A QMCF-MD Investigation of the Structure and Dynamics of Ce4+ in Aqueous Solution
View Author Information
Theoretical Chemistry Division, Institute of General, Inorganic and Theoretical Chemistry, University of Innsbruck, Innrain 80-82, A-6020 Innsbruck, Austria
*E-mail: [email protected]. Tel.: +43-512-507-57102. Fax: +43-512-507-57199.
Abstract
A quantum-mechanical charge-field molecular dynamics simulation has been performed for a tetravalent Ce ion in aqueous solution. In this framework, the complete first and second hydration spheres are treated by ab initio quantum mechanics supplemented by an electrostatic embedding technique, making the construction of non-Coulombic solute–solvent potentials unnecessary. During the 10 ps of simulation time, the structural aspects of the solution were analyzed by various methods. Experimental results such as the mean Ce–O bond distance and the predicted first-shell coordination number were compared to the results obtained from the simulation resolving some ambiguities in the literature. The dynamics of the system were characterized by mean ligand residence times and frequency/force constant calculations. Furthermore, Ce–O and Ce–H angular radial distribution plots were employed, yielding deeper insight into the structural and dynamical aspects of the system.
Cited By
This article is cited by 22 publications.
- Cailin A. Buchanan, Eunbyeol Ko, Spencer Cira, Mahalingam Balasubramanian, Bryan R. Goldsmith, Nirala Singh. Structures and Free Energies of Cerium Ions in Acidic Electrolytes. Inorganic Chemistry 2020, 59
(17)
, 12552-12563. https://doi.org/10.1021/acs.inorgchem.0c01645
- Gökhan Elmaci, Carolin E. Frey, Philipp Kurz, and Birgül Zümreoğlu-Karan . Water Oxidation Catalysis by Birnessite@Iron Oxide Core–Shell Nanocomposites. Inorganic Chemistry 2015, 54
(6)
, 2734-2741. https://doi.org/10.1021/ic502908w
- Ali Kalaji, S. Skanthakumar, Mercouri G. Kanatzidis, John F. Mitchell, and L. Soderholm . Changing Hafnium Speciation in Aqueous Sulfate Solutions: A High-Energy X-ray Scattering Study. Inorganic Chemistry 2014, 53
(12)
, 6321-6328. https://doi.org/10.1021/ic500938k
- Oliver M. D. Lutz, Christoph B. Messner, Thomas S. Hofer, Matthias Glätzle, Christian W. Huck, Günther K. Bonn, and Bernd M. Rode . Combined Ab Initio Computational and Infrared Spectroscopic Study of the cis- and trans-Bis(glycinato)copper(II) Complexes in Aqueous Environment. The Journal of Physical Chemistry Letters 2013, 4
(9)
, 1502-1506. https://doi.org/10.1021/jz400288c
- Shiyu Hu, Donghui Wang, Rujia Guo, Feng Chen. Sulfur ligated oxoiron(IV) centre in fenton-like reaction: Theoretical postulation and experimental verification. Catalysis Communications 2022, 172 , 106536. https://doi.org/10.1016/j.catcom.2022.106536
- Wahyu Dita Saputri, Harno Dwi Pranowo, Manuel J. Schuler, Thomas S. Hofer. Cu
2+
in liquid ammonia—The impact of solvent flexibility and electron correlation in ab initio quantum mechanical charge field molecular dynamics. Journal of Computational Chemistry 2020, 41
(25)
, 2168-2176. https://doi.org/10.1002/jcc.26379
- Eléonor Acher, Michel Masella, Valérie Vallet, Florent Réal. Properties of the tetravalent actinide series in aqueous phase from a microscopic simulation self-consistent engine. Physical Chemistry Chemical Physics 2020, 22
(4)
, 2343-2350. https://doi.org/10.1039/C9CP04912F
- Wahyu Dita Saputri, Yuniawan Hidayat, Karna Wijaya, Harno Dwi Pranowo, Thomas S. Hofer. Investigation of the preferential solvation and dynamical properties of Cu+ in 18.6% aqueous ammonia solution using ab initio quantum mechanical charge field (QMCF) molecular dynamics and NBO analysis. Journal of Molecular Liquids 2019, 275 , 859-866. https://doi.org/10.1016/j.molliq.2018.11.022
