Due to the high surface: volume ratio and the extraordinary properties arising from the nanoscale (optical, electric, magnetic, etc.), nanoparticles (NPs) are excellent candidates for multiple applications. In this context, nanoscience is opening a wide range of modern technologies in biological and biomedical fields, among others. However, one of the main drawbacks that still delays its fast evolution and effectiveness is related to the behavior of nanomaterials in the presence of biological fluids. Unfortunately, biological fluids are characterized by high ionic strengths which usually induce NP aggregation. Besides this problem, the high content in biomacromolecules—such as lipids, sugars, nucleic acids and, especially, proteins—also affects NP stability and its viability for some applications due to, for example, the formation of the protein corona around the NPs. Here, we will review the most common strategies to achieve stable NPs dispersions in high ionic strength fluids and, also, antifouling strategies to avoid the protein adsorption.
We report on the effect of using decanoic acid as capping ligand on the synthesis of iron oxide nanoparticles by thermal decomposition of an organic iron precursor in organic medium. This procedure allowed us to control the particle size within 5 nm and about 30 nm by modifying the precursor-to-capping ligand ratio in a systematic fashion and to further expand the particle size range up to about 50 nm by adjusting the final synthesis temperature. The nanoparticles also showed high saturation magnetization of about 80-83 emu/g at low temperature, almost size-independent and close to the value for the bulk counterpart. Decanoic acid-coated nanoparticles were transferred to water by using tetramethylammonium hydroxide, which allowed further coating with silica in a tetraethyl orthosilicate solution. Consequently, these iron oxide nanoparticles are tunable in size and highly magnetic, and they could become suitable candidates for various biomedical applications such as contrast agents for magnetic resonance imaging and magnetic carriers for drug delivery.
The properties of magnetic nanoparticles tend to be depressed by the unavoidable presence of a magnetically inactive surface layer. However, outstanding magnetic properties with a room-temperature magnetization near the bulk value can be produced by high-temperature synthesis methods involving capping with organic acid. The capping molecules are not magnetic, so the origin of the enhanced magnetization remains elusive. In this work, we present a real-space characterization on the subnanometer scale of the magnetic, chemical, and structural properties of iron-oxide nanoparticles via aberration-corrected scanning transmission electron microscopy. For the first time, electron magnetic chiral dichroism is used to map the magnetization of nanoparticles in real space with subnanometer spatial resolution. We find that the surface of the nanoparticles is magnetically ordered. Combining the results with density functional calculations, we establish how magnetization is restored in the surface layer. The bonding with the acid's O atoms results in O-Fe atomic configuration and distances close to bulk values. We conclude that the nature and number of molecules in the capping layer is an essential ingredient in the fabrication of nanoparticles with optimal magnetic properties.
We investigate the effect of surfactant-mediated, asymmetric silver overgrowth of gold nanorods on their intrinsic optical properties. From concentration-dependent experiments, we established a close correlation of the extinction in the UV/vis/NIR frequency range and the morphological transition from gold nanorods to Au@Ag cuboids. Based on this correlation, a generic methodology for in situ monitoring of the evolution of the cuboid morphology was developed and applied in time-dependent experiments. We find that growth rates are sensitive to the substitution of the surfactant headgroup by comparison of benzylhexadecyldimethylammonium chloride (BDAC) with hexadecyltrimethylammonium chloride (CTAC). The time-dependent overgrowth in BDAC proceeds about 1 order of magnitude slower than in CTAC, which allows for higher control during silver overgrowth. Furthermore, silver overgrowth results in a qualitatively novel optical feature: Upon excitation inside the overlap region of the interband transition of gold and intraband of silver, the gold core acts as a retarding element. The much higher damping of the gold core compared to the silver shell in Au@Ag cuboids induces mirror charges at the core/shell interface as shown by electromagnetic simulations. Full control over the kinetic growth process consequently allows for precise tailoring of the resonance wavelengths of both modes. Tailored and asymmetric silver-overgrown gold nanorods are of particular interest for large-scale fabrication of nanoparticles with intrinsic metamaterial properties. These building blocks could furthermore find application in optical sensor technology, light harvesting, and information technology.
The design of the 3D architecture surfaces with both space- and time-dependent functionality (cell attraction, pH-trigged self-cleaning, antiseptic/disinfection) is in the focus. The innovative story includes: sonochemical surface activation, formation of feedback surface component (pH-responsible micelles), proof of responsive activity (time resolved cell adhesion and bacteria deactivation) and space adhesion selectivity (surface patterning).
Encoded particles are one of the most powerful approaches for multiplex high-throughput screening. Surface-enhanced Raman scattering (SERS) based codification can, in principle, avoid many of the intrinsic limitations due to conventional alternatives, as it decreases the reading time and particle size while allowing for almost unlimited codification. Unfortunately, methods for the synthetic preparation of these particles are tedious; often subjected to limited reproducibility (associated with large fluctuations in the size distributions of the polymers employed in the standard protocols); and to date, limited to a small amount of molecules. Herein, we report a universal, one-pot, inexpensive, and scalable synthetic protocol for the fabrication of SERS-encoded nanoparticles. This synthetic strategy is highly reproducible, independent of the chemical nature and size of the Raman code used (31 different codes were tested) and scalable in the liter range without affecting the final properties of the encoded structures. Furthermore, the SERS efficiency of the fabricated encoded nanoparticles is superior to that of the materials produced by conventional methods, while showing a remarkable reproducibility from batch to batch. This encoding strategy can easily be applied to nanoparticles of different materials and shapes.
Here, a new surface enhanced Raman spectroscopy (SERS) platform suitable for gas phase sensing based on the extended organization of poly-N-isopropylacrylamide (pNIPAM)-coated nanostars over large areas is presented. This system yields high and homogeneous SERS intensities, and simultaneously traps organic chemical agents as pollutants from the gas phase. pNIPAM-coated gold nanostars were organized into parallel linear arrays. The optical properties of the fabricated substrates are investigated, and applicability for advanced sensing is demonstrated through the detection in the gas phase of pyrene traces, a well-known polyaromatic hydrocarbon.
The magnetic behavior of Fe 3Àx O 4 nanoparticles synthesized by either high-temperature decomposition of an organic iron precursor or low-temperature coprecipitation in aqueous conditions is compared. Transmission electron microscopy, x-ray absorption spectroscopy, x-ray magnetic circular dichroism, and magnetization measurements show that nanoparticles synthesized by thermal decomposition display high crystal quality and bulklike magnetic and electronic properties, while nanoparticles synthesized by coprecipitation show much poorer crystallinity and particlelike phenomenology, including reduced magnetization, high closure fields, and shifted hysteresis loops. The key role of the crystal quality is thus suggested, because particlelike behavior for particles larger than about 5 nm is observed only when the particles are structurally defective. These conclusions are supported by Monte Carlo simulations. It is also shown that thermal decomposition is capable of producing nanoparticles that, after further stabilization in physiological conditions, are suitable for biomedical applications such as magnetic resonance imaging or biodistribution studies. V
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