Determining population densities in bimodal micellar solutions using contrast-variation small angle neutron scattering
Abstract
Self-assembly of amphiphilic polymers in water is of fundamental and practical importance. Significant amounts of free unimers and associated micellar aggregates often coexist over a wide range of phase regions. The thermodynamic and kinetic properties of the microphase separation are closely related to the relative population density of unimers and micelles. Although the scattering technique has been employed to identify the structure of micellar aggregates as well as their time-evolution, the determination of the population ratio of micelles to unimers remains a challenging problem due to their difference in scattering power. In this work, using small-angle neutron scattering (SANS), we present a comprehensive structural study of amphiphilic n-dodecyl-PNIPAm polymers, which shows a bimodal size distribution in water. By adjusting the deuterium/hydrogen ratio of water, the intra-micellar polymer and water distributions are obtained from the SANS spectra. The micellar size and number density are further determined, and the population densities of micelles and unimers are calculated to quantitatively address the degree of micellization at different temperatures. Our method can be used to provide an in-depth insight into the solution properties of microphase separation, which are present in many amphiphilic systems.
- Authors:
-
[1];
[1];
[1];
[3];
[1];
[1];
[1]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); National Tsing Hua Univ., Hsinchu (Taiwan)
- National Tsing Hua Univ., Hsinchu (Taiwan)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
- OSTI Identifier:
- 1720248
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 153; Journal Issue: 18; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; polymers; self-assembly; neutron scattering
Citation Formats
Huang, Ronger, Tung, Chi-Huan, Chang, Dongsook, Lam, Christopher N., Do, Changwoo, Shinohara, Yuya, Chang, Shou-Yi, Wang, Yangyang, Hong, Kunlun, and Chen, Wei-Ren. Determining population densities in bimodal micellar solutions using contrast-variation small angle neutron scattering. United States: N. p., 2020.
Web. doi:10.1063/5.0024410.
Huang, Ronger, Tung, Chi-Huan, Chang, Dongsook, Lam, Christopher N., Do, Changwoo, Shinohara, Yuya, Chang, Shou-Yi, Wang, Yangyang, Hong, Kunlun, & Chen, Wei-Ren. Determining population densities in bimodal micellar solutions using contrast-variation small angle neutron scattering. United States. https://doi.org/10.1063/5.0024410
Huang, Ronger, Tung, Chi-Huan, Chang, Dongsook, Lam, Christopher N., Do, Changwoo, Shinohara, Yuya, Chang, Shou-Yi, Wang, Yangyang, Hong, Kunlun, and Chen, Wei-Ren. Wed .
"Determining population densities in bimodal micellar solutions using contrast-variation small angle neutron scattering". United States. https://doi.org/10.1063/5.0024410. https://www.osti.gov/servlets/purl/1720248.
@article{osti_1720248,
title = {Determining population densities in bimodal micellar solutions using contrast-variation small angle neutron scattering},
author = {Huang, Ronger and Tung, Chi-Huan and Chang, Dongsook and Lam, Christopher N. and Do, Changwoo and Shinohara, Yuya and Chang, Shou-Yi and Wang, Yangyang and Hong, Kunlun and Chen, Wei-Ren},
abstractNote = {Self-assembly of amphiphilic polymers in water is of fundamental and practical importance. Significant amounts of free unimers and associated micellar aggregates often coexist over a wide range of phase regions. The thermodynamic and kinetic properties of the microphase separation are closely related to the relative population density of unimers and micelles. Although the scattering technique has been employed to identify the structure of micellar aggregates as well as their time-evolution, the determination of the population ratio of micelles to unimers remains a challenging problem due to their difference in scattering power. In this work, using small-angle neutron scattering (SANS), we present a comprehensive structural study of amphiphilic n-dodecyl-PNIPAm polymers, which shows a bimodal size distribution in water. By adjusting the deuterium/hydrogen ratio of water, the intra-micellar polymer and water distributions are obtained from the SANS spectra. The micellar size and number density are further determined, and the population densities of micelles and unimers are calculated to quantitatively address the degree of micellization at different temperatures. Our method can be used to provide an in-depth insight into the solution properties of microphase separation, which are present in many amphiphilic systems.},
doi = {10.1063/5.0024410},
journal = {Journal of Chemical Physics},
number = 18,
volume = 153,
place = {United States},
year = {Wed Nov 11 00:00:00 EST 2020},
month = {Wed Nov 11 00:00:00 EST 2020}
}
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