Barnett Institute of Chemical and Biological Analysis, ‡Department of Pharmaceutical Sciences in the Bouve College of Health Sciences, and §Department of Chemistry and Chemical Biology, Northeastern University , Boston, Massachusetts 02115, United States.
Chem Res Toxicol. 2013 Oct 21;26(10):1424-9. doi: 10.1021/tx400051j. Epub 2013 Oct 8.
We investigate the limit of detection for obtaining NMR data of a DNA adduct using modern microscale NMR instrumentation, once the adduct has been isolated at the picomole level. Eighty nanograms (130 pmol) of a DNA adduct standard, N-(2'-deoxyguanosin-8-yl)-2-acetylaminofluorene 5'-monophosphate (AAF-dGMP), in 1.5 μL of D₂O with 10% methanol-d₄, in a vial, was completely picked up as a droplet suspended in a fluorocarbon liquid and loaded efficiently into a microcoil probe. This work demonstrates a practical manual method of droplet microfluidic sample loading, previously demonstrated using automated equipment, which provides a severalfold advantage over conventional flow injection. Eliminating dilution during injection and confining the sample to the observed volume produce the full theoretical mass sensitivity of a microcoil, comparable to that of a microcryo probe. With 80 ng, an NMR spectrum acquired over 40 h showed all of the resonances seen in a standard spectrum of AAF-dGMP, with a signal-to-noise ratio of at least 10, despite broadening due to previously noted effects of conformational exchange. Even with this broadening to 5 Hz, a two-dimensional total correlation spectroscopy spectrum was acquired on 1.6 μg in 18 h. This work helps to define the utility of NMR in combination with other analytical methods for the structural characterization of a small amount of a DNA adduct.
我们研究了在分离出皮摩尔级别的 DNA 加合物后,使用现代微量 NMR 仪器获取 NMR 数据的检测极限。将 80 纳克(130 皮摩尔)的 DNA 加合物标准品 N-(2'-脱氧鸟嘌呤-8-基)-2-乙酰氨基氟苯 5'-单磷酸(AAF-dGMP)置于 1.5 μL 的 D₂O 中,其中含有 10%甲醇-d₄,置于小瓶中,然后将其完全作为悬浮在氟碳液体中的液滴提取出来,并高效地装入微线圈探头中。这项工作展示了一种实用的手动液滴微流控样品加载方法,该方法之前已经使用自动化设备进行了演示,与传统的流动注射相比,它具有数倍的优势。在注入过程中消除稀释并将样品限制在观察到的体积内,可以产生微线圈的全部理论质量灵敏度,与微晶探头相当。使用 80 ng,在 40 h 内获得的 NMR 光谱显示了 AAF-dGMP 标准光谱中所有可见的共振,信噪比至少为 10,尽管由于先前注意到的构象交换的影响而存在展宽。即使展宽到 5 Hz,也可以在 18 h 内获得 1.6 μg 的二维全相关光谱。这项工作有助于定义 NMR 与其他分析方法结合使用,以对少量 DNA 加合物进行结构表征的用途。