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Direct 17O Isotopic Labeling of Oxides Using Mechanochemistry.
Chen, Chia-Hsin; Gaillard, Emeline; Mentink-Vigier, Frédéric; Chen, Kuizhi; Gan, Zhehong; Gaveau, Philippe; Rebière, Bertrand; Berthelot, Romain; Florian, Pierre; Bonhomme, Christian; Smith, Mark E; Métro, Thomas-Xavier; Alonso, Bruno; Laurencin, Danielle.
Afiliação
  • Chen CH; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
  • Gaillard E; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
  • Mentink-Vigier F; National High Magnetic Field Laboratory (NHMFL), Florida State University, Tallahassee, Florida 32306, United States.
  • Chen K; National High Magnetic Field Laboratory (NHMFL), Florida State University, Tallahassee, Florida 32306, United States.
  • Gan Z; National High Magnetic Field Laboratory (NHMFL), Florida State University, Tallahassee, Florida 32306, United States.
  • Gaveau P; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
  • Rebière B; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
  • Berthelot R; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
  • Florian P; Conditions Extrêmes et Matériaux: Haute Température et Irradiation (CEMHTI), UPR 3079, CNRS, Université d'Orléans, 45071 Orléans, France.
  • Bonhomme C; Laboratoire de Chimie de la Matière Condensée de Paris, UMR 7574, CNRS, Sorbonne Université, Paris 75005, France.
  • Smith ME; Vice-Chancellor's Office, Highfield Campus, University of Southampton, University Road, Southampton SO17 1BJ, U.K.
  • Métro TX; Department of Chemistry, Lancaster University, Bailrigg, Lancaster LA1 4YB, U.K.
  • Alonso B; IBMM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
  • Laurencin D; ICGM, Univ. Montpellier, CNRS, ENSCM, Montpellier 34090, France.
Inorg Chem ; 59(18): 13050-13066, 2020 Sep 21.
Article em En | MEDLINE | ID: mdl-32167301
ABSTRACT
While 17O NMR is increasingly being used for elucidating the structure and reactivity of complex molecular and materials systems, much effort is still required for it to become a routine analytical technique. One of the main difficulties for its development comes from the very low natural abundance of 17O (0.04%), which implies that isotopic labeling is generally needed prior to NMR analyses. However, 17O-enrichment protocols are often unattractive in terms of cost, safety, and/or practicality, even for compounds as simple as metal oxides. Here, we demonstrate how mechanochemistry can be used in a highly efficient way for the direct 17O isotopic labeling of a variety of s-, p-, and d-block oxides, which are of major interest for the preparation of functional ceramics and glasses Li2O, CaO, Al2O3, SiO2, TiO2, and ZrO2. For each oxide, the enrichment step was performed under ambient conditions in less than 1 h and at low cost, which makes these synthetic approaches highly appealing in comparison to the existing literature. Using high-resolution solid-state 17O NMR and dynamic nuclear polarization, atomic-level insight into the enrichment process is achieved, especially for titania and alumina. Indeed, it was possible to demonstrate that enriched oxygen sites are present not only at the surface but also within the oxide particles. Moreover, information on the actual reactions occurring during the milling step could be obtained by 17O NMR, in terms of both their kinetics and the nature of the reactive species. Finally, it was demonstrated how high-resolution 17O NMR can be used for studying the reactivity at the interfaces between different oxide particles during ball-milling, especially in cases when X-ray diffraction techniques are uninformative. More generally, such investigations will be useful not only for producing 17O-enriched precursors efficiently but also for understanding better mechanisms of mechanochemical processes themselves.

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Guideline Idioma: En Ano de publicação: 2020 Tipo de documento: Article

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Guideline Idioma: En Ano de publicação: 2020 Tipo de documento: Article