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Adsorption Dynamics of Redox Active Species onto Polarized Surfaces of Sensitized NiO.

ABSTRACT: Mesoporous NiO films were deposited by means of a screen printing technique onto fluorine-doped tin oxide transparent electrodes and consequently sensitized with Erythrosin B (EryB) dye. The obtained colored NiO material was used as a working electrode in a three-electrode cell to study the evolution of the triple semiconductor/dye/electrolyte interface upon electrochemical polarization in dark conditions. The electrolyte was a solution of I3 -/I- in acetonitrile, with the redox couple representing the typical redox shuttle of dye-sensitized solar cells (DSCs). The adopted electrochemical conditions were devised in order to simulate the actual electrical environment of the NiO/dye photocathode in a light-soaked DSC. The use of a benchmark sensitizer EryB and of the most widely used redox mediator I3 -/I- is particularly meaningful for the study of the adsorption dynamics and the determination of possible degradative phenomena on the basis of the behavior of numerous analogue systems. Therefore, for the first time, the evolution of the NiO/EryB/I3 -/I- multiple interface was investigated combining the electrochemical characterization with ex situ spectroscopic analysis by means of X-ray photoelectron spectroscopy. The resulting picture shows that EryB in the immobilized state promotes the redox processes based on the I3 -/I- couple. Moreover, the EryB sensitizer inhibits the phenomena of recombination between the metal oxide semiconductor and the redox couple.

SUBMITTER: Marrani AG

PROVIDER: S-EPMC6648089 | biostudies-literature | 2019 Jan

REPOSITORIES: biostudies-literature

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Adsorption Dynamics of Redox Active Species onto Polarized Surfaces of Sensitized NiO.

Marrani Andrea G AG Bonomo Matteo M Dini Danilo D

ACS omega 20190118 1

Mesoporous NiO films were deposited by means of a screen printing technique onto fluorine-doped tin oxide transparent electrodes and consequently sensitized with Erythrosin B (EryB) dye. The obtained colored NiO material was used as a working electrode in a three-electrode cell to study the evolution of the triple semiconductor/dye/electrolyte interface upon electrochemical polarization in dark conditions. The electrolyte was a solution of I3 -/I- in acetonitrile ...[more]

PMID: 31459425

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Project description:Silicon (Si) is suggested to be an important/essential nutrient for bone and connective tissue health. Silicon-substituted hydroxyapatite (Si-HA) has silicate ions incorporated into its lattice structure and was developed to improve attachment to bone and increase new bone formation. Here we investigated the direct adsorption of silicate species onto an HA coated surface as a cost effective method of incorporating silicon on to HA surfaces for improved implant osseointegration, and determined changes in surface characteristics and osteoblast cell adhesion. Plasma-sprayed HA-coated stainless steel discs were incubated in silica dispersions of different concentrations (0-42 mM Si), at neutral pH for 12 h. Adsorbed Si was confirmed by XPS analysis and quantified by ICP-OES analysis following release from the HA surface. Changes in surface characteristics were determined by AFM and measurement of surface wettability. Osteoblast cell adhesion was determined by vinculin plaque staining. Maximum Si adsorption to the HA coated disc occurred after incubation in the 6 mM silica dispersion and decreased progressively with higher silica concentrations, while no adsorption was observed with dispersions below 6 mM Si. Comparison of the Si dispersions that produced the highest and lowest Si adsorption to the HA surface, by TEM-based analysis, revealed an abundance of small amorphous nanosilica species (NSP) of ~1.5 nm in diameter in the 6 mM Si dispersion, with much fewer and larger NSP in the 42 mM Si dispersions. 29Si-NMR confirmed that the NSPs in the 6 mM silica dispersion were polymeric and similar in composition to the larger NSPs in the 42 mM Si dispersion, suggesting that the latter were aggregates of the former. Amorphous NSP adsorbed from the 6 mM dispersion on to a HA-coated disc surface increased the surface's water contact angle by 53°, whereas that adsorbed from the 42 mM dispersion decreased the contact angle by 18°, indicating increased and decreased hydrophobicity, respectively. AFM showed an increase in surface roughness of the 6 mM Si treated surface, which correlated well with an increase in number of vinculin plaques. These findings suggest that NSP of the right size (relative to charge) adsorb readily to the HA surface, changing the surface characteristics and, thus, improving osteoblast cell adhesion. This treatment provides a simple way to modify plasma-coated HA surfaces that may enable improved osseointegration of bone implants.

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Adsorption Dynamics of Redox Active Species onto Polarized Surfaces of Sensitized NiO.

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Adsorption Dynamics of Redox Active Species onto Polarized Surfaces of Sensitized NiO.

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