Hierarchical Self-Assembly of Nano-Fibrils in Mineralized Collagen

Zhang, W.; Liao, Susan; Cui, Fu Zhai

doi:10.1021/cm030080g

Cited by 374 publications

(299 citation statements)

References 28 publications

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“…The typical needle-like morphology of HA crystals was well represented on 3D morphologies only, with aspect ratio measurements of nanocrystals close to that of synthesized HA [43]. The SAED images indicated a polycrystalline diffractogram for braided structures [34] (Figure 10) with preferential orientation extending along the c-axis, as also confirmed from the values of intensity ratio (Figure 6). This preferential orientation of the deposited crystals along the c-axis of the template is a typical feature of calcium phosphate noted in human bone and dentin where the c-axes of HA crystals align parallel to longitudinal axis of type I collagen fibrils [44].…”

Section: Discussionsupporting

confidence: 60%

Elucidation of differential mineralisation on native and regenerated silk matrices

Midha¹,

Tripathi²,

Geng

et al. 2016

Materials Science and Engineering: C

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Bone mineralisation is a well-orchestrated procedure triggered by a protein-based template inducing the nucleation of hydroxyapatite (HA) nanocrystals on the matrix. In an attempt to fabricate superior nanocomposites from silk fibroin, textile braided structures made of natively spun fibres of Bombyx mori silkworm were compared against regenerated fibroin (lyophilised and films) underpinning the influence of intrinsic properties of fibroin matrices on HA nucleation. We found that native braids could bind Ca 2+ ions through electrostatic attraction, which initiated the nucleation and deposition of HA, as evidenced by discrete shift in amide peaks via ATR-FTIR. This phenomenon also suggests the involvement of amide linkages in promoting HA nucleation on fibroin. Moreover, CaCl 2 -SBF immersion of native braids resulted in preferential growth of HA along the c-axis, forming needle-like nanocrystals and possessing Ca/P ratio comparable to commercial HA. Though regenerated lyophilised matrix also witnessed prominent peak shift in amide linkages, HA growth was restricted to (211) plane only, albeit at a significantly lower intensity than braids. Regenerated films, on the other hand, provided no crystallographic evidence of HA deposition within 7 days of SBF immersion. The present work sheds light on the primary fibroin structure of B.mori which probably plays a crucial role in regulating template-induced biomineralisation on the matrix. We also found that intrinsic material properties such as surface roughness, geometry, specific surface area, tortuosity and secondary conformation exert influence in modulating the extent of mineralisation. Thus our work generates useful insights and warrants future studies to further investigate the potential of bone mimetic, silk/mineral nanocomposite matrices for orthopaedic applications.

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Section: Discussionsupporting

confidence: 60%

Elucidation of differential mineralisation on native and regenerated silk matrices

Midha¹,

Tripathi²,

Geng

et al. 2016

Materials Science and Engineering: C

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“…An ordered composite powder of HAp and organic molecules was also prepared through self-organization by interplay at the organic-inorganic interface [20][21][22][23][24][25][26][27][28]. A composite material with a hierarchical structure was fabricated by the self-assembly of nanofibrils of mineralized collagen [29]. Recently, three-dimensional bonelike composites were fabricated by the calcification of hydrogels [30].…”

Section: Introductionmentioning

confidence: 99%

Preparation of hierarchically organized calcium phosphate–organic polymer composites by calcification of hydrogel

Furuichi

Oaki

Ichimiya

et al. 2006

Science and Technology of Advanced Materials

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A novel type of calcium phosphate-organic polymer composite having a hierarchical structure was prepared by calcification of a poly(acrylic acid) hydrogel. Macroscopically, an organic gel containing phosphate ions was transformed into an opaque solid material by diffusion of calcium ions. We observed the formation of micrometer-scale layered structures consisting of nanoscale crystals of hydroxylapatite (HAp) in the opaque products. The laminated architecture resulting from the periodic precipitation of calcium phosphate varied with the reaction conditions, such as the concentrations of the precursor ions and the density of the gel. The nanoscopic structure of HAp crystals was modified by the addition of gelatin to the polymer matrix. q

