The effect of hydration on molecular chain mobility and the viscoelastic behavior of resilin-mimetic protein-based hydrogels

Truong, My Y.; Dutta, Naba K.; Choudhury, Namita Roy; Kim, Misook; Elvin, Christopher M.; Nairn, Kate M.; Hill, Anita J.

doi:10.1016/j.biomaterials.2011.07.064

Cited by 69 publications

(108 citation statements)

References 60 publications

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“…These differences are suggested to arise from the intrinsic disparities in the properties of the polymer chains of these two systems, given that the crosslinking densities and chemistries are similar between the PEG control and the RLP hydrogels. Among the RLP hydrogels, a slight increase in stress relaxation is observed with an increase in RLP concentration, suggesting that the higher-concentration samples are less elastomeric, consistent with the reported importance of hydration in the elastomeric behavior of RLPs (Gosline et al, 2002; Truong et al, 2011). …”

Section: Resultssupporting

confidence: 80%

“…The hydrated RLP hydrogels exhibited improved elastomeric properties over those for the hydrogels formed in situ in the oscillatory rheology experiments; this is probably due to the fact that water behaves as a lubricant for the RLP polymer networks by enhancing the exchange of hydrogen bonds and reducing charge interactions between polar amino acid side chains thus increasing chain flexibility. These dynamic features of the polypeptide chain promote conformational changes that further dissipate the energy input, lowering the stiffness and providing a higher resistance to fracture (Gosline et al, 2002; Nairn et al, 2008; Woody, 2009; Kappiyoor et al, 2011; Truong et al, 2011). Taken together, the outstanding elastomeric mechanical properties of the RLP hydrogels, under various loading conditions, recommend the potential use of RLP-based hydrogels for vocal fold tissue regeneration applications.…”

Section: Resultsmentioning

confidence: 99%

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Transient dynamic mechanical properties of resilin-based elastomeric hydrogels

Kiick

2014

Front. Chem.

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The outstanding high-frequency properties of emerging resilin-like polypeptides (RLPs) have motivated their development for vocal fold tissue regeneration and other applications. Recombinant RLP hydrogels show efficient gelation, tunable mechanical properties, and display excellent extensibility, but little has been reported about their transient mechanical properties. In this manuscript, we describe the transient mechanical behavior of new RLP hydrogels investigated via both sinusoidal oscillatory shear deformation and uniaxial tensile testing. Oscillatory stress relaxation and creep experiments confirm that RLP-based hydrogels display significantly reduced stress relaxation and improved strain recovery compared to PEG-based control hydrogels. Uniaxial tensile testing confirms the negligible hysteresis, reversible elasticity and superior resilience (up to 98%) of hydrated RLP hydrogels, with Young's modulus values that compare favorably with those previously reported for resilin and that mimic the tensile properties of the vocal fold ligament at low strain (<15%). These studies expand our understanding of the properties of these RLP materials under a variety of conditions, and confirm the unique applicability, for mechanically demanding tissue engineering applications, of a range of RLP hydrogels.

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Section: Resultssupporting

confidence: 80%

Section: Resultsmentioning

confidence: 99%

Transient dynamic mechanical properties of resilin-based elastomeric hydrogels

Kiick

2014

Front. Chem.

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“…However, some differences in the viscoelastic properties of F0, F12 and F18 were observed. Swelling of the material by water sorption during thermal cycling is considered to affect the viscoelastic properties 36) . The water sorption for F0 was larger than that for the other materials, which suggests that the viscoelastic deformation of F0 could be affected by the thermal cycling process.…”

Section: Discussionmentioning

confidence: 99%

Influence of monomer content on the viscoelasticity, water sorption and solubility of experimental fluorinated soft lining materials

et al. 2015

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The influence of monomer content on the viscoelasticity, water sorption and solubility of experimental fluorinated soft lining materials was investigated. Changes in the viscoelastic properties of the materials were also examined after thermal cycling. Four fluorinated soft lining materials containing different amounts of methoxy diethylene glycol methacrylate (MDGMA) and tridecafluorooctyl methacrylate (13FMA) were prepared. The viscoelastic displacement for specimens containing 13FMA was found to be less than that without 13FMA (p<0.05), and the values tended to decrease with increasing 13FMA content. Reduction of the MDGMA content and addition of 13FMA caused a decrease of water sorption and solubility (p<0.05). Thermal cycling was found to affect the viscoelastic deformation of the specimens without 13FMA and those specimens with relatively large amounts of 13FMA.

