* Corresponding Author
Investigation of the Structural and Dynamical Properties of Cu+ in Liquid Ammonia: A Quantum Mechanical Charge Field (QMCF) Molecular Dynamics Study
https://doi.org/10.22146/ijc.26809 Wahyu Dita Saputri(1), Karna Wijaya(2), Ria Armunanto(3*)
(1) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(2) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(3) Department of Chemistry, Faculty of Mathematics and Natural Sciences, Universitas Gadjah Mada, Sekip Utara, Yogyakarta 55281, Indonesia
(*) Corresponding Author
Abstract
A quantum mechanical charge field (QMCF) molecular dynamics (MD) simulation has been carried out to describe the structural and dynamical properties of Cu+ ion in liquid ammonia. The first and second shells were treated by ab initio quantum mechanics at the Hartree−Fock (HF) level with the DZP-Dunning basis set for ammonia and LANL2DZ ECP basis set for Cu. The system was equilibrated for 4 ps, then the trajectory data was collected every fifth step for 20 ps at 235.15 K. The structural analysis showed that in the first solvation shell, Cu+ is solvated by 4 ammonia molecules forming a stable structure of tetrahedral with Cu-N bond length of 2.15 Å, whereas in the second solvation shell there are 29 ammonia molecules that have an average distance of 4.79 Å to Cu+ ion. Mean residence time of 3.06 ps was observed for the ammonia ligand in the second solvation shell indicating for a highly unstable structure of the solvation shell. The obtained structure of the first solvation shell from this simulation is in excellent agreement with experimental data.
Keywords
Full Text:
Full Text PDFReferences
[1] Feng, S., dos Santos, M.C., Bruno R. Carvalho, B.R., Lv, R., Li, Q., Fujisawa, K., Elías, A.L., Lei, Y., Perea-López, N., Endo, M., Pan, M., Pimenta, M.A., and Terrones, M., 2016, Ultrasensitive molecular sensor using N-doped graphene through enhanced Raman scattering, Sci. Adv., 2 (7), 1–13.
[2] Wei, F., Zhang, T., Liu, X., Li, X., Jiang, N., Liu, Z., Bian, Z., Zhao, Y., Lu, Z., and Huang, C., 2014, Efficient nondoped organic light-emitting diodes with CuI complex emitter, Org. Electron., 15 (11), 3292–3297.
[3] Hakim, L., Saputri, W.D., and Ulfa, S.M., 2016 Molecular dynamics simulation of a reversible hydrophobic-hydrophilic functionalized surface, Proceeding of the International Electronics Symposium (IES), 9-30 September 2016, Denpasar, Indonesia, 215–218.
[4] Vita, N., Landolfi, G., Baslé, A., Platsaki, S., Lee, J., Waldron, K.J., and Dennison, C., 2016, Bacterial cytosolic proteins with a high capacity for Cu(I) that protect against copper toxicity, Sci. Rep., 6, 39065.
[5] Chmielarz, L., and Jabłońska, M., 2015, Advances in selective catalytic oxidation of ammonia to dinitrogen: A review, RSC Adv., 5, 43408–43431.
[6] Kwak, J.H., Lee, J.H., Burton, S.D., Lipton, A.S., Peden, C.H.F., and Szanyi, J., 2013, A common intermediate for N2 formation in enzymes and zeolites : Side-on Cu–nitrosyl complexes, Angew. Chem.Int. Ed., 52 (10), 9985–9989.
[7] Inoue, K., Ohashi, K., Iino, T., Judai, K., Nishi, N., and Sekiya, H., 2007, Coordination and solvation of copper ion: Infrared photodissociation spectroscopy of Cu+(NH3)n (n = 3-8), Phys. Chem. Chem. Phys., 9 (34), 4793–4802.
[8] Nilsson, K.B., and Persson I., 2004, The coordination chemistry of copper(I) in liquid ammonia, trialkyl and triphenyl phosphite, and tri-n-butylphosphine solution, Dalton Trans., 9, 1312–1319.
[9] Holland, P.M., and Castleman, A.W., 1982, Thomson equation revisited in light of ion-clustering experiments, J. Phys. Chem., 86 (21), 4181–4188.
[10] Rode, B.M., Hofer, T.S., Randolf, B.R., Schwenk, C.F., Xenides, D., and Vchirawongkwin, V., 2005, Ab initio quantum mechanical charge field (QMCF) molecular dynamics: A QM/MM - MD procedure for accurate simulations of ions and complexes, Theor. Chem. Acc., 115 (2-3), 77–85.
