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Intermolecular interactions of biofunctional polymers

The characterization of biopolymer systems consisting of different components with emphasis on bioactive interactions is a challenge again and again. Our first attempts to characterize biocomplexes and aggregation behavior of bioactive molecules led to the development of novel physicochemical approaches with high application potential.  

 

The focus of our research is based on three different types of interaction:

1.    interactions between similar biopolymers (e.g. aggregation or cross-linking) for stimuli-responsive size changes 

Overview of molecular conformations of dendronized glycopolymers as a function of pH, concentration and generation number determined by AF4 in combination with light scattering. (Boye, Biomacromolecules, 2012)

 

2.    non-covalent interactions between large host polymers and smaller guest molecules (e.g. complexation studies) for targeted drug-delivery

  • quantification of loading efficiency by AF4 in combination with UV and LS detection
Complexation studies of guest-host systems by AF4-LS: Quantification of complexed molecules by UV and LS detection. (Boye, J. Chromatogr. A 2010)
AF4 complexation studies of PPI glycodendrimers towards therapeutic adenosine analogues (Gorzkiewicz, Boye, et al, Macromolecular Rapid Communications, 2019)
  • loading studies of stimuli-responsive polymersomes with enzymes by AF4: quantification of cargo amount and loaction information by correlation of scaling parameters, apparent density and cargo properties
pH responsive polymersomes and their loading with small cargo molecules (Gumz, Advanced Science, 2019)

 

3.    bioconjugation to fabricate supramolecular structures (e.g. studies of biohybrid structures or polyplexes) as e.g. sensor materials

From 1D rods to 3D networks: Structural transformation of biohybrid structures consisting of biotin-avidin interactions. (Boye, Macromolecules 2015)

 

The determination of multicomponent or aggregate distribution together with a characterization of scaling parameters enables a deep insight into structure-property-relationship. Large dimensions, high molar masses and extremely high functionality are characteristic for these molecules, accompanied by challenging molecular characterization. Using AF4 coupled to static light scattering, dynamic light scattering as well as using complementary methods such as AFM and MD simulations we can shed light on the interactions of biopolymer systems.

References

  1. M. Gorzkiewicz, D. Appelhans, S. Boye, A. Lederer, B. Voit Effect of the structure of therapeutic adenosine analogues on stability and surface electrostatic potential of their complexes with poly(propyleneimine) dendrimers Macromolecular Rapid Communications (2019) accepted
  2. H. Gumz, S. Boye, B. Lyisan, V. Krönert, P. Formanek, B. Voit, A. Lederer, D. Appelhans Towards functional synthetic cells: In-depth study of nanoparticle and enzyme diffusion through a cross-linked polymersome membrane  Advanced Science (2019) 6, (7), 1970037
  3. A. Lederer, S. Boye, D. Appelhans Advanced AF4 characterization of dendritic biomacromolecules, their self-assembly, and hybrid formation Chapter in "Recent Progress in Separation of Macromolecules and Particulates", ACS Publisher 1281 (2018) 171-187
  4. J. Zessin, F. Fischer, A. Heerwig, A. Kick, S. Boye, M. Stamm, A. Kiriy, M. Mertig Tunable fluorescene of a semiconducting polythiophene positioned on DNA origami Nano Letters  (2017) 17, 5163-5170
  5. F. Ennen, P. Fenner, G. Stoychev, S. Boye, A. Lederer, B. Voit, D. Appelhans Coil-like enzymatic biohybrid structures fabricated by rational design: Controlling size and enzyme activity over sequential nanoparticle bioconjugation and filtration steps ACS Applied Materials & Interfaces (2016), 8 (9), 6261-6268
  6. F. Ennen, P. Fenner, S. Boye, A. Lederer, H. Komber, B. Voit, D.Appelhans Sphere-Like Protein-Glycopolymer Nanostructures Tailored by Polyassociation Biomacromolecules (2016), 17 (1), 32-45
  7. A. Taubert, T. Mai , S. Boye , J. Yuan , A. Voelkel , M. Graewert , C. Guenter, A. Lederer Poly(ethylene oxide)-based block copolymers with very high molecular weights for biomimetic calcium phosphate mineralization RSC Advances 2015, 5, 103494-103505
  8. C. Striegler, M. Franke, M. Müller, S. Boye, U. Oertel, A. Janke, L. Schellkopf, B. Voit, D. Appelhans Amino acid modified hyperbranched poly(ethylene imine) with disaccharide decoration as anionic core-shell architecture: Influence of the pH and molecular architecture on solution behaviour Polymer 2015, 80, 188-204
  9. R.-P. Nzé, T. Nicolai, C. Chassenieux, E. Nicol, S. Boye, A. Lederer Effect of connectivity on the structure and the liquid-solid transition of dense suspensions of soft colloids Macromolecules 2015, 48, (21) 7995-8002
  10. S. Boye, A. Lederer et al. From 1D rods to 3D networks: A biohybrid topological diversity investigated by asymmetrical flow field-flow fractionation Macromolecules 2015, 48,  4607-4619
  11. E. Haladjova, M. Geisler, S. Boye, A. Lederer et al. Asymmetric Flow Field-Flow Fractionation Investigation of Magnetopolyplexes  Macromol. Chem. Phys. 2015, 216, 1862-1867
  12. M. A. Yassin, S. Boye, A. Lederer et al. Overcoming Concealment Effects of Targeting Moieties in the PEG Corona: Controlled Permeable Polymersomes Decorated with Folate-Antennae for Selective Targeting of Tumor Cells small 2015 11 (13), 1580-1591
  13. T. Mai, S. Boye, A. Lederer et al. Poly(ethylene oxide)-b-poly(3-sulfopropyl methycrylate) block copolymers for calcium phosphate mineralization and biofilm inhibition Biomacromolecules 2014, 15, 3901-3914
  14. F. Ennen, S. Boye, A. Lederer et al. Biohybrid structures consisting of biotinylated glycodendrimers and proteins: influence of the biotin ligand's number and chemical nature on the biotin-avidin conjugation Polymer Chemistry 2014, 5, 1323-133
  15. S. Boye et al. pH Triggered Aggregate Shape of Different Generations Lysine-Dendronized Maleimide Copolymers with Maltose Shell Biomacromolecules 2012, 13 (12), 4222-4235
  16. S. Boye et al. An Alternative Route to Dye-Polymer Complexation Studies using Asymmetrical Flow Field-Flow Fractionation J. Chromatogr. A 2010, 1217, 4841–4849