Introducing Hyaluronic Acid into Supramolecular Polymers and Hydrogels

Silvia Varela-Aramburu; Lu Su; Jesús Mosquera; Giulia Morgese; Sandra M C Schoenmakers; Ruth Cardinaels; Anja R.A. Palmans; E.W. Meijer

doi:10.1021/acs.biomac.1c00927

Introducing Hyaluronic Acid into Supramolecular Polymers and Hydrogels

Silvia Varela-Aramburu, Lu Su, Jesús Mosquera, Giulia Morgese, Sandra M C Schoenmakers, Ruth Cardinaels, Anja R.A. Palmans (Corresponding author), E.W. Meijer (Corresponding author)

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Abstract

The use of supramolecular polymers to construct functional biomaterials is gaining more attention due to the tunable dynamic behavior and fibrous structures of supramolecular polymers, which resemble those found in natural systems, such as the extracellular matrix. Nevertheless, to obtain a biomaterial capable of mimicking native systems, complex biomolecules should be incorporated, as they allow one to achieve essential biological processes. In this study, supramolecular polymers based on water-soluble benzene-1,3,5-tricarboxamides (BTAs) were assembled in the presence of hyaluronic acid (HA) both in solution and hydrogel states. The coassembly of BTAs bearing tetra(ethylene glycol) at the periphery (BTA-OEG4) and HA at different ratios showed strong interactions between the two components that led to the formation of short fibers and heterogeneous hydrogels. BTAs were further covalently linked to HA (HA-BTA), resulting in a polymer that was unable to assemble into fibers or form hydrogels due to the high hydrophilicity of HA. However, coassembly of HA-BTA with BTA-OEG4 resulted in the formation of long fibers, similar to those formed by BTA-OEG4 alone, and hydrogels were produced with tunable stiffness ranging from 250 to 700 Pa, which is 10-fold higher than that of hydrogels assembled with only BTA-OEG4. Further coassembly of BTA-OEG4 fibers with other polysaccharides showed that except for dextran, all polysaccharides studied interacted with BTA-OEG4 fibers. The possibility of incorporating polysaccharides into BTA-based materials paves the way for the creation of dynamic complex biomaterials.

Original language	English
Pages (from-to)	4633-4641
Number of pages	9
Journal	Biomacromolecules
Volume	22
Issue number	11
DOIs	https://doi.org/10.1021/acs.biomac.1c00927
Publication status	Published - 8 Nov 2021

Funding

Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013), Swiss National Science Foundation (SNSF “Early PostDoc Mobility” P2EZP2-178435), Marie Skłodowska-Curie postdoctoral fellowship (794016), and European Research Council Advanced Grant (788618 SYNMAT- ERC-2017-ADG 10025006). The authors acknowledge the ICMS Animation Studio for providing the artwork. S.V.-A. and G.M. acknowledge the funding received by Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013). J.M. acknowledges a Marie Skłodowska-Curie postdoctoral fellowship (794016) for financial support. G.M. acknowledges the funding received by the Swiss National Science Foundation (SNSF “Early PostDoc Mobility” P2EZP2 - 178435). R.C. acknowledges TA Instruments for providing the DHR-3 rheometer under the Young Distinguished Rheologist Award instrument grant. S.S. and E.W.M acknowledge the European Research Council (H2020-EU.1.1., SYNMAT project, ID 788618).

Funders	Funder number
Marie Skłodowska‐Curie
Horizon 2020 Framework Programme	794016, 788618
H2020 European Research Council
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung	P2EZP2-178435
Nederlandse Organisatie voor Wetenschappelijk Onderzoek	024.003.013

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10.1021/acs.biomac.1c00927

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title = "Introducing Hyaluronic Acid into Supramolecular Polymers and Hydrogels",

