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Correlação entre difusão iônica e estrutura em fluoretos vítreos cristalinos.; Ionic diffusion and structure correlation for vitreous and crystalline fluorides.

Pulcinelli, Sandra Helena
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Tese de Doutorado Formato: application/pdf
Publicado em 26/03/1987 PT
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O estudo de propriedades de transporte das fases vítreas do sistema LixTh1-xF4-3x por RMN do 7Li e do 19F mostrou que tanto os ions Li+ quanto F- são condutores. O lítio é móvel para todas as temperaturas estudadas e atua como cátion modificador do retículo, enquanto que o flúor é condutor apenas acima de 373K. Por espectroscopia vibracional ficou evidenciada a variação do número de coordenação do Th (de 8,5 a 9,5) em função da composição. No sistema LixU1-xF4-3x verificou-se que o átomo de urânio assume coordenação 8, independentemente da composição. O paramagnetismo dos vidros de urânio, determinado por medidas magnéticas e de RPE, é devido ao paramagnetismo inerente ao átomo de urânio isolado impedindo o estudo destas amostras por RMN. A determinação da estrutura cristalina da fase Li3ThF7 utilizando difração de raios-X por monocristal mostrou que este material cristaliza-se no grupo espacial P4/ncc do sistema tetragonal; a=6,200(1)Å, c=12,937(2)Å, Z=4 moléculas/cela unitária. A estrutura é formada por camadas de poliedros (ThF9) ,com quatro vértices comuns no plano ab. Os átomos de lítio localizam-se entre estas cama das ligando os poliedros [ThF9) ao longo do eixo c. Há uma desordem dos átomos de lítio que ocupam os sítios 8f e 16g na proporção 1:3. O efeito quadrupolar observado por RMN do 7Li na fase cristalina...

Fenômenos de transporte em líquidos iônicos; Transport phenomena in ionic liquids

Monteiro, Marcelo José
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Tese de Doutorado Formato: application/pdf
Publicado em 03/09/2010 PT
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A procura por fontes de energia confiáveis para motores elétricos, levou a grande esforços de síntese de novos eletrólitos para uso em baterias de íon-Li, de modo a aliar eficiência e segurança. Líquidos iônicos têm sido largamente estudados para este propósito. Misturas do sal Li(CF3SO2)2N, LiTf2N, no líquido iônico (LI) formado pelo cátion 1-butil-2,3-dimetilimidazólio, BMMI, e o ânion (CF3SO2)2N-, bis(trifluorometanosulfonil)imideto, Tf2N, foram preparadas em diferentes concentrações. A adição do sal de lítio a este liquido iônico diminuiu a mobilidade de todas as espécies, especialmente o Li+. A condutividade estimada usando os dados de difusão (NMRPGSE), os dados da espectroscopia Raman e as simulações por Dinâmica Molecular sugerem a formação de agregados compostos por ânions Tf2N em torno do Li+, com os oxigênios do Tf2N direcionados para o cátion Li+. Estes agregados aumentam conforme aumenta a concentração de LiTf2N, contribuindo para a diminuição da condutividade. Para contornar este obstáculo, foram sintetizados líquidos iônicos contendo um átomo de oxigênio na estrutura do cátion, de modo a promover a competição com os oxigênios do Tf2N pelo cátion Li+, prevenindo Li+ de formar agregados de grande massa e melhorando sua difusividade. Os cations escolhidos foram o 1...

