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|Title:||Rapid activation of diazirine biomaterials with the blue light photocatalyst||Authors:||Djordjevic, Ivan
Kaku, Tanvi Sushil
Ang, Elwin Wei Jian
Steele, Terry W. J.
|Keywords:||Engineering::Materials::Biomaterials||Issue Date:||2021||Source:||Djordjevic, I., Wicaksono, G., Šolić, I., Singh, J., Kaku, T. S., Lim, S., Ang, E. W. J., Blancafort, L. & Steele, T. W. J. (2021). Rapid activation of diazirine biomaterials with the blue light photocatalyst. ACS Applied Materials and Interfaces, 13(31), 36839-36848. https://dx.doi.org/10.1021/acsami.1c08581||Project:||RG17/18
|Journal:||ACS Applied Materials and Interfaces||Abstract:||Carbene-based macromolecules are an emerging new stimuli-sensitive class of biomaterials that avoid the impediments of free radical polymerization but maintain a rapid liquid-to-biorubber transition. Activation of diazirine-grafted polycaprolactone polyol (CaproGlu) is limited to UVA wavelengths that have tissue exposure constraints and limited light intensities. For the first time, UVA is circumvented with visible light-emitting diodes at 445 nm (blue) to rapidly activate diazirine-to-carbene covalent cross-linking. Iridium photocatalysts serve to initiate diazirine, despite having little to no absorption at 445 nm. CaproGlu's liquid organic matrix dissolves the photocatalyst with no solvents required, creating a light transparent matrix. Considerable differences in cross-linking chemistry are observed in UVA vs visible/photocatalyst formulations. Empirical analysis and theoretical calculations reveal a more efficient conversion of diazirine directly to carbene with no diazoalkane intermediate detected. Photorheometry results demonstrate a correlation between shear moduli, joules light dose, and the lower limits of photocatalyst concentration required for the liquid-to-biorubber transition. Adhesion strength on ex vivo hydrated tissues exceeds that of cyanoacrylates, with a fixation strength of up to 20 kg·f·cm2. Preliminary toxicity assessment on leachates and materials directly in contact with mammalian fibroblast cells displays no signs of fibroblast cytotoxicity.||URI:||https://hdl.handle.net/10356/152662||ISSN:||1944-8244||DOI:||10.1021/acsami.1c08581||Rights:||This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials and Interfaces, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsami.1c08581.||Fulltext Permission:||embargo_20220818||Fulltext Availability:||With Fulltext|
|Appears in Collections:||IGS Journal Articles|
MSE Journal Articles
SCBE Journal Articles
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