The Effects of Oxidation States and Spin States of Chromium Interaction with <i>Sargassum Sp</i>.: A Spectroscopic and Density Functional Theoretical Study — Oak Academic Publishing
Research ArticleOpen AccessGoogle Scholar indexed
The Effects of Oxidation States and Spin States of Chromium Interaction with <i>Sargassum Sp</i>.: A Spectroscopic and Density Functional Theoretical Study
Centre for Advanced Research in Sciences (CARS), Dhaka University, Dhaka, Bangladesh
,
Department of Chemistry, Dhaka University, Dhaka, Bangladesh
,
National University, Gazipur, Bangladesh
,
Department of Theoretical and Computational Chemistry, Dhaka University, Dhaka, Bangladesh
,
Department of Theoretical and Computational Chemistry, Dhaka University, Dhaka, Bangladesh
,
Department of Theoretical and Computational Chemistry, Dhaka University, Dhaka, Bangladesh
1 Centre for Advanced Research in Sciences (CARS), Dhaka University, Dhaka, Bangladesh
2 Department of Chemistry, Dhaka University, Dhaka, Bangladesh
3 National University, Gazipur, Bangladesh
4 Department of Theoretical and Computational Chemistry, Dhaka University, Dhaka, Bangladesh
5 Department of Theoretical and Computational Chemistry, Dhaka University, Dhaka, Bangladesh
6 Department of Theoretical and Computational Chemistry, Dhaka University, Dhaka, Bangladesh
The study of various oxidation states of chromium with Sargassum sp . is of particular interest since hexavalent chromium is reduced to trivalent chromium in an aqueous solution. In this study, a systematic density functional theory (DFT) calculations were performed to study the interactions of transition metal chromium ion with different oxidation states and spin states with the Sar gassum sp . decorated with carboxylate (acetate) at the wB97XD/6-311++ G(d,p) level of theory. The structures and binding energies of chromium met al - carboxylate complexes at various oxidation states and spin states in gas phase were examined. The coordination strength of Cr(VI) with the acetate ligand was predominantly the strongest compare d to the other oxidation states. Vibrational frequency analysis, for the homoleptic monomers of tris [ Cr III (AC) 3 ] 0 and [Cr VI (AC) 3 ] 3+ complexes, illustrate good harmony with the experimental and theoretical calculated frequencies. Using the time - dependent DFT (TD-DFT) at the level of CAM-B3LYP/6-311++G(d,p), the vertical excitation energies were obtained. The stabilization energies derived using the second order perturbation theory, E ij (2) , of NBO analysis confirmed the greater charge transfer for the observed trends in the metal binding. The calculated binding energies (ΔE) and interactions energies S E ij (2) favor the formation of [Cr VI (AC) 3 ] 3+ complexes. The findings of this study identify efficient electronic factors as major contributors to the metal binding affinities, with promising possibilities for the design of metal-ligand complexes and sensing of the metal ions.
KeywordsTransition MetalTime Dependent Density Functional TheoryBinding EnergySpectroscopyElectronic Properties and Homoleptic Coordinated Complex
Shupack, S.I. (1991) The Chemistry of Chromium and Some Resulting Analytical Problems. Environmental Health Perspectives, 92, 7-11. https://doi.org/10.1289/ehp.91927
Campbell, J.A. and Whiteker, R.A. (1969) A Periodic Table Based on Potential-pH Diagrams. Journal of Chemical Education, 46, 90-92. https://doi.org/10.1021/ed046p90
Mitewa, M. and Bontchev, P. (1985) Chromium (V) Coordination Chemistry. Co-Ordination Chemistry Reviews, 61, 241-272. https://doi.org/10.1016/0010-8545(85)80006-0