Síntese de filmes automontados de poli(o-metoxianilina) e nanopartículas de pentóxido de vanádio como cátodos em baterias de íon-lítio em líquido iônico; Self assembly of poly(o-methoxyaniline) and vanadium pentoxide nanoparticles as cathodes for lithium-ion batteries in ionic liquid

Nogueira, Filipe Braga
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Dissertação de Mestrado Formato: application/pdf
Publicado em 01/11/2012 PT
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O presente trabalho utilizou a técnica de automontagem camada-por-camada para produzir eletrodos híbridos de poli(o-metoxianilina) e nanopartículas de pentóxido de vanádio. Foram obtidos filmes acusticamente rígidos, homogêneos com relação à massa depositada e com crescimento linear com o número de bicamadas depositadas. A caracterização eletroquímica foi realizada por voltametria cíclica, onde esse filme apresentou alta capacidade de intercalação/desintercalação de íons lítio e de forma reversível. A capacidade eletroquímica desse filme foi então comparada com filmes automontados de poli(dialildimetilamônio)/V2O5 e polialilamina/V2O5. O filme de Poli(dialildimetilamônio) apresentou um crescimento irregular com dissolução das nanopartículas, o que resultou em uma capacidade eletroquímica extremamente inferior ao filme de poli(o-metoxianilina). O filme de polialilamina apresentou uma deposição mais eficiente de V2O5 que o filme de poli(o-metoxianilina), entretanto essa maior quantidade de pentóxido de vanádio não refletiu em um aumento da capacidade do eletrodo. Os resultados de espectroscopia de impedância eletroquímica mostram que o filme de polialilamina é significativamente mais resistivo que o filme de poli(o-metoxianilina). Essa diminuição da condutividade...

Estudos de difusão e trocas iônicas de vanádio, cromo, manganês e ferro no berilo incolor; Studies of diffusion and ionic exchanges of vanadium, chromium, manganese, and iron in colorless beryl

Mittani, Juan Carlos Ramírez
Fonte: Biblioteca Digitais de Teses e Dissertações da USP Publicador: Biblioteca Digitais de Teses e Dissertações da USP
Tipo: Tese de Doutorado Formato: application/pdf
Publicado em 05/12/2002 PT
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Neste trabalho a difusão de V, Cr, Mn e Fe por troca iônica, eletrodifusão e implante iônico foi efetuada na amostra natural de berilo incolor (goshenita). As medidas de termoluminescência (TL), ressonância spin paramagnética (EPR) e absorção ótica (AO) foram feitas na amostra natural com a finalidade de comparar as amostras apos a difusão em alguns casos a observação da variação das propriedades medidas. A amostra natural após a irradiação - delta com 10 Gy apresentou 3 picos TL a aproximadamente 150, 250 e 320ºC. Para altas doses o primeiro pico aumentou muito sua intensidade, sobrepondo-se sobre os outros dois picos de temperaturas altas. A amostra natural apresentou sinais EPR referentes aos íons Mn POT.2+ localizados na posição de Al POT.3+ e Fe POT.3+ no canal do cristal. As amostras irradiadas com altas doses de até 10 POT.6 Gy, além dos sinais mencionados, apresentaram novos sinais referentes ao CH IND.3, CO POT.-IND.3, H POT.GRAUS e Fe POT.3+. Este último íon, localizado em um ambiente tetraédrico, tem sinais na região de campos magnéticos baixos. As medidas de obsorção ótica na amostra natural apresentaram bandas muito intensas das moléculas de H IND.2O, situadas no canal, o que indica que os canais dessas amostras estão entupidos destas. A banda típica na região de 820 nm devido ao Fe POT.2+ no canal foi...

The electrochemical reduction of the purines guanine and adenine at platinum electrodes in several room temperature ionic liquids

