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ABSTRACT: Why waste space? In the first stage of the multiphase biomineralization of collagen, silicic acid precursors (purple) infiltrated the collagen fibril (yellow) and condensed into amorphous silica to give a hierarchical composite. Amorphous calcium phosphate precursors (red) then filled the intrafibrillar spaces of the silicified collagen, where the precipitation and maturation of apatite crystallites (blue) occurred to complete the process.
Angewandte Chemie International Edition 04/2013; · 13.45 Impact Factor
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Lina Niu,
Kai Jiao,
Heonjune Ryou,
Anibal Diogenes,
Cynthia K Y Yiu,
Annalisa Mazzoni,
Ji-Hua Chen, Dwayne D Arola,
Kenneth M Hargreaves,
David H Pashley,
Franklin R Tay
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ABSTRACT: Unlike man-made composite materials, natural biominerals containing composites usually demonstrate different levels of sophisticated hierarchical structures which are responsible for their mechanical properties and other metabolic functions. However, the complex spatial organizations of the organic-inorganic phases are far beyond what they be achieved by contemporary engineering techniques. Here, we demonstrate that carbonated apatite present in collagen matrices derived from fish scale and bovine bone may be replaced by amorphous silica, using an approach that simulates what is utilized by phylogenetically ancient glass sponges. The structural hierarchy of these collagen-based biomaterials is replicated by the infiltration and condensation of fluidic polymer-stabilized silicic acid precursors within the intrafibrillar milieu of type I collagen fibrils. This facile biomimetic silicification strategy may be used for fabricating silica-based, three-dimensional functional materials with specific morphological and hierarchical requirements.
Biomacromolecules 04/2013; · 5.48 Impact Factor
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ABSTRACT: The enamel of human teeth is generally regarded as a brittle material with low fracture toughness. Consequently, the contributions of this tissue in resisting tooth fracture and the importance of its complex microstructure have been largely overlooked. In this study an experimental evaluation of the crack growth resistance of human enamel was conducted to characterize the role of rod (i.e. prism) orientation and degree of decussation on the fracture behavior of this tissue. Incremental crack growth was achieved in-plane, with the rods in directions longitudinal or transverse to their axes. Results showed that the fracture resistance of enamel is both inhomogeneous and spatially anisotropic. Cracks extending transverse to the rods in the outer enamel undergo a lower rise in toughness with extension, and achieve significantly lower fracture resistance than in the longitudinal direction. Though cracks initiating at the surface of teeth may begin extension towards the dentin-enamel junction, they are deflected by the decussated rods and continue growth about the tooth's periphery, transverse to the rods in the outer enamel. This process facilitates dissipation of fracture energy and averts cracks from extending towards the dentin and vital pulp.
Acta biomaterialia 09/2012; · 3.98 Impact Factor
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Li-Na Niu,
Kai Jiao,
Yi-Pin Qi,
Sergey Nikonov,
Cynthia K Y Yiu, Dwayne D Arola,
Shi-Qiang Gong,
Ahmed El-Marakby,
Marcela R O Carrilho,
Mark W Hamrick,
Kenneth M Hargreaves,
Anibal Diogenes,
Ji-Hua Chen,
David H Pashley,
Franklin R Tay
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ABSTRACT: Traditional bone regeneration strategies relied on supplementation of biomaterials constructs with stem or progenitor cells or growth factors. By contrast, cell homing strategies employ chemokines to mobilize stem or progenitor cells from host bone marrow and tissue niches to injured sites. Although silica-based biomaterials exhibit osteogenic and angiogenic potentials, they lack cell homing capability. Stromal cell-derived factor-1 (SDF-1) plays a pivotal role in mobilization and homing of stem cells to injured tissues. In this work, we demonstrated that 3-dimensional collagen scaffolds infiltrated with intrafibrillar silica are biodegradable and highly biocompatible. They exhibit improved compressive stress-strain responses and toughness over nonsilicified collagen scaffolds. They are osteoconductive and up-regulate expressions of osteogenesis- and angiogenesis-related genes more significantly than nonsilicified collagen scaffolds. In addition, these scaffolds reversibly bind SDF-1α for sustained release of this chemokine, which exhibits in vitro cell homing characteristics. When implanted subcutaneously in an in vivo mouse model, SDF-1α-loaded silicified collagen scaffolds stimulate the formation of ectopic bone and blood capillaries within the scaffold and abrogate the need for cell seeding or supplementation of osteogenic and angiogenic growth factors. Intrafibrillar-silicified collagen scaffolds with sustained SDF-1α release represent a less costly and complex alternative to contemporary cell seeding approaches and provide new therapeutic options for in situ hard tissue regeneration.-Niu, L.-N., Jiao, K., Qi, Y.-P., Nikonov, S., Yiu, C. K. Y., Arola, D. D., Gong, S.-Q., El-Marakby, A., Carrilho, M. R. O., Hamrick, M. W., Hargreaves, K. M., Diogenes, A., Chen, J.-H., Pashley, D. H., Tay, F. R. Intrafibrillar silicification of collagen scaffolds for sustained release of stem cell homing chemokine in hard tissue regeneration.