Dittert, I.M., Vilar, V.J.P., da Silva, E.A.B., de Souza, S.M.A.G.U., de Souza, A.A.U., Botelho, C.M.S. and Boaventura, R.A.R. (2012) Adding Value to Marine Macro-Algae Laminaria digitata through Its Use in the Separation and Recovery of Trivalent Chromium Ions from Aqueous Solution. Chemical Engineering Journal, 193-194, 348-357. https://doi.org/10.1016/j.cej.2012.04.048
Zheng, Y.-M., Liu, T., Jiang, J., Yang, L., Fan, Y., Wee, A.T.S. and Chen, J.P. (2011) Characterization of Hexavalent Chromium Interaction with Sargassum by X-Ray Absorption Fine Structure Spectroscopy, X-Ray Photoelectron Spectroscopy, and Quantum Chemistry Calculation. Journal of Colloid and Interface Science, 356, 741-748. https://doi.org/10.1016/j.jcis.2010.12.070
Mehandzhiyski, A.Y., Riccardi, E., van Erp, T.S., Koch, H., Åstrand, P.-O., Trinh, T.T. and Grimes, B.A. (2015) Density Functional Theory Study on the Interactions of Metal Ions with Long Chain Deprotonated Carboxylic Acids. Journal of Physical Chemistry A, 119, 10195-10203. https://doi.org/10.1021/acs.jpca.5b04136
Turowski, P.N., Bino, A. and Lippard, S.J. (1990) μ-Hydroxobis(μ-forma-to)hexaaquadichromium(III), an Intermediate in the Formation of Basic Chromium Carboxylates. Angewandte Chemie International Edition English, 29, 811-812. https://doi.org/10.1002/anie.199008111
Ellis, T., Glass, M., Harton, A., Folting, K., Huffman, J.C. and Vincent, J.B. (1994) Synthetic Models for Low-Molecular-Weight Chromium-Binding Substance: Synthesis and Characterization of Oxo-Bridged Tetranuclear Chromium(III) Assemblies. Inorganic Chemistry, 33, 5522-5527. https://doi.org/10.1021/ic00102a028
Eshel, M., Bino, A., Felner, I., Johnston, D.C., Luban, M. and Miller, L.L. (2000) Poly-Nuclear Chromium (III) Carboxylates. 1. Synthesis, Structure, and Magnetic Properties of an Octanuclear Complex with a Ring Structure. Inorganic Chemistry, 39, 1376-1380. https://doi.org/10.1021/ic9907009
Blann, K., Bollmann, A., de Bod, H., Dixon, J.T., Killian, E., Nongodlwana, P., Maumela, M.C., Maumela, H., McConnell, A.E., Morgan, D.H., Overett, M.J., Prétorius, M., Kuhlmann, S. and Wasserscheid, P. (2007) Ethylene Tetramerisation: Subtle Effects Exhibited by N-Substituted Diphosphinoamine Ligands. Journal of Catalysis, 249, 244-249. https://doi.org/10.1016/j.jcat.2007.04.009
Rao, C.N.R., Natarajan, S. and Vaidhyanathan, R. (2004) Metal Carboxylates with Open Architectures. Angewandte Chemie International Edition English, 43, 1466-1496. https://doi.org/10.1002/anie.200300588
Warner, A. (1908) ZurTheorie der Beizenfarbstoffe. Berichte der Deutschen Chemischen Gesellschaft, 41, 2383-2386. https://doi.org/10.1002/cber.190804102149
Kambe, K. (1950) On the Paramagnetic Susceptibilities of Some Polynuclear Complex Salts. Journal of Physical Society Japan, 5, 48-51. https://doi.org/10.1143/JPSJ.5.48
Erre, L.S., Micera, G., Glowiak, T. and Kozlowski, H. (1997) Chromium(III) Acetate, Chromium(III) Acetate Hydroxide, or μ3-Oxo-esakis-(μ2-acetato-O,O’) Tria-quatrichromium(III) Acetate? Determining the Structure of a Complex Compound by Analytical and Spectroscopic Methods. Journal of Chemical Education, 74, 432. https://doi.org/10.1021/ed074p432
Kapoor, R. and Sharma, R. (1983) Anhydrous Chromium(III) Carboxylates: Reactions of CrO3 with Carboxylic Acid Anhydrides. Zeitschrift für Naturforschung, 38, 42. https://doi.org/10.1515/znb-1983-0110
Sydora, O.L., Hart, R.T., Eckert, N.A., Martinez Baez, E., Clark, A.E. and Benmore, C.J. (2018) A Homoleptic Chromium(III) Carboxylate. Dalton Transactions, 47, 4790-4793. https://doi.org/10.1039/C8DT00029H