Zanoni, Maria Valnice Boldrin; Rogers, Emma I.; Hardacre, Christopher; Compton, Richard G.
Fonte: Universidade Estadual Paulista Publicador: Universidade Estadual Paulista
Tipo: Artigo de Revista Científica Formato: 115-121
ENG
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The reduction of guanine was studied by microelectrode voltammetry in the room temperature ionic liquids (RTILs) N-hexyltriethylammonium bis (trifluoromethanesulfonyl) imide [N6,2,2,2][N(Tf)2], 1-butyl-3-methylimidazolium hexafluorosphosphate [C4mim][PF6], N-butyl-N-methyl-pyrrolidinium bis(trifluoromethanesulfonyl)imide [C4mpyrr][N(Tf)2], 1-butyl-3-methylimidazolium bis(trifluoromethanesulfonyl)imide [C4mim][N(Tf)2], N-butyl-N-methyl-pyrrolidinium dicyanamide [C4mpyrr][N(NC)2] and tris(P-hexyl)-tetradecylphosphonium trifluorotris(pentafluoroethyl)phosphate [P14,6,6,6][FAP] on a platinum microelectrode. In [N6,2,2,2][NTf2] and [P14,6,6,6][FAP], but not in the other ionic liquids studied, guanine reduction involves a one-electron, diffusion-controlled process at very negative potential to produce an unstable radical anion, which is thought to undergo a dimerization reaction, probably after proton abstraction from the cation of the ionic liquid. The rate of this subsequent reaction depends on the nature of the ionic liquid, and it is faster in the ionic liquid [P14,6,6,6][FAP], in which the formation of the resulting dimer can be voltammetrically monitored at less negative potentials than required for the reduction of the parent molecule. Adenine showed similar behaviour to guanine but the pyrimidines thymine and cytosine did not; thymine was not reduced at potentials less negative than required for solvent (RTIL) decomposition while only a poorly defined wave was seen for cytosine. The possibility for proton abstraction from the cation in [N6...

Caracterização de superfícies de vidros expostas a vapores de KNO3

Saggioro, Bruno Zaniboni
Fonte: Universidade Estadual Paulista (UNESP) Publicador: Universidade Estadual Paulista (UNESP)
Tipo: Dissertação de Mestrado Formato: xi, 128 f. : il., gráfs., tabs.
POR
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Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES); Fundação de Amparo à Pesquisa do Estado de São Paulo (FAPESP); Pós-graduação em Física - IGCE; Superfícies de vidro plano comercial (flotado) e de vidros sintetizados no laboratório com diferentes concentrações em massa de SnO2 foram expostos aos vapores resultantes da decomposição de KNO3 fundido a uma temperatura um pouco abaixo da temperatura de transição vítrea. Medidas de EDS mostram um aumento da concentração dos íons K+ na superfície com o aumento do tempo de exposição aos vapores. Alguns destes íons migraram para o interior dos vidros, conforme mostram as medidas do perfil de concentração. Os coeficientes de difusão foram determinados utilizando a técnica de Bolztzman-Matano. Esta mudança na concentração de K+ provocou modificações estruturais na superfície, alterando algumas de suas propriedades físico-químicas. Espectros de reflexão no infravermelho foram realizadas nestas amostras e mostraram que as alterações mais pronunciadas ocorreram na banda em tono de 950 cm-1. A dureza Vickers aumenta com o tempo de exposição. O índice de refração foi determinado pelos métodos de Brewster e refratometria Abbe. Constatou-se que quanto maior o tempo de exposição aos vapores...

Modelagem numerica da salinização da agua de formação e da migração secundaria de hidrocarbonetos na Bacia de Sergipe; Numerical modelling of formation water salinity and secondary migration of hydrocarbon in Sergipe Basin

Andre De Gasperi
Fonte: Biblioteca Digital da Unicamp Publicador: Biblioteca Digital da Unicamp
Tipo: Dissertação de Mestrado Formato: application/pdf
Publicado em 07/12/1999 PT
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Neste trabalho foram modelados numericamente a salinização da água de formação e a migração secundária e acumulação dos hidrocarbonetos que preenchem os reservatórios do Membro Carmópolis, da Formação Muribeca, na Bacia de Sergipe. O modelo geológico-geoquímico que serviu de base para a modelagem numérica da salinização foi reproduzido utilizando um simulador de difusão iônica construído para este fim. A simulação considerou a infiltração de água meteórica em porções localizadas nas bordas da bacia, a dissolução de sal da unidade sobreposta e a difusão iônica lateral, como os principais processos controladores da salinização da água de formação. A modelagem da migração secundária e acumulação de hidrocarbonetos na área foi realizada utilizando um simulador de escoamento comercial. A simulação exigiu duas fontes distintas de hidrocarbonetos, configurando duas rotas de migração. Este processo ocorreu inicialmente por migração vertical, através de zona de falha, seguido por deslocamento lateral focalizado, através das rochas carreadoras, até o óleo acumular nas estruturas ou escapar para superfície, nas bordas da bacia; In the present study, formation water salinity and secondary migration and accumulation of hydrocarbon in reservoir rocks of Carmópolis Member...