[11] Hofer, T.S., Rode, B.M., Pribil, A.B., and Randolf, B.R., 2010, Simulations of liquids and solutions based on quantum mechanical forces, Adv. Inorg. Chem., 62 (10), 143–175.
[12] Weiss, A.K.H., Hofer, T.S., and Kurt, M.A., 2013, Exploiting the capabilities of quantum chemical simulations to characterise the hydration of molecular compounds Alexander, RSC Adv., 3 (6), 1606–1635.
[13] Canaval, L.R., and Rode, B.M., 2014, The hydration properties of Eu(II) and Eu(III): An ab initio quantum mechanical molecular dynamics study, Chem. Phys. Lett., 618, 78–82.
[14] Hofer, T.S., Rode, B.M., Pribil, A.B., and Randolf, B.R., 2010, Ab initio quantum mechanical charge field molecular dynamics: a nonparametrized first-principle approach to liquids and solutions, Adv. Quantum Chem., 59, 213–246.
[15] Messner, C.B., Lutz, O.M.D., Rainer, M., Huck, C.W., Hofer, T.S., Rode, B.M., and Bonn, G.K., 2014, Structure and dynamics of chromatographically relevant Fe(III)-chelates, J. Phys. Chem. B, 118 (42), 12232–12238.
[16] Kirkwood, J.G., and Boggs, E.M., 1942, The radial distribution function in liquids, J. Chem. Phys., 10, 394–402.
[17] Hofer, T.S., Tran, H.T., Schwenk, C.F., and Rode, B.M., 2004, Characterization of dynamics and reactivities of solvated ions by ab initio simulations, J. Comput. Chem., 25 (2), 211–217.
[18] Berendsen, H.J.C., Postma, J.P.M., van Gunsteren, W.F., Dinola, A., and Haak, J.R., 1984, Molecular dynamics with coupling to an external bath, J. Chem. Phys., 81, 3684–3690.
[19] Wadt, W.R., Hay, P.J., Wadt, W.A., and Hay, P.J., 1985, Ab initio effective core potentials for molecular calculations. Potentials for main group elements Na to Bi, J. Chem. Phys., 82, 284–298.
[20] Dunning, T.H., 1970, Gaussian basis functions for use in molecular calculations. I. Contraction of (9s5p) atomic basis sets for the first-row atoms, J. Chem. Phys., 53 (7), 2823–2833.
[21] Steffen, C., Thomas, K., Huniar, U., Hellweg, A., Rubner, O., and Schroer, A., 2010, TmoleX--a graphical user interface for turbomole, J. Comput. Chem., 31 (16), 2967–2970.
[22] Ahlrichs, R., Bar, M., Marco, H., Horn, H., and Ktjlmel, C., 1989, Electronic structure calculations on workstation computers: The program system turbomole, Chem. Phys. Lett., 162 (3), 165–169.
[23] Humphrey, W., Dalke, A., and Schulten, K., 1996, VMD : Visual molecular dynamics, J. Mol. Graphics, 14 (1), 33–38.
[24] Wu, D.Y., Hayashi, M., Shiu, Y.J., Liang, K.K., Chang, C.H., Yeh, Y.L., and Lin, S.H., 2003, A A quantum chemical study of bonding interaction, vibrational frequencies, force constants, and vibrational coupling of pyridine-Mn (M = Cu, Ag, Au; n = 2-4), J. Phys. Chem. A, 107, 9658–9667.
[25] Keller, S., Pertegás, A., Longo, G., Martínez, L., Cerdá, J., Junquera-Hernández, J.M., Prescimone, A., Constable, E.C., Housecroft, C.E., Ortí, E., and Bolink, H.J., 2016, Shine bright or live long: Substituent effects in [Cu(N^N)(P^P)]+-based light-emitting electrochemical cells where N^N is a 6-substituted 2,2′-bipyridine, J. Mater. Chem. C, 4 (17), 3857–3871.
[26] Pranowo, H.D., Setiaji, A.H.B., and Rode, B.M., 1999, Cu+ in liquid ammonia and in water: Intermolecular potential function and Monte Carlo simulation, J. Phys. Chem. A, 103 (1), 11115–11120.
DOI: https://doi.org/10.22146/ijc.26809
Article Metrics
Abstract views : 2813
| 
views : 4019
Copyright (c) 2017 Indonesian Journal of Chemistry
This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.
Indonesian Journal of Chemistry (ISSN 1411-9420 /e-ISSN 2460-1578) - Chemistry Department, Universitas Gadjah Mada, Indonesia.