作者: Michael J. Van Stipdonk , Winnie Chien , Victor Anbalagan , Kellis Bulleigh , Dorothy Hanna
DOI: 10.1021/JP046565P
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摘要: We report here that electrospray ionization (ESI) of uranyl nitrate dissolved in a mixture H 2 O and acetone causes the formation doubly charged, gas-phase complexes containing UO + "solvated" by neutral ligands.Using mild conditions, dominant species observed ESI mass spectrum contained ion coordinated five ligands, consistent with proposed most-stable structures solution phase. However, chemical shift data, peak shapes, plot fractional abundance versus desolvation temperature suggest gas phase, under ion-trapping ejection conditions imposed, equatorial ligands are less stable than those four. Multiple-stage tandem spectrometry showed uranyl-acetone dissociate via elimination through pathways involve reactive collisions adventitious trap. At no point was complete removal to generate achieved. also used complex ions similar composition ligand number but different charge state for an investigation influence on tendency add association reactions. found addition fifth molecule initially four is more facile charged species. The singly shows significant back-reaction eliminate ligand, suggesting intrinsic difference preferred coordination U(VI) U(V)