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Journal Articles Physical Chemistry Chemical Physics Year : 2019

Quantitative determination of the phosphorus environment in lithium aluminosilicate glasses using solid-state NMR techniques

Abstract

We investigated using solid-state NMR spectroscopy the short-range structural features in lithium aluminosilicate glasses with the addition of P2O5 and considering various Al2O3/Li2O ratios. The phosphorus environment is determined quantitatively using P-31 Magic Angle Spinning NMR constrained by results obtained from P-31-Al-27 Multiple-Quantum Coherence-based NMR techniques. Phosphorus is mainly located as orthophosphate and pyrophosphate species in glasses with a low amount of Al2O3. These depolymerized units disappear with increasing Al2O3 content and a strong affinity of PO4 tetrahedra for aluminum is revealed, which reduces phase separation. The local environments of framework (Si and Al) and charge-balancing (Li) cations are also studied through NMR experiments to assess the influence of P2O5 addition. The Si environment is mostly modified by the presence of P2O5 in glasses containing a low amount of Al2O3, with an increase of Q4Si species in relation to phase separation phenomena observed in these compositions. Conversely, P2O5 addition does not have a significant influence on the Al-27 NMR response. Li-7 NMR spectra reflect a change in the structural role of Li when P2O5 or Al2O3 is added. The observed structural changes can be rationalized to improve our knowledge of the structure-property relationships, focusing, in particular, on phase separation and nucleation/crystallization processes that are strongly affected by the presence of P and the evolution of its local environment with composition.
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Dates and versions

hal-02276094 , version 1 (06-12-2023)

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Pauline Glatz, Monique Comte, Lionel Montagne, Bertrand Doumert, Laurent Cormier. Quantitative determination of the phosphorus environment in lithium aluminosilicate glasses using solid-state NMR techniques. Physical Chemistry Chemical Physics, 2019, 21 (33), pp.18370-18379. ⟨10.1039/c9cp03181b⟩. ⟨hal-02276094⟩
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