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Journal of the American Chemical Society 134, 30 (2012) 12611-12628
(87)Sr solid-state NMR as a structurally sensitive tool for the investigation of materials: antiosteoporotic pharmaceuticals and bioactive glasses.
Christian Bonhomme1, Christel Gervais1, Nicolas Folliet1, Frédérique Pourpoin@ccr.Jussieu.Fr Pourpoint1, Cristina Coelho Diogo2, Johnatan Lao3, Edouard Jallot3, Josephine Lacroix3, Jean-Marie Nedelec4, Dinu Iuga5, John Hanna6, Mark E. Smith6, Ye Xiang7, Jincheng Du7, Danielle Laurencin8

Strontium is an element of fundamental importance in biomedical science. Indeed, it has been demonstrated that Sr(2+) ions can promote bone growth and inhibit bone resorption. Thus, the oral administration of Sr-containing medications has been used clinically to prevent osteoporosis, and Sr-containing biomaterials have been developed for implant and tissue engineering applications. The bioavailability of strontium metal cations in the body and their kinetics of release from materials will depend on their local environment. It is thus crucial to be able to characterize, in detail, strontium environments in disordered phases such as bioactive glasses, to understand their structure and rationalize their properties. In this paper, we demonstrate that (87)Sr NMR spectroscopy can serve as a valuable tool of investigation. First, the implementation of high-sensitivity (87)Sr solid-state NMR experiments is presented using (87)Sr-labeled strontium malonate (with DFS (double field sweep), QCPMG (quadrupolar Carr-Purcell-Meiboom-Gill), and WURST (wideband, uniform rate, and smooth truncation) excitation). Then, it is shown that GIPAW DFT (gauge including projector augmented wave density functional theory) calculations can accurately compute (87)Sr NMR parameters. Last and most importantly, (87)Sr NMR is used for the study of a (Ca,Sr)-silicate bioactive glass of limited Sr content (only 9 wt %). The spectrum is interpreted using structural models of the glass, which are generated through molecular dynamics (MD) simulations and relaxed by DFT, before performing GIPAW calculations of (87)Sr NMR parameters. Finally, changes in the (87)Sr NMR spectrum after immersion of the glass in simulated body fluid (SBF) are reported and discussed.
1 :  LCMCP (site Paris VI) - Laboratoire de Chimie de la Matière Condensée de Paris (site Paris VI)
2 :  IMPC - Institut des Matériaux de Paris Centre
3 :  LPC - Laboratoire de Physique Corpusculaire [Clermont-Ferrand]
4 :  ICCF - Institut de Chimie de Clermont-Ferrand
5 :  Department of Physics
6 :  Solid State NMR Group, University of Warwick
7 :  Department of Materials Science and Engineering (Dallas, USA)
8 :  ICG ICMMM - Institut Charles Gerhardt - Institut de Chimie Moléculaire et des Matériaux de Montpellier