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Self‐assembly mechanism of PEG‐b‐PCL and PEG‐b‐PBO‐b‐PCL amphiphilic copolymer micelles in aqueous solution from coarse grain modeling

Sadeghi, Maryam S. and Moghbeli, Mohammad Reza and Goddard, William A., III (2021) Self‐assembly mechanism of PEG‐b‐PCL and PEG‐b‐PBO‐b‐PCL amphiphilic copolymer micelles in aqueous solution from coarse grain modeling. Journal of Polymer Science, 59 (7). pp. 614-626. ISSN 2642-4150. doi:10.1002/pol.20200864. https://resolver.caltech.edu/CaltechAUTHORS:20210305-075944764

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Abstract

We followed the self‐assembly of high‐molecular weight MePEG‐b‐PCL (poly(methyl ethylene glycol)‐block‐poly(ε‐caprolactone)) diblock and MePEG‐b‐PBO‐b‐PCL (poly(methyl ethylene glycol)‐block‐poly(1,2‐butylene oxide)‐block‐poly(ε‐caprolactone)) into micelles using molecular dynamics simulation with a coarse grain (CG) force field based on quantum mechanics (CGq FF). The triblock polymer included a short poly(1,2‐butylene oxide) (PBO) at the hydrophilic‐hydrophobic interface of these systems. Keeping the hydrophilic length fixed (MePEG₄₅), we considered 250 chains in which the hydrophobic length changed from PCL₄₄ or PBO₆‐b‐PCL₄₃ to PCL₆₂ or PBO₉‐b‐PCL₆₁. The polymers were solvated in explicit water for 2 μs of simulations at 310.15 K. We found that the longer diblock system undergoes a morphological transition from an intermediate rod‐like micelle to a prolate‐sphere, while the micelle formed from the longer triblock system is a stable rod‐like micelle. The two shorter diblock and triblock systems show similar self‐assembly processes, both resulting in slightly prolate‐spheres. The dynamics of the self‐assembly is quantified in terms of chain radius of gyration, shape anisotropy, and hydration of the micelle cores. The final micelle structures are analyzed in terms of the local density components. We conclude that the CG model accurately describes the molecular mechanisms of self‐assembly and the equilibrium micellar structures of hydrophilic and hydrophobic chains, including the quantity of solvent trapped inside the micellar core.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1002/pol.20200864DOIArticle
ORCID:
AuthorORCID
Sadeghi, Maryam S.0000-0003-3771-566X
Moghbeli, Mohammad Reza0000-0003-2729-1883
Goddard, William A., III0000-0003-0097-5716
Additional Information:© 2021 Wiley Periodicals LLC. Issue Online: 01 April 2021; Version of Record online: 03 March 2021; Manuscript accepted: 04 February 2021; Manuscript revised: 02 February 2021; Manuscript received: 20 December 2020. Funding information: DOE, Grant/Award Numbers: DE‐AC05‐00OR22725, DE‐SC0017710. Data availability statement: The data that support the findings of this study are available on request from the corresponding author.
Funders:
Funding AgencyGrant Number
Department of Energy (DOE)DE‐AC05‐00OR22725
Department of Energy (DOE)DE‐SC0017710
Subject Keywords:coarse grain model; diblock copolymer; quantum mechanics; self‐assembly; triblock copolymer
Issue or Number:7
DOI:10.1002/pol.20200864
Record Number:CaltechAUTHORS:20210305-075944764
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20210305-075944764
Official Citation:Sadeghi, MS, Moghbeli, MR, Goddard, WA. Self‐assembly mechanism of PEG‐b‐PCL and PEG‐b‐PBO‐b‐PCL amphiphilic copolymer micelles in aqueous solution from coarse grain modeling. J Polym Sci. 2021; 59: 614–626. https://doi.org/10.1002/pol.20200864
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:108323
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:08 Mar 2021 23:45
Last Modified:08 Apr 2021 22:10

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