Interfacial electron transfer (ET) of biological macromolecules such as metalloproteins is the key process in bioelectrochemistry, enzymatic electrocatalysis, artificial ET chains, single-molecule electronic amplification and rectification, and other phenomena associated with the area of bioelectronics. A key challenge in molecular bioelectronics is to improve the efficiency of long-range charge transfer. The present work shows that this can be achieved by nanoparticle (NP) assisted assembly of cytochrome c (cyt c) on macroscopic single-crystalline electrode surfaces. We present the synthesis and characterization of water-soluble gold nanoparticles (AuNPs) with core diameter 3−4 nm and their application for the enhancement of long-range interfacial ET of a heme protein. Gold nanoparticles were electrostatically conjugated with cyt c to form nanoparticle−protein hybrid ET systems with well-defined stoichiometry. The systems were investigated in homogeneous solution and at liquid/solid interface. Conjugation of cyt c results in a small but consistent broadening of the nanoparticle plasmon band. This phenomenon can be explained in terms of long-range electronic interactions between the gold nanoparticle and the protein molecule. When the nanoparticle−protein conjugates are assembled on Au(111) surfaces, long-range interfacial ET across a physical distance of over 50 Å via the nanoparticle becomes feasible. Moreover, significant enhancement of the interfacial ET rate by more than an order of magnitude compared with that of cyt c in the absence of AuNPs is observed. AuNPs appear to serve as excellent ET relays, most likely by facilitating the electronic coupling between the protein redox center and the electrode surface.
The objective of this study was to evaluate the protective effects of five different emulsifiers on lipid oxidation in 70% fish oil-in-water emulsions to be used as delivery systems for long chain polyunsaturated omega-3 fatty acids to foods. The emulsifiers were either phospholipid (PL) based or protein based. The PL-based emulsifiers were soy lecithin and two milk PL concentrates (with either 20 or 75% PL). The protein-based emulsifiers were whey protein isolate and sodium caseinate. Lipid oxidation was studied at two pH values (pH 4.5 and 7.0) and results were compared to lipid oxidation in neat fish oil. Lipid oxidation was followed by determination of peroxide values and volatile oxidation products. Emulsions were furthermore imaged by confocal and cryo-scanning electron microscopy. Results showed that emulsions prepared at high pH with proteins oxidized less than or equally to neat oil, whereas, all other emulsions oxidized more. In addition, there was a tendency toward a faster progression in lipid oxidation at low pH compared to high pH for emulsions prepared with protein-based emulsifiers. The opposite was observed for emulsions prepared with PL-based emulsifiers. Hence, at low pH PL-based emulsions may be more suitable as delivery systems than protein-based emulsions. Moreover, the quality of the PLbased emulsifiers seemed to affect lipid oxidation. Practical applications:Results from the present study give an insight into the physical and oxidative stability of 70% fish oil-in-water emulsions prepared with whey protein isolate, sodium caseinate, milk phospholipids, or soy lecithin. The emulsions can be used as delivery systems for fish oil to foods. However, only emulsions prepared with proteins at high pH offered advantages with respect to better oxidative stability during storage compared to neat fish oil. Thus, when fish oil is added to a food product in a delivery emulsion, the type of emulsion used should be carefully considered.
This work addresses dimensional measurements performed with the scanning electron microscope (SEM) using 3D reconstruction of surface topography through stereo-photogrammetry. The paper presents both theoretical and experimental investigations, on the effects of instrumental variables and measurement parameters on reconstruction accuracy. Investigations were performed on a novel sample, specifically developed and implemented for the tests. The description is based on the model function introduced by Piazzesi and adapted for eucentrically tilted stereopairs. Two main classes of influencing factors are recognized: the first one is related to the measurement operation and the instrument set-up; the second concerns the quality of scanned images and represents the major criticality in the application of SEMs for 3D characterizations.
We present repeated structural and electrical measurements on individual multiwalled carbon nanotubes, alternating between electrical measurements under ambient conditions and transmission electron microscopy (TEM). The multiwalled carbon nanotubes made by chemical vapor deposition were manipulated onto cantilever electrodes extending from a specially designed microfabricated chip. Repeated TEM investigations were then made of the progressive destruction of the nanotube structure induced by Joule heating in air. The electrical measurements indicate that the studied nanotubes behave as diffusive conductors with remarkably predictable electrical properties despite extensive structural damage.
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