The FASEB Journal 08/2012; · 5.71 Impact Factor
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Shi-qiang Gong,
Li-Na Niu,
Lisa K Kemp,
Cynthia K Y Yiu,
Heonjune Ryou,
Yi-Pin Qi,
John D Blizzard,
Sergey Nikonov,
Martha G Brackett,
Regina L W Messer,
Christine D Wu,
Jing Mao,
L Bryan Brister,
Frederick A Rueggeberg, Dwayne D Arola,
David H Pashley,
Franklin R Tay
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ABSTRACT: The design of antimicrobial polymers to address healthcare issues and minimize environmental problems is an important endeavor with both fundamental and practical implications. Quaternary ammonium silane-functionalized methacrylate (QAMS) represents an example of antimicrobial macromonomers synthesized by a sol-gel chemical route; these compounds possess flexible Si-O-Si bonds. In present work, a partially hydrolyzed QAMS co-polymerized with 2,2-[4(2-hydroxy 3-methacryloxypropoxy)-phenyl]propane is introduced. This methacrylate resin was shown to possess desirable mechanical properties with both a high degree of conversion and minimal polymerization shrinkage. The kill-on-contact microbiocidal activities of this resin were demonstrated using single-species biofilms of Streptococcus mutans (ATCC 36558), Actinomyces naeslundii (ATCC 12104) and Candida albicans (ATCC 90028). Improved mechanical properties after hydration provided the proof-of-concept that QAMS-incorporated resin exhibits self-repair potential via water-induced condensation of organic modified silicate (ormosil) phases within the polymerized resin matrix.
Acta biomaterialia 05/2012; 8(9):3270-82. · 3.98 Impact Factor
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ABSTRACT: The hoof plays an important role in the health and well-being of dairy animals. Consequently, mechanical properties of the
hoof horn and changes in this tissue with nutrition or environmental factors are important concerns. A novel experimental
approach for evaluating the mechanical behaviour of hoof horn has been developed. The process is comprised of obtaining incremental
slices of hoof horn, stamping samples from selected zones of the sectioned tissue, performing uniaxial tensile tests and evaluating
the mechanical response using digital image correlation (DIC). From a combination of unique methods of extraction and evaluation,
the process enables hoof horn tissue to be characterized as a function of distance from the dermal-epidermal junction, within
specific regions of the claw and as a function of hydration. In addition, the methods enable both the elastic and inelastic
response of the tissue to be quantified. A preliminary study was performed to validate the new approach. In this manuscript
the methods of evaluation are described and demonstrated through an examination of the mechanical behaviour of bovine hoof
horn at two different levels of hydration.
Journal of Materials Science 04/2012; 42(4):1108-1115. · 2.02 Impact Factor
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Angewandte Chemie International Edition 12/2011; 50(49):11688-91. · 13.45 Impact Factor
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ABSTRACT: Biocalcification of collagen matrices with calcium phosphate and biosilicification of diatom frustules with amorphous silica are two discrete processes that have intrigued biologists and materials scientists for decades. Recent advancements in the understanding of the mechanisms involved in these two biomineralisation processes have resulted in the use of biomimetic strategies to replicate these processes separately using polyanionic, polycationic or zwitterionic analogues of extracellular matrix proteins to stabilise amorphous mineral precursor phases. To date, there is a lack of a universal model that enables the subtleties of these two apparently dissimilar biomineralisation processes to be studied together. Here, we utilise the eggshell membrane as a universal model for differential biomimetic calcification and silicification. By manipulating the eggshell membrane to render it permeable to stabilised mineral precursors, it is possible to introduce nanostructured calcium phosphate or silica into eggshell membrane fibre cores or mantles. We provide a model for infiltrating the two compartmental niches of a biopolymer membrane with different intrafibre minerals to obtain materials with potentially improved structure-property relationships.
