title: Flow-induced conformational changes in gelatin structure and colloidal stabilization.
abstract: Flow can change the rate at which solutes adsorb on surfaces by changing mass transfer to the surface, but moreover, flow can induce changes in the conformation of macromolecules in solution by providing sufficient stresses to perturb the segmental distribution function. However, there are few studies where the effect of flow on macromolecules has been shown to alter the structure of macromolecules adsorbed on surfaces. We have studied how the local energy dissipation alters the adsorption of gelatin onto polystyrene nanoparticles ( r = 85 nm). The change in the nature of the adsorbed layer is manifest in the change in the ability of the nanoparticles to resist aggregation. Circular dichroism spectroscopy was used to assess conformational changes in gelatin, and dynamic light scattering was used to assess the colloid stability. Experiments were conducted in a vortex jet mixer where energy density and mixing times have been quantified; mixing of the gelatin and unstable nanoparticles occurs on the order of milliseconds. The adsorption of the gelatin provides steric stabilization to the nanoparticles. We found that the stability of the gelatin-adsorbed nanoparticles increased with increasing mixing velocities: when the mixing velocities were changed from 0.9 to 550 m/s, the radius of the nanoclusters (aggregates) formed 12 h after the mixing decreased from 2620 to 600 nm. Increasing temperature also gave rise to similar trends in the stability behavior with increasing temperature, leading to increasing colloid stability. Linear flow birefringence studies also suggested that the velocity fields in the mixer are sufficiently strong to produce conformational changes in the gelatin. These results suggest that the energy dissipation produced by mixing can activate conformational changes in gelatin to alter its adsorption on the surfaces of nanoparticles. Understanding how such conformational changes in gelatin can be driven by local fluid mechanics and how these changes are related to the adsorption behavior of gelatin is very important both industrially and scientifically.
authors.affiliation: Department of Chemical Engineering, Princeton University, Princeton, New Jersey 08544, USA.
authors.forename: Mustafa
authors.initials: M
authors.lastname: Akbulut
authors.forename: Naveen K
authors.initials: NK
authors.lastname: Reddy
authors.forename: Bernd
authors.initials: B
authors.lastname: Bechtloff
authors.forename: Sebastian
authors.initials: S
authors.lastname: Koltzenburg
authors.forename: Jan
authors.initials: J
authors.lastname: Vermant
authors.forename: Robert K
authors.initials: RK
authors.lastname: Prud'homme
mesh_terms: D000327:Adsorption; D002942:Circular Dichroism; D003102:Colloids / Q000737:chemistry*; D005780:Gelatin / Q000737:chemistry*; D008027:Light; D015233:Models, Statistical; D008968:Molecular Conformation; D053758:Nanoparticles / Q000737:chemistry; D036103:Nanotechnology / Q000379:methods; D010316:Particle Size; D011108:Polymers / Q000737:chemistry; D011137:Polystyrenes / Q000737:chemistry; D012542:Scattering, Radiation; D055672:Static Electricity; D013696:Temperature
chemical_list: D003102:Colloids; D011108:Polymers; D011137:Polystyrenes; D005780:Gelatin