The determination of the thermodynamic constants of MgUO2(CO3)32−complex in NaClO4and NaCl media by time-resolved luminescence spectroscopy, and applications in different geochemical contexts
| Autor: | Pascal E. Reiller, Chengming Shang |
|---|---|
| Přispěvatelé: | Service d'études analytiques et de réactivité des surfaces (SEARS), Département de Physico-Chimie (DPC), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay, Laboratoire de développement Analytique Nucléaire Isotopique et Elémentaire (LANIE), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université Paris-Saclay-Département de Physico-Chimie (DPC) |
| Rok vydání: | 2021 |
| Předmět: |
Quenching (fluorescence)
Chemistry Analytical chemistry 010501 environmental sciences 010402 general chemistry 01 natural sciences Concentration ratio 0104 chemical sciences Ion Inorganic Chemistry Specific ion interaction theory [SDU.STU.GC]Sciences of the Universe [physics]/Earth Sciences/Geochemistry Stability constants of complexes Ionic strength [CHIM.COOR]Chemical Sciences/Coordination chemistry Luminescence Spectroscopy ComputingMilieux_MISCELLANEOUS 0105 earth and related environmental sciences |
| Zdroj: | Dalton Transactions Dalton Transactions, 2021, 50 (12), pp.4363-4379. ⟨10.1039/d0dt04124f⟩ Dalton Transactions, Royal Society of Chemistry, 2021, 50 (12), pp.4363-4379. ⟨10.1039/d0dt04124f⟩ |
| ISSN: | 1477-9234 1477-9226 |
| DOI: | 10.1039/d0dt04124f |
| Popis: | The formation constants and specific ion interaction coefficients of MgUO2(CO3)32− complex were determined in 0.1 to 1.0 mol kgw−1 NaCl and 0.10 to 2.21 mol kgw−1 NaClO4 media in the framework of the specific ion interaction theory (SIT), by time-resolved laser-induced luminescence spectroscopy. The upper limits of ionic strength were chosen in order to limit luminescence quenching effects generated by high concentrations of Cl− and ClO4− already observed during our earlier studies on CanUO2(CO3)3(4−2n)− complexes (Shang & Reiller, Dalton Trans., 49, 466; Shang et al., Dalton Trans., 49, 15443). The cumulative formation constant determined is , and the specific ion interaction coefficients are e(MgUO2(CO3)32−, Na+) = 0.19 ± 0.11 kgw mol−1 in NaClO4 and e(MgUO2(CO3)32−, Na+) = 0.09 ± 0.16 kgw mol−1 in NaCl. Two gratings of 300 and 1800 lines per mm were used to acquire MgUO2(CO3)32− luminescence spectra, where the high-resolution 1800 lines per mm grating detected slight spectral shifts for the principal luminescent bands relative to CanUO2(CO3)3(4−2n)−. The applications of the consistent set of thermodynamic constants and e values for MnUO2(CO3)3(4−2n)− (M = Mg and Ca) were examined in different geochemical contexts, where Mg over Ca concentration ratio varies to help defining the relative importance of these species. |
| Databáze: | OpenAIRE |
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