Combining fast magic angle spinning dynamic nuclear polarization with indirect detection to further enhance the sensitivity of solid-state NMR spectroscopy

IF 1.8 3区 化学 Q4 CHEMISTRY, PHYSICAL Solid state nuclear magnetic resonance Pub Date : 2020-10-01 DOI:10.1016/j.ssnmr.2020.101685
Zhuoran Wang , Michael P. Hanrahan , Takeshi Kobayashi , Frédéric A. Perras , Yunhua Chen , Frank Engelke , Christian Reiter , Armin Purea , Aaron J. Rossini , Marek Pruski
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引用次数: 17

Abstract

Dynamic nuclear polarization (DNP) and indirect detection are two commonly applied approaches for enhancing the sensitivity of solid-state NMR spectroscopy. However, their use in tandem has not yet been investigated. With the advent of low-temperature fast magic angle spinning (MAS) probes with 1.3-mm diameter rotors capable of MAS at 40 ​kHz it becomes feasible to combine these two techniques. In this study, we performed DNP-enhanced 2D indirectly detected heteronuclear correlation (idHETCOR) experiments on 13C, 15N, 113Cd and 89Y nuclei in functionalized mesoporous silica, CdS nanoparticles, and Y2O3 nanoparticles. The sensitivity of the 2D idHETCOR experiments was compared with those of DNP-enhanced directly-detected 1D cross polarization (CP) and 2D HETCOR experiments performed with a standard 3.2-mm rotor. Due to low CP polarization transfer efficiencies and large proton linewidth, the sensitivity gains achieved by indirect detection alone were lower than in conventional (non-DNP) experiments. Nevertheless, despite the smaller sample volume the 2D idHETCOR experiments showed better absolute sensitivities than 2D HETCOR experiments for nuclei with the lowest gyromagnetic ratios. For 89Y, 2D idHETCOR provided 8.2 times better sensitivity than the 1 D89Y-detected CP experiment performed with a 3.2-mm rotor.

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将快速魔角自旋动态核极化与间接探测相结合,进一步提高固态核磁共振光谱的灵敏度
动态核极化(DNP)和间接探测是提高固体核磁共振光谱灵敏度的两种常用方法。然而,它们的串联使用尚未进行研究。随着具有直径1.3 mm转子的低温快速魔角纺丝(MAS)探头的出现,使这两种技术的结合成为可能。在本研究中,我们对功能化介孔二氧化硅、CdS纳米粒子和Y2O3纳米粒子中的13C、15N、113Cd和89Y核进行了dnp增强的2D间接检测异核相关(idHETCOR)实验。将二维idHETCOR实验的灵敏度与dnp增强直接检测1D交叉偏振(CP)和使用标准3.2 mm转子进行的二维HETCOR实验进行了比较。由于CP极化传递效率低和质子线宽大,间接检测获得的灵敏度增益低于常规(非dnp)实验。然而,尽管样品体积较小,但二维idHETCOR实验对最低回旋磁比的原子核的绝对灵敏度优于二维HETCOR实验。对于89Y, 2D idHETCOR的灵敏度比使用3.2 mm转子进行的1 d89y检测的CP实验高8.2倍。
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来源期刊
CiteScore
5.30
自引率
9.40%
发文量
42
审稿时长
72 days
期刊介绍: The journal Solid State Nuclear Magnetic Resonance publishes original manuscripts of high scientific quality dealing with all experimental and theoretical aspects of solid state NMR. This includes advances in instrumentation, development of new experimental techniques and methodology, new theoretical insights, new data processing and simulation methods, and original applications of established or novel methods to scientific problems.
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