Nano-sized metal particles are attracting much interest in industrial and biomedical applications due to the recent progress and development of nanotechnology, and the surface-modifications by appropriate polymers are key techniques to stably express their characteristics. Herein, we applied cyclic poly(ethylene glycol) (c-PEG), having no chemical inhomogeneity, to provide a polymer topology-dependent stabilization for the surface-modification of gold nanoparticles (AuNPs) through physisorption. By simply mixing c-PEG, but not linear counterparts, enables AuNPs to maintain dispersibility through freezing, lyophilization, or heating. Surprisingly, c-PEG endowed AuNPs with even better dispersion stability than thiolated PEG (HS–PEG–OMe). The stronger affinity of c-PEG was confirmed by DLS, ζ-potential, and FT-IR. Furthermore, the c-PEG system exhibited prolonged blood circulation and enhanced tumor accumulation in mice. Our data suggests that c-PEG induces physisorption on AuNPs, supplying sufficient stability toward bio-medical applications, and would be an alternative approach to the gold–sulfur chemisorption.
A series of aryl nitrile-based ligands were prepared to investigate the effect of their electrophilicity on the affinity against the cysteine proteases rhodesain and human cathepsin L. Density functional theory calculations provided relative reactivities of the nitriles, enabling prediction of their biological affinity and cytotoxicity and a clear structure-activity relationship.
The dielectric permittivity (ε') of a polymeric material can be significantly increased when blended with conductive fillers at concentrations approaching percolation threshold. However, reproducible synthesis of such composites is after decades of research still a major challenge and a bottleneck for their application. Difficulties arise in controlling size and shape of the filler as well as in its homogenous distribution within the composite. These parameters strongly affect the dielectric as well as the mechanical properties of the composite. While a substantial amount of literature is dealing with the influence of conductive filler on the dielectric properties of composites, little is known about their mechanical properties. It is therefore still an important goal to synthesize materials with simultaneously high ε' and good mechanical properties. Here, we report the synthesis of dielectric elastomers that combine key properties such as high flexibility and stretchability, high thermal stability, increased ε', low dielectric loss and conductivity. Such materials were prepared by solution processing using quasi-spherical silver nanoparticles (AgNPs) of defined size in a polydimethylsiloxane matrix (M w = 692 kDa). To prevent percolation, the AgNPs were coated with a thin silica shell (<4 nm). To increase their compatibility with the silicone matrix, these core/shell nanoparticles were passivated with a silane reagent. The insulating silica shell around the particles precisely defines the minimum approach distance between the cores as twice the shell thickness. The dielectric properties of those passivated particles (filler) were measured in pellets and found to have an almost frequency independent value of ε' = 90 and a very low loss factor tan δ = 0.023 at high frequencies. When such particles were used as filler in a polydimethylsiloxane matrix, composites with low dielectric losses were obtained. A composite containing 31 vol% filler with ε' = 21 and a tan δ = 0.03 at ~1 kHz was achieved. At a AgNPs volume fraction of 20%, the composite has a ε' = 5.9 at ~1 kHz, a dielectric strength of 13.4 V/µm, elastic modulus as low as 350 kPa at 100% strain, and a strain at break of 800%. Due to the high specific energy density per volume at low electric fields, these composites are attractive materials in applications involving low electric fields.A composite of Ag/SiO 2 core/shell nanoparticles 20 vol% in polydimethylsiloxane with ε' = 5.9, E b = 13.4 V/µm, Y 100% = 350 kPa, a strain at break of 800% is presented.
a Core/shell nanoparticles having metallic silver nanoparticle cores of y38 nm in diameter and silica shells of different thicknesses ranging from y3.6-20 nm were prepared. For the silica coating, a slightly modified Stöber method was used which allowed preparing grams of core/shell nanoparticles for the first time. The particles were characterized by UV-vis spectroscopy, dynamic light scattering, scanning electron microscopy, transmission electron microscopy, and energy-dispersive X-ray scattering. Their dielectric properties were measured as pellets in parallel-plate capacitors. It was found that the permittivity is much influenced by the silica shell thickness with an increase in permittivity for thinner shells. A shell thickness of 20 ¡ 2 nm allowed fabrication of capacitors which have similar characteristics to those of silica, thus, there is no influence of the metal core on the dielectric properties anymore. However, by decreasing the silica shell to 17 ¡ 2, 8 ¡ 1.5, and 6.6 ¡ 1.5 nm the permittivity at high frequencies is increasing from 10, 34, to 41, respectively. The insulator to metal transition was observed for a silica shell thickness of 3.6 ¡ 1 nm.Functionalization of the silica surface with a hydrophobic coating removes surface adsorbed water as observed by the flat dielectric permittivity over a large frequency domain.
Conductive inks consisting of graphene and carbon black conductive fillers into a polydimethylsiloxane (PDMS) matrix, which can be processed into thin films by screen printing are developed. The influence of filler composition and content on mechanical and electrical properties of the conductive composites is investigated. The best composites were evaluated as electrode material for dielectric elastomer actuators and for piezoelectric sensors. With increasing filler content, the electrical properties of the resulting composites of graphite nanoplates (GNPs) or a binary mixture of GNPs and carbon black (CB) with PDMS (Mw = 139 kg/mol) are enhanced. Hence, PDMS composites filled with GNPs (42 wt.%) or a binary mixture of GNPs/CB (300/150 ratio, 30 wt.% of total filler loading) exhibited constant contact resistance values of 0.5 and 5 Ω determined in life-cycle test, respectively, thus rendering them suitable as electrode materials for piezosensors. On the other hand, dielectric elastomer actuators require more flexible electrode materials, which could be tuned by varying the polymer molecular weight and by reducing the filler content. Therefore, a composite consisting of PDMS (Mw = 692 kg/mol) and a binary filler mixture of GNPs/CB (150/75 ratio, 18 wt.% of total filler loading) was used for producing the electrodes of dielectric elastomer transducers (DETs). The produced DETs with different electrode thicknesses were characterized in terms of their performance. The negligible hysteresis of the electrode materials is favorable for sensor and actuator applications.
Polysiloxane elastomers containing varying mo2009l% of trifluoropropyl groups were investigated in dielectric elastomer actuators.
Two complementary topics are discussed: (i) the continuous production of silver nanoparticles (AgNPs) and (ii) the measurement of reaction yield by X-ray absorption near-edge spectroscopy (XANES). The continuous polyol synthesis of AgNPs in grams amount and in the size range of 7–104 nm was carried out in the segmented flow tubular reactor (SFTR). Particle size was tailored by controlling the synthesis parameters such as temperature, reactant concentrations, and polyvinylpyrrolidone (PVP) molecular weight. The continuous production was tested for 4 h, and the product has shown constant particle size distribution over the whole production time. Reliable continuous production of 2.3 g h–1 of ∼100 nm AgNPs can be achieved with a lab-scale SFTR. The produced particles were fully characterized with respect to size, size distribution, and chemical purity. To better understand the growth mechanism, synchrotron-radiation high-resolution X-ray diffraction, and X-ray absorption spectroscopy data were collected directly on the AgNPs suspension. In particular, from XANES experiments, the conversion yield of Ag+ to Ag0 was measured. The results are consistent with a two-step process where PVP controls the particle nucleation while growth is ensured by thermally induced ethylene glycol oxidation.
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