Higher Magnetic Fields, Finer MOF Structural Information: 17O Solid-State NMR at 35.2 T

Autor: Bryan E. G. Lucier, Xiaoling Wang, Shijia Jiang, Kuizhi Chen, Christel Gervais, Zhehong Gan, Ivan Hung, Christian Bonhomme, Yining Huang, Vinicius Abilio Martins, Jun Xu, Anmin Zheng
Přispěvatelé: Department of Chemistry, University of Western Ontario, University of Western Ontario (UWO), Nankai University (NKU), National High Magnetic Field Laboratory (NHMFL), Florida State University [Tallahassee] (FSU), Spectroscopie, Modélisation, Interfaces pour L'Environnement et la Santé (LCMCP-SMiLES), Laboratoire de Chimie de la Matière Condensée de Paris (LCMCP), Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Sorbonne Université (SU)-Centre National de la Recherche Scientifique (CNRS), Wuhan Institute of Physics and Mathematics, National Natural Science Foundation of China (Project 21904071), Open Funds (KF1818) of the State Key Laboratory of Fine Chemicals, Natural Sciences and Engineering Research Council (NSERC) of Canada for a Discovery Grant, NSF DMR-1644779 and the State of Florida, NSF (DMR-1039938 and DMR-0603042) and NIH (BTRR 1P41 GM122698)
Rok vydání: 2020
Předmět:
Zdroj: Journal of the American Chemical Society
Journal of the American Chemical Society, American Chemical Society, 2020, 142 (35), pp.14877-14889. ⟨10.1021/jacs.0c02810⟩
J Am Chem Soc
ISSN: 1520-5126
0002-7863
Popis: International audience; The spectroscopic study of oxygen, a vital element in materials, physical, and life sciences, is of tremendous fundamental and practical importance. 17O solid-state NMR (SSNMR) spectroscopy has evolved into an ideal site-specific characterization tool, furnishing valuable information on the local geometric and bonding environments about chemically distinct and, in some favorable cases, crystallographically inequivalent oxygen sites. However, 17O is a challenging nucleus to study via SSNMR, as it suffers from low sensitivity and resolution, owing to the quadrupolar interaction and low 17O natural abundance. Herein, we report a significant advance in 17O SSNMR spectroscopy. 17O isotopic enrichment and the use of an ultrahigh 35.2 T magnetic field have unlocked the identification of many inequivalent carboxylate oxygen sites in the as-made and activated phases of the metal–organic framework (MOF) α-Mg3(HCOO)6. The subtle 17O spectral differences between the as-made and activated phases yield detailed information about host–guest interactions, including insight into nonconventional O···H–C hydrogen bonding. Such weak interactions often play key roles in the applications of MOFs, such as gas adsorption and biomedicine, and are usually difficult to study via other characterization routes. The power of performing 17O SSNMR experiments at an ultrahigh magnetic field of 35.2 T for MOF characterization is further demonstrated by examining activation of the MIL-53(Al) MOF. The sensitivity and resolution enhanced at 35.2 T allows partially and fully activated MIL-53(Al) to be unambiguously distinguished and also permits several oxygen environments in the partially activated phase to be tentatively identified. This demonstration of the very high resolution of 17O SSNMR recorded at the highest magnetic field accessible to chemists to date illustrates how a broad variety of scientists can now study oxygen-containing materials and obtain previously inaccessible fine structural information.
Databáze: OpenAIRE
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