高等学校化学学报

高等学校化学学报

• 研究论文 • 上一篇    下一篇

甲基羟基铀酰离子与水的复分解反应

胡斌1, 陈兰慧3, 郇延富2, 张燮1, 李明2, 梁华正1, 陈焕文1,2   

    1. 东华理工大学应用化学系, 抚州 344000;
    2. 吉林大学化学学院, 长春 130021;
    3. 东北师范大学化学学院功能材料研究所, 长春 130024
  • 收稿日期:2007-08-13 修回日期:1900-01-01 出版日期:2008-05-10 发布日期:2008-05-10
  • 通讯作者: 陈焕文

Metathetical Reaction of Organic Uranyl Species with Water in the Gas Phase

HU Bin1, CHEN Lan-Hui3, HUAN Yan-Fu2, ZHANG Xie1, LI Ming2, LIANG Hua-Zheng1, CHEN Huan-Wen1,2*   

    1. Department of Applied Chemistry, East China Institute of Technology Institution, Fuzhou 344000, China;
    2. College of Chemistry, Jilin University, Changchun 130021, China;
    3. Institute of Functional Material Chemistry, Faculty of Chemistry, Northeast Normal University, Changchun 130024, China
  • Received:2007-08-13 Revised:1900-01-01 Online:2008-05-10 Published:2008-05-10
  • Contact: CHEN Huan-Wen

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被引次数

9

摘要： 以醋酸铀酰为主要试剂, 在负离子检测模式下, 采用电喷雾串联质谱法制备了甲基羟基铀酰负离子. 实验发现, 气相中的甲基羟基铀酰离子与水分子发生分子离子复分解反应, 并用串联质谱法对反应产生的离子性产物进行了结构确认, 提出了反应的可能机理. 热力学计算结果表明, 该反应的ΔGReaction为-473.0 kJ/mol, ΔHReaction为-236.5 kJ/mol, ΔSSystem为0.792 kJ·mol-1·K-1. 该反应的速率常数为2.26 s-1.

关键词: 气相复分解反应, 醋酸铀酰, 电喷雾质谱, 碰撞诱导解离, 分子离子反应

Abstract: Negatively charged organic uranyl species(CH3UO2OH) was prepared and characterized with electrospray ionization tandem mass spectrometry implemented on an LTQ-MS instrument. Experimentally, it was found that ionic species of CH3UO2OH underwent metathetical reaction with water molecules present in the ion trap to produce negative ions of m/z 304 and a neutral methane species in the gas phase. The transient state of the reaction was observed and identified in the gas phase by tandem mass spectrometry. The mechanism was discussed in detail. The Gibbs free energy(ΔrG), enthalpy(ΔrH) and entropy(ΔrS) for the reaction were calculated, on the basis of the experimental measurements, to be -473.0 kJ/mol, -236.5 kJ/mol and 0.792 kJ·mol-1·K-1, respectively. The reaction rate constant was experimentally estimated to be 2.26 s-1.

Key words: Gas-phase metathesis, Uranyl acetate, Electrospray ionization, Collision-induced dissociation, Ion/molecule reaction

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