Matin, M.A., Mazharul, M.I., Bredow, T. and Aziz, M.A. (2017) The Effects of Oxidation States, Spin States and Solvents on Molecular Structure, Stability and Spectroscopic Properties of Fe-Catechol Complexes: A Theoretical Study. Advances in Chemical Engineering and Science, 7, 137-153. https://doi.org/10.4236/aces.2017.72011
Foster, J.P. and Weinhold, F. (1980) Natural Hybrid Orbitals. Journal American Chemical Society, 102, 7211-7218. https://doi.org/10.1021/ja00544a007
Reed, A.E. and Weinhold, F. (1983) Natural Bond Orbital Analysis of Near-Hartree-Fock Water Dimer. Journal of Chemical Physics, 78, 4066-4073. https://doi.org/10.1063/1.445134
Pearson, R.G. (1993) The Principle of Maximum Hardness. Accounts of Chemical Research, 26, 250-255. https://doi.org/10.1021/ar00029a004
Pearson, R.G. (1992) The Electronic Chemical Potential and Chemical Hardness. Journal of Molecular Structure: THEOCHEM, 255, 261-270. https://doi.org/10.1016/0166-1280(92)85014-C
Parr, R.G., Szentpály, L.V. and Liu, S. (1999) Electrophilicity Index. Journal of American Chemical Society, 121, 1922-1924. https://doi.org/10.1021/ja983494x
Chai, J.-D. and Head-Gordon, M. (2008) Long-Range Corrected Hybrid Density Functionals with Damped Atom-Atom Dispersion Corrections. Physical Chemistry Chemical Physics, 10, 6615-6620. https://doi.org/10.1039/b810189b
Rassolov, V.A., Pople, J.A., Ratner, M.A. and Windus, T.L. (1998) 6-31G* Basis Set for Atoms K through Zn. Journal of Chemical Physics, 109, 1223-1229. https://doi.org/10.1063/1.476673
Ditchfield, R., Hehre, W.J. and Pople, J.A. (1971) Self-Consistent Molecular-Orbital Methods. IX. An Extended Gaussian-Type Basis for Molecular-Orbital Studies of Organic Molecules. Journal of Chemical Physics, 54, 724-728. https://doi.org/10.1063/1.1674902
Hehre, W.J., Ditchfield, R. and Pople, J.A. (1972) Self-Consistent Molecular Orbital Methods. XII. Further Extensions of Gaussian-Type Basis Sets for Use in Molecular Orbital Studies of Organic Molecules. Journal of Chemical Physics, 56, 2257-2261. https://doi.org/10.1063/1.1677527
Frisch, M.J., Trucks, G.W., Schlegel, H.B., Scuseria, G.E., Robb, M.A., Cheeseman, J.R., Scalmani, G., Barone, V., Petersson, G.A., Nakatsuji, H., Li, X., Caricato, M., Marenich, A.V., Bloino, J., Janesko, B.G., Gomperts, R., Mennucci, B., Hratchian, H.P., Ortiz, J.V., Izmaylov, A.F., Sonnenberg, J.L., Williams-Young, D., Ding, F., Lipparini, F., Egidi, F., Goings, J., Peng, B., Petrone, A., Henderson, T., Ranasinghe, D., Zakrzewski, V.G., Gao, J., Rega, N., Zheng, G., Liang, W., Hada, M., Ehara, M., Toyota, K., Fukuda, R., Hasegawa, J., Ishida, M., Nakajima, T., Honda, Y., Kitao, O., Nakai, H., Vreven, T., Thros-sell, K., Montgomery, J.A., Peralta, J.E., Ogliaro, F., Bearpark, M.J., Heyd, J.J., Brothers, E.N., Kudin, K.N., Staroverov, V.N., Keith, T.A., Kobayashi, R., Normand, J., Raghavacha-ri, K., Rendell, A.P., Burant, J.C., Iyengar, S.S., Tomasi, J., Cossi, M., Millam, J.M., Klene, M., Adamo, C., Cammi, R., Ochterski, J.W., Martin, R.L., Morokuma, K., Farkas, O., Foresman, J.B. and Fox, D.J. (2016) Gaussian 16, Revision B.01. Gaussian, Inc., Wallingford.
Matin, M.A., Chitumalla, R.K., Lim, M., Gao, X. and Jang, J. (2015) Density Functional Theory Study on the Cross-Linking of Mussel Adhesive Proteins. Journal of Physical Chemistry B, 119, 5496-5504. https://doi.org/10.1021/acs.jpcb.5b01152
Spellmeyer, D.C. (2005) Annual Reports in Computational Chemistry. Elsevier, Amsterdam.
