A theoretical and experimental study of lead substitution in calcium hydroxyapatite

被引：77

作者：

Ellis, DE ^{[1
]}

Terra, J

Warschkow, O

Jiang, M

González, GB

Okasinski, JS

Bedzyk, MJ

Rossi, AM

Eon, JG

机构：

[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA

[2] Northwestern Univ, Mat Res Ctr, Evanston, IL 60208 USA

[3] Ctr Brasileiro Pesquisas Fis, Rio De Janeiro, Brazil

[4] Univ Sydney, Sch Phys, Sydney, NSW 2005, Australia

[5] Yantai Univ, Dept Phys, Yantai, Peoples R China

[6] European Synchrotron Radiat Facil, F-38043 Grenoble, France

[7] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA

[8] Univ Fed Rio de Janeiro, Inst Quim, Rio De Janeiro, Brazil

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2006年 / 8卷 / 08期

关键词：

D O I：

10.1039/b509254j

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Characterization of lead substitution for calcium in hydroxyapatite (CaHA) is carried out, using experimental techniques and Density Functional theoretical (DFT) analyses. Theoretical modeling is used to obtain information of the Pb chemical environment for occupancy at either Ca(I) or Ca(II) sites of CaHA. Effects of the larger ionic radius of Pb 12 compared to Ca 12 are apparent in embedded cluster calculations of local chemical bonding properties. DFT periodic planewave pseudopotential studies are used to provide first-principles predictions of local structural relaxation and site preference for Pb(x)Ca(10-x)HA over the composition range x <= 6. General characteristics of the polycrystalline material are verified by X-ray diffraction and FTIR analysis, showing the presence of a single phase of CaHA structure. A short range structure around lead is proposed in order to interpret the Pb L-edge EXAFS spectrum of the solid solution Ca(6.6)Pb(3.4)HA. In this concentration we observe that lead mainly occupies Ca( II) sites; the EXAFS fit slightly favors Pb clustering, while theory indicates the importance of Pb-Pb avoidance on site (II).

引用

页码：967 / 976

页数：10

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