Gaëlle Mellot

Sorbonne Université

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Jutta Rieger

Institut Parisien de Chimie Moléculaire

François Stoffelbach

Institut Parisien de Chimie Moléculaire

Laurent Bouteiller

Institut Parisien de Chimie Moléculaire

Jean‐Michel Guigner

Institut de minéralogie, de physique des matériaux et de cosmochimie

Costantino Creton

ESPCI Paris

Rint P. Sijbesma

Eindhoven University of Technology

Diederik van Luijk

Eindhoven University of Technology

Jacques Jestin

Laboratoire Léon Brillouin

Jacques Jestin

CEA Paris-Saclay

Yingjun Chen

Fudan University

Cooperative Institutions

Centre National de la Recherche Scientifique

Sorbonne Université

Délégation Paris 6

UPMC Health System

Institut Parisien de Chimie Moléculaire

Sciences et Ingénierie de la Matière Molle

Laboratoire de Chimie des Polymères Organiques

Commissariat à l'Énergie Atomique et aux Énergies Alternatives

3M (United States)

Délégation Ile-de-France Villejuif

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Crucial Role of the Spacer in Tuning the Length of Self-Assembled Nanorods

Macromolecules (2020)

Shuaiyuan Han Gaëlle Mellot Sandrine Pensec Jutta Rieger François Stoffelbach

Polymeric supramolecular nanorods were prepared in toluene by self-assembly of tris(urea) stickers connected on both sides through alkyl spacers of different lengths to short polystyrene (PS) arms. Several tris(urea) initiators or chain transfer agents were synthesized straightforwardly and used to grow well-defined PS arms via atom transfer radical polymerization (ATRP) or reversible addition fragmentation chain transfer (RAFT) polymerization. Self-assembly was investigated by means of Fourier-transform infrared (FTIR) spectroscopy and light/neutron scattering. A dramatic impact of the spacer separating the tris(urea) sticker from the PS arms on the extent of self-assembly was observed in toluene as long as the degree of polymerization of the PS arms (x) was kept short (x ∼ 10). Indeed, supramolecular nanorods several hundreds of nanometers in length for a few nanometers in radius were obtained with a spacer consisting of nine atoms, whereas five times shorter nanorods were obtained for a spacer of only five atoms, and spherical particles were found in the absence of any spacer, all other parameters remaining unchanged. These results reveal the possibility to tune the length of polymer-decorated supramolecular nanorods with minimal modification of the assembling sticker and without affecting the functionality of the rods.

Nanorod

Atom-transfer radical-polymerization

Polystyrene

Hydrodynamic radius

10.1021/acs.macromol.9b01928

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Citations (10)

Bisurea-Functionalized RAFT Agent: A Straightforward and Versatile Tool toward the Preparation of Supramolecular Cylindrical Nanostructures in Water

Macromolecules (2018)

Gaëlle Mellot Jean‐Michel Guigner Jacques Jestin Laurent Bouteiller François Stoffelbach

We report a versatile and simple approach to produce cylindrical micelles by the direct dissolution of polymers in water. The developed strategy relies on a RAFT agent functionalized by a bisurea sticker that allowed to synthesize a series of α-bisurea-functionalized poly(N,N-dimethylacrylamide) (PDMAc), poly(acrylic acid) (PAA), polyacrylamide (PAM), and poly(2-(N,N-dimethylamino)ethyl acrylate) (PDMAEA) with number-average degrees of polymerization (DPn) varying from about 10 to 50. Their spontaneous self-assembly in water was studied by electron microscopy (cryo-TEM), neutron scattering (SANS), and calorimetry (ITC) analyses which showed that long cylindrical micelles are spontaneously formed in water. The crucial role of the bisurea sticker end-groups was established by comparison with the corresponding bisurea-free model polymers that only formed spherical micelles. Finally, we have shown that it is possible to trigger reversibly the assembly/disassembly of the nanofibers by pH changes.

Raft

10.1021/acs.macromol.8b02156

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Citations (25)

Beyond Simple AB Diblock Copolymers: Application of Bifunctional and Trifunctional RAFT Agents to PISA in Water

Macromolecular Rapid Communications (2018)

Gaëlle Mellot Patricia Beaunier Jean‐Michel Guigner Laurent Bouteiller Jutta Rieger

The influence of the macromolecular reversible addition-fragmentation chain transfer (macro-RAFT) agent architecture on the morphology of the self-assemblies obtained by aqueous RAFT dispersion polymerization in polymerization-induced self-assembly (PISA) is studied by comparing amphiphilic AB diblock, (AB)2 triblock, and triarm star-shaped (AB)3 copolymers, constituted of N,N-dimethylacrylamide (DMAc = A) and diacetone acrylamide (DAAm = B). Symmetrical triarm (AB)3 copolymers could be synthesized for the first time in a PISA process. Spheres and higher order morphologies, such as worms or vesicles, could be obtained for all types of architectures and the parameters that determine their formation have been studied. In particular, we found that the total DPn of the PDMAc and the PDAAm segments, i.e., the same overall molar mass, at the same Mn (PDMAc)/Mn (PDAAm) ratio, rather than the individual length of the arms determined the morphologies for the linear (AB)2 and star shaped (AB)3 copolymers obtained by using the bi- and trifunctional macro-RAFT agents.

