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通过动态共价键实现甲醇中可交换质子的SABRE超极化

SABRE Hyperpolarization of Exchangeable Protons in Methanol- through Dynamic Covalent Bonds.

作者信息

Zhan Xiao, Guo Zhanhong, Sun Huijun, Dai Anran, Zhang Min, Cui Xiaohong, Wang Xinchang, Tian Zhongqun, Chen Zhong

机构信息

School of Electronic Science and Engineering, Fujian Provincial Key Laboratory of Plasma and Magnetic Resonance, Xiamen University, Xiamen 361005, China.

State Key Laboratory for Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.

出版信息

Anal Chem. 2023 Aug 8;95(31):11613-11620. doi: 10.1021/acs.analchem.3c01049. Epub 2023 Jul 24.

Abstract

Utilizing -hydrogen (-H)-induced hyperpolarization to increase the sensitivity of nuclear magnetic resonance, especially signal amplification by reversible exchange (SABRE), has been widely studied. Here, we achieved hyperpolarization of exchangeable protons in methanol- by introducing dynamic covalent bonds as reversible exchange following the SABRE process. To release the hyperpolarized CDOH, the pyridine-based ligands with aldehyde groups underwent acetal exchange between the aldehyde and hydroxyl groups of CDOH after being first hyperpolarized by SABRE. Our mechanistic study highlights the importance of the reversible exchange of functional groups and chemical kinetics in realizing hyperpolarization of exchangeable protons in methanol-. Our work broadens SABRE's chemical system compatibility and possible applications.

摘要

利用氢(-H)诱导的超极化来提高核磁共振的灵敏度,特别是通过可逆交换进行信号放大(SABRE),已经得到了广泛研究。在这里,我们通过引入动态共价键作为SABRE过程后的可逆交换,实现了甲醇中可交换质子的超极化。为了释放超极化的CDOH,带有醛基的吡啶基配体在首先通过SABRE进行超极化后,在CDOH的醛基和羟基之间进行了缩醛交换。我们的机理研究突出了官能团的可逆交换和化学动力学在实现甲醇中可交换质子超极化方面的重要性。我们的工作拓宽了SABRE的化学体系兼容性和可能的应用范围。

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