Water-Gas Shift Reaction


Reina, TR; Gonzalez-Castano, M; Lopez-Flores, V; Martinez, LMT; Zitolo, A; Ivanova, S; Xu, WQ; Centeno, MA; Rodriguez, JA; Odriozola, JA
Journal of the American Chemical Society, 144 (2022) 446-453
Química de Superficies y Catálisis

ABSTRACT ▼

The active forms of Au and Pt in CeO2-based catalysts for the water-gas shift (WGS) reaction are an issue that remains unclear, although it has been widely studied. On one hand, ionic species might be responsible for weakening the Ce-O bonds, thus increasing the oxygen mobility and WGS activity. On the other hand, the close contact of Au or Pt atoms with CeO2 oxygen vacancies at the metal-CeO2 interface might provide the active sites for an efficient reaction. In this work, using in situ X-ray absorption spectroscopy, we demonstrate that both Au and Pt remain unoxidized during the reaction. Remarkable differences involving the dynamics established by both species under WGS atmospheres were recognized. For the prereduced Pt catalyst, the increase of the conversion coincided with a restructuration of the Pt atoms into cuboctahedrical metallic particles without significant variations on the overall particle size. Contrary to the relatively static behavior of Pt-0, Au-0 nanoparticles exhibited a sequence of particle splitting and agglomeration while maintaining a zero oxidation state despite not being located in a metallic environment during the process. High WGS activity was obtained when Au atoms were surrounded by oxygen. The fact that Au preserves its unoxidized state indicates that the chemical interaction between Au and oxygen must be necessarily electrostatic and that such an electrostatic interaction is fundamental for a top performance in the WGS process.


Enero, 2022 | DOI: 10.1021/jacs.1c10481

Iron-catalyzed graphitization for the synthesis of nanostructured graphitic carbons


Hunter, RD; Ramirez-Rico, J; Schnepp, Z
Journal of Materials Chemistry A, 10 (2022) 4489-4516
Materiales de Diseño para la Energía y Medioambiente

ABSTRACT ▼

Carbons are versatile and diverse materials that have numerous applications across energy and environmental sciences. Carbons with a graphitic structure are particularly appealing due to their high chemical stability, large surface areas and high thermal and electronic conductivity. Numerous methods exist to produce nanostructured graphitic carbons but some of these can be energy-intensive and/or have problems with scalability. One option that is being increasingly explored is the process of iron-catalyzed graphitization. This simply involves the pyrolysis of carbon-rich precursors in the presence of an iron catalyst and has been used to produce carbons with a wide range of structures and properties. This review will examine the current field of iron-catalyzed graphitization, with a focus on molecular organic or biomass precursors. Bio-derived precursors are particularly attractive as a potential option for sustainable production of graphitic carbons. We start with a brief introduction to some key carbon structures, the current applications in which they are employed and some of the key methods that have been developed to produce nanostructured graphitic carbons. We will then review the history of catalytic graphitization before evaluating the wide range of conditions and precursors that have been employed in catalytic graphitization. Finally, this review will investigate the current challenges facing iron-catalyzed graphitization, looking particularly at the limitations of the current understanding of the mechanistic aspects of graphitization, with a view to outlining where research in this field might progress.


Febrero, 2022 | DOI: 10.1039/d1ta09654k

Photocatalytic oxidation of pollutants in gas-phase via Ag3PO4-based semiconductor photocatalysts: Recent progress, new trends, and future perspectives


Y. Naciri; A. Hsini; A. Bouziani; R. Djellabi; Z. Ajmal; M. Laabd; J.A. Navío; A. Mills; C.L. Bianchi; H.Li; B. Bakiz; A. Albourine
Critical Reviews in Environmental Science and Technology, 52 (2022) 2339-2382
Fotocatálisis Heterogénea: Aplicaciones

