Tuning the Properties of Nanocomposites by Trapping Them in Deep Metastable States

Zhengping Zhou; Vera Bocharova; Rajeev Kumar; Anne Caroline Genix; Bobby Carroll; Subarna Samanta; Ivan Popov; Amanda Young-Gonzales; Alexander Kisliuk; Seung Pyo Jeong; Jan Ilavsky; Alexei P. Sokolov

doi:10.1021/acsapm.1c01623

Tuning the Properties of Nanocomposites by Trapping Them in Deep Metastable States

Zhengping Zhou, Vera Bocharova, Rajeev Kumar, Anne Caroline Genix, Bobby Carroll, Subarna Samanta, Ivan Popov, Amanda Young-Gonzales, Alexander Kisliuk, Seung Pyo Jeong, Jan Ilavsky, Alexei P. Sokolov

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

Abstract

The interfacial region formed in a polymer matrix around nanoparticles (NPs) controls many macroscopic properties of polymer nanocomposites (PNCs). However, understanding the factors controlling the structure and properties of the interfacial region remains a challenge. We demonstrated that the initial trapping of polymer chains at surfaces of NPs in solution strongly affects the macroscopic properties of PNCs. The most surprising result is that the differences in properties of PNCs persist even after an extremely long thermal annealing time. We ascribe the observed changes to the formation of an interfacial layer that is trapped in a deep metastable state already in solution. Furthermore, the presented analysis suggests that the PNC equilibration time is defined by the chain desorption time that can be extremely long and, in some cases, even not accessible on a reasonable experimental time scale. These results highlight the importance of polymer solution concentrations on the formation of an interfacial layer and the macroscopic properties of PNCs.

Original language	English
Pages (from-to)	3174-3182
Number of pages	9
Journal	ACS Applied Polymer Materials
Volume	4
Issue number	5
DOIs	https://doi.org/10.1021/acsapm.1c01623
State	Published - May 13 2022

Funding

This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. S.S. acknowledges partial financial support from NSF (DMR-1904657) for some of the dielectric measurements and data analysis. Theory and simulations were a portion of this research was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. This research used resources of the National Energy Research Scientific Computing Center (NERSC) and the Compute and Data Environment for Science (CADES) at the Lawrence Berkeley National Laboratory and the Oak Ridge National Laboratory, which are supported by the Office of Science of the U.S. Department of Energy under Contract no. DE-AC02-05CH11231 and DE-AC05-00OR22725, respectively. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract no. DE-AC02-06CH11357.

Funders	Funder number
National Science Foundation
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering

Keywords

Brillouin light scattering
Polymer nanocomposites
SCFT calculations
interfacial layer model
photon correlation spectroscopy

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10.1021/acsapm.1c01623

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abstract = "The interfacial region formed in a polymer matrix around nanoparticles (NPs) controls many macroscopic properties of polymer nanocomposites (PNCs). However, understanding the factors controlling the structure and properties of the interfacial region remains a challenge. We demonstrated that the initial trapping of polymer chains at surfaces of NPs in solution strongly affects the macroscopic properties of PNCs. The most surprising result is that the differences in properties of PNCs persist even after an extremely long thermal annealing time. We ascribe the observed changes to the formation of an interfacial layer that is trapped in a deep metastable state already in solution. Furthermore, the presented analysis suggests that the PNC equilibration time is defined by the chain desorption time that can be extremely long and, in some cases, even not accessible on a reasonable experimental time scale. These results highlight the importance of polymer solution concentrations on the formation of an interfacial layer and the macroscopic properties of PNCs.",

keywords = "Brillouin light scattering, Polymer nanocomposites, SCFT calculations, interfacial layer model, photon correlation spectroscopy",

author = "Zhengping Zhou and Vera Bocharova and Rajeev Kumar and Genix, {Anne Caroline} and Bobby Carroll and Subarna Samanta and Ivan Popov and Amanda Young-Gonzales and Alexander Kisliuk and Jeong, {Seung Pyo} and Jan Ilavsky and Sokolov, {Alexei P.}",

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AU - Bocharova, Vera

AU - Kumar, Rajeev

AU - Genix, Anne Caroline

AU - Carroll, Bobby

AU - Samanta, Subarna

AU - Popov, Ivan

AU - Young-Gonzales, Amanda

AU - Kisliuk, Alexander

AU - Jeong, Seung Pyo

AU - Ilavsky, Jan

AU - Sokolov, Alexei P.

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N2 - The interfacial region formed in a polymer matrix around nanoparticles (NPs) controls many macroscopic properties of polymer nanocomposites (PNCs). However, understanding the factors controlling the structure and properties of the interfacial region remains a challenge. We demonstrated that the initial trapping of polymer chains at surfaces of NPs in solution strongly affects the macroscopic properties of PNCs. The most surprising result is that the differences in properties of PNCs persist even after an extremely long thermal annealing time. We ascribe the observed changes to the formation of an interfacial layer that is trapped in a deep metastable state already in solution. Furthermore, the presented analysis suggests that the PNC equilibration time is defined by the chain desorption time that can be extremely long and, in some cases, even not accessible on a reasonable experimental time scale. These results highlight the importance of polymer solution concentrations on the formation of an interfacial layer and the macroscopic properties of PNCs.

AB - The interfacial region formed in a polymer matrix around nanoparticles (NPs) controls many macroscopic properties of polymer nanocomposites (PNCs). However, understanding the factors controlling the structure and properties of the interfacial region remains a challenge. We demonstrated that the initial trapping of polymer chains at surfaces of NPs in solution strongly affects the macroscopic properties of PNCs. The most surprising result is that the differences in properties of PNCs persist even after an extremely long thermal annealing time. We ascribe the observed changes to the formation of an interfacial layer that is trapped in a deep metastable state already in solution. Furthermore, the presented analysis suggests that the PNC equilibration time is defined by the chain desorption time that can be extremely long and, in some cases, even not accessible on a reasonable experimental time scale. These results highlight the importance of polymer solution concentrations on the formation of an interfacial layer and the macroscopic properties of PNCs.

KW - Brillouin light scattering

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KW - SCFT calculations

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KW - photon correlation spectroscopy

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Tuning the Properties of Nanocomposites by Trapping Them in Deep Metastable States

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Keywords

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