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1.
Inorg Chem ; 63(1): 247-255, 2024 Jan 08.
Artículo en Inglés | MEDLINE | ID: mdl-38101323

RESUMEN

To elucidate the impact of a high entropy elemental distribution of the lattice site on the magnetic properties in oxide compounds, a series of complex perovskites BaBO3 (B = Y, Fe, Ti, Zr, Hf, Nb, and Ta) with different Fe content ratios (0, 0.2, 0.3, and 0.4) have been synthesized and thoroughly characterized. In this complex oxide series, superconducting quantum interference device magnetometry reveals a gradual change of a well-defined magnetic phase transition and B-site magnetic moment, which correlates with the Fe content. More importantly, a comprehensive analysis of the sample with a 0.4-Fe content (40% on the B-site) including magnetization, heat capacity, neutron diffraction, and muon-spin rotation measurements suggests that in the low-temperature state, a short-range antiferromagnetic correlation may exist, which could result from the magnetic interaction of Fe ions and consequent redistribution of associated d-electrons.

2.
Inorg Chem ; 62(12): 4999-5007, 2023 Mar 27.
Artículo en Inglés | MEDLINE | ID: mdl-36907992

RESUMEN

High-entropy hydroxides are an emerging subcategory of high-entropy materials (HEMs), not only because they can serve as tailorable precursors to high-entropy oxides (HEOs) but also because they can have unique high-entropy properties themselves. Many hydroxide crystal structures that are important for various applications are yet to be studied within the context of high-entropy materials, and it is unknown if they can take a high-entropy form (typically five or more incorporated cations). One such material is the dawsonite-type structure, which is a material with applications in both catalysis and ceramics. This work focuses on the adaptation of a dawsonite-type structure (NH4M(OH)2CO3) into a high-entropy material. Through a coprecipitation synthesis method, dawsonite-type materials readily took a high-entropy form with five cations that were equimolar and homogeneously distributed. The specific chemistries investigated were Al, Cr, Fe, and Ga with a fifth cation that was varied with increasing ionic radius (In, Er, Ho, Y, Eu, Ce, La). High-entropy dawsonites also exhibit the ″memory effects″ of non-high-entropy dawsonites. This work extends the field of high-entropy materials to include a structure that can serve as a material platform for the synthesis of high-entropy catalytic materials and ceramic powders.

3.
Membranes (Basel) ; 12(5)2022 Apr 27.
Artículo en Inglés | MEDLINE | ID: mdl-35629797

RESUMEN

Point-of-use ceramic filters are one of the strategies to address problems associated with waterborne diseases to remove harmful microorganisms in water sources prior to its consumption. In this study, development of adsorption-based ceramic depth filters composed of alumina platelets was achieved using spray granulation (calcined at 800 °C). Their virus retention performance was assessed using cartridges containing granular material (4 g) with two virus surrogates: MS2 and fr bacteriophages. Both materials showed complete removal, with a 7 log10 reduction value (LRV) of MS2 up to 1 L. MgAl2O4-modified Al2O3 granules possessed a higher MS2 retention capacity, contrary to the shortcomings of retention limits in pure Al2O3 granules. No significant decline in the retention of fr occurred during filtration tests up to 2 L. The phase composition and morphology of the materials were preserved during filtration, with no magnesium or aluminum leakage during filtration, as confirmed by X-ray diffractograms, electron micrographs, and inductively coupled plasma-optical emission spectrometry. The proposed MgAl2O4-modified Al2O3 granular ceramic filter materials offer high virus retention, achieving the criterion for virus filtration as required by the World Health Organization (LRV ≥ 4). Owing to their high thermal and chemical stability, the developed materials are thus suitable for thermal and chemical-free regeneration treatments.

4.
RSC Adv ; 12(40): 26362-26371, 2022 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-36275118

RESUMEN

High-entropy materials are compositionally complex materials which often contain five or more elements. The most commonly studied materials in this field are alloys and oxides, where their composition allows for tunable materials properties. High-entropy layered double hydroxides have been recently touted as the next focus for the field of high-entropy materials to expand into. However, most previous work on multi-cationic layered double hydroxides has focused on syntheses with 5 or less cations in the structure. To bridge this gap into high-entropy materials, this work explores the range and extent of different compositional combinations for high-entropy double layered hydroxides. Specifically, pure layered double hydroxides were synthesized with different combinations of 7 cations (Mg, Co, Cu, Zn, Ni, Al, Fe, Cr) as well as one combination of 8 cations by utilizing a hydrothermal synthesis method. Furthermore, magnetic properties of the 8-cation LDH were investigated.

5.
Nat Commun ; 13(1): 3753, 2022 07 07.
Artículo en Inglés | MEDLINE | ID: mdl-35798724

RESUMEN

The biomaterial with the highest known tensile strength is a unique composite of chitin and goethite (α-FeO(OH)) present in teeth from the Common Limpet (Patella vulgata). A biomimetic based on limpet tooth, with corresponding high-performance mechanical properties is highly desirable. Here we report on the replication of limpet tooth developmental processes ex vivo, where isolated limpet tissue and cells in culture generate new biomimetic structures. Transcriptomic analysis of each developmental stage of the radula, the organ from which limpet teeth originate, identifies sequential changes in expression of genes related to chitin and iron processing. We quantify iron and chitin metabolic processes in the radula and grow isolated radula cells in vitro. Bioinspired material can be developed with electrospun chitin mineralised by conditioned media from cultured radula cells. Our results inform molecular processes behind the generation of limpet tooth and establish a platform for development of a novel biomimetic with comparable properties.


Asunto(s)
Gastrópodos , Diente , Animales , Materiales Biocompatibles , Biomimética , Quitina/química , Hierro
6.
J Phys Condens Matter ; 31(22): 225402, 2019 Jun 05.
Artículo en Inglés | MEDLINE | ID: mdl-30794999

RESUMEN

To study the anomalous thermoelastic behavior of bcc V, Nb, Ta as well as fcc Pd and Pt a density functional theory (DFT) based model is used, which allows for the calculation of the elastic constant [Formula: see text] and [Formula: see text] as a function of temperature. Available experimental [Formula: see text] trends are correctly reproduced indicating that the electronic structure mechanisms enabling anomalous behavior are captured by the model. A DFT based correlative investigation between V, Nb, Ta, Pd and Pt with anomalous thermoelastic properties and Mo and Cu with ordinary behavior reveals a high density of states (DOS) at the Fermi level to be a necessary but not sufficient condition for an anomalous thermoelastic behavior. In addition, anomalous metals in contrast to ordinary metals reallocate electronic states in the vicinity of the Fermi level upon lattice distortion, causing an increase in bond strength as identified by crystal orbital Hamilton population (COHP) analysis. Hence, we have identified the combination of high DOS and electronic reallocation upon lattice distortion to be the physical origin for anomalous thermoelastic behavior in metals. The absence of an anomaly for [Formula: see text]-type distortion in V, Nb, Ta, Pd and Pt is suggested to be due to the less pronounced reallocation of states compared to [Formula: see text]-type distortion.

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