Stern Quentin, Verhaeghe Guillaume, El Daraï Théo, Montarnal Damien, Huu Le Nghia, Veyre Laurent, Thieuleux Chloé, Bocquelet Charlotte, Cala Olivier, Jannin Sami
Université Claude Bernard Lyon 1, CRMN UMR-5082, CNRS, ENS Lyon, Villeurbanne, 69100, France.
Université de Lyon, Institut de Chimie de Lyon, Laboratory of Catalysis, Polymerization, Processes and Materials, CP2M UMR 5128 CNRS-UCB Lyon 1 CPE Lyon 43 Bd du 11 Novembre 1918, 69616, Villeurbanne, France.
Angew Chem Int Ed Engl. 2024 Dec 2;63(49):e202409510. doi: 10.1002/anie.202409510. Epub 2024 Oct 31.
The low sensitivity of liquid-state nuclear magnetic resonance (NMR) can be overcome by hyperpolarizing nuclear spins by dissolution dynamic nuclear polarization (dDNP). It consists of transferring the near-unity polarization of unpaired electron spins of stable radicals to the nuclear spins of interest at liquid helium temperatures, below 2 K, before melting the sample in view of hyperpolarized liquid-state magnetic resonance experiments. Reaching such a temperature is challenging and requires complex instrumentation, which impedes the deployment of dDNP. Here, we propose organic conductive polymers such as polyaniline (PANI) as a new class of polarizing matrices and report H polarizations of up to 5 %. We also show that C spins of a host solution impregnated in porous conductive polymers can be hyperpolarized by relayed DNP. Such conductive polymers can be synthesized as chiral and display current induced spin selectivity leading to electron spin hyperpolarization close to unity without the need for low temperatures nor high magnetic fields. Our results show the feasibility of solid-state DNP in conductive polymers that are known to exhibit chirality-induced spin selectivity.
通过溶解动态核极化(dDNP)使核自旋超极化,可以克服液态核磁共振(NMR)灵敏度低的问题。它包括在低于2K的液氦温度下,将稳定自由基未成对电子自旋的近乎完全极化转移到感兴趣的核自旋上,然后鉴于超极化液态磁共振实验将样品熔化。达到这样的温度具有挑战性,并且需要复杂的仪器设备,这阻碍了dDNP的应用。在此,我们提出聚苯胺(PANI)等有机导电聚合物作为一类新型的极化基质,并报告了高达5%的氢极化率。我们还表明,浸渍在多孔导电聚合物中的主体溶液的碳自旋可以通过中继DNP实现超极化。这种导电聚合物可以合成为手性的,并表现出电流诱导的自旋选择性,从而在无需低温和高磁场的情况下使电子自旋超极化接近完全极化。我们的结果表明,在已知表现出手性诱导自旋选择性的导电聚合物中进行固态DNP是可行的。