Solution-Phase Magnetic Mechanistic Study of Ni-Seamed Pyrogallol[4]arene Nanocapsules Reveal Presence of Novel Cylindrical and Spherical Species.

Autor: Kumari H; James L. Winkle College of Pharmacy, University of Cincinnati, 231 Albert Sabin Way, Medical Science Building 3109C, Cincinnati, OH 45267-0514, USA., Dennis CL; National Institute of Standards and Technology, 100 Bureau Drive, Gaithersburg, MD 20899-8552, USA., Kline SR; National Institute of Standards and Technology, 100 Bureau Drive, Gaithersburg, MD 20899-8552, USA., Mossine AV; Department of Chemistry, University of Missouri-Columbia, 601 S. College Avenue, Columbia, MO 65211, USA., Deakyne CA; Department of Chemistry, University of Missouri-Columbia, 601 S. College Avenue, Columbia, MO 65211, USA., Atwood JL; Department of Chemistry, University of Missouri-Columbia, 601 S. College Avenue, Columbia, MO 65211, USA.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2022 Jul 25; Vol. 61 (30), pp. e202203010. Date of Electronic Publication: 2022 Apr 21.
DOI: 10.1002/anie.202203010
Abstrakt: The magnetic properties of nickel-seamed C-pyrogallol[4]arene (PgC 3 Ni) hexamers and dimers are studied for the first time in solution. The combination of small-angle neutron scattering and superconducting quantum interference device magnetometer measurements of the solution species reveal their paramagnetic and weakly antiferromagnetic behaviour. Surprisingly, the magnetic results indicated the presence of an unprecedented 13 Å-radius species, larger than both the dimeric and hexameric nanocapsules with both octahedral and square-planar metal centers. To confirm the presence of this novel species, we performed a mechanistic study of PgC 3 Ni as a function of temperature and solvent and deduced the presence of two additional new species: a) an 11 Å cylinder with Ni atoms seaming the tubular framework and b) an 8 Å-radius sphere with non-interacting Ni centers located within the internal cavity. Select parameters that shift the equilibrium towards desired species are also identified.
(© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
Databáze: MEDLINE