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Photo-crosslinkable poly(aspartic acid) for light-based additive manufacturing : chain-growth versus step-growth crosslinking

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Abstract
Crosslinked poly(aspartic acid) (pAsp) hydrogels have been evaluated in various applications benefitting from their biocompatibility and biodegradability. Several crosslinking mechanisms for pAsp derivatives have been investigated, yet research focusing on functionalization of pAsp with photo-crosslinkable moieties is scarce. However, the latter would be beneficial for processing of pAsp through light-based additive manufacturing techniques. pAsp was functionalized comparing two types of photo-crosslinkable moieties (i.e. norbornene versus methacrylate), resulting in a thiol-ene step-growth crosslinking mechanism and a chain-growth mechanism, respectively. The influence of the crosslinking mechanism on the photo-crosslinking kinetics, mechanical properties and biocompatibility of the hydrogels was studied. Hydrogels based on norbornene-modified pAsp with Li-TPO-L photo-initiator and a thiol-based crosslinker showed fast crosslinking kinetics and a high swelling ratio, along with a relatively low storage modulus of 29.4 +/- 1.3 kPa. Methacrylate-modified pAsp formulations with Li-TPO-L crosslinked slower and exhibited a lower swelling ratio, yet a higher storage modulus (135.1 +/- 4.7 kPa). Both hydrogel materials were non-cytotoxic to cells growing in their vicinity. The applicability of the hydrogels to serve as materials for digital light processing (DLP) and two-photon polymerization (2PP) was elucidated. Both materials were processable via DLP and 2PP, offering possibilities towards processing of these materials into constructs serving biomedical applications.
Keywords
Organic Chemistry, Polymers and Plastics, General Physics and Astronomy, Materials Chemistry, Photo-crosslinkable poly(aspartic acid), Chain-growth crosslinking, Step-growth crosslinking, Light-based additive manufacturing, Non-cytotoxic hydrogels, POLYASPARTIC ACID, VOLUME CHANGE, HYDROGELS, GELATIN, REDOX, BIODEGRADATION, NANOPARTICLES, CHEMISTRY, POLYMERS

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MLA
De Grave, Lauren, et al. “Photo-Crosslinkable Poly(Aspartic Acid) for Light-Based Additive Manufacturing : Chain-Growth versus Step-Growth Crosslinking.” EUROPEAN POLYMER JOURNAL, vol. 190, 2023, doi:10.1016/j.eurpolymj.2023.112017.
APA
De Grave, L., Di Meo, C., Gréant, C., Van Durme, B., Gérard, M., La Gatta, A., … Van Vlierberghe, S. (2023). Photo-crosslinkable poly(aspartic acid) for light-based additive manufacturing : chain-growth versus step-growth crosslinking. EUROPEAN POLYMER JOURNAL, 190. https://doi.org/10.1016/j.eurpolymj.2023.112017
Chicago author-date
De Grave, Lauren, Celeste Di Meo, Coralie Gréant, Bo Van Durme, Melanie Gérard, Annalisa La Gatta, Chiara Schiraldi, Lieven Thorrez, Katrien V. Bernaerts, and Sandra Van Vlierberghe. 2023. “Photo-Crosslinkable Poly(Aspartic Acid) for Light-Based Additive Manufacturing : Chain-Growth versus Step-Growth Crosslinking.” EUROPEAN POLYMER JOURNAL 190. https://doi.org/10.1016/j.eurpolymj.2023.112017.
Chicago author-date (all authors)
De Grave, Lauren, Celeste Di Meo, Coralie Gréant, Bo Van Durme, Melanie Gérard, Annalisa La Gatta, Chiara Schiraldi, Lieven Thorrez, Katrien V. Bernaerts, and Sandra Van Vlierberghe. 2023. “Photo-Crosslinkable Poly(Aspartic Acid) for Light-Based Additive Manufacturing : Chain-Growth versus Step-Growth Crosslinking.” EUROPEAN POLYMER JOURNAL 190. doi:10.1016/j.eurpolymj.2023.112017.
Vancouver
1.
De Grave L, Di Meo C, Gréant C, Van Durme B, Gérard M, La Gatta A, et al. Photo-crosslinkable poly(aspartic acid) for light-based additive manufacturing : chain-growth versus step-growth crosslinking. EUROPEAN POLYMER JOURNAL. 2023;190.
IEEE
[1]
L. De Grave et al., “Photo-crosslinkable poly(aspartic acid) for light-based additive manufacturing : chain-growth versus step-growth crosslinking,” EUROPEAN POLYMER JOURNAL, vol. 190, 2023.
@article{01H032VCRQ623AKY3ADGAFJ40Y,
  abstract     = {{Crosslinked poly(aspartic acid) (pAsp) hydrogels have been evaluated in various applications benefitting from their biocompatibility and biodegradability. Several crosslinking mechanisms for pAsp derivatives have been investigated, yet research focusing on functionalization of pAsp with photo-crosslinkable moieties is scarce. However, the latter would be beneficial for processing of pAsp through light-based additive manufacturing techniques. pAsp was functionalized comparing two types of photo-crosslinkable moieties (i.e. norbornene versus methacrylate), resulting in a thiol-ene step-growth crosslinking mechanism and a chain-growth mechanism, respectively. The influence of the crosslinking mechanism on the photo-crosslinking kinetics, mechanical properties and biocompatibility of the hydrogels was studied. Hydrogels based on norbornene-modified pAsp with Li-TPO-L photo-initiator and a thiol-based crosslinker showed fast crosslinking kinetics and a high swelling ratio, along with a relatively low storage modulus of 29.4 +/- 1.3 kPa. Methacrylate-modified pAsp formulations with Li-TPO-L crosslinked slower and exhibited a lower swelling ratio, yet a higher storage modulus (135.1 +/- 4.7 kPa). Both hydrogel materials were non-cytotoxic to cells growing in their vicinity. The applicability of the hydrogels to serve as materials for digital light processing (DLP) and two-photon polymerization (2PP) was elucidated. Both materials were processable via DLP and 2PP, offering possibilities towards processing of these materials into constructs serving biomedical applications.}},
  articleno    = {{112017}},
  author       = {{De Grave, Lauren and Di Meo, Celeste and Gréant, Coralie and Van Durme, Bo and Gérard, Melanie and La Gatta, Annalisa and Schiraldi, Chiara and Thorrez, Lieven and Bernaerts, Katrien V. and Van Vlierberghe, Sandra}},
  issn         = {{0014-3057}},
  journal      = {{EUROPEAN POLYMER JOURNAL}},
  keywords     = {{Organic Chemistry,Polymers and Plastics,General Physics and Astronomy,Materials Chemistry,Photo-crosslinkable poly(aspartic acid),Chain-growth crosslinking,Step-growth crosslinking,Light-based additive manufacturing,Non-cytotoxic hydrogels,POLYASPARTIC ACID,VOLUME CHANGE,HYDROGELS,GELATIN,REDOX,BIODEGRADATION,NANOPARTICLES,CHEMISTRY,POLYMERS}},
  language     = {{eng}},
  pages        = {{11}},
  title        = {{Photo-crosslinkable poly(aspartic acid) for light-based additive manufacturing : chain-growth versus step-growth crosslinking}},
  url          = {{http://doi.org/10.1016/j.eurpolymj.2023.112017}},
  volume       = {{190}},
  year         = {{2023}},
}

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