De novo design of functional co-assembling organic-inorganic hydrogels for hierarchical mineralization and neovascularization

Okesola, B. O. et al. (2021) De novo design of functional co-assembling organic-inorganic hydrogels for hierarchical mineralization and neovascularization. ACS Nano, 15, pp. 11202-11217. (doi: 10.1021/acsnano.0c09814) (PMID:34180656)

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Synthetic nanostructured materials incorporating both organic and inorganic components offer a unique, powerful, and versatile class of materials for widespread applications due to the distinct, yet complementary, nature of the intrinsic properties of the different constituents. We report a supramolecular system based on synthetic nanoclay (Laponite, Lap) and peptide amphiphiles (PAs, PAH3) rationally designed to coassemble into nanostructured hydrogels with high structural integrity and a spectrum of bioactivities. Spectroscopic and scattering techniques and molecular dynamic simulation approaches were harnessed to confirm that PAH3 nanofibers electrostatically adsorbed and conformed to the surface of Lap nanodisks. Electron and atomic force microscopies also confirmed an increase in diameter and surface area of PAH3 nanofibers after coassembly with Lap. Dynamic oscillatory rheology revealed that the coassembled PAH3-Lap hydrogels displayed high stiffness and robust self-healing behavior while gas adsorption analysis confirmed a hierarchical and heterogeneous porosity. Furthermore, this distinctive structure within the three-dimensional (3D) matrix provided spatial confinement for the nucleation and hierarchical organization of high-aspect ratio hydroxyapatite nanorods into well-defined spherical clusters within the 3D matrix. Applicability of the organic–inorganic PAH3-Lap hydrogels was assessed in vitro using human bone marrow-derived stromal cells (hBMSCs) and ex vivo using a chick chorioallantoic membrane (CAM) assay. The results demonstrated that the organic–inorganic PAH3-Lap hydrogels promote human skeletal cell proliferation and, upon mineralization, integrate with the CAM, are infiltrated by blood vessels, stimulate extracellular matrix production, and facilitate extensive mineral deposition relative to the controls.

Item Type:Articles
Additional Information:The work was supported by the ERC Starting Grant (STROFUNSCAFF), the Medical Research Council (UK Regenerative Medicine Platform Acellular/Smart Materials-3D Architecture, MR/R015651/1) to A.M., J.I.D., and R.O., and the AO Foundation (AOCMF-17-19M). B.O.O. was supported by the Henry Royce Institute for Advanced Materials, funded through Engineering and Physical Sciences Research Council (EPSRC) grants (EP/R00661X/1, EP/ S019367/1, EP/P025021/1, and EP/P025498/1). D.J.A. thanks EPSRC for an award of a fellowship (EP/L021978/2).
Glasgow Author(s) Enlighten ID:Adams, Dave
Authors: Okesola, B. O., Mendoza-Martinez, A. K., Cidonio, G., Derkus, B., Boccorch, D. K., Osuna de la Peña, D., Elsharkawy, S., Wu, Y., Dawson, J. I., Wark, A. W., Knani, D., Adams, D. J., Oreffo, R. O.C., and Mata, A.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:ACS Nano
Publisher:American Chemical Society
ISSN (Online):1936-086X
Published Online:28 June 2021
Copyright Holders:Copyright © 2021 The Authors
First Published:First published in ACS Nano 15: 11202-11217
Publisher Policy:Reproduced under a Creative Commons licence

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
174004Multicomponent Supramolecular HydrogelsDave AdamsEngineering and Physical Sciences Research Council (EPSRC)EP/L021978/2Chemistry
301095UKRMP2 Acellular/Smart Materials 3D Architecture HubManuel Salmeron-SanchezMedical Research Council (MRC)MMRE_P75176 (MR/R015651/1ENG - Biomedical Engineering