Numerous different photonics and biomedical applications depend on the fluorescent polymer micro- and nanoparticles. Besides optical or spectroscopic properties, the performance of the polymer nanoparticles is determined by their size, size distribution, and surface charge. Moreover, in order to realize a very uniform performance, the functional polymer nanoparticles should be of high homogeneity and demand for the preparation in a minimum number of synthesis steps. Here, we present a microfluidic-assisted synthesis of different types of reproducible fluorescent polymer nanoparticles with tuned size (40 nm up to 600 nm) and surface charge (ζ potential=-52 mV up to +45 mV). Four different preparation strategies were introduced for fluorophore-functionalized nanoparticles: (a) noncovalent binding of fluorophores with high loading, (b) covalent linking of fluorophores with enhanced stability, (c) surface-anchored fluorophores by hydrophobic interactions for triple function at the same time, and (d) surface immobilization of biomolecules and fluorophore by ionic as well as secondary interactions. In this way, four different classes of nanoparticles suited for different applications were prepared with a spherical shape as a model system. Moreover, the principle has been extended to the different types of nonspherical and composite polymer nanoparticles.
In this work, a wet-chemical synthesis method for gold-silver core-shell particles with nanometer precise adjustable silver shell thicknesses is presented. Typically wet-chemical syntheses lead to relatively large diameter size distributions and losses in the yield of the desired particle structure due to thermodynamical effects. With the here explained synthesis method in micro fluidic segment sequences, a combinatorial in situ parameter screening of the reactant concentration ratios by programmed flow rate shifts in conjunction with efficient segment internal mixing conditions is possible. The highly increased mixing rates ensure a homogeneous shell deposition on all presented gold core particles while the amount of available silver ions was adjusted by automated flow rate courses, from which the synthesis conditions for exactly tunable shell thicknesses between 1.1 and 6.1 nm could be derived. The findings according to the homogeneity of size and particle structure were confirmed by differential centrifugal sedimentation (DCS), scanning and transmission electron microscopy (SEM, TEM) and X-ray photoelectron spectroscopy (XPS) measurements. In UV-Vis measurements, a significant contribution of the core metal was found in the shape of the extinction spectra in the case of thin shells. These results were confirmed by theoretical calculations.
The well-known concept of electrical charging for the stabilization of colloidal solutions is extended to a general concept for explanation of behavior of nanoparticles during their formation, in their response behavior on chemical or electrochemical stress, and in particle/ particle interactions. This concept helps to understand the formation of polynuclear sphere-like plasmonic nanoparticles of gold, the surprising high stability of extended flat silver nanoprisms, and their switch-like transformation as well as the formation of special types of nanoparticle assemblies. It can be used for controlling the size of nanoparticles, for the synthesis of composite micro and nanoparticles, and for the generation of different classes of nonspherical polymer particles by particle/particle interactions during the process of particle growth. The reported experimental examples were mainly obtained by microfluidic experiments, which supplied a high homogeneity of the product particles. This high homogeneity is an excellent basis for studying the nanoparticle behavior in analogy to molecular processes and helps to get new insights in to the importance of electrical effects for nanoparticle synthesis and nanoparticle assembling.
The residence time distribution (RTD) characteristics of three microreactors containing different passive mixing structures, namely, a three dimensional serpentine structure, a split-and-recombine structure and a staggered herringbone structure, were investigated and compared. An experimental input-response technique was applied which required deconvolution of the measured data by modeling of the RTD. The proposed technique provides useful information on optimized application and operation of microfluidic devices. The serpentine reactor and the split-and-recombine reactor show improvement in RTD behaviour, i.e., narrowing of RTD curves, at Re-numbers > 30 due to effective transversal mixing and therefore reduced axial dispersion. In the case of the staggered herringbone structure, dead volumes could be observed which considerably affect the RTD.
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