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Artículos SCI



2024


Química de Superficies y Catálisis

Highly active and selective ZIF-derived cobalt catalyst for methanol conversion to dimethyl carbonate

Wang, LP; Meng, FH; Ding, PF; Nawaz, MA; Li, Z
Applied Organometallic Chemistry (2024) e7537

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The oxidative carbonylation of methanol to synthesize dimethyl carbonate (DMC) has been extensively studied over Cu-based catalysts, but the activity and selectivity are not high. The Co catalysts exhibit high DMC selectivity, but the difficulty in recycling homogeneous Co catalyst and the low conversion of heterogeneous Co catalyst limit the application of Co catalysts. Here, the core–shell ZIFs materials were synthesized and carbonized to obtain solid core–shell cobalt catalysts, and then the catalytic performance for methanol conversion to DMC was investigated. The CoNC@NC catalyst, carbonized from Z67@Z8 with Z67 as the core and Z8 as the shell, shows that the carbonized NC shell effectively suppressed the aggregation of Co NPs and the Co NPs were only 15.4 nm, which was much smaller than those of NC@CoNC (34.5 nm) and CoNC (48.1 nm) catalysts. Compared with the CoNC catalyst, CoNC@NC significantly improved the pulse chemisorption of CH3OH and CO, leading to a significant increase in methanol conversion from 6.9% to 17.1%. Furthermore, the deactivation rate of the CoNC@NC catalyst (22.8%) was much lower than that of CoNC (59.4%) after five reaction cycles. The results of this work provide a new strategy for the design and preparation of solid cobalt catalysts for the oxidative carbonylation of methanol to DMC.


Mayo, 2024 | DOI: 10.1002/aoc.7537

Materiales Semiconductores para la Sostenibilidad

Multifold Enhanced Photon Upconversion in a Composite Annihilator System Sensitized by Perovskite Nanocrystals

Chua, XW; Dai, LJ; Anaya, M; Salway, H; Ruggeri, E; Bi, PQ; Yang, ZH; Stranks, SD; Yang, L
ACS Nano (2024)

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Photon upconversion via triplet-triplet annihilation (TTA-UC) provides a pathway to overcoming the thermodynamic efficiency limits in single-junction solar cells by allowing the harvesting of sub-bandgap photons. Here, we use mixed halide perovskite nanocrystals (CsPbX3, X = Br/I) as triplet sensitizers, with excitation transfer to 9,10-diphenylanthracene (DPA) and/or 9,10-bis[(triisopropylsilyl)ethynyl]anthracene (TIPS-An) which act as the triplet annihilators. We observe that the upconversion efficiency is five times higher with the combination of both annihilators in a composite system compared to the sum of the individual single-acceptor systems. Our work illustrates the importance of using a composite system of annihilators to enhance TTA upconversion, demonstrated in a perovskite-sensitized system, with promise for a range of potential applications in light-harvesting, biomedical imaging, biosensing, therapeutics, and photocatalysis.


Mayo, 2024 | DOI: 10.1021/acsnano.4c03753

Fotocatálisis Heterogénea: Aplicaciones

Novel heterostructured NaTaO3/WO3 systems with improved photocatalytic properties for water decontamination under UV and Visible illumination

Hernández-Laverde, M; Murcia, JJ; Navío, JA; Hidalgo, MC
Journal of Materials Science (2024)

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In this work, we present the preparation of NaTaO3/WO3 systems, a broad-bandgap and a narrow-bandgap semiconductor, respectively, for photocatalytic applications. The samples were prepared by two different methods, microwave-assisted and conventional hydrothermal method, with different NaTaO3/WO3 molar ratios. All samples were extensively characterized, and the photocatalytic behavior was studied in the degradation reaction of rhodamine B under simulated solar illumination. A significant synergistic effect in the coupling of the two components could be observed, with an important improvement in the rhodamine degradation rate, especially for the microwave-prepared sample with 1:1 (NaTaO3/WO3) molar ratio. The enhancement of the activity can be explained by the formation of type II and Z-Scheme heterojunctions. The obtained results are promising for the development of more efficient photocatalyst materials under solar or visible illumination.


