Steuerung von dissipative molekulare Strukturen

• Antragsteller: Professor Dr. Job Boekhoven
• Fachliche Zuordnung: Statistische Physik, Nichtlineare Dynamik, Komplexe Systeme, Weiche und fluide Materie, Biologische Physik ; Organische Molekülchemie - Synthese, Charakterisierung ; Polymermaterialien
• Förderung: Förderung von 2018 bis 2023
• Projektkennung: Deutsche Forschungsgemeinschaft (DFG) - Projektnummer 411722921

• Erstellungsjahr: 2023

Zusammenfassung der Projektergebnisse

Biological molecular assemblies, like the microtubules or the actin network, almost always exist out of equilibrium. In contrast, human-made molecular assemblies typically exist in equilibrium with their environment. Inspired by biological assemblies, researchers have started exploring artificial dissipative non-equilibrium materials. These dissipative assemblies have superior properties compared to their in-equilibrium counterparts, which include the ability to be controlled over space and time, rapidly switch morphology in response to a small change in their environment and the ability to self-heal. Researchers have reported exciting dissipative molecular assemblies driven by chemical fuels. However, there remains a fundamental need for more understanding of the governing principles of these assemblies. For instance, we must understand how the fuel consumption rate affects morphology. Alternatively, we cannot predict how the size of the assemblies scales with the kinetics of building block activation. This fundamental knowledge hampers us from applying these materials the versatilely as biology does. This three-year project aimed to understand how the kinetics of building block activation and deactivation affect the morphology, size, and stability of chemically fueled assemblies. We started by developing assemblies in which the building block activation rate equals deactivation, a so-called steady state. We then coupled the chemical reaction cycle to the phase separation into droplets, where we found exciting new behaviors. In the second part of the project, we elucidated the mechanism by which chemically fueled supramolecular materials could self-heal. In future works, we will use the droplets as a platform for synthesizing life. We will combine these self-sustaining compartments with self-replicating molecules as a genotype. The selfhealing materials will be studied more deeply, and the mechanisms we have found will be generalized towards other materials, including rubbers.

Projektbezogene Publikationen (Auswahl)

• Active coacervate droplets as a model for membraneless organelles and protocells. Nature Communications, 11(1).
  Donau, Carsten; Späth, Fabian; Sosson, Marilyne; Kriebisch, Brigitte A. K.; Schnitter, Fabian; Tena-Solsona, Marta; Kang, Hyun-Seo; Salibi, Elia; Sattler, Michael; Mutschler, Hannes & Boekhoven, Job
  
• Regulating Chemically Fueled Peptide Assemblies by Molecular Design. Journal of the American Chemical Society, 142(33), 14142-14149.
  Dai, Kun; Fores, Jennifer Rodon; Wanzke, Caren; Winkeljann, Benjamin; Bergmann, Alexander M.; Lieleg, Oliver & Boekhoven, Job
  
• Synthesis and characterization of chemically fueled supramolecular materials driven by carbodiimide-based fuels. Nature Protocols, 16(8), 3901-3932.
  Schnitter, Fabian; Bergmann, Alexander M.; Winkeljann, Benjamin; Rodon, Fores Jennifer; Lieleg, Oliver & Boekhoven, Job
  
• A chemically fueled supramolecular glue for self-healing gels. Chemical Science, 13(38), 11411-11421.
  Rodon-Fores, Jennifer; Würbser, Michaela A.; Kretschmer, Martin; Rieß, Benedikt; Bergmann, Alexander M.; Lieleg, Oliver & Boekhoven, Job
  
• Phase Transitions in Chemically Fueled, Multiphase Complex Coacervate Droplets. Angewandte Chemie, 134(46).
  Donau, Carsten; Späth, Fabian; Stasi, Michele; Bergmann, Alexander M. & Boekhoven, Job
  
• Regulating DNA-Hybridization Using a Chemically Fueled Reaction Cycle. Journal of the American Chemical Society, 144(48), 21939-21947.
  Stasi, Michele; Monferrer, Alba; Babl, Leon; Wunnava, Sreekar; Dirscherl, Christina Felicitas; Braun, Dieter; Schwille, Petra; Dietz, Hendrik & Boekhoven, Job
  
• Tunable induced circular dichroism in gels. Chirality, 34(3), 550-558.
  Xue, Yu; Fehn, Natalie; Brandt, Viktoria Katharina; Stasi, Michele; Boekhoven, Job; Heiz, Ueli & Kartouzian, Aras
  
• Tuning the Kinetic Trapping in Chemically Fueled Self‐Assembly**. ChemSystemsChem, 5(1).
  Kriebisch, Brigitte A. K.; Kriebisch, Christine M. E.; Bergmann, Alexander M.; Wanzke, Caren; Tena‐Solsona, Marta & Boekhoven, Job
  
• The chemistry of chemically fueled droplets. Trends in Chemistry, 5(1), 45-60.
  Donau, Carsten & Boekhoven, Job