TETHERED project

For many years, polymers were built exclusively from strong bonds. Nowadays, inspired by nature, scientists have realized the importance of weak bonds, which are reversible and introduce dynamic behaviors into otherwise static systems. Incorporating such bonds into polymeric materials give them appealing properties such as self-healing, stimuli responsiveness, ability to resist fracture, or facilitated recycling. However, it also introduces important drawbacks such as lower mechanical strength or permanent deformation under stress, so that compromises had to be made for more than two decades. To solve this issue, we propose to develop materials containing weak bonds while suppressing the major drawbacks. The central concept is the use of tethered weak bonds: bonds in which the components stay in close proximity after bond rupture thanks to a molecular tether linking them. We will study these materials across all length and time scales, from the single molecule level to the macroscopic level, and will investigate both the rupture of bonds and their reformation. The obtained results will allow the development of a predictive model linking material structure and mechanical properties that will be valuable for the future development of weak bond-based materials showing enhanced properties.

 

EoS partners

Publications

 

Design and Applications of Dynamic Hydrogels Based on Reversible C=N Bonds

H. Yang, C.A. Fustin

Macromol. Chem. Phys. 2023, 2300211

DOI: 10.1002/macp.202300211

 

Dynamics of ring-containing polymers: Macromolecular rotaxanes, polyrotaxanes and slide-ring networks

S. Ghiassinejad, M. Ahmadi, E. van Ruymbeke, C.A. Fustin

Progr. Polym. Sci. 2024, 155, 101854

DOI: 10.1016/j.progpolymsci.2024.101854

 

Effect of Ring Mobility on the Dynamics of the Slide-Ring Gels

S. Ghiassinejad, A. Kumar Sharma, C.A. Fustin, E. van Ruymbeke

Chem. Mater. 2024, 36, 8311-8322

DOI: 10.1021/acs.chemmater.4c01235

 

Viscoelastic Properties of Metallo-Supramolecular Networks: Relationship Between Sticker/Entanglement Dynamics and Terminal Relaxation

P. de Wergifosse, R. Lyons, C.A. Fustin, E. van Ruymbeke

Macromolecules 2025, 58, 222-239

DOI: 10.1021/acs.macromol.4c01300

 

Response of a tethered Zn-bis-terpyridine complex to an external mechanical force: A computational study of the roles of the tether and solvent

S. Ghose, A.S. Duwez, C.A. Fustin, F. Remacle

Phys. Chem. 2025, 129, 3423-3434

DOI: 10.1021/acs.jpca.4c08639

 

Tuning the Viscoelastic Properties of Dioxazaborocane Vitrimers via Chemical Design of the Functional Groups

A. Quinteros-Sedano, E. van Ruymbeke

Macromolecules 2026, 59, 1781-1788

DOI: 10.1021/acs.macromol.5c032433

 

Nonlinear Shear and Extensional Rheology of Telechelic Metallosupramolecular Networks

P. de Wergifosse, M. Dalne, A. Quinteros-Sedano, E. van Ruymbeke

Macromolecules 2026, 59, 4636-4649

DOI: 10.1021/acs.macromol.6c00463

 

Multiple template site nitrogen atom deletions from rotaxanes, catenanes and a molecular knot

D P Couto, Q Lin, J B M Whittingham, D J Tetlow, J Zhong, P Howlader and D A Leigh

J. Am. Chem. Soc. 2025, 147, 33304-33314

DOI: 10.1021/jacs.5c12617

 

A double exponential chirp waveform for noisy rheology

J. L. Waeterloos, G. H. McKinley, C. Clasen

Rheologica Acta 2025, 64, 633-646

DOI: 10.1007/s00397-025-01521-y

 

Second normal stress difference measurement via interfacial deformation of stratified flow into a closed-channel

L. Passaro, E. Pashkovski, C. Clasen

Rheologica Acta 2025, 64, 801-813

DOI: 10.1007/s00397-025-01521-y

 

Elastic, strong and tough ionically conductive elastomers

B. Yiming, S. Hubert, A. Cartier, B. Bresson, G. Mello, A. Ringuede, C. Creton

Nature Commun. 2025, 16, 431

DOI: 10.1038/s41467-024-55472-8

 

Force Reveals Hidden Conformations and Dissociation Pathways in Individual π-Interacting Dimers

C. Franceschini, D. Brandt, M. Ledent, T. Carabin, H. Traeger, J. M. Clough, L. Muccioli, A. S. Duwez, C. Weder, Y. Olivier, D. Sluysmans

Angew. Chem. Int. Ed. 2026, ahead of print

DOI: 10.1002/anie.9238302

 

Stretchable Ionic Conductors: Balancing Mechanical Properties and Ionic Conductivity

B. Yiming, Z. Jia, C. Creton

Chem. Rev. 2025, 125, 10457–10491

DOI: 10.1021/acs.chemrev.5c00257