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Towards Overhauser DNP in supercritical CO(2).

S G J van Meerten1, M C D Tayler1, A P M Kentgens1

  • 1Radboud University, Institute for Molecules and Materials, Heyendaalseweg 135, 6525AJ Nijmegen, The Netherlands.

Journal of Magnetic Resonance (San Diego, Calif. : 1997)
|April 16, 2016
PubMed
Summary

Supercritical CO2 shows promise as a low-viscosity solvent for Overhauser Dynamic Nuclear Polarization (ODNP), enabling faster molecular motion crucial for enhanced NMR sensitivity.

Keywords:
CO(2)Dynamic Nuclear PolarizationOverhauserSupercritical

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Area of Science:

  • Physical Chemistry
  • Magnetic Resonance Imaging
  • Chemical Engineering

Background:

  • Overhauser Dynamic Nuclear Polarization (ODNP) enhances NMR sensitivity by transferring electron spin polarization to nuclei.
  • The efficiency of ODNP relies on fast local translational dynamics, favored by low-viscosity solvents.
  • High magnetic fields, common in NMR, benefit from such efficient polarization transfer.

Purpose of the Study:

  • Investigate supercritical CO2 as a potential low-viscosity solvent for ODNP.
  • Determine the translational dynamics and Overhauser cross-relaxation of toluene in high-pressure CO2.
  • Assess the feasibility of supercritical CO2 for future high-field ODNP applications.

Main Methods:

  • Measurement of diffusion constants and longitudinal nuclear relaxation rates (T1) of toluene in high-pressure CO2.
  • Analysis of (1)H T1 changes with TEMPO radical addition to determine Overhauser cross-relaxation.
  • Comparison of experimental data with calculations from the Force Free Hard Sphere (FFHS) model.

Main Results:

  • Translational correlation times for toluene in supercritical CO2 were found to be in the range of 2-4 ps.
  • These correlation times are dependent on temperature, pressure, and toluene concentration.
  • Preliminary ODNP experiments were conducted at 3.4T using superheated water and toluene/CO2 systems.

Conclusions:

  • Supercritical CO2 exhibits suitable properties for enhancing ODNP efficiency due to its low viscosity and resulting fast molecular dynamics.
  • The identified short correlation times support the potential of supercritical CO2 as a solvent for advanced high-field ODNP techniques.
  • This research opens avenues for novel applications of ODNP in various scientific fields requiring high NMR sensitivity.