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Apatite Coating of Iron Oxide Nanoparticles by Alternate Addition of Calcium and Phosphate Solutions: A Calcium and Carboxylate (Ca-COO) Complex-Mediated Apatite Deposition

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Abstract

Apatite is a biocompatible material widely used to encapsulate iron-oxide nanoparticles (IONPs) for biomedical applications, such as drug-delivery or fluorescent probe agent. Apatite-coated IONPs are commonly fabricated by initially incubating carboxylate-functionalized IONPs in calcium solution and directly adding phosphate solution to initiate apatite precipitation (direct-addition method). Apatite precipitation took place not only on IONPs surface but also in the bulk solution, resulting in apatite-IONPs mixture instead of coated structure. In this study, robust apatite-coated IONPs structure were aimed by modifying steps in direct-addition method. Initially, carboxylate-functionalized IONPs were incubated in calcium solution, physically separated from the incubating calcium solution by external magnet, and then separately reacted with phosphate solution to induce apatite deposition (alternate-addition method). Fourier-transform infrared (FTIR) analysis showed that a calcium solution at a concentration of 0.8 mol/L was required to initiate the formation of the calcium-carboxylate (Ca-COO) complex. The formation of non-stoichiometric apatite was confirmed for IONPs with Ca-COO complex, as evidenced by X-ray diffraction and FTIR analysis. The alternate-addition method produced apatite coating in the form of flake-like structures, which also exhibited strong adhesion to IONPs surface. In contrast, direct-addition method mainly produced agglomerate of apatite particles that weakly associated with IONPs. Both of apatite-coating methods did not alter the magnetic properties of IONPs. The simple modification of reaction steps in the widely used apatite-coating method was demonstrated to be beneficial in producing robust apatite-coated IONPs structure.

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Authors and Affiliations

  1. Department of Materials Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, S7-6, 2-12-1 Ookayama, Meguro, Tokyo, 152-8550, Japan

    Vincent Irawan & Toshiyuki Ikoma

  2. National Institute of Materials Science, 1-2-1 Sengen, Tsukuba, Ibaraki, 305-0047, Japan

    Masaki Takeguchi

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  1. Vincent Irawan
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10904_2019_1255_MOESM1_ESM.tif

Supplementary material 1 Supplementary Figure 1 Schematic representation of direct-addition and alternate-addition method (TIFF 467 kb)

10904_2019_1255_MOESM2_ESM.tif

Supplementary material 2 Supplementary Figure 2 (left figure) Selected area of CaP-0.8 is indicated by yellow box; (right figures) RGB map is a combined image of separate elemental mapping of Fe, Ca, O, and P (TIFF 1690 kb)

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Irawan, V., Takeguchi, M. & Ikoma, T. Apatite Coating of Iron Oxide Nanoparticles by Alternate Addition of Calcium and Phosphate Solutions: A Calcium and Carboxylate (Ca-COO) Complex-Mediated Apatite Deposition. J Inorg Organomet Polym 30, 1132–1140 (2020). https://doi.org/10.1007/s10904-019-01255-4

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