Lead-enhanced gas-phase stability of multiply charged EDTA anions: a combined experimental and theoretical study
文献类型：期刊论文
| 作者 | Liu, Chunxiao ; Ouyang, Yongzhong ; Jia, Bin ; Zhu, Zhiqiang ; Shi, Jianbo ; Chen, Huanwen |
| 刊名 | JOURNAL OF MASS SPECTROMETRY
 |
| 出版日期 | 2012 |
| 卷号 | 47期号:6页码:769－777 |
| 关键词 | multiply charged anions EDTA-Pb(II) complexes molecular capacitor gas-phase stability extractive electrospray ionization mass spectrometry |
| ISSN号 | 1076-5174 |
| 中文摘要 | 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. Copyright (C) 2012 John Wiley & Sons, Ltd. |
| WOS记录号 | WOS:000305528300012 |
| 公开日期 | 2014-11-04 |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/7717]  |
| 专题 | 生态环境研究中心_环境化学与生态毒理学国家重点实验室 |
| 推荐引用方式 GB/T 7714 | Liu, Chunxiao,Ouyang, Yongzhong,Jia, Bin,et al. Lead-enhanced gas-phase stability of multiply charged EDTA anions: a combined experimental and theoretical study[J]. JOURNAL OF MASS SPECTROMETRY,2012,47(6):769－777. |
| APA | Liu, Chunxiao,Ouyang, Yongzhong,Jia, Bin,Zhu, Zhiqiang,Shi, Jianbo,&Chen, Huanwen.(2012).Lead-enhanced gas-phase stability of multiply charged EDTA anions: a combined experimental and theoretical study.JOURNAL OF MASS SPECTROMETRY,47(6),769－777. |
| MLA | Liu, Chunxiao,et al."Lead-enhanced gas-phase stability of multiply charged EDTA anions: a combined experimental and theoretical study".JOURNAL OF MASS SPECTROMETRY 47.6(2012):769－777. |
入库方式： OAI收割
来源：生态环境研究中心
浏览0
下载0
收藏0
其他版本
除非特别说明，本系统中所有内容都受版权保护，并保留所有权利。