Periodic Reporting for period 4 - SYNMAT (Synthesis of Functional Multi-Component Supramolecular Systems and Materials)
Reporting period: 2023-04-01 to 2024-09-30
This ERC proposal had as the overall objectives to understand and advance supramolecular polymers for societal benefit. The following problem/issue are being addressed. The challenge at the heart of this research is the design and synthesis of complex supramolecular materials with tailored functions. Traditional methods of polymerization, whether covalent or non-covalent, have limitations in achieving the sophisticated architectures required for advanced applications in biomedicine, sustainability, and energy conversion. A major gap exists between self-assembly processes and more controlled multi-step synthetic approaches, restricting the ability to design highly functional materials. Addressing this limitation requires novel synthetic strategies that allow for greater precision and complexity in material design. With our long history in supramolecular polymers, we have those structures are main component to address important topics for society. Materials science plays a crucial role in healthcare, environmental sustainability, and renewable energy. Developing functional supramolecular polymers could lead to breakthroughs in:
1) Regenerative Medicine – New biomaterials could support stem cell and organoid growth, enabling advancements in tissue engineering and artificial extracellular matrices.
2) Sustainable Materials – The ability to engineer self-assembling materials contributes to eco-friendly polymers that reduce reliance on non-biodegradable plastics.
3) Green Hydrogen Production – Innovations in chiral supramolecular structures could improve the efficiency of electrochemical water splitting, a key technology for clean energy solutions.
By bridging gaps in polymer chemistry, this research opens the door to next-generation materials that are not only structurally complex but also offer real-world benefits in these critical areas. The overall are objectives the following. This ERC project aimed to push the boundaries of supramolecular polymer chemistry by introducing multi-step non-covalent synthesis techniques. The overarching goal was to expand the possibilities for creating functional materials that go beyond what is achievable with self-assembly alone. The research was divided into three interconnected areas:
1) Comparing Supramolecular and Covalent Polymers.
2) Developing Multi-Component Hydrogels for Biomedical Applications.
3) Harnessing Chirality for Spin-Selective Chemistry and Sustainable Energy.
By closing the gap between self-assembly and controlled non-covalent synthesis, this project has opened new doors for the design of lifelike materials with practical applications. The results provide a foundation for further scientific advancements, with far-reaching implications in biomedicine, sustainability, and renewable energy.
1) Regenerative Medicine – New biomaterials could support stem cell and organoid growth, enabling advancements in tissue engineering and artificial extracellular matrices.
2) Sustainable Materials – The ability to engineer self-assembling materials contributes to eco-friendly polymers that reduce reliance on non-biodegradable plastics.
3) Green Hydrogen Production – Innovations in chiral supramolecular structures could improve the efficiency of electrochemical water splitting, a key technology for clean energy solutions.
By bridging gaps in polymer chemistry, this research opens the door to next-generation materials that are not only structurally complex but also offer real-world benefits in these critical areas. The overall are objectives the following. This ERC project aimed to push the boundaries of supramolecular polymer chemistry by introducing multi-step non-covalent synthesis techniques. The overarching goal was to expand the possibilities for creating functional materials that go beyond what is achievable with self-assembly alone. The research was divided into three interconnected areas:
1) Comparing Supramolecular and Covalent Polymers.
2) Developing Multi-Component Hydrogels for Biomedical Applications.
3) Harnessing Chirality for Spin-Selective Chemistry and Sustainable Energy.
By closing the gap between self-assembly and controlled non-covalent synthesis, this project has opened new doors for the design of lifelike materials with practical applications. The results provide a foundation for further scientific advancements, with far-reaching implications in biomedicine, sustainability, and renewable energy.
Throughout the project, several major discoveries were made:
1) Nanoscopic morphology of water-soluble supramolecular polymers. Advanced techniques were used to map out the nanoscopic morphology of water-soluble supramolecular polymers, significantly enhancing the understanding of their structural behavior.
2) Synthesis of novel discrete oligomers. Despite initial challenges, the team successfully synthesized discrete oligomers and nitrogen-based discotic molecules that self-assemble into supramolecular polymers, aligning with project goals.
3) Bridging covalent and non-covalent polymerization. A groundbreaking method was developed to close the gap between covalent and non-covalent polymers, unlocking new possibilities for designing sustainable materials.
4) Breakthrough in bioactive hydrogels. Using super-resolution microscopy, we observed unexpected clustering of receptors and ligands in dynamic hydrogels. This discovery brings supramolecular hydrogels closer to mimicking natural extracellular matrices, advancing the field of biomedical materials.
5) Discovery of a unique gel-sol-gel-sol transition. A novel material was identified that undergoes a reversible phase transition—transforming from a hydrogel to a liquid upon dilution, then back to a gel upon further dilution. This dilution-induced self-assembly is a unique phenomenon in multicomponent supramolecular systems.
6) Advancing chirality-driven chemistry for green energy. The project demonstrated that chiral molecules could enhance the oxygen evolution reaction (OER) in electrochemical water splitting, particularly in systems with a high nitrogen/carbon ratio.
