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Hyperpolarizing Small Molecules using Parahydrogen and Solid-State Spin Diffusion
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DOI：10.1002/anie.202319341.png)
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Abstract
En 中文
Parahydrogen-induced polarization (PHIP) is an inexpensive way to produce hyperpolarized molecules with polarization levels of >10 % in the solution-state, but is strongly limited in generality since it requires chemical reactions/ interactions with H-2. Here we report a new method to widen the scope of PHIP hyperpolarization: a source molecule is produced via PHIP with high C-13 polarization, and precipitated out of solution together with a target species. Spin diffusion within the solid carries the polarization onto( 13)C spins of the target, which can then be dissolved for solution-state applications. We name this method PHIP-SSD (PHIP with solid-state spin diffusion) and demonstrate it using PHIP-polarized [1-C-13]-fumarate as the source molecule, to polarize different 13C-labelled target molecules. C-13 polarizations of between 0.01 and 3 % were measured on [1-C-13]-benzoic acid, depending on the molar ratio of fumarate:benzoate in the solid state. We also show that PHIP-SSD does not require specific co-crystallization conditions by grinding dry powders of target molecules together with solid fumarate crystals, and obtain C-13 signal enhancements of between 100 and 200 on [C-13,N-15(2)]-urea, [1-C-13]-pyruvate, and [1-C-13]-benzoic acid. This approach appears to be a promising new strategy for facile hyperpolarization based on PHIP.
Keywords:
hyperpolarization
NMR
parahydrogen
spin diffusion
Journal
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16.9
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5.6W
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53.0W