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“…This observation indicates that hydration is vital for the native mechanical function of glow-worm silk, as is the case for flagelliform silk (Bonthrone et al, 1992;Guinea et al, 2010) as well as other silks and non-silk elastomeric proteins (Porter and Vollrath, 2009;Truong et al, 2011). The functional importance of hydration is reflected by other experimental results obtained in this study, including: a) the relative abundance of hydrophilic residues in the silk compared to previously described silk fibres (Table 1); b) the low crystalline fraction of glow-worm silk inferred by comparison of X-ray scattering patterns and amino acid analysis; c) the presence of protease inhibitors in silk (Table 2) which may protect silk proteins with high solvent accessibility from degradation by environmental proteases; and d) the ability for freshly harvested silk, but not dried silk, to be solubilised in 1% SDS (Section 3.3).…”

Section: The Importance Of Hydrationmentioning

confidence: 99%

The other prey-capture silk: Fibres made by glow-worms (Diptera: Keroplatidae) comprise cross-β-sheet crystallites in an abundant amorphous fraction

Walker

Weisman

Trueman

et al. 2015

Comparative Biochemistry and Physiology Part B: Biochemistry an

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The other prey-capture silk: Fibres made by glow-worms (Diptera: Keroplatidae) comprise cross-β-sheet crystallites in an abundant amorphous fraction, Comparative Biochemistry and Physiology, Part B (2015), doi: 10.1016/j.cbpb.2015 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. Keywords: silk; Arachnocampa; glow-worm; cross-β-sheet; flagelliform; extensibility; disordered A C C E P T E D M A N U S C R I P T ACCEPTED MANUSCRIPT AbstractGlow-worms (larvae of dipteran genus Arachnocampa) are restricted to moist habitats where they capture flying prey using snares composed of highly extensible silk fibres and sticky mucus droplets.Little is known about the composition or structure of glow-worm snares, or the extent of possible convergence between glow-worm and arachnid capture silks. We characterised Arachnocampa richardsae silk and mucus using X-ray scattering, Fourier transform infrared spectroscopy and amino acid analysis. Silk but not mucus contained crystallites of the cross-β-sheet type, which occur in unrelated insect silks but have not been reported previously in fibres used for prey capture. Mucus proteins were rich in Gly (28.5%) and existed in predominantly a random coil structure, typical of many adhesive proteins. In contrast, the silk fibres were unusually rich in charged and polar residues, particularly Lys (18.1%), which we propose is related to their use in a highly hydrated state.Comparison of X-ray scattering, infrared spectroscopy and amino acid analysis data suggests that silk fibres contain a high fraction of disordered protein. We suggest that in the native hydrated state, silk fibres are capable of extension via deformation of both disordered regions and cross-β-sheet crystallites, and that high extensibility is an adaptation promoting successful prey capture. This study illustrates the rich variety of protein motifs that are available for recruitment into biopolymers, and how convergently evolved materials can nevertheless be based on fundamentally different protein structures.

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The effect of hydration on molecular chain mobility and the viscoelastic behavior of resilin-mimetic protein-based hydrogels

Cited by 69 publications

References 60 publications

Transient dynamic mechanical properties of resilin-based elastomeric hydrogels

Transient dynamic mechanical properties of resilin-based elastomeric hydrogels

Influence of monomer content on the viscoelasticity, water sorption and solubility of experimental fluorinated soft lining materials

The other prey-capture silk: Fibres made by glow-worms (Diptera: Keroplatidae) comprise cross-β-sheet crystallites in an abundant amorphous fraction

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