Interactions of Al(III), La(III), Gd(III), and Lu(III) with the fused silica/water interface studied by second harmonic generation

David S. Jordan, Jessica N. Malin, Franz M. Geiger

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23 Scopus citations

Abstract

The interactions of the trivalent metal cations Al(III), La(III), Gd(III), and Lu(III) with the silica/water interface were studied using the nonlinear optical technique of second harmonic generation (SHG). Specifically, the Eisenthal (3) technique was used to quantify the thermodynamics of trivalent ion adsorption to the bare fused silica surface. SHG adsorption isotherms were measured and fit with the triple layer surface complexation model to obtain adsorption free energies, binding constants, and interfacial charge densities. The adsorption free energy for Al(III) was found to be 37.2(5) kJ/mol, while the adsorption free energies for the three trivalent lanthanide cations ranged from 29.9(9) to 32.2(7) kJ/mol. Despite identical ionic charges, the metals under investigation displayed different affinities for the fused silica/water interface, and this finding is analyzed and interpreted in the context of size-dependent metal cation properties and metal ion speciation. The thermodynamic results from this work are valuable benchmarks for computer simulations of trivalent metal transport in the environment.

Original languageEnglish (US)
Pages (from-to)5862-5867
Number of pages6
JournalEnvironmental Science and Technology
Volume44
Issue number15
DOIs
StatePublished - Aug 1 2010

ASJC Scopus subject areas

  • General Chemistry
  • Environmental Chemistry

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