A comparative study of the complexation of Np(V) with N,N-dimethyl-3-oxa-glutaramic acid and related ligands: thermodynamics, optical properties and structural aspects

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Complexation of Np(V) with N,N-dimethyl-3-oxa-glutaramic acid (DMOGA) was studied in comparison with its diamide analog, N,N,N{prime},N{prime}-tetramethyl-3-oxa-glutaramide (TMOGA), and dicarboxylate analog, oxydiacetic acid (ODA). Thermodynamic parameters, including the stability constant and the enthalpy of complexation, were determined by spectrophotometry and calorimetry. Single-crystal structure of NpO{sub 2}(H{sub 2}O)(DMOGA){center_dot}H{sub 2}O(c) was identified by X-ray diffractometry using synchrotron radiation. Like ODA and TMOGA, DMOGA forms a tridentate Np(V) complex, with three oxygen atoms coordinating to the linear NpO{sub 2}{sup +} moiety via the equatorial plane. The stability constants, enthalpy and entropy of complexation generally decrease in the order ODA > DMOGA > TMOGA, suggesting ... continued below

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Rao, Linfeng; Tian, Guoxin & Teat, Simon J. March 29, 2010.

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Complexation of Np(V) with N,N-dimethyl-3-oxa-glutaramic acid (DMOGA) was studied in comparison with its diamide analog, N,N,N{prime},N{prime}-tetramethyl-3-oxa-glutaramide (TMOGA), and dicarboxylate analog, oxydiacetic acid (ODA). Thermodynamic parameters, including the stability constant and the enthalpy of complexation, were determined by spectrophotometry and calorimetry. Single-crystal structure of NpO{sub 2}(H{sub 2}O)(DMOGA){center_dot}H{sub 2}O(c) was identified by X-ray diffractometry using synchrotron radiation. Like ODA and TMOGA, DMOGA forms a tridentate Np(V) complex, with three oxygen atoms coordinating to the linear NpO{sub 2}{sup +} moiety via the equatorial plane. The stability constants, enthalpy and entropy of complexation generally decrease in the order ODA > DMOGA > TMOGA, suggesting that the complexation is entropy driven and the substitution of a carboxylate group with an amide group reduces the strength of complexation with Np(V) due to the decrease in the entropy of complexation.

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3326

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  • Journal Name: Dalton Transactions; Journal Volume: 39; Journal Issue: 13

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  • Report No.: LBNL-3475E
  • Grant Number: DE-AC02-05CH11231
  • DOI: 10.1039/b922851a | External Link
  • Office of Scientific & Technical Information Report Number: 984351
  • Archival Resource Key: ark:/67531/metadc1014525

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  • March 29, 2010

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  • Oct. 14, 2017, 8:36 a.m.

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  • Oct. 17, 2017, 6:10 p.m.

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Rao, Linfeng; Tian, Guoxin & Teat, Simon J. A comparative study of the complexation of Np(V) with N,N-dimethyl-3-oxa-glutaramic acid and related ligands: thermodynamics, optical properties and structural aspects, article, March 29, 2010; Berkeley, California. (digital.library.unt.edu/ark:/67531/metadc1014525/: accessed October 17, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.