Hydroxyapatites: Key Structural Questions and Answers from Dynamic Nuclear Polarization

César Leroy, Fabien Aussenac, Laure Bonhomme-Coury, Akiyoshi Osaka, Satoshi Hayakawa, Florence Babonneau, Cristina Coelho-Diogo, Christian Bonhomme

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11 Citations (Scopus)

Abstract

We demonstrate that NMR/DNP (Dynamic Nuclear Polarization) allows an unprecedented description of carbonate substituted hydroxyapatite (CHAp). Key structural questions related to order/disorder and clustering of carbonates are tackled using distance sensitive DNP experiments using 13C-13C recoupling. Such experiments are easily implemented due to unprecedented DNP gain (orders of magnitude). DNP is efficiently mediated by quasi one-dimensional spin diffusion through the hydroxyl columns present in the CHAp structure (thought of as "highways" for spin diffusion). For spherical nanoparticles and Φ < 100 nm, it is numerically shown that spin diffusion allows their study as a whole. Most importantly, we demonstrate also that the DNP study at 100 K leads to data which are comparable to data obtained at room temperature (in terms of spin dynamics and line shape resolution). Finally, all 2D DNP experiments can be interpreted in terms of domains exhibiting well identified types of substitution: local order and carbonate clustering are clearly favored.

Original languageEnglish
Pages (from-to)10201-10207
Number of pages7
JournalAnalytical Chemistry
Volume89
Issue number19
DOIs
Publication statusPublished - Oct 3 2017

ASJC Scopus subject areas

  • Analytical Chemistry

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    Leroy, C., Aussenac, F., Bonhomme-Coury, L., Osaka, A., Hayakawa, S., Babonneau, F., Coelho-Diogo, C., & Bonhomme, C. (2017). Hydroxyapatites: Key Structural Questions and Answers from Dynamic Nuclear Polarization. Analytical Chemistry, 89(19), 10201-10207. https://doi.org/10.1021/acs.analchem.7b01332