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Title: Generating molecularly-controlled biomaterials using host-guest guided peptide amphiphile self-assembly
Author: Redondo Gómez, Carlos A.
ISNI:       0000 0004 9355 5178
Awarding Body: Queen Mary University of London
Current Institution: Queen Mary, University of London
Date of Award: 2020
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Supramolecular chemistry offers a unique opportunity to assemble biomaterials with molecular precision. Though biomaterials based on self-assembling peptides often exhibit limited control over their hierarchical assembly, mechanical properties or biological relevance. This dissertation addresses these challenges by bringing together the scopes of peptide self-assembly and hostguest interactions. The thesis opens with a literature revision chapter on supramolecular biomaterials and multicomponent self-assembly as a strategy to design complex biomedically relevant hydrogels. The following three experimental chapters constitute examples of biomedically relevant peptide amphiphile (PA)-based hydrogels based on the co-assembly of peptides bearing host-guest recognition motifs. Firstly, a report on a new family of supramolecular hydrogels based on the non-covalent crosslinking between PAs bearing either h-Cyclodextrin (hCD) or Adamantane (Ada) host-guest cues is presented. The resulting hydrogels exhibit enhanced mechanical properties, including stiffness and resistance to degradation, while retaining good in vitro biocompatibility. The next chapter explores on the non-covalent tethering of biologically relevant epitopes to self-assembled PA nanofibers through hCD/Ada complexations as a modular approach for developing more complex and dynamic PA hydrogels. Incorporating host-guest peptide pairs endowed control from nano to macroscale in the materials, as well as its mechanical control, biological tunability and the possibility to imprint them higher levels of dynamic spatiotemporal properties. Lastly, the use of another host-guest interaction family based on the ternary complexation of aromatic amino acid-bearing PAs and cucurbit[8]uril (CB[8]) is presented. An unreported non-ionic gelation mechanism is presented as well as the structural and mechanical comparison of the PA-CB[8] gels versus conventional ionically-gelled PAs. Altogether, this work presents new approaches to develop more controlled and functional peptide-based nanomaterials with broad implications in the self-assembling and bioengineering communities.
Supervisor: Not available Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available