Supercritical fluid processing of natural based polymers doped with ionic liquids

Martins, M.; Craveiro, R.; Paiva, A.; Duarte, Ana Rita C.; Reis, R. L.
Fonte: Elsevier Publicador: Elsevier
Tipo: Artigo de Revista Científica
Publicado em /04/2014 ENG
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Some approaches have been developed in our group to investigate the role of ionic liquids as process and property modifiers of natural-based polymers. In our previous work, we proposed the use of ionic liquids as plasticizing agents for the creation of porous structures from a semi-crystalline natural-based polymer. The current work intended to complement the previous studies, evaluating the ability of ionic liquid (IL) to plasticize blends of starch with poly (lactic) acid, with different ratios of starch and PLA of 50:50 and 30:70, and its effect on supercritical fluid foaming process (SCF) and providing more insights on the mechanisms involved. For this purpose, SPLA blends were modified and processed using 1-butyl-3-methylimidazolium chloride ([bmim]Cl). Supercritical fluid foaming was studied at different soaking times (1, 3 and 6 h) using carbon dioxide at 20.0 MPa and 40 oC. The blends were characterized by different techniques, such as infra-red spectroscopy, differential scanning calorimetry and compression and tensile mechanical analysis. The morphology of the foamed structures was analyzed by scanning electron microscopy and micro-computed tomography. The results suggest that after 3h of soaking time an equilibrium state of carbon dioxide into the bulk samples is attained...

Ionic diffusion in voltage-clamped isolated cardiac myocytes. Implications for Na,K-pump studies.

Mogul, D J; Singer, D H; Ten Eick, R E
Fonte: PubMed Publicador: PubMed
Tipo: Artigo de Revista Científica
Publicado em /09/1989 EN
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The whole-cell voltage-clamp technique employing electrolyte-filled micro-pipette suction electrodes is widely used to investigate questions requiring an electrophysiological approach. With this technique, the ionic composition of the cytosol is assumed to be strongly influenced (as result of diffusion) by the ionic composition of the solution contained in the electrode. If this assumption is valid for isolated cardiac myocytes, the technique would be particularly powerful for studying the dependence of their Na,K-pump on the intracellular [Na+]. However, the relationship between the concentrations of ions in the solution filling the electrode and those in the cytosol has not been established. The relationship was investigated to determine in particular whether the [Na+] at the intracellular cation ligand binding sites for the Na-pump ([ Na+]ps) can be set and clamped by [Na+] in the pipette electrode ([ Na+]pip). If [Na+]pip can set and clamp [Na+]ps, this would provide a means for defining the dependence of the Na,K-pump on intracellular [Na+]. The relationship between [Na+]pip and [Na+]ps was analyzed using two approaches. First, a mathematical model of three-dimensional ionic diffusion within a whole-cell patch-clamped myocyte was developed and the effects of experimental parameters on mean [Na+]ps were investigated. When typical experimental values were simulated...

