Understanding a Host–Guest Model System through 129Xe NMR Spectroscopic Experiments and Theoretical Studies†
Emmanuelle Dubost
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorCorresponding Author
Jean-Pierre Dognon
Laboratoire de Chimie Moléculaire et Catalyse pour l'Energie, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Jean-Pierre Dognon, Laboratoire de Chimie Moléculaire et Catalyse pour l'Energie, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Patrick Berthault, Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorBernard Rousseau
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorGaëlle Milanole
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorChristophe Dugave
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorYves Boulard
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorEstelle Léonce
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorCéline Boutin
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorCorresponding Author
Patrick Berthault
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Jean-Pierre Dognon, Laboratoire de Chimie Moléculaire et Catalyse pour l'Energie, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Patrick Berthault, Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorEmmanuelle Dubost
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorCorresponding Author
Jean-Pierre Dognon
Laboratoire de Chimie Moléculaire et Catalyse pour l'Energie, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Jean-Pierre Dognon, Laboratoire de Chimie Moléculaire et Catalyse pour l'Energie, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Patrick Berthault, Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorBernard Rousseau
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorGaëlle Milanole
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorChristophe Dugave
iBiTec-S/SCBM, LabEx LERMIT, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorYves Boulard
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorEstelle Léonce
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorCéline Boutin
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorCorresponding Author
Patrick Berthault
Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Jean-Pierre Dognon, Laboratoire de Chimie Moléculaire et Catalyse pour l'Energie, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Patrick Berthault, Laboratoire Structure et Dynamique par Résonance Magnétique, IRAMIS/NIMBE, URA 3299 CEA/CNRS, CEA Saclay, 91191 Gif-sur-Yvette (France)
Search for more papers by this authorFor this research, access to the HPC resources of [CCRT/CINES/IDRIS] was granted under the allocation x2014086146 made by GENCI (Grand Equipement National de Calcul Intensif). Support from the French Ministry of Research (project ANR-12-BSV5-0003) and from the Fondation pour la Recherche Médicale (project DCM20111223065) is acknowledged.
Graphical Abstract
How hosts handle a noble guest: A combination of NMR spectroscopy and quantum chemistry enabled thorough analysis of the noncovalent interactions inside a xenon–host complex. The validation of this approach with a family of cryptophane hosts derived by treatment of the structure shown with H2O2 paves the way for the design of potent smart hyperpolarized 129Xe NMR sensors.
Abstract
Gaining an understanding of the nature of host–guest interactions in supramolecular complexes involving heavy atoms is a difficult task. Described herein is a robust simulation method applied to complexes between xenon and members of a cryptophane family. The calculated chemical shift of xenon caged in a H2O2 probe, as modeled by quantum chemistry with complementary-orbital, topological, and energy-decomposition analyses, is in excellent agreement with that observed in hyperpolarized 129Xe NMR spectra. This approach can be extended to other van der Waals complexes involving heavy atoms.
Supporting Information
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