Organic acid cross-linked 3D printed cellulose nanocomposite bioscaffolds with controlled porosity, mechanical strength, and biocompatibility

Štiglic, Andreja Dobaj; Gürer, Fazilet; Lackner, Florian; Bračič, Doris; Winter, Armin; Gradišnik, Lidija; Makuc, Damjan; Kargl, Rupert; Duarte, Isabel; Plavec, Janez; Maver, Uroš; Beaumont, Marco; Kleinschek, Karin Stana; Mohan, Tamilselvan

doi:10.1016/j.isci.2022.104263

Cited by 17 publications

(42 citation statements)

References 60 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…All NFC/CMC curves in Figure exhibit one slope change corresponding to the simultaneous deprotonation of the carboxyl groups of NFC and CMC (pH 2–7 in Figure A and pH 2–9 in Figure B). This is consistent with the data in the literature. , The carboxylate charges of neat NFC and CMC were 0.35 ± 0.05 mmol/g and 3.51 ± 0.17 mmol/g, respectively. A significant difference in the charges between the non-cross-linked and the CA cross-linked scaffolds can be clearly seen.…”

Section: Resultssupporting

confidence: 93%

“…All freeze-dried scaffolds were cross-linked by DHT heat treatment at 120 °C for 24 h, as reported elsewhere. , The CA cross-linked scaffolds were neutralized with 0.1 M NaOH (60 min), rinsed with Milli-Q water (24 h), and air-dried at room temperature. These dried scaffolds were designated as “NC/CAx” where x is the concentration of CA in wt %.…”

Section: Methodsmentioning

confidence: 99%

“…This is consistent with the data in the literature. 33,62 The carboxylate charges of neat NFC and CMC were 0.35 ± 0.05 mmol/g and 3.51 ± 0.17 mmol/g, respectively. A significant difference in the charges between the non-cross-linked and the CA cross-linked scaffolds can be clearly seen.…”

Section: Scaffold Preparation and Glycosyltransferasesmentioning

confidence: 99%

“…They can also be used to fabricate scaffolds with tailored properties and well-defined architectures that are controlled and consistent in their internal architecture, outer geometry, strand size, and pore size and distribution. By controlling the latter, the dimensional and mechanical properties of the scaffolds can be improved. ,, Moreover, 3D printing allows us to fabricate scaffolds from plethora of materials without a material lost and at low cost. , However, the research on the development of stable and porous scaffolds through 3D printing from NFC-based composites for enzyme immobilization is still in its infancy. This motivated us to develop chemically cross-linked NFC-based scaffolds from an ink consisting of NFC, CMC, and citric acid and apply them for the single and coimmobilization of enzymes and compare their efficiency.…”

Section: Introductionmentioning

confidence: 99%

“…This motivated us to develop chemically cross-linked NFC-based scaffolds from an ink consisting of NFC, CMC, and citric acid and apply them for the single and coimmobilization of enzymes and compare their efficiency. The scaffolds were prepared by the combination of direct-ink-writing (DIW) 3D printing, freeze-drying, and dehydrothermal (DHT) treatment. , The latter treatment in the dry state induces a cross-linking of NFC and CMC with CA via an ester bond. , The CA cross-linked scaffolds can provide not only an exceptional mechanical and dimensional stability in the aqueous environment but also an adequate porosity or porous structure, hydrophilicity, and fluid uptake capacity. NFC in combination with other charged polysaccharides like CMC not only offers a better environment and compatibility but also exhibits a high surface-to-volume ratio, size (fibril width: 5–20 nm), specific strength and stiffness, and hydrophilicity.…”

Section: Introductionmentioning

confidence: 99%

See 4 more Smart Citations

3D Printed Porous Nanocellulose-Based Scaffolds As Carriers for Immobilization of Glycosyltransferases

Lackner

Liu

Štiglic

et al. 2022

ACS Appl. Bio Mater.

