Injectable thiol-ene hydrogel of galactoglucomannan and cellulose nanocrystals in delivery of therapeutic inorganic ions with embedded bioactive glass nanoparticles

Qingbo Wang; Wenyang Xu; Rajesh Koppolu; Bas van Bochove; Jukka Seppälä; Leena Hupa; Stefan Willför; Chunlin Xu; Xiaoju Wang

doi:10.1016/j.carbpol.2021.118780

Injectable thiol-ene hydrogel of galactoglucomannan and cellulose nanocrystals in delivery of therapeutic inorganic ions with embedded bioactive glass nanoparticles

Qingbo Wang, Wenyang Xu, Rajesh Koppolu, Bas van Bochove, Jukka Seppälä, Leena Hupa, Stefan Willför, Chunlin Xu, Xiaoju Wang^*

^*Corresponding author for this work

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

34 Citations (Scopus)

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Abstract

We propose an injectable nanocomposite hydrogel that is photo-curable via light-induced thiol-ene addition between methacrylate modified O-acetyl-galactoglucomannan (GGMMA) and thiolated cellulose nanocrystal (CNC-SH). Compared to free-radical chain polymerization, the orthogonal step-growth of thiol-ene addition allows a less heterogeneous hydrogel network and more rapid crosslinking kinetics. CNC-SH reinforced the GGMMA hydrogel as both a nanofiller and a crosslinker to GGMMA resulting in an interpenetrating network via thiol-ene addition. Importantly, the mechanical stiffness of the GGMMA/CNC-SH hydrogel is mainly determined by the stoichiometric ratio between the thiol groups on CNC-SH and the methacrylate groups in GGMMA. Meanwhile, the bioactive glass nanoparticle (BaGNP)-laden hydrogels of GGMMA/CNC-SH showed a sustained release of therapeutic ions in simulated body fluid in vitro, which extended the bioactive function of hydrogel matrix. Furthermore, the suitability of the GGMMA/CNC-SH formulation as biomaterial resin to fabricate digitally designed hydrogel constructs via digital light processing (DLP) lithography printing was evaluated.

Original language	English
Article number	118780
Journal	Carbohydrate Polymers
Volume	276
DOIs	https://doi.org/10.1016/j.carbpol.2021.118780
Publication status	Published - 15 Jan 2022
MoE publication type	A1 Journal article-refereed

Funding

Qingbo Wang would like to acknowledge the financial support from the China Scholarship Council (Student ID 201907960002 ) and KAUTE Foundation (Project number 20190031 ) to his doctoral study at Åbo Akademi University (ÅAU), Finland. Xiaoju Wang would like to thank Academy of Finland ( 333158 ) as well as Jane and Aatos Erkko Foundation for their funds to her research at ÅAU. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) and has used the Aalto University Bioeconomy Facilities. Luyao Wang, Yury Brusentsev, and Sara Lund are respectively acknowledged for their technical assistance on TEM, NMR, and elemental analysis. Adrian Stiller and Jaana Paananen are acknowledged for their assistance on BaGNP dissolution experiments. Qingbo Wang would like to acknowledge the financial support from the China Scholarship Council (Student ID 201907960002) and KAUTE Foundation (Project number 20190031) to his doctoral study at ?bo Akademi University (?AU), Finland. Xiaoju Wang would like to thank Academy of Finland (333158) as well as Jane and Aatos Erkko Foundation for their funds to her research at ?AU. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) and has used the Aalto University Bioeconomy Facilities. Luyao Wang, Yury Brusentsev, and Sara Lund are respectively acknowledged for their technical assistance on TEM, NMR, and elemental analysis. Adrian Stiller and Jaana Paananen are acknowledged for their assistance on BaGNP dissolution experiments.

Keywords

Bioactive glass nanoparticles
Galactoglucomannan methacrylate
Photo-crosslinkable injectable hydrogels
Thiol-ene chemistry
Thiolated cellulose nanocrystal

