Monitoring Crystallization Processes in Confined Porous Materials by Dynamic Nuclear Polarization Solid-State Nuclear Magnetic Resonance
| Autor: | Fabio Ziarelli, Marie Juramy, Pierre Thureau, Romain Chèvre, Eric Besson, Stéphane Viel, Stéphane Gastaldi, Paolo Cerreia Vioglio, Kenneth D. M. Harris, Giulia Mollica |
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| Přispěvatelé: | Institut de Chimie Radicalaire (ICR), Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), ANR-18-CE29-0007,CHARMING,CHANGEMENT DE PARADIGME POUR LA CONCEPTION D'AGENT DE POLARISATION POUR LA PDN(2018), ANR-11-IDEX-0001,Amidex,INITIATIVE D'EXCELLENCE AIX MARSEILLE UNIVERSITE(2011), European Project: 758498,ERC-2017-STG,STRUCTURE(2018) |
| Rok vydání: | 2021 |
| Předmět: |
Magnetic Resonance Spectroscopy
010402 general chemistry 01 natural sciences Biochemistry Article Catalysis law.invention Cyclic N-Oxides Colloid and Surface Chemistry law Phase (matter) Metastability [CHIM.CRIS]Chemical Sciences/Cristallography [CHIM]Chemical Sciences Crystallization Nanoscopic scale Chemistry [CHIM.MATE]Chemical Sciences/Material chemistry General Chemistry Nuclear magnetic resonance spectroscopy Silicon Dioxide 0104 chemical sciences Solid-state nuclear magnetic resonance Chemical physics Mesoporous material Porous medium Porosity |
| Zdroj: | Journal of the American Chemical Society Journal of the American Chemical Society, American Chemical Society, 2021, 143, pp.6095-6103. ⟨10.1021/jacs.0c12982⟩ Journal of the American Chemical Society, 2021, 143, pp.6095-6103. ⟨10.1021/jacs.0c12982⟩ |
| ISSN: | 1520-5126 0002-7863 |
| Popis: | International audience; Establishing mechanistic understanding of crystallization processes at the molecular level is challenging, as it requires both the detection of transient solid phases and monitoring the evolution of both liquid and solid phases as a function of time. Here, we demonstrate the application of dynamic nuclear polarization (DNP) enhanced NMR spectroscopy to study crystallization under nanoscopic confinement, revealing a viable approach to interrogate different stages of crystallization processes. We focus on crystallization of glycine within the nanometric pores (7−8 nm) of a tailored mesoporous SBA-15 silica material with wall-embedded TEMPO radicals. The results show that the early stages of crystallization, characterized by the transition from the solution phase to the first crystalline phase, are straightforwardly observed using this experimental strategy. Importantly, the NMR sensitivity enhancement provided by DNP allows the detection of intermediate phases that would not be observable using standard solid-state NMR experiments. Our results also show that the metastable β polymorph of glycine, which has only transient existence under bulk crystallization conditions, remains trapped within the pores of the mesoporous SBA-15 silica material for more than 200 days. |
| Databáze: | OpenAIRE |
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