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Polymerization-Induced Self-Assembly (PISA)

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Dear Colleagues,

Polymerization-induced self-assembly (PISA) is an emerging platform technology allowing the production of copolymer-based nano-objects of various shapes (sphere, wormlike micelles and vesicles) in both polar and non-polar solvents. Compared to other multistep assembly techniques such as solvent displacement methods, PISA is a one-pot approach requiring simple operating conditions to produce nano-objects at high solids concentration (up to 50 wt%), which is a significant benefit for a potential scale-up. Although thermally/photo-initiated RAFT polymerizations are by far the most commonly employed methods in PISA, the scoop of the latter has been extended in recent years to other energy sources and polymerization mechanisms.

This Special Issue intends to cover works carrying out PISA to increase our knowledge on:

Development of new reactive steric stabilizers and/or core-forming nanoobjects;
Preparation of smart polymeric nanoobjects;
Extension of the scoop of PISA to additional polymerization methods;
Use of the resulting nanoobjects in biomedical, cosmetic, food, environment, and energy fields.

As Guest Editors, we cordially invite contributions in the form of original research articles or reviews on this amazing research field.

Dr. Khalid Ferji
Prof. Dr. Jean-Luc Six
Guest Editors

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Research

14 pages, 4262 KiB

Open AccessArticle

Synthesis and Characterization of Temperature-Responsive N-Cyanomethylacrylamide-Containing Diblock Copolymer Assemblies in Water

by Nicolas Audureau, Fanny Coumes, Clémence Veith, Clément Guibert, Jean-Michel Guigner, François Stoffelbach and Jutta Rieger

Polymers 2021, 13(24), 4424; https://doi.org/10.3390/polym13244424 - 16 Dec 2021

Cited by 7 | Viewed by 2679

Abstract

We have previously demonstrated that poly(N-cyanomethylacrylamide) (PCMAm) exhibits a typical upper-critical solution temperature (UCST)-type transition, as long as the molar mass of the polymer is limited, which was made possible through the use of reversible addition-fragmentation chain transfer (RAFT) radical polymerization. In this research article, we use for the first time N-cyanomethylacrylamide (CMAm) in a typical aqueous dispersion polymerization conducted in the presence of poly(N,N-dimethylacrylamide) (PDMAm) macroRAFT agents. After assessing that well-defined PDMAm-b-PCMAm diblock copolymers were formed through this aqueous synthesis pathway, we characterized in depth the colloidal stability, morphology and temperature-responsiveness of the dispersions, notably using cryo-transmission electron microscopy (cryo-TEM), dynamic light scattering (DLS), small angle X-ray scattering (SAXS) and turbidimetry. The combined analyses revealed that stable nanometric spheres, worms and vesicles could be prepared when the PDMAm block was sufficiently long. Concerning the thermoresponsiveness, only diblocks with a PCMAm block of a low degree of polymerization (DP_n,PCMAm < 100) exhibited a UCST-type dissolution upon heating at low concentration. In contrast, for higher DP_n,PCMAm, the diblock copolymer nano-objects did not disassemble. At sufficiently high temperatures, they rather exhibited a temperature-induced secondary aggregation of primary particles. In summary, we demonstrated that various morphologies of nano-objects could be obtained via a typical polymerization-induced self-assembly (PISA) process using PCMAm as the hydrophobic block. We believe that the development of this aqueous synthesis pathway of novel PCMAm-based thermoresponsive polymers will pave the way towards various applications, notably as thermoresponsive coatings and in the biomedical field. Full article

(This article belongs to the Special Issue Polymerization-Induced Self-Assembly (PISA))

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14 pages, 2900 KiB

Open AccessArticle

Dextran-Coated Latex Nanoparticles via Photo-RAFT Mediated Polymerization Induced Self-Assembly

by Valeria Lizeth Romero Castro, Brahim Nomeir, Ana Andreea Arteni, Malika Ouldali, Jean-Luc Six and Khalid Ferji

Polymers 2021, 13(23), 4064; https://doi.org/10.3390/polym13234064 - 23 Nov 2021

Cited by 14 | Viewed by 3643

Abstract

Polysaccharide coated nanoparticles represent a promising class of environmentally friendly latex to replace those stabilized by small toxic molecular surfactants. We report here an in situ formulation of free-surfactant core/shell nanoparticles latex consisting of dextran-based diblock amphiphilic copolymers. The synthesis of copolymers and the immediate latex formulation were performed directly in water using a photo-initiated reversible addition fragmentation chain transfer-mediated polymerization induced self-assembly strategy. A hydrophilic macromolecular chain transfer-bearing photosensitive thiocarbonylthio group (eDexCTA) was first prepared by a modification of the reducing chain end of dextran in two steps: (i) reductive amination by ethylenediamine in the presence of sodium cyanoborohydride, (ii) then introduction of CTA by amidation reaction. Latex nanoparticles were then formulated in situ by chain-extending eDexCTA using 2-hydroxypropyl methacrylate (HPMA) under 365 nm irradiation, leading to amphiphilic dextran-b-poly(2-hydroxypropyl methacrylate) diblock copolymers (DH_X). Solid concentration (SC) and the average degree of polymerization -

\overset{ˉ}{X_{n}}

- of PHPMA block (X) were varied to investigate their impact on the size and the morphology of latex nanoparticles termed here SCDH_X. Light scattering and transmission electron microscopy analysis revealed that SCDH_X form exclusively spherical nano-objects. However, the size of nano-objects, ranging from 20 nm to 240 nm, increases according to PHPMA block length. Full article

(This article belongs to the Special Issue Polymerization-Induced Self-Assembly (PISA))

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