Biomaterials 08/2011; 32(34):8743-52. · 7.40 Impact Factor
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ABSTRACT: The use of magnetic resonance (MR) imaging in conjunction with an endorectal coil is currently the clinical standard for the diagnosis of prostate cancer because of the increased sensitivity and specificity of this approach. However, imaging in this manner provides images and spectra of the prostate in the deformed state because of the insertion of the endorectal coil. Such deformation may lead to uncertainties in the localization of prostate cancer during therapy. We propose a novel 3-D elastic registration procedure that is based on the minimization of a physically motivated strain energy function that requires the identification of similar features (points, curves, or surfaces) in the source and target images. The Gauss-Seidel method was used in the numerical implementation of the registration algorithm. The registration procedure was validated on synthetic digital images, MR images from prostate phantom, and MR images obtained on patients. The registration error, assessed by averaging the displacement of a fiducial landmark in the target to its corresponding point in the registered image, was 0.2 ± 0.1 pixels on synthetic images. On the prostate phantom and patient data, the registration errors were 1.0 ± 0.6 pixels (0.6 ± 0.4 mm) and 1.8 ± 0.7 pixels (1.1 ± 0.4 mm), respectively. Registration also improved image similarity (normalized cross-correlation) from 0.72 ± 0.10 to 0.96 ± 0.03 on patient data. Registration results on digital images, phantom, and prostate data in vivo demonstrate that the registration procedure can be used to significantly improve both the accuracy of localized therapies such as brachytherapy or external beam therapy and can be valuable in the longitudinal follow-up of patients after therapy.
Journal of Digital Imaging 08/2011; 24(4):573-85. · 1.25 Impact Factor
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ABSTRACT: Inability of chemical phosphorylation of sodium trimetaphosphate to induce intrafibrillar mineralization of type I collagen may be due to the failure to incorporate a biomimetic analog to stabilize amorphous calcium phosphates (ACP) as nanoprecursors. This study investigated adsorption/desorption characteristics of hydrolyzed and pH-adjusted sodium trimetaphosphate (HPA-Na(3)P(3)O(9)) to collagen. Based on those results, a 5-minute treatment time with 2.8 wt% HPA-Na(3)P(3)O(9) was used in a single-layer reconstituted collagen model to confirm that both the ACP-stabilization analog and matrix phosphoprotein analog must be present for intrafibrillar mineralization. The results of that model were further validated by complete remineralization of phosphoric-acid-etched dentin treated with the matrix phosphoprotein analog and lined with a remineralizing lining composite, and with the ACP-stabilization analog supplied in simulated body fluid. An understanding of the basic processes involved in intrafibrillar mineralization of reconstituted collagen fibrils facilitates the design of novel tissue engineering materials for hard tissue repair and regeneration.
Journal of dental research 10/2010; 90(1):82-7. · 3.46 Impact Factor
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ABSTRACT: Natural biominerals are formed through metastable amorphous precursor phases via a bottom-up, nanoparticle-mediated mineralization mechanism. Using an acid-etched human dentin model to create a layer of completely demineralized collagen matrix, a bio-inspired mineralization scheme has been developed based on the use of dual biomimetic analogs. These analogs help to sequester fluidic amorphous calcium phosphate nanoprecursors and function as templates for guiding homogeneous apatite nucleation within the collagen fibrils. By adopting this scheme for remineralizing adhesive resin-bonded, completely demineralized dentin, we have been able to redeposit intrafibrillar and extrafibrillar apatites in completely demineralized collagen matrices that are imperfectly infiltrated by resins. This study utilizes a spectrum of completely and partially demineralized dentin collagen matrices to further validate the necessity for using a biomimetic analog-containing medium for remineralizing resin-infiltrated partially demineralized collagen matrices in which remnant seed crystallites are present. In control specimens in which biomimetic analogs are absent from the remineralization medium, remineralization could only be seen in partially demineralized collagen matrices, probably by epitaxial growth via a top-down crystallization approach. Conversely, in the presence of biomimetic analogs in the remineralization medium, intrafibrillar remineralization of completely demineralized collagen matrices via a bottom-up crystallization mechanism can additionally be identified. The latter is characterized by the transition of intrafibrillar minerals from an inchoate state of continuously braided microfibrillar electron-dense amorphous strands to discrete nanocrystals, and ultimately into larger crystalline platelets within the collagen fibrils. Biomimetic remineralization via dual biomimetic analogs has the potential to be translated into a functional delivery system for salvaging failing resin-dentin bonds.