Access to Document

10.1016/j.carbpol.2021.118780Licence: CC BY

1-s2.0-S014486172101167X-mainFinal published version, 4.16 MBLicence: CC BY

https://urn.fi/URN:NBN:fi-fe2023030329304

Cite this

@article{fe98a86e5d034e6b9df2cafd6ba81592,

title = "Injectable thiol-ene hydrogel of galactoglucomannan and cellulose nanocrystals in delivery of therapeutic inorganic ions with embedded bioactive glass nanoparticles",

abstract = "We propose an injectable nanocomposite hydrogel that is photo-curable via light-induced thiol-ene addition between methacrylate modified O-acetyl-galactoglucomannan (GGMMA) and thiolated cellulose nanocrystal (CNC-SH). Compared to free-radical chain polymerization, the orthogonal step-growth of thiol-ene addition allows a less heterogeneous hydrogel network and more rapid crosslinking kinetics. CNC-SH reinforced the GGMMA hydrogel as both a nanofiller and a crosslinker to GGMMA resulting in an interpenetrating network via thiol-ene addition. Importantly, the mechanical stiffness of the GGMMA/CNC-SH hydrogel is mainly determined by the stoichiometric ratio between the thiol groups on CNC-SH and the methacrylate groups in GGMMA. Meanwhile, the bioactive glass nanoparticle (BaGNP)-laden hydrogels of GGMMA/CNC-SH showed a sustained release of therapeutic ions in simulated body fluid in vitro, which extended the bioactive function of hydrogel matrix. Furthermore, the suitability of the GGMMA/CNC-SH formulation as biomaterial resin to fabricate digitally designed hydrogel constructs via digital light processing (DLP) lithography printing was evaluated.",

keywords = "Bioactive glass nanoparticles, Galactoglucomannan methacrylate, Photo-crosslinkable injectable hydrogels, Thiol-ene chemistry, Thiolated cellulose nanocrystal",

author = "Qingbo Wang and Wenyang Xu and Rajesh Koppolu and \{van Bochove\}, Bas and Jukka Sepp{\"a}l{\"a} and Leena Hupa and Stefan Willf{\"o}r and Chunlin Xu and Xiaoju Wang",

note = "Funding Information: Qingbo Wang would like to acknowledge the financial support from the China Scholarship Council (Student ID 201907960002 ) and KAUTE Foundation (Project number 20190031 ) to his doctoral study at {\AA}bo Akademi University ({\AA}AU), Finland. Xiaoju Wang would like to thank Academy of Finland ( 333158 ) as well as Jane and Aatos Erkko Foundation for their funds to her research at {\AA}AU. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) and has used the Aalto University Bioeconomy Facilities. Luyao Wang, Yury Brusentsev, and Sara Lund are respectively acknowledged for their technical assistance on TEM, NMR, and elemental analysis. Adrian Stiller and Jaana Paananen are acknowledged for their assistance on BaGNP dissolution experiments. Funding Information: Qingbo Wang would like to acknowledge the financial support from the China Scholarship Council (Student ID 201907960002) and KAUTE Foundation (Project number 20190031) to his doctoral study at ?bo Akademi University (?AU), Finland. Xiaoju Wang would like to thank Academy of Finland (333158) as well as Jane and Aatos Erkko Foundation for their funds to her research at ?AU. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) and has used the Aalto University Bioeconomy Facilities. Luyao Wang, Yury Brusentsev, and Sara Lund are respectively acknowledged for their technical assistance on TEM, NMR, and elemental analysis. Adrian Stiller and Jaana Paananen are acknowledged for their assistance on BaGNP dissolution experiments. Publisher Copyright: {\textcopyright} 2021 The Authors",

year = "2022",

month = jan,

day = "15",

doi = "10.1016/j.carbpol.2021.118780",

language = "English",

volume = "276",

journal = "Carbohydrate Polymers",

issn = "0144-8617",

publisher = "Elsevier",

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TY - JOUR

T1 - Injectable thiol-ene hydrogel of galactoglucomannan and cellulose nanocrystals in delivery of therapeutic inorganic ions with embedded bioactive glass nanoparticles

AU - Wang, Qingbo

AU - Xu, Wenyang

AU - Koppolu, Rajesh

AU - van Bochove, Bas

AU - Seppälä, Jukka

AU - Hupa, Leena

AU - Willför, Stefan

AU - Xu, Chunlin

AU - Wang, Xiaoju

N1 - Funding Information: Qingbo Wang would like to acknowledge the financial support from the China Scholarship Council (Student ID 201907960002 ) and KAUTE Foundation (Project number 20190031 ) to his doctoral study at Åbo Akademi University (ÅAU), Finland. Xiaoju Wang would like to thank Academy of Finland ( 333158 ) as well as Jane and Aatos Erkko Foundation for their funds to her research at ÅAU. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) and has used the Aalto University Bioeconomy Facilities. Luyao Wang, Yury Brusentsev, and Sara Lund are respectively acknowledged for their technical assistance on TEM, NMR, and elemental analysis. Adrian Stiller and Jaana Paananen are acknowledged for their assistance on BaGNP dissolution experiments. Funding Information: Qingbo Wang would like to acknowledge the financial support from the China Scholarship Council (Student ID 201907960002) and KAUTE Foundation (Project number 20190031) to his doctoral study at ?bo Akademi University (?AU), Finland. Xiaoju Wang would like to thank Academy of Finland (333158) as well as Jane and Aatos Erkko Foundation for their funds to her research at ?AU. This work is also part of activities within the Johan Gadolin Process Chemistry Centre (PCC) and has used the Aalto University Bioeconomy Facilities. Luyao Wang, Yury Brusentsev, and Sara Lund are respectively acknowledged for their technical assistance on TEM, NMR, and elemental analysis. Adrian Stiller and Jaana Paananen are acknowledged for their assistance on BaGNP dissolution experiments. Publisher Copyright: © 2021 The Authors

PY - 2022/1/15

Y1 - 2022/1/15

N2 - We propose an injectable nanocomposite hydrogel that is photo-curable via light-induced thiol-ene addition between methacrylate modified O-acetyl-galactoglucomannan (GGMMA) and thiolated cellulose nanocrystal (CNC-SH). Compared to free-radical chain polymerization, the orthogonal step-growth of thiol-ene addition allows a less heterogeneous hydrogel network and more rapid crosslinking kinetics. CNC-SH reinforced the GGMMA hydrogel as both a nanofiller and a crosslinker to GGMMA resulting in an interpenetrating network via thiol-ene addition. Importantly, the mechanical stiffness of the GGMMA/CNC-SH hydrogel is mainly determined by the stoichiometric ratio between the thiol groups on CNC-SH and the methacrylate groups in GGMMA. Meanwhile, the bioactive glass nanoparticle (BaGNP)-laden hydrogels of GGMMA/CNC-SH showed a sustained release of therapeutic ions in simulated body fluid in vitro, which extended the bioactive function of hydrogel matrix. Furthermore, the suitability of the GGMMA/CNC-SH formulation as biomaterial resin to fabricate digitally designed hydrogel constructs via digital light processing (DLP) lithography printing was evaluated.

AB - We propose an injectable nanocomposite hydrogel that is photo-curable via light-induced thiol-ene addition between methacrylate modified O-acetyl-galactoglucomannan (GGMMA) and thiolated cellulose nanocrystal (CNC-SH). Compared to free-radical chain polymerization, the orthogonal step-growth of thiol-ene addition allows a less heterogeneous hydrogel network and more rapid crosslinking kinetics. CNC-SH reinforced the GGMMA hydrogel as both a nanofiller and a crosslinker to GGMMA resulting in an interpenetrating network via thiol-ene addition. Importantly, the mechanical stiffness of the GGMMA/CNC-SH hydrogel is mainly determined by the stoichiometric ratio between the thiol groups on CNC-SH and the methacrylate groups in GGMMA. Meanwhile, the bioactive glass nanoparticle (BaGNP)-laden hydrogels of GGMMA/CNC-SH showed a sustained release of therapeutic ions in simulated body fluid in vitro, which extended the bioactive function of hydrogel matrix. Furthermore, the suitability of the GGMMA/CNC-SH formulation as biomaterial resin to fabricate digitally designed hydrogel constructs via digital light processing (DLP) lithography printing was evaluated.

KW - Bioactive glass nanoparticles

KW - Galactoglucomannan methacrylate

KW - Photo-crosslinkable injectable hydrogels

KW - Thiol-ene chemistry

KW - Thiolated cellulose nanocrystal

UR - https://www.scopus.com/pages/publications/85120990213

U2 - 10.1016/j.carbpol.2021.118780

DO - 10.1016/j.carbpol.2021.118780

M3 - Article

AN - SCOPUS:85120990213

SN - 0144-8617

VL - 276

JO - Carbohydrate Polymers

JF - Carbohydrate Polymers

M1 - 118780

ER -

Injectable thiol-ene hydrogel of galactoglucomannan and cellulose nanocrystals in delivery of therapeutic inorganic ions with embedded bioactive glass nanoparticles

Abstract

Funding

Keywords

Access to Document

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SusCellInk: Sustainable nanocellulose-based bioinks towards diverse material functionalities and therapeutic delivery of bioactive cues

Cite this

Injectable thiol-ene hydrogel of galactoglucomannan and cellulose nanocrystals in delivery of therapeutic inorganic ions with embedded bioactive glass nanoparticles

Abstract

Funding

Keywords

Access to Document

Other files and links

Fingerprint

Projects

SusCellInk: Sustainable nanocellulose-based bioinks towards diverse material functionalities and therapeutic delivery of bioactive cues

Cite this