ABSTRACT ▼

Air pollution has become a significant challenge for both developing and developed nations. due to its close association with numerous fatal diseases such as cancer, respiratory, heart attack, and brain stroke. Over recent years, heterogeneous semiconductor photocatalysis has emerged as an effective approach to air remediation due to the ease of scale-up, ready application in the field, use of solar light and ready availability of a number of different effective photocatalysts. To date, most work in this area has been conducted using UV-absorbing photocatalysts, such as TiO2 and ZnO; However, recent studies have revealed Ag3PO4 as an attractive, visible-light-absorbing alternative, with a bandgap of 2.43 eV. In particular, this material has been shown to be an excellent photocatalyst for the removal of many types of pollutants in the gas phase. However, the widespread application of Ag3PO4 is restricted due to its tendency to undergo photoanodic corrosion and the poor reducing power of its photogenerated conductance band electrons, which are unable to reduce O2 to superoxide •O2 −. These limitations are critically evaluated in this review. In addition, recent studies on the modification of Ag3PO4 via combination with the conventional heterojunctions or Z-scheme junctions, as well as the photocatalytic mechanistic pathways for enhanced gas-pollutants removal, are summarized and discussed. Finally, an overview is given on the future developments that are required in order to overcome these challenges and so stimulate further research into this promising field.


Julio, 2022 | DOI: 10.1080/10643389.2021.1877977

Flame confinement in biomass combustion systems for particles abatement


Ciria, D; Orihuela, MP; Moreno-Naranjo, P; Chacartegui, R; Ramirez-Rico, J; Becerra, JA
Energy Conversion and Management, 264 (2022) 115706
Materiales de Diseño para la Energía y Medioambiente

ABSTRACT ▼

This work explores the use of open-pore, inert ceramic foams with different pore sizes as particle abatement systems in small biomass combustion systems. Porous foams made of silicon carbide with pore sizes 10 to 60 pores-per-inch were installed in an in-house designed combustion unit operated with wood pellets. Their effects on the temperature distribution inside the chamber, particulate and gases emissions were studied using different airflow rates in the reaction-limited regime (low equivalence ratio) to minimise stoichiometric factors. The influence of pore size, foam position with respect to the flame and space velocity were assessed. The confinement of the flame with inert foams was found to substantially modify the temperature distribution in the combustion chamber, improve the air-fuel mixture, and favour the thermal decomposition of the pellet, leading to a reduction in particulate emissions when compared to free-flame combustion at the same experimental conditions. In general, the amount of particulate matter was found to decrease by up to one order of magnitude as the pore size of the foam was reduced, while the temperature gradient in the combustion chamber was increased. Nitrogen oxides and carbon dioxide emissions were essentially unchanged, irrespectively of the pore size of the foam. It is expected that these values will be improved with longer residence times, as happens in operations with reduced excess air ratios. These results suggest that it is possible to control pollutants derived from domestic heating within the most restrictive current regulations on particulate emissions by integrating flame confinement designs with better operating practices and efficient abatement systems.


Julio, 2022 | DOI: 10.1016/j.enconman.2022.115706

Greaseproof, hydrophobic, and biodegradable food packaging bioplastics from C6-fluorinated cellulose esters


Guzman-Puyol, S; Tedeschi, G; Goldoni, L; Benitez, JJ; Ceseracciu, L; Koschella, A; Heinze, T; Athanassiou, A; Heredia-Guerrera, JA
Food Hydrocolloids, 128 (2022) 107562
Materiales de Diseño para la Energía y Medioambiente

