Solvation Entropy as a Lever for Steering the Macroscopic Properties of a Functional Supramolecular Helical Polymer

H Huanjun Kong (Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France) M Mayte A. Martínez‐Aguirre (Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France) Y Yan Li T Tomoyuki Ikai (Department of Molecular and Macromolecular Chemistry, Graduate School of Engineering) E Eiji Yashima (Department of Molecular and Macromolecular Chemistry, Graduate School of Engineering) G Gangamallaiah Velpula (Division of Molecular Imaging and Photonics, Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium) S Steven De Feyter (Division of Molecular Imaging and Photonics, Department of Chemistry) P Pierre‐Antoine Albouy (Laboratoire de Physique des Solides CNRS Université Paris‐Sud Université Paris‐Saclay Orsay 91400 France) K Komivi Akpo (Service de Chimie des Matériaux Nouveaux Institut de Recherche sur les Matériaux Université de Mons Place du Parc, 20 Mons B‐7000 Belgium) P Patrick Brocorens (Service de Chimie des Matériaux Nouveaux Institut de Recherche sur les Matériaux Université de Mons Place du Parc, 20 Mons B‐7000 Belgium) R Roberto Lazzaroni (Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons, Place du Parc 20, Mons 7000, Belgium) L Laurent Bouteiller (Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France) M Matthieu Raynal (Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France)

Abstract

Abstract Solvent‐solute interactions are utterly important in supramolecular polymers (SPs), yet the high responsivity of SPs to solvent polarity makes it challenging to play on other solvation effects to tune their macroscopic properties in a rational manner. Herein, we report the characterization at various scales of the assembly properties of a C 2 ‐symmetric benzene‐1,3,5‐tricarboxamide monomer with two (1 S )‐methylheptyl moieties and one diphenylphosphino group as lateral chains. Our investigation reveals a highly cooperative structural transition between two SP states, which can exquisitely be tuned by solvents of similar polarities, leading to variation of the transition temperature (T*) over a range of 85 K. The structural transition was detected in 4 pure solvents and 13 toluene/cosolvent mixtures; a fair relationship is determined between T* and the solvent molar volume. The transition is only weakly favored by enthalpy (by ca. 2 kJ.mol −1 at 286 K). However, minimization of the entropic cost leads to a notable increase in the T*. This allows a fine tuning of the thermothickening and catalytic properties of the resulting SPs auguring that solvation, and notably solvation entropy, may constitute an important lever for steering SPs structure and properties.

Article Details

Volume / Issue Vol. 65, Issue 3
Published January 16, 2026
ISSN 1433-7851
Publisher Wiley

Journal Info

Angewandte Chemie International Edition

Wiley

ISSN: 1433-7851 Physical Sciences

Authors (13)

H

Huanjun Kong

Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France

M

Mayte A. Martínez‐Aguirre

Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France

Y

Yan Li

T

Tomoyuki Ikai

Department of Molecular and Macromolecular Chemistry, Graduate School of Engineering

E

Eiji Yashima

Department of Molecular and Macromolecular Chemistry, Graduate School of Engineering

G

Gangamallaiah Velpula

Division of Molecular Imaging and Photonics, Department of Chemistry, KU Leuven, Celestijnenlaan 200F, Leuven 3001, Belgium

S

Steven De Feyter

Division of Molecular Imaging and Photonics, Department of Chemistry

P

Pierre‐Antoine Albouy

Laboratoire de Physique des Solides CNRS Université Paris‐Sud Université Paris‐Saclay Orsay 91400 France

K

Komivi Akpo

Service de Chimie des Matériaux Nouveaux Institut de Recherche sur les Matériaux Université de Mons Place du Parc, 20 Mons B‐7000 Belgium

P

Patrick Brocorens

Service de Chimie des Matériaux Nouveaux Institut de Recherche sur les Matériaux Université de Mons Place du Parc, 20 Mons B‐7000 Belgium

R

Roberto Lazzaroni

Laboratory for Chemistry of Novel Materials, Materials Research Institute, University of Mons, Place du Parc 20, Mons 7000, Belgium

L

Laurent Bouteiller

Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France

M

Matthieu Raynal

Sorbonne Université CNRS Institut Parisien de Chimie Moléculaire 4 Place Jussieu Paris 75005 France