Improving printability of a thermoresponsive hydrogel biomaterial ink by nanoclay addition

Hu, Chen; Hahn, Lukas; Yang, Mengshi; Altmann, Alexander; Stahlhut, Philipp; Groll, Jürgen; Luxenhofer, Robert

doi:10.1007/s10853-020-05190-5

Cited by 42 publications

(48 citation statements)

References 59 publications

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“…Poly(MeOx)‐poly(2‐ n‐ propyl‐2‐oxazine) has recently been reported as a thermoreversible gelator for 3D printing. [ 210 ] Laponite clays were used to improve the rheology of these materials to allow the printing of high‐resolution structures with good shape fidelity. The mixing of additives to modify rheology of thermoreversible gelators is underexploited outside of poloxamer 407 and is a promising way of enhancing these systems without the need for additional synthetic steps.…”

Section: Thermoreversible Gelatorsmentioning

confidence: 99%

Polymers Exhibiting Lower Critical Solution Temperatures as a Route to Thermoreversible Gelators for Healthcare

Cook

Haddow

Kirton

et al. 2020

Adv Funct Materials

131

113

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The ability to trigger changes to material properties with external stimuli, so‐called “smart” behavior, has enabled novel technologies for a wide range of healthcare applications. Response to small changes in temperature is particularly attractive, where material transformations may be triggered by contact with the human body. Thermoreversible gelators are materials where warming triggers reversible phase change from low viscosity polymer solution to a gel state. These systems can be generated by the exploitation of macromolecules with lower critical solution temperatures included in their architectures. The resultant materials are attractive for topical and mucosal drug delivery, as well as for injectables. In addition, the materials are attractive for tissue engineering and 3D printing. The fundamental science underpinning these systems is described, along with progress in each class of material and their applications. Significant opportunities exist in the fundamental understanding of how polymer chemistry and nanoscience describe the performance of these systems and guide the rational design of novel systems. Furthermore, barriers to translating technologies must be addressed, for example, rigorous toxicological evaluation is rarely conducted. As such, applications remain tied to narrow fields, and advancements will be made where the existing knowledge in these areas may be applied to novel problems of science.

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Section: Thermoreversible Gelatorsmentioning

confidence: 99%

Polymers Exhibiting Lower Critical Solution Temperatures as a Route to Thermoreversible Gelators for Healthcare

Cook

Haddow

Kirton

et al. 2020

Adv Funct Materials

131

113

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“…Previously, a diblock copolymer comprising a hydrophilic PMeOx block and a thermoresponsive PnPrOzi block (PMeOx-b-PnPrOzi = P0) has been introduced as bioink 32 of which the printability and shape fidelity could be significantly improved by addition of Laponite XLG. 33 However, utilization of the bioink for prolonged studies is hampered by dissolution in long-term cell culture. Therefore, additional chemical crosslinking after printing is necessary, for which we chose the well-known post-polymerization modification approach enabling Diels-Alder chemistry.…”

Section: Resultsmentioning

confidence: 99%

Biomechanical and Biological Performances of Diels-Alder Crosslinked Thermogelling Bioink

Hahn¹,

Beudert²,

Gutmann³

et al. 2021

Preprint

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Hydrogels are key components in bioink formulations to ensure printability and stability in biofabrication. In this study a well-known post-polymerization modification approach is introduced into thermogelling diblock copolymers, comprising poly(2-methyl-2-oxazoline) and thermoresponsive poly(2-n-propyl-2-oxazine). While the thermogelling and shear-thinning properties allow excellent printability, trigger-less cell-friendly Diels-Alder click-chemistry yields long-term shape-fidelity. The introduced platform enables easy incorporation of cell-binding moieties (RGD-peptide) for cellular interaction. The hydrogel was functionalized with RGD-peptides using thiol-maleimide chemistry and growth as well as morphology of fibroblast seeded on top of the hydrogels confirmed the cell adhesion facilitated by the peptides. Finally, bioink formulations were tested for biocompatibility by incorporating fibroblasts homogenously inside polymer solution pre-printing and exhibited good cytocompatibility after the printing process and crosslinking. The established bioink system combining a two-step approach by physical precursor gelation followed by additional chemical stabilization offers a broad versatility for further biomechanical adaptation or bioresponsive peptide modification.

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“…This led to a considerable improvement of printability of the hydrogel, as evidenced in reduced strand‐fusion and strongly enhance shape fidelity. [ 84 ] Important to note, it appears that the interaction of clay and pMeOx differs considerably from the interactions of clay and PEG, as very recently studied by Le Coeur et al. [ 85 ] The authors observed an increase of storage modulus with increasing concentration of pMeOx in pMeOx/Laponite hydrogels above certain critical concentration, while in case of PEG/Laponite, the storage modulus values reached a plateau.…”

Section: Self‐assembled Poly(2‐oxazoline)smentioning

confidence: 96%

Poly(2‐oxazoline)‐ and Poly(2‐oxazine)‐Based Self‐Assemblies, Polyplexes, and Drug Nanoformulations—An Update

Zahoranová

Luxenhofer

2021

Adv Healthcare Materials

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For many decades, poly(2‐oxazoline)s and poly(2‐oxazine)s, two closely related families of polymers, have led the life of a rather obscure research topic with only a few research groups world‐wide working with them. This has changed in the last five to ten years, presumably triggered significantly by very promising clinical trials of the first poly(2‐oxazoline)‐based drug conjugate. The huge chemical and structural toolbox poly(2‐oxazoline)s and poly(2‐oxazine)s has been extended very significantly in the last few years, but their potential still remains largely untapped. Here, specifically, the developments in macromolecular self‐assemblies and non‐covalent drug delivery systems such as polyplexes and drug nanoformulations based on poly(2‐oxazoline)s and poly(2‐oxazine)s are reviewed. This highly dynamic field benefits particularly from the extensive synthetic toolbox poly(2‐oxazoline)s and poly(2‐oxazine)s offer and also may have the largest potential for a further development. It is expected that the research dynamics will remain high in the next few years, particularly as more about the safety and therapeutic potential of poly(2‐oxazoline)s and poly(2‐oxazine)s is learned.

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Improving printability of a thermoresponsive hydrogel biomaterial ink by nanoclay addition

Cited by 42 publications

References 59 publications

Polymers Exhibiting Lower Critical Solution Temperatures as a Route to Thermoreversible Gelators for Healthcare

Polymers Exhibiting Lower Critical Solution Temperatures as a Route to Thermoreversible Gelators for Healthcare

Biomechanical and Biological Performances of Diels-Alder Crosslinked Thermogelling Bioink

Poly(2‐oxazoline)‐ and Poly(2‐oxazine)‐Based Self‐Assemblies, Polyplexes, and Drug Nanoformulations—An Update

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