Structuring supramolecular hyaluronan hydrogels via peptide self-assembly for modulating the cell microenvironment

Yuan, Yichen; Shi, Yonghui; Banerjee, Jayati; Sadeghpour, Amin; Azevedo, Helena S.

doi:10.1016/j.mtbio.2023.100598

Cited by 4 publications

(6 citation statements)

References 58 publications

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“…63 Azevedo et al used positively charged, amphipathic peptides for the supramolecular cross-linking of native hyaluronan and could regulate the structural and mechanical properties of the resulting hybrid hydrogels through the peptide sequence employed. 64 Overall, such hybrid gels offer great potential to combine different properties (i.e., one labile and one slow degrading gel) within a single material. 65 To introduce structural organization in biomaterials, elastinlike proteins (ELPs), short repetitive sequences which provide elasticity and mechanical stability, can be used and have been well studied by the Heilshorn lab.…”

Section: ■ Simplicity Enables Complexity; a Supramolecular Approachmentioning

confidence: 99%

Using Chemistry To Recreate the Complexity of the Extracellular Matrix: Guidelines for Supramolecular Hydrogel–Cell Interactions

Rijns,

Baker,

Dankers

2024

J. Am. Chem. Soc.

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Hydrogels have emerged as a promising class of extracellular matrix (ECM)-mimicking materials in regenerative medicine. Here, we briefly describe current state-of-the-art of ECM-mimicking hydrogels, ranging from natural to hybrid to completely synthetic versions, giving the prelude to the importance of supramolecular interactions to make true ECM mimics. The potential of supramolecular interactions to create ECM mimics for cell culture is illustrated through a focus on two different supramolecular hydrogel systems, both developed in our laboratories. We use some recent, significant findings to present important design principles underlying the cell−material interaction. To achieve cell spreading, we propose that slow molecular dynamics (monomer exchange within fibers) is crucial to ensure the robust incorporation of cell adhesion ligands within supramolecular fibers. Slow bulk dynamics (stress−relaxation�fiber rearrangements, τ 1/2 ≈ 1000 s) is required to achieve cell spreading in soft gels (<1 kPa), while gel stiffness overrules dynamics in stiffer gels. Importantly, this resonates with the findings of others which specialize in different material types: cell spreading is impaired in case substrate relaxation occurs faster than clutch binding and focal adhesion lifetime. We conclude with discussing considerations and limitations of the supramolecular approach as well as provide a forward thinking perspective to further understand supramolecular hydrogel−cell interactions. Future work may utilize the presented guidelines underlying cell−material interactions to not only arrive at the next generation of ECM-mimicking hydrogels but also advance other fields, such as bioelectronics, opening up new opportunities for innovative applications.

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Section: ■ Simplicity Enables Complexity; a Supramolecular Approachmentioning

confidence: 99%

Using Chemistry To Recreate the Complexity of the Extracellular Matrix: Guidelines for Supramolecular Hydrogel–Cell Interactions

Rijns,

Baker,

Dankers

2024

J. Am. Chem. Soc.

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“…More recently, the supramolecular crosslinking of native HA with amphipathic cationic peptides into hydrogels with different structural organizations was first reported by Azevedo and coworkers. [ 91 ] The self‐assembly propensity of the peptides into β‐sheet structures was shown to regulate their interaction with HA chains and their subsequent diffusion within the highly viscous HA solution. The obtained gels provide a biomimetic environment for cells, composed of an ECM polymer and nanofibrous peptides, and were able to support the formation and cultivation of human mesenchymal stem cell (hMSC) spheroids.…”

Section: Ha Hydrogels: Types and Fabrication Approachesmentioning

confidence: 99%

Bioengineered Hyaluronan Hydrogels for the Delivery of Molecular and Cellular Therapies

Silva,

Azevedo

2023

Advanced Therapeutics

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Hyaluronan (HA) is an extracellular matrix (ECM)‐based polymer with unique physicochemical properties including biocompatibility, biodegradability, viscoelasticity, and high‐water retention. However, its solubility in water drastically reduces its half‐life in vivo. Through judicious chemical modifications, its structure is easily crosslinked and can conjugate with numerous therapeutic molecules, extending their therapeutic function. Throughout this review, an overview of crosslinking methods to create HA hydrogels is provided, including covalent (permanent, transient/dynamic) and noncovalent chemistries, as well as the use of nonmodified HA in supramolecular hydrogels. HA‐based injectable hydrogels are very appealing as a three‐dimensional network for the delivery of therapeutic molecules (drugs and biomolecules) and stem cells. HA hydrogels are capable of mimicking important features of the native ECM and can provide spatiotemporal signals to regulate cell fate. The final part of the review also describes the application of HA hydrogels as vehicles for delivering stem cells and therapeutics, capable of modulating cell behavior.

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“…However, the effect of these synthetic terminal groups should be carefully considered when applied in biological fields, particularly in vivo [ [34] , [35] , [36] , [37] ]. Furthermore, minor alterations in peptide sequences could significantly influence the assembly process [ 38 ], making it challenging to predict gel formation and develop hydrogels with desired properties [ 34 ]. Most importantly, the rapid degradation of L-peptide hydrogels poses an obstacle to their applications in tissue engineering and regenerative medicine [ 39 ].…”

Section: Introductionmentioning

confidence: 99%

Biostable hydrogels consisting of hybrid β-sheet fibrils assembled by a pair of enantiomeric peptides

Tan,

Hou,

Shi

et al. 2024

Materials Today Bio

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Structuring supramolecular hyaluronan hydrogels via peptide self-assembly for modulating the cell microenvironment

Cited by 4 publications

References 58 publications

Using Chemistry To Recreate the Complexity of the Extracellular Matrix: Guidelines for Supramolecular Hydrogel–Cell Interactions

Using Chemistry To Recreate the Complexity of the Extracellular Matrix: Guidelines for Supramolecular Hydrogel–Cell Interactions

Bioengineered Hyaluronan Hydrogels for the Delivery of Molecular and Cellular Therapies

Biostable hydrogels consisting of hybrid β-sheet fibrils assembled by a pair of enantiomeric peptides

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