Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/152662
Title: Rapid activation of diazirine biomaterials with the blue light photocatalyst
Authors: Djordjevic, Ivan
Wicaksono, Gautama
Šolić, Ivan
Singh, Juhi
Kaku, Tanvi Sushil
Lim, Sierin
Ang, Elwin Wei Jian
Blancafort, Lluís
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
MOE2018-T2-2-114
NGF/2018/05
H19/01/a0/0II9
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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