The coordination of uranyl in water: A combined quantum chemical and molecular simulation study

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The coordination of uranyl in water: A combined quantum chemical and molecular simulation study. / Hagberg, Daniel; Karlström, Gunnar; Roos, Björn; Gagliardi, L.

I: Journal of the American Chemical Society, Vol. 127, Nr. 41, 2005, s. 14250-14256.

Forskningsoutput: TidskriftsbidragArtikel i vetenskaplig tidskrift

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TY - JOUR

T1 - The coordination of uranyl in water: A combined quantum chemical and molecular simulation study

AU - Hagberg, Daniel

AU - Karlström, Gunnar

AU - Roos, Björn

AU - Gagliardi, L

N1 - The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Theoretical Chemistry (S) (011001039)

PY - 2005

Y1 - 2005

N2 - The coordination environment of uranyl in water has been studied using a combined quantum mechanical and molecular dynamics approach. Multiconfigurational wave function calculations have been performed to generate pair potentials between uranyl and water. The quantum chemically determined energies have been used to fit parameters in a polarizable force field with an added charge transfer term. Molecular dynamics simulations have been performed for the uranyl ion and up to 400 water molecules. The results show a uranyl ion with five water molecules coordinated in the equatorial plane. The U-O(H2O) distance is 2.40 angstrom, which is close to the experimental estimates. A second coordination shell starts at about 4.7 angstrom from the uranium atom. No hydrogen bonding is found between the uranyl oxygens and water. Exchange of waters between the first and second solvation shell is found to occur through a path intermediate between association and interchange. This is the first fully ab initio determination of the solvation of the uranyl ion in water.

AB - The coordination environment of uranyl in water has been studied using a combined quantum mechanical and molecular dynamics approach. Multiconfigurational wave function calculations have been performed to generate pair potentials between uranyl and water. The quantum chemically determined energies have been used to fit parameters in a polarizable force field with an added charge transfer term. Molecular dynamics simulations have been performed for the uranyl ion and up to 400 water molecules. The results show a uranyl ion with five water molecules coordinated in the equatorial plane. The U-O(H2O) distance is 2.40 angstrom, which is close to the experimental estimates. A second coordination shell starts at about 4.7 angstrom from the uranium atom. No hydrogen bonding is found between the uranyl oxygens and water. Exchange of waters between the first and second solvation shell is found to occur through a path intermediate between association and interchange. This is the first fully ab initio determination of the solvation of the uranyl ion in water.

U2 - 10.1021/ja0526719

DO - 10.1021/ja0526719

M3 - Article

VL - 127

SP - 14250

EP - 14256

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

SN - 1520-5126

IS - 41

ER -