TY - JOUR

T1 - Sr Solid-State NMR as a Structurally Sensitive Tool for the Investigation of Materials

T2 - Antiosteoporotic Pharmaceuticals and Bioactive Glasses

AU - Bonhomme, Christian

AU - Gervais, Christel

AU - Folliet, Nicolas

AU - Pourpoint, Frédérique

AU - Coelho Diogo, Cristina

AU - Lao, Jonathan

AU - Jallot, Edouard

AU - Lacroix, Joséphine

AU - Nedelec, Jean-Marie

AU - Iuga, Dinu

AU - Hanna, John V.

AU - Smith, Mark E.

AU - Xiang, Ye

AU - Du, Jincheng

AU - Laurencin, Danielle

PY - 2012/8/1

Y1 - 2012/8/1

N2 - Strontium is an element of fundamental importance in biomedical science. Indeed, it has been demonstrated that Sr2+ 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 87Sr NMR spectroscopy can serve as a valuable tool of investigation. First, the implementation of high-sensitivity 87Sr solid-state NMR experiments is presented using 87Sr-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 87Sr NMR parameters. Last and most importantly, 87Sr 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 87Sr NMR parameters. Finally, changes in the 87Sr NMR spectrum after immersion of the glass in simulated body fluid (SBF) are reported and discussed.

AB - Strontium is an element of fundamental importance in biomedical science. Indeed, it has been demonstrated that Sr2+ 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 87Sr NMR spectroscopy can serve as a valuable tool of investigation. First, the implementation of high-sensitivity 87Sr solid-state NMR experiments is presented using 87Sr-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 87Sr NMR parameters. Last and most importantly, 87Sr 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 87Sr NMR parameters. Finally, changes in the 87Sr NMR spectrum after immersion of the glass in simulated body fluid (SBF) are reported and discussed.

U2 - 10.1021/ja303505g

DO - 10.1021/ja303505g

M3 - Journal article

VL - 134

SP - 12611

EP - 12628

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 0002-7863

IS - 30

ER -