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1.
J Mater Chem B ; 12(10): 2494-2504, 2024 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-38170794

RESUMO

At the time when pathogens are developing robust resistance to antibiotics, the demand for implant surfaces with microbe-killing capabilities has significantly risen. To achieve this goal, profound understanding of the underlying mechanisms is crucial. Our study demonstrates that graphene oxide (GO) nano films deposited on stainless steel (SS316L) exhibit superior antibacterial features. The physicochemical properties of GO itself play a pivotal role in influencing biological events and their diversity may account for the contradictory results reported elsewhere. However, essential properties of GO coatings, such as oxygen content and the resulting electrical conductivity, have been overlooked so far. We hypothesize that the surface potential and electrical resistance of the oxygen content in the GO-nano films may induce bacteria-killing events on conductive metallic substrates. In our study, the GO applied contains 52 wt% of oxygen, and thus exhibits insulating properties. When deposited as a nano film on an electrically conducting steel substrate, GO flakes generate a Schottky barrier at the interface. This barrier, consequently, impedes the transfer of electrons to the underlying conductive substrate. As a result, this creates reactive oxygen species (ROS), leading to bacterial death. We confirmed the presence of GO coatings and their hydrolytic stability by using X-ray photoelectron spectroscopy (XPS), µRaman spectroscopy, scanning electron microscopy (SEM), and Kelvin probe force microscopy (KPFM) measurements. The biological evaluation was performed on the MG63 osteoblast-like cell line and two selected bacteria species: S. aureus and P. aeruginosa, demonstrating both the cytocompatibility and antibacterial behavior of GO-coated SS316L substrates. We propose a two-step bactericidal mechanism: electron transfer from the bacteria membrane to the substrate, followed by ROS generation. This mechanism finds support in changes observed in contact angle, surface potential, and work function, identified as decisive factors. By addressing overlooked factors and effectively bridging the gap between understanding and practicality, we present a transformative approach for implant surfaces, combating microbial resistance, and offering new application possibilitie.


Assuntos
Antibacterianos , Grafite , Staphylococcus aureus , Espécies Reativas de Oxigênio/metabolismo , Antibacterianos/farmacologia , Antibacterianos/química , Metais/farmacologia , Oxigênio/farmacologia
2.
Membranes (Basel) ; 13(5)2023 Apr 29.
Artigo em Inglês | MEDLINE | ID: mdl-37233543

RESUMO

Dual-phase membranes are increasingly attracting attention as a solution for developing stable oxygen permeation membranes. Ce0.8Gd0.2O2-δ-Fe3-xCoxO4 (CGO-F(3-x)CxO) composites are one group of promising candidates. This study aims to understand the effect of the Fe/Co-ratio, i.e., x = 0, 1, 2, and 3 in Fe3-xCoxO4, on microstructure evolution and performance of the composite. The samples were prepared using the solid-state reactive sintering method (SSRS) to induce phase interactions, which determines the final composite microstructure. The Fe/Co ratio in the spinel structure was found to be a crucial factor in determining phase evolution, microstructure, and permeation of the material. Microstructure analysis showed that all iron-free composites had a dual-phase structure after sintering. In contrast, iron-containing composites formed additional phases with a spinel or garnet structure which likely contributed to electronic conductivity. The presence of both cations resulted in better performance than that of pure iron or cobalt oxides. This demonstrated that both types of cations were necessary to form a composite structure, which then allowed sufficient percolation of robust electronic and ionic conducting pathways. The maximum oxygen flux is jO2 = 0.16 and 0.11 mL/cm2·s at 1000 °C and 850 °C, respectively, of the 85CGO-FC2O composite, which is comparable oxygen permeation flux reported previously.

3.
Nano Lett ; 23(7): 2945-2951, 2023 Apr 12.
Artigo em Inglês | MEDLINE | ID: mdl-36972518

RESUMO

Utilizing advanced transmission electron microscopy (TEM), the structure at the (110)-type twin boundary (TB) of Ce-doped GdFeO3 (C-GFO) has been investigated with picometer precision. Such a TB is promising to generate local ferroelectricity within a paraelectric system, while precise knowledge about its structure is still largely missing. In this work, a direct measurement of the cation off-centering with respect to the neighboring oxygen is enabled by integrated differential phase contrast (iDPC) imaging, and up to 30 pm Gd off-centering is highly localized at the TB. Further electron energy loss spectroscopy (EELS) analysis demonstrates a slight accumulation of oxygen vacancies at the TB, a self-balanced behavior of Ce at the Gd sites, and a mixed occupation of Fe2+ and Fe3+ at the Fe sites. Our results provide an informative picture with atomic details at the TB of C-GFO, which is indispensable to further push the potential of grain boundary engineering.

