화학공학소재연구정보센터
Journal of Physical Chemistry B, Vol.121, No.29, 7156-7162, 2017
Transferred Overhauser DNP: A Fast, Efficient Approach for Room Temperature C-13 ODNP at Moderately Low Fields and Natural Abundance
Overhauser dynamic nuclear polarization (ODNP) is investigated at a moderately low field (1.2 T) for natural abundance C-13 NMR of small molecules in solution state at room temperature. It is shown that ODNP transferred from H-1 to C-13 by NMR coherence transfer is in general significantly more efficient than direct ODNP of C-13. Compared to direct C-13 ODNP, we demonstrate over 4-fold higher C-13 sensitivity (signal-to-noise ratio, SNR), achieved in one-eighth of the measurement time by transferred ODNP (t-ODNP). Compared to the C-13 signal arising from Boltzmann equilibrium in a fixed measurement time, this is equivalent to about 1500-fold enhancement of C-13 signal by t-ODNP, as against a direct C-13 ODNP signal enhancement of about 4S-fold, both at a moderate ESR saturation factor of about 0.25. This owes in part to the short polarization times characteristic of H-1. Typically, t-ODNP reflects the essentially uniform ODNP enhancements of all protons in a molecule. Although the purpose of this work is to establish the superiority of t-ODNP vis-a-vis direct C-13 ODNP, a comparison is also made of the SNR in t-ODNP experiments with standard high resolution NMR as well. Finally, the potential of t-ODNP experiments for 2D heteronuclear correlation spectroscopy of small molecules is demonstrated in 2D H-1-C-13 HETCOR experiments at natural abundance, with decoupling in both dimensions.