Langmuir, 21 (24), 11040 -11047, 2005. 10.1021/la051998k S0743-7463(05)01998-0
Web Release Date: October 11, 2005

Copyright © 2005 American Chemical Society

Phase Behavior and 3D Structure of Strongly Attractive Microsphere-Nanoparticle Mixtures

James F. Gilchrist, Angel T. Chan, Eric R. Weeks, and Jennifer A. Lewis*

Materials Science and Engineering Department and Frederick Seitz Materials Research Laboratory, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, and Physics Department, Emory University, Atlanta, Georgia 30322

Received July 22, 2005

Abstract:

We investigate the phase behavior and 3D structure of strongly attractive mixtures of silica microspheres and polystyrene nanoparticles. These binary mixtures are electrostatically tuned to promote a repulsion between like-charged (microsphere-microsphere and nanoparticle-nanoparticle) species and a strong attraction between oppositely charged (microsphere-nanoparticle) species. Using confocal fluorescence scanning microscopy, we directly observe the 3D structure of colloidal phases assembled from these mixtures as a function of varying composition. In the absence of nanoparticle additions, the charged-stabilized microspheres assemble into a polycrystalline array upon sedimentation. With increasing nanoparticle volume fraction, nanoparticle bridges form between microspheres, inducing their flocculation. At even higher nanoparticle volume fractions, the microspheres become well coated with nanoparticles, leading to their charge reversal and subsequent restabilization. We demonstrate how this fluid-gel-fluid transition can be utilized to control the morphology of the colloidal phases formed under gravity-driven sedimentation.


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