Raft

10.1002/marc.201800315

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Citations (44)

Correction: Mechanochemical tools for polymer materials

Chemical Society Reviews (2021)

Yingjun Chen Gaëlle Mellot Diederik van Luijk Costantino Creton Rint P. Sijbesma

Correction for ‘Mechanochemical tools for polymer materials’ by Yinjun Chen et al., Chem. Soc. Rev., 2021, 50, 4100–4140, DOI: 10.1039/D0CS00940G.

10.1039/d1cs90042k

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Citations (6)

Combination of the supramolecular chemistry and the RAFT-mediated PISA to synthesize nanofibers in water

HAL (Le Centre pour la Communication Scientifique Directe) (2019)

Gaëlle Mellot

Raft

Source

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Citations (0)

Templated PISA: Driving Polymerization‐Induced Self‐Assembly towards Fibre Morphology

Angewandte Chemie (2018)

Gaëlle Mellot Jean‐Michel Guigner Laurent Bouteiller François Stoffelbach Jutta Rieger

Abstract Dispersions of block copolymer fibres in water have many potential applications and can be obtained by polymerization‐induced self‐assembly (PISA), but only under very restricted experimental conditions. In order to enlarge this experimental window, we introduced a supramolecular moiety, a hydrogen‐bonded bis‐urea sticker, in the macromolecular reversible addition fragmentation chain transfer (RAFT) agent to drive the morphology of the nano‐objects produced by RAFT‐mediated PISA towards the fibre morphology. This novel concept is tested in the synthesis of a series of poly( N , N ‐dimethylacrylamide)‐b‐poly(2‐methoxyethyl acrylate) (PDMAc‐b‐PMEA) diblock copolymers prepared by dispersion polymerization in water. The results prove that the introduction of the templating bis‐urea stickers into PISA greatly promotes the formation of fibres in a large experimental window.

Chain transfer

Raft

Dispersion polymerization

Moiety

Morphology

10.1002/ange.201809370

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Citations (35)

Unexpected thermo-responsiveness of bisurea-functionalized hydrophilic polymers in water

Journal of Colloid and Interface Science (2020)

Gaëlle Mellot Jean‐Michel Guigner Jacques Jestin Laurent Bouteiller François Stoffelbach

Cloud point

Supramolecular Polymers

Raft

10.1016/j.jcis.2020.07.147

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Citations (7)

Mechanochemical tools for polymer materials

Chemical Society Reviews (2021)

Yinjun Chen Gaëlle Mellot Diederik van Luijk Costantino Creton Rint P. Sijbesma

This review aims to provide a field guide for the implementation of mechanochemistry in synthetic polymers by summarizing the molecules, materials, and methods that have been developed in this field.

10.1039/d0cs00940g

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Citations (324)

Templated PISA: Driving Polymerization‐Induced Self‐Assembly towards Fibre Morphology

Angewandte Chemie International Edition (2018)

Gaëlle Mellot Jean‐Michel Guigner Laurent Bouteiller François Stoffelbach Jutta Rieger

Dispersions of block copolymer fibres in water have many potential applications and can be obtained by polymerization-induced self-assembly (PISA), but only under very restricted experimental conditions. In order to enlarge this experimental window, we introduced a supramolecular moiety, a hydrogen-bonded bis-urea sticker, in the macromolecular reversible addition fragmentation chain transfer (RAFT) agent to drive the morphology of the nano-objects produced by RAFT-mediated PISA towards the fibre morphology. This novel concept is tested in the synthesis of a series of poly(N,N-dimethylacrylamide)-b-poly(2-methoxyethyl acrylate) (PDMAc-b-PMEA) diblock copolymers prepared by dispersion polymerization in water. The results prove that the introduction of the templating bis-urea stickers into PISA greatly promotes the formation of fibres in a large experimental window.

Chain transfer

Dispersion polymerization

Raft

Moiety

Morphology

10.1002/anie.201809370

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Citations (102)

Structural insights into nanofibers formed by templated polymerization-induced self-assembly through combined SANS and AFM characterizations

Journal of Molecular Liquids (2025)

Gaëlle Mellot Mathieu Chevereau Laurent Bouteiller François Stoffelbach Marylène Vayer

10.1016/j.molliq.2025.127104

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Citations (0)