Virus-like particles as crosslinkers in fibrous biomimetic hydrogels: approaches towards capsid rupture and gel repair

Schoenmakers, Daniël C.; Schoonen, Lise; Rutten, Mcm Marcel; Nolte, Roeland J. M.; Rowan, Alan E.; Hest, Jan C. M. van; Kouwer, Paul H. J.

doi:10.1039/c7sm02320k

“…The only difference is a reduced slope/stiffening index (Table 1), which becomes more and more apparent with increasing pre-stress. A similar reduction in slope was observed for PIC networks crosslinked with virus capsids (Schoenmakers et al, 2018b). We conclude that the difference in stiffening index for PIC-A4B4 and PIC-0 originates from the rupture of CC crosslinks, while the overall stressstiffening response of the hydrogel is determined by the hydrophobically bundled PIC network.…”

Section: Network Topology Effects On Hydrogelssupporting

confidence: 73%

“…This increase in G' is unexpected and has further not been observed for any other crosslinked PIC network (Deshpande et al, 2016;Deshpande et al, 2017;Schoenmakers et al, 2018a;Schoenmakers et al, 2018b). As the L p of individual PIC polymers decreases with lowering the temperature, a decrease in G' is expected for bundled PIC networks as long as the network structure is not altered (Kouwer et al, 2013).…”

Section: Network Topologymentioning

confidence: 88%

“…To fully utilize the potential of PIC hydrogels as cytoskeleton and ECM mimics, several types of crosslinks have previously been introduced into PIC networks. These include short double-stranded DNA oligonucleotides (Deshpande et al, 2016) and stimuli-responsive DNA motifs (Deshpande et al, 2017) as well as self-assembled virus capsids (Schoenmakers et al, 2018b) and covalent triazole crosslinks (Schoenmakers et al, 2018a). In the majority of these studies, the focus was placed on understanding the effect of these crosslinks on the non-linear stress-stiffening response.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Grad¹,

Tunn²,

Voerman³

et al. 2020

Preprint

View full text Add to dashboard Cite

Biological materials combine stress relaxation and self-healing with non-linear stress-strain responses. These characteristic features are a direct result of hierarchical self-assembly, which often results in fiber-like architectures. Even though structural knowledge is rapidly increasing, it has remained a challenge to establish relationships between microscopic and macroscopic structure and function. Here, we focus on understanding how network topology determines the viscoelastic properties, i.e. stress relaxation, of biomimetic hydrogels. We have dynamically crosslinked two different synthetic polymers with one and the same crosslink. The first polymer, a polyisocyanopeptide (PIC), self-assembles into semi-flexible, fiber-like bundles and thus displays stress-stiffening, similar to many biopolymer networks. The second polymer, 4-arm poly(ethylene glycol) (starPEG), serves as a reference network with well-characterized structural and viscoelastic properties. Using one and the same coiled coil crosslink allows us to decouple the effects of crosslink kinetics and network topology on the stress relaxation behavior of the resulting hydrogel networks. We show that the fiber-containing PIC network displays a relaxation time approximately two orders of magnitude slower than the starPEG network. This reveals that crosslink kinetics is not the only determinant for stress relaxation. Instead, we propose that the different network topologies determine the ability of elastically active network chains to relax stress. In the starPEG network, each elastically active chain contains exactly one crosslink. In the absence of entanglements, crosslink dissociation thus relaxes the entire chain. In contrast, each polymer is crosslinked to the fiber bundle in multiple positions in the PIC hydrogel. The dissociation of a single crosslink is thus not sufficient for chain relaxation. This suggests that tuning the number of crosslinks per elastically active chain in combination with crosslink kinetics is a powerful design principle for tuning stress relaxation in polymeric materials. The presence of a higher number of crosslinks per elastically active chain thus yields materials with a slow macroscopic relaxation time but fast dynamics at the microscopic level. Using this principle for the design of synthetic cell culture matrices will yield materials with excellent long-term stability combined with the ability to locally reorganize, thus facilitating cell motility, spreading and growth.

show abstract

“…This increase in G' is unexpected and has further not been observed for any other crosslinked PIC network (Deshpande et al, 2016;Deshpande et al, 2017;Schoenmakers et al, 2018a;Schoenmakers et al, 2018b). As the L p of individual PIC polymers decreases with lowering the temperature, a decrease in G' is expected for bundled PIC networks as long as the network structure is not altered (Kouwer et al, 2013).…”

