Hostname: page-component-586b7cd67f-t7fkt Total loading time: 0 Render date: 2024-11-29T07:27:39.434Z Has data issue: false hasContentIssue false
  • English
  • Français

H2S and HS- Adsorption on a Charged Cu Surface in an Electrolyte: Effect of Ionic Strength

Published online by Cambridge University Press:  10 February 2011

W. D. Wilson  and
C. M. Schaldach
W. D. Wilson
Affiliation:
Sandia National Laboratories, Livermore, CA 94550
C. M. Schaldach
Affiliation:
University of California, Berkeley, CA 94720
Get access

Abstract

We present a method for the calculation of the binding and rotational energies of neutral (H2S) and charged (HS-) molecules impinging upon a charged (Cu <100>) surface in the presence of an electrolyte. A molecular surface is constructed surrounding the H2S and HS- molecules forming boundary elements. A coupled Schrödinger-Poisson-Boltzmann iterative procedure treats the electronic structure of the molecules at the 6–31G**/MP2 level of theory and includes solvation effects through the single and double layers of charge induced by the electronic distribution. The molecule, together with its charged layers, forms a Molecular Single and Double Layer (MSDL), an object which then interacts with a Gouy-Chapman plane within the electrolyte. The additional induced charge at the molecular surface resulting from this electric field is obtained by solving a second set of boundary element equations. Repulsive interactions between the atoms of the molecule and those of the surface are obtained using a rigid-ion Hartree-Fock method. Binding energies of the molecule to the surface are determined as a function of the real surface charge imposed and also the ionic strength of the solution. It is found that surface charges can completely (180°) reorient these molecules and that the counterions in the solution can completely screen binding effects of even large surface charges.

Work supported by the United States Department of Energy under contract #DE-AC04–94AL85000.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 492: Symposium S – Microscopic Simulation of Interfacial Phenomena in Solids… , 1997 , 207
Copyright
Copyright © Materials Research Society 1998

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

REFERENCES

1. Huang, H.H., Tsai, W.-T., Lee, J.-T., Corrosion 52, 708 (1996).Google Scholar
2. Galtayries, A. and Bonnelle, J.-P., Surface and Interface Analysis 23, 71 (1995).Google Scholar
3. Tidblad, J. and Graedel, T.E., Corrosion Science 38, 2201 (1996).Google Scholar
4. Graedel, T.E., et al, Corrosion Science 25, 1163 (1985).Google Scholar
5. Gadre, S.R., Pundlik, S.S., Shrivastava, I.H., Proc. Indian Acad. Sci. (Chem. Sci.) 106, 303 (1994).Google Scholar
6. Chipot, C., et al, J. Phys. Chem. 96, 10276 (1992).Google Scholar
7. Wilson, W.D., Schaldach, C.M., Bourcier, W.L., Chem. Phys. Lett. 267, 431 (1997).Google Scholar
8. Gouy, G., J. Phys. 9, 457 (1910); Ann. Phys. 7, 129 (1917).Google Scholar
9. Chapman, D.L., Phil. Mag. 25, 475 (1913).Google Scholar
10. Israelachvili, J.N., Intermolecular and Surface Forces. (Academic Press, London, 1992).Google Scholar
11. Jackson, J.D., Classical Electrodynamics. (John Wiley and Sons, New York, 1962).Google Scholar
12. Wilson, W.D. and Schaldach, C.M., Proc. Int. Conf. on Corrosion, Montreal, May, 1997.Google Scholar
13. Wilson, W.D. and Bisson, C.L., Phys. Rev. B 3, 3984 (1971). A similar method was independently introduced byGoogle Scholar
Gordon, R.G. and Kim, Y.S., J. Chem. Phys. 56, 3122 (1972).Google Scholar
14. Finnis, M.W., Acta. Metall. Mater. Suppl. 40, S25 (1992).Google Scholar