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.
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14 November 2022
Research Article|
November 08 2022
Dynamics of equilibrium-linked colloidal networks
Special Collection:
Colloidal Gels
Taejin Kwon
;
Taejin Kwon
(Conceptualization, Data curation, Formal analysis, Investigation, Methodology, Validation, Writing – original draft, Writing – review & editing)
1
McKetta Department of Chemical Engineering, University of Texas at Austin
, Austin, Texas 78712, USA
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Tanner A. Wilcoxson
;
Tanner A. Wilcoxson
(Conceptualization, Data curation, Formal analysis, Investigation, Methodology, Validation, Writing – original draft, Writing – review & editing)
1
McKetta Department of Chemical Engineering, University of Texas at Austin
, Austin, Texas 78712, USA
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Delia J. Milliron
;
Delia J. Milliron
(Conceptualization, Funding acquisition, Supervision, Writing – original draft, Writing – review & editing)
1
McKetta Department of Chemical Engineering, University of Texas at Austin
, Austin, Texas 78712, USA
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Thomas M. Truskett
Thomas M. Truskett
a)
(Conceptualization, Funding acquisition, Project administration, Supervision, Writing – original draft, Writing – review & editing)
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
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
Note: This paper is part of the JCP Special Topic on Colloidal Gels.
J. Chem. Phys. 157, 184902 (2022)
Article history
Received:
September 09 2022
Accepted:
October 19 2022
Citation
Taejin Kwon, Tanner A. Wilcoxson, Delia J. Milliron, Thomas M. Truskett; Dynamics of equilibrium-linked colloidal networks. J. Chem. Phys. 14 November 2022; 157 (18): 184902. https://doi.org/10.1063/5.0125125
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