化学学报 ›› 2009, Vol. 67 ›› Issue (12): 1331-1335. 上一篇    下一篇

研究论文

新化合物五氧化铀的电喷雾串联质谱法制备与表征

胡 斌a 陈焕文a,b 张 燮a 杨水平a 冯守华*,b

  

  1. (a东华理工大学应用化学系 抚州 344000)
    (b吉林大学化学学院 长春 130012)

  • 投稿日期:2008-07-24 修回日期:2008-11-13 发布日期:2009-06-28
  • 通讯作者: 冯守华

Preparation and Characterization of UO5 by Using Electrospray Ionization Tandem Mass Spectrometry

Hu, Bin a Chen, Huanwen a,b Zhang, Xie a Yang, Shuiping a Feng, Shouhua *,b   

  1. (a Department of Applied Chemistry, East China Institute of Technology, Fuzhou 344000)
    (b College of Chemistry, Jilin University, Changchun 130012)
  • Received:2008-07-24 Revised:2008-11-13 Published:2009-06-28
  • Contact: Feng, Shouhua

采用醋酸铀酰为原料在气相中制备了HOUO2OH负离子, 在一定条件下再与O2反应, 从而制备了UO5负离子, 并采用串联质谱法对UO5进行了表征, 考察了生成条件对制备UO5负离子的影响. 初步实验表明在不同能量作用下UO5负离子能释放出O2. 探讨了气相中负离子与分子反应生成UO5负离子的可能机理, 指出通过调控分子与离子的碰撞时间和碰撞能量可以控制离子的电子活动半径, 合适的能量可使电子云的半径落在rinert≤rReactiverreactive≤rdecomposition之间, 从而促进某些化学反应的进行, 以合成某些通常状况下难以生成的物质.

关键词: 串联质谱, UO5, 反应时间, 碰撞能量, 气相反应, 醋酸铀酰

Negatively charged organic uranyl species (HOUO2OH), prepared with uranyl acetate using electrospray ionization multiple-stage tandem mass spectrometry, was reacted with oxygen to yield a novel UO5 anion species in the gas phase. The molecular structure of UO5 was confirmed by using collision-induced dissociation (CID) mass spectrometry experiments. The effects of experimental parameters on the yield of UO5 anion were experimentally evaluated. Upon gas phase collisions, UO5 anions released oxygen when a certain amount of energy was deposited on the UO5 anions. The data have shown that the electron cloud radius (r) of the polyatom anion (e.g. HOUO2OH) was tunable within the range rinert≤rreactive≤rdecomposition by changing the collision energy of CID. This mechanism can be further used to catalyze a certain type of chemical reactions.

Key words: ESI tandem mass spectrometry, UO5, reaction time, collision energy, gas-phase reaction, uranyl acetate