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Title: Structural Emergence in Particle Dispersions

Abstract

Particle dispersions, such as pigment-based inks, comprise weakly bound, milled nanoparticles. The properties of these pigments depend on both their chemical composition and a rather complex structural hierarchy which emerges from these dispersions. The emergence of structure under semidilute conditions is related to the structure of the dilute particles, the particle spacing (mesh size), processing history, and the interaction potential. Kinetic simulations could predict such emergence using these input parameters. In this paper, organic pigments are studied as an example of the importance of emergent structure to predict properties such as brilliance and opacity. Organic pigments are used to impart color to commercial inks, plastics, coatings, and cosmetics. In many cases, dilute pigments are mass fractal structures consisting of aggregated nanoparticles held together by weak van der Waals forces. In water, surfactant is added to create a pigment dispersion (an ink). The final properties of a pigment emerge from a complex interplay between aggregation and dispersion of aggregates as a function of concentration. Samples of the organic pigment yellow 14, PY14, were milled to four primary particle sizes to study the effect on structural emergence. The interaction between surfactant-stabilized PY14 aggregates in an aqueous medium was quantified by the secondmore » virial coefficient, A2, which reflects long-range interactions. The degree of aggregation is associated with short-range attractive interactions between primary particles. In this series of pigments, the degree of aggregation increases dramatically with reduction in primary particle size. Concurrently, the second-order virial coefficient, A2, increases reflecting stronger long-range repulsive interactions with particle size. Structural emergence can be understood through the percolation concentration and the filler mesh size. A2 is translated into a repulsive interaction potential for use in dissipative particle dynamics simulations to enable predictive modeling. Furthermore, this description of the interactions between dispersed pigment aggregates allows for a more scientific and predictive approach to understand structural emergence.« less

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1];  [2];  [2]
  1. Univ. of Cincinnati, OH (United States)
  2. Sun Chemical Corporation, Cincinnati, OH (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1419875
Grant/Contract Number:  
AC02-06CH11357; CMMI-1635865; CMMI-1636036
Resource Type:
Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 33; Journal Issue: 49; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
ENGLISH
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; dyes and pigments; nanoparticles; particle size; colloids; scattering

Citation Formats

Mulderig, Andrew, Beaucage, Gregory, Vogtt, Karsten, Jiang, Hanqiu, Jin, Yan, Clapp, Lisa, and Henderson, Donald C. Structural Emergence in Particle Dispersions. United States: N. p., 2017. Web. https://doi.org/10.1021/acs.langmuir.7b03033.
Mulderig, Andrew, Beaucage, Gregory, Vogtt, Karsten, Jiang, Hanqiu, Jin, Yan, Clapp, Lisa, & Henderson, Donald C. Structural Emergence in Particle Dispersions. United States. https://doi.org/10.1021/acs.langmuir.7b03033
Mulderig, Andrew, Beaucage, Gregory, Vogtt, Karsten, Jiang, Hanqiu, Jin, Yan, Clapp, Lisa, and Henderson, Donald C. Thu . "Structural Emergence in Particle Dispersions". United States. https://doi.org/10.1021/acs.langmuir.7b03033. https://www.osti.gov/servlets/purl/1419875.
@article{osti_1419875,
title = {Structural Emergence in Particle Dispersions},
author = {Mulderig, Andrew and Beaucage, Gregory and Vogtt, Karsten and Jiang, Hanqiu and Jin, Yan and Clapp, Lisa and Henderson, Donald C.},
abstractNote = {Particle dispersions, such as pigment-based inks, comprise weakly bound, milled nanoparticles. The properties of these pigments depend on both their chemical composition and a rather complex structural hierarchy which emerges from these dispersions. The emergence of structure under semidilute conditions is related to the structure of the dilute particles, the particle spacing (mesh size), processing history, and the interaction potential. Kinetic simulations could predict such emergence using these input parameters. In this paper, organic pigments are studied as an example of the importance of emergent structure to predict properties such as brilliance and opacity. Organic pigments are used to impart color to commercial inks, plastics, coatings, and cosmetics. In many cases, dilute pigments are mass fractal structures consisting of aggregated nanoparticles held together by weak van der Waals forces. In water, surfactant is added to create a pigment dispersion (an ink). The final properties of a pigment emerge from a complex interplay between aggregation and dispersion of aggregates as a function of concentration. Samples of the organic pigment yellow 14, PY14, were milled to four primary particle sizes to study the effect on structural emergence. The interaction between surfactant-stabilized PY14 aggregates in an aqueous medium was quantified by the second virial coefficient, A2, which reflects long-range interactions. The degree of aggregation is associated with short-range attractive interactions between primary particles. In this series of pigments, the degree of aggregation increases dramatically with reduction in primary particle size. Concurrently, the second-order virial coefficient, A2, increases reflecting stronger long-range repulsive interactions with particle size. Structural emergence can be understood through the percolation concentration and the filler mesh size. A2 is translated into a repulsive interaction potential for use in dissipative particle dynamics simulations to enable predictive modeling. Furthermore, this description of the interactions between dispersed pigment aggregates allows for a more scientific and predictive approach to understand structural emergence.},
doi = {10.1021/acs.langmuir.7b03033},
journal = {Langmuir},
number = 49,
volume = 33,
place = {United States},
year = {2017},
month = {11}
}

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