Mayo, 2024 | DOI: 10.1007/s10853-024-09699-x

Materiales Coloidales

Nanoparticulated Bimodal Contrast Agent for Ultra-High-Field Magnetic Resonance Imaging and Spectral X-ray Computed Tomography

González-Mancebo, D; Becerro, AI; Caro, C; Gómez-González, E; Luisa, GMM; Ocaña, M
Inorganic Chemistry, 63(23) (2024) 10648-10656

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Bimodal medical imaging based on magnetic resonance imaging (MRI) and computed tomography (CT) is a well-known strategy to increase the diagnostic accuracy. The most recent advances in MRI and CT instrumentation are related to the use of ultra-high magnetic fields (UHF-MRI) and different working voltages (spectral CT), respectively. Such advances require the parallel development of bimodal contrast agents (CAs) that are efficient under new instrumental conditions. In this work, we have synthesized, through a precipitation reaction from a glycerol solution of the precursors, uniform barium dysprosium fluoride nanospheres with a cubic fluorite structure, whose size was found to depend on the Ba/(Ba + Dy) ratio of the starting solution. Moreover, irrespective of the starting Ba/(Ba + Dy) ratio, the experimental Ba/(Ba + Dy) values were always lower than those used in the starting solutions. This result was assigned to lower precipitation kinetics of barium fluoride compared to dysprosium fluoride, as inferred from the detailed analysis of the effect of reaction time on the chemical composition of the precipitates. A sample composed of 34 nm nanospheres with a Ba0.51Dy0.49F2.49 stoichiometry showed a transversal relaxivity (r(2)) value of 147.11 mM(-1)s(-1) at 9.4 T and gave a high negative contrast in the phantom image. Likewise, it produced high X-ray attenuation in a large range of working voltages (from 80 to 140 kVp), which can be attributed to the presence of different K-edge values and high Z elements (Ba and Dy) in the nanospheres. Finally, these nanospheres showed negligible cytotoxicity for different biocompatibility tests. Taken together, these results show that the reported nanoparticles are excellent candidates for UHF-MRI/spectral CT bimodal imaging CAs.


Mayo, 2024 | DOI: 10.1021/acs.inorgchem.4c01114

Fotocatálisis Heterogénea: Aplicaciones

Photocatalytic activity enhancement by noble metal deposition on faceted F-TiO2 synthesised by microwave assisted method. A study of selective oxidation of gas-phase ethanol in a FBPR reactor

Hernández-Laverde, M; Murcia, JJ; Morante, N; Sannino, D; Vaiano, V; Navío, JA; Hidalgo, MC
Catalysis Today, 433 (2024) 114645

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In the present work, fluorinated titanium dioxide (TiO2-F) with high exposition of facet {001} was prepared by following a facile and high yield hydrothermal method assisted by microwave. This faceted TiO2 was then modified by Au or Ag deposition at two different metal loadings (0.125 and 0.25 wt%). A wide physicochemical characterisation of the materials was performed. X-ray difractograms showed high {001} facet exposition in all materials. By X-ray fluorescence it was found that the different samples contained about 5% of fluor. All samples presented high surface area and high uniformity and homogeneity of particles, which highlights the good properties that can be achieved by the microwave synthesis method compared to conventional hydrothermal methods. Oxidation state of the noble metals was studied by XPS. On the other side, TiO2-F and the metallised titania powders were immobilised on polystyrene pellets (PS) for evaluating their gas photocatalytic activity in volatile organic compounds (VOCs) decontamination by following the reaction of photoxidation of ethanol in gas phase. It was found that activity was considerably improved by the addition of noble metals, obtaining high conversion and selectivity to CO2. It is remarkable that the selectivity to CO is almost zero. The highest efficiency was found for the faceted TiO2-F sample with the lowest Au loading (0.125 wt%) immobilised on PS where 91% ethanol conversion and 100% CO2 selectivity were achieved. Different reaction variables were also studied.


Mayo, 2024 | DOI: 10.1016/j.cattod.2024.114645

 

 

 

 

 

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