Yanai, T., Tew, D.P. and Handy, N.C. (2004) A New Hybrid Exchange-Correlation Functional Using the Coulomb-Attenuating Method (CAM-B3LYP). Chemical Physics Letters, 393, 51-57. https://doi.org/10.1016/j.cplett.2004.06.011
Sutton, C.C.R., da Silva, G. and Franks, G.V. (2015) Modeling the IR Spectra of Aqueous Metal Carboxylate Complexes: Correlation between Bonding Geometry and Stretching Mode Wavenumber Shifts. Chemistry—A European Journal, 21, 6801-6805. https://doi.org/10.1002/chem.201406516
Deacon, G.B. and Phillips, R.J. (1980) Relationships between the Carbon-Oxygen Stretching Frequencies of Carboxylato Complexes and the Type of Carboxylate Coordination. Coordination Chemistry Reviews, 33, 227-250. https://doi.org/10.1016/S0010-8545(00)80455-5
Hsu, L.-Y. and Nordman, C.E. (1983) Structures of Two Forms of Sodium Acetate, Na + C 2 H 3 O 2 - . Acta Crystallographica Section C, 39, 690-694. https://doi.org/10.1107/S0108270183005946
Boys, S.F. and Bernardi, F. (1970) The Calculation of Small Molecular Interactions by the Differences of Separate Total Energies. Some Procedures with Reduced Errors. Molecular Physics, 19, 553-566. https://doi.org/10.1080/00268977000101561
Barone, V. and Cossi, M. (1998) Quantum Calculation of Molecular Energies and Energy Gradients in Solution by a Conductor Solvent Model. Journal of Physical Chemistry A, 102, 1995-2001. https://doi.org/10.1021/jp9716997
Cossi, M., Rega, N., Scalmani, G. and Barone, V. (2003) Energies, Structures, and Electronic Properties of Molecules in Solution with the C-PCM Solvation Model. Journal Computational Chemistry, 24, 669-681. https://doi.org/10.1002/jcc.10189
Tomasi, J., Mennucci, B. and Cammi, R. (2005) Quantum Mechanical Continuum Solvation Models. Chemical Review, 105, 2999-3094. https://doi.org/10.1021/cr9904009
Quintelas, C., Rocha, Z., Silva, B., Fonseca, B., Figueiredo, H. and Tavares, T. (2009) Removal of Cd(II), Cr(VI), Fe(III) and Ni(II) from Aqueous Solutions by an E. coli Bio-Film Supported on Kaolin. Chemical Engineering Journal, 149, 319-324. https://doi.org/10.1016/j.cej.2008.11.025
Aksoy and Özer, M.S.U. (2003) Potentiometric and Spectroscopic Studies with Chromium(III) Complexes of Hydroxysalicylic Acid Derivatives in Aqueous Solution. Turkish Journal Chemistry, 27, 667-673.
Valencia-Centeno, Y., Ureña-Núñez, F., Sánchez-Mendieta, V., Morales-Luckie, R.A., López-Castañares, R. and Huerta, L. (2008) Synthesis and Structural Characterization of Tris(methacrylato)chromium(III). Journal of Coordination Chemistry, 61, 1589-1598. https://doi.org/10.1080/00958970701599611
Reed, A.E., Weinstock, R.B. and Weinhold, F. (1985) Natural Population Analysis. Journal of Chemical Physics, 83, 735-746. https://doi.org/10.1063/1.449486
Singh, U.C. and Kollman, P.A. (1984) An Approach to Computing Electrostatic Charges for Molecules. Journal of Computational Chemistry, 5, 129-145. https://doi.org/10.1002/jcc.540050204
Breneman, C.M. and Wiberg, K.B. (1990) Determining Atom-Centered Monopoles from Molecular Electrostatic Potentials. The Need for High Sampling Density in Formamide Conformational Analysis, Journal of Computational Chemistry, 11, 361-373. https://doi.org/10.1002/jcc.540110311
Chirlian, L.E. and Francl, M.M. (1987) Atomic Charges Derived from Electrostatic Potentials: A Detailed Study. Journal of Computational Chemistry, 8, 894-905. https://doi.org/10.1002/jcc.540080616
Hu, H., Lu, Z. and Yang, W. (2007) Fitting Molecular Electrostatic Potentials from Quantum Mechanical Calculations. Journal of Chemical Theory and Computation, 3, 1004-1013. https://doi.org/10.1021/ct600295n
Reed, A.E., Curtiss, L.A. and Weinhold, F. (1988) Intermolecular Interactions from a Natural Bond Orbital, Donor-Acceptor Viewpoint. Chemical Review, 88, 899-926. https://doi.org/10.1021/cr00088a005