Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 26, Issue 63, Pages 14385-14396Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202001469
Keywords
electrochemistry; europium; ionic liquids; rare earths; UV; Vis spectroscopy
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Funding
- Commissariat a l'Energie Atomique et aux Energies Alternatives (CEA)
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Separation processes based on room temperature ionic liquids (RTIL) and electrochemical refining are promising strategies for the recovery of lanthanides from primary ores and electronic waste. However, they require the speciation of dissolved elements to be known with accuracy. In the present study, Eu coordination and Eu-III/Eu(II)electrochemical behavior as a function of water content in 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIm][NTf2]) was investigated using UV-visible spectrophotometry, time-resolved laser fluorescence spectroscopy, electrochemistry, and X-ray absorption spectroscopy.In situmeasurements were performed in spectroelectrochemical cells. Under anhydrous conditions, Eu(III)and Eu(II)were complexed by NTf2, forming Eu-O and Eu-(N,O) bonds with the anion sulfoxide function and N atoms, respectively. This complexation resulted in a greater stability of Eu-II, and in quasi-reversible oxidation-reduction with an E-0' potential of 0.18 V versus the ferrocenium/ferrocene (Fc(+)/Fc) couple. Upon increasing water content, progressive incorporation of water in the Eu(III)coordination sphere occurred. This led to reversible oxidation-reduction reactions, but also to a decrease in stability of the +II oxidation state (E-0'=-0.45 V vs. Fc(+)/Fc in RTIL containing 1300 mmwater).
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