Ionic Conductances of Extracellular Shunt Pathway in Rabbit Ileum : Influence of shunt on transmural sodium transport and electrical potential differences

Frizzell, Raymond A.; Schultz, Stanley G.
Fonte: The Rockefeller University Press Publicador: The Rockefeller University Press
Tipo: Artigo de Revista Científica
Publicado em 01/03/1972 EN
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The unidirectional influxes of Na, K, and Cl into isolated strips of rabbit ileum are comprised of movements across the mucosal membrane of the epithelial cells and ionic diffusion into an extracellular shunt pathway. A large fraction of the Na influx across the mucosal membrane alone is inhibited by Li, suggesting the participation of a carrier mechanism in the influx process. The partial ionic shunt conductances of Na, K, and Cl account for at least 82% of the total tissue conductance. The calculated shunt permeabilities (P) are (in centimeters per hour) PK = 0.040, PNa = 0.035, and PCl = 0.019, so that PK:PNa:PCl = 1.14:1.00:0.55. Diffusion potentials across the tissue resulting from isotonic replacement of NaCl in the mucosal solution with mannitol or KCl are described by the Goldman constant-field equation together with the above permeabilities of the shunt pathway. These observations are not consistent with permeation through a fixed-charge pore but can be explained by a model featuring constant ionic partition into a neutral-polar pore that traverses the tight junction. Such a pore may be lined with either fixed dipoles or fixed dipolar ions oriented such that electronegative groups influence the permselective properties of the diffusion pathway. The essential feature of both models is that electroneutrality is maintained by means of fixed membrane components and does not depend upon the presence of mobile counterions.

Influence of the Electrolyte Film Thickness on Charge Dynamics of Ionic Liquids in Ionic Electroactive Devices

Lin, Junhong; Liu, Yang; Zhang, Q.M.
Fonte: PubMed Publicador: PubMed
Tipo: Artigo de Revista Científica
Publicado em 10/02/2012 EN
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Developing advanced ionic electroactive devices such as ionic actuators and supercapacitors requires the understanding of ionic diffusion and drifting processes, which depend on the distances over which the ions travel, in these systems. The charge dynamics of [C4mim][PF6] ionic liquid films and Aquivion membranes with 40 wt% [C2mim][TfO] were investigated over a broad film thickness (d) range. It was found that the double layer charging time τDL follows the classic model τDL = λDd/(2D) very well, where D is the diffusion coefficient and λD the Debye length. In the longer time regimes (t ≫ τDL) where diffusion dominates, the charge dynamics become voltage dependent. For low applied voltage, the later stage charge process seems to follow the d2 dependence. However, at high voltages (> 0.5 V) in which significant device responses occur, the charging process does not show d2 dependence so that τdiff = d2/(4D), corresponding to the ion diffusion from the bulk region, was not observed.

Fast Ionic Diffusion-Enabled Nanoflake Electrode by Spontaneous Electrochemical Pre-Intercalation for High-Performance Supercapacitor

Mai, Liqiang; Li, Han; Zhao, Yunlong; Xu, Lin; Xu, Xu; Luo, Yanzhu; Zhang, Zhengfei; Ke, Wang; Niu, Chaojiang; Zhang, Qingjie
Fonte: Nature Publishing Group Publicador: Nature Publishing Group
Tipo: Artigo de Revista Científica
Publicado em 24/04/2013 EN
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Layered intercalation compounds NaxMnO2 (x = 0.7 and 0.91) nanoflakes have been prepared directly through wet electrochemical process with Na+ ions intercalated into MnO2 interlayers spontaneously. The as-prepared NaxMnO2 nanoflake based supercapacitors exhibit faster ionic diffusion with enhanced redox peaks, tenfold-higher energy densities up to 110 Wh·kg−1 and higher capacitances over 1000 F·g−1 in aqueous sodium system compared with traditional MnO2 supercapacitors. Due to the free-standing electrode structure and suitable crystal structure, NaxMnO2 nanoflake electrodes also maintain outstanding electrochemical stability with capacitance retention up to 99.9% after 1000 cycles. Besides, pre-intercalation effect is further studied to explain this enhanced electrochemical performance. This study indicates that the suitable pre-intercalation is effective to improve the diffusion of electrolyte cations and other electrochemical performance for layered oxides, and suggests that the as-obtained nanoflakes are promising materials to achieve the hybridization of both high energy and power density for advanced supercapacitors.

