• 主题
高级搜索  >
历史搜索 清空历史
首页> 外文期刊>Journal of mass spectrometry: JMS >Lead-enhanced gas-phase stability of multiply charged EDTA anions: a combined experimental and theoretical study
【24h】

Lead-enhanced gas-phase stability of multiply charged EDTA anions: a combined experimental and theoretical study

机译：多电荷EDTA阴离子的铅增强气相稳定性：结合实验和理论研究

获取原文
获取原文并翻译 | 示例
           
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

Besides their fundamental importance, multiply charged anions (MCAs) are considered as promising molecular capacitors for which their intrinsic stabilities are of great significance. Herein, the gas-phase stabilities of ethylenediaminetetraacetic acid (EDTA) anions (i.e. [EDTA-nH]n?, n?=?1-4) and their Pb(II) complexes (i.e. [EDTA?+?Pb-nH](2-n)?, n?=?3, 4) have been investigated using an approach that combines extractive electrospray ionization mass spectrometry (EESI-MS) measurements, Car-Parrinello molecular dynamics simulations and density functional theory/Tao-Perdew-Staroverov-Scuseria calculations. The EESI-MS data showed that the doubly charged EDTA anions in the form of [EDTA-2H]2? and [EDTA?+?Pb-4H]2? were much more abundantly observed than the singly charged species such as [EDTA-H]? and [EDTA?+?Pb-3H]?, respectively. The calculation results indicated that [EDTA-2H]2? and [EDTA?+?Pb-4H]2? anions were thermodynamically more stable than the [EDTA-H]? and [EDTA?+?Pb-3H]? species in the gas phase, respectively. The [EDTA?+?Pb-3H]? anions preferred five-coordinated structure, whereas [EDTA?+?Pb-4H]2? anions formed either five-coordinated or six-coordinated structures. The calculations further revealed that significant electron clouds drifting from the ligand EDTA to the metal Pb(II) ions and the large distances between the carboxylic groups reduced the Coulomb repulsion among the excess electrons of these MCAs. Our data demonstrated that EESI-MS combined with theoretic calculations were able to provide a deep insight into the fundamental behavior of stability of MCAs in the gas phase and, thus, might be useful tools for studying MCAs for potential molecular capacitors.
机译：除了它们的基本重要性外，多重电荷阴离子（MCA）还被认为是很有前途的分子电容器，其固有稳定性具有重要意义。此处，乙二胺四乙酸（EDTA）阴离子（即[EDTA-nH] n，n 2 ＝α1-4）及其Pb（II）配合物（即[EDTAα+αPb-nH]）的气相稳定性。 （2-n）?， n？=？3，4）已采用结合萃取电喷雾电离质谱（EESI-MS）测量，Car-Parrinello分子动力学模拟和密度泛函理论/ Tao-Perdew- Staroverov-Scuseria计算。 EESI-MS数据表明，双电荷的EDTA阴离子为[EDTA-2H] 2？和[EDTA ++ Pb-4H] 2？是否比[EDTA-H]等单电荷物种丰富得多？和[EDTA + + Pb-3H] 2。计算结果表明[EDTA-2H] 2≤2。和[EDTA ++ Pb-4H] 2？阴离子在热力学上比[EDTA-H]稳定。和[EDTA？+？Pb-3H]？在气相中的种类。 [EDTA ++ Pb-3H]？阴离子优选为五配位结构，而[EDTA + + Pb-4H] 2-为优选。阴离子形成五配位或六配位的结构。计算进一步表明，大量的电子云从配体EDTA漂移到金属Pb（II）离子，并且羧基之间的距离较大，从而降低了这些MCA多余电子之间的库仑排斥力。我们的数据表明，EESI-MS与理论计算相结合能够深入了解MCA在气相中的稳定性基本行为，因此，可能是研究潜在分子电容器MCA的有用工具。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱：kefu@zhangqiaokeyan.com

京公网安备：11010802029741号 ICP备案号：京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有

  • 客服微信

  • 服务号