Acta biomaterialia 07/2010; 6(7):2740-50. · 3.98 Impact Factor
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Archives of oral biology 12/2009; 54(12):1125-7. · 1.65 Impact Factor
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ABSTRACT: Calcium phosphate cement (CPC) has in situ-setting ability and bioactivity, but the brittleness and low strength limit CPC to only non-load-bearing bone repairs. Human umbilical cord mesenchymal stem cells (hUCMSCs) can be harvested without an invasive procedure required for the commonly studied bone marrow MSCs. However, little has been reported on hUCMSC delivery via bioactive scaffolds for bone tissue engineering. The objectives of this study were to develop CPC scaffolds with improved resistance to fatigue and fracture, and to investigate hUCMSC delivery for bone tissue engineering. In fast fracture, CPC with 15% chitosan and 20% polyglactin fibers (CPC-chitosan-fiber scaffold) had flexural strength of 26mPa, higher than 10mPa for CPC control (p<0.05). In cyclic loading, CPC-chitosan-fiber specimens that survived 2x10(6) cycles had the maximum stress of 10MPa, compared to 5MPa of CPC control. CPC-chitosan-fiber specimens that failed after multiple cycles had a mean stress-to-failure of 9MPa, compared to 5.8MPa for CPC control (p<0.05). hUCMSCs showed excellent viability when seeded on CPC and CPC-chitosan-fiber scaffolds. The percentage of live cells reached 96-99%. Cell density was about 300cells/mm(2) at day 1; it proliferated to 700cells/mm(2) at day 4. Wst-1 assay showed that the stronger CPC-chitosan-fiber scaffold had hUCMSC viability that matched the CPC control (p>0.1). In summary, this study showed that chitosan and polyglactin fibers substantially increased the fatigue resistance of CPC, and that hUCMSCs had excellent proliferation and viability on the scaffolds.
Biomaterials 10/2009; 31(5):840-7. · 7.40 Impact Factor
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ABSTRACT: This study tested the hypothesis that the use of ethylenediamine tetraacetic acid (EDTA) as a final irrigant causes canal wall erosion only after prolonged use of 5.25% sodium hypochlorite (NaOCl) as the initial irrigant.
Two irrigation protocols were employed: (1) 5.25% NaOCl as the initial irrigant for 10 min and 17% EDTA as the final irrigant for 2 min; and (2) 5.25% NaOCl for 60 min and 17% EDTA for 2 min. Flexural strengths of dentine beams prepared from human mid-coronal dentine were evaluated using a miniature three-point bending device after they were irrigated with either protocol. Transmission electron microscopy was used to examine the conditions of instrumented canal walls irrigated with either protocol after they were bonded with methacrylate resin-based sealers.
Immersion of dentine beams in NaOCl for 60 min instead of 10 min prior to the use of EDTA resulted in a significant (p<0.001) decline in flexural strength. For both NaOCl initial rinsing times, a 2-min final irrigation with EDTA created similar 0.5 microm thick demineralisation fronts. However, extensive surface and subsurface erosion of radicular dentine was seen only when the dentine was immersed in NaOCl for 60 min.
The apparent aggressiveness of EDTA in causing canal wall erosion is attributed to the prolonged use of NaOCl. The associated decline in dentine flexural strength has potential clinical relevance when thin pulp chamber dentine is immersed in NaOCl for lengthy periods during canal instrumentation. This may render root-treated teeth more prone to vertical fracture.
