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Inorg Chem ; 2020 Aug 07.
Artigo em Inglês | MEDLINE | ID: mdl-32806009


The potential of the perovskite system Nd1-xSrxCoO3-δ (x = 1/3 and 2/3) as cathode material for solid oxide fuel cells (SOFCs) has been investigated via detailed structural, electrical, and electrochemical characterization. The average structure of x = 1/3 is orthorhombic with a complex microstructure consisting of intergrown, adjacent, perpendicularly oriented domains. This orthorhombic symmetry remains throughout the temperature range 373-1073 K, as observed by neutron powder diffraction. A higher Sr content of x = 2/3 leads to stabilization of the cubic perovskite with a homogeneous microstructure and with a higher oxygen vacancy content and cobalt oxidation state than the orthorhombic phase at SOFC operation temperature. Both materials are p-type electronic conductors with high total conductivities of 690 and 1675 S·cm-1 at 473 K in air for x = 1/3 and 2/3, respectively. Under working conditions, both compounds exhibit similar electronic conductivities, since x = 2/3 loses more oxygen on heating than x = 1/3, associated with a greater loss of p-type charger carriers. However, composite cathodes prepared with Nd1/3Sr2/3CoO3-δ and Ce0.8Gd0.2O2-δ present lower ASR values (0.10 Ω·cm2 at 973 K in air) than composites prepared with Nd2/3Sr1/3CoO3-δ and Ce0.8Gd0.2O2-δ (0.34 Ω·cm2). The high activity for the oxygen electrochemical reaction at intermediate temperatures is likely attributable to a large disordered oxygen-vacancy concentration, resulting in a very promising SOFC cathode for real devices.

Nanomaterials (Basel) ; 9(10)2019 Sep 24.
Artigo em Inglês | MEDLINE | ID: mdl-31554306


The zeolitic imidazolate framework-8 (ZIF-8) combines a significantly high microporosity with an excellent thermal, chemical, and hydrothermal stability. Here, we demonstrated that ZIF-8 can display significant levels of protonic conductivity through a water-mediated surface transport mechanism associated to the presence of di-coordinated Zn ions revealed by X-ray photoelectron spectroscopy. A set of powders with particle sizes from 2.8 µm down to 80 nm studied by dynamic water vapour sorption analysis was used to demonstrate that water adsorbs predominantly in the micropore cavities of microcrystalline ZIF-8, whereas adsorption on the external surface becomes the dominant contribution for the nanostructured material. Impedance spectroscopy in turn revealed that the protonic conductivity of the nanocrystalline ZIF-8 was two orders of magnitude higher than that of the micron-sized powders, reaching approximately 0.5 mS·cm-1 at 94 °C and 98% relative humidity. Simple relations were derived in order to estimate the potential gains in water uptake and conductivity as a function of the particle size. This new strategy combining particle nanostructuring with surface defects, demonstrated here for one of the most know metal organic framework, is of general application to potentially boost the conductivity of other materials avoiding chemical functionalization strategies that in most if not all cases compromise their chemical stability, particularly under high humidity and high temperature conditions.

ChemSusChem ; 10(14): 2978-2989, 2017 07 21.
Artigo em Inglês | MEDLINE | ID: mdl-28594114


The perovskite series Sr2 CoNb1-x Tix O6-δ (0≤x≤1) was investigated in the full compositional range to assess its potential as cathode material for solid oxide fuel cell (SOFC). The variation of transport properties and thus, the area specific resistances (ASR) are explained by a detailed investigation of the defect chemistry. Increasing the titanium content from x=0-1 produces both oxidation of Co3+ to Co4+ (from 0 up to 40 %) and oxygen vacancies (from 6.0 to 5.7 oxygen atom/formula unit), although each charge compensation mechanism predominates in different compositional ranges. Neutron diffraction reveals that samples with high Ti-contents lose a significant amount of oxygen upon heating above 600 K. Oxygen is partially recovered upon cooling as the oxygen release and uptake show noticeably different kinetics. The complex defect chemistry of these compounds, together with the compositional changes upon heating/cooling cycles and atmospheres, produce a complicated behavior of electrical conductivity. Cathodes containing Sr2 CoTiO6-δ display low ASR values, 0,13â€…Ω cm2 at 973 K, comparable to those of the best compounds reported so far, being a very promising cathode material for SOFC.

Condutividade Elétrica , Fontes de Energia Elétrica , Óxidos/química , Eletrodos , Oxigênio/química , Pressão , Temperatura
Dalton Trans ; 44(23): 10867-74, 2015 Jun 21.
Artigo em Inglês | MEDLINE | ID: mdl-25881558


Layered-type ordering and oxygen vacancies ordering are revealed in GdBaMnFeO(6-δ) perovskite. Selected area electron diffraction and high-resolution transmission electron microscopy results indicate a modulation of the crystal structure. Ba and Gd ordering in (001)(p) layers is confirmed by high angle annular dark field scanning transmission electron microscopy and electron energy-loss spectroscopy. These techniques also revealed formation of layer-stacking defects in the crystals. Direct imaging of the oxygen sublattice is obtained by phase image reconstruction. Location of the oxygen vacancies in the (GdO)(x) layers is achieved by analysis of the intensity of the averaged phase image. Physical properties of the GdBaMnFeO(6-δ) perovskite, are likely to be strongly affected by its ordering effects and crystal microstructure. In this sense, layered-type GdBaMnFeO(6-δ) perovskite show better electrochemical properties as cathodes in SOFCs than ion disordered Gd(0.5)Ba(0.5)Mn(0.5)Fe(0.5)O(3-δ) perovskite.