Microgels are spherical hydrogels with physicochemical properties ideal for many biomedical applications. For example, microgels can be used as individual carriers for suspension cell culture or jammed/annealed into granular hydrogels with micron-scale pores highly permissive to molecular transport and cell proliferation/migration. Conventionally, laborious optimization processes are often needed to create microgels with different moduli, sizes, and compositions. This work presents a new microgel and granular hydrogel preparation workflow using gelatin-norbornene-carbohydrazide (GelNB-CH). As a gelatin-derived macromer, GelNB-CH presents cell adhesive and degradable motifs while being amenable to three orthogonal click chemistries, namely the thiol-norbornene photo-click reaction, hydrazone bonding, and the inverse electron demand Diels-Alder (iEDDA) click reaction. The thiol-norbornene photo-click reaction (with thiol-bearing crosslinkers) and hydrazone bonding (with aldehyde-bearing crosslinkers) were used to crosslink the microgels and to realize on-demand microgel stiffening, respectively. The tetrazine-norbornene iEDDA click reaction (with tetrazine-bearing crosslinkers) was used to anneal microgels into granular hydrogels. In addition to materials development, we demonstrated the value of the triple-click chemistry granular hydrogels culturing human mesenchymal stem cells and pancreatic cancer cells.
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http://dx.doi.org/10.1039/d3lp00249g | DOI Listing |
PLoS One
November 2024
Institute of Biological Chemistry, Biophysics and Bioengineering, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh, United Kingdom.
ACS Biomater Sci Eng
December 2024
Department of Biomedical Engineering, University of Virginia, Charlottesville, Virginia 22903, United States.
Advancing three-dimensional (3D) tissue constructs is central to creating models and engineered tissues that recapitulate biology. Materials that are permissive to cellular behaviors, including proliferation, morphogenesis of multicellular structures, and motility, will support the emergence of tissue structures. Granular hydrogels in which there is no interparticle cross-linking exhibit dynamic properties that may be permissive to such cellular behaviors.
View Article and Find Full Text PDFAdv Healthc Mater
November 2024
Translational Tissue Engineering Centre, Johns Hopkins University School of Medicine, Baltimore, MD, 21213, USA.
The interplay between biomaterials and host immune responses critically determines outcomes in tissue restoration. Recent studies suggest that physicochemical properties of materials can dictate pro-regenerative versus pro-fibrotic responses and have begun to define the key immune cell types and signals governing these divergent effects. This emerging understanding enables the engineering of regenerative biomaterials capable of functional restoration in situ.
View Article and Find Full Text PDFLangmuir
December 2024
Department of Chemical and Biological Sciences S.N. Bose National Centre for Basic Sciences Block-JD, Sector-III, Salt Lake Kolkata-700106, India.
We report an instantaneous room-temperature phase separation of 1 mM bovine serum albumin solution in the presence of (20% acetic acid+0.2 M NaCl), a routinely used food preservative; an opaque liquid-like phase (L) coexists in equilibrium with a granular gel like phase (G). Interestingly, neither 20% acetic acid nor 0.
View Article and Find Full Text PDFSmall
November 2024
Soft Materials Laboratory - Institute of Materials in École Polytechnique Fédérale de Lausanne, Lausanne, 1015, Switzerland.
Direct ink writing (DIW) enables 3D printing of macroscopic objects with well-defined structures and compositions that controllably change over length scales of order 100 µm. Unfortunately, only a limited number of materials can be processed through DIW because it imparts stringent rheological requirements on inks. This limitation can be overcome for soft materials, if they are formulated as microparticles that, if jammed, fulfill the rheological requirements to be printed.
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