, Volume 25, Issue 1, pp 485–502 | Cite as

Dual-responsive composite hydrogels based on TEMPO-oxidized cellulose nanofibril and poly(N-isopropylacrylamide) for model drug release

Original Paper


Dual responsive composite hydrogels were successfully prepared by combining cellulose nanofibril (CNF) isolated by 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-mediated oxidation with thermally responsive poly(N-isopropylacrylamide) (PNIPAAm) for drug release at 10 wt% CNF loading and − 20 °C polymerization temperature. pH responsive hydrogels were acquired by adjusting the carboxyl charge level of the CNF during TEMPO-mediated oxidation. CNF–PNIPAAm hydrogels fabricated were characterized in regards to compressive strength, functional group, low critical solution temperature (LCST), and swelling ratio of the hydrogels at different temperatures from 20 to 60 °C and pH levels from 2 to 10. Finally, the drug release behavior of these hydrogels was also investigated using methylene blue as a model drug. As the carboxylate content increases, the dual responsiveness of hydrogel improved at the expense of the compression strength. The CNF–PNIPAAm hydrogels were swollen and translucent below the LCST, and shrunken and opaque above the LCST. The Higuchi and the Krosmeyer and Peppas model was best-fitted to the drug release behavior of these hydrogels at pH 10 and pH 2, respectively. The results also indicated that a proper selection of polymerization temperature provided a way of tuning the dual-responsiveness of the hydrogels. These results also suggest that the CNF–PNIPAAm hydrogels can release drugs on demand.


Cellulose nanofibrils TEMPO PNIPAAm Hydrogel Dual-responsiveness Model drug release 



This work was financially supported by Joint Research Program through the National Research Foundation (NRF) of Korea and funded by the Ministry of Education, Science and Technology (Grant No: 2016K1A3A1A12953690).

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary material

10570_2017_1585_MOESM1_ESM.docx (1.9 mb)
Supplementary material 1 (DOCX 1932 kb)


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© Springer Science+Business Media B.V., part of Springer Nature 2017

Authors and Affiliations

  1. 1.Department of Wood and Paper SciencesKyungpook National UniversityDaeguRepublic of Korea
  2. 2.Institute of Agricultural Science and TechnologyKyungpook National UniversityDaeguRepublic of Korea
  3. 3.Department of Chemical SciencesUniversity of PadovaPadovaItaly

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