Spectrophotometry and Luminescence Spectroscopy of Acetohydroxamate Complexes of Trivalent Lanthanide and Actinide Ions

被引:0
作者
Sergei I. Sinkov
Gregory R. Choppin
Robin J. Taylor
机构
[1] Pacific Northwest National Laboratory,Department of Chemistry and Biochemistry
[2] Florida State University,Nexia Solutions
[3] British Technology Centre,undefined
[4] Sellafield,undefined
来源
Journal of Solution Chemistry | 2007年 / 36卷
关键词
Lanthanides; Actinides; Acetohydroxamic acid; Complexation; Optical absorbance spectroscopy; Time resolved luminescence spectroscopy; Hydration;
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中图分类号
学科分类号
摘要
The complexation chemistries of acetohydroxamic acid (HA) with the trivalent Eu, Tb and Cm ions have been probed by combinations of Optical Absorbance Spectroscopy (OAS), Time Resolved Laser Induced Fluorescence Spectroscopy (TRLIFS) and emission spectroscopy, with some rather unexpected trends being observed. The formation of four complexed species was established for all three metal cations by OAS. The magnitudes of the formation constants of the respective M(A)n3−n complexes suggested a much stronger binding efficiency of HA for the first two complexation steps than the third and fourth steps. Tb(III) and Eu(III) TRLIFS data both suggested a final octadentate tetrakis-hydroxamato complex in which the metal ion is close to being fully dehydrated. Step-wise dehydration of Tb(III) by successive ligands did not appear to proceed as expected for a bidentate ligand. Of the EuAn complexes, only the tetrakis species was found to luminesce, with HA causing an unusually strong quenching effect for all other Eu species. Cm(III) complexation appeared similar to the lanthanide analogs.
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页码:815 / 830
页数:15
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