NMR-Based Structural Biology, Max Planck Institute for Biophysical Chemistry, Am Fassberg 11, D-37077 Göttingen, Germany.
J Magn Reson. 2012 Jan;214(1):159-65. doi: 10.1016/j.jmr.2011.11.001. Epub 2011 Nov 18.
The Non-Hydrogenative Parahydrogen-Induced Polarization (NH-PHIP) technique, which is referred to as Signal Amplification by Reversible Exchange (SABRE), has been reported to be applicable to various substrates and catalysts. For more detailed studies, pyridine was mainly examined in the past. Here, we examined several pyrazole derivatives towards their amenability to this method using Crabtree's Catalyst, which is the polarization transfer catalyst that is best documented. Additionally, the dependence of the signal enhancement on the field strength, at which the polarization step takes place, was examined for pyridine and four different pyrazoles. To achieve this, the polarization step was performed at numerous previously determined magnetic fields in the stray field of the NMR spectrometer. The substrate dependence of the field dependence proved to be relatively small for the different pyrazoles and a strong correlation to the field dependence for pyridine was observed. Reducing the number of spins in the catalyst by deuteration leads to increased enhancement. This indicates that more work has to be invested in order to be able to reproduce the SABRE field dependence by simulations.
非加氢氘极化(NH-PHIP)技术,也被称为可逆交换信号放大(SABRE),已经被报道适用于各种底物和催化剂。在过去的研究中,主要以吡啶作为更详细研究的对象。在这里,我们使用经过最好记录的极化转移催化剂 Crabtree 催化剂,研究了几种吡唑衍生物对这种方法的适用性。此外,还研究了吡啶和四种不同吡唑在极化步骤发生的磁场强度对信号增强的依赖性。为了实现这一点,在 NMR 光谱仪的杂散场中,在以前确定的多个磁场下进行极化步骤。不同吡唑的磁场依赖性的底物依赖性相对较小,并且观察到与吡啶的磁场依赖性的强相关性。通过氘代减少催化剂中的自旋数会导致增强增加。这表明,为了能够通过模拟重现 SABRE 磁场依赖性,还需要投入更多的工作。