Poly(ɛ-caprolactone) (PCL) is a biocompatible, biodegradable, and highly mechanically resilient FDA-approved material (for specific biomedical applications, e.g. as drug delivery devices, in sutures, or as an adhesion barrier), rendering it a promising candidate to serve bone tissue engineering. However, in vivo monitoring of PCL-based implants, as well as biodegradable implants in general, and their degradation profiles pose a significant challenge, hindering further development in the tissue engineering field and subsequent clinical adoption. To address this, photo-cross-linkable mechanically resilient PCL networks are developed and functionalized with a radiopaque monomer, 5-acrylamido-2,4,6-triiodoisophthalic acid (AATIPA), to enable non-destructive in vivo monitoring of PCL-based implants. The covalent incorporation of AATIPA into the crosslinked PCL networks does not significantly affect their crosslinking kinetics, mechanical properties, or thermal properties, but it increases their hydrolysis rate and radiopacity. Complex and porous 3D designs of radiopaque PCL networks can be effectively monitored in vivo. This work paves the way toward non-invasive monitoring of in vivo degradation profiles and early detection of potential implant malfunctions.

Center for Advanced Preclinical Imaging 1st Faculty of Medicine Charles University Salmovská 3 Prague 2 Prague 12000 Czech Republic

Institute of Biophysics and Informatics 1st Faculty of Medicine Charles University Salmovská 1 Prague 2 Prague 12000 Czech Republic

Institute of Macromolecular Chemistry Czech Academy of Sciences Heyrovského sq 2 Prague 6 Prague 16206 Czech Republic

Institute of Organic Chemistry and Biochemistry Czech Academy of Sciences Flemingovo sq 2 Prague 6 Prague 16000 Czech Republic

Polymer Chemistry and Biomaterials Group Department of Organic and Macromolecular Chemistry Centre of Macromolecular Chemistry Ghent University Krijgslaan 281 Building S4 Belgie Ghent 9000 Belgium

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