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Magnesium(II)-ATP Complexes in 1-Ethyl-3-Methylimidazolium Acetate Solutions Characterized by 31Mg β-Radiation-Detected NMR Spectroscopy


McFadden, Ryan M L; Szunyogh, Dániel; Bravo‐Frank, Nicholas; Johannsen, Silke; Sigel, Roland K O; et al (2022). Magnesium(II)-ATP Complexes in 1-Ethyl-3-Methylimidazolium Acetate Solutions Characterized by 31Mg β-Radiation-Detected NMR Spectroscopy. Angewandte Chemie Internationale Edition, 61(35):e202207137.

Abstract

The complexation of MgII with adenosine 5′-triphosphate (ATP) is omnipresent in biochemical energy conversion, but is difficult to interrogate directly. Here we use the spin-urn:x-wiley:14337851:media:anie202207137:anie202207137-math-0001 β-emitter 31Mg to study MgII-ATP complexation in 1-ethyl-3-methylimidazolium acetate (EMIM-Ac) solutions using β-radiation-detected nuclear magnetic resonance (β-NMR). We demonstrate that (nuclear) spin-polarized 31Mg, following ion-implantation from an accelerator beamline into EMIM-Ac, binds to ATP within its radioactive lifetime before depolarizing. The evolution of the spectra with solute concentration indicates that the implanted 31Mg initially bind to the solvent acetate anions, whereafter they undergo dynamic exchange and form either a mono- (31Mg-ATP) or di-nuclear (31MgMg-ATP) complex. The chemical shift of 31Mg-ATP is observed up-field of 31MgMg-ATP, in accord with quantum chemical calculations. These observations constitute a crucial advance towards using β-NMR to probe chemistry and biochemistry in solution.

Abstract

The complexation of MgII with adenosine 5′-triphosphate (ATP) is omnipresent in biochemical energy conversion, but is difficult to interrogate directly. Here we use the spin-urn:x-wiley:14337851:media:anie202207137:anie202207137-math-0001 β-emitter 31Mg to study MgII-ATP complexation in 1-ethyl-3-methylimidazolium acetate (EMIM-Ac) solutions using β-radiation-detected nuclear magnetic resonance (β-NMR). We demonstrate that (nuclear) spin-polarized 31Mg, following ion-implantation from an accelerator beamline into EMIM-Ac, binds to ATP within its radioactive lifetime before depolarizing. The evolution of the spectra with solute concentration indicates that the implanted 31Mg initially bind to the solvent acetate anions, whereafter they undergo dynamic exchange and form either a mono- (31Mg-ATP) or di-nuclear (31MgMg-ATP) complex. The chemical shift of 31Mg-ATP is observed up-field of 31MgMg-ATP, in accord with quantum chemical calculations. These observations constitute a crucial advance towards using β-NMR to probe chemistry and biochemistry in solution.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Scopus Subject Areas:Physical Sciences > Catalysis
Physical Sciences > General Chemistry
Uncontrolled Keywords:General Chemistry, Catalysis
Language:English
Date:26 August 2022
Deposited On:10 Jan 2023 17:05
Last Modified:29 May 2024 01:42
Publisher:Wiley-VCH Verlag
ISSN:1433-7851
OA Status:Green
Free access at:PubMed ID. An embargo period may apply.
Publisher DOI:https://doi.org/10.1002/anie.202207137
PubMed ID:35718746
  • Content: Published Version
  • Language: English
  • Licence: Creative Commons: Attribution-NonCommercial-NoDerivatives 4.0 International (CC BY-NC-ND 4.0)