In comparison to what I applied for, two additional new chemical platforms have been developed for the synthesis of sequence-defined oligomers (Soete et al., Polym. Chem 2022 and De Franceschi et al., Polym. Chem. 2022).
The second platform - based on the use of a uniform soluble support - allows for the first time the preparation of around 15 gram batches of sequence-defined macromolecules (vs mg-scale using solid supports previously), with potential for much higher scales applicable in a material context (cf. subproject 1).
The methodology, initially developed based on a thiolactone chemistry-based protocol, has been further extended to the formation of oligoamides with different functional groups, either at the end of the chain or as side-chains. The functional end groups were successfully used as crosslinking point to form polymeric networks via thiol-ene chemistry (De Franceschi et al., Chem. Sci. 2024), which is one of the first reports world-wide in which crosslinked materials based on sequence-defined macromolecules has been reported (related to subproject 3).
In parallel, Initial investigations have been performed in order to better understand fundamental aspects in covalent adaptable networks such as the correlation between the composition of a reactive polymer segment to the rate of network rearrangement (Van Lijsebetten et al. Chem. Sci 2022), how to obtain reprocessable thermoset materials with minimal deformation/creep (Van Lijsebetten et al. Angew. Chem., 2022), the development and screening of other dynamic chemistries such as the beta-amino amide approach (Nguyen et al. Polym. Chem. 2024) or the Aza-Michael chemistry (Nguyen et al. Macromolecules 2024) etc (subproject 3). These studies were completed by the first exploration how to control the thermal debonding of epoxy-based adhesives (Van Lijsebetten et al. Adv. Mater. 2023), which is related to one of the deliverables in subproject 4.
In parallel, we collaborate – as planned – with the research group of Prof. Ivo Vankelecom with strong membrane expertise, for providing an alternative pathway making use of nanofiltration membranes for the upscaling of sequence defined structures (Subproject 2). This is planned to be reported in the upcoming 6 months.
In summary, with regard to the 8 milestones mentioned in the application, 5 have been at least partially tackled and published/disseminated (M1.1 M1.2 M2.2 M3.2 M4.1) while ongoing research about the other milestones is in full progress and/or planned in the near future.