Fast Ionic Diffusion-Enabled Nanoflake Electrode by Spontaneous Electrochemical Pre-Intercalation for High-Performance Supercapacitor

Mai, Liqiang; Li, Han; Zhao, Yunlong; Xu, Lin; Xu, Xu; Luo, Yanzhu; Zhang, Zhengfei; Ke, Wang; Niu, Chaojiang; Zhang, Qingjie
Fonte: Nature Publishing Group Publicador: Nature Publishing Group
Tipo: Artigo de Revista Científica
EN_US
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Layered intercalation compounds Na(_{x})MnO(_{2}) (x = 0.7 and 0.91) nanoflakes have been prepared directly through wet electrochemical process with Na(^{+}) ions intercalated into MnO(_{2}) interlayers spontaneously. The as-prepared Na(_{x})MnO(_{2}) nanoflake based supercapacitors exhibit faster ionic diffusion with enhanced redox peaks, tenfold-higher energy densities up to 110 Wh·kg(^{-1}) and higher capacitances over 1000 F·g(^{-1}) in aqueous sodium system compared with traditional MnO(_{2}) supercapacitors. Due to the free-standing electrode structure and suitable crystal structure, Na(_{x})MnO(_{2}) nanoflake electrodes also maintain outstanding electrochemical stability with capacitance retention up to 99.9% after 1000 cycles. Besides, pre-intercalation effect is further studied to explain this enhanced electrochemical performance. This study indicates that the suitable pre-intercalation is effective to improve the diffusion of electrolyte cations and other electrochemical performance for layered oxides, and suggests that the as-obtained nanoflakes are promising materials to achieve the hybridization of both high energy and power density for advanced supercapacitors.; Chemistry and Chemical Biology

Spherical N-carboxyethylchitosan/hydroxyapatite nanoparticles prepared by ionic diffusion process in a controlled manner

Zhu, A.; Lu, Y.; Zhou, Y.; Dai, S.
Fonte: Kluwer Academic Publ Publicador: Kluwer Academic Publ
Tipo: Artigo de Revista Científica
Publicado em //2010 EN
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The nanocomposites containing hydroxyapatite (HA) and biomacromolecules have attracted considerable research interest in implants, tissue scaffolds and drug controlled delivery. In this study, the N-carboxyethylchitosan/hydroxyapatite (NCECS/HA) nanoparticles were prepared by the ionic diffusion process in a controlled manner. The crystallization, particle size, size distribution and aggregation morphology of the NCECS/HA nanocomposites were dependent on the mole ratio of the glucosamine unit in NCECS to the Ca(2+). Fourier transform-infrared spectroscopic (FTIR) result indicated that there are chemical bonds formed between NCECS and HA. X-ray diffraction (XRD) analysis showed that the crystallization of HA in NCECS matrix was significantly retarded. Transmission electron microscopy (TEM) results revealed that NCECS/HA nanocomposites have the spherical morphology with the diameter ranging from 10 to 40 nm. The NCECS mineralization is driven by the self-assembly of NCECS and HA. These NCECS/HA nanocomposites have potential applications as the carrier for the controlled delivery of growth factors and drugs.; Aiping Zhu, Yan Lu, Yao Zhou, Sheng Dai

