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1.
Phys Chem Chem Phys ; 25(42): 29127-29134, 2023 Nov 01.
Artículo en Inglés | MEDLINE | ID: mdl-37869878

RESUMEN

This work investigates how configurational entropy in oxides could affect proton conductivity. For this purpose, three samples of different elemental compositions are synthesized. Five, six and seven elements were introduced into the A-site of ANbO4, forming La1/5 Nd1/5 Sm1/5Gd1/5 Eu1/5NbO4, La1/6Nd1/6Sm1/6Gd1/6Eu1/6Ho1/6NbO4 and La1/7Nd1/7Sm1/7Gd1/7Eu1/7Ho1/7Er1/7NbO4, respectively. The high configuration disorder changes the local environment, which can have a notable effect on many properties, including proton transport, which is the focus of this work. The conductivity was measured in different atmospheres; dry and wet and in a different temperature range (600-800 °C) to compare the proton transport as well as study the effect of temperature. A homogenous single-phase monoclinic fergusonite was obtained for the three samples. Proton conductivity, measured by means of comparing the conductivity in dry and wet atmospheres, was observed in all samples. La1/5 Nd1/5 Sm1/5Gd1/5 Eu1/5NbO4 exhibited the highest conductivity, about 3.0 × 10-6 S cm-1 at 800 °C in the wet atmosphere, while in the dry atmosphere it was about 2.2 × 10-6 S cm-1 at the same temperature, which implies a modest proton conductivity in this class of materials.

2.
Materials (Basel) ; 14(9)2021 Apr 23.
Artículo en Inglés | MEDLINE | ID: mdl-33922744

RESUMEN

Sol-gel layers have been the subject of many studies in recent decades. However, very little information exists about layers in which carbon structures are developed in situ. Using the spin-coating method, we obtained thin iron-doped SiO2/C composite films. The results of Raman spectroscopy showed that our samples consisted of graphitic forms and polymers. The latter's contribution decreases with rising temperature. FTIR and EDS studies show changes in carbon distribution on top of the layer, depending on the sintering temperature. The samples sintered at 800 °C showed a significant increase in the contribution of carbon forms to the layer's surface. Therefore, high conductivity can be observed in this sample. The results of XPS spectroscopy showed that the contribution of sp3 hybridized carbon increases after etching. The total electrical conductivity, studied by a DC four-wire technique, increased with the temperature and showed almost linear characteristics with significant changes below 150 K. The reduced activation energy plot has a positive temperature coefficient, which is a characteristic property of the conductive polymers in a metallic regime of conductivity.

3.
ACS Omega ; 5(47): 30395-30404, 2020 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-33283087

RESUMEN

We have studied alkaline-earth-metal-doped Y3GaO6 as a new family of oxide-ion conductor. Solid solutions of Y3GaO6 and 2% -Ca2+-, -Sr2+-, and -Ba2+-doped Y3GaO6, i.e., Y(3-0.06)M0.06GaO6-δ (M = Ca2+, Sr2+, and Ba2+), were prepared via a conventional solid-state reaction route. X-ray Rietveld refined diffractograms of all the compositions showed the formation of an orthorhombic structure having the Cmc21 space group. Scanning electron microscopy (SEM) images revealed that the substitution of alkaline-earth metal ions promotes grain growth. Aliovalent doping of Ca2+, Sr2+, and Ba2+ enhanced the conductivity by increasing the oxygen vacancy concentration. However, among all of the studied dopants, 2% Ca2+-doped Y3GaO6 was found to be more effective in increasing the ionic conductivity as ionic radii mismatch is minimum for Y3+/Ca2+. The total conductivity of 2% Ca-doped Y3GaO6 composition calculated using the complex impedance plot was found to be ∼0.14 × 10-3 S cm-1 at 700 °C, which is comparable to many other reported solid electrolytes at the same temperature, making it a potential candidate for future electrolyte material for solid oxide fuel cells (SOFCs). Total electrical conductivity measurement as a function of oxygen partial pressure suggests dominating oxide-ion conduction in a wide range of oxygen partial pressure (ca. 10-20-10-4 atm). The oxygen-ion transport is attributed to the presence of oxygen vacancies that arise from doping and conducting oxide-ion layers of one, two-, or three-dimensional channels within the crystal structure. The oxide-ion migration pathways were analyzed by the bond valence site energy (BVSE)-based approach. Photoluminescence analysis, dilatometry, Fourier transform infrared (FTIR) spectroscopy, and scanning electron microscopy studies were also performed to verify the experimental findings.

4.
Materials (Basel) ; 13(4)2020 Feb 21.
Artículo en Inglés | MEDLINE | ID: mdl-32098087

RESUMEN

In this work, Fe-doped strontium titanate SrTi1-xFexO3-x/2-δ, for x = 0-1 (STFx), has been fabricated and studied. The structure and microstructure analysis showed that the Fe amount in SrTi1-xFexO3-x/2-δ has a great influence on the lattice parameter and microstructure, including the porosity and grain size. Oxygen nonstoichiometry studies performed by thermogravimetry at different atmospheres showed that the Fe-rich compositions (x > 0.3) exhibit higher oxygen vacancies concentration of the order of magnitude 1022-1023 cm-3. The proton uptake investigations have been done using thermogravimetry in wet conditions, and the results showed that the compositions with x < 0.5 exhibit hydrogenation redox reactions. Proton concentration at 400 °C depends on the Fe content and was estimated to be 1.0 × 10-2 mol/mol for SrTi0.9Fe0.1O2.95 and 1.8 × 10-5 mol/mol for SrTi0.5Fe0.5O2.75. Above 20 mol% of iron content, a significant drop of proton molar concentrations at 400 °C was observed. This is related to the stronger overlapping of Fe and O orbitals after reaching the percolation level of approximately 30 mol% of the iron in SrTi1-xFexO3-x/2-δ. The relation between the proton concentration and Fe dopant content has been discussed in relation to the B-site average electronegativity, oxygen nonstoichiometry, and electronic structure.

5.
Beilstein J Nanotechnol ; 8: 1094-1103, 2017.
Artículo en Inglés | MEDLINE | ID: mdl-28685110

RESUMEN

Graphene oxide was functionalized with simultaneous reduction to produce phosphonated reduced graphene oxide in a novel, fully scalable, one-pot method. The phosphonic derivative of graphene was obtained through the reaction of graphene oxide with phosphorus trichloride in water. The newly synthesized reduced graphene oxide derivative was fully characterized by using spectroscopic methods along with thermal analysis. The morphology of the samples was examined by electron microscopy. The electrical studies revealed that the functionalized graphene derivative behaves in a way similar to chemically or thermally reduced graphene oxide, with an activation energy of 0.014 eV.

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