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ATP-Ion Complexation and Lithium's Bioactive Form in Cellular Solutions.

Julian M Delgado1, Peter S Klein2, Sameer Varma1,3

  • 1Department of Molecular Biosciences, University of South Florida, 4202 E. Fowler Ave., Tampa FL-33620, United States.

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Lithium (Li+) can bind to ATP-Mg complexes, influencing its therapeutic action in bipolar disorder. This study reveals Li+ can exist in both free and bound forms within cells, impacting its molecular mechanism.

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Area of Science:

  • Biochemistry
  • Computational Chemistry
  • Pharmacology

Background:

  • Lithium (Li+) is a crucial treatment for bipolar disorder, but its precise molecular mechanism remains elusive.
  • Understanding the bioactive form of Li+ is essential for all proposed therapeutic action hypotheses.
  • The cellular distribution of free versus adenosine triphosphate (ATP)-bound Li+ is a key unknown.

Purpose of the Study:

  • To investigate the binding interactions between Li+, other monovalent cations (Na+, K+), and magnesium-bound ATP (ATP·Mg) under cellular conditions.
  • To determine the fraction of free versus ATP-bound Li+ at physiological concentrations.
  • To provide structural, thermodynamic, and kinetic insights into ion-ATP binding relevant to Li+ therapy.

Main Methods:

  • Molecular dynamics (MD) simulations using the polarizable AMOEBA-HFC force field.
  • Benchmarking MD force field against quantum mechanical and experimental data.
  • Kinetic modeling parameterized with MD and experimental data.

Main Results:

  • ATP·Mg possesses two binding sites for monovalent cations, capable of simultaneous binding.
  • Li+ competes with Na+ and K+ for these ATP·Mg binding sites.
  • While Li+ has a high affinity, its cellular sequestration by ATP·Mg is concentration-dependent, with up to 50% binding at physiological extremes, influenced by ATP levels.

Conclusions:

  • Both free and ATP-bound forms of Li+ can coexist at significant fractions within cells.
  • This finding offers a basis for exploring the molecular mechanisms of Li+ action in bipolar disorder treatment.
  • The study provides novel insights into ion-ATP interactions in cellular environments and identifies Li+'s bioactive form.