Servizio Comunitario di Informazione in materia di Ricerca e Sviluppo - CORDIS

Periodic Report Summary 1 - SUPOLEN (Supramolecular assembly of polymeric structures: a novel route to enhance soft materials properties)

Supramolecular polymeric assemblies represent an emerging, promising class of systems with superior versatility compared to their covalent polymeric counterparts (see figure). They offer exciting new opportunities for stimuli-responsive structures exhibiting reversible tunable properties, with applications in foodstuff, coatings, cost-efficient processes or biomedical areas.

To explore their potential and define strategies for designing novel materials amenable to contemporary needs, a fundamental understanding of their very complex and diverse multiscale supramolecular structure and dynamics is needed. In this regard, a synergy of synthetic chemistry (including both model and industrial systems), physical experiment and modeling are necessary. The objective of SUPOLEN is to understand and tailor the structure and dynamics of supramolecular polymers based on well-defined building blocks, mainly monodisperse linear and star-like polymers. The systematic, thorough study of their behavior offers many possibilities for tailoring their organization and dynamic response, and allows tackling important questions such as:

1. understanding the combined effect of the dynamics of the associating groups (strength, position, number and nature) and the internal dynamics of the building blocks (entanglements and architecture);
2. exploring the role played by external stimuli;
3. investigating their behavior in solution as well as in the melt; and
4. developing predictive tools for designing new materials.

To this end, we focus on specific systems in order to propose a global picture to explain their dynamics and properties.

For example, as entangled chains bearing sticky groups along their backbone, we worked on well-defined thermoplastic elastomers (TPEs). Scattering data for the TPEs allowed us to determine the average size and organization of the crystallite formed by the association of the hard blocks. These ones were found to be in rod-like structures. Furthermore, higher order of organization was also pointed out, involving the association of several rod-like structures into larger objects. Thanks for flash DSC measurements, we could further investigate the association dynamics of these systems and demonstrate the possible existence of temperature and rate-dependent pseudo-equilibrium states in which the systems could be trapped. This allowed us to understand the linear viscoelastic properties and in particular, the thixotropy of these samples, in function of their thermal history: it was concluded that the final properties and elasticity of such TPEs are strongly dependent on the mobility of the entire chains. These ones need to be able to move and diffuse in order to create stronger crystallite structures, giving rise to enhanced material properties. We are now developing coarse-grained modelling in order to rationalize these finding and exploit them for the development of new smart TPEs.

As another example, the dynamics and self-healing properties of supramolecular polymers formed by telechelic entangled star chains were investigated. Supramolecular bonds were created from metal-ligand associations (see Figure) or via multiple hydrogen bonding. We determined their main characteristics, both in the linear and nonlinear regimes of deformations, with special attention to the inter-connected dynamics of supramolecular bonds and of the entanglement as well as the thermo-rheological properties of such materials. We are now trying to summarize all these results into a global molecular picture.

Based on our results, we would like to exploit the combined effect of supramolecular and entanglement dynamics to investigate the development of new, smart materials, which combine properties which cannot be combined in more classical polymer materials, such as shape memory and self-healing properties, or toughness and extensibility.

These scientific results have been made possible through the multidisciplinarity and complementarity of project partners. Exchange visits and industrial secondments, as well as regular project meetings, allow students to collaborate.
Students have been trained to a high level through modules relating to polymer science. An elementary module gave students a bird’s-eye view of selected aspects of polymers such as synthesis, dynamics, rheology, light-scattering and industrial applications. Following this, students have had opportunities to follow more advanced courses: computational physics and (hands-on) advanced molecular rheology. In addition, a summer school has also been organized by SUPOLEN. Students received an intense week of high-level lectures with world-class experts in their field.

An active programme with our 3 industrial partners has ensured that students receive significant exposure to industry – mainly through industrial secondments, exchange of industry-relevant samples, cross-linking of theory and simulation with industry needs, and an industrial workshop.
This training has complemented students’ access to local training, which has been defined in a personal career development plan for each student.

Dissemination activities have been taken on by the students themselves, with newsletters published after every meeting, and youtube videos posted. Publications and attendance at conferences also offer a way to disseminate scientific knowledge – to date SUPOLEN has published 16 articles, and presented at 24 conferences.

Project coordinator: Prof. Evelyne van Ruymbeke, Université catholique de Louvain
Project website:

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Life Sciences