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The effect of hydrogen bonding on diffusion and permeability in UV-cured Polyacrylate-based networks for controlled release

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journal contribution
posted on 13.01.2022, 17:35 authored by Bing Wu, Walter Chassé, Klaus Zick, Michael D Mantle, Andreas HeiseAndreas Heise, Dermot F Brougham, Victor M Litvinov
Polyacrylates are important polymers widely used in pharmaceutical industry such as drug coatings due to their low cost, processability and ease of functionalisation. Chemical functionalities (e.g. H-bonding) can be easily included to modulate the transport of low molecular weight drug-like entities through the network. Understanding how such microscopic structural modifications determine macroscopic diffusion is critical for designing next generation responsive polymers. In this study pulsed field gradient (PFG) 1H NMR measurements of the self-diffusion of a dye molecule (Eosin Y) in a series of polyacrylate networks with differing H-bonding strength were undertaken; it was found that the diffusion of Eosin Y is significantly reduced in networks with H-bonding. Detailed analyses by 1H NMR relaxometry and double quantum (DQ) NMR show that H-bonding can also reduce polymer chain mobility. Furthermore, DSC thermoporometry showed a significant increase in the average network mesh size potentially due to the pre-organization of H-bonding containing monomer during network curing. By introducing the H-bonding disrupter, LiClO4, it was found that the diffusivity of solute becomes positively correlated to the average mesh size across the series of networks. Hence, a modified diffusion model based on hydrodynamic theory is proposed to separate the direct (solute-network) H-bonding contribution to solute diffusion from the indirect contribution arising from monomer pre-ordering induced mesh size reduction. Finally, it is shown that the same direct and indirect contributions to microscopic diffusivity, arising from the H-bond strength of the co-monomers, also contribute significantly to the macroscopic membrane permeability which is similarly subject to H-bond disruption.

Funding

EU FP7 Marie Curie Actions under the NEOGEL project (Grant No. 316973)

EU Horizon2020 Marie Curie Cofund project (Grant No. 713279)

Science Foundation Ireland (Grant Agreement No. 16/IA/4584)

History

Comments

The original article is available at https://www.sciencedirect.com/

Published Citation

Wu B. et al. The effect of hydrogen bonding on diffusion and permeability in UV-cured Polyacrylate-based networks for controlled release. J Control Release. 2020;327:150-160

Publication Date

30 July 2020

PubMed ID

32738286

Department/Unit

  • Chemistry

Research Area

  • Biomaterials and Regenerative Medicine
  • Chemistry and Pharmaceutical Sciences

Publisher

Elsevier BV

Version

  • Published Version (Version of Record)