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Proton Environments in Biomimetic Calcium Phosphates Formed from Mesoporous Bioactive CaO-SiO2-P2O5 Glasses in Vitro: Insights from Solid-State NMR
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
Stockholm University, Faculty of Science, Department of Materials and Environmental Chemistry (MMK).
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Number of Authors: 9
2017 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 121, no 24, 13223-13238 p.Article in journal (Refereed) Published
Abstract [en]

When exposed to body fluids, mesoporous bioactive glasses (MBGs) of the CaO-SiO2-P2O5 system develop a bone-bonding surface layer that initially consists of amorphous calcium phosphate (ACP), which transforms into hydroxy-carbonate apatite (HCA) with a very similar composition as bone/dentin mineral. Information from various H-1-based solid-state nuclear magnetic resonance (NMR) experiments was combined to elucidate the evolution of the proton speciations both at the MBG surface and within each ACP/HCA constituent of the biomimetic :phosphate layer a formed when each of three MBGs with distinct Ca, Si; and P contents was immersed in a simulated body fluid (SBF) for variable periods between 15 min and 30 days. Directly excited magic-angle-spinning (MAS) H-1 NMR spectra mainly reflect the MBG component, whose surface is rich in water and silanol (SiOH) moieties. Double-quantum-single-quantum correlation H-1 NMR experimentation At fast MAS revealed their interatomic proximities. The comparatively minor H species of each ACP and HCA component were probed selectively by heteronuclear H-1-P-31 NMR experimentation. The initially prevailing ACP phase comprises H2O and nonapatitic.HPO42-/PO43- groups, whereas for prolonged MBG soaking Over days, a well-progressed ACP -> HCA transformation was evidenced by a dominating (OH)-H-1 resonance from HCA. We show that H-1-detected H-1 -> P-31 cross polarization NMR is markedly more sensitive than utilizing powder X-ray diffraction or P-31 NMR for detecting the onset of HCA formation, notably so for P-bearing (M)BGs. In relation to the long-standing controversy as to whether bone mineral comprises ACP and/or forms via an ACP precursor, we discuss a recently accepted structural core-shell picture of both synthetic and biological HCA, highlighting the close relationship between the disordered surface layer and ACP.

Place, publisher, year, edition, pages
2017. Vol. 121, no 24, 13223-13238 p.
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Chemical Sciences
Identifiers
URN: urn:nbn:se:su:diva-145198DOI: 10.1021/acs.jpcc.7b03469ISI: 000404201900030PubMedID: 28663772OAI: oai:DiVA.org:su-145198DiVA: diva2:1128967
Available from: 2017-07-31 Created: 2017-07-31 Last updated: 2017-07-31Bibliographically approved

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Yu, YangStevensson, BaltzarEdén, Mattias
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