Self Cite

View full text Add to dashboard Cite

Biocatalysis is increasingly becoming an alternative method for the synthesis of industrially relevant complex molecules. This can be realized by using enzyme immobilized polysaccharide-based 3D scaffolds as compatible carriers, with defined properties. Especially, immobilization of either single or multiple enzymes on a 3D printed polysaccharide scaffold, exhibiting well-organized interconnected porous structure and morphology, is a versatile approach to access the performance of industrially important enzymes. Here, we demonstrated the use of nanocellulose-based 3D porous scaffolds for the immobilization of glycosyltransferases, responsible for glycosylation in natural biosynthesis. The scaffolds were produced using an ink containing nanofibrillated cellulose (NFC), carboxymethyl cellulose (CMC), and citric acid. Direct-ink-writing 3D printing followed by freeze-drying and dehydrothermal treatment at elevated temperature resulted in chemically cross-linked scaffolds, featuring tunable negative charges (2.2−5.0 mmol/g), pore sizes (10−800 μm), fluid uptake capacity, and exceptional dimensional and mechanical stability in the wet state. The negatively charged scaffolds were applied to immobilize two sugar nucleotide-dependent glycosyltransferases (C-glycosyltransferase, Z basic2 -CGT; sucrose synthase, Z basic2 -SuSy), each harboring a cationic binding module (Z basic2 ) to promote charge-based enzyme adsorption. Both enzymes were immobilized at ∼30 mg of protein/g of dry carrier (∼20% yield), independent of the scaffold used. Their specific activities were 0.50 U/mg (Z basic2 -CGT) and 0.19 U/mg (Z basic2 -SuSy), corresponding to an efficacy of 37 and 18%, respectively, compared to the soluble enzymes. The glycosyltransferases were coimmobilized and shown to be active in a cascade reaction to give the natural C-glycoside nothofagin from phloretin (1.0 mM; ∼95% conversion). All enzyme bound scaffolds showed reusability of a maximum of 5 consecutive reactions. These results suggest that the 3D printed and cross-linked NFC/CMC-based scaffolds could present a class of solid carriers for enzyme (co)-immobilization, with promising applications in glycosyltransferase-catalyzed synthesis and other fields of biocatalysis.

show abstract

Section: Resultssupporting

confidence: 93%

Section: Methodsmentioning

confidence: 99%

Section: Scaffold Preparation and Glycosyltransferasesmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 3 more Smart Citations

3D Printed Porous Nanocellulose-Based Scaffolds As Carriers for Immobilization of Glycosyltransferases

Lackner

Liu

Štiglic

et al. 2022

ACS Appl. Bio Mater.

Self Cite

View full text Add to dashboard Cite

show abstract

3D‐Printed Anisotropic Nanofiber Composites with Gradual Mechanical Properties

Lackner

Knechtl

Novak

et al. 2023

Adv Materials Technologies

Self Cite

View full text Add to dashboard Cite

3D printing of bio‐based nanomaterials into complex structures with design flexibility, structural anisotropy, and long‐term stability is a key issue for biomedical applications. Herein, 3D‐printed and ionically crosslinked structures with anisotropic, water‐proof, and tunable mechanical properties are fabricated using a polysaccharide ink composed of nanocellulose, alginate, and CaCO3 nanoparticles. The excellent shear thinning properties of the ink, combined with double or even triple extrusion, allow printing of complex structures (tubes, buckets, ears, and boat models) with high shape fidelity even after crosslinking. The anisotropically printed and crosslinked structures can be mechanically tuned by controlling the fiber orientation via the printing path, the amount of crosslinker, the type of acid used for crosslinking (weak to strong), and the storage medium. This allows for tailored flexibility and a tensile modulus of the materials in wet state ranging from 1 to 30 MPa. Application of hydrostatic pressure of 160–600 mmHg for 24 h with a physiological fluid to a tubular structure, a model for the cardiovascular system, shows no leakage or rupture in the tube. The great design freedom offered by 3D printing and spatially controlled structural anisotropy enable the production of tailored materials for soft robotics or biomedical applications.

show abstract

Direct ink writing of multifunctional nanocellulose and allyl-modified gelatin biomaterial inks for the fabrication of mechanically and functionally graded constructs

Cianciosi

Simon

Bartolf‐Kopp

et al. 2023

Carbohydrate Polymers

View full text Add to dashboard Cite

Organic acid cross-linked 3D printed cellulose nanocomposite bioscaffolds with controlled porosity, mechanical strength, and biocompatibility

Cited by 17 publications

References 60 publications

3D Printed Porous Nanocellulose-Based Scaffolds As Carriers for Immobilization of Glycosyltransferases

3D Printed Porous Nanocellulose-Based Scaffolds As Carriers for Immobilization of Glycosyltransferases

3D‐Printed Anisotropic Nanofiber Composites with Gradual Mechanical Properties

Direct ink writing of multifunctional nanocellulose and allyl-modified gelatin biomaterial inks for the fabrication of mechanically and functionally graded constructs

Contact Info

Product

Resources

About