alternating-magnetic-field-responsive-hybrid-gelatin-microgels-for

Alternating Magnetic Field-Responsive Hybrid Gelatin Microgels for Controlled Drug Release

Magnetically-responsive nano/micro-engineered biomaterials that enable a tightly controlled, on-demand drug delivery have been developed as new types of ...

Kent State University

Colloidal suspensions are susceptible to gravitationally induced phase separation. This can be mitigated by the formation of a particle network caused by depletion attraction. The effectiveness of this network in supporting the buoyant weight of the suspension can be characterized by its compressional modulus. We measure the compressional modulus for emulsion networks induced by depletion attraction and present a model that quantitatively predicts their gravitational stability. We also determine the relationship between the strength of the depletion attraction and the magnitude of the compressional modulus.

Gravitational stability of suspensions of attractive colloidal particles.

Dilute oil dispersions of fractal carbon black particles with attractive van der Waals interactions display continuous shear thickening followed by shear thinning at high shear rates. The shear thickening transition occurs at gamma c approximately 10(2)-10(3) s(-1) and is driven by hydrodynamic breakup of clusters. Pre-shearing dispersions at shear rates gamma>gamma c produces enhanced-modulus gels where G' approximately sigma pre-shear 1.5-2 and is directly proportional to the residual stress in the gel measured at a fixed sample age. The observed data can be accounted for using a simple scaling model for the breakup of fractal clusters under shear stress.

Shear thickening and scaling of the elastic modulus in a fractal colloidal system with attractive interactions.

This is to report a study of chain conformation of poly(dimethylsiloxane) (PDMS) in spread monolayers at the air/water interface (A/W) with the aid of vibrational sum frequency spectroscopy (VSFS). We find that methyl groups of PDMS chains at the interface are completely disordered in the dilute regime of the surface density. At higher surface densities, however, the two methyl groups on the repeating unit point into the air asymmetrically; one points more normal to the interface, whereas the other lies more parallel to the interface. In the first collapsed regime, where the surface pressure of the PDMS monolayer reaches a plateau value of 8.7 mN/m, the signal intensity at 2915 cm (-1), assigned to the symmetric vibrational frequency of the methyl groups, is found independent of the surface density. On the basis of this finding, we propose that PDMS chains, in the first collapse regime at the A/W, form asymmetric layers. Thus, our proposal lends support to earlier works by Langevin's group to refute a widely speculated helix model that was based on energy minimization in the crystalline state of PDMS. In short, the energy consideration in the bulk crystalline state does not provide meaningful guidance as to the chain conformation of the monolayer at the A/W.

Chain conformation of poly(dimethyl siloxane) at the air/water interface by sum frequency generation.

We use confocal microscopy to explore shear melting of colloidal glasses, which occurs at strains of approximately 0.08, coinciding with a strongly non-Gaussian step size distribution. For larger strains, the particle mean square displacement increases linearly with strain and the step size distribution becomes Gaussian. The effective diffusion coefficient varies approximately linearly with shear rate, consistent with a modified Stokes-Einstein relationship in which thermal energy is replaced by shear energy and the length scale is set by the size of cooperatively moving regions consisting of approximately 3 particles.

Shear melting of a colloidal glass.

We report interesting self-assembly structures of nematic liquid-crystal colloid (NLCC) networks, which are arrested during cooling from the isotropic temperature to room temperature. The NLCC is composed of sterically stabilized colloidal particles and a nematic liquid crystal (NLC) with nematic-isotropic transition temperature (T_{NI}) that is much higher than those of previously studied 4-Cyano-4'-pentylbiphenyl and N-(4-Methoxybenzylidene)-4-butylaniline. We find that the structure of NLCCs depends on T(NI), cooling rates, and boundary conditions, varying from cellular network to hierarchical fern structures in different length scales. Our time-lapse study shows that the transition from the cellular network to the fern structure directly corresponds to the transition from a spinodal demixing to a nucleation-and-growth mechanism.

Dynamic arrest of nematic liquid-crystal colloid networks.

A two-dimensional (2D) solid lacks long-range positional order and is diffusive by means of the cooperative motion of particles. We find from molecular dynamics simulations of hard discs that 2D colloids in solid and hexatic phases show seemingly Fickian but strongly heterogeneous dynamics. Beyond translational relaxation time, the mean-square displacement is linear with time, t, implying that discs would undergo Brownian diffusion and the self-part of the van Hove correlation function [G(s)(r,t)] might be Gaussian. But dynamics is still heterogeneous and G(s)(r,t) is exponential at large r and oscillatory with multiple peaks at intermediate length. We attribute the existence of several such peaks to the observation that there are several clusters of discs with discretized mobility. The cluster of marginally mobile discs grows with time and begins to percolate around translational relaxation time while clusters of fast discs emerge in the middle of the marginally mobile cluster.

Simulation study of seemingly Fickian but heterogeneous dynamics of two dimensional colloids.

In this study, we present gelatin-based thermoresponsive colloidal microgels that enable the controlled release of drugs by volume phase transition. The microgel was fabricated by physically entrapping poly(N-isopropylacrylamide-co-acrylamide) chains as a minor component within three-dimensional gelatin networks crosslinked by genipin. We demonstrate that our gelatin-based thermoresponsive microgel exhibits a tunable deswelling to temperature increase, which positively correlated to the release of bovine serum albumin (BSA) as a function of poly(N-isopropylacrylamide-co-acrylamide) concentration. The microgel was enzymatically degradable by collagenase treatment. The extent of BSA release and biodegradability were tuned by controlling the crosslinking degree of the gelatin matrix. Meeting a great need for design and synthesis of auto-degenerating smart microgels that enable the controlled release of therapeutic proteins in responsive to external stimuli, our gelatin-based microgels that satisfy both thermoresponsivity and biodegradability have a great potential in tissue engineering applications as a soft microdevice element for drug delivery.

Article	Year
Gravitational stability of suspensions of attractive colloidal particles. Physical review letters\| PubMed ID: 17678267	2007
Shear thickening and scaling of the elastic modulus in a fractal colloidal system with attractive interactions. Physical review. E, Statistical, nonlinear, and soft matter physics\| PubMed ID: 18643204	2008
Chain conformation of poly(dimethyl siloxane) at the air/water interface by sum frequency generation. Langmuir : the ACS journal of surfaces and colloids\| PubMed ID: 18710265	2008
Shear melting of a colloidal glass. Physical review letters\| PubMed ID: 20366655	2010
Dynamic arrest of nematic liquid-crystal colloid networks. Physical review. E, Statistical, nonlinear, and soft matter physics\| PubMed ID: 24229199	2013
Simulation study of seemingly Fickian but heterogeneous dynamics of two dimensional colloids. Physical review letters\| PubMed ID: 25166201	2013
Biodegradable colloidal microgels with tunable thermosensitive volume phase transitions for controllable drug delivery. Journal of colloid and interface science\| PubMed ID: 25797395	2015

Chanjoong Kim

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