Quantifying diffusion in biofilms : from model hydrogels to living biofilms

Golmohamadi, Mahmood
Fonte: Université de Montréal Publicador: Université de Montréal
Tipo: Thèse ou Mémoire numérique / Electronic Thesis or Dissertation
EN
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Les biofilms sont des communautés de microorganismes incorporés dans une matrice exo-polymérique complexe. Ils sont reconnus pour jouer un rôle important comme barrière de diffusion dans les systèmes environnementaux et la santé humaine, donnant lieu à une résistance accrue aux antibiotiques et aux désinfectants. Comme le transfert de masse dans un biofilm est principalement dû à la diffusion moléculaire, il est primordial de comprendre les principaux paramètres influençant les flux de diffusion. Dans ce travail, nous avons étudié un biofilm de Pseudomonas fluorescens et deux hydrogels modèles (agarose et alginate) pour lesquels l’autodiffusion (mouvement Brownien) et les coefficients de diffusion mutuels ont été quantifiés. La spectroscopie par corrélation de fluorescence a été utilisée pour mesurer les coefficients d'autodiffusion dans une volume confocal de ca. 1 m3 dans les gels ou les biofilms, tandis que les mesures de diffusion mutuelle ont été faites par cellule de diffusion. En outre, la voltamétrie sur microélectrode a été utilisée pour évaluer le potentiel de Donnan des gels afin de déterminer son impact sur la diffusion. Pour l'hydrogel d'agarose, les observations combinées d'une diminution du coefficient d’autodiffusion et de l’augmentation de la diffusion mutuelle pour une force ionique décroissante ont été attribuées au potentiel de Donnan du gel. Des mesures de l'effet Donnan (différence de -30 mV entre des forces ioniques de 10-4 et 10-1 M) et l'accumulation correspondante d’ions dans l'hydrogel (augmentation d’un facteur de 13 par rapport à la solution) ont indiqué que les interactions électrostatiques peuvent fortement influencer le flux de diffusion de cations...

Non-ionic diffusion and carrier-mediated transport drive extracellullar pH regulation of mouse colonic crypts.

Chu, S; Montrose, M H
Fonte: PubMed Publicador: PubMed
Tipo: Artigo de Revista Científica
Publicado em 01/08/1996 EN
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1. Extracellular pH (pHo) regulation within mouse colonic crypt lumens is stimulated by transepithelial gradients of short-chain fatty acids (SCFAs). Current work assesses underlying mechanisms contributing to pHo regulation. 2. Crypt luminal alkalinization was saturable by apical SCFA (substrate concentration activating half-maximal transport (KT) of isobutyrate = 45 mM). However, saturation was consistent with either carrier-mediated SCFA flux or non-ionic diffusion, because the non-ionized form was titrated by luminal alkalinization. Direct acidification of apical perfusates increased the magnitude of SCFA-induced luminal alkalinization, roughly in the same proportion to the increased concentration of non-ionized SCFA in the crypt lumen. 3. Transepithelial gradients of an alternative weak acid (CO2) produce pHo changes similar to SCFA. In contrast, a weak base (NH3) changes pHo with reverse dependence on the orientation of the transepithelial gradient compared with SCFA. Results implicate non-ionic diffusion in pHo regulation, and suggest that pHo changes may underly SCFA-stimulated bicarbonate secretion and ammonium absorption. 4. SCFA metabolism plays a minor role in extracellular pH regulation. An avidly metabolized SCFA (N-butyrate) augments crypt luminal alkalinization only slightly (0.08 pH units) versus a poorly metabolized SCFA (isobutyrate). 5. Apical addition of 1 mM 4...

Oxygen diffusion pathways in brownmillerite SrCoO2.5: Influence of structure and chemical potential

Mitra, Chandrima; Meyer, Tricia; Lee, Ho Nyung; Reboredo, Fernando A.
Fonte: Universidade Cornell Publicador: Universidade Cornell
Tipo: Artigo de Revista Científica
Publicado em 29/08/2014
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To design and discover new materials for next-generation energy materials such as solid-oxide fuel cells (SOFCs), a fundamental understanding of their ionic properties and behaviors is essential. The potential applicability of a material for SOFCs is critically determined by the activation energy barrier of oxygen along various diffusion pathways. In this work, we investigate interstitial-oxygen (Oi) diffusion in brownmillerite oxide SrCoO2.5, employing a first-principles approach. Our calculations indicate highly anisotropic ionic diffusion pathways, which result from its anisotropic crystal structure. The one-dimensional-ordered oxygen vacancy channels are found to provide the easiest diffusion pathway with an activation energy barrier height of 0.62 eV. The directions perpendicular to the vacancy channels have higher energy barriers for Oint diffusion. In addition, we have studied migration barriers for oxygen vacancies that could be present as point defects within the material. This in turn could also facilitate the transport of oxygen. Interestingly, for oxygen vacancies, the lowest barrier height was found to occur within the octahedral layer with an energy of 0.82 eV. Our results imply that interstitial migration would be highly one-dimensional in nature. Oxygen vacancy transport...