Section: Bundle Formation and Network Topology Of Coiled Coil-crosslimentioning

confidence: 61%

“…To fully utilize the potential of PIC hydrogels as cytoskeleton and ECM mimics, several types of crosslinks have previously been introduced into PIC networks. These include short double-stranded DNA oligonucleotides (Deshpande et al, 2016) and stimuli-responsive DNA motifs (Deshpande et al, 2017) as well as self-assembled virus capsids (Schoenmakers et al, 2018b) and covalent triazole crosslinks (Schoenmakers et al, 2018a). In the majority of these studies, the focus was placed on understanding the effect of these crosslinks on the non-linear stress-stiffening response.…”

Section: Introductionmentioning

confidence: 99%

Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Grad¹,

Tunn²,

Voerman³

et al. 2020

Preprint

0

View full text Add to dashboard Cite

Biological materials combine stress relaxation and self-healing with non-linear stress-strain responses. These characteristic features are a direct result of hierarchical self-assembly, which often results in fiber-like architectures. Even though structural knowledge is rapidly increasing, it has remained a challenge to establish relationships between microscopic and macroscopic structure and function. Here, we focus on understanding how network topology determines the viscoelastic properties, i.e. stress relaxation, of biomimetic hydrogels. We have dynamically crosslinked two different synthetic polymers with one and the same crosslink. The first polymer, a polyisocyanopeptide (PIC), self-assembles into semi-flexible, fiber-like bundles and thus displays stress-stiffening, similar to many biopolymer networks. The second polymer, 4-arm poly(ethylene glycol) (starPEG), serves as a reference network with well-characterized structural and viscoelastic properties. Using one and the same coiled coil crosslink allows us to decouple the effects of crosslink kinetics and network topology on the stress relaxation behavior of the resulting hydrogel networks. We show that the fiber-containing PIC network displays a relaxation time approximately two orders of magnitude slower than the starPEG network. This reveals that crosslink kinetics is not the only determinant for stress relaxation. Instead, we propose that the different network topologies determine the ability of elastically active network chains to relax stress. In the starPEG network, each elastically active chain contains exactly one crosslink. In the absence of entanglements, crosslink dissociation thus relaxes the entire chain. In contrast, each polymer is crosslinked to the fiber bundle in multiple positions in the PIC hydrogel. The dissociation of a single crosslink is thus not sufficient for chain relaxation. This suggests that tuning the number of crosslinks per elastically active chain in combination with crosslink kinetics is a powerful design principle for tuning stress relaxation in polymeric materials. The presence of a higher number of crosslinks per elastically active chain thus yields materials with a slow macroscopic relaxation time but fast dynamics at the microscopic level. Using this principle for the design of synthetic cell culture matrices will yield materials with excellent long-term stability combined with the ability to locally reorganize, thus facilitating cell motility, spreading and growth.

show abstract

Stimuli‐Responsive Nanocomposite Hydrogels for Biomedical Applications

Lavrador

¹

,

Esteves

²

,

Gaspar

³

et al. 2020

Adv Funct Materials

View full text Add to dashboard Cite

The complex tissue‐specific physiology that is orchestrated from the nano‐ to the macroscale, in conjugation with the dynamic biophysical/biochemical stimuli underlying biological processes, has inspired the design of sophisticated hydrogels and nanoparticle systems exhibiting stimuli‐responsive features. Recently, hydrogels and nanoparticles have been combined in advanced nanocomposite hybrid platforms expanding their range of biomedical applications. The ease and flexibility of attaining modular nanocomposite hydrogel constructs by selecting different classes of nanomaterials/hydrogels, or tuning nanoparticle‐hydrogel physicochemical interactions widely expands the range of attainable properties to levels beyond those of traditional platforms. This review showcases the intrinsic ability of hybrid constructs to react to external or internal/physiological stimuli in the scope of developing sophisticated and intelligent systems with application‐oriented features. Moreover, nanoparticle‐hydrogel platforms are overviewed in the context of encoding stimuli‐responsive cascades that recapitulate signaling interplays present in native biosystems. Collectively, recent breakthroughs in the design of stimuli‐responsive nanocomposite hydrogels improve their potential for operating as advanced systems in different biomedical applications that benefit from tailored single or multi‐responsiveness.

show abstract

Virus-like particles as crosslinkers in fibrous biomimetic hydrogels: approaches towards capsid rupture and gel repair

Cited by 11 publications

References 51 publications

Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels

Stimuli‐Responsive Nanocomposite Hydrogels for Biomedical Applications

Contact Info

Product

Resources

About