skip to main content


Title: Micromechanical Properties of Microstructured Elastomeric Hydrogels
Abstract

Local, micromechanical environment is known to influence cellular function in heterogeneous hydrogels, and knowledge gained in micromechanics will facilitate the improved design of biomaterials for tissue regeneration. In this study, a system comprising microstructured resilin‐like polypeptide (RLP)–poly(ethylene glycol) (PEG) hydrogels is utilized. The micromechanical properties of RLP‐PEG hydrogels are evaluated with oscillatory shear rheometry, compression dynamic mechanic analysis, small‐strain microindentation, and large‐strain indentation and puncture over a range of different deformation length scales. The measured elastic moduli are consistent with volume averaging models, indicating that volume fraction, not domain size, plays a dominant role in determining the low strain mechanical response. Large‐strain indentation under a confocal microscope enables the visualization of the microstructured hydrogel micromechanical deformation, emphasizing the translation, rotation, and deformation of RLP‐rich domains. The fracture initiation energy results demonstrate that failure of the composite hydrogels is controlled by the RLP‐rich phase, and their independence with domain size suggested that failure initiation is controlled by multiple domains within the strained volume. This approach and findings provide new quantitative insight into the micromechanical response of soft hydrogel composites and highlight the opportunities in employing these methods to understand the physical origins of mechanical properties of soft synthetic and biological materials.

 
more » « less
NSF-PAR ID:
10458045
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
Macromolecular Bioscience
Volume:
20
Issue:
5
ISSN:
1616-5187
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract

    A rapid and facile approach to predictably control integration between two materials with divergent properties is introduced. Programmed integration between photopolymerizable soft and stiff hydrogels is investigated due to their promise in applications such as tissue engineering where heterogeneous properties are often desired. The spatial control afforded by grayscale 3D printing is leveraged to define regions at the interface that permit diffusive transport of a second material in‐filled into the 3D printed part. The printing parameters (i.e., effective exposure dose) for the resin are correlated directly to mesh size to achieve controlled diffusion. Applying this information to grayscale exposures leads to a range of distances over which integration is achieved with high fidelity. A prescribed finite distance of integration between soft and stiff hydrogels leads to a 33% increase in strain to failure under tensile testing and eliminates failure at the interface. The feasibility of this approach is demonstrated in a layer‐by‐layer 3D printed part fabricated by stereolithography, which is subsequently infilled with a soft hydrogel containing osteoblastic cells. In summary, this approach holds promise for applications where integration of multiple materials and living cells is needed by allowing precise control over integration and reducing mechanical failure at contrasting material interfaces.

     
    more » « less
  2. Abstract

    3D bioprinting is a promising technology to fabricate custom geometries for tissue engineering. However, most bioprintable hydrogels are weak and fragile, difficult to handle, and cannot mimic the mechanical behaviors of the native soft elastic tissues. A visible light crosslinked, single‐network, elastic, and biocompatible hydrogel system based on an acrylate triblock copolymer of poly(ethylene glycol) PEG and polycaprolactone (PCL) (PEG‐PCL‐DA) is developed. To enable its application in the bioprinting of soft tissues, the hydrogel system is modified on its printability and biodegradability. Furthermore, it is hypothesized that this elastic material can better transmit pulsatile forces to cells, leading to enhanced cellular response under mechanical stimulation. This central hypothesis is tested using vascular conduits with smooth muscle cells (SMCs) cultured under pulsatile forces in a custom‐made bioreactor. The results show that vascular conduits made of PEG‐PCL‐DA hydrogel faithfully recapitulate the rapid stretch and recoil under the pulsatile pressure from 1 to 3 Hz frequency, which induces a contractile SMC phenotype, consistently upregulating the core contractile transcription factors. In summary, this work demonstrates the potential of elastic hydrogel for 3D bioprinting of soft tissues by fine‐tuning the printability, and biodegradability, while possessing robust elastic properties suitable for manual handling and biomechanical stimulation.

     
    more » « less
  3. Abstract

    The core of this research is separated into three domains, the ultrahigh strain rate response of elastomeric polymers, laser‐induced shock waves , and terahertz time‐domain spectroscopy (THz‐TDS). Elastomers, e.g., polyurea, constitute an advance class of materials suitable for many applications, specifically in high impact loading scenarios, thus, a laser‐induced shock wave (LSW) experimental technique is used to investigate the mechanical response of shock‐loaded polyurea. LSW can submit samples to a strain rate exceeding 106s−1at low strains, enabling determination of material intrinsic failure modes. The large deformation induced during shock loading may alter the macromolecule structure, which can only be detected spectroscopically. Therefore, this research incorporated terahertz bulk spectroscopy to detect and report molecular conformational changes. Microscopy techniques were also used to elucidate changes in the microscale properties, morphology, and topography. The interpretation of the results explicated brittle failure in terms of partial and total spallation and, remarkably, ductile failure leading to plastic deformation, including plastic bulging and adiabatic shearing, not previously associated with LSW technique. Furthermore, spectral changes found in the terahertz regime substantiated the validity of terahertz spectroscopy in elucidating the underlying mechanism associated with the impact mitigating properties of dynamically loaded polyurea.

     
    more » « less
  4. Abstract

    We introduce laser cavitation rheology (LCR) as a minimally-invasive optical method to characterize mechanical properties within the interior of biological and synthetic aqueous soft materials at high strain-rates. We utilized time-resolved photography to measure cavitation bubble dynamics generated by the delivery of focused 500 ps duration laser radiation at λ = 532 nm within fibrin hydrogels at pulse energies ofEp = 12, 18 µJ and within polyethylene glycol (600) diacrylate (PEG (600) DA) hydrogels atEp = 2, 5, 12 µJ. Elastic moduli and failure strains of fibrin and PEG (600) DA hydrogels were calculated from these measurements by determining parameter values which provide the best fit of the measured data to a theoretical model of cavitation bubble dynamics in a Neo-Hookean viscoelastic medium subject to material failure. We demonstrate the use of this method to retrieve the local, interior elastic modulus of these hydrogels and both the radial and circumferential failure strains.

     
    more » « less
  5. Hydrogels are a class of soft, highly deformable materials formed by swelling a network of polymer chains in water. With mechanical properties that mimic biological materials, hydrogels are often proposed for load bearing biomedical or other applications in which their deformation and failure properties will be important. To study the failure of such materials a means for the measurement of deformation fields beyond simple uniaxial tension tests is required. As a non-contact, full-field deformation measurement method, Digital Image Correlation (DIC) is a good candidate for such studies. The application of DIC to hydrogels is studied here with the goal of establishing the accuracy of DIC when applied to hydrogels in the presence of large strains and large strain gradients. Experimental details such as how to form a durable speckle pattern on a material that is 90% water are discussed. DIC is used to measure the strain field in tension loaded samples containing a central hole, a circular edge notch and a sharp crack. Using a nonlinear, large deformation constitutive model, these experiments are modeled using the finite element method (FEM). Excellent agreement between FEM and DIC results for all three geometries shows that the DIC measurements are accurate up to strains of over 10, even in the presence of very high strain gradients near a crack tip. The method is then applied to verify a theoretical prediction that the deformation field in a cracked sample under relaxation loading, i.e. constant applied boundary displacement, is stationary in time even as the stress relaxes by a factor of three. 
    more » « less