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Title: Simulation of macromolecule self-assembly in solution: A multiscale approach

One of the most common processes to produce polymer nanoparticles is to induce self-assembly by using the solvent-displacement method, in which the polymer is dissolved in a “good” solvent and the solution is then mixed with an “anti-solvent”. The polymer ability to self-assemble in solution is therefore determined by its structural and transport properties in solutions of the pure solvents and at the intermediate compositions. In this work, we focus on poly-ε-caprolactone (PCL) which is a biocompatible polymer that finds widespread application in the pharmaceutical and biomedical fields, performing simulation at three different scales using three different computational tools: full atomistic molecular dynamics (MD), population balance modeling (PBM) and computational fluid dynamics (CFD). Simulations consider PCL chains of different molecular weight in solution of pure acetone (good solvent), of pure water (anti-solvent) and their mixtures, and mixing at different rates and initial concentrations in a confined impinging jets mixer (CIJM). Our MD simulations reveal that the nano-structuring of one of the solvents in the mixture leads to an unexpected identical polymer structure irrespectively of the concentration of the two solvents. In particular, although in pure solvents the behavior of the polymer is, as expected, very different, at intermediate compositions, themore » PCL chain shows properties very similar to those found in pure acetone as a result of the clustering of the acetone molecules in the vicinity of the polymer chain. We derive an analytical expression to predict the polymer structural properties in solution at different solvent compositions and use it to formulate an aggregation kernel to describe the self-assembly in the CIJM via PBM and CFD. Simulations are eventually validated against experiments.« less
Authors:
; ;  [1] ;  [2] ;  [3]
  1. Dipartimento di Scienza Applicata e Tecnologia, Istituto di Ingegneria Chimica, Politecnico di Torino, C.so Duca degli Abruzzi 24, 10129 Torino (Italy)
  2. School of Chemistry, The University of Manchester, Oxford Road, Manchester M13 9PL, UnitedKingdom (United Kingdom)
  3. School of Chemical Engineering and Analytical Science, The University of Manchester, Oxford Road, Manchester M13 9PL, UnitedKingdom (United Kingdom)
Publication Date:
OSTI Identifier:
22494363
Resource Type:
Journal Article
Resource Relation:
Journal Name: AIP Conference Proceedings; Journal Volume: 1695; Journal Issue: 1; Conference: GT70 international conference on polymer processing with resulting morphology and properties: Feet in the present and eyes at the future, Salerno (Italy), 15-17 Oct 2015; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; 36 MATERIALS SCIENCE; ABUNDANCE; ACETONE; AGGLOMERATION; BALANCES; COMPUTERIZED SIMULATION; CONCENTRATION RATIO; FLUID MECHANICS; MIXERS; MOLECULAR DYNAMICS METHOD; MOLECULAR WEIGHT; NANOPARTICLES; NANOSTRUCTURES; POLYMERS; WATER