Journal of dentistry 10/2009; 38(3):201-6. · 2.00 Impact Factor
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ABSTRACT: This study examined changes in elastic modulus, mineral density and ultrastructure of resin-infiltrated dentin after biomimetic remineralization. Sixty demineralized dentin beams were infiltrated with Clearfil Tri-S Bond, One-Step or Prime&Bond NT. They were immersed in simulated body fluid (SBF) for 1 week to maximize water sorption before determining the baseline elastic moduli. For each adhesive (N = 20) half of the beams remained immersed in SBF (control). The rest were immersed in a biomimetic remineralization medium. The elastic moduli were measured weekly for 15 additional weeks. Representative remineralized specimens were evaluated by X-ray microtomography and transmission electron microscopy (TEM). The elastic moduli of control resin-infiltrated dentin remained consistently low, while those immersed in the biomimetic remineralization medium increased by 55-118% after 4 months. X-ray microtomography of the remineralized specimens revealed decreases in mineral density from the beam surface to the beam core that were indicative of external mineral aggregation and internal mineral deposition. Interfibrillar and intrafibrillar remineralization of resin-sparse intertubular dentin were seen under TEM, together with remineralized peritubular dentin. Biomimetic remineralization occurs by diffusion of nanoprecursors and biomimetic analogs in completely demineralized resin-infiltrated dentin and proceeds without the contribution of materials released from a mineralized dentin base.
Acta biomaterialia 10/2009; 6(4):1453-61. · 3.98 Impact Factor
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ABSTRACT: Degradation of hybrid layers created in primary dentin occurs as early as 6 months in vivo. Biomimetic remineralization utilizes "bottom-up" nanotechnology principles for interfibrillar and intrafibrillar remineralization of collagen matrices. This study examined whether imperfect hybrid layers created in primary dentin can be remineralized. Coronal dentin surfaces were prepared from extracted primary molars and bonded using Adper Prompt L-Pop and a composite. One-millimeter-thick specimen slabs of the resin-dentin interface were immersed in a Portland cement-based remineralization medium that contained two biomimetic analogs to mimic the sequestration and templating functions of dentin noncollagenous proteins. Specimens were retrieved after 1-6 months. Confocal laser scanning microscopy was used for evaluating the permeability of hybrid layers to Rhodamine B. Transmission electron microscopy was used to examine the status of remineralization within hybrid layers. Remineralization at different locations of the hybrid layers corresponded with quenching of fluorescence within similar locations of those hybrid layers. Remineralization was predominantly intrafibrillar in nature as interfibrillar spaces were filled with adhesive resin. Biomimetic remineralization of imperfect hybrid layers in primary human dentin is a potential means for preserving bond integrity. The success of the current proof-of-concept, laterally diffusing remineralization protocol warrants development of a clinically applicable biomimetic remineralization delivery system.
Journal of Biomedical Materials Research Part A 09/2009; 93(4):1225-34. · 2.63 Impact Factor
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ABSTRACT: In this study the crack growth resistance behavior and fracture toughness of human tooth enamel were quantified using incremental crack growth measures and conventional fracture mechanics. Results showed that enamel undergoes an increase in crack growth resistance (i.e. rising R-curve) with crack extension from the outer to the inner enamel, and that the rise in toughness is a function of distance from the dentin enamel junction (DEJ). The outer enamel exhibited the lowest apparent toughness (0.67+/-0.12 MPam(0.5)), and the inner enamel exhibited a rise in the growth toughness from 1.13 MPam(0.5)/mm to 3.93 MPam(0.5)/mm. The maximum crack growth resistance at fracture (i.e. fracture toughness (K(c))) ranged from 1.79 to 2.37 MPam(0.5). Crack growth in the inner enamel was accompanied by a host of mechanisms operating from the micro- to the nano-scale. Decussation in the inner enamel promoted crack deflection and twist, resulting in a reduction of the local stress intensity at the crack tip. In addition, extrinsic mechanisms such as bridging by unbroken ligaments of the tissue and the organic matrix promoted crack closure. Microcracking due to loosening of prisms was also identified as an active source of energy dissipation. In summary, the unique microstructure of enamel in the decussated region promotes crack growth toughness that is approximately three times that of dentin and over ten times that of bone.
