Dataset Information

Unravelling Guest Dynamics in Crystalline Molecular Organics Using ²H Solid-State NMR and Molecular Dynamics Simulation.

ABSTRACT: ²H solid-state NMR and atomistic molecular dynamics (MD) simulations are used to understand the disorder of guest solvent molecules in two cocrystal solvates of the pharmaceutical furosemide. Traditional approaches to interpreting the NMR data fail to provide a coherent model of molecular behavior and indeed give misleading kinetic data. In contrast, the direct prediction of the NMR properties from MD simulation trajectories allows the NMR data to be correctly interpreted in terms of combined jump-type and libration-type motions. Time-independent component analysis of the MD trajectories provides additional insights, particularly for motions that are invisible to NMR. This allows a coherent picture of the dynamics of molecules restricted in molecular-sized cavities to be determined.

SUBMITTER: Erastova V

PROVIDER: S-EPMC11240262 | biostudies-literature | 2024 Jul

REPOSITORIES: biostudies-literature

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Publications

Unravelling Guest Dynamics in Crystalline Molecular Organics Using <sup>2</sup>H Solid-State NMR and Molecular Dynamics Simulation.

Erastova Valentina V Evans Ivana R IR Glossop William N WN Guryel Songül S Hodgkinson Paul P Kerr Hannah E HE Oganesyan Vasily S VS Softley Lorna K LK Wickins Helen M HM Wilson Mark R MR

Journal of the American Chemical Society 20240627 27

<sup>2</sup>H solid-state NMR and atomistic molecular dynamics (MD) simulations are used to understand the disorder of guest solvent molecules in two cocrystal solvates of the pharmaceutical furosemide. Traditional approaches to interpreting the NMR data fail to provide a coherent model of molecular behavior and indeed give misleading kinetic data. In contrast, the direct prediction of the NMR properties from MD simulation trajectories allows the NMR data to be correctly interpreted in terms of ...[more]

PMID: 38935813

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Project description:99Tc is one of the most problematic fission products in the nuclear fuel cycle owing to its large inventory in used nuclear fuel, long half-life, potential radiation hazard, high environmental mobility of its major species 99TcO4 -, and its redox-active nature. Ideally, 99TcO4 - should be removed at the first stage, when the used fuel rods are dissolved in highly concentrated nitric acid solution, which can substantially reduce its interference with the solvent extraction process through catalytic redox reactions with the key actinides and diminish the chance of discharge into the environment as the volatile species during the waste vitrification process. However, this task cannot be achieved by any of the reported anion-scavenging materials including traditional polymeric anion-exchange resins, inorganic cationic framework materials, and recently developed cationic metal-organic framework materials, because they either are not stable under the extreme conditions of the combined high acidity and strong radiation field or do not possess the required uptake selectivity towards 99TcO4 - in the presence of a huge excess of competing anions such as NO3 - and SO4 2-. Herein, we present the first study of 99TcO4 - removal under extreme conditions by a two-dimensional conjugated cationic covalent organic framework material, SCU-COF-1. This material exhibits ultrahigh acid stability, great resistance towards both large-dose β and γ irradiation and unprecedented 99TcO4 - uptake capabilities including extremely fast sorption kinetics (sorption equilibrium can be reached within 1 min), ultrahigh uptake capacity (702.4 mg g-1 for the surrogate ReO4 - at a slightly elevated temperature), and good anion-exchange selectivity towards 99TcO4 -. These excellent features endow SCU-COF-1 with the practical capabilities of separating 99TcO4 - from both simulant highly acidic fuel reprocessing solutions (3 M nitric acid) and low-activity waste streams at the US legacy nuclear site. The anion-exchange mechanism and the 99TcO4 - uptake selectivity are further demonstrated and clearly visualized by the molecular dynamics simulation investigations.

Dataset Information

Unravelling Guest Dynamics in Crystalline Molecular Organics Using ²H Solid-State NMR and Molecular Dynamics Simulation.

Publications

Unravelling Guest Dynamics in Crystalline Molecular Organics Using <sup>2</sup>H Solid-State NMR and Molecular Dynamics Simulation.

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Unravelling Guest Dynamics in Crystalline Molecular Organics Using 2H Solid-State NMR and Molecular Dynamics Simulation.

Publications

Unravelling Guest Dynamics in Crystalline Molecular Organics Using <sup>2</sup>H Solid-State NMR and Molecular Dynamics Simulation.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Unravelling Guest Dynamics in Crystalline Molecular Organics Using ²H Solid-State NMR and Molecular Dynamics Simulation.