3D Printing of Biocompatible Nanocellulose-reinforced Hydrogels <italic style="font-style: italic">via</italic> Polymerizable Ternary Deep Eutectic Solvent Assistance

Vitaly K. Vorobiov; Maria P. Sokolova; Yuliya A. Nashchekina; Veronika S. Andreeva; Ivan S. Kuryndin; Yulia E. Gorshkova; Ruslan Y. Smyslov; Eugene V. Sivtsov; Michael A. Smirnov

doi:10.1007/s10118-025-3452-1

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3D Printing of Biocompatible Nanocellulose-reinforced Hydrogels via Polymerizable Ternary Deep Eutectic Solvent Assistance

RESEARCH ARTICLE | Updated：2025-12-03

- 3D Printing of Biocompatible Nanocellulose-reinforced Hydrogels via Polymerizable Ternary Deep Eutectic Solvent Assistance
- Chinese Journal of Polymer Science Vol. 43, Issue 12, Pages: 2285-2298(2025)
- Affiliations：
  
  a.Branch of Petersburg Nuclear Physics Institute named by B.P. Konstantinov of National Research Centre «Kurchatov Institute» - Institute of Macromolecular Compounds, St. Petersburg 199004, Russia
  b.Institute of Cytology of the Russian Academy of Sciences, Center of Cell Technologies, St. Petersburg 194064, Russia
  c.Joint Institute for Nuclear Research, Dubna 141980, Russia
  d.Institute of Physics, Kazan Federal University, Kazan 420008, Russia
  e.Institute of Biomedical Systems and Biotechnology, Graduate School of Biomedical Systems and Technology, Peter the Great St. Petersburg Polytechnic University (SPbPU), St. Petersburg 19525, Russia
  f.Saint Petersburg State Institute of Technology, St. Petersburg 190013, Russia
- Author bio：
  
  vitaly.vorobiov.rrt@gmail.com (V.K.V.)
  smirnov_michael@mail.ru (M.A.S.)
- Funds：
- DOI：10.1007/s10118-025-3452-1
  CLC：
- Received：18 June 2025，
  
  Accepted：10 September 2025，
  
  Online First：12 November 2025，
  
  Published：15 December 2025
- Accepted：
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Vorobiov, V. K.; Sokolova, M. P.; Nashchekina, Y. A.; Andreeva, V. S.; Kuryndin, I. S.; Gorshkova, Y. E.; Smyslov, R. Y.; Sivtsov, E. V.; Smirnov, M. A. 3D printing of biocompatible nanocellulose-reinforced hydrogels via polymerizable ternary deep eutectic solvent assistance. Chinese J. Polym. Sci. 2025, 43, 2285–2298

Vitaly K. Vorobiov, Maria P. Sokolova, Yuliya A. Nashchekina, et al. 3D Printing of Biocompatible Nanocellulose-reinforced Hydrogels via Polymerizable Ternary Deep Eutectic Solvent Assistance[J]. Chinese Journal of Polymer Science, 2025, 43(12): 2285-2298. DOI: 10.1007/s10118-025-3452-1.
Vorobiov, V. K.; Sokolova, M. P.; Nashchekina, Y. A.; Andreeva, V. S.; Kuryndin, I. S.; Gorshkova, Y. E.; Smyslov, R. Y.; Sivtsov, E. V.; Smirnov, M. A. 3D printing of biocompatible nanocellulose-reinforced hydrogels via polymerizable ternary deep eutectic solvent assistance. Chinese J. Polym. Sci. 2025, 43, 2285–2298 DOI： 10.1007/s10118-025-3452-1.

Vitaly K. Vorobiov, Maria P. Sokolova, Yuliya A. Nashchekina, et al. 3D Printing of Biocompatible Nanocellulose-reinforced Hydrogels via Polymerizable Ternary Deep Eutectic Solvent Assistance[J]. Chinese Journal of Polymer Science, 2025, 43(12): 2285-2298. DOI: 10.1007/s10118-025-3452-1. DOI：

摘要

This work demonstrates 3D printing of composite hydrogels using DES/CNF-based inks. DES reduces CNF agglomeration

enabling better printability than aqueous dispersions

and enhances mechanical properties exceeding molded counterparts owing to layered architecture and filler alignment. The prepared materials are non-toxic and exhibit cartilage-like mechanics

demonstrating potential for biomedical applications.

Abstract

Two- and three-component deep eutectic solvents (DES) based on acrylic acid (AA)

acrylamide (AAm)

and choline chloride (ChCl) were used to disintegrate bacterial cellulose into cellulose nanofibers (CNF). As a result

polymerizable precursors suitable for 3D printing with CNF as a rheology modifier and reinforcer with formation of interpenetrating double polymer network were obtained after UV curing. Composite hydrogels were formed by replacing ChCl with water. It was found that the introduction of amide groups into the acrylate polymer matrix resulted in an increase in compressive strength. The layered architecture of the 3D printed products provides greater mechanical strength compared to molded products. The structure of the composites was investigated using wide-angle X-ray scattering (WAXS)

small-angle X-ray scattering (SAXS)

atomic force microscopy (AFM) and polarized light microscopy. These studies suggest that the enhanced mechanical properties of the 3D printed hydrogels are associated with swelling and branching of CNF in the DES

as well as alignment of the filler during extrusion. For comparative analysis

composite hydrogels were also prepared using aqueous solutions of AA and AA/AAm with dispersed CNF. However

the 3D printing process was hampered in this case due to cellulose agglomeration. Mechanical testing revealed the formation of premature microcracks in these samples

which were not observed in composites produced using DES. Cytotoxicity of the composite hydrogels was also tested. The results provide valuable insights into the production of strong (up to 3.4 MPa) homogeneous composite hydrogels using 3D printing with nanocellulose filler.

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Laboratory of Polymer Physics and Chemistry, Beijing National Laboratory of Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences

China Academy of Cultural Heritage

School of Conservation Science & Technology for Cultural Heritage, Key Laboratory of Materials and Technology for Unearthed Cultural Heritage Conservation, Shaanxi University of Science & Technology

University of Chinese Academy of Sciences

MOE Key Laboratory of Macromolecular Synthesis and Functionalization, Department of Polymer Science and Engineering, Zhejiang University

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3D Printing of Biocompatible Nanocellulose-reinforced Hydrogels via Polymerizable Ternary Deep Eutectic Solvent Assistance

DOI：10.1007/s10118-025-3452-1

摘要

Abstract

关键词

Keywords

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