4.
J Biomed Mater Res A ; 111(9): 1322-1332, 2023 09.
Artigo em Inglês | MEDLINE | ID: mdl-36924189

RESUMO

Hemocompatibility is the most significant criterion for blood-contacting materials in successful in vivo applications. Prior to the clinical tests, in vitro analyses must be performed on the biomaterial surfaces in accordance with the ISO 10993-4 standards. Designing a bio-functional material requires engineering the surface structure and chemistry, which significantly influence the blood cell activity according to earlier studies. In this study, we elucidate the role of surface terminations and polymorphs of SiC single crystals in the initial stage of the contact coagulation. We present a detailed analysis of phase, roughness, surface potential, wettability, consequently, reveal their effect on cytotoxicity and hemocompatibility by employing live/dead stainings, live cell imaging, ELISA and Micro BCA protein assay. Our results showed that the surface potential and the wettability strongly depend on the crystallographic polymorph as well as the surface termination. We show, for the first time, the key role of SiC surface termination on platelet activation. This dependency is in good agreement with the results of our in vitro analysis and points out the prominence of cellular anisotropy. We anticipate that our experimental findings bridge the surface properties to the cellular activities, and therefore, pave the way for tailoring advanced hemocompatible surfaces.


Assuntos
Coagulação Sanguínea , Ativação Plaquetária , Materiais Biocompatíveis/química , Molhabilidade , Propriedades de Superfície , Teste de Materiais , Adesividade Plaquetária
5.
ACS Appl Mater Interfaces ; 13(29): 34227-34237, 2021 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-34264641

RESUMO

Lithium metal batteries are gaining increasing attention due to their potential for significantly higher theoretical energy density than conventional lithium ion batteries. Here, we present a novel mechanochemical modification method for lithium metal anodes, involving roll-pressing the lithium metal foil in contact with ionic liquid-based solutions, enabling the formation of an artificial solid electrolyte interphase with favorable properties such as an improved lithium ion transport and, most importantly, the suppression of dendrite growth, allowing homogeneous electrodeposition/-dissolution using conventional and highly conductive room temperature alkyl carbonate-based electrolytes. As a result, stable cycling in symmetrical Li∥Li cells is achieved even at a high current density of 10 mA cm-2. Furthermore, the rate capability and the capacity retention in NMC∥Li cells are significantly improved.

6.
Beilstein J Nanotechnol ; 12: 1380-1391, 2021.
Artigo em Inglês | MEDLINE | ID: mdl-34987951

RESUMO

In this study, a dual phase composite (CSO-FC2O) consisting of 60 vol % Ce0.8Sm0.2O1.9 as oxygen-conductive phase and 40 vol % FeCo2O4 as electron-conductive phase was synthesized. TEM measurements showed a relatively pure dual-phase material with only minor amounts of a tertiary (Sm,Ce)(Fe,Co)O3 perovskite phase and isolated residues of a rock salt phase at the grain boundaries. The obtained material was used as a model to demonstrate that a combination of polarization relaxation measurements and Kelvin probe force microscopy (KPFM)-based mapping of the Volta potential before and after the end of polarization can be used to determine the chemical diffusion coefficient of the ceria component of the composite. The KPFM measurements were performed at room temperature and show diffusion coefficients in the range of 3 × 10-13 cm2·s-1, which is comparable to values measured for single-phase Gd-doped ceria thin films using the same method.

7.
ACS Appl Mater Interfaces ; 9(31): 26219-26225, 2017 Aug 09.
Artigo em Inglês | MEDLINE | ID: mdl-28708371

RESUMO

The increasing threat of multidrug-resistance organisms is a cause for worldwide concern. Progressively microorganisms become resistant to commonly used antibiotics, which are a healthcare challenge. Thus, the discovery of new antimicrobial agents or new mechanisms different from those used is necessary. Here, we report an effective and selective antimicrobial activity of microstructured ZnO (Ms-ZnO) agent through the design of a novel star-shaped morphology, resulting in modulation of surface charge orientation. Specifically, we find that Ms-ZnO particles are composed of platelet stacked structure, which generates multiple Schottky barriers due to the misalignment of crystallographic orientations. We also demonstrated that this effect allows negative charge accumulation in localized regions of the structure to act as "charged domain walls", thereby improving the antimicrobial effectiveness by electric discharging effect. We use a combination of field emission scanning electron microscopy (FE-SEM), SEM-cathodoluminescence imaging, and Kelvin probe force microscopy (KPFM) to determine that the antimicrobial activity is a result of microbial membrane physical damage caused by direct contact with the Ms-ZnO agent. It is important to point out that Ms-ZnO does not use the photocatalysis or the Zn2+ released as the main antimicrobial mechanism, so consequently this material would show low toxicity and robust stability. This approach opens new possibilities to understand both the physical interactions role as main antimicrobial mechanisms and insight into the coupled role of hierarchical morphologies and surface functionality on the antimicrobial activity.

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