Multivalent dendrimers presenting spatially controlled clusters of binding epitopes in thermoresponsive hyaluronan hydrogels

Seelbach, Ryan J.; Fransen, Peter; Peroglio, Marianna; Pulido, Daniel; López‐Chicón, Patrícia; Duttenhoefer, Fabian; Sauerbier, Sebastian; Freiman, Thomas M.; Niemeyer, Philipp; Semino, Carlos E.; Alberício, Fernando; Alini, Mauro; Royo, Míriam; Mata, Álvaro; Eglin, David

doi:10.1016/j.actbio.2014.06.028

Cited by 21 publications

(28 citation statements)

References 37 publications

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“…2–5 Natural systems routinely use the coiled-coil motif to modulate ligand–receptor interactions. 6,7 The ability to control ligand presentation on surfaces, for example, density, multivalency, and interligand distance, represent new opportunities for functional control and have great potential to meet demands for tissue engineering, 8–10 regenerative medicine, 11,12 and drug delivery. 13–15 …”

Section: Introductionmentioning

confidence: 99%

Understanding Peptide Oligomeric State in Langmuir Monolayers of Amphiphilic 3-Helix Bundle-Forming Peptide-PEG Conjugates

Lund

Ang²,

Shu³

et al. 2016

Biomacromolecules

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Coiled-coil peptide–polymer conjugates are an emerging class of biomaterials. Fundamental understanding of the coiled-coil oligomeric state and assembly process of these hybrid building blocks is necessary to exert control over their assembly into well-defined structures. Here, we studied the effect of peptide structure and PEGylation on the self-assembly process and oligomeric state of a Langmuir monolayer of amphiphilic coiled-coil peptide–polymer conjugates using X-ray reflectivity (XR) and grazing-incidence X-ray diffraction (GIXD). Our results show that the oligomeric state of PEGylated amphiphiles based on 3-helix bundle-forming peptide is surface pressure dependent, a mixture of dimers and trimers was formed at intermediate surface pressure but transitions into trimers completely upon increasing surface pressure. Moreover, the interhelical distance within the coiled-coil bundle of 3-helix peptide-PEG conjugate amphiphiles was not perturbed under high surface pressure. Present studies provide valuable insights into the self-assembly process of hybrid peptide–polymer conjugates and guidance to develop biomaterials with controlled multivalency of ligand presentation.

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Section: Introductionmentioning

confidence: 99%

Understanding Peptide Oligomeric State in Langmuir Monolayers of Amphiphilic 3-Helix Bundle-Forming Peptide-PEG Conjugates

Lund

Ang²,

Shu³

et al. 2016

Biomacromolecules

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show abstract

“…152, 178 When thiol is used in a stoichiometric excess to acrylate, the fast Michael addition reaction contributes to the initial network formation and the slow disulfide bond formation gradually increases gel stiffness. 179, 180 Depending on the molecular weight of HA and PEG, percent functional group incorporation in HA, concentrations of HA and PEG and thiol/acrylate ratio, hydrogels with elastic modulus varying from 11 Pa to 3500 Pa have been prepared. 181 Co-crosslinking thiolated HA with other thiolated biomacromolecules (heparin or gelatin) creates a more complex network containing immobilized biological cues for growth factor sequestration or for integrin engagement.…”

Section: Modular Synthesis Of Hybrid Hydrogel Networkmentioning

confidence: 99%

Modular and orthogonal synthesis of hybrid polymers and networks

2015

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Biomaterials scientists strive to develop polymeric materials with distinct chemical make-up, complex molecular architectures, robust mechanical properties and defined biological functions by drawing inspirations from biological systems. Salient features of biological designs include (1) repetitive presentation of basic motifs; and (2) efficient integration of diverse building blocks. Thus, an appealing approach to biomaterials synthesis is to combine synthetic and natural building blocks in a modular fashion employing novel chemical methods. Over the past decade, orthogonal chemistries have become powerful enabling tools for the modular synthesis of advanced biomaterials. These reactions require building blocks with complementary functionalities, occur under mild conditions in the presence of biological molecules and living cells and proceed with high yield and exceptional selectivity. These chemistries have facilitated the construction of complex polymers and networks in a step-growth fashion, allowing facile modulation of materials properties by simple variations of the building blocks. In this review, we first summarize features of several types of orthogonal chemistries. We then discuss recent progress in the synthesis of step growth linear polymers, dendrimers and networks that find application in drug delivery, 3D cell culture and tissue engineering. Overall, orthogonal reactions and modulular synthesis have not only minimized the steps needed for the desired chemical transformations but also maximized the diversity and functionality of the final products. The modular nature of the design, combined with the potential synergistic effect of the hybrid system, will likely result in novel hydrogel matrices with robust structures and defined functions.

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“…[40][41][42] For example, an injectable composite hydrogel was formed through cross-linking of HA and dendritic structures bearing integrin peptides to improve biofunctionality of thermo-responsive HA hydrogels. [43] In our research, we report that when PAMAM dendrimers bearing multiple vinyl sulfone groups mix with thiolated HA, an in situ fast cross-linking hydrogel is formed in aqueous conditions within 30 s under experimental conditions, which is the fastest hydrogel ever reported up to date among HA and dendrimer hydrogels. Live cell staining assay of rat bone marrow stem cells (rBMSC) indicated that cells were live in the synthesized hydrogels and incorporation of RGD peptide enhanced cell attachment to hydrogel matrix.…”

Section: Introductionmentioning

confidence: 93%

Synthesis of PAMAM dendrimer-based fast cross-linking hydrogel for biofabrication

Luckanagul

Allen

et al. 2015

Journal of Biomaterials Science, Polymer Edition

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Hydrogels possess great potential in biofabrication because they allow cell encapsulation and proliferation in a highly hydrated three-dimensional environment, and they provide biologically relevant chemical and physical signals. However, development of hydrogel systems that mimic the complexity of natural extracellular matrix remains a challenge. In this study, we report the development of a binary hydrogel system containing a synthetic poly(amido amine) (PAMAM) dendrimer and a natural polymer, i.e., hyaluronic acid (HA), to form a fast cross-linking hydrogel. Live cell staining experiment and cell viability assay of bone marrow stem cells demonstrated that cells were viable and proliferating in the in situ formed PAMAM/HA hydrogel system. Furthermore, introduction of a Arginylglycylaspartic acid (RGD) peptide into the hydrogel system significantly improved the cell viability, proliferation, and attachment. Therefore, this PAMAM/HA hydrogel system could be a promising platform for various applications in biofabrication.

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Multivalent dendrimers presenting spatially controlled clusters of binding epitopes in thermoresponsive hyaluronan hydrogels

Cited by 21 publications

References 37 publications

Understanding Peptide Oligomeric State in Langmuir Monolayers of Amphiphilic 3-Helix Bundle-Forming Peptide-PEG Conjugates

Understanding Peptide Oligomeric State in Langmuir Monolayers of Amphiphilic 3-Helix Bundle-Forming Peptide-PEG Conjugates

Modular and orthogonal synthesis of hybrid polymers and networks

Synthesis of PAMAM dendrimer-based fast cross-linking hydrogel for biofabrication

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