Detection of nucleotides in positive-mode electrospray ionization mass spectrometry using multiply-charged cationic ion-pairing reagents

Detection of nucleotides in positive-mode electrospray ionization mass spectrometry using multiply-charged cationic ion-pairing reagents
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DOI:
10.1007/s00216-010-3949-4
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发表时间:
2010-09-01
影响因子:
4.3
通讯作者:
Armstrong, Daniel W.
Armstrong, Daniel W.
中科院分区:
化学2区
文献类型:
--
作者:
Dodbiba, Edra;Breitbach, Zachary S.;Armstrong, Daniel W.

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核苷酸是一类在生物系统中发挥重要作用的分子。开发了一种检测核苷酸的新方法。这些分子可以作为单体或低聚物和聚合物的成分存在。因此,它们带有一到几个负电荷。在本研究中,使用不同的阳离子离子对试剂与 28 种核苷酸单体和含核苷酸化合物中的每一种形成复合物。通过使用这种方法,这组离散的阴离子能够在正模式电喷雾电离质谱中作为带正电的复合物进行检测。还对在单离子监测(SIM)离子模式下表现最好的离子对试剂完成了串联质谱实验,并且大多数阴离子的灵敏度进一步降低。与正 SIM 模式相比,胸苷二磷酸等化合物的检测限提高了 100 倍,与负模式相比提高了 750 倍。在正离子模式下分析时,一些核苷酸没有表现出灵敏度的显着增加,但总的来说,本文开发的新方法比负离子模式下的传统检测具有更高的灵敏度。
Nucleotides are a class of molecules that play an essential role in biological systems. A new method has been developed in the detection of nucleotides. These molecules can exist as monomers or constituents of oligomers and polymers. As such, they carry from one to several negative charges. In this study, different cationic ion-pairing reagents were used to complex with each of the 28 nucleotide monomers and nucleotide containing compounds. By using this method, this discrete set of anions was able to be detected in the positive-mode electrospray ionization mass spectrometry, as positively charged complexes. Tandem mass spectrometry experiments were also completed on the ion-pairing reagents that performed the best in the single ion monitoring (SIM) ion mode, and the sensitivity was lowered even further for most of the anions. Limits of detection for compounds such as thymidine diphosphate were improved as much as 100 times compared to the positive SIM mode, and 750 times when compared to the negative mode. A few nucleotides did not show a significant increase in sensitivity when analyzed in the positive ion mode, but in general the new method developed herein resulted in a much greater sensitivity than traditional detection in the negative mode.