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Visual and in situ Raman spectroscopic observations of the liquid-liquid immiscibility in aqueous uranyl sulfate solutions at temperatures up to 420 °C
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Liquidliquid immiscibility was observed in aqueous UO2SO4 solution at ≥285.8 ± 0.5 °C.

The immiscible liquids are either UO2SO4-rich (Urich) or UO2SO4-poor (Upoor).

Analyses of UO22+ and SO42− spectra imply increasing ion association upon heating.

Decrease of ion hydration in Urich phase due to increasing concentration upon heating.

Reversible strong UO22+–SO42− association results in the liquidliquid immiscibility.

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