NMR study of ion dynamics and charge storage in ionic liquid supercapacitors

Forse, Alexander C.; Griffin, John M.; Merlet, Celine; Bayley, Paul M.; Wang, Hao; Simon, Patrice; Grey, Clare P.
Fonte: ACS Publicador: ACS
Tipo: Article; published version
EN
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This is the final version. It first appeared at http://pubs.acs.org/doi/abs/10.1021/jacs.5b03958.; Ionic liquids are emerging as promising new electrolytes for supercapacitors. While their higher operating voltages allow the storage of more energy than organic electrolytes, they cannot currently compete in terms of power performance. More fundamental studies of the mechanism and dynamics of charge storage are required to facilitate the development and application of these materials. Here we demonstrate the application of nuclear magnetic resonance spectroscopy to study the structure and dynamics of ionic liquids confined in porous carbon electrodes. The measurements reveal that ionic liquids spontaneously wet the carbon micropores in the absence of any applied potential and that on application of a potential supercapacitor charging takes place by adsorption of counterions and desorption of co-ions from the pores. We find that adsorption and desorption of anions surprisingly plays a more dominant role than that of the cations. Having elucidated the charging mechanism, we go on to study the factors that affect the rate of ionic diffusion in the carbon micropores in an effort to understand supercapacitor charging dynamics. We show that the line shape of the resonance arising from adsorbed ions is a sensitive probe of their effective diffusion rate...

Molecular dynamics estimates of ion diffusion in model hydrophobic and KcsA potassium channels

Allen, Toby; Kuyucak, Serdar; Chung, Shin-Ho
Fonte: Elsevier Publicador: Elsevier
Tipo: Artigo de Revista Científica
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Molecular dynamics simulations are carried out to obtain estimates of diffusion coefficients of biologically important Na+, K+, Ca2+ and Cl- ions in hydrophobic cylindrical channels with varying radii and large reservoirs. Calculations for the cylindrical channels are compared to those for the KcsA potassium channel, for which the protein structure has recently been determined from X-ray diffraction experiments. Our results show that ion diffusion is maintained at reasonably high levels even within narrow channels, and does not support the very small diffusion coefficients used in some continuum models in order to fit experimental data. The present estimates of ion diffusion coefficients are useful in the calculation of channel conductance using the Poisson-Nernst-Planck theory, or Brownian dynamics.

Structural Aspects Related to Lithium Intercalation and Ionic Dynamics: Frequency Response Analysis of (Sn x,Ti1-x)O2 Based Systems

Bueno,Paulo R.; Bulhões,Luis O.S.
Fonte: Sociedade Portuguesa de Electroquímica Publicador: Sociedade Portuguesa de Electroquímica
Tipo: Artigo de Revista Científica Formato: text/html
Publicado em 01/01/2008 EN
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Diffusion models capable of describing the ionic diffusion inside host materials, e.g. oxides, during intercalation processes, have been reported in the literature. However, the majority of the models do not succeed in establishing a good correlation between diffusion and structural environment. What is frequently described is the influence of an addition solid state reaction. In this paper we discuss about such additional reaction and its influence on the diffusion. The responses were evaluated by means of impedance patterns analyzed in (Sn x,Ti1-x)O2 binary systems whose structural disorder control provides a way to evaluate how such structural disorder influences the global diffusion.