Citrate Improves Collagen Mineralization via Interface Wetting: A Physicochemical Understanding of Biomineralization Control

Shao, Changyu; Zhao, Ruibo; Jiang, Shuqin; Yao, Shasha; Wu, Zhifang; Jin, Biao; Yang, Yuling; Pan, Haihua; Tang, Ruikang

doi:10.1002/adma.201704876

Cited by 169 publications

(157 citation statements)

References 55 publications

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“…Recently, the important structural role of citrate in regulating bone hydroxylapatite-like (HA) minerals has been uncovered: citrate molecules are not only studded on the surface of apatite nanocrystals [116] and bridged between the apatite mineral platelets, stabilizing bone apatite [117, 118], but also control the size and crystallinity of HA particles [119]. In addition to citrate-HA interactions, citrate-collagen (the primary bone organic matrix) interactions promote collagen biomineralization by improving the wetting effect at the collagen-mineral interface to directly regulate the mineralization process [120]. All the above studies demonstrate that citrate is a strongly bound and integral part of native bone, serving as a key mineralization regulator.…”

Section: Biology Considerations For Biomaterials Design and Applicationmentioning

confidence: 99%

Citrate chemistry and biology for biomaterials design

Gerhard

Lü

et al. 2018

Biomaterials

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Leveraging the multifunctional nature of citrate in chemistry and inspired by its important role in biological tissues, a class of highly versatile and functional citrate-based materials (CBBs) has been developed via facile and cost-effective polycondensation. CBBs exhibiting tunable mechanical properties and degradation rates, together with excellent biocompatibility and processability, have been successfully applied in vitro and in vivo for applications ranging from soft to hard tissue regeneration, as well as for nanomedicine designs. We summarize in the review, chemistry considerations for CBBs design to tune polymer properties and to introduce functionality with a focus on the most recent advances, biological functions of citrate in native tissues with the new notion of degradation products as cell modulator highlighted, and the applications of CBBs in wound healing, nanomedicine, orthopedic, cardiovascular, nerve and bladder tissue engineering. Given the expansive evidence for citrate's potential in biology and biomaterial science outlined in this review, it is expected that citrate based materials will continue to play an important role in regenerative engineering.

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Section: Biology Considerations For Biomaterials Design and Applicationmentioning

confidence: 99%

Citrate chemistry and biology for biomaterials design

Gerhard

Lü

et al. 2018

Biomaterials

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“…Along with pAsp, it is likely that citrate and inorganic ions, such as Mg 2+ and PO 4 3− , contributed to the crystal structures seen in the current study. It has been proposed that citrate penetrates collagen fibrils where it then provides additional nucleation sites for intrafibrillar calcium‐phosphate crystal growth (Shao et al, ). Additionally, when adsorbed on collagen fibrils, citrate has been reported to improve wetting between collagen and the mineral precursor phase (Shao et al, ).…”

Section: Discussionmentioning

confidence: 99%

“…It has been proposed that citrate penetrates collagen fibrils where it then provides additional nucleation sites for intrafibrillar calcium‐phosphate crystal growth (Shao et al, ). Additionally, when adsorbed on collagen fibrils, citrate has been reported to improve wetting between collagen and the mineral precursor phase (Shao et al, ). These effects appear to promote intrafibrillar mineralization, even in the absence of pAsp (Delgado‐López et al, ).…”

Section: Discussionmentioning

confidence: 99%

Use of tendon to produce decellularized sheets of mineralized collagen fibrils for bone tissue repair and regeneration

Grue

Veres

2019

J Biomed Mater Res

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With demand for alternatives to autograft and allograft materials continuing to rise, development of new scaffolds for bone tissue repair and regeneration remains of significant interest. Engineered collagen‐calcium phosphate (CaP) constructs can offer desirable attributes, including absence of foreign body response and possession of inherent osteogenic potential. Despite their promise, current collagen‐CaP constructs are limited to nonload‐bearing applications. In this article, we describe a process for creating decellularized sheets of highly aligned, natively cross‐linked, and mineralized collagen fibrils, which may be useful for developing multilaminate collagen‐CaP constructs with improved mechanical properties. Decellularized bovine tendons were cryosectioned to produce thin sheets of aligned collagen fibrils. Mineralization of the sheets was then performed using an alternate soaking method incorporating a polymer‐induced liquid precursor (PILP) process to promote intrafibrillar mineralization, along with incorporation of physiologically relevant amounts of citrate, Mg, and carbonate. Characteristics of the produced scaffolds were assessed using energy‐dispersive X‐ray spectroscopy (EDX), scanning electron microscopy (SEM), and transmission electron microscopy (TEM). Scaffolds were also compared with both native bovine cortical bone and pure hydroxyapatite using X‐ray powder diffraction (XRD), and Fourier transform infrared spectroscopy attenuated total reflection (FTIR‐ATR). Structural and chemical analyses show that the scaffold preparation process that we described is successful in creating mineralized collagen sheets, possessing a mineral phase similar to that found in bone as well as a close association between collagen fibrils and mineral plates.

