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1.
ACS Omega ; 7(50): 46915-46921, 2022 Dec 20.
Artículo en Inglés | MEDLINE | ID: mdl-36570301

RESUMEN

MgMn2O4 with a tetragonal spinel structure shows promise as a positive-electrode material in magnesium rechargeable batteries (MRBs), which have drawn considerable attention as post lithium-ion batteries. However, the material currently suffers from poor cycle performance. In this study, we attempt to improve the cycle performance of MgMn2O4 via the Zr modification of its particle surface. X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy demonstrate that the surface modification is successfully performed by immersing MgMn2O4 powder into a Zr-containing aqueous solution, followed by heat treatment. However, Zr segregation is observed at high Zr concentration. Furthermore, structural analyses using synchrotron X-rays indicate that the Zr modification has an influence on the bulk structure of the MgMn2O4 powder. The positive-electrode properties of the powders are investigated using discharge/charge cycle tests, which show that Zr modification can drastically improve the cycle performance and coulombic efficiency. These improvements are supposed to be due to suppression of an unexpected reaction by the Zr-surface modification and lower structural distortion after the modification. These findings clearly demonstrate the significant potential of surface modification as a method for obtaining high-performance MRBs.

2.
Sci Rep ; 12(1): 18097, 2022 Oct 27.
Artículo en Inglés | MEDLINE | ID: mdl-36302884

RESUMEN

In this work, we focus on Mg-Fe-O and Mg-Ni-O with Mg-rich compositions as positive-electrode materials for magnesium rechargeable batteries, and prepare them by a thermal decomposition of precipitates obtained by a solution method. It is indicated from X-ray diffraction patterns that the Mg-Fe-O and Mg-Ni-O samples have the spinel and rocksalt structures, respectively. X-ray absorption near edge structures indicate that Fe and Ni are trivalent and divalent, respectively, in the Mg-rich oxides. From charge/discharge cycle test, it is demonstrated that the Mg-Fe-O shows higher discharge capacity than the other and then has good cycle performance while keeping a discharge capacity over 100 mA h g-1. To gain deeper understanding on a relationship between the electrode properties and the crystal structure of the Mg-Fe-O, the crystal structure is investigated by a Rietveld refinement using a synchrotron X-ray diffraction profile and an analysis on total correlation functions. It is indicated from these studies that a vacant octahedral site in the spinel structure is partially occupied by the excess Mg in the synthesized sample. This structural feature might result in a stable charge/discharge cycle performance of the Mg-rich Mg-Fe-O.

3.
Inorg Chem ; 58(9): 5664-5670, 2019 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-30994342

RESUMEN

Research has recently been focused on high-performance next-generation batteries to replace secondary batteries due to capacity limitations and safety concerns. The Mg secondary battery is one candidate to realize high energy density storage batteries for practical applications. Ni and Co typically exhibit desirable electrochemical characteristics; therefore, we have attempted to synthesize new rock-salt compositions, Mg xNi yCo zO2 ( x + y + z ≤ 2.0), as cathode materials for Mg rechargeable batteries, and investigated their crystal structures and electrochemical characteristics. The materials were synthesized by the reverse coprecipitation method. Powder X-ray diffraction and transmission electron microscopy analyses showed the obtained samples were a single phase of the rock-salt structure with the space group Fm3̅ m. The vacancies at the metal sites were estimated by Rietveld analysis to determine the new chemical composition of Mg xNi yCo z□2- x- y- zO2 (0.41 < x < 0.64, 0.82 < y < 1.23, 0.24 < z < 0.61). Charge-discharge tests indicated the discharge characteristics varied according to the Mg composition and the Ni/Co ratio. The Co and Mg compositions were considered to facilitate the insertion/deinsertion of Mg2+. The present new material has the potential to be a superior cathode material for Mg secondary batteries by first-principles calculations.

4.
Nanoscale ; 11(10): 4523-4530, 2019 Mar 07.
Artículo en Inglés | MEDLINE | ID: mdl-30806403

RESUMEN

Oxide ion-conducting porous films were produced on a substrate by evaporation-induced self-assembly of rare earth-doped CeO2 (REDC) nanocubes 4-5 nm in size and subsequent mild calcination at 400 °C. Mesocrystalline structures comprising iso-oriented REDC nanocubes were formed by ordered assembly based on strict attachment of their {100} faces. Enhanced oxide-ion conductivities in a temperature range of 250-350 °C were observed on the mesocrystalline films consisting of Sm-doped CeO2 (SDC) nanocubes. The specific electrical properties of the mesocrystalline films are ascribed to improved surface-ion conduction due to a large specific surface area and a high crystallographic connectivity of SDC nanocubes.