abstract = "The use of supramolecular polymers to construct functional biomaterials is gaining more attention due to the tunable dynamic behavior and fibrous structures of supramolecular polymers, which resemble those found in natural systems, such as the extracellular matrix. Nevertheless, to obtain a biomaterial capable of mimicking native systems, complex biomolecules should be incorporated, as they allow one to achieve essential biological processes. In this study, supramolecular polymers based on water-soluble benzene-1,3,5-tricarboxamides (BTAs) were assembled in the presence of hyaluronic acid (HA) both in solution and hydrogel states. The coassembly of BTAs bearing tetra(ethylene glycol) at the periphery (BTA-OEG4) and HA at different ratios showed strong interactions between the two components that led to the formation of short fibers and heterogeneous hydrogels. BTAs were further covalently linked to HA (HA-BTA), resulting in a polymer that was unable to assemble into fibers or form hydrogels due to the high hydrophilicity of HA. However, coassembly of HA-BTA with BTA-OEG4 resulted in the formation of long fibers, similar to those formed by BTA-OEG4 alone, and hydrogels were produced with tunable stiffness ranging from 250 to 700 Pa, which is 10-fold higher than that of hydrogels assembled with only BTA-OEG4. Further coassembly of BTA-OEG4 fibers with other polysaccharides showed that except for dextran, all polysaccharides studied interacted with BTA-OEG4 fibers. The possibility of incorporating polysaccharides into BTA-based materials paves the way for the creation of dynamic complex biomaterials. ",

author = "Silvia Varela-Aramburu and Lu Su and Jes{\'u}s Mosquera and Giulia Morgese and Schoenmakers, {Sandra M C} and Ruth Cardinaels and Palmans, {Anja R.A.} and E.W. Meijer",

note = "Funding Information: Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013), Swiss National Science Foundation (SNSF “Early PostDoc Mobility” P2EZP2-178435), Marie Sk{\l}odowska-Curie postdoctoral fellowship (794016), and European Research Council Advanced Grant (788618 SYNMAT- ERC-2017-ADG 10025006). Funding Information: The authors acknowledge the ICMS Animation Studio for providing the artwork. S.V.-A. and G.M. acknowledge the funding received by Gravitation Program “Materials Driven Regeneration,” funded by the Netherlands Organization for Scientific Research (024.003.013). J.M. acknowledges a Marie Sk{\l}odowska-Curie postdoctoral fellowship (794016) for financial support. G.M. acknowledges the funding received by the Swiss National Science Foundation (SNSF “Early PostDoc Mobility” P2EZP2 - 178435). R.C. acknowledges TA Instruments for providing the DHR-3 rheometer under the Young Distinguished Rheologist Award instrument grant. S.S. and E.W.M acknowledge the European Research Council (H2020-EU.1.1., SYNMAT project, ID 788618). Publisher Copyright: {\textcopyright} 2021 The Authors. Published by American Chemical Society.",

year = "2021",

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doi = "10.1021/acs.biomac.1c00927",

language = "English",

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AU - Varela-Aramburu, Silvia

AU - Su, Lu

AU - Mosquera, Jesús

AU - Morgese, Giulia

AU - Schoenmakers, Sandra M C

AU - Cardinaels, Ruth

AU - Palmans, Anja R.A.

AU - Meijer, E.W.

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PY - 2021/11/8

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N2 - The use of supramolecular polymers to construct functional biomaterials is gaining more attention due to the tunable dynamic behavior and fibrous structures of supramolecular polymers, which resemble those found in natural systems, such as the extracellular matrix. Nevertheless, to obtain a biomaterial capable of mimicking native systems, complex biomolecules should be incorporated, as they allow one to achieve essential biological processes. In this study, supramolecular polymers based on water-soluble benzene-1,3,5-tricarboxamides (BTAs) were assembled in the presence of hyaluronic acid (HA) both in solution and hydrogel states. The coassembly of BTAs bearing tetra(ethylene glycol) at the periphery (BTA-OEG4) and HA at different ratios showed strong interactions between the two components that led to the formation of short fibers and heterogeneous hydrogels. BTAs were further covalently linked to HA (HA-BTA), resulting in a polymer that was unable to assemble into fibers or form hydrogels due to the high hydrophilicity of HA. However, coassembly of HA-BTA with BTA-OEG4 resulted in the formation of long fibers, similar to those formed by BTA-OEG4 alone, and hydrogels were produced with tunable stiffness ranging from 250 to 700 Pa, which is 10-fold higher than that of hydrogels assembled with only BTA-OEG4. Further coassembly of BTA-OEG4 fibers with other polysaccharides showed that except for dextran, all polysaccharides studied interacted with BTA-OEG4 fibers. The possibility of incorporating polysaccharides into BTA-based materials paves the way for the creation of dynamic complex biomaterials.

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Introducing Hyaluronic Acid into Supramolecular Polymers and Hydrogels

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