Fluorous and organic extraction systems; A Comparison from the perspectives of coordination structures, interfaces, and bulk extraction phases

Ueda, Yuki; Micheau, C.; Akutsu, Kazuhiro*; Tokunaga, Kohei; Yamada, Masako*; Yamada, Norifumi*; Bourgeois, D.*; Motokawa, Ryuhei

Langmuir, 40(46), p.24257 - 24271, 2024/11

https://doi.org/10.1021/acs.langmuir.4c02268

Microscopic structures in liquid-liquid extraction, such as structuration between extractants or extracted complexes in bulk organic phases and at interfaces, can influence macroscopic phenomena, such as the distribution behavior of solutes, including extraction efficiency, selectivity, and phase separation of the organic phase. In this study, we correlated the macroscopic behavior of the extraction of Zr(IV) ions from nitric acid solutions with microscopic structural information in order to understand at the molecular level the key factors contributing to the higher metal ion extraction performance in the fluorous extraction system comprising fluorous phosphate (TFP) in perfluorohexane as compared to the analogous organic extraction system comprising organic phosphate (THP) in n-hexane. Extended X-ray absorption fine structure, neutron reflectometry, and small-angle neutron scattering revealed the local coordination structure around the Zr(IV) ion, the accumulation of extractant molecules at the interface, and the structuration of extractant molecules in the bulk extraction phase, respectively. In the fluorous extraction system, extractant aggregates with were formed after contact with nitric acid. In contrast, in the organic extraction system, only extractant dimers were formed. We speculate that differences in the local coordination structure around the Zr(IV) ion and the structuration of the extractant molecules in the bulk extraction phase contribute to the high Zr(IV) extraction performance in the fluorous extraction system. In particular, the size of the aggregates hardly changed with increasing Zr(IV) concentration in the fluorous phase, which may be closely related to the absence of phase splitting in the fluorous extraction system.

Organization of malonamides from the interface to the organic bulk phase

Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Akutsu, Kazuhiro*; Yamada, Norifumi*; Yamada, Masako*; Moussaoui, S. A.*; Makombe, E.*; Meyer, D.*; Berthon, L.*; et al.

Journal of Molecular Liquids, 401, p.124372_1 - 124372_12, 2024/05

https://doi.org/10.1016/j.molliq.2024.124372

Foam flotation of clay particles using a bifunctional amine surfactant

Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Bauduin, P.*; Girard, L.*; Diat, O.*

Langmuir, 39(31), p.10965 - 10977, 2023/07

https://doi.org/10.1021/acs.langmuir.3c01213

Small-angle neutron scattering study; Nanostructure of emulsion droplets

Ueda, Yuki; Micheau, C.; Nagano, Tetsushi*; Motokawa, Ryuhei

no journal, , 

no abstracts in English

Small-angle neutron scattering diffractometer SANS-J for nuclear separation chemistry

Motokawa, Ryuhei; Ueda, Yuki; Micheau, C.; Bourgeois, D.*; Dourdain, S.*; Diat, O.*

no journal, , 

Flotation process using pH-sensitive surfactant; From foam structure to extraction efficiency

Micheau, C.; Motokawa, Ryuhei; Ueda, Yuki; Bauduin, P.*; Diat, O.*; Girard, L.*

no journal, , 

Deuterated malonamide synthesis to probe interfacial mechanisms involved in solvent extraction process

Micheau, C.; Ueda, Yuki; Motokawa, Ryuhei; Akutsu, Kazuhiro*

no journal, , 

Differences in extraction mechanisms between fluorous and organic extraction systems; Structuring extractants at the interface and in the bulk extracting phase

Ueda, Yuki; Micheau, C.; Motokawa, Ryuhei; Tokunaga, Kohei; Akutsu, Kazuhiro*; Yamada, Norifumi*

no journal, , 

no abstracts in English

Small-angle neutron scattering for nanostructural analysis in solvent extraction systems

Motokawa, Ryuhei; Ueda, Yuki; Micheau, C.

no journal, , 

no abstracts in English