Biomaterials 06/2009; 30(23-24):4037-46. · 7.40 Impact Factor
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ABSTRACT: Cracks and craze lines are often observed in the enamel of human teeth, but they rarely cause tooth fracture. The present study evaluates fatigue crack growth in human enamel, and compares that to the fatigue response of sintered hydroxyapatite (HAp) with similar crystallinity, chemistry and density. Miniature inset compact tension (CT) specimens were prepared that embodied a small piece of enamel (N=8) or HAp (N=6). The specimens were subjected to mode I cyclic loads and the steady state crack growth responses were modeled using the Paris Law. Results showed that the fatigue crack growth exponent (m) for enamel (m=7.7+/-1.0) was similar to that for HAp (m=7.9+/-1.4), whereas the crack growth coefficient (C) for enamel (C=8.7 E-04 (mm/cycle)x(MPa m(0.5))(-m)) was significantly lower (p<0.0001) than that for HAp (C=2.0 E+00 (mm/cycle)x(MPa m(0.5))(-m)). Micrographs of the fracture surfaces showed that crack growth in the enamel occurred primarily along the prism boundaries. In regions of decussation, the microstructure promoted microcracking, crack bridging, crack deflection and crack bifurcation. Working in concert, these mechanisms increased the crack growth resistance and resulted in a sensitivity to crack growth (m) similar to bone and lower than that of human dentin. These mechanisms of toughening were not observed in the crack growth response of the sintered HAp. While enamel is the most highly mineralized tissue of the human body, the microstructural arrangement of the prisms promotes exceptional resistance to crack growth.
Biomaterials 10/2008; 29(36):4847-54. · 7.40 Impact Factor
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ABSTRACT: In this study the influence of tubule orientation on the strength of human dentin under static and cyclic loads was examined. Rectangular beams were sectioned from the coronal dentin of virgin extracted molars (N=83) and then loaded in quasi-static 4-point flexure or 4-point flexural fatigue to failure. The flexure strength, energy to fracture and fatigue strength were evaluated for specimens with the dentin tubules aligned parallel (theta=0 degrees ) and perpendicular (theta=90 degrees ) to the plane of maximum normal stress. Results from monotonic loading showed that both the flexural strength and energy to fracture of dentin specimens with theta=0 degrees were significantly greater than those with theta=90 degrees . Furthermore, the apparent endurance strength of dentin with theta=0 degrees (44MPa) was significantly greater than that of the dentin with theta=90 degrees (24MPa). The ratio of apparent endurance strength (for fully reversed loading) to the flexure strength for theta=0 degrees and theta=90 degrees was 0.41 and 0.28, respectively. Although the influence of tubule orientation was most important to mechanical behavior, the flexure strength and energy to fracture also decreased with an increase in tubule density. According to differences in the fatigue strength with tubule orientation, restorative practices promoting large cyclic normal stresses perpendicular to the tubules would be more likely to facilitate fatigue failure in dentin with cyclic loading.
Biomaterials 04/2006; 27(9):2131-40. · 7.40 Impact Factor
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ABSTRACT: The fracture of restored teeth is a significant obstacle to lifelong oral health. Recent studies suggest that fatigue cracks originate at flaws introduced during cavity preparation and that fatigue crack growth is a principle cause of restored tooth fractures. In this study, the rate of fatigue crack growth in bovine dentin was estimated under mode I cyclic loading. Double cantilever beam (DCB) specimens were obtained from bovine molars and subjected to high cycle fatigue loading (10(5) < N < 10(6)). The fatigue crack growth rates were measured and used to estimate the crack growth exponent and coefficient according to the Paris Law. The average fatigue crack growth exponent was 4.7 +/- 0.6 for crack growth parallel to the dentin tubules, which was significantly larger than 4.3 +/- 0.5 for crack growth perpendicular to the tubules (t-test, CI > 80%). Although the crack growth rates varied considerably, there was no significant dependence on tubule orientation or tubule density. However, specific features of the fracture surfaces and tendencies for crack curving away from the tubules suggested preferential fatigue crack growth perpendicular to the dentin tubules. Results from this study are being used to guide an experimental investigation of fatigue crack growth in human dentin.
Journal of Biomedical Materials Research Part A 10/2003; 67(1):78-86. · 2.63 Impact Factor