In conclusion, the research was highly successful after a somewhat slow start. The results are unforeseen and it is only the beginning. Where the overall objective remains challenging the results in the endeavor to reach that ultimate goal, we discovered many new aspects; see also below. Up to now, 29 papers are published (all open access), but many more are still in the process of writing. The results obtained are also a start for new projects mainly in collaboration with others. Especially where our new functional materials can be used in optoelectronic devices and biomaterial applications. Finally, the project created a completely new insights into the original of homochirality in nature, which has now become the major research topic of the group today. Without the ERC results, this idea which is a spin-off from the so-called Chirality-Induced Spin Selectivity (CISS) effect could never been emerged.
The project has pushed the boundaries of supramolecular chemistry, revealing that combining covalent and non-covalent synthesis offers far greater potential than previously anticipated. The unexpected self-assembly behaviors, receptor clustering, and chirality-driven chemistry highlight the vast, untapped possibilities in functional materials. Beyond fundamental science, these discoveries have direct implications for biomedicine, sustainable polymers, and green energy technologies.
1) Nanoscopic morphology of water-soluble supramolecular polymers. Advanced techniques were used to map out the nanoscopic morphology of water-soluble supramolecular polymers, significantly enhancing the understanding of their structural behavior.
2) Synthesis of novel discrete oligomers. Despite initial challenges, the team successfully synthesized discrete oligomers and nitrogen-based discotic molecules that self-assemble into supramolecular polymers, aligning with project goals.
3) Bridging covalent and non-covalent polymerization. A groundbreaking method was developed to close the gap between covalent and non-covalent polymers, unlocking new possibilities for designing sustainable materials.
4) Breakthrough in bioactive hydrogels. Using super-resolution microscopy, we observed unexpected clustering of receptors and ligands in dynamic hydrogels. This discovery brings supramolecular hydrogels closer to mimicking natural extracellular matrices, advancing the field of biomedical materials.
5) Discovery of a unique gel-sol-gel-sol transition. A novel material was identified that undergoes a reversible phase transition—transforming from a hydrogel to a liquid upon dilution, then back to a gel upon further dilution. This dilution-induced self-assembly is a unique phenomenon in multicomponent supramolecular systems.
6) Advancing chirality-driven chemistry for green energy. The project demonstrated that chiral molecules could enhance the oxygen evolution reaction (OER) in electrochemical water splitting, particularly in systems with a high nitrogen/carbon ratio.
In conclusion, the research was highly successful after a somewhat slow start. The results are unforeseen and it is only the beginning. Where the overall objective remains challenging the results in the endeavor to reach that ultimate goal, we discovered many new aspects; see also below. Up to now, 29 papers are published (all open access), but many more are still in the process of writing. The results obtained are also a start for new projects mainly in collaboration with others. Especially where our new functional materials can be used in optoelectronic devices and biomaterial applications. Finally, the project created a completely new insights into the original of homochirality in nature, which has now become the major research topic of the group today. Without the ERC results, this idea which is a spin-off from the so-called Chirality-Induced Spin Selectivity (CISS) effect could never been emerged.
The project has pushed the boundaries of supramolecular chemistry, revealing that combining covalent and non-covalent synthesis offers far greater potential than previously anticipated. The unexpected self-assembly behaviors, receptor clustering, and chirality-driven chemistry highlight the vast, untapped possibilities in functional materials. Beyond fundamental science, these discoveries have direct implications for biomedicine, sustainable polymers, and green energy technologies.
Now at the end of this very successful ERC project, it can be stated that the number of unexpected results were obtained that emerged by studying the research topics as described. We could not expect that studying supramolecular polymers using multiple components, so many new phenomena emerged. Or this three examples can be mentioned here. First the clustering of receptors and ligands in dynamic systems where the receptors are on a supported bilayer and the ligands in a supramolecular polymer, gave totally new insights into the dynamic nature of the interactions. Reciprocity in dynamics of supramolecular biosystems for the clustering of ligands and receptors showed unprecedented multivalency and activity; work that is with PNAS. Secondly, we discovered a unique gel-sol-gel-sol transitions by dilution, making the so-called dilution-induced assembly a well-accepted phenomenon with deep impact in many fields of science and engineering, work that is published in Science. Thirdly, as a follow-up on using chiral surfactants in combination with achiral water-soluble supramolecular polymers, we observed an unprecedented and not expected amplification of asymmetry and it is now the main focus for the follow-up projects in the group. .
Finally and maybe the most impressive finding is the observation of highly ordered liquid-liquid phase separated phases using very long and highly supramolecular fibers. This work is published in Nature and is now part of many research groups in biomaterials for interactions of biomaterials and cells. .
Finally and maybe the most impressive finding is the observation of highly ordered liquid-liquid phase separated phases using very long and highly supramolecular fibers. This work is published in Nature and is now part of many research groups in biomaterials for interactions of biomaterials and cells. .