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“…Within this highly organized scaffold, apatite crystallites form nanometer-scale platelets (6-9) with their [001] axes preferentially aligned parallel to the fibril axis (10)(11)(12)(13)(14)(15) and the platelet faces defined by {100} crystal planes (16). Recent in vitro investigations of hydroxyapatite (HAP) formation within collagen fibrils revealed a multistage process in which amorphous calcium phosphate (ACP) first infiltrated through the hole zones and then converted into HAP platelets with initial mineral deposition occurring near the hole zones (11,13).…”

mentioning

confidence: 99%

Energetic basis for the molecular-scale organization of bone

Tao

Battle

Pan

et al. 2014

Proc. Natl. Acad. Sci. U.S.A.

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The remarkable properties of bone derive from a highly organized arrangement of coaligned nanometer-scale apatite platelets within a fibrillar collagen matrix. The origin of this arrangement is poorly understood and the crystal structures of hydroxyapatite (HAP) and the nonmineralized collagen fibrils alone do not provide an explanation. Moreover, little is known about collagen-apatite interaction energies, which should strongly influence both the molecular-scale organization and the resulting mechanical properties of the composite. We investigated collagen-mineral interactions by combining dynamic force spectroscopy (DFS) measurements of binding energies with molecular dynamics (MD) simulations of binding and atomic force microscopy (AFM) observations of collagen adsorption on single crystals of calcium phosphate for four mineral phases of potential importance in bone formation. In all cases, we observe a strong preferential orientation of collagen binding, but comparison between the observed orientations and transmission electron microscopy (TEM) analyses of native tissues shows that only calcium-deficient apatite (CDAP) provides an interface with collagen that is consistent with both. MD simulations predict preferred collagen orientations that agree with observations, and results from both MD and DFS reveal large values for the binding energy due to multiple binding sites. These findings reconcile apparent contradictions inherent in a hydroxyapatite or carbonated apatite (CAP) model of bone mineral and provide an energetic rationale for the molecular-scale organization of bone.biomineralization | bone | protein-mineral interface | dynamic force spectroscopy B one is a natural protein-mineral composite consisting of nonstoichiometric nanometer-scale carbonated apatite crystallites inside a fibrillar protein matrix. The matrix is mainly composed of type I collagen and is organized on multiple length scales (1, 2). At the shortest scale, three polypeptide chains form a triple helix referred to as a tropocollagen molecule that is ∼300 nm in length and 1.5 nm in diameter. These helices are arranged in a quasi-hexagonal bundle in which they overlap and intertwine to form microfibrils containing "hole zones," where there is a gap between the N termini of one helix and the C termini of another (3-5). These microfibrils are further bundled both laterally and longitudinally to form native collagen (3, 4).Within this highly organized scaffold, apatite crystallites form nanometer-scale platelets (6-9) with their [001] axes preferentially aligned parallel to the fibril axis (10-15) and the platelet faces defined by {100} crystal planes (16). Recent in vitro investigations of hydroxyapatite (HAP) formation within collagen fibrils revealed a multistage process in which amorphous calcium phosphate (ACP) first infiltrated through the hole zones and then converted into HAP platelets with initial mineral deposition occurring near the hole zones (11, 13). In vitro transmission electron microscopy (TEM) and atomic force microscop...

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Hierarchical Self-Assembly of Nano-Fibrils in Mineralized Collagen

Cited by 374 publications

References 28 publications

Elucidation of differential mineralisation on native and regenerated silk matrices

Elucidation of differential mineralisation on native and regenerated silk matrices

Preparation of hierarchically organized calcium phosphate–organic polymer composites by calcification of hydrogel

Energetic basis for the molecular-scale organization of bone

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