ABSTRACT ▼

Tridecafluorononanoic acid (TFNA), a C6-fluorinated carboxylic acid, was esterified with cellulose at different molar ratios (0:1, 1:1, 2:1, and 3:1) in a trifluoroacetic acid (TFA):trifluoroacetic anhydride (TFAA):CHCl3 (2:1:1, v:v:v) solvent mixture. Free-standing films were obtained for all formulations and are presented as alternatives to composites and blends of paper with fluorinated molecules. Mechanical properties were investigated by tensile tests, and a plasticizer effect of fluorinated chains was observed. Interestingly, the wettability of these new cellulose derivatives was similar or even better than other common cellulose derivatives and fluorinated poly-mers employed in food packaging. Hydrodynamic properties were also improved by addition of TFNA, resulting in materials with water vapor permeability values comparable to other cellulose-based food packaging materials. In addition, films with the higher amounts of TFNA showed the required oil resistance for papers used in food packaging applications, as determined by the Kit Test. Finally, the biodegradation of these C6-fluorinated cel-lulose esters, assessed by biological oxygen demand (BOD) in seawater, was higher than typical bio-based polymers used in food packaging. The bioplastic synthesized at a molar ratio 1:1 (TFNA:cellulose) showed excellent performances in terms of greaseproof, hydrophobicity, ductility, and biodegradability, representing a sustainable alternative to typical plastics used in food packaging.


Julio, 2022 | DOI: 10.1016/j.foodhyd.2022.107562

Sustainable routes for acetic acid production: Traditional processes vs a low-carbon, biogas-based strategy


Martin-Espejo, JL; Gandara-Loe, J; Odriozola, JA; Reima, TR; Pastor-Pérez, L
Science of the Total Environment, 840 (2022) 156663
Química de Superficies y Catálisis

ABSTRACT ▼

The conversion of biogas, mainly formed of CO2 and CH4, into high-value platform chemicals is increasing attention in a context of low-carbon societies. In this new paradigm, acetic acid (AA) is deemed as an interesting product for the chemical industry. Herein we present a fresh overview of the current manufacturing approaches, compared to potential low-carbon alternatives. The use of biogas as primary feedstock to produce acetic acid is an auspicious alternative, representing a step-ahead on carbon-neutral industrial processes. Within the spirit of a circular economy, we propose and analyse a new BIO-strategy with two noteworthy pathways to potentially lower the environmental impact. The generation of syngas via dry reforming (DRM) combined with CO2 utilisation offers a way to produce acetic acid in a two-step approach (BIO-Indirect route), replacing the conventional, petroleum-derived steam reforming process. The most recent advances on catalyst design and technology are discussed. On the other hand, the BIO-Direct route offers a ground-breaking, atom-efficient way to directly generate acetic acid from biogas. Nevertheless, due to thermodynamic restrictions, the use of plasma technology is needed to directly produce acetic acid. This very promising approach is still in an early stage. Particularly, progress in catalyst design is mandatory to enable low-carbon routes for acetic acid production.


Septiembre, 2022 | DOI: 10.1016/j.scitotenv.2022.156663

Optoelectronic Devices Based on Scaffold Stabilized Black-Phase CsPbI3 Nanocrystals


Romero-Perez, C; Rubino, A; Calio, L; Calvo, ME; Miguez, H
Advanced Optical Materials (2022) 2102112
Materiales Ópticos Multifuncionales

ABSTRACT ▼

The optoelectronic properties of lead halide perovskites are intimately related to their crystalline phase. For the case of cesium lead iodide (CsPbI3) several polymorphs meet the Goldschmidt tolerance factor, which determines their stability, and form broad band absorber and luminescent phases. However, at room temperature none of them are stable, which prevents their use in optoelectronics. In this work, bare CsPbI3 nanocrystals are synthesized in the sub-10 nm range in the "black", light emitting, crystalline phase, using a pore controlled SiO2 matrix that limits crystal size and confers a certain degree of strain that favors their stability. Quantum confinement effects allow the tuning of the optical properties of the CsPbI3 nanocrystals by means of the crystal size. Their suitability as optoelectronic materials is demonstrated by building scaffold supported CsPbI3 quantum dot based photovoltaic and light emitting devices.


Enero, 2022 | DOI: 10.1002/adom.202102112

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