The coordination of uranyl in water: A combined quantum chemical and molecular simulation study
(2005) In Journal of the American Chemical Society 127(41). p.14250-14256- Abstract
- 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... (More)
- 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. (Less)
Please use this url to cite or link to this publication:
https://lup.lub.lu.se/record/152688
- author
- Hagberg, Daniel LU ; Karlström, Gunnar LU ; Roos, Björn LU and Gagliardi, L
- organization
- publishing date
- 2005
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Journal of the American Chemical Society
- volume
- 127
- issue
- 41
- pages
- 14250 - 14256
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- wos:000232605600048
- scopus:26844509303
- ISSN
- 1520-5126
- DOI
- 10.1021/ja0526719
- language
- English
- LU publication?
- yes
- additional info
- 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)
- id
- ff414b14-0467-46a1-b343-52f8064a8bb1 (old id 152688)
- date added to LUP
- 2016-04-01 16:34:02
- date last changed
- 2023-02-14 19:53:05
@article{ff414b14-0467-46a1-b343-52f8064a8bb1, abstract = {{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.}}, author = {{Hagberg, Daniel and Karlström, Gunnar and Roos, Björn and Gagliardi, L}}, issn = {{1520-5126}}, language = {{eng}}, number = {{41}}, pages = {{14250--14256}}, publisher = {{The American Chemical Society (ACS)}}, series = {{Journal of the American Chemical Society}}, title = {{The coordination of uranyl in water: A combined quantum chemical and molecular simulation study}}, url = {{http://dx.doi.org/10.1021/ja0526719}}, doi = {{10.1021/ja0526719}}, volume = {{127}}, year = {{2005}}, }