SUPPORTING INFORMATION

Table S1. Chemometrics and curve-fitting data for the FTIR-spectra of the UO2(NO3)2.3H2O and UO2(NO3)2.6H2O within 3500–3000 cm-1 region (Fig. S1).

UO2(NO3)2.6H2O / UO2(NO3)2.3H2O
xc1 / 3583.11 / ±1.39 / 3582.20 / ±1.77
A1 / 5.26 / ±1.72 / 1.66 / ±1.01
xc2 / 3502.49 / ±3.22
A2 / 1.41 / ±3.51
xc3 / 3527.61 / ±0.88 / 3446.67 / ±0.21
A3 / 3.28 / ±1.12 / 1.47 / ±2.21
xc4 / 3469.85 / ±0.03 / 3352.49 / ±1.35
A4 / 25.75 / ±1.67 / 3.68 / ±2.77
xc5 / 3409.65 / ±1.52 / 3282.59 / ±3.15
A5 / 34.04 / ±1.46 / 1.83 / ±3.56
xc6 / 3287.06 / ±0.31 / 3188.86 / ±3.22
A6 / 7.23 / ±5.05 / 4.97 / ±0.44
xc7 / 3237.42 / ±2.11
A7 / 12.13 / ±0.94
c2/DoF / 7.32.10-6 / 1.09.10-6
r2 / 0.99932 / 0.99362


Table S2. Thermodynamics of the studied complexes of uranyl ion.

UO2(NO3)2.3H2O / UO2(NO3)2.6H2O / UO3 / C≣U=O
ETS / -545.82 / -535.30 / -699.71 / -584.03
DEUPSS / -53776.61 / -37956.89 / -2426.70 / -7044.60
DEPSS / -45577.90 / -34682.32 / -2435.48 / -7398.42
DESP / -164.52 / -23401.60 / 4.75 / 218.91
DET / -45742.42 / -58083.92 / -2430.73 / -7179.51
DED / -20.69 / -20.82 / -8.45 / -6.84
DER / 4.37 / 4.36 / 3.77 / 6.33
DETNS / 12.01 / 11.56 / 3.63 / 6.86
DG / -45730.42 / -58072.36 / -2427.10 / -7172.65

ETS – total free energy in solution [a.u.]; DEUPSS – Unpolar solute/Solvent interaction energy [kcal.mol-1]; DEPSS – Polar solute/Solvent interaction energy [kcal.mol-1]; DESP – solute polarization energy [kcal.mol-1]; DET – Total electrostatic energy [kcal.mol-1]; DED – Dispersion energy [kcal.mol-1]; DER – Repulsion energy [kcal.mol-1]; DETNS – Total nonelectrostatic energy [kcal.mol-1]; DG – free Gibbs energy [kcal.mol-1].


Table S3. Chemometrics and curve-fitting data for the IR-spectra of the binary mixtures of UO2(NO3)2.3H2O and UO2(NO3)2.6H2O within 750–650 cm-1 region (Fig. 1).

xc1 / 722.53 / ±0.12 / 722.50 / ±0.11 / 722.46 / ±0.10 / 722.47 / ±0.10 / 722.45 / ±0.10
A1 / 0.74 / ±0.01 / 1.06 / ±0.01 / 1.30 / ±0.02 / 1.63 / ±0.02 / 1.90 / ±0.03
xc2 / 740.83 / ±0.43247 / 740.03 / ±0.51 / 739.65 / ±0.45 / 739.55 / ±0.53 / 739.23 / ±0.52
A2 / 0.31 / ±0.04 / 0.27 / ±0.01 / 0.23 / ±0.04 / 0.25 / ±0.05 / 0.23 / ±0.04
xc3 / 750.65 / ±0.56 / 750.10 / ±0.42 / 750.01 / ±0.29 / 750.11 / ±0.26 / 750.09 / ±0.21
A3 / 0.33 / ±0.03 / 0.61 / ±0.05 / 0.83 / ±0.04 / 1.03 / ±0.05 / 1.25 / ±0.05
xc4 / 772.67 / ±1.54 / 772.31 / ±1.12 / 771.97 / ±0.08 / 772.22 / ±1.07 / 772.64 / ±0.11
A4 / 0.02 / ±0.01 / 0.075 / ±0.01 / 0.10 / ±0.02 / 0.10 / ±0.02
c2/DoF / 2.73.10-6 / 5.65.10-6 / 7.73.10-6 / 0.00001 / 0.00002
r2 / 0.99144 / 0.99104 / 0.99242 / 0.99242 / 0.99192

Figure S1. Solid-state FT-IR spectra of the UO2(NO3)2.3H2O and UO2(NO3)2.6H2O in nujol within 4000–400 cm-1 region; The spectrum of nujol matrix; Curve-fitted patterns within 3500–3000 cm-1 region.


Theoretical data for C≣U(OH)+

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------VARIATIONAL PCM RESULTS ------

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<Psi(0)| H |Psi(0)> (a.u.) = -469.865969

<Psi(0)|H+V(0)/2|Psi(0)> (a.u.) = -472.832276

<Psi(0)|H+V(f)/2|Psi(0)> (a.u.) = -471.653961

<Psi(f)| H |Psi(f)> (a.u.) = -465.978375

<Psi(f)|H+V(f)/2|Psi(f)> (a.u.) = -467.708711

Total free energy in sol.

(with non electrost.terms) (a.u.) = -467.700267

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(Unpol.Solute)-Solvent (kcal/mol) = -1861.39

(Polar.Solute)-Solvent (kcal/mol) = -1085.80

Solute Polarization (kcal/mol) = 2439.50

Total Electrostatic (kcal/mol) = 1353.70

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Cavitation energy (kcal/mol) = 9.14

Dispersion energy (kcal/mol) = -5.75

Repulsion energy (kcal/mol) = 1.90

Total non electr. (kcal/mol) = 5.30

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DeltaG (solv) (kcal/mol) = 1359.00

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Theoretical data for HC≡U=O+

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------VARIATIONAL PCM RESULTS ------

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<Psi(0)| H |Psi(0)> (a.u.) = -586.373774

<Psi(0)|H+V(0)/2|Psi(0)> (a.u.) = -588.914798

<Psi(0)|H+V(f)/2|Psi(0)> (a.u.) = -588.895511

<Psi(f)| H |Psi(f)> (a.u.) = -586.351415

<Psi(f)|H+V(f)/2|Psi(f)> (a.u.) = -588.903954

Total free energy in sol.

(with non electrost.terms) (a.u.) = -588.895995

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(Unpol.Solute)-Solvent (kcal/mol) = -1594.52

(Polar.Solute)-Solvent (kcal/mol) = -1601.74

Solute Polarization (kcal/mol) = 14.03

Total Electrostatic (kcal/mol) = -1587.71

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Cavitation energy (kcal/mol) = 8.85

Dispersion energy (kcal/mol) = -6.02

Repulsion energy (kcal/mol) = 2.17

Total non electr. (kcal/mol) = 4.99

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DeltaG (solv) (kcal/mol) = -1582.72

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