- Shigang Shen, Xueru Chi, Jingran Dong, Shuying Huo, Hongwu Tian, Liyao Xu, Tiesheng Shi. Oxidation of the drug tiopronin by Cerium(IV) in perchloric acid media: Kinetic and mechanistic analyses. Journal of Molecular Liquids 2017, 246 , 1-6. https://doi.org/10.1016/j.molliq.2017.09.009
- Muhammad Saleh, Thomas S. Hofer. Structure and dynamics of Ni2+ in liquid ammonia: A quantum mechanical charge field molecular dynamics (QMCF-MD) study. Chemical Physics Letters 2016, 661 , 274-278. https://doi.org/10.1016/j.cplett.2016.09.002
- Zoel Codolà, Laura Gómez, Scott T. Kleespies, Lawrence Que Jr, Miquel Costas, Julio Lloret-Fillol. Evidence for an oxygen evolving iron–oxo–cerium intermediate in iron-catalysed water oxidation. Nature Communications 2015, 6
(1)
https://doi.org/10.1038/ncomms6865
- Lorenz R. Canaval, Peter P. Passler, Bernd M. Rode. The hydration properties of Gd(III) and Tb(III): An ab initio quantum mechanical molecular dynamics study. Chemical Physics Letters 2015, 625 , 116-120. https://doi.org/10.1016/j.cplett.2015.02.043
- Lorenz R. Canaval, Bernd M. Rode. The hydration properties of Eu(II) and Eu(III): An ab initio quantum mechanical molecular dynamics study. Chemical Physics Letters 2015, 618 , 78-82. https://doi.org/10.1016/j.cplett.2014.10.060
- Niko Prasetyo, Lorenz R. Canaval, Karna Wijaya, Ria Armunanto. Lithium(I) in liquid ammonia: A quantum mechanical charge field (QMCF) molecular dynamics simulation study. Chemical Physics Letters 2015, 619 , 158-162. https://doi.org/10.1016/j.cplett.2014.11.066
- Andreas O. Tirler, Thomas S. Hofer. Structure and Dynamics of the Uranyl Tricarbonate Complex in Aqueous Solution: Insights from Quantum Mechanical Charge Field Molecular Dynamics. The Journal of Physical Chemistry B 2014, 118
(45)
, 12938-12951. https://doi.org/10.1021/jp503171g
- Aya Matsuda, Hirotoshi Mori. Theoretical Study on the Hydration Structure of Divalent Radium Ion Using Fragment Molecular Orbital–Molecular Dynamics (FMO–MD) Simulation. Journal of Solution Chemistry 2014, 43
(9-10)
, 1669-1675. https://doi.org/10.1007/s10953-014-0235-7
- Oliver M.D. Lutz, Christoph B. Messner, Thomas S. Hofer, Lorenz R. Canaval, Guenther K. Bonn, Christian W. Huck. Computational Vibrational Spectroscopy of glycine in aqueous solution – Fundamental considerations towards feasible methodologies. Chemical Physics 2014, 435 , 21-28. https://doi.org/10.1016/j.chemphys.2014.03.003
- Lorenz R. Canaval, Alexander K.H. Weiss, Bernd M. Rode. Structure and dynamics of the Th4+-ion in aqueous solution – An ab initio QMCF-MD study. Computational and Theoretical Chemistry 2013, 1022 , 94-102. https://doi.org/10.1016/j.comptc.2013.08.020
- Manuel Hitzenberger, Thomas S. Hofer, Alexander K. H. Weiss. Solvation properties and behaviour of lutetium(III) in aqueous solution—A quantum mechanical charge field (QMCF) study. The Journal of Chemical Physics 2013, 139
(11)
https://doi.org/10.1063/1.4820879
- Syed Tarique Moin, Thomas S. Hofer, Alexander K. H. Weiss, Bernd M. Rode. Dynamics of ligand exchange mechanism at Cu(II) in water: An
ab initio
quantum mechanical charge field molecular dynamics study with extended quantum mechanical region. The Journal of Chemical Physics 2013, 139
(1)
https://doi.org/10.1063/1.4811114
- Simon A. Cotton. Scandium, yttrium, the lanthanides. Annual Reports Section "A" (Inorganic Chemistry) 2013, 109 , 208. https://doi.org/10.1039/c3ic90017g
- Philipp A. Pedevilla, Thomas S. Hofer, Bernhard R. Randolf, Bernd M. Rode. Simulation of Ir(III) in Aqueous Solution: The Most Inert Ion Hydrate. Australian Journal of Chemistry 2012, 65
(12)
, 1582. https://doi.org/10.1071/CH12303