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Increasing the Negative Charge of a Macroanion in the Gas Phase via Sequential Charge Inversion Reactions

机译:通过顺序电荷转化反应增加气相中大阴离子的负电荷

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摘要

Protonated and deprotonated biological molecules in the gas phase play an important role in life sciences research. The structural information accessible from the ions is highly dependent upon their charge states. Therefore, it is desirable to develop means for increasing absolute charge states, particularly for ionization methods, such as MALDI, that yield relatively low charge ions. The work presented here demonstrates the formation of a doubly deprotonated polypeptide or oligonucleotide ion (dianion) from a singly deprotonated analogue via two sequential ion/ion proton-transfer reactions involving charge inversion. The high exoergicity and the large cross section arising from the long-range attractive Coulomb potential of ion/ion reactions make this process plausible. In this example, an overall efficiency of conversion of singly charged ions to doubly charged ions of roughly 8% for polypeptide was noted while lower efficiency (roughly 2%) observed with an oligonucleotide is likely due to a greater degree of neutralization. No other approach to increasing the net negative charge of an anion in the gas phase has as yet been reported.
机译:气相中质子化和去质子化的生物分子在生命科学研究中起着重要作用。从离子可访问的结构信息高度依赖于其电荷状态。因此,期望开发出用于增加绝对电荷态的装置,特别是用于产生相对低电荷离子的电离方法(例如MALDI)的装置。此处介绍的工作证明了通过两个依次进行的涉及电荷反转的离子/离子质子转移反应,由单个去质子化的类似物形成了一个双重去质子化的多肽或寡核苷酸离子(二价阴离子)。离子/离子反应的远距离吸引力库仑电势引起的高散热性和大横截面,使该过程合理。在该实施例中,注意到多肽的单电荷离子转化为双电荷离子的总效率约为8%,而寡核苷酸观察到的较低效率(约2%)可能是由于较高的中和度。迄今为止,还没有其他方法可以增加气相中阴离子的净负电荷。

著录项

  • 期刊名称 other
  • 作者

    Min He; Scott A. McLuckey;

  • 作者单位
  • 年(卷),期 -1(76),14
  • 年度 -1
  • 页码 4189–4192
  • 总页数 7
  • 原文格式 PDF
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