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“…The main aim of this work was not the study of basic mechanisms of collagen mineralization and the effect of citrate in this process, which was already reported [17,18], but the preparation for the first time of a new luminescent bioinspired composite Col/Ap material. Therefore the luminescent properties properties of the as-synthesised samples were fully investigated.…”

Section: Luminescent Properties Of Eu 3+ -Doped Mineralized Collagen mentioning

confidence: 99%

“…Recently, Hu et al [13] using nuclear magnetic resonance ( 13 C-NMR) have revealed that citrate accounts for about 5.5 wt % of total organic matrix of bone and it is strongly bound to the surface of the apatite nanoparticles (1 molecule/2 nm 2 ). Its presence and abundance should not be considered adventitious but would reflect an important role in the biomineralization process [13,14]; therefore, the study of the effect of citrate in the formation of biomimetic apatite nanoplatelets as well as in collagen mineralization has become a subject of intense research in the last years [15][16][17][18][19]. The last results have shown that the use of citrate is an interesting and straightforward nature inspired strategy to control the chemical-physical features of the apatite for the development of improved nanoparticle-based biomaterials [20][21][22].…”

Section: Introductionmentioning

confidence: 99%

Bioinspired Mineralization of Type I Collagen Fibrils with Apatite in Presence of Citrate and Europium Ions

Morales¹,

Fernández-Penas²,

Verdugo‐Escamilla³

et al. 2018

Crystals

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Synthetic nanostructured hybrid composites based on collagen and nanocrystalline apatites are interesting materials for the generation of scaffolds for bone tissue engineering. In this work, mineralized collagen fibrils were prepared in the presence of citrate and Eu 3+ . Citrate is an indispensable and essential structural/functional component of bone. Eu 3+ endows the mineralized fibrils of the necessary luminescent features to be potentially employed as a diagnostic tool in biomedical applications. The assembly and mineralization of collagen were performed by the neutralization method, which consists in adding dropwise a Ca(OH) 2 solution to a H 3 PO 4 solution containing the dispersed type I collagen until neutralization. In the absence of citrate, the resultant collagen fibrils were mineralized with nanocrystalline apatites. When citrate was added in the titrant solution in a Citrate/Ca molar ratio of 2 or 1, it acted as an inhibitor of the transformation of amorphous calcium phosphate (ACP) to nanocrystalline apatite. The addition of Eu 3+ and citrate in the same titrant solution lead to the formation of Eu 3+ -doped citrate-coated ACP/collagen fibrils. Interestingly, the relative luminescent intensity and luminescence lifetime of this latter composite were superior to those of Eu 3+ -doped apatite/collagen prepared in absence of citrate. The cytocompatibility tests, evaluated by the 3-(4,5-Dimethylthiazol-2-yl)-2,5-diphenyltetrazolium bromide) (MTT) colorimetric assay in a dose-dependent manner on GTL-16 human gastric carcinoma cells, on MG-63 human osteosarcoma cells and on the m17.ASC, a spontaneously immortalized mouse mesenchymal stem cell clone from subcutaneous adipose tissue, show that, in general, all samples are highly cytocompatible.

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Citrate Improves Collagen Mineralization via Interface Wetting: A Physicochemical Understanding of Biomineralization Control

Cited by 169 publications

References 55 publications

Citrate chemistry and biology for biomaterials design

Citrate chemistry and biology for biomaterials design

Use of tendon to produce decellularized sheets of mineralized collagen fibrils for bone tissue repair and regeneration

Bioinspired Mineralization of Type I Collagen Fibrils with Apatite in Presence of Citrate and Europium Ions

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