Zero-field nuclear magnetic resonance of chemically exchanging systems
Zero-field nuclear magnetic resonance of chemically exchanging systems
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DOI：
10.1038/s41467-019-10787-9
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发表时间：
2019-07-05
影响因子：
16.6
通讯作者：
Pines, Alexander
中科院分区：
文献类型：
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作者：
Barskiy, Danila A.;Taylen, Michael C. D.;Pines, Alexander
零场至超低场核磁共振(ZULF)是一种新兴的精密化学分析工具。在这项工作中，我们研究了动力学过程，并研究了化学交换对ZULF核磁共振J谱的影响。我们发展了一种可以在存在化学交换的情况下定量计算J谱的计算方法，并将其应用于研究[N-15]铵((NH4+)-N-15)的水溶液作为模型体系。我们表明，依赖于pH的化学交换对J光谱有很大影响，在某些情况下，可能导致光谱特征的退化和完全消失。为了展示ZULF核磁共振在化学和生物医学方面的潜在应用，我们展示了通过溶解动态核极化(DDNP)超极化的[2-C-13]丙酮酸的ZULF核磁共振谱。我们展望了可负担和可扩展的ZULF核磁共振与超极化相结合的应用，以研究体内的化学交换现象以及在无法实现高场核磁共振检测的情况下的化学交换现象。
Zero- to ultralow-field (ZULF) nuclear magnetic resonance (NMR) is an emerging tool for precision chemical analysis. In this work, we study dynamic processes and investigate the influence of chemical exchange on ZULF NMR J-spectra. We develop a computational approach that allows quantitative calculation of J-spectra in the presence of chemical exchange and apply it to study aqueous solutions of [N-15]ammonium ((NH4+)-N-15) as a model system. We show that pH-dependent chemical exchange substantially affects the J-spectra and, in some cases, can lead to degradation and complete disappearance of the spectral features. To demonstrate potential applications of ZULF NMR for chemistry and biomedicine, we show a ZULF NMR spectrum of [2-C-13]pyruvic acid hyperpolarized via dissolution dynamic nuclear polarization (dDNP). We foresee applications of affordable and scalable ZULF NMR coupled with hyperpolarization to study chemical exchange phenomena in vivo and in situations where high-field NMR detection is not possible to implement.