Dynamics of equilibrium-linked colloidal networks

Author:

Kwon Taejin1ORCID,Wilcoxson Tanner A.1ORCID,Milliron Delia J.1ORCID,Truskett Thomas M.12ORCID

Affiliation:

1. McKetta Department of Chemical Engineering, University of Texas at Austin, Austin, Texas 78712, USA

2. Department of Physics, University of Texas at Austin, Austin, Texas 78712, USA

Abstract

Colloids that attractively bond to only a few neighbors (e.g., patchy particles) can form equilibrium gels with distinctive dynamic properties that are stable in time. Here, we use a coarse-grained model to explore the dynamics of linked networks of patchy colloids whose average valence is macroscopically, rather than microscopically, constrained. Simulation results for the model show dynamic hallmarks of equilibrium gel formation and establish that the colloid–colloid bond persistence time controls the characteristic slow relaxation of the self-intermediate scattering function. The model features re-entrant network formation without phase separation as a function of linker concentration, centered at the stoichiometric ratio of linker ends to nanoparticle surface bonding sites. Departures from stoichiometry result in linker-starved or linker-saturated networks with reduced connectivity and shorter characteristic relaxation times with lower activation energies. Underlying the re-entrant trends, dynamic properties vary monotonically with the number of effective network bonds per colloid, a quantity that can be predicted using Wertheim’s thermodynamic perturbation theory. These behaviors suggest macroscopic in situ strategies for tuning the dynamic response of colloidal networks.

Funder

National Science Foundation

Welch Foundation

Publisher

AIP Publishing

Subject

Physical and Theoretical Chemistry,General Physics and Astronomy

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