Synergistic complexation of phenol functionalized polymer induced in situ microfiber formation for 3D printing of marine-based hydrogels

H. Jafari; C. Delporte; K.V. Bernaerts; H. Alimoradi; L. Nie; D. Podstawczyk; K.C. Tam; A. Shavandi

doi:10.1039/d1gc04347a

Synergistic complexation of phenol functionalized polymer induced in situ microfiber formation for 3D printing of marine-based hydrogels

H. Jafari^*, C. Delporte, K.V. Bernaerts, H. Alimoradi, L. Nie, D. Podstawczyk, K.C. Tam^*, A. Shavandi^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

Abstract

The design of 3D printable bio-based hydrogels with enhanced mechanical properties and minimal chemical modification can open new opportunities in the field of biomedical applications. A facile and safe approach is proposed to prepare mechanically reinforced chitosan-based hydrogels via a phenolated polyelectrolyte complex (PHEC) and enzyme-mediated crosslinking. PHEC was formed between phenolated chitosan and alginate, leading to the formation of in situ phenol-functionalized microfibers that exhibited excellent 3D printability. The synergistic complexation enhanced the loss modulus (60 times), toughness, flexibility, and moldability of hydrogel as well as dynamic viscosity (20 times) of the hydrogel precursor compared to individual phenolated chitosan and alginate hydrogels. This complexation endowed the material with excellent printability without sacrificing the hydrogel's elasticity. This study proposes a strategy to design tough and 3D printable marine-based hydrogels based on the synergistic complexation of a phenolated polyelectrolyte complex and enzyme-mediated crosslinking.

Original language	English
Pages (from-to)	2409-2422
Number of pages	14
Journal	Green Chemistry
Volume	24
Issue number	6
Early online date	5 Jan 2022
DOIs	https://doi.org/10.1039/d1gc04347a
Publication status	Published - 21 Mar 2022

Keywords

ELECTROSTATIC INTERACTIONS
CHITOSAN HYDROGELS
HIGH-STRENGTH
ALGINATE
DERIVATIVES
PROPERTY
STRATEGY
TOUGH

Access to Document

10.1039/d1gc04347a

Cite this

@article{1984c8c51fa1490c942520c779678d5e,

title = "Synergistic complexation of phenol functionalized polymer induced in situ microfiber formation for 3D printing of marine-based hydrogels",

abstract = "The design of 3D printable bio-based hydrogels with enhanced mechanical properties and minimal chemical modification can open new opportunities in the field of biomedical applications. A facile and safe approach is proposed to prepare mechanically reinforced chitosan-based hydrogels via a phenolated polyelectrolyte complex (PHEC) and enzyme-mediated crosslinking. PHEC was formed between phenolated chitosan and alginate, leading to the formation of in situ phenol-functionalized microfibers that exhibited excellent 3D printability. The synergistic complexation enhanced the loss modulus (60 times), toughness, flexibility, and moldability of hydrogel as well as dynamic viscosity (20 times) of the hydrogel precursor compared to individual phenolated chitosan and alginate hydrogels. This complexation endowed the material with excellent printability without sacrificing the hydrogel's elasticity. This study proposes a strategy to design tough and 3D printable marine-based hydrogels based on the synergistic complexation of a phenolated polyelectrolyte complex and enzyme-mediated crosslinking.",

keywords = "ELECTROSTATIC INTERACTIONS, CHITOSAN HYDROGELS, HIGH-STRENGTH, ALGINATE, DERIVATIVES, PROPERTY, STRATEGY, TOUGH",

author = "H. Jafari and C. Delporte and K.V. Bernaerts and H. Alimoradi and L. Nie and D. Podstawczyk and K.C. Tam and A. Shavandi",

note = "Funding Information: H. J and A. S. acknowledge funding from Innoviris Brussels, Belgium ( https://innoviris.brussels ) under the project 2019 – BRIDGE – 4: RE4BRU. The content is solely the responsibility of the authors and does not necessarily represent the official views of the above-mentioned funding agency. The authors would like to thank Dr V{\'e}ronique Fontaine for her assistance with the antibacterial test. Publisher Copyright: {\textcopyright} 2022 the Owner Societies.",

year = "2022",

month = mar,

day = "21",

doi = "10.1039/d1gc04347a",

language = "English",

volume = "24",

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journal = "Green Chemistry",

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publisher = "Royal Society of Chemistry",

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T1 - Synergistic complexation of phenol functionalized polymer induced in situ microfiber formation for 3D printing of marine-based hydrogels

AU - Jafari, H.

AU - Delporte, C.

AU - Bernaerts, K.V.

AU - Alimoradi, H.

AU - Nie, L.

AU - Podstawczyk, D.

AU - Tam, K.C.

AU - Shavandi, A.

N1 - Funding Information: H. J and A. S. acknowledge funding from Innoviris Brussels, Belgium ( https://innoviris.brussels ) under the project 2019 – BRIDGE – 4: RE4BRU. The content is solely the responsibility of the authors and does not necessarily represent the official views of the above-mentioned funding agency. The authors would like to thank Dr Véronique Fontaine for her assistance with the antibacterial test. Publisher Copyright: © 2022 the Owner Societies.

PY - 2022/3/21

Y1 - 2022/3/21

N2 - The design of 3D printable bio-based hydrogels with enhanced mechanical properties and minimal chemical modification can open new opportunities in the field of biomedical applications. A facile and safe approach is proposed to prepare mechanically reinforced chitosan-based hydrogels via a phenolated polyelectrolyte complex (PHEC) and enzyme-mediated crosslinking. PHEC was formed between phenolated chitosan and alginate, leading to the formation of in situ phenol-functionalized microfibers that exhibited excellent 3D printability. The synergistic complexation enhanced the loss modulus (60 times), toughness, flexibility, and moldability of hydrogel as well as dynamic viscosity (20 times) of the hydrogel precursor compared to individual phenolated chitosan and alginate hydrogels. This complexation endowed the material with excellent printability without sacrificing the hydrogel's elasticity. This study proposes a strategy to design tough and 3D printable marine-based hydrogels based on the synergistic complexation of a phenolated polyelectrolyte complex and enzyme-mediated crosslinking.

AB - The design of 3D printable bio-based hydrogels with enhanced mechanical properties and minimal chemical modification can open new opportunities in the field of biomedical applications. A facile and safe approach is proposed to prepare mechanically reinforced chitosan-based hydrogels via a phenolated polyelectrolyte complex (PHEC) and enzyme-mediated crosslinking. PHEC was formed between phenolated chitosan and alginate, leading to the formation of in situ phenol-functionalized microfibers that exhibited excellent 3D printability. The synergistic complexation enhanced the loss modulus (60 times), toughness, flexibility, and moldability of hydrogel as well as dynamic viscosity (20 times) of the hydrogel precursor compared to individual phenolated chitosan and alginate hydrogels. This complexation endowed the material with excellent printability without sacrificing the hydrogel's elasticity. This study proposes a strategy to design tough and 3D printable marine-based hydrogels based on the synergistic complexation of a phenolated polyelectrolyte complex and enzyme-mediated crosslinking.

KW - ELECTROSTATIC INTERACTIONS

KW - CHITOSAN HYDROGELS

KW - HIGH-STRENGTH

KW - ALGINATE

KW - DERIVATIVES

KW - PROPERTY

KW - STRATEGY

KW - TOUGH

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DO - 10.1039/d1gc04347a

M3 - Article

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JF - Green Chemistry

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