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De Novo design of functional coassembling organic–inorganic hydrogels for hierarchical mineralization and neovascularization

De Novo design of functional coassembling organic–inorganic hydrogels for hierarchical mineralization and neovascularization
De Novo design of functional coassembling organic–inorganic hydrogels for hierarchical mineralization and neovascularization
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.
biomineralization, coassembly, laponite, multicomponent biomaterials, nanocomposite hydrogels, peptide amphiphiles, supramolecular
1936-0851
11202–11217
Oreffo, Richard
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Okesola, Babatunde O.
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Mendoza-Martinez, Ana Karen
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Cidonio, Gianluca
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Derkus, Burak
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Boccorh, Delali
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Osuna de la Pena, David
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Elsharkawy, Sherif
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Wu, Yuanhao
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Dawson, Jonathan
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Wark, Alastair
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Knani, Dafna
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Adams, Dave J.
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Mata, Alvaro
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Oreffo, Richard
ff9fff72-6855-4d0f-bfb2-311d0e8f3778
Okesola, Babatunde O.
45408cc8-db61-485a-807b-695e2301d8f5
Mendoza-Martinez, Ana Karen
336327f6-09b7-44cc-bc49-0a15f0e43433
Cidonio, Gianluca
558ad583-899a-4d8c-b42b-bc1c354c8757
Derkus, Burak
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Boccorh, Delali
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Osuna de la Pena, David
ddb4d1e0-3386-43a8-9a69-136de0a8d077
Elsharkawy, Sherif
db09f342-b6b3-447b-9d01-ffc9771f1c83
Wu, Yuanhao
020953e1-848a-4f74-8abc-bd532afa7600
Dawson, Jonathan
b220fe76-498d-47be-9995-92da6c289cf3
Wark, Alastair
8a2d6da3-28db-4ce7-b5e2-c52bff282c3a
Knani, Dafna
da2c9283-ee3c-4876-bad2-36483cc78df0
Adams, Dave J.
d95e4f11-7580-43cb-802d-ad8ac0161c8a
Mata, Alvaro
c67ceb11-02c5-429c-a5e6-308c322f176b

Oreffo, Richard, Okesola, Babatunde O., Mendoza-Martinez, Ana Karen, Cidonio, Gianluca, Derkus, Burak, Boccorh, Delali, Osuna de la Pena, David, Elsharkawy, Sherif, Wu, Yuanhao, Dawson, Jonathan, Wark, Alastair, Knani, Dafna, Adams, Dave J. and Mata, Alvaro (2021) De Novo design of functional coassembling organic–inorganic hydrogels for hierarchical mineralization and neovascularization. ACS Nano, 15 (7), 11202–11217. (doi:10.1021/acsnano.0c09814).

Record type: Article

Abstract

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.

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Accepted/In Press date: 27 April 2021
e-pub ahead of print date: 28 June 2021
Published date: 27 July 2021
Keywords: biomineralization, coassembly, laponite, multicomponent biomaterials, nanocomposite hydrogels, peptide amphiphiles, supramolecular

Identifiers

Local EPrints ID: 450764
URI: http://eprints.soton.ac.uk/id/eprint/450764
ISSN: 1936-0851
PURE UUID: d8ce0ef7-1e4f-497f-b4e4-3a1dbf9e4df1
ORCID for Richard Oreffo: ORCID iD orcid.org/0000-0001-5995-6726
ORCID for Jonathan Dawson: ORCID iD orcid.org/0000-0002-6712-0598

Catalogue record

Date deposited: 10 Aug 2021 16:31
Last modified: 26 Nov 2021 02:53

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Contributors

Author: Richard Oreffo ORCID iD
Author: Babatunde O. Okesola
Author: Ana Karen Mendoza-Martinez
Author: Gianluca Cidonio
Author: Burak Derkus
Author: Delali Boccorh
Author: David Osuna de la Pena
Author: Sherif Elsharkawy
Author: Yuanhao Wu
Author: Jonathan Dawson ORCID iD
Author: Alastair Wark
Author: Dafna Knani
Author: Dave J. Adams
Author: Alvaro Mata

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