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      Amorphous calcium phosphate phase-mediated crystal nucleation kinetics and pathway

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          Abstract

          Generally, a solution nucleation model is used to study biomineralization kinetics. However, we found that the amorphous calcium phosphate (ACP)-mediated hydroxyapatite (HAP) nucleation in simulated body fluids (SBF) had a different profile from the linear relationship between ln J and ln −2 S ( J, nucleation rate; S, supersaturation). This behaviour was alternatively explained by a developed heterogeneous nucleation theory, which indicated that HAP was nucleated at the ACP–solution interface via a polymorph transformation. Based upon this new model, we demonstrated experimentally that the embedded polymer molecules inside ACP were inert on HAP nucleation kinetics; rather, the polymers adsorbed on ACP surface could inhibit HAP nucleation from ACP. It further confirmed the heterogeneous nucleation pathway of HAP on the precursor phase. The present study provides an in-depth understanding of HAP formation for ACP-mediated crystallization.

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          Ion-association complexes unite classical and non-classical theories for the biomimetic nucleation of calcium phosphate.

          Nico A J M Sommerdijk, Isabel de Andrade, Paul H H Bomans … (2012)
          Despite its importance in many industrial, geological and biological processes, the mechanism of crystallization from supersaturated solutions remains a matter of debate. Recent discoveries show that in many solution systems nanometre-sized structural units are already present before nucleation. Still little is known about the structure and role of these so-called pre-nucleation clusters. Here we present a combination of in situ investigations, which show that for the crystallization of calcium phosphate these nanometre-sized units are in fact calcium triphosphate complexes. Under conditions in which apatite forms from an amorphous calcium phosphate precursor, these complexes aggregate and take up an extra calcium ion to form amorphous calcium phosphate, which is a fractal of Ca(2)(HPO(4))(3)(2-) clusters. The calcium triphosphate complex also forms the basis of the crystal structure of octacalcium phosphate and apatite. Finally, we demonstrate how the existence of these complexes lowers the energy barrier to nucleation and unites classical and non-classical nucleation theories.
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            Amorphous calcium phosphates: synthesis, properties and uses in biomaterials.

            C Combes, C Rey (2010)
            This review paper on amorphous calcium phosphates (ACPs) provides an update on several aspects of these compounds which have led to many studies and some controversy since the 1970s, particularly because of the lack of irrefutable proof of the occurrence of an ACP phase in mineralised tissues of vertebrates. The various synthesis routes of ACPs with different compositions are reported and the techniques used to characterise this phase are reviewed. We focus on the various physico-chemical properties of ACPs, especially the reactivity in aqueous media, which have been exploited to prepare bioactive bone substitutes, particularly in the form of coatings and cements for orthopaedic applications and composites for dental applications. 2010 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
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              Amorphous calcium (ortho)phosphates.

              Sergey Dorozhkin (2010)
              Amorphous calcium phosphates (ACPs) represent a unique class of biomedically relevant calcium orthophosphate salts, having variable chemical but essentially identical glass-like physical properties, in which there is neither translational nor orientational long-range ordering of the atomic positions. Normally, ACPs are the first solid phases, precipitated after a rapid mixing of aqueous solutions containing ions of Ca(2+) and PO₄³⁻; however, other production techniques are known. Interestingly, ACPs prepared by wet-chemical techniques were found to have a relatively constant chemical composition over a relatively wide range of preparation conditions, which suggests the presence of a well-defined local structural unit, presumably with the structure of Ca₉(PO₄)₆ - so-called Posner cluster. However, the presence of similar clusters in ACPs produced by other techniques remains uncertain. All ACPs are thermodynamically unstable compounds and, unless stored in dry conditions or doped by stabilizers, spontaneously tend to transform to crystalline calcium orthophosphates, mainly to calcium apatites. This solution instability of ACPs and their easy transformation to crystalline phases are of a great biological relevance. Specifically, the initiating role ACPs play in matrix vesicle biomineralization raises the importance of ACPs from a mere laboratory curiosity to that of a key intermediate in skeletal calcification. In addition, due to significant chemical and structural similarities with calcified mammalian tissues, as well as excellent biocompatibility and bioresorbability, all types of ACPs are very promising candidates for the manufacture of artificial bone grafts. This review summarizes the current knowledge on the occurrence, preparation, composition, structure, major properties and biomedical applications of ACPs. To assist readers in looking for the specific details on ACPs, a great number of references have been collected and systematized. Copyright © 2010 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
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                Author and article information

                Journal
                Journal ID (publisher-id): FDISE6
                Title: Faraday Discussions
                Abbreviated Title: Faraday Discuss.
                Publisher: Royal Society of Chemistry (RSC)
                ISSN (Print): 1359-6640
                ISSN (Electronic): 1364-5498
                Publication date Created: 2015
                Publication date (Electronic): 2015
                Volume: 179
                Pages: 451-461
                Affiliations
                [1 ]Centre for Biomaterials & Biopathways, and Department of Chemistry
                [2 ]Zhejiang University
                [3 ]Hangzhou
                [4 ]China
                [5 ]Qiushi Academy for Advanced Studies
                Article
                DOI: 10.1039/C4FD00212A
                PubMed ID: 25876510
                SO-VID: 29529fc0-9e70-4b08-a843-7ccc6e1648d8
                Copyright © © 2015
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