Behaviour of complexes of f-elements in the environment - An experimental and theoretical analysis

作者：Ivanova Bojidarka^*; Spiteller Michael

来源：Journal of Molecular Structure, 2017, 1127: 199-211.

DOI：10.1016/j.molstruc.2016.07.101

• Lanthanides
• Actinides
• Sorption
• Minerals
• Environmental chemistry
• Mass spectrometry
• Quantum chemistry
• Aquatic systems

The paper provides a comprehensive study of lanthanide and actinide complexes to a matter of key area in the field of the chemistry, i.e. environmental analytical chemistry. The content has involved: (i) solution and sorption behaviour of lanthanides (Ln(n+), Ln = Ce, Pr, Nd, Pm, Sm, Eu, Gd, Tb, Py, Ho, Er, Tm, Yb and Lu) onto Y(O)O(H) minerals (Y = Fe, Mn or Si); (ii) ligand exchange processes with participation of inorganic OH-, F-, Cl-, Br-, SO42-, SO32-, IO3-, NO32-, CO32- and/or HCO3- ligands as well as mixed ligand complexes, including solvent molecules such as {[LnOR](2+)}, {[Ln(OR)(2)](+)} (R = CH3OH, CH3CH2CH2OH) and {[Ln(CH3CN)(x)(H2O)(z)](3+)} (x = 68, z = 04); (iii) the actinide speciation has involved different oxidation states (+4)(+6) and ions {[UOH](3+)}, {[UX](3+)} (X = F or Cl), {[UFx]y(+/-)} (x = 2-6, y = 0-2), {[U(CO3)(x)](y-)} (x = 4 or 5, y = 4 or 6), {[U(SO4)](2+)], {[U(NO3)](3+)}, {[U(NO3)(2)](2+)}, [[UO2(CO3)(3)](5-)}, {[(UO2)(x)(OH)(z)](y+/-)} (x = 1-4, y = 1 or 2, z = 1-7), {[UO2Fx](y+/-)} (x = 1-4, y = 1 or 2), {[UO2(CO3)(x)](y-)} (x = 2, or 3, y = 2, or 4), {[(UO2)(2)(CO3)(OH)(3)](-)}, {[(UO2)(3)O(OH)(2)(HCO3)](+)}, {[(UO2)(11)(CO3)(6)(OH)(12)](2-)}, {[UO2(SO4)(x)](y-)}, (x = 2 or 3, y = 2 or 4), {[UO2SiO(OH)(3)](+)}, {[AnC(x)](y+/-)} (x,y = 1 and 2), {[CAnH](+/-)}, {[C(x)Any](0)} (x,y = 2 and 3), {[AnH(x)](y+)} (x = 1-3, y = 0-5), {[AnX(n)](m+/-)} (n = 1-6, m = 1-4, X = F-, Br-, I-), {[AnO(x)F(z)](y+/-)} (x, z = 1 or 2, y = 0, 1 and 2), {[AnN(x)](y+)} (x = 1 and 2), {[An(x)O(z)(OH)(n)](y+/-)} (x = 1-3, z = 1-4, y = 0, 1 or 2, n = 0 or 1) and An(n+) (n = 0-6) at An = Th, Pa, U, Np, Pu, Am, Cm, Bk, Cf, Es, Fm, Md, No and Lr, respectively. Correlation analysis between thermodynamic parameters, accounting for different surface interactions of adsorbed species and experimental mass spectrometric data, including liquid, semi-liquid and solid-state measurements in a large set of experimental conditions such as pH = 2-13, low and intermediate ionic strength, solvent type, epsilon = 078.0, variety of solvent proton accepting and donating numbers and T = 25400 degrees C has carried out.

• 出版日期2017-1-5