T. Pedroso de Almeida
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12 records found
1
Intrinsic self-healing materials have received significant attention due to the characteristic recovery after damage properties through reversible dynamic covalent and non-covalent interactions. Furthermore, functional recovery with reliable mechanical properties are highly keen as protective coatings, specifically for devices and sensors vulnerable to abrasion in severe environments. Here, we present a functional hierarchical nanostructure capable of multiple micro-sized healings, with enhanced mechanical hardness due to the incorporation of graphene oxide (rGO) nanoplatelets. A self-healing multilayered nanocomposite formed by poly(ethylene imine) (PEI) and poly(acrylic acid) (PAA) was easily assembled by the layer-by-layer (LbL) technique. The addition of the rGO nanoplatelets in the LbL nanostructure resulted in a 13-fold increase in hardness (0.4 ± 0.1 GPa) when compared to the (PEI/PAA) architecture (0.03 ± 0.01 GPa). In addition, the nanocomposite presents an enhanced insulating electrical behavior (∼ 4.10−8 S/cm) despite the addition of the rGO nanoplatelets. Raman and Zeta Potential analysis indicated a possible wrapping of the rGOs by PEI, justifying the observed insulating electrical characteristics. The nanocomposite presents good hydrophobicity with a water contact angle of 136°, interesting to extend the lifetime and protect underlying layers from humidity, degradation, and encrustation. Therefore, we propose an attractive hydrophobic, electrically insulating, and mechanically resistant multifunctional coating for high-performance electronic interfaces from minor cuts and abrasions, dispensing maintainer intervention.
Various enzymes utilize hydrogen peroxide as an oxidant. Such “peroxizymes” are potentially very attractive catalysts for a broad range of oxidation reactions. Most peroxizymes, however, are inactivated by an excess of H2O2. The electrochemical reduction of oxygen can be used as an in situ generation method for hydrogen peroxide to drive the peroxizymes at high operational stabilities. Using conventional electrode materials, however, also necessitates significant overpotentials, thereby reducing the energy efficiency of these systems. This study concerns a method to coat a gas-diffusion electrode with oxidized carbon nanotubes (oCNTs), thereby greatly reducing the overpotential needed to perform an electroenzymatic halogenation reaction. In comparison to the unmodified electrode, with the oCNTs-modified electrode the overpotential can be reduced by approximately 100 mV at comparable product formation rates.
The selective oxidation of trans-2-hexen-1-ol to the corresponding aldehyde using a recombinant aryl alcohol oxidase from Pleurotus eryngii (PeAAOx) is reported. Especially using the two liquid phase system to overcome solubility and product inhibition issues enabled to achieve more than 2.200.000 catalytic turnovers for the production enzyme as well as molar product concentrations, pointing towards an economic feasible reaction.
The biocatalytic preparation of trans-hex-2-enal from trans-hex-2-enol using a novel aryl alcohol oxidase from Pleurotus eryngii (PeAAOx) is reported. As O2-dependent enzyme PeAAOx-dependent reactions are generally plagued by the poor solubility of O2 in aqueous media and mass transfer limitations resulting in poor reaction rates. These limitations were efficiently overcome by conducting the reaction in a flow-reactor setup reaching unpreceded catalytic activities for the enzyme in terms of turnover frequency (up to 38 s-1) and turnover numbers (more than 300000) pointing towards preparative usefulness of the proposed reaction scheme.
Microfluidic devices based on polydimethylsiloxane shown a plethora of experimental possibilities due to good transparency, flexibility and ability to adhere reversibly and irreversibly to distinct materials. Though PDMS is a milestone in microfluidic developments, its cost and handling directed the field to search for new options. 3D printing technology nowadays starts a revolution offering materials and possibilities that can contribute positively to current methodologies. Here we explored the fused deposition modeling 3D printing technique to obtain integrated, transparent and sealed microchannels made with polylactic acid, a cheap alternative material to set up microfluidic systems. Using a home-made 3D printer, devices could be assembled in a simplified process, enabling the integration of different materials such as paper, glass, wire and polymers within the microchannel. To demonstrate the efficacy of this approach, a 3D-printed electronic tongue sensor was built, enabling the distinction of basic tastes below the human threshold.
Graphene is a breakthrough 2D material due to its unique mechanical, electrical, and thermal properties, with considerable responsiveness in real applications. However, the coverage of large areas with pristine graphene is a challenge and graphene derivatives have been alternatively exploited to produce hybrid and composite materials that allow for new developments, considering also the handling of large areas using distinct methodologies. For electronic applications there is significant interest in the investigation of the electrical properties of graphene derivatives and related composites to determine whether the characteristic 2D charge transport of pristine graphene is preserved. Here, we report a systematic study of the charge transport mechanisms of reduced graphene oxide chemically functionalized with sodium polystyrene sulfonate (PSS), named as GPSS. GPSS was produced either as quantum dots (QDs) or nanoplatelets (NPLs), being further nanostructured with poly(diallyldimethylammonium chloride) through the layer-by-layer (LbL) assembly to produce graphene nanocomposites with molecular level control. Current-voltage (I-V) measurements indicated a meticulous growth of the LbL nanostructures onto gold interdigitated electrodes (IDEs), with a space-charge-limited current dominated by a Mott-variable range hopping mechanism. A 2D intra-planar conduction within the GPSS nanostructure was observed, which resulted in effective charge carrier mobility (μ) of 4.7 cm2 V-1 s-1 for the QDs and 34.7 cm2 V-1 s-1 for the NPLs. The LbL assemblies together with the dimension of the materials (QDs or NPLs) were favorably used for the fine tuning and control of the charge carrier mobility inside the LbL nanostructures. Such 2D charge conduction mechanism and high μ values inside an interlocked multilayered assembly containing graphene-based nanocomposites are of great interest for organic devices and functionalization of interfaces.