Cobalt-Catalyzed Hyperpolarization of Structurally Intact Olefins
Cobalt-Catalyzed Hyperpolarization of Structurally Intact Olefins
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DOI：
10.1021/acscatal.0c03727
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发表时间：
2021-02-01
期刊：
影响因子：
12.9
通讯作者：
Fout, Alison R.
中科院分区：
文献类型：
--
作者：
Muhammad, Safiyah R.;Greer, Rianna B.;Fout, Alison R.
通过可逆交换的信号放大（SABRE）是一种工具，其通过仲氢和所选的含氮/氧/硫底物之间的非氢化相互作用产生超极化物质，传统上使用铱催化剂。这一领域的发展已经允许扩大的基板范围，适用于超极化的应用，包括磁共振成像。在这里，我们报告了利用钴基催化剂的超极化结构完整的烯烃通过SABRE-like机制。各种烯烃底物的超极化表现出使用NMR光谱，并产生信号增强值高达类似150倍的H-1共振在14.1 T。极化转移到C-13（近150倍）和F-19证明没有使用同位素标记或射频脉冲序列的应用程序，使用和不使用微特斯拉领域。这些结果证明并提供了对第一第一行过渡金属催化剂平台的进一步了解，该第一第一行过渡金属催化剂平台能够促进在铱SABRE化学中传统上未观察到的结构完整的底物的显著信号增强。
Signal amplification by reversible exchange (SABRE) is a tool that generates hyperpolarized species via non-hydrogenative interactions between parahydrogen and selected nitrogen-/oxygen-/sulfur-containing substrates, traditionally with an iridium catalyst. The development of this field has allowed for a broadened substrate range amenable to hyperpolarization for applications including magnetic resonance imaging. Herein, we report the utilization of a cobalt-based catalyst for the hyperpolarization of structurally intact olefins via a SABRE-like mechanism. The hyperpolarization of a variety of olefinic substrates is exhibited using NMR spectroscopy and yields signal enhancement values of up to similar to 150-fold for H-1 resonances at 14.1 T. Transfer of polarization to C-13 (nearly 150-fold) and F-19 is demonstrated without the use of isotopic labeling or the application of radio-frequency pulse sequences, both with and without the use of microtesla fields. These results demonstrate and provide further insights into the first first-row transition metal catalyst platform capable of facilitating the dramatic signal enhancement of structurally intact substrates not traditionally observed with iridium SABRE chemistry.