5.
Chem Commun (Camb) ; 55(17): 2517-2520, 2019 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-30741273

RESUMEN

The atomic structure of a spinel-type MgCo2O4 nanoparticle was investigated by the reverse Monte Carlo modelling using X-ray and neutron total scattering data. It is found that Mg at an octahedral site induces a significant structural distortion, while Mg at a tetrahedral site is considered to move easily to a vacant site. Based on the results, we propose a guideline for the development of a better positive electrode material for a Mg rechargeable battery.

6.
J Org Chem ; 83(21): 13574-13579, 2018 Nov 02.
Artículo en Inglés | MEDLINE | ID: mdl-30351927

RESUMEN

The treatment of PdCl2 with K2CO3 and HCO2H in dioxane gives black precipitates, which are an effective catalyst for the semireduction of alkynes to alkenes using formic acid as a reductant. Even 0.05 mol % Pd promoted the reduction reaction of tolane in high yield with high selectivity.

7.
ACS Omega ; 3(1): 898-905, 2018 Jan 31.
Artículo en Inglés | MEDLINE | ID: mdl-31457936

RESUMEN

We report a simple room-temperature synthesis route for increasing the reactivity of a TiO2 photocatalyst using a solution plasma process (SPP). Hydrogen radicals generated from the SPP chamber interact with the TiO2 photocatalyst feedstock, transforming its crystalline phase and introducing oxygen vacancy defects. In this work, we examined a pure anatase TiO2 as a model feedstock because of its photocatalytic attributes and well-characterized properties. After the SPP treatment, the pure anatase crystalline phase was transformed to an anatase/brookite heterocrystalline phase with oxygen vacancies. Furthermore, the SPP treatment promoted the absorption of both UV and visible light by TiO2. As a result, TiO2 treated by the SPP for 3 h showed a high gaseous photocatalytic performance (91.1%) for acetaldehyde degradation to CO2 compared with the activity of untreated TiO2 (51%). The SPP-treated TiO2 was also more active than nitrogen-doped TiO2 driven by visible light (66%). The overall photocatalytic performance was related to the SPP treatment time. The SPP technique could be used to enhance the activity of readily available feedstocks with a short processing time. These results demonstrate the potential of this method for modifying narrow-band gap metal oxides, metal sulfides, and polymer composite-based catalyst materials. The modifications of these materials are not limited to photocatalysts and could be used in a wide range of energy and environment-based applications.

8.
ACS Omega ; 3(5): 5453-5458, 2018 May 31.
Artículo en Inglés | MEDLINE | ID: mdl-31458750

RESUMEN

Solid electrolytes with compositions of (100 - x)(0.75Li2S·0.25P2S5)·xLiBH4 (mol %, 0 ≤ x ≤ 100) were mechanochemically prepared from the 75Li2S·25P2S5 (mol %) glass and LiBH4 crystal. The samples with x ≥ 43 have crystalline phases and those with x ≤ 33 formed a glassy phase. The crystalline phase was identified as argyrodite Li6PS5(BH4). The x = 50 sample formed a crystalline phase and demonstrated a high lithium-ion conductivity of 1.8 × 10-3 S cm-1 at 25 °C with an activation energy of 16 kJ·mol-1. The argyrodite-type crystal with a BH4 - anion that occupies the halide site is a novel and promising solid electrolyte.

9.
J Biomed Mater Res A ; 65(3): 379-85, 2003 Jun 01.
Artículo en Inglés | MEDLINE | ID: mdl-12746885

RESUMEN

Three mannosylerythritol lipids (MEL-A, -B, and -C), yeast glycolipid biosurfactants, were independently attached to poly (2-hydroxyethyl methacrylate) beads (PHEMA), and the three obtained MEL-PHEMA composites were examined for their binding affinity to human immunoglobulin G (HIgG). Of the three composites, the composite bearing MEL-A exhibited the highest binding capacity for HIgG. The binding amount of HIgG increased with increased applied concentration, reaching 106 mg HIgG (per g of composite), with a binding yield of 81%. Interestingly, the protein binding to the composite appeared to follow two different modes (Langmuir type and Freundlich type) depending on the applied concentration. The binding amount of human serum albumin to the composite was much smaller than that of HIgG. The bound human serum albumin, however, had minimal effect on the subsequent binding of HIgG, indicating that the two proteins have different binding sites onto the composite. More significantly, the bound HIgG was efficiently recovered under significantly mild elution conditions: Approximately 90% of the protein was eluted from the composite with phosphate buffer at pH 7. These results indicate that the glycolipid biosurfactant may have great potential as an affinity ligand material for HIgG.


Asunto(s)
Glucolípidos/química , Inmunoglobulina G/química , Albúmina Sérica/química , Tensoactivos/química , Sitios de Unión , Humanos , Cinética , Ligandos , Conformación Molecular , Unión Proteica , Saccharomyces cerevisiae/química
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