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In situ Electron Paramagnetic Resonance Investigation of Isotope-selective Breathing in MIL-53 during Dihydrogen Adsorption.
Chemistry
January 2025
University of Leipzig, Physics and Geoscience, Linnestr. 5, 4103, Leipzig, GERMANY.
The development of smart materials capable of separating dihydrogen isotopologues has risen recently. Among potential candidates, the flexible MIL-53 (Al) has been gaining attention due to its structural flexibility providing the so-called ''breathing mechanism'' that can be useful to separate hydrogen isotopologues selectively. In the present work, an in situ continuous wave electron paramagnetic resonance investigation has been proven as a sensitive technique to follow the isotopologue-selective adsorption-desorption of dihydrogen species on the paramagnetic metal-doped MIL-53 (Al0.
View Article and Find Full Text PDFA recyclable dynamic semiconducting polymer consisting of Pauli-paramagnetic diradicaloids promoted and stabilized by catechol-boron coordination.
Chem Sci
January 2025
Key Laboratory of Flexible Optoelectronic Materials and Technology, Ministry of Education, Jianghan University Wuhan 430056 P. R. China
Coordination between 5,5',6,6'-tetrahydroxyindigo (4OH-ID) and boron tribromide unexpectedly affords a novel dynamic covalent polymer, namely P(ID-O-B), consisting of alternating indigo and indigo diradicaloid units. The catechol-boron dynamic bond plays a vital role in promoting the diradicaloid formation and stabilizing the formed diradicaloid segments. The diradicaloid segment in the polymer has a triplet ground state and a thermally populated doublet state, which has been confirmed by the EPR study.
View Article and Find Full Text PDFHypershifted spin spectroscopy with dynamic nuclear polarization at 1.4 K.
Sci Adv
December 2024
Laboratoire des Biomolécules, LBM, Département de Chimie, École Normale Supérieure, PSL University, Sorbonne Université, CNRS, 75005 Paris, France.
Dynamic nuclear polarization (DNP) enhances nuclear magnetic resonance (NMR) sensitivity by transferring polarization from unpaired electrons to nuclei, but nearby nuclear spins are difficult to detect or "hidden" due to strong electron-nuclear couplings that hypershift their NMR resonances. Here, we detect these hypershifted spins in a frozen glycerol-water mixture doped with TEMPOL at ~1.4 K using spin diffusion enhanced saturation transfer (SPIDEST), which indirectly reveals their spectrum.
View Article and Find Full Text PDFFerromagnetic Exchange and Slow Magnetic Relaxation in Cobalt Bis(1,2-dithiolene)-Bridged Dilanthanide Complexes.
Inorg Chem
December 2024
Department of Chemistry, University of California, Berkeley, California 94720, United States.
The construction of multinuclear lanthanide-based molecules with significant magnetic exchange interactions represents a key challenge in the realization of single-molecule magnets with high operating temperatures. Here, we report the synthesis and magnetic characterization of two series of heterobimetallic compounds, (Cp*Ln)(μ-Co(pdt)) (Ln = Y, Gd, Dy; pdt = 1,2-diphenylethylenedithiolate) and [K(18-crown-6)][(Cp*Ln)(μ-Co(pdt))] (Ln = Y, Gd), featuring two lanthanide centers bridged by a cobalt bis(1,2-dithiolene) complex. Dc magnetic susceptibility data collected for the Gd congeners indicate significant Gd-Co ferromagnetic exchange interactions with fits affording = +11.
View Article and Find Full Text PDFHigh-field pulsed EPR spectroscopy under magic angle spinning.
Sci Adv
August 2024
School of Chemistry, Tel-Aviv University, 6997801 Tel-Aviv, Israel.
In this work, we demonstrate the first pulsed electron paramagnetic resonance (EPR) experiments performed under magic angle spinning (MAS) at high magnetic field. Unlike nuclear magnetic resonance (NMR) and dynamic nuclear polarization (DNP), commonly performed at high magnetic fields and under MAS to maximize sensitivity and resolution, EPR is usually measured at low magnetic fields and, with the exception of the Spiess group work in the late 1990s, never under MAS, due to great instrumentational challenges. This hampers the investigation of DNP mechanisms, in which electron spin dynamics play a central role, because no experimental data about the latter under DNP-characteristic conditions are available.
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