University of Oulu

Hujaya, S., Lorite, G., Vainio, S., Liimatainen, H. (2018) Polyion complex hydrogels from chemically modified cellulose nanofibrils: Structure-function relationship and potential for controlled and pH-responsive release of doxorubicin. Acta Biomaterialia, 75, 346-357. doi:10.1016/j.actbio.2018.06.013

Polyion complex hydrogels from chemically modified cellulose nanofibrils : structure-function relationship and potential for controlled and pH-responsive release of doxorubicin

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Author: Hujaya, Sry D.1; Lorite, Gabriela S.2; Vainio, Seppo J.3;
Organizations: 1Fibre and Particle Engineering Research Unit, University of Oulu
2Microelectronics Research Unit, University of Oulu
3Laboratory of Developmental Biology, Biocenter Oulu, University of Oulu
Format: article
Version: accepted version
Access: open
Online Access: PDF Full Text (PDF, 1.8 MB)
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Language: English
Published: Elsevier, 2018
Publish Date: 2020-06-08


Herein, we report the fabrication of a polyion complex hydrogel from two oppositely charged derivatives of cellulose nanofibrils (CNF). CNF was produced from dissolving pulp through subsequent periodate oxidation, chemical modification, and microfluidization. Three different durations for periodate oxidation (30 min, 120 min, and 180 min) resulted in three different aldehyde contents. Further, two types of chemical modifications were introduced to react with the resulting aldehydes: chlorite oxidation to yield anionic CNF with carboxylic acid groups (DCC) and imination with Girard’s reagent T to yield cationic CNF containing quaternary ammonium groups (CDAC). Functional group contents were assessed using conductometric titration and elemental analysis, while nanofibril morphologies were assessed using atomic force microscopy (AFM). Longer durations of periodate oxidation did not yield different width profile but was found to decrease fibril length. The formation of self-standing hydrogel through mixing of DCC and CDAC dispersions was investigated. Oscillatory rheology was performed to assess the relative strengths of different gels. Self-standing hydrogels were obtained from mixture of DCC180 and CDAC180 dispersions in acetate buffer at pH 4 and 5 at a low concentration of 0.5% w/w that displayed approximately 10-fold increase in storage and loss moduli compared to those of the individual dispersions. Self-standing gels containing doxorubicin (an anticancer drug) displayed pH-responsive release profiles. At physiological pH 7.4, approximately 65% of doxorubicin was retained past a burst release regime, while complete release was observed within 5 days at pH 4. Biocompatibility of DCC180, CDAC180, and their mixture were investigated through quantification of the metabolic activity of NIH3T3 cells in vitro. No significant cytotoxicity was observed at concentrations up to 900 µg/mL. In short, the nanocellulose-based polyion complex hydrogels obtained in this study are promising nature-derived materials for biomedical applications.

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Series: Acta biomaterialia
ISSN: 1742-7061
ISSN-E: 1878-7568
ISSN-L: 1742-7061
Volume: 75
Pages: 346 - 357
DOI: 10.1016/j.actbio.2018.06.013
Type of Publication: A1 Journal article – refereed
Field of Science: 216 Materials engineering
217 Medical engineering
221 Nanotechnology
Funding: The authors kindly acknowledge financial support from the Academy of Finland (projects NanoBioMass (307535), CNT4Tissue, 206038, 121647, 250900 and 260056), the Sigrid Jusélius Foundation, and the European Community’s Seventh Framework Program FP7/2009 under grant agreement 305608 (EURenOmics: European Consortium for High-Throughput Research in Rare Kidney Diseases).
EU Grant Number: (305608) EURENOMICS - European Consortium for High-Throughput Research in Rare Kidney Diseases
Academy of Finland Grant Number: 307535
Detailed Information: 307535 (Academy of Finland Funding decision)
121647 (Academy of Finland Funding decision)
250900 (Academy of Finland Funding decision)
260056 (Academy of Finland Funding decision)
Copyright information: © 2018. This manuscript version